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Sample records for fuel isotopic composition

  1. Usage of burnt fuel isotopic compositions from engineering codes in Monte-Carlo code calculations

    Energy Technology Data Exchange (ETDEWEB)

    Aleshin, Sergey S.; Gorodkov, Sergey S.; Shcherenko, Anna I. [Nuclear Research Centre ' ' Kurchatov Institute' ' , Moscow (Russian Federation)

    2015-09-15

    A burn-up calculation of VVER's cores by Monte-Carlo code is complex process and requires large computational costs. This fact makes Monte-Carlo codes usage complicated for project and operating calculations. Previously prepared isotopic compositions are proposed to use for the Monte-Carlo code (MCU) calculations of different states of VVER's core with burnt fuel. Isotopic compositions are proposed to calculate by an approximation method. The approximation method is based on usage of a spectral functionality and reference isotopic compositions, that are calculated by engineering codes (TVS-M, PERMAK-A). The multiplication factors and power distributions of FA and VVER with infinite height are calculated in this work by the Monte-Carlo code MCU using earlier prepared isotopic compositions. The MCU calculation data were compared with the data which were obtained by engineering codes.

  2. Derivation of correction factor to be applied for calculated results of PWR fuel isotopic composition by ORIGEN2 code

    Energy Technology Data Exchange (ETDEWEB)

    Suyama, Kenya; Nomura, Yasushi [Japan Atomic Energy Research Inst., Tokai, Ibaraki (Japan). Tokai Research Establishment; Murazaki, Minoru [Tokyo Nuclear Service Inc., Tokyo (Japan); Mochizuki, Hiroki [The Japan Research Institute Ltd., Tokyo (Japan)

    2001-11-01

    For providing conservative PWR spent fuel compositions from the view point of nuclear criticality safety, correction factors applicable for result of burnup calculation by ORIGEN2 were evaluated. Its conservativeness was verified by criticality calculations using MVP. To calculate these correction factors, analyses of spent fuel isotopic composition data were performed by ORIGEN2. Maximum or minimum value of the ratio of calculation result to experimental data was chosen as correction factor. These factors are given to each set of fuel assembly and ORIGEN2 library. They could be considered as the re-definition of recommended isotopic composition given in Nuclear Criticality Safety Handbook. (author)

  3. Validation of the scale system for PWR spent fuel isotopic composition analyses

    Energy Technology Data Exchange (ETDEWEB)

    Hermann, O.W.; Bowman, S.M.; Parks, C.V. [Oak Ridge National Lab., TN (United States); Brady, M.C. [Sandia National Laboratories, Las Vegas, NV (United States)

    1995-03-01

    The validity of the computation of pressurized-water-reactor (PWR) spent fuel isotopic composition by the SCALE system depletion analysis was assessed using data presented in the report. Radiochemical measurements and SCALE/SAS2H computations of depleted fuel isotopics were compared with 19 benchmark-problem samples from Calvert Cliffs Unit 1, H. B. Robinson Unit 2, and Obrigheim PWRs. Even though not exhaustive in scope, the validation included comparison of predicted and measured concentrations for 14 actinides and 37 fission and activation products. The basic method by which the SAS2H control module applies the neutron transport treatment and point-depletion methods of SCALE functional modules (XSDRNPM-S, NITAWL-II, BONAMI, and ORIGEN-S) is described in the report. Also, the reactor fuel design data, the operating histories, and the isotopic measurements for all cases are included in detail. The underlying radiochemical assays were conducted by the Materials Characterization. Center at Pacific Northwest Laboratory as part of the Approved Testing Material program and by four different laboratories in Europe on samples processed at the Karlsruhe Reprocessing Plant.

  4. Nitrogen Isotope Composition of Thermally Produced NOx from Various Fossil-Fuel Combustion Sources.

    Science.gov (United States)

    Walters, Wendell W; Tharp, Bruce D; Fang, Huan; Kozak, Brian J; Michalski, Greg

    2015-10-06

    The nitrogen stable isotope composition of NOx (δ(15)N-NOx) may be a useful indicator for NOx source partitioning, which would help constrain NOx source contributions in nitrogen deposition studies. However, there is large uncertainty in the δ(15)N-NOx values for anthropogenic sources other than on-road vehicles and coal-fired energy generating units. To this end, this study presents a broad analysis of δ(15)N-NOx from several fossil-fuel combustion sources that includes: airplanes, gasoline-powered vehicles not equipped with a three-way catalytic converter, lawn equipment, utility vehicles, urban buses, semitrucks, residential gas furnaces, and natural-gas-fired power plants. A relatively large range of δ(15)N-NOx values was measured from -28.1‰ to 8.5‰ for individual exhaust/flue samples that generally tended to be negative due to the kinetic isotope effect associated with thermal NOx production. A negative correlation between NOx concentrations and δ(15)N-NOx for fossil-fuel combustion sources equipped with selective catalytic reducers was observed, suggesting that the catalytic reduction of NOx increases δ(15)N-NOx values relative to the NOx produced through fossil-fuel combustion processes. Combining the δ(15)N-NOx measured in this study with previous published values, a δ(15)N-NOx regional and seasonal isoscape was constructed for the contiguous U.S., which demonstrates seasonal and regional importance of various NOx sources.

  5. Nitrogen Stable Isotope Composition of Various Fossil-fuel Combustion Nitrogen Oxide Sources

    Science.gov (United States)

    Walters, W.; Michalski, G. M.; Fang, H.

    2015-12-01

    Nitrogen oxides (NOx = NO + NO2) are important trace gases that impact atmospheric chemistry, air quality, and climate. In order to help constrain NOx source contributions, the nitrogen (N) stable isotope composition of NOx (δ15N-NOx) may be a useful indicator for NOx source partitioning. However, despite anthropogenic emissions being the most prevalent source of NOx, there is still large uncertainty in the δ15N-NOx values for anthropogenic sources. To this end, this study provides a detailed analysis of several fossil-fuel combustion NOx sources and their δ15N-NOx values. To accomplish this, exhaust or flue samples from several fossil-fuel combustion sources were sampled and analyzed for their δ15N-NOx that included airplanes, gasoline-powered vehicles not equipped with a catalytic converter, gasoline-powered lawn tools and utility vehicles, diesel-electric buses, diesel semi-trucks, and natural gas-burning home furnace and power plant. A relatively large range of δ15N-NOx values were measured from -28.1 to 0.3‰ for individual exhaust/flue samples with cold started diesel-electric buses contributing on average the lowest δ15N-NOx values at -20.9‰, and warm-started diesel-electric buses contributing on average the highest values of -1.7‰. The NOx sources analyzed in this study primarily originated from the "thermal production" of NOx and generally emitted negative δ15N-NOx values, likely due to the kinetic isotope effect associated with its production. It was found that there is a negative correlation between NOx concentrations and δ15N-NOx for fossil-fuel combustion sources equipped with catalytic NOx reduction technology, suggesting that the catalytic reduction of NOx may have an influence on δ15N-NOx values. Based on the δ15N-NOx values reported in this study and in previous studies, a δ15N-NOx regional and seasonal isoscape was constructed for the contiguous United States. The constructed isoscape demonstrates the seasonal importance of various

  6. Evaluation of isotopic composition of fast reactor core in closed nuclear fuel cycle

    Science.gov (United States)

    Tikhomirov, Georgy; Ternovykh, Mikhail; Saldikov, Ivan; Fomichenko, Peter; Gerasimov, Alexander

    2017-09-01

    The strategy of the development of nuclear power in Russia provides for use of fast power reactors in closed nuclear fuel cycle. The PRORYV (i.e. «Breakthrough» in Russian) project is currently under development. Within the framework of this project, fast reactors BN-1200 and BREST-OD-300 should be built to, inter alia, demonstrate possibility of the closed nuclear fuel cycle technologies with plutonium as a main source of energy. Russia has a large inventory of plutonium which was accumulated in the result of reprocessing of spent fuel of thermal power reactors and conversion of nuclear weapons. This kind of plutonium will be used for development of initial fuel assemblies for fast reactors. The closed nuclear fuel cycle concept of the PRORYV assumes self-supplied mode of operation with fuel regeneration by neutron capture reaction in non-enriched uranium, which is used as a raw material. Operating modes of reactors and its characteristics should be chosen so as to provide the self-sufficient mode by using of fissile isotopes while refueling by depleted uranium and to support this state during the entire period of reactor operation. Thus, the actual issue is modeling fuel handling processes. To solve these problems, the code REPRORYV (Recycle for PRORYV) has been developed. It simulates nuclide streams in non-reactor stages of the closed fuel cycle. At the same time various verified codes can be used to evaluate in-core characteristics of a reactor. By using this approach various options for nuclide streams and assess the impact of different plutonium content in the fuel, fuel processing conditions, losses during fuel processing, as well as the impact of initial uncertainties on neutron-physical characteristics of reactor are considered in this study.

  7. A Fast Numerical Method for the Calculation of the Equilibrium Isotopic Composition of a Transmutation System in an Advanced Fuel Cycle

    Directory of Open Access Journals (Sweden)

    F. Álvarez-Velarde

    2012-01-01

    Full Text Available A fast numerical method for the calculation in a zero-dimensional approach of the equilibrium isotopic composition of an iteratively used transmutation system in an advanced fuel cycle, based on the Banach fixed point theorem, is described in this paper. The method divides the fuel cycle in successive stages: fuel fabrication, storage, irradiation inside the transmutation system, cooling, reprocessing, and incorporation of the external material into the new fresh fuel. The change of the fuel isotopic composition, represented by an isotope vector, is described in a matrix formulation. The resulting matrix equations are solved using direct methods with arbitrary precision arithmetic. The method has been successfully applied to a double-strata fuel cycle with light water reactors and accelerator-driven subcritical systems. After comparison to the results of the EVOLCODE 2.0 burn-up code, the observed differences are about a few percents in the mass estimations of the main actinides.

  8. Review of Technical Issues Related to Predicting Isotopic Compositions and Source Terms for High-Burnup LWR Fuel

    Energy Technology Data Exchange (ETDEWEB)

    Gauld, I. C.; Parks, C. V.

    2000-12-11

    This report has been prepared to review the technical issues important to the prediction of isotopic compositions and source terms for high-burnup, light-water-reactor (LWR) fuel as utilized in the licensing of spent fuel transport and storage systems. The current trend towards higher initial 235U enrichments, more complex assembly designs, and more efficient fuel management schemes has resulted in higher spent fuel burnups than seen in the past. This trend has led to a situation where high-burnup assemblies from operating LWRs now extend beyond the area where available experimental data can be used to validate the computational methods employed to calculate spent fuel inventories and source terms. This report provides a brief review of currently available validation data, including isotopic assays, decay heat measurements, and shielded dose-rate measurements. Potential new sources of experimental data available in the near term are identified. A review of the background issues important to isotopic predictions and some of the perceived technical challenges that high-burnup fuel presents to the current computational methods are discussed. Based on the review, the phenomena that need to be investigated further and the technical issues that require resolution are presented. The methods and data development that may be required to address the possible shortcomings of physics and depletion methods in the high-burnup and high-enrichment regime are also discussed. Finally, a sensitivity analysis methodology is presented. This methodology is currently being investigated at the Oak Ridge National Laboratory as a computational tool to better understand the changing relative significance of the underlying nuclear data in the different enrichment and burnup regimes and to identify the processes that are dominant in the high-burnup regime. The potential application of the sensitivity analysis methodology to help establish a range of applicability for experimental

  9. SCALE 5.1 Predictions of PWR Spent Nuclear Fuel Isotopic Compositions

    Energy Technology Data Exchange (ETDEWEB)

    Radulescu, Georgeta [ORNL; Gauld, Ian C [ORNL; Ilas, Germina [ORNL

    2010-03-01

    The purpose of this calculation report is to document the comparison to measurement of the isotopic concentrations for pressurized water reactor (PWR) spent nuclear fuel determined with the Standardized Computer Analysis for Licensing Evaluation (SCALE) 5.1 (Ref. ) epletion calculation method. Specifically, the depletion computer code and the cross-section library being evaluated are the twodimensional (2-D) transport and depletion module, TRITON/NEWT,2, 3 and the 44GROUPNDF5 (Ref. 4) cross-section library, respectively, in the SCALE .1 code system.

  10. Spent fuel isotopic composition data base system on WWW. SFCOMPO on W3

    Energy Technology Data Exchange (ETDEWEB)

    Suyama, Kenya [Japan Atomic Energy Research Inst., Tokai, Ibaraki (Japan). Tokai Research Establishment

    1997-11-01

    Spent Fuel Composition Data Base System `SFCOMPO` has been developed on IBM compatible PC. This data base system is not widely used, since users must purchase the data base software by themselves. `SFCOMPO on W3` is a system to overcome this problem. User can search and visualize the data in the data base by accessing WWW server through the Internet from local machine. Only a browsing software to access WWW should be prepared. It enables us to easily search data of spent fuel composition if we can access the Internet. This system can be operated on WWW server machine which supports use of Common Gateway Interface (CGI). This report describes the background of the development of SFCOMPO on W3 and is it`s user`s manual. (author)

  11. Monte-Carlo code calculation of 3D reactor core model with usage of burnt fuel isotopic compositions, obtained by engineering codes

    Energy Technology Data Exchange (ETDEWEB)

    Aleshin, Sergey S.; Gorodkov, Sergey S.; Shcherenko, Anna I. [National Research Centre ' Kurchatov Institute' , Moscow (Russian Federation)

    2016-09-15

    A burn-up calculation of large systems by Monte-Carlo code (MCU) is complex process and it requires large computational costs. Previously prepared isotopic compositions are proposed to be used for the Monte-Carlo code calculations of different system states with burnt fuel. Isotopic compositions are calculated by an approximation method. The approximation method is based on usage of a spectral functionality and reference isotopic compositions, that are calculated by the engineering codes (TVS-M, BIPR-7A and PERMAK-A). The multiplication factors and power distributions of FAs from a 3-D reactor core are calculated in this work by the Monte-Carlo code MCU using earlier prepared isotopic compositions. The separate conditions of the burnt core are observed. The results of MCU calculations were compared with those that were obtained by engineering codes.

  12. The scheme for evaluation of isotopic composition of fast reactor core in closed nuclear fuel cycle

    Science.gov (United States)

    Saldikov, I. S.; Ternovykh, M. Yu; Fomichenko, P. A.; Gerasimov, A. S.

    2017-01-01

    The PRORYV (i.e. «Breakthrough» in Russian) project is currently under development. Within the framework of this project, fast reactors BN-1200 and BREST-OD-300 should be built to, inter alia, demonstrate possibility of the closed nuclear fuel cycle technologies with plutonium as a main source of power. Russia has a large inventory of plutonium which was accumulated in the result of reprocessing of spent fuel of thermal power reactors and conversion of nuclear weapons. This kind of plutonium will be used for development of initial fuel assemblies for fast reactors. To solve the closed nuclear fuel modeling tasks REPRORYV code was developed. It simulates the mass flow for nuclides in the closed fuel cycle. This paper presents the results of modeling of a closed nuclear fuel cycle, nuclide flows considering the influence of the uncertainty on the outcome of neutron-physical characteristics of the reactor.

  13. Comment: collection of assay data on isotopic composition in LWR spent fuel

    Energy Technology Data Exchange (ETDEWEB)

    Naito, Yoshitaka; Kurosawa, Masayoshi; Suyama, Kenya [Japan Atomic Energy Research Inst., Tokai, Ibaraki (Japan). Tokai Research Establishment

    1997-03-01

    Many assay data of LWR spent fuels have been collected from reactors in the world and some of them are already stored in the database SFCOMPO which was constructed on a personal computer IBM PC/AT. On the other hand, Group constant libraries for burnup calculation code ORIGEN-II were generated from the nuclear data file JENDL3.2. These libraries were evaluated by using the assay data in SFCOMPO. (author)

  14. Zinc isotopic composition of particulate matter generated during the combustion of coal and coal + tire-derived fuels.

    Science.gov (United States)

    Borrok, David M; Gieré, Reto; Ren, Minghua; Landa, Edward R

    2010-12-01

    Atmospheric Zn emissions from the burning of coal and tire-derived fuel (TDF) for power generation can be considerable. In an effort to lay the foundation for tracking these contributions, we evaluated the Zn isotopes of coal, a mixture of 95 wt % coal + 5 wt % TDF, and the particulate matter (PM) derived from their combustion in a power-generating plant. The average Zn concentrations and δ(66)Zn were 36 mg/kg and 183 mg/kg and +0.24‰ and +0.13‰ for the coal and coal + TDF, respectively. The δ(66)Zn of the PM sequestered in the cyclone-type mechanical separator was the lightest measured, -0.48‰ for coal and -0.81‰ for coal+TDF. The δ(66)Zn of the PM from the electrostatic precipitator showed a slight enrichment in the heavier Zn isotopes relative to the starting material. PM collected from the stack had the heaviest δ(66)Zn in the system, +0.63‰ and +0.50‰ for the coal and coal + TDF, respectively. Initial fractionation during the generation of a Zn-rich vapor is followed by temperature-dependent fractionation as Zn condenses onto the PM. The isotopic changes of the two fuel types are similar, suggesting that their inherent chemical differences have only a secondary impact on the isotopic fractionation process.

  15. A sensitivity study on DUPIC fuel composition

    Energy Technology Data Exchange (ETDEWEB)

    Choi, Hang Bok; Roh, Gyu Hong

    1997-01-01

    In DUPIC fuel cycle, the spent pressurized water reactor (PWR) fuel is refabricated as a DUPIC fuel by a dry process. Because the spent PWR fuel composition depends on the initial enrichment and burnup condition of PWR fuel, the composition of a DUPIC fuel is not uniquely defined. Therefore, for the purpose of reducing the effects of such a composition heterogeneity on core performance, a composition adjustment of DUPIC fuel was studies. The composition adjustment was made in two steps: mixing two spent PWR fuel assemblies of higher and lower {sup 239}Pu contents and blending in fresh uranium with the mixed spent PWR fuels. Because the fuel and core performances depend on both the absolute amount of fissile isotopes and the ratio of major fissile isotope contents, a parametric study was performed to determine the reference compositions of {sup 235}U and {sup 239}Pu. The reference enrichments of {sup 235}U and {sup 239}Pu were determined such that the DUPIC core performance is comparable to that of a natural uranium core with high spent PWR fuel utilization and low fuel cycle cost. Under this condition, it is possible to utilize 90% of spent PWR fuels as the DUPIC fuel formula. On average, the amounts of slightly enriched and depleted uranium used for blending correspond to 8.6% and 10.6%, respectively, of the mass of candidate spent PWR fuels. (author). 16 refs., 30 tabs., 9 figs.

  16. Atomic Weights and Isotopic Compositions

    Science.gov (United States)

    SRD 144 Atomic Weights and Isotopic Compositions (Web, free access)   The atomic weights are available for elements 1 through 111, and isotopic compositions or abundances are given when appropriate.

  17. Determination of plutonium content in high burnup pressurized water reactor fuel samples and its use for isotope correlations for isotopic composition of plutonium.

    Science.gov (United States)

    Joe, Kihsoo; Jeon, Young-Shin; Han, Sun-Ho; Lee, Chang-Heon; Ha, Yeong-Keong; Song, Kyuseok

    2012-06-01

    The content of plutonium isotopes in high burnup pressurized water reactor fuel samples was examined using both alpha spectrometry and mass spectrometry after anion exchange separation. The measured values were compared with results calculated by the ORIGEN-2 code. On average, the ratios (m/c) of the measured values (m) over the calculated values (c) were 1.22±0.16 for (238)Pu, 1.02±0.14 for (239)Pu, 1.08±0.06 for (240)Pu, 1.06±0.16 for (241)Pu, and 1.13±0.08 for (242)Pu. Using the Pu data obtained in this work, correlations were derived between the alpha activity ratios of (238)Pu/((239)Pu+(240)Pu), the alpha specific activities of Pu, and the atom % abundances of the Pu isotopes. Using these correlations, the atom % abundances of the plutonium isotopes in the target samples were calculated. These calculated results agreed within a range from 2 to 8% of the experimentally derived values according to the isotopes of plutonium.

  18. Standard test method for analysis of isotopic composition of uranium in nuclear-grade fuel material by quadrupole inductively coupled plasma-mass spectrometry

    CERN Document Server

    American Society for Testing and Materials. Philadelphia

    2000-01-01

    1.1 This test method is applicable to the determination of the isotopic composition of uranium (U) in nuclear-grade fuel material. The following isotopic weight percentages are determined using a quadrupole inductively coupled plasma-mass spectrometer (Q-ICP-MS): 233U, 234U, 235U, 236U, and 238U. The analysis can be performed on various material matrices after acid dissolution and sample dilution into water or dilute nitric (HNO3) acid. These materials include: fuel product, uranium oxide, uranium oxide alloys, uranyl nitrate (UNH) crystals, and solutions. The sample preparation discussed in this test method focuses on fuel product material but may be used for uranium oxide or a uranium oxide alloy. Other preparation techniques may be used and some references are given. Purification of the uranium by anion-exchange extraction is not required for this test method, as it is required by other test methods such as radiochemistry and thermal ionization mass spectroscopy (TIMS). This test method is also described i...

  19. The effect of the composition of plutonium loaded on the reactivity change and the isotopic composition of fuel produced in a fast reactor

    Science.gov (United States)

    Blandinskiy, V. Yu.

    2014-12-01

    This paper presents the results of a numerical investigation into burnup and breeding of nuclides in metallic fuel consisting of a mixture of plutonium and depleted uranium in a fast reactor with sodium coolant. The feasibility of using plutonium contained in spent nuclear fuel from domestic thermal reactors and weapons-grade plutonium is discussed. It is shown that the largest production of secondary fuel and the least change in the reactivity over the reactor lifetime can be achieved when employing plutonium contained in spent nuclear fuel from a reactor of the RBMK-1000 type.

  20. Composite nuclear fuel assembly

    Energy Technology Data Exchange (ETDEWEB)

    Dollard, W.J.; Ferrari, H.M.

    1982-04-27

    An open lattice elongated nuclear fuel assembly including small diameter fuel rods disposed in an array spaced a selected distance above an array of larger diameter fuel rods for use in a nuclear reactor having liquid coolant flowing in an upward direction. Plenums are preferably provided in the upper portion of the upper smaller diameter fuel rods and in the lower portion of the lower larger diameter fuel rods. Lattice grid structures provide lateral support for the fuel rods and preferably the lowest grid about the upper rods is directly and rigidly affixed to the highest grid about the lower rods.

  1. Zinc isotopic compositions of breast cancer tissue.

    Science.gov (United States)

    Larner, Fiona; Woodley, Laura N; Shousha, Sami; Moyes, Ashley; Humphreys-Williams, Emma; Strekopytov, Stanislav; Halliday, Alex N; Rehkämper, Mark; Coombes, R Charles

    2015-01-01

    An early diagnostic biomarker for breast cancer is essential to improve outcome. High precision isotopic analysis, originating in Earth sciences, can detect very small shifts in metal pathways. For the first time, the natural intrinsic Zn isotopic compositions of various tissues in breast cancer patients and controls were determined. Breast cancer tumours were found to have a significantly lighter Zn isotopic composition than the blood, serum and healthy breast tissue in both groups. The Zn isotopic lightness in tumours suggests that sulphur rich metallothionein dominates the isotopic selectivity of a breast tissue cell, rather than Zn-specific proteins. This reveals a possible mechanism of Zn delivery to Zn-sequestering vesicles by metallothionein, and is supported by a similar signature observed in the copper isotopic compositions of one breast cancer patient. This change in intrinsic isotopic compositions due to cancer has the potential to provide a novel early biomarker for breast cancer.

  2. An extension of the validation of SCALE (SAS2H) isotopic predictions for PWR spent fuel

    Energy Technology Data Exchange (ETDEWEB)

    DeHart, M.D.; Hermann, O.W.

    1996-09-01

    Isotopic characterization of spent fuel via depletion and decay calculations is necessary for determination of source terms. Unlike fresh fuel assumptions typically used in criticality safety analysis of spent fuel configurations, burnup credit applications also rely on depletion and decay calculations to predict spent fuel composition; these isotopics are used in subsequent criticality calculations to assess the reduced worth of spent fuel. To validate the depletion codes and data, experiment is compared with predictions; such comparisons have been done in earlier ORNL work. This report describes additional independent measurements and corresponding calculations as a supplement. The current work includes measured isotopic data from 19 spent fuel samples from the Italian Trino Vercelles PWR and the US Turkey Point-3 PWR. In addition, an approach to determine biases and uncertainties between calculated and measured isotopic concentrations is discussed, together with a method to statistically combine these terms to obtain a conservative estimate of spent fuel isotopic concentrations. Results on combination of measured-to-calculated ratios are presented. The results described herein represent an extension to a new reactor design and spent fuel samples with enrichment as high as 3.9 wt% {sup 235}U. Consistency with the earlier work for each of two different cross-section libraries suggests that the estimated biases for each of the isotopes in the earlier work are reasonably good estimates.

  3. Numerical modeling of radioactive neutron capture influence of Hf isotopic composition dynamics rate in the RBMK-1500 reactor

    CERN Document Server

    Jurkevicius, A; Auzelyte, V; Remeikis, V

    2000-01-01

    The nuclide composition of the nuclear fuel and isotopic composition of the hafnium in the radial neutron flux detectors of the RBMK-1500 reactor were numerically modelled. The sequence SAS2 from package SCALE 4.3 was used for calculations. The nuclear fuel nuclide concentrations, the concentration of Hf isotopes, the neutron absorption rate on Hf isotopes and summary absorption rate dependences on the fuel assembly burn up are presented. (author)

  4. Lead Isotope Characterization of Petroleum Fuels in Taipei, Taiwan

    Directory of Open Access Journals (Sweden)

    Pei-Hsuan Yao

    2015-04-01

    Full Text Available Leaded gasoline in Taiwan was gradually phased out from 1983 to 2000. However, it is unclear whether unleaded gasoline still contributes to atmospheric lead (Pb exposure in urban areas. In this study, Pb isotopic compositions of unleaded gasolines, with octane numbers of 92, 95, 98, and diesel from two local suppliers in Taipei were determined by multi-collector inductively coupled plasma mass spectrometry with a two-sigma uncertainty of ± 0.02 %. Lead isotopic ratios of vehicle exhaust (208Pb/207Pb: 2.427, 206Pb/207Pb: 1.148, as estimated from petroleum fuels overlap with the reported aerosol data. This agreement indicates that local unleaded petroleum fuels, containing 10–45 ng·Pb·g−1, are merely one contributor among various sources to urban aerosol Pb. Additionally, the distinction between the products of the two companies is statistically significant in their individual 208Pb/206Pb ratios (p-value < 0.001, t test. Lead isotopic characterization appears to be applicable as a “fingerprinting” tool for tracing the sources of Pb pollution.

  5. Nuclear reactor composite fuel assembly

    Energy Technology Data Exchange (ETDEWEB)

    Burgess, Donn M. (Richland, WA); Marr, Duane R. (West Richland, WA); Cappiello, Michael W. (Richland, WA); Omberg, Ronald P. (Richland, WA)

    1980-01-01

    A core and composite fuel assembly for a liquid-cooled breeder nuclear reactor including a plurality of elongated coextending driver and breeder fuel elements arranged to form a generally polygonal bundle within a thin-walled duct. The breeder elements are larger in cross section than the driver elements, and each breeder element is laterally bounded by a number of the driver elements. Each driver element further includes structure for spacing the driver elements from adjacent fuel elements and, where adjacent, the thin-walled duct. A core made up of the fuel elements can advantageously include fissile fuel of only one enrichment, while varying the effective enrichment of any given assembly or core region, merely by varying the relative number and size of the driver and breeder elements.

  6. An Extension of the Validation of SCALE (SAS2H) Isotopic Predictions for PWR Spent Fuel

    Energy Technology Data Exchange (ETDEWEB)

    DeHart, M.D.

    1993-01-01

    Isotopic characterization of spent fuel via depletion and decay calculations is necessary for determination of source terms for subsequent system analyses involving heat transfer, radiation shielding, isotopic migration, etc. Unlike fresh fuel assumptions typically employed in the criticality safety analysis of spent fuel configurations, burnup credit applications also rely on depletion and decay calculations to predict the isotopic composition of spent fuel. These isotopics are used in subsequent criticality calculations to assess the reduced worth of spent fuel. To validate the codes and data used in depletion approaches, experimental measurements are compared with numerical predictions for relevant spent fuel samples. Such comparisons have been performed in earlier work at the Oak Ridge National Laboratory (ORNL). This report describes additional independent measurements and corresponding calculations, which supplement the results of the earlier work. The current work includes measured isotopic data from 19 spent fuel samples obtained from the Italian Trino Vercelles pressurized-water reactor (PWR) and the U.S. Turkey Point Unit 3 PWR. In addition, an approach to determine biases and uncertainties between calculated and measured isotopic concentrations is discussed, together with a method to statistically combine these terms to obtain a conservative estimate of spent fuel isotopic concentrations. Results are presented based on the combination of measured-to-calculated ratios for earlier work and the current analyses. The results described herein represent an extension to a new reactor design not included in the earlier work, and spent fuel samples with enrichment as high as 3.9 wt % {sup 235}U. Results for the current work are found to be, for the most part, consistent with the findings of the earlier work. This consistency was observed for results obtained from each of two different cross-section libraries and suggests that the estimated biases determined for

  7. Fuel preparation for use in the production of medical isotopes

    Science.gov (United States)

    Policke, Timothy A.; Aase, Scott B.; Stagg, William R.

    2016-10-25

    The present invention relates generally to the field of medical isotope production by fission of uranium-235 and the fuel utilized therein (e.g., the production of suitable Low Enriched Uranium (LEU is uranium having 20 weight percent or less uranium-235) fuel for medical isotope production) and, in particular to a method for producing LEU fuel and a LEU fuel product that is suitable for use in the production of medical isotopes. In one embodiment, the LEU fuel of the present invention is designed to be utilized in an Aqueous Homogeneous Reactor (AHR) for the production of various medical isotopes including, but not limited to, molybdenum-99, cesium-137, iodine-131, strontium-89, xenon-133 and yttrium-90.

  8. Composite Solid Fuel: Research of Formation Parameters

    Directory of Open Access Journals (Sweden)

    Tabakaev Roman

    2016-01-01

    Full Text Available Involving of local low-grade fuels resources in fuel and energy balance is actual question of research in the present. In this paper the possibility of processing low-grade fuel in the solid fuel composite was considered. The aim of the work is to define the optimal parameters for formation of the solid composite fuel. A result of researches determined that dextrin content in the binder allows to obtain solid composite fuel having the highest strength. The drying temperature for the various fuels was determined: for pellets production was 20-80 °C, for briquettes – 20-40 °C.

  9. FUEL COMPOSITION FOR NUCLEAR REACTORS

    Science.gov (United States)

    Andersen, J.C.

    1963-08-01

    A process for making refractory nuclear fuel elements involves heating uranium and silicon powders in an inert atmosphere to 1600 to 1800 deg C to form USi/sub 3/; adding silicon carbide, carbon, 15% by weight of nickel and aluminum, and possibly also molybdenum and silicon powders; shaping the mixture; and heating to 1700 to 2050 deg C again in an inert atmosphere. Information on obtaining specific compositions is included. (AEC)

  10. Nickel isotopic composition of the mantle

    Science.gov (United States)

    Gall, Louise; Williams, Helen M.; Halliday, Alex N.; Kerr, Andrew C.

    2017-02-01

    This paper presents a detailed high-precision study of Ni isotope variations in mantle peridotites and their minerals, komatiites as well as chondritic and iron meteorites. Ultramafic rocks display a relatively large range in δ60 Ni (permil deviation in 60 Ni /58 Ni relative to the NIST SRM 986 Ni isotope standard) for this environment, from 0.15 ± 0.07‰ to 0.36 ± 0.08‰, with olivine-rich rocks such as dunite and olivine cumulates showing lighter isotope compositions than komatiite, lherzolite and pyroxenite samples. The data for the mineral separates shed light on the origin of these variations. Olivine and orthopyroxene display light δ60 Ni whereas clinopyroxene and garnet are isotopically heavy. This indicates that peridotite whole-rock δ60 Ni may be controlled by variations in modal mineralogy, with the prediction that mantle melts will display variable δ60 Ni values due to variations in residual mantle and cumulate mineralogy. Based on fertile peridotite xenoliths and Phanerozoic komatiite samples it is concluded that the upper mantle has a relatively homogeneous Ni isotope composition, with the best estimate of δ60Nimantle being 0.23 ± 0.06‰ (2 s.d.). Given that >99% of the Ni in the silicate Earth is located in the mantle, this also defines the Ni isotope composition of the Bulk Silicate Earth (BSE). This value is nearly identical to the results obtained for a suite of chondrites and iron meteorites (mean δ60 Ni 0.26 ± 0.12‰ and 0.29 ± 0.10‰, respectively) showing that the BSE is chondritic with respect to its Ni isotope composition, with little to no Ni mass-dependent isotope fractionation resulting from core formation.

  11. Benchmark of SCALE (SAS2H) isotopic predictions of depletion analyses for San Onofre PWR MOX fuel

    Energy Technology Data Exchange (ETDEWEB)

    Hermann, O.W.

    2000-02-01

    The isotopic composition of mixed-oxide (MOX) fuel, fabricated with both uranium and plutonium, after discharge from reactors is of significant interest to the Fissile Materials Disposition Program. The validation of the SCALE (SAS2H) depletion code for use in the prediction of isotopic compositions of MOX fuel, similar to previous validation studies on uranium-only fueled reactors, has corresponding significance. The EEI-Westinghouse Plutonium Recycle Demonstration Program examined the use of MOX fuel in the San Onofre PWR, Unit 1, during cycles 2 and 3. Isotopic analyses of the MOX spent fuel were conducted on 13 actinides and {sup 148}Nd by either mass or alpha spectrometry. Six fuel pellet samples were taken from four different fuel pins of an irradiated MOX assembly. The measured actinide inventories from those samples has been used to benchmark SAS2H for MOX fuel applications. The average percentage differences in the code results compared with the measurement were {minus}0.9% for {sup 235}U and 5.2% for {sup 239}Pu. The differences for most of the isotopes were significantly larger than in the cases for uranium-only fueled reactors. In general, comparisons of code results with alpha spectrometer data had extreme differences, although the differences in the calculations compared with mass spectrometer analyses were not extremely larger than that of uranium-only fueled reactors. This benchmark study should be useful in estimating uncertainties of inventory, criticality and dose calculations of MOX spent fuel.

  12. Compositions and methods for treating nuclear fuel

    Energy Technology Data Exchange (ETDEWEB)

    Soderquist, Chuck Z; Johnsen, Amanda M; McNamara, Bruce K; Hanson, Brady D; Smith, Steven C; Peper, Shane M

    2014-01-28

    Compositions are provided that include nuclear fuel. Methods for treating nuclear fuel are provided which can include exposing the fuel to a carbonate-peroxide solution. Methods can also include exposing the fuel to an ammonium solution. Methods for acquiring molybdenum from a uranium comprising material are provided.

  13. Compositions and methods for treating nuclear fuel

    Energy Technology Data Exchange (ETDEWEB)

    Soderquist, Chuck Z; Johnsen, Amanda M; McNamara, Bruce K; Hanson, Brady D; Smith, Steven C; Peper, Shane M

    2013-08-13

    Compositions are provided that include nuclear fuel. Methods for treating nuclear fuel are provided which can include exposing the fuel to a carbonate-peroxide solution. Methods can also include exposing the fuel to an ammonium solution. Methods for acquiring molybdenum from a uranium comprising material are provided.

  14. Estimation of the activity and isotopic composition of the fuel elements of the reactor in decaying; Estimacion de la actividad y composicion isotopica de los elementos combustibles del reactor en decaimiento

    Energy Technology Data Exchange (ETDEWEB)

    Aguilar H, F. [ININ, 52045 Ocoyoacac, Estado de Mexico (Mexico)

    2001-03-15

    At the present time its are had 59 fuel elements, 3 control bars with follower and 2 instrumented irradiated fuels that its are decaying in the pool of the reactor. The burnt one that its have these fuels is not uniform, the quantity of U-235 that contain at the moment it varies between 33.5 g up to 35.2 and its have a decay of at least 12 years. The burnt of the fuels was obtained with the CREMAT code, this burnt was takes like base to estimate the current isotopic inventory and the activity of the same ones using the ORIGEN2 code. (Author)

  15. Validation of SCALE (SAS2H) Isotopic Predictions for BWR Spent Fuel

    Energy Technology Data Exchange (ETDEWEB)

    Hermann, O.W.

    1998-01-01

    Thirty spent fuel samples obtained from boiling-water-reactor (BWR) fuel pins have been modeled at Oak Ridge National Laboratory using the SAS2H sequence of the SCALE code system. The SAS2H sequence uses transport methods combined with the depletion and decay capabilities of the ORIGEN-S code to estimate the isotopic composition of fuel as a function of its burnup history. Results of these calculations are compared with chemical assay measurements of spent fuel inventories for each sample. Results show reasonable agreement between measured and predicted isotopic concentrations for important actinides; however, little data are available for most fission products considered to be important for spent fuel concerns (e.g., burnup credit, shielding, source-term calculations, etc.). This work is a follow-up to earlier works that studied the ability to predict spent fuel compositions in pressurized-water-reactor (PWR) fuel pins. Biases and uncertainties associated with BWR isotopic predictions are found to be larger than those of PWR calculations. Such behavior is expected, as the operation of a BWR is significantly more complex than that of a PWR plant, and in general the design of a BWR has a more heterogeneous configuration than that of a PWR. Nevertheless, this work shows that the simple models employed using SAS2H to represent such complexities result in agreement to within 5% (and often less than 1%) or less for most nuclides important for spent fuel applications. On the other hand, however, the set of fuel samples analyzed represent a small subset of the BWR fuel population, and results reported herein may not be representative of the full population of BWR spent fuel.

  16. Validation of SCALE (SAS2H) isotopic predictions for BWR spent fuel

    Energy Technology Data Exchange (ETDEWEB)

    Hermann, O.W.; DeHart, M.D.

    1998-09-01

    Thirty spent fuel samples obtained from boiling-water-reactor (BWR) fuel pins have been modeled at Oak Ridge National Laboratory using the SAS2H sequence of the SCALE code system. The SAS2H sequence uses transport methods combined with the depletion and decay capabilities of the ORIGEN-S code to estimate the isotopic composition of fuel as a function of its burnup history. Results of these calculations are compared with chemical assay measurements of spent fuel inventories for each sample. Results show reasonable agreement between measured and predicted isotopic concentrations for important actinides; however, little data are available for most fission products considered to be important for spent fuel concerns (e.g., burnup credit, shielding, source-term calculations, etc.). This work is a follow-up to earlier works that studied the ability to predict spent fuel compositions in pressurized-water-reactor (PWR) fuel pins. Biases and uncertainties associated with BWR isotopic predictions are found to be larger than those of PWR calculations. Such behavior is expected, as the operation of a BWR is significantly more complex than that of a PWR plant, and in general the design of a BWR has a more heterogeneous configuration than that of a PWR. Nevertheless, this work shows that the simple models employed using SAS2H to represent such complexities result in agreement to within 5% (and often less than 1%) or less for most nuclides important for spent fuel applications. On the other hand, however, the set of fuel samples analyzed represent a small subset of the BWR fuel population, and results reported herein may not be representative of the full population of BWR spent fuel.

  17. HTGR spent fuel composition and fuel element block flow

    Energy Technology Data Exchange (ETDEWEB)

    Hamilton, C.J.; Holder, N.D.; Pierce, V.H.; Robertson, M.W.

    1976-07-01

    The High-Temperature Gas-Cooled Reactor (HTGR) utilizes the thorium-uranium fuel cycle. Fully enriched uranium fissile material and thorium fertile material are used in the initial reactor core and for makeup fuel in the recycle core loadings. Bred /sup 233/U and unburned /sup 235/U fissile materials are recovered from spent fuel elements, refabricated into recycle fuel elements, and used as part of the recycle core loading along with the makeup fuel elements. A typical HTGR employs a 4-yr fuel cycle with approximately one-fourth of the core discharged and reloaded annually. The fuel element composition, including heavy metals, impurity nuclides, fission products, and activation products, has been calculated for discharged spent fuel elements and for reload fresh fuel and recycle fuel elements for each cycle over the life of a typical HTGR. Fuel element compositions are presented for the conditions of equilibrium recycle. Data describing compositions for individual reloads throughout the reactor life are available in a detailed volume upon request. Fuel element block flow data have been compiled based on a forecast HTGR market. Annual block flows are presented for each type of fuel element discharged from the reactors for reprocessing and for refabrication.

  18. DESIGN OF LSDS FOR ISOTOPIC FISSILE ASSAY IN SPENT FUEL

    Directory of Open Access Journals (Sweden)

    YONGDEOK LEE

    2013-12-01

    Full Text Available A future nuclear energy system is being developed at Korea Atomic Energy Research Institute (KAERI, the system involves a Sodium Fast Reactor (SFR linked with the pyro-process. The pyro-process produces a source material to fabricate a SFR fuel rod. Therefore, an isotopic fissile content assay is very important for fuel rod safety and SFR economics. A new technology for an analysis of isotopic fissile content has been proposed using a lead slowing down spectrometer (LSDS. The new technology has several features for a fissile analysis from spent fuel: direct isotopic fissile assay, no background interference, and no requirement from burnup history information. Several calculations were done on the designed spectrometer geometry: detection sensitivity, neutron energy spectrum analysis, neutron fission characteristics, self shielding analysis, and neutron production mechanism. The spectrum was well organized even at low neutron energy and the threshold fission chamber was a proper choice to get prompt fast fission neutrons. The characteristic fission signature was obtained in slowing down neutron energy from each fissile isotope. Another application of LSDS is for an optimum design of the spent fuel storage, maximization of the burnup credit and provision of the burnup code correction factor. Additionally, an isotopic fissile content assay will contribute to an increase in transparency and credibility for the utilization of spent fuel nuclear material, as internationally demanded.

  19. Analysis of high burnup pressurized water reactor fuel using uranium, plutonium, neodymium, and cesium isotope correlations with burnup

    Energy Technology Data Exchange (ETDEWEB)

    Kim, Jung Suk; Jeon, Young Shin; Park, Soon Dal; Ha, Yeong Keong; Song, Kyu Seok [Nuclear Chemistry Research Division, Korea Atomic Energy Research Institute, Daejeon (Korea, Republic of)

    2015-12-15

    The correlation of the isotopic composition of uranium, plutonium, neodymium, and cesium with the burnup for high burnup pressurized water reactor fuels irradiated in nuclear power reactors has been experimentally investigated. The total burnup was determined by Nd-148 and the fractional {sup 235}U burnup was determined by U and Pu mass spectrometric methods. The isotopic compositions of U, Pu, Nd, and Cs after their separation from the irradiated fuel samples were measured using thermal ionization mass spectrometry. The contents of these elements in the irradiated fuel were determined through an isotope dilution mass spectrometric method using {sup 233}U, {sup 242}Pu, {sup 150}Nd, and {sup 133}Cs as spikes. The activity ratios of Cs isotopes in the fuel samples were determined using gamma-ray spectrometry. The content of each element and its isotopic compositions in the irradiated fuel were expressed by their correlation with the total and fractional burnup, burnup parameters, and the isotopic compositions of different elements. The results obtained from the experimental methods were compared with those calculated using the ORIGEN-S code.

  20. Target-fueled nuclear reactor for medical isotope production

    Science.gov (United States)

    Coats, Richard L.; Parma, Edward J.

    2017-06-27

    A small, low-enriched, passively safe, low-power nuclear reactor comprises a core of target and fuel pins that can be processed to produce the medical isotope .sup.99Mo and other fission product isotopes. The fuel for the reactor and the targets for the .sup.99Mo production are the same. The fuel can be low enriched uranium oxide, enriched to less than 20% .sup.235U. The reactor power level can be 1 to 2 MW. The reactor is passively safe and maintains negative reactivity coefficients. The total radionuclide inventory in the reactor core is minimized since the fuel/target pins are removed and processed after 7 to 21 days.

  1. Impact of statistical uncertainty of the neutron spectrum in the isotopic evolution of fuel; Impacto de la incertidumbre estadistica del espectro neutronico en la evoluacion isotopica del combustible

    Energy Technology Data Exchange (ETDEWEB)

    Ortega, P.

    2012-07-01

    The results obtained and presented in this study for different calculation conditions (number of stories, number of steps burning, etc.) and their simultaneous impact on neutron spectrum and isotopic composition and a methodology is proposed to determine the minimum parameters for calculation given uncertainty in the results of isotopic composition with high burnup, both UO{sub 2} and MOX fuel.

  2. A highly combustible composite solid fuel

    Energy Technology Data Exchange (ETDEWEB)

    Sonetaka, K.; Iketani, Y.; Nisino, A.; Takeuti, Y.

    1983-07-12

    To increase the combustibility, the briqueted solid fuel is coated with an auxiliary fuel which is characterized by high flamability. The composition ofthe basic fuel includes a solid fuel with a high combustion temperature and seeming density (mineral coal, activated charcoal, coke, graphite and a carbonized product), a desulfurizing agent (CaCO3 or MgO), a combustion promotor (Ca(CO3)2, KNO3, sodium acetate, iron oxalate) and forming additives (bentonite, clay or talc) or a binder (pitch, tar, methylcellulose or cement). The auxiliary fuel has the very same composition, but is characterized by a low ignition temperature and density (for instance, due to the addition of sawdust). The obtained two layer composite fuel is characterized by improved ignitibility and combustibility.

  3. THE NITROGEN ISOTOPIC COMPOSITION OF METEORITIC HCN

    Energy Technology Data Exchange (ETDEWEB)

    Pizzarello, Sandra, E-mail: pizzar@asu.edu [Department of Chemistry and Biochemistry, Arizona State University, Tempe, AZ 85018-1604 (United States)

    2014-12-01

    HCN is ubiquitous in extraterrestrial environments and is central to current theories on the origin of early solar system organic compounds such as amino acids. These compounds, observed in carbonaceous meteorites, were likely important in the origin and/or evolution of early life. As part of our attempts to understand the origin(s) of meteoritic CN{sup –}, we have analyzed the {sup 15}N/{sup 14}N isotopic composition of HCN gas released from water extracts of the Murchison meteorite and found its value to be near those of the terrestrial atmosphere. The findings, when evaluated viz-a-viz molecular abundances and isotopic data of meteoritic organic compounds, suggest that HCN formation could have occurred during the protracted water alteration processes known to have affected the mineralogy of many asteroidal bodies during their solar residence. This was an active synthetic stage, which likely involved simple gasses, organic molecules, their presolar precursors, as well as mineral catalysts and would have lead to the formation of molecules of differing isotopic composition, including some with solar values.

  4. Aerosol carbon isotope composition over Baltic Sea

    Science.gov (United States)

    Garbaras, Andrius; Pabedinskas, Algirdas; Masalaite, Agne; Petelski, Tomasz; Gorokhova, Elena; Sapolaite, Justina; Ezerinskis, Zilvinas; Remeikis, Vidmantas

    2017-04-01

    Particulate carbonaceous matter is significant contributor to ambient particulate matter originating from intervening sources which contribution is difficult to quantify due to source diversity, chemical complexity and processes during atmospheric transport. Carbon isotope analysis can be extremely useful in source apportionment of organic matter due to the unique isotopic signatures associated with anthropocentric (fossil fuel), continental (terrestrial plants) and marine sources, and is particularly effective when these sources are mixed (Ceburnis et al., 2011;Ceburnis et al., 2016). We will present the isotope ratio measurement results of aerosol collected during the cruise in the Baltic Sea. Sampling campaign of PM10 and size segregated aerosol particles was performed on the R/V "Oceania" in October 2015. Air mass back trajectories were prevailing both from the continental and marine areas during the sampling period. The total carbon concentration varied from 1 µg/m3 to 8 µg/m3. Two end members (δ13C = -25‰ and δ13C = -28 ‰ ) were established from the total stable carbon isotope analysis in PM10 fraction. δ13C analysis in size segregated aerosol particles revealed δ13C values being highest in the 1 - 2.5 µm range (δ13C = -24.9 ‰ ) during continental transport, while lowest TC δ13C values (δ13C ≈ -27 ‰ ) were detected in the size range D50 dual carbon pools contributing to organic matter enrichment in marine aerosol, Scientific Reports, 6, 2016. Masalaite, A., Remeikis, V., Garbaras, A., Dudoitis, V., Ulevicius, V., and Ceburnis, D.: Elucidating carbonaceous aerosol sources by the stable carbon δ13C TC ratio in size-segregated particles, Atmospheric Research, 158, 1-12, 2015.

  5. Nuclear fuel elements having a composite cladding

    Science.gov (United States)

    Gordon, Gerald M.; Cowan, II, Robert L.; Davies, John H.

    1983-09-20

    An improved nuclear fuel element is disclosed for use in the core of nuclear reactors. The improved nuclear fuel element has a composite cladding of an outer portion forming a substrate having on the inside surface a metal layer selected from the group consisting of copper, nickel, iron and alloys of the foregoing with a gap between the composite cladding and the core of nuclear fuel. The nuclear fuel element comprises a container of the elongated composite cladding, a central core of a body of nuclear fuel material disposed in and partially filling the container and forming an internal cavity in the container, an enclosure integrally secured and sealed at each end of said container and a nuclear fuel material retaining means positioned in the cavity. The metal layer of the composite cladding prevents perforations or failures in the cladding substrate from stress corrosion cracking or from fuel pellet-cladding interaction or both. The substrate of the composite cladding is selected from conventional cladding materials and preferably is a zirconium alloy.

  6. Composition and methods for improved fuel production

    Energy Technology Data Exchange (ETDEWEB)

    Steele, Philip H.; Tanneru, Sathishkumar; Gajjela, Sanjeev K.

    2015-12-29

    Certain embodiments of the present invention are configured to produce boiler and transportation fuels. A first phase of the method may include oxidation and/or hyper-acidification of bio-oil to produce an intermediate product. A second phase of the method may include catalytic deoxygenation, esterification, or olefination/esterification of the intermediate product under pressurized syngas. The composition of the resulting product--e.g., a boiler fuel--produced by these methods may be used directly or further upgraded to a transportation fuel. Certain embodiments of the present invention also include catalytic compositions configured for use in the method embodiments.

  7. The isotopic composition of CO in vehicle exhaust

    Science.gov (United States)

    Naus, Stijn; Röckmann, Thomas; Popa, Elena

    2017-04-01

    The isotopic composition of atmospheric carbon monoxide (CO) and its sources can be a powerful tool to help constrain the CO budget, but data on the isotopic composition of CO sources is sparse. We investigated the isotopic composition (13C16O and 12C18O) of one of the main sources of CO in urban areas: traffic emissions. Samples from individual passenger cars and atmospheric samples from polluted areas were measured. The results show strong indications that CO emissions from traffic are dominated by a small subset of cars or driving conditions, which, in this study, were cold petrol cars. The spread in isotopic composition of the full dataset was large, but this dominant subset showed a relatively stable isotopic composition. Therefore, the individual car samples result in a well-defined overall traffic signature, which was in agreement with the atmospheric isotopic signature derived from the atmospheric samples.

  8. Compound-Specific Isotope Analysis of Diesel Fuels in a Forensic Investigation

    Science.gov (United States)

    Muhammad, Syahidah; Frew, Russell; Hayman, Alan

    2015-02-01

    Compound-specific isotope analysis (CSIA) offers great potential as a tool to provide chemical evidence in a forensic investigation. Many attempts to trace environmental oil spills were successful where isotopic values were particularly distinct. However, difficulties arise when a large data set is analyzed and the isotopic differences between samples are subtle. In the present study, discrimination of diesel oils involved in a diesel theft case was carried out to infer the relatedness of the samples to potential source samples. This discriminatory analysis used a suite of hydrocarbon diagnostic indices, alkanes, to generate carbon and hydrogen isotopic data of the compositions of the compounds which were then processed using multivariate statistical analyses to infer the relatedness of the data set. The results from this analysis were put into context by comparing the data with the δ13C and δ2H of alkanes in commercial diesel samples obtained from various locations in the South Island of New Zealand. Based on the isotopic character of the alkanes, it is suggested that diesel fuels involved in the diesel theft case were distinguishable. This manuscript shows that CSIA when used in tandem with multivariate statistical analysis provide a defensible means to differentiate and source-apportion qualitatively similar oils at the molecular level. This approach was able to overcome confounding challenges posed by the near single-point source of origin i.e. the very subtle differences in isotopic values between the samples.

  9. Analysis of Experimental Data for High Burnup PWR Spent Fuel Isotopic Validation - Vandellos II Reactor

    Energy Technology Data Exchange (ETDEWEB)

    Ilas, Germina [ORNL; Gauld, Ian C [ORNL

    2011-01-01

    This report is one of the several recent NUREG/CR reports documenting benchmark-quality radiochemical assay data and the use of the data to validate computer code predictions of isotopic composition for spent nuclear fuel, to establish the uncertainty and bias associated with code predictions. The experimental data analyzed in the current report were acquired from a high-burnup fuel program coordinated by Spanish organizations. The measurements included extensive actinide and fission product data of importance to spent fuel safety applications, including burnup credit, decay heat, and radiation source terms. Six unique spent fuel samples from three uranium oxide fuel rods were analyzed. The fuel rods had a 4.5 wt % {sup 235}U initial enrichment and were irradiated in the Vandellos II pressurized water reactor operated in Spain. The burnups of the fuel samples range from 42 to 78 GWd/MTU. The measurements were used to validate the two-dimensional depletion sequence TRITON in the SCALE computer code system.

  10. Nuclear reactor composite fuel assembly. [LMFBR

    Energy Technology Data Exchange (ETDEWEB)

    Burgess, D.M.; Cappiello, M.W.; Marr, D.R.; Omberg, R.P.

    1980-11-25

    A core and composite fuel assembly are described for a liquid-cooled breeder nuclear reactor including a plurality of elongated coextending driver and breeder fuel elements arranged to form a generally polygonal bundle within a thin-walled duct. The breeder elements are larger in cross section than the driver elements, and each breeder element is laterally bounded by a number of the driver elements. Each driver element further includes structure for spacing the driver elements from adjacent fuel elements and, where adjacent, the thin-walled duct. A core made up of the fuel elements can advantageously include fissile fuel of only one enrichment, while varying the effective enrichment of any given assembly or core region, merely by varying the relative number and size of the driver and breeder elements.

  11. Magnesium Isotopic Composition of Subducting Marine Sediments

    Science.gov (United States)

    Hu, Y.; Teng, F. Z.; Plank, T. A.; Huang, K. J.

    2015-12-01

    Subducted marine sediments have recently been called upon to explain the heterogeneous Mg isotopic composition (δ26Mg, ‰) found in mantle wehrlites (-0.39 to +0.09 [1]) in the context of a homogeneous mantle (-0.25 ± 0.07 [2]). However, no systematic measurements of δ26Mg on marine sediments are currently available to provide direct support to this model. To characterize the Mg inputs to global subduction zones, we measured δ26Mg data for a total of 90 marine sediments collected from 12 drill sites outboard of the world's major subduction zones. These sediments span a 1.73‰ range in δ26Mg. The detritus-dominated sediments have δ26Mg (-0.59 to +0.53) comparable to those of weathered materials on continents (e.g. -0.52 to +0.92 [3]), while the calcareous oozes yield δ26Mg (as light as -1.20) more similar to the seawater value (-0.83 [4]). The negative correlation between δ26Mg and CaO/Al2O3 in these sediments indicates the primary control of mineralogy over the Mg isotopic distribution among different sediment types, as carbonates are enriched in light Mg isotopes (-5.10 to -0.40 [5]) whereas clay-rich weathering residues generally have heavier δ26Mg (e.g. up to +0.65 in saprolite [6]). In addition, chemical weathering and grain-size sorting drive sediments to a heavier δ26Mg, as indicated by the broad positive trends between δ26Mg with CIA (Chemical Index of Alteration [7]) and Al2O3/SiO2, respectively. Collectively, the arc systems sampled in this study represent ~30% of global arc length and the extrapolated global Mg flux of subducting marine sediments accounts for ~9% of the yearly Mg riverine input with a flux-weighted average δ26Mg at -0.26. Subduction of these heterogeneous sediments may not cause significant mantle heterogeneity on a global scale, but the highly variable Mg fluxes and δ26Mg of sediments delivered to different trenches are capable of producing local mantle variations. Volcanic rocks sourced from these mantle domains are thus

  12. Discrimination of source reactor type by multivariate statistical analysis of uranium and plutonium isotopic concentrations in unknown irradiated nuclear fuel material.

    Science.gov (United States)

    Robel, Martin; Kristo, Michael J

    2008-11-01

    The problem of identifying the provenance of unknown nuclear material in the environment by multivariate statistical analysis of its uranium and/or plutonium isotopic composition is considered. Such material can be introduced into the environment as a result of nuclear accidents, inadvertent processing losses, illegal dumping of waste, or deliberate trafficking in nuclear materials. Various combinations of reactor type and fuel composition were analyzed using Principal Components Analysis (PCA) and Partial Least Squares Discriminant Analysis (PLSDA) of the concentrations of nine U and Pu isotopes in fuel as a function of burnup. Real-world variation in the concentrations of (234)U and (236)U in the fresh (unirradiated) fuel was incorporated. The U and Pu were also analyzed separately, with results that suggest that, even after reprocessing or environmental fractionation, Pu isotopes can be used to determine both the source reactor type and the initial fuel composition with good discrimination.

  13. Composite nozzle design for reactor fuel assembly

    Energy Technology Data Exchange (ETDEWEB)

    Marlatt, G.R.; Allison, D.K.

    1984-01-24

    A composite nozzle is described for a fuel assembly adapted for installation on the upper or lower end thereof and which is constructed from two components. The first component includes a casting weldment or forging designed to carry handling loads, support fuel assembly weight and flow loads, and interface with structural members of both the fuel assembly and reactor internal structures. The second component of the nozzle consists of a thin stamped bore machine flow plate adapted for attachment to the casting body. The plate is designed to prevent fuel rods from being ejected from the core and provide orifices for coolant flow to a predetermined value and pressure drop which is consistent with the flow at other locations in the core.

  14. Isotopic compositional Characteristics of Terrigenous Natural Gases in China

    Institute of Scientific and Technical Information of China (English)

    沈平; 徐永昌

    1993-01-01

    The C and H isotopic compositions of the methane in more than 160 gas samples from 10 basins in China are presented in this paper.The natural gases are classified as four types: biogenic gas ,bio-thermocatalytic transitional gas, gas associated with condensate oil ,and coal-type gas. The isotopic compositions of these gases closely related to the depositional basins, the types of organic matter,the stages of thermal evolution and the genetic characteristics of different gas reservoirs.Studies of the C and H isotopic compositions of terrigenous natural gases will provide valua-ble information on the prospecting and development of natural gases of different genetic types.

  15. Isotope composition and volume of Earth’s early oceans

    OpenAIRE

    Pope, Emily C.; Bird, Dennis K.; Rosing, Minik T.

    2012-01-01

    Oxygen and hydrogen isotope compositions of Earth’s seawater are controlled by volatile fluxes among mantle, lithospheric (oceanic and continental crust), and atmospheric reservoirs. Throughout geologic time the oxygen mass budget was likely conserved within these Earth system reservoirs, but hydrogen’s was not, as it can escape to space. Isotopic properties of serpentine from the approximately 3.8 Ga Isua Supracrustal Belt in West Greenland are used to characterize hydrogen and oxygen isotop...

  16. Reactor Fuel Isotopics and Code Validation for Nuclear Applications

    Energy Technology Data Exchange (ETDEWEB)

    Francis, Matthew W. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Weber, Charles F. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Pigni, Marco T. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Gauld, Ian C. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

    2015-02-01

    Experimentally measured isotopic concentrations of well characterized spent nuclear fuel (SNF) samples have been collected and analyzed by previous researchers. These sets of experimental data have been used extensively to validate the accuracy of depletion code predictions for given sets of burnups, initial enrichments, and varying power histories for different reactor types. The purpose of this report is to present the diversity of data in a concise manner and summarize the current accuracy of depletion modeling. All calculations performed for this report were done using the Oak Ridge Isotope GENeration (ORIGEN) code, an internationally used irradiation and decay code solver within the SCALE comprehensive modeling and simulation code. The diversity of data given in this report includes key actinides, stable fission products, and radioactive fission products. In general, when using the current ENDF/B-VII.0 nuclear data libraries in SCALE, the major actinides are predicted to within 5% of the measured values. Large improvements were seen for several of the curium isotopes when using improved cross section data found in evaluated nuclear data file ENDF/B-VII.0 as compared to ENDF/B-V-based results. The impact of the flux spectrum on the plutonium isotope concentrations as a function of burnup was also shown. The general accuracy noted for the actinide samples for reactor types with burnups greater than 5,000 MWd/MTU was not observed for the low-burnup Hanford B samples. More work is needed in understanding these large discrepancies. The stable neodymium and samarium isotopes were predicted to within a few percent of the measured values. Large improvements were seen in prediction for a few of the samarium isotopes when using the ENDF/B-VII.0 libraries compared to results obtained with ENDF/B-V libraries. Very accurate predictions were obtained for 133Cs and 153Eu. However, the predicted values for the stable ruthenium and rhodium isotopes varied

  17. The Late Quaternary Oxygen Isotope Composition of Lake Michigan

    Science.gov (United States)

    MacDonald, R. A.; Longstaffe, F. J.; Crowe, A. S.

    2007-12-01

    We present stable isotope records for porewater (oxygen, hydrogen) and biogenic carbonates (oxygen, carbon; ostracode and clam shells) in sediment cores from the Chippewa, Milwaukee and South Chippewa Basins of Lake Michigan. The oxygen and hydrogen isotope compositions of porewater from the South Chippewa Basin core showed very little variation with depth. At the maximum depth of 16.6m, δ18O values were within 2‰ and δD values were within 12‰ of modern Lake Michigan water (average δ18O = -5.9‰; average δD = -45‰); original porewater compositions have not been preserved. The oxygen isotope results for the biogenic carbonates, by comparison, provide a record of the isotopic composition of Lake Michigan over the last ~11,000 years, including significant incursions of very low-18O water, as first reported by Colman et al. (1990) and Forester et al. (1994). The low-18O waters originated from the retreating Laurentide ice sheet and may have been routed through Lakes Agassiz and Superior and discharged as large volumes over very short intervals of time. Periods characterized by much higher oxygen isotope compositions likely record the isotopic composition of regional precipitation over the catchment area. In summary, the large variations in the oxygen isotope composition of early Lake Michigan water arose from regional climate change and changing water sources during the times of ice-sheet retreat.

  18. Isotopic composition of precipitation in Ljubljana (Slovenia

    Directory of Open Access Journals (Sweden)

    Polona Vreča

    2008-12-01

    Full Text Available The stable isotopic composition of hydrogen and oxygen (δ2H and δ18O and tritium activity (3H are monitored in monthly precipitation at Ljubljana since 1981. Here we present complete set of numerical data and the statistical analysis for period 1981–2006. Seasonal variations of δ2H and δ18O are observed and are typical for continental stations of the Northern Hemisphere. The weighted mean δ2H and δ18O values are –59 ‰ and –8.6 ‰, respectively.The orthogonal Local Meteoric Water Line is δ2H = (8.06 ± 0.08δ18O + (9.84 ± 0.71, and the temperature coefficient of δ18O is 0.29 ‰/°C. Deuterium excess weighted mean value is 9.5 ‰ and indicates the prevailing influence of the Atlantic air masses. Tritium activity in monthly precipitation shows also seasonal variations which are superposed to the decreasing trend of mean annual activity.

  19. Isotopic compositions of boron in sediments and their implications

    Digital Repository Service at National Institute of Oceanography (India)

    Shirodkar, P.V.; Yingkai, X.

    of sediments are mostly closer to the boron isotopic composition of minerals. Such low delta sup(11)B values are attributed to the presence of borates, ulexite and other carbonate minerals in sediments of the salt lakes of Qaidam Basin....

  20. Isotopic compositions of the elements 2013 (IUPAC Technical Report)

    Science.gov (United States)

    Meija, Juris; Coplen, Tyler B.; Berglund, Michael; Brand, Willi A.; De Bièvre, Paul; Gröning, Manfred; Holden, Norman E.; Irrgeher, Johanna; Loss, Robert D.; Walczyk, Thomas; Prohaska, Thomas

    2016-01-01

    The Commission on Isotopic Abundances and Atomic Weights (ciaaw.org) of the International Union of Pure and Applied Chemistry (iupac.org) has revised the Table of Isotopic Compositions of the Elements (TICE). The update involved a critical evaluation of the recent published literature. The new TICE 2013 includes evaluated data from the “best measurement” of the isotopic abundances in a single sample, along with a set of representative isotopic abundances and uncertainties that accommodate known variations in normal terrestrial materials.

  1. Oxygen isotopic composition of carbon dioxide in the middle atmosphere

    OpenAIRE

    Liang, Mao-Chang; Blake, Geoffrey A.; Lewis, Brenton R.; Yung, Yuk L.

    2007-01-01

    The isotopic composition of long-lived trace molecules provides a window into atmospheric transport and chemistry. Carbon dioxide is a particularly powerful tracer, because its abundance remains >100 parts per million by volume (ppmv) in the mesosphere. Here, we successfully reproduce the isotopic composition of CO2 in the middle atmosphere, which has not been previously reported. The mass-independent fractionation of oxygen in CO2 can be satisfactorily explained by the exchange reaction with...

  2. Advanced composite polymer electrolyte fuel cell membranes

    Energy Technology Data Exchange (ETDEWEB)

    Wilson, M.S.; Zawodzinski, T.A.; Gottesfeld, S.; Kolde, J.A.; Bahar, B.

    1995-09-01

    A new type of reinforced composite perfluorinated polymer electrolyte membrane, GORE-SELECT{trademark} (W.L. Gore & Assoc.), is characterized and tested for fuel cell applications. Very thin membranes (5-20 {mu}m thick) are available. The combination of reinforcement and thinness provides high membrane, conductances (80 S/cm{sup 2} for a 12 {mu}m thick membrane at 25{degrees}C) and improved water distribution in the operating fuel cell without sacrificing longevity or durability. In contrast to nonreinforced perfluorinated membranes, the x-y dimensions of the GORE-SELECT membranes are relatively unaffected by the hydration state. This feature may be important from the viewpoints of membrane/electrode interface stability and fuel cell manufacturability.

  3. A first roadmap for kryptology. [isotopic composition from supernovae

    Science.gov (United States)

    Heymann, D.; Dziczkaniec, M.

    1980-01-01

    Studies of the complex variations of the isotopic composition of xenon in the solar system have been christened 'xenology'. In the title of the present investigation, the word 'kryptology' is employed to indicate the primary objective of the reported studies. This objective is related to the prediction of the isotopic composition of krypton which comes from a number of specific locations of a supernova in association with the isotopic compositions of xenon from these locations. Krypton is a logical candidate for testing the stellar theory on geochemical grounds, taking into account also the point of view of nucleosynthesis, because the isotopes of xenon and krypton are formed by the same thermonuclear processes in stars. The data and arguments presented in the investigation show that the treatment by Heymann and Dziczkaniec (1979), although not wrong, is too simplistic, because it has ignored the possibility of holdup and arrest in Xe network.

  4. The procedure and results of calculations of the equilibrium isotopic composition of a demonstration subcritical molten salt reactor

    Science.gov (United States)

    Nevinitsa, V. A.; Dudnikov, A. A.; Blandinskiy, V. Yu.; Balanin, A. L.; Alekseev, P. N.; Titarenko, Yu. E.; Batyaev, V. F.; Pavlov, K. V.; Titarenko, A. Yu.

    2015-12-01

    A subcritical molten salt reactor with an external neutron source is studied computationally as a facility for incineration and transmutation of minor actinides from spent nuclear fuel of reactors of VVER-1000 type and for producing 233U from 232Th. The reactor configuration is chosen, the requirements to be imposed on the external neutron source are formulated, and the equilibrium isotopic composition of heavy nuclides and the key parameters of the fuel cycle are calculated.

  5. The procedure and results of calculations of the equilibrium isotopic composition of a demonstration subcritical molten salt reactor

    Energy Technology Data Exchange (ETDEWEB)

    Nevinitsa, V. A., E-mail: Neviniza-VA@nrcki.ru; Dudnikov, A. A.; Blandinskiy, V. Yu.; Balanin, A. L.; Alekseev, P. N. [National Research Centre Kurchatov Institute (Russian Federation); Titarenko, Yu. E.; Batyaev, V. F.; Pavlov, K. V.; Titarenko, A. Yu., E-mail: yuri.titarenko@itep.ru [Institute for Theoretical and Experimental Physics (Russian Federation)

    2015-12-15

    A subcritical molten salt reactor with an external neutron source is studied computationally as a facility for incineration and transmutation of minor actinides from spent nuclear fuel of reactors of VVER-1000 type and for producing {sup 233}U from {sup 232}Th. The reactor configuration is chosen, the requirements to be imposed on the external neutron source are formulated, and the equilibrium isotopic composition of heavy nuclides and the key parameters of the fuel cycle are calculated.

  6. The ruthenium isotopic composition of the oceanic mantle

    Science.gov (United States)

    Bermingham, K. R.; Walker, R. J.

    2017-09-01

    The approximately chondritic relative, and comparatively high absolute mantle abundances of the highly siderophile elements (HSE), suggest that their concentrations in the bulk silicate Earth were primarily established during a final ∼0.5 to 1% of ;late accretion; to the mantle, following the cessation of core segregation. Consequently, the isotopic composition of the HSE Ru in the mantle reflects an amalgamation of the isotopic compositions of late accretionary contributions to the silicate portion of the Earth. Among cosmochemical materials, Ru is characterized by considerable mass-independent isotopic variability, making it a powerful genetic tracer of Earth's late accretionary building blocks. To define the Ru isotopic composition of the oceanic mantle, the largest portion of the accessible mantle, we report Ru isotopic data for materials from one Archean and seven Phanerozoic oceanic mantle domains. A sample from a continental lithospheric mantle domain is also examined. All samples have identical Ru isotopic compositions, within analytical uncertainties, indicating that Ru isotopes are well mixed in the oceanic mantle, defining a μ100Ru value of 1.2 ± 7.2 (2SD). The only known meteorites with the same Ru isotopic composition are enstatite chondrites and, when corrected for the effects of cosmic ray exposure, members of the Main Group and sLL subgroup of the IAB iron meteorite complex which have a collective CRE corrected μ100Ru value of 0.9 ± 3.0. This suggests that materials from the region(s) of the solar nebula sampled by these meteorites likely contributed the dominant portion of late accreted materials to Earth's mantle.

  7. Calcium isotopic compositions of mid-ocean ridge basalts

    Science.gov (United States)

    Zhu, H.; Zhang, Z.; Sun, W.; Wang, G. Q.

    2015-12-01

    Previous studies have demonstrated that Earth's mantle has heterogeneous calcium isotopic compositions. But the reason why mantle has its heterogeneity remains uncertain. In general, δ44/40Ca values of mantle xenolith samples have a variation of >0.45‰. While ultramafic rocks, especially dunites, have higher δ44/40Ca values than volcanic rocks, and there is a positive correlation between δ44/40Ca and Ca/Mg. These phenomena imply that the heterogeneity of Ca isotopic compositions of mantle xenolith samples might result from different degrees of melt extraction, as indicated by large Ca isotopic fractionation between co-existing clinopyroxene and orthopyroxene. However, because ancient marine carbonate has its own unique calcium isotopic characteristics, recycling of even a small amount of ancient marine carbonates into the mantle could also cause the heterogeneity of Ca isotopes in Earth's mantle. This could be the reason why oceanic island basalts (OIB) have lighter Ca isotopic compositions than the mantle xenolith. Thus, the lighter Ca isotopic compositions in the mantle source cannot only be ascribed to magmatic processes. Therefore, it is more important to know calcium isotopic characteristics during partial melting and oceanic crust contamination.Mid-ocean ridge basalts (MORB) are formed from the partial melts of the upper mantle and are rarely affected by crustal contamination. Different types of MORB, including D-MORB, N-MORB and E-MORB, have experienced different degrees of partial melting and contamination of enriched end-members. Here we report calcium isotopic characteristic of different types of MORB, we believe it will be very helpful to understand the behaviors of Ca isotopes during partial melting and it is possible to provide further information to discover the reason why calcium isotopic compositions is heterogeneous in Earth's mantle. This work was supported by Natural Science Foundation of China (No. 41373007, No. 41490632 and No. 91328204

  8. Dissolution Flowsheet for High Flux Isotope Reactor Fuel

    Energy Technology Data Exchange (ETDEWEB)

    Daniel, W. E. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Rudisill, T. S. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); O' Rourke, P. E. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Karay, N. S [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)

    2016-09-27

    As part of the Spent Nuclear Fuel (SNF) processing campaign, H-Canyon is planning to begin dissolving High Flux Isotope Reactor (HFIR) fuel in late FY17 or early FY18. Each HFIR fuel core contains inner and outer fuel elements which were fabricated from uranium oxide (U3O8) dispersed in a continuous Al phase using traditional powder metallurgy techniques. Fuels fabricated in this manner, like other SNF’s processed in H-Canyon, dissolve by the same general mechanisms with similar gas generation rates and the production of H2. The HFIR fuel cores will be dissolved and the recovered U will be down-blended into low-enriched U. HFIR fuel was previously processed in H-Canyon using a unique insert in both the 6.1D and 6.4D dissolvers. Multiple cores will be charged to the same dissolver solution maximizing the concentration of dissolved Al. The objective of this study was to identify flowsheet conditions through literature review and laboratory experimentation to safely and efficiently dissolve the HFIR fuel in H-Canyon. Laboratory-scale experiments were performed to evaluate the dissolution of HFIR fuel using both Al 1100 and Al 6061 T6 alloy coupons. The Al 1100 alloy was considered a representative surrogate which provided an upper bound on the generation of flammable (i.e., H2) gas during the dissolution process. The dissolution of the Al 6061 T6 alloy proceeded at a slower rate than the Al 1100 alloy and was used to verify that the target Al concentration in solution could be achieved for the selected Hg concentration. Mass spectrometry and Raman spectroscopy were used to provide continuous monitoring of the concentration of H2 and other permanent gases in the dissolution offgas allowing the development of H2 generation rate profiles. The H2 generation rates were subsequently used to evaluate if a full HFIR core could be dissolved in an H-Canyon dissolver without exceeding 60% of the calculated lower

  9. Dissolution Flowsheet for High Flux Isotope Reactor Fuel

    Energy Technology Data Exchange (ETDEWEB)

    Daniel, W. E. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Rudisill, T. S. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); O' Rourke, P. E. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Karay, N. S [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)

    2016-09-27

    As part of the Spent Nuclear Fuel (SNF) processing campaign, H-Canyon is planning to begin dissolving High Flux Isotope Reactor (HFIR) fuel in late FY17 or early FY18. Each HFIR fuel core contains inner and outer fuel elements which were fabricated from uranium oxide (U3O8) dispersed in a continuous Al phase using traditional powder metallurgy techniques. Fuels fabricated in this manner, like other SNF’s processed in H-Canyon, dissolve by the same general mechanisms with similar gas generation rates and the production of H2. The HFIR fuel cores will be dissolved and the recovered U will be down-blended into low-enriched U. HFIR fuel was previously processed in H-Canyon using a unique insert in both the 6.1D and 6.4D dissolvers. Multiple cores will be charged to the same dissolver solution maximizing the concentration of dissolved Al. The objective of this study was to identify flowsheet conditions through literature review and laboratory experimentation to safely and efficiently dissolve the HFIR fuel in H-Canyon. Laboratory-scale experiments were performed to evaluate the dissolution of HFIR fuel using both Al 1100 and Al 6061 T6 alloy coupons. The Al 1100 alloy was considered a representative surrogate which provided an upper bound on the generation of flammable (i.e., H2) gas during the dissolution process. The dissolution of the Al 6061 T6 alloy proceeded at a slower rate than the Al 1100 alloy, and was used to verify that the target Al concentration in solution could be achieved for the selected Hg concentration. Mass spectrometry and Raman spectroscopy were used to provide continuous monitoring of the concentration of H2 and other permanent gases in the dissolution offgas, allowing the development of H2 generation rate profiles. The H2 generation rates were subsequently used to evaluate if a full HFIR core could be dissolved in an H-Canyon dissolver without exceeding 60% of the

  10. Isotopic compositions of cometary matter returned by Stardust.

    Science.gov (United States)

    McKeegan, Kevin D; Aléon, Jerome; Bradley, John; Brownlee, Donald; Busemann, Henner; Butterworth, Anna; Chaussidon, Marc; Fallon, Stewart; Floss, Christine; Gilmour, Jamie; Gounelle, Matthieu; Graham, Giles; Guan, Yunbin; Heck, Philipp R; Hoppe, Peter; Hutcheon, Ian D; Huth, Joachim; Ishii, Hope; Ito, Motoo; Jacobsen, Stein B; Kearsley, Anton; Leshin, Laurie A; Liu, Ming-Chang; Lyon, Ian; Marhas, Kuljeet; Marty, Bernard; Matrajt, Graciela; Meibom, Anders; Messenger, Scott; Mostefaoui, Smail; Mukhopadhyay, Sujoy; Nakamura-Messenger, Keiko; Nittler, Larry; Palma, Russ; Pepin, Robert O; Papanastassiou, Dimitri A; Robert, François; Schlutter, Dennis; Snead, Christopher J; Stadermann, Frank J; Stroud, Rhonda; Tsou, Peter; Westphal, Andrew; Young, Edward D; Ziegler, Karen; Zimmermann, Laurent; Zinner, Ernst

    2006-12-15

    Hydrogen, carbon, nitrogen, and oxygen isotopic compositions are heterogeneous among comet 81P/Wild 2 particle fragments; however, extreme isotopic anomalies are rare, indicating that the comet is not a pristine aggregate of presolar materials. Nonterrestrial nitrogen and neon isotope ratios suggest that indigenous organic matter and highly volatile materials were successfully collected. Except for a single (17)O-enriched circumstellar stardust grain, silicate and oxide minerals have oxygen isotopic compositions consistent with solar system origin. One refractory grain is (16)O-enriched, like refractory inclusions in meteorites, suggesting that Wild 2 contains material formed at high temperature in the inner solar system and transported to the Kuiper belt before comet accretion.

  11. Nonlinear burn condition control in tokamaks using isotopic fuel tailoring

    Science.gov (United States)

    Boyer, Mark D.; Schuster, Eugenio

    2015-08-01

    One of the fundamental problems in tokamak fusion reactors is how to control the plasma density and temperature in order to regulate the amount of fusion power produced by the device. Control of these parameters will be critical to the success of burning plasma experiments like ITER. The most previous burn condition control efforts use either non-model based control designs or techniques based on models linearized around particular operating points. Such strategies limit the potential operational space and must be carefully retuned or redesigned to accommodate changes in operating points or plasma parameters. In this work, a nonlinear dynamic model of the spatial averages of energy and ion species densities is used to synthesize a nonlinear feedback controller for stabilizing the burn condition. The nonlinear model-based control strategy guarantees a much larger operational space than previous linear controllers. Because it is not designed around a particular operating point, the controller can be used to move from one burn condition to another. The proposed scheme first attempts to use regulation of the auxiliary heating power to reject temperature perturbations, then, if necessary, uses isotopic fuel tailoring as a way to reduce fusion heating during positive temperature perturbations. A global model of hydrogen recycling is incorporated into the model used for design and simulation, and the proposed control scheme is tested for a range of recycling model parameters. As we find the possibility of changing the isotopic mix can be limited for certain unfavorable recycling conditions, we also consider impurity injection as a back-up method for controlling the system. A simple supervisory control strategy is proposed to switch between the primary and back-up control schemes based on stability and performance criteria. A zero-dimensional simulation study is used to study the performance of the control scheme for several scenarios and model parameters. Finally, a one

  12. Zinc isotope fractionation during magmatic differentiation and the isotopic composition of the bulk Earth

    Science.gov (United States)

    Chen, Heng; Savage, Paul S.; Teng, Fang-Zehn; Helz, Rosalind T.; Moynier, Frédéric

    2013-01-01

    he zinc stable isotope system has been successfully applied to many and varied fields in geochemistry, but to date it is still not completely clear how this isotope system is affected by igneous processes. In order to evaluate the potential application of Zn isotopes as a proxy for planetary differentiation and volatile history, it is important to constrain the magnitude of Zn isotopic fractionation induced by magmatic differentiation. In this study we present high-precision Zn isotope analyses of two sets of chemically diverse, cogenetic samples from Kilauea Iki lava lake, Hawaii, and Hekla volcano, Iceland, which both show clear evidence of having undergone variable and significant degrees of magmatic differentiation. The Kilauea Iki samples display small but resolvable variations in Zn isotope composition (0.26‰66Zn66Zn defined as the per mille deviation of a sample's 66Zn/64Zn compositional ratio from the JMC-Lyon standard), with the most differentiated lithologies exhibiting more positive δ66Zn values. This fractionation is likely a result of the crystallization of olivine and/or Fe–Ti oxides, which can both host Zn in their crystal structures. Samples from Hekla have a similar range of isotopic variation (0.22‰66Zn66Zn=0.28±0.05‰ (2s.d.).

  13. Iron isotope composition of some Archean and Proterozoic iron formations

    Science.gov (United States)

    Planavsky, Noah; Rouxel, Olivier J.; Bekker, Andrey; Hofmann, Axel; Little, Crispin T. S.; Lyons, Timothy W.

    2012-03-01

    Fe isotopes can provide new insight into redox-dependent biogeochemical processes. Precambrian iron formations (IF) are deserving targets for Fe isotope studies because they are composed predominantly of authigenic Fe phases and record a period of unprecedented iron deposition in Earth's history. We present Fe isotope data for bulk samples from 24 Archean and Proterozoic IF and eight Phanerozoic Fe oxide-rich deposits. These data reveal that many Archean and early Paleoproterozoic iron formations were a sink for isotopically heavy Fe, in contrast to later Proterozoic and Phanerozoic Fe oxide-rich rocks. The positive δ56Fe values in IF are best explained by delivery of particulate ferric oxides formed in the water column to the sediment-water interface. Because IF are a net sink for isotopically heavy Fe, there must be a corresponding pool of isotopically light Fe in the sedimentary record. Earlier work suggested that Archean pyritic black shales were an important part of this light sink before 2.35 billion years ago (Ga). It is therefore likely that the persistently and anomalously low δ56Fe values in shales are linked with the deposition of isotopically heavy Fe in IF in the deeper parts of basins. IF deposition produced a residual isotopically light dissolved Fe pool that was captured by pyritic Fe in shales. Local dissimilatory Fe reduction in porewater and associated diagenetic reactions resulting in pyrite and carbonate precipitation may have further enhanced Fe isotope heterogeneity in marine sediments, and an 'iron shuttle' may have transported isotopically light Fe from shelf sediments to the basin. Nevertheless, water-column processing of hydrothermally delivered Fe likely had the strongest influence on the bulk iron isotope composition of Archean and Paleoproterozoic iron formations and other marine sediments.

  14. Soil Carbon: Compositional and Isotopic Analysis

    Energy Technology Data Exchange (ETDEWEB)

    Moran, James J.; Alexander, M. L.; Laskin, Alexander

    2016-11-01

    This is a short chapter to be included in the next edition of the Encyclopedia of Soil Science. The work here describes techniques being developed at PNNL for investigating organic carbon in soils. Techniques discussed include: laser ablation isotope ratio mass spectrometry, laser ablation aerosol mass spectrometry, and nanospray desorption electrospray ionization mass spectrometry.

  15. Stable isotope composition of human fingernails from Slovakia

    Energy Technology Data Exchange (ETDEWEB)

    Grolmusová, Zuzana, E-mail: zuzana.grolmusova@geology.sk [Comenius University in Bratislava, Faculty of Mathematics, Physics and Informatics, Department of Experimental Physics, Mlynská dolina F2, 842 48 Bratislava (Slovakia); State Geological Institute of Dionýz Štúr, Laboratory of Isotope Geology, Mlynská dolina 1, 817 04 Bratislava (Slovakia); Rapčanová, Anna [Comenius University in Bratislava, Faculty of Mathematics, Physics and Informatics, Department of Experimental Physics, Mlynská dolina F2, 842 48 Bratislava (Slovakia); Michalko, Juraj; Čech, Peter [State Geological Institute of Dionýz Štúr, Laboratory of Isotope Geology, Mlynská dolina 1, 817 04 Bratislava (Slovakia); Veis, Pavel [Comenius University in Bratislava, Faculty of Mathematics, Physics and Informatics, Department of Experimental Physics, Mlynská dolina F2, 842 48 Bratislava (Slovakia); State Geological Institute of Dionýz Štúr, Laboratory of Isotope Geology, Mlynská dolina 1, 817 04 Bratislava (Slovakia)

    2014-10-15

    Stable isotope composition of human fingernails has proven to be useful for documenting human dietary information and geographical patterns in archeological, forensic, anthropological and biological studies. Therefore, it is of interest to detect all factors influencing the stable isotopic composition in the certain regions in the world. Carbon and nitrogen isotope data of human fingernail keratin from 52 individuals from Slovakia were reported in this study. The online combustion and continuous flow isotope-ratio mass spectrometer Delta V Advantage was used for δ{sup 13}C and δ{sup 15}N analysis of fingernail keratin samples from 24 vegetarian and 28 omnivorous individuals. A group of people with frequent meat consumption showed enrichment in {sup 13}C and {sup 15}N isotopes in fingernails. A similar trend was observed with increasing seafood in an individual's diet. Moreover a significant difference was revealed between smokers and nonsmokers for both δ{sup 13}C and δ{sup 15}N values. These data were compared to previously published δ{sup 13}C and δ{sup 15}N fingernail values from across the globe. This study brings new information on the stable isotope signature of individuals from Slovakia and characterizes the Central European region for the first time. The stable isotope composition of fingernails is influenced by the frequency of meat and seafood consumption as well as smoking. - Highlights: • This study deals with stable isotope analyses of fingernails from Slovak volunteers. • δ{sup 13}C and δ{sup 15}N values of vegetarian and omnivore fingernails were compared. • Influence of sex, diet and smoking was studied.

  16. Carbon isotopic composition of individual Precambrian microfossils.

    Science.gov (United States)

    House, C H; Schopf, J W; McKeegan, K D; Coath, C D; Harrison, T M; Stetter, K O

    2000-08-01

    Ion microprobe measurements of carbon isotope ratios were made in 30 specimens representing six fossil genera of microorganisms petrified in stromatolitic chert from the approximately 850 Ma Bitter Springs Formation, Australia, and the approximately 2100 Ma Gunflint Formation, Canada. The delta 13C(PDB) values from individual microfossils of the Bitter Springs Formation ranged from -21.3 +/- 1.7% to -31.9 +/- 1.2% and the delta 13C(PDB) values from microfossils of the Gunflint Formation ranged from -32.4 +/- 0.7% to -45.4 +/- 1.2%. With the exception of two highly 13C-depleted Gunflint microfossils, the results generally yield values consistent with carbon fixation via either the Calvin cycle or the acetyl-CoA pathway. However, the isotopic results are not consistent with the degree of fractionation expected from either the 3-hydroxypropionate cycle or the reductive tricarboxylic acid cycle, suggesting that the microfossils studied did not use either of these pathways for carbon fixation. The morphologies of the microfossils suggest an affinity to the cyanobacteria, and our carbon isotopic data are consistent with this assignment.

  17. Composition heterogeneity analysis for DUPIC fuel(I) - Statistical analysis

    Energy Technology Data Exchange (ETDEWEB)

    Choi, Hang Bok [Korea Atomic Energy Research Institute, Taejon (Korea)

    1999-08-01

    The fuel composition heterogeneity effect on reactor performance parameters was assessed by refueling simulations for three DUPIC fuel options of fuel composition heterogeneity control: the fissile content adjustment, the reactivity control by slightly enriched and depleted uranium, and the reactivity control by natural uranium. For each DUPIC fuel option, the simulations were performed using 30 heterogeneous fuel types which were determined by the agglomerative hierarchical clustering method. The heterogeneity effect was considered during the refueling simulation by randomly selecting fuel types for the refueling operation. The refueling simulations of the heterogeneous core have shown that the key performance parameters such as the maximum channel power (MCP), maximum bundle power (MBP), and channel power peaking factor (CPPF) are close to those of the core that has single fuel type. For the three DUPIC fuel options, the uncertainties of MCP, MBP, and CPPF due to the fuel composition heterogeneity are less than 0.6, 1.5 and 0.8%, respectively, including the uncertainty of the group-average fuel property. This study has shown that the three DUPIC fuel options reduces the composition heterogeneity effectively and the zone power control system has a sufficient margin to adjust the perturbations cased by the fuel composition heterogeneity. 15 refs., 28 figs.,10 tabs. (Author)

  18. What controls the isotopic composition of Greenland surface snow?

    Directory of Open Access Journals (Sweden)

    H. C. Steen-Larsen

    2013-10-01

    Full Text Available Water stable isotopes in Greenland ice core data provide key paleoclimatic information, and have been compared with precipitation isotopic composition simulated by isotopically-enabled atmospheric models. However, post-deposition processes linked with snow metamorphism remain poorly documented. For this purpose, a monitoring of the isotopic composition (δ18O, δD of surface water vapor, precipitation and samples of top (0.5 cm snow surface has been conducted during two summers (2011–2012 at NEEM, NW Greenland. The measurements also include a subset of 17O-excess measurements over 4 days, and the measurements span the 2012 Greenland heat wave. Our observations are consistent with calculations assuming isotopic equilibrium between surface snow and water vapor. We observe a strong correlation between surface vapor δ18O and air temperature (0.85 ± 0.11 ‰ °C−1 (R = 0.76 for 2012. The correlation with air temperature is not observed in precipitation data or surface snow data. Deuterium excess (d-excess is strongly anti-correlated with δ18O with a stronger slope for vapor than for precipitation and snow surface data. During nine 1–5 days periods between precipitation events, our data demonstrate parallel changes of δ18O and d-excess in surface snow and surface vapor. The changes in δ18O of the vapor are similar or larger than those of the snow δ18O. It is estimated that 6 to 20% of the surface snow mass is exchanged with the atmosphere using the CROCUS snow model. In our data, the sign of surface snow isotopic changes is not related to the sign or magnitude of sublimation or condensation. Comparisons with atmospheric models show that day-to-day variations in surface vapor isotopic composition are driven by synoptic weather and changes in air mass trajectories and distillation histories. We suggest that, in-between precipitation events, changes in the surface snow isotopic composition are driven by these changes in surface vapor isotopic

  19. What controls the isotopic composition of Greenland surface snow?

    Directory of Open Access Journals (Sweden)

    H. C. Steen-Larsen

    2014-02-01

    Full Text Available Water stable isotopes in Greenland ice core data provide key paleoclimatic information, and have been compared with precipitation isotopic composition simulated by isotopically enabled atmospheric models. However, post-depositional processes linked with snow metamorphism remain poorly documented. For this purpose, monitoring of the isotopic composition (δ18O, δD of near-surface water vapor, precipitation and samples of the top (0.5 cm snow surface has been conducted during two summers (2011–2012 at NEEM, NW Greenland. The samples also include a subset of 17O-excess measurements over 4 days, and the measurements span the 2012 Greenland heat wave. Our observations are consistent with calculations assuming isotopic equilibrium between surface snow and water vapor. We observe a strong correlation between near-surface vapor δ18O and air temperature (0.85 ± 0.11‰ °C−1 (R = 0.76 for 2012. The correlation with air temperature is not observed in precipitation data or surface snow data. Deuterium excess (d-excess is strongly anti-correlated with δ18O with a stronger slope for vapor than for precipitation and snow surface data. During nine 1–5-day periods between precipitation events, our data demonstrate parallel changes of δ18O and d-excess in surface snow and near-surface vapor. The changes in δ18O of the vapor are similar or larger than those of the snow δ18O. It is estimated using the CROCUS snow model that 6 to 20% of the surface snow mass is exchanged with the atmosphere. In our data, the sign of surface snow isotopic changes is not related to the sign or magnitude of sublimation or deposition. Comparisons with atmospheric models show that day-to-day variations in near-surface vapor isotopic composition are driven by synoptic variations and changes in air mass trajectories and distillation histories. We suggest that, in between precipitation events, changes in the surface snow isotopic composition are driven by these changes in near

  20. What controls the isotopic composition of Greenland surface snow?

    Science.gov (United States)

    Steen-Larsen, H. C.; Masson-Delmotte, V.; Hirabayashi, M.; Winkler, R.; Satow, K.; Prié, F.; Bayou, N.; Brun, E.; Cuffey, K. M.; Dahl-Jensen, D.; Dumont, M.; Guillevic, M.; Kipfstuhl, S.; Landais, A.; Popp, T.; Risi, C.; Steffen, K.; Stenni, B.; Sveinbjörnsdottír, A. E.

    2014-02-01

    Water stable isotopes in Greenland ice core data provide key paleoclimatic information, and have been compared with precipitation isotopic composition simulated by isotopically enabled atmospheric models. However, post-depositional processes linked with snow metamorphism remain poorly documented. For this purpose, monitoring of the isotopic composition (δ18O, δD) of near-surface water vapor, precipitation and samples of the top (0.5 cm) snow surface has been conducted during two summers (2011-2012) at NEEM, NW Greenland. The samples also include a subset of 17O-excess measurements over 4 days, and the measurements span the 2012 Greenland heat wave. Our observations are consistent with calculations assuming isotopic equilibrium between surface snow and water vapor. We observe a strong correlation between near-surface vapor δ18O and air temperature (0.85 ± 0.11‰ °C-1 (R = 0.76) for 2012). The correlation with air temperature is not observed in precipitation data or surface snow data. Deuterium excess (d-excess) is strongly anti-correlated with δ18O with a stronger slope for vapor than for precipitation and snow surface data. During nine 1-5-day periods between precipitation events, our data demonstrate parallel changes of δ18O and d-excess in surface snow and near-surface vapor. The changes in δ18O of the vapor are similar or larger than those of the snow δ18O. It is estimated using the CROCUS snow model that 6 to 20% of the surface snow mass is exchanged with the atmosphere. In our data, the sign of surface snow isotopic changes is not related to the sign or magnitude of sublimation or deposition. Comparisons with atmospheric models show that day-to-day variations in near-surface vapor isotopic composition are driven by synoptic variations and changes in air mass trajectories and distillation histories. We suggest that, in between precipitation events, changes in the surface snow isotopic composition are driven by these changes in near-surface vapor

  1. Oxygen Isotope Composition of Nitrate Produced by Freshwater Nitrification

    Science.gov (United States)

    Boshers, D.; Granger, J.; Bohlke, J. K.

    2016-12-01

    Measurements of the naturally occurring nitrogen and oxygen stable isotope ratios of nitrate (NO3-), δ15N and δ18O, can be used to determine the source, dispersal, and fate of natural and contaminant NO3- in aquatic environments. To this end, it is necessary to know the extent to which NO3- isotopologues are modified by biological reactions, as heavy and light isotopes have different reaction rates. The purpose of this study was to determine the influence of the δ18O of ambient water on the isotope composition of NO3- produced during nitrification, the biological oxidation of ammonium (NH4+) to nitrite (NO2-) and then NO3-, which is poorly constrained in freshwater systems. To determine the δ18O of NO3- produced by nitrification in freshwater, we collected water from a stream in New England, which we amended with NH4+ and with increments of 18O-enriched water, to monitor the isotope composition of NO3- produced by a natural consortium of nitrifiers. Added NH4+ was completely oxidized to NO3- over 26 days. The final δ18O of nitrified NO3- revealed sensitivity to the δ18O of water mediated by (a) isotopic equilibration between water and NO2- and (b) kinetic isotope fractionation during O-atom incorporation from water into NO2- and NO3-. Our results concur with nitrifying culture experiments that have demonstrated analogous sensitivity of the δ18O of nitrified NO3- to equilibrium and kinetic O isotope effects (Buchwald et al. 2012), as well as show that these dynamics need to be considered to interpret NO3- isotope distribution in freshwater environments.

  2. Measurement of Plutonium Isotopic Composition - MGA

    Energy Technology Data Exchange (ETDEWEB)

    Vo, Duc Ta [Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

    2015-08-21

    In this module, we will use the Canberra InSpector-2000 Multichannel Analyzer with a high-purity germanium detector (HPGe) and the MGA isotopic anlysis software to assay a variety of plutonium samples. The module provides an understanding of the MGA method, its attributes and limitations. You will assess the system performance by measuring a range of materials similar to those you may assay in your work. During the final verification exercise, the results from MGA will be combined with the 240Pueff results from neutron coincidence or multiplicity counters so that measurements of the plutonium mass can be compared with the operator-declared (certified) values.

  3. Demonstration of femtosecond laser ablation inductively coupled plasma mass spectrometry for uranium isotopic measurements in U-10Mo nuclear fuel foils

    Energy Technology Data Exchange (ETDEWEB)

    Havrilla, George Joseph [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Gonzalez, Jhanis [Applied Spectra Inc., Fremont, CA (United States)

    2015-06-10

    The use of femtosecond laser ablation inductively coupled plasma mass spectrometry was used to demonstrate the feasibility of measuring the isotopic ratio of uranium directly in U-10Mo fuel foils. The measurements were done on both the flat surface and cross sections of bare and Zr clad U-10Mo fuel foil samples. The results for the depleted uranium content measurements were less than 10% of the accepted U235/238 ratio of 0.0020. Sampling was demonstrated for line scans and elemental mapping over large areas. In addition to the U isotopic ratio measurement, the Zr thickness could be measured as well as trace elemental composition if required. A number of interesting features were observed during the feasibility measurements which could provide the basis for further investigation using this methodology. The results demonstrate the feasibility of using fs-LA-ICP-MS for measuring the U isotopic ratio in U-10Mo fuel foils.

  4. Authentication of bell peppers using boron and strontium isotope compositions

    Science.gov (United States)

    Rosner, Martin; Pritzkow, Wolfgang; Vogl, Jochen; Voerkelius, Susanne

    2010-05-01

    The wrong declaration of food in terms of geographical origin and production method is a major problem for the individual consumer and public regulatory authorities. The authentication of food matrices using H-C-N-O-S isotopic compositions is already well established. However, specific questions require additional isotopic systems, which are more diagonstic for the source reservoires involved or production methods used. Here we present B and Sr isotopic compositions of bell peppers from Europe (Germany, Austria, Netherlands, Spain) and Israel to verfiy their origin. The bell peppers' B isotopic compositions between different locations are highly variable (d11BNISTSRM951 -8 to +35 ‰), whereas the 87Sr/86Sr ratios are all close to modern seawater Sr isotopic composition of about 0.7092 (0.7078 to 0.7107), but still can reliably be distinguished. Distinct isotopically heavy and light B isotopic fingerprints are obtained for bell peppers from Israel and the Netherlands. Samples from Germany, Austria, and Spain display overlapping d11B values between 0 and +12 ‰. Bell peppers from Israel show high d11B values (+28 to +35 ‰) combined with 87Sr/86Sr ratios slightly more unradiogenic than modern seawater (ca 0.7079). Bell peppers from the Netherlands, however, show low d11B values (-8 ‰) combinded with 87Sr/86Sr ratios of modern seawater (approx. 0.7085). Mainly based on diagnostic B isotopic compositions bell peppers from Israel and the Netherlands can be related to a specific geographical growing environment (Israel) or production method (Netherlands). The isotope fingerprints of bell peppers from the Netherlands are consistent with growing conditions in greenhouses typical for the Netherlands vegetable farming. Using optimized production methods crops in greenhouses were supplied with nutritients by liquid fertilizers on artificial substrates. As most fertilizers derive from non-marine salt deposits, fertilization typically imprints invariant d11B values close

  5. Isotope composition and volume of Earth's early oceans.

    Science.gov (United States)

    Pope, Emily C; Bird, Dennis K; Rosing, Minik T

    2012-03-20

    Oxygen and hydrogen isotope compositions of Earth's seawater are controlled by volatile fluxes among mantle, lithospheric (oceanic and continental crust), and atmospheric reservoirs. Throughout geologic time the oxygen mass budget was likely conserved within these Earth system reservoirs, but hydrogen's was not, as it can escape to space. Isotopic properties of serpentine from the approximately 3.8 Ga Isua Supracrustal Belt in West Greenland are used to characterize hydrogen and oxygen isotope compositions of ancient seawater. Archaean oceans were depleted in deuterium [expressed as δD relative to Vienna standard mean ocean water (VSMOW)] by at most 25 ± 5‰, but oxygen isotope ratios were comparable to modern oceans. Mass balance of the global hydrogen budget constrains the contribution of continental growth and planetary hydrogen loss to the secular evolution of hydrogen isotope ratios in Earth's oceans. Our calculations predict that the oceans of early Earth were up to 26% more voluminous, and atmospheric CH(4) and CO(2) concentrations determined from limits on hydrogen escape to space are consistent with clement conditions on Archaean Earth.

  6. Tracing anthropogenic thallium in soil using stable isotope compositions.

    Science.gov (United States)

    Kersten, Michael; Xiao, Tangfu; Kreissig, Katharina; Brett, Alex; Coles, Barry J; Rehkämper, Mark

    2014-08-19

    Thallium stable isotope data are used in this study, for the first time, to apportion Tl contamination in soils. In the late 1970s, a cement plant near Lengerich, Germany, emitted cement kiln dust (CKD) with high Tl contents, due to cocombustion of Tl-enriched pyrite roasting waste. Locally contaminated soil profiles were obtained down to 1 m depth and the samples are in accord with a binary mixing relationship in a diagram of Tl isotope compositions (expressed as ε(205)Tl, the deviation of the (205)Tl/(203)Tl ratio of a sample from the NIST SRM 997 Tl isotope standard in parts per 10(4)) versus 1/[Tl]. The inferred mixing endmembers are the geogenic background, as defined by isotopically light soils at depth (ε(205)Tl ≈ -4), and the Tl emissions, which produce Tl-enriched topsoils with ε(205)Tl as high as ±0. The latter interpretation is supported by analyses of the CKD, which is also characterized by ε(205)Tl ≈ ± 0, and the same ε(205)Tl value was found for a pyrite from the deposit that produced the cocombusted pyrite roasting waste. Additional measurements for samples from a locality in China, with outcrops of Tl sulfide mineralization and associated high natural Tl backgrounds, reveal significant isotope fractionation between soils (ε(205)Tl ≈ +0.4) and locally grown green cabbage (ε(205)Tl between -2.5 and -5.4). This demonstrates that biological isotope fractionation cannot explain the isotopically heavy Tl in the Lengerich topsoils and the latter are therefore clearly due to anthropogenic Tl emissions from cement processing. Our results thus establish that isotopic data can reinforce receptor modeling for the toxic trace metal Tl.

  7. Characteristics of carbon and hydrogen isotopic compositions of light hydrocarbons

    Institute of Scientific and Technical Information of China (English)

    沈平

    1995-01-01

    Light hydrocarbons named in the present paper refer to the natural gas-associated light oil and condensate 46 light oil and condensate samples from 11 oil-bearing basins of China were collected and their carbon and hydrogen isotopic compositions were analysed in terms of their total hydrocarbons, saturated hydrocarbons and a part of aromatic fractions, and gas-source materials and their sedimentary environments were discussed based on the above-mentioned data and the geological background of each area. From the view of carbon and hydrogen isotopic composition of total hydrocarbons and saturated hydrocarbons, it is revealed that the condensate related to coal-bearing strata is enriched in 13C and D while that related to the source material of type I-II is enriched in 12C. In general, the isotopic composition of carbon is mainly attributed to the inheriting effect of their source materials, whereas that of hydrogen principally reflects the correlationship between hydrogen isotopes and the sedimentary envi

  8. The isotopic composition of solar flare accelerated neon

    Science.gov (United States)

    Mewaldt, R. A.; Spalding, J. D.; Stone, E. C.; Vogt, R. E.

    1979-01-01

    The individual isotopes of neon in energetic solar-flare particles have been clearly resolved with a rms mass resolution of 0.20 amu. The ratios found are Ne-20/Ne-22 = 7.6 (+2.0, -1.8) and Ne-21/Ne-22 of no more than about 0.11 in the 11-26 MeV per nucleon interval. This isotopic composition is essentially the same as that of meteoritic planetary neon-A and is significantly different from that of the solar wind.

  9. Stable isotope composition and volume of Early Archaean oceans

    DEFF Research Database (Denmark)

    Pope, Emily Catherine; Rosing, Minik Thorleif; Bird, Dennis K.

    Oxygen and hydrogen isotope compositions of seawater are controlled by volatile fluxes between mantle, lithospheric (oceanic and continental crust) and atmospheric reservoirs. Throughout geologic time oxygen was likely conserved within these Earth system reservoirs, but hydrogen was not, as it can...... escape to space [1]. Hydrogen isotope ratios of serpentinites from the ~3.8Ga Isua Supracrustal Belt in West Greenland are between -53 and -99‰; the highest values are in antigorite ± lizardite serpentinites from a low-strain lithologic domain where hydrothermal reaction of Archaean seawater with oceanic...

  10. Do foraminifera accurately record seawater neodymium isotope composition?

    Science.gov (United States)

    Scrivner, Adam; Skinner, Luke; Vance, Derek

    2010-05-01

    Palaeoclimate studies involving the reconstruction of past Atlantic meridional overturning circulation increasingly employ isotopes of neodymium (Nd), measured on a variety of sample media (Frank, 2002). In the open ocean, Nd isotopes are a conservative tracer of water mass mixing and are unaffected by biological and low-temperature fractionation processes (Piepgras and Wasserburg, 1987; Lacan and Jeandel, 2005). For decades, benthic foraminifera have been widely utilised in stable isotope and geochemical studies, but have only recently begun to be exploited as a widely distributed, high-resolution Nd isotope archive (Klevenz et al., 2008), potentially circumventing the difficulties associated with other methods used to recover past deep-water Nd isotopes (Klevenz et al., 2008; Rutberg et al., 2000; Tachikawa et al., 2004). Thus far, a single pilot study (Klevenz et al., 2008) has indicated that core-top sedimentary benthic foraminifera record a Nd isotope composition in agreement with the nearest available bottom seawater data, and has suggested that this archive is potentially useful on both millennial and million-year timescales. Here we present seawater and proximal core-top foraminifer Nd isotope data for samples recovered during the 2008 "RETRO" cruise of the Marion Dufresne. The foraminifer samples comprise a depth-transect spanning 3000m of the water column in the Angola Basin and permit a direct comparison between high-resolution water column and core-top foraminiferal Nd isotope data. We use these data to assess the reliability of both planktonic and benthic foraminifera as recorders of water column neodymium isotope composition. Frank, M., 2002. Radiogenic isotopes: Tracers of past ocean circulation and erosional input, Rev. Geophys., 40 (1), 1001, doi:10.1029/2000RG000094. Klevenz, V., Vance, D., Schmidt, D.N., and Mezger, K., 2008. Neodymium isotopes in benthic foraminifera: Core-top systematics and a down-core record from the Neogene south Atlantic

  11. C-isotope composition of fossil sedges and grasses

    Science.gov (United States)

    Kurschner, Wolfram M.

    2010-05-01

    C4 plants differ from C3 plants regarding their anatomy and their C-isotope composition. Both features can be used in the geological record to determine the presence of C4 plants. Yet, the evolution of the C4 pathway in the fossil record is enigmatic as palaeobotanical and geological evidence for C4 plants is sparse. The oldest structural evidence for Kranz anatomy has been found in Late Miocene permineralized grass leaf remains. But studies on the C-isotope composition of sedimentary organic matter indicate that abundant C4 biomass was present in N-America and Asia throughout the Miocene in expanding savannahs and grasslands. The success of C4 plants appears to be related also to an increasing seasonal aridity in the tropical climate belts and the co-evolution of grazers. However, C- isotope composition of palaeosols or vertebrate teeth only allows to estimate the abundance of C4 plant biomass in the vegetation or in the diet without further taxonomical specification which plant groups would have had C4 metabolism. In this contribution the first extensive C-isotope analysis of fossil seeds of sedges and a few grasses are presented. The age of the carpological material ranges from Late Eocene to Pliocene and was collected from several central European brown coal deposits. The 52 different taxa studied include several species of Carex, Cladiocarya, Eriopherum, Eleocharis, Scirpus, Sparganium. Most of them representing herbaceous elements of a (sub)tropical vegetation growing near the edge of a lake. The C-isotope composition of the fossil seeds varies between -30 and -23 o/oo indicating C3 photosynthesis. This first systematic inventory shows that C4 plants were absent in the European (sub)tropical brown coal forming wetland vegetation during the Tertiary. These preliminary data are in agreement with phylogenetic studies which predict the origin of C4 plants outside the European realm.

  12. Spent fuel composition database system on WWW. SFCOMPO on WWW Ver.2

    Energy Technology Data Exchange (ETDEWEB)

    Mochizuki, Hiroki [Japan Research Institute, Ltd., Tokyo (Japan); Suyama, Kenya; Nomura, Yasushi; Okuno, Hiroshi [Japan Atomic Energy Research Inst., Tokai, Ibaraki (Japan). Tokai Research Establishment

    2001-08-01

    'SFCOMPO on WWW Ver.2' is an advanced version of 'SFCOMPO on WWW' ('Spent Fuel Composition Database System on WWW') released in 1997. This new version has a function of database management by an introduced relational database software 'PostgreSQL' and has various searching methods. All of the data required for the calculation of isotopic composition is available from the web site of this system. This report describes the outline of this system and the searching method using Internet. In addition, the isotopic composition data and the reactor data of the 14 LWRs (7 PWR and 7 BWR) registered in this system are described. (author)

  13. Boron isotopic compositions of some boron minerals

    Energy Technology Data Exchange (ETDEWEB)

    Oi, Takao; Musashi, Masaaki; Ossaka, Tomoko; Kakihana, Hidetake (Sophia Univ., Tokyo (Japan)); Nomura, Masao; Okamoto, Makoto (Tokyo Institute of Technology (Japan))

    1989-12-01

    Boron minerals that have different structural formulae but are supposed to have the same geologic origin have been collected and analyzed for the {sup 11}B/{sup 10}B isotopic ratio. It has been reconfirmed that minerals of marine origin have higher {sup 11}B/{sup 10}B ratios than those of nonmarine origin. It has been found that the sequence of decreasing {sup 11}B/{sup 10}B values among the minerals with the same geologic origin is; borax, tincal, kernite (Na borates) > ulexite (Na/Ca borate) > colemanite, iyoite, meyerhofferite (Ca borates). This sequence is explainable on the basis of the difference in crystal structure among the minerals. That is, minerals with high BO{sub 3}/BO{sub 4} ratios, (the ratio of the number of the BO{sub 3} triangle units to the number of the BO{sub 4} tetrahedron units in the structural formula of a mineral) have higher {sup 11}B/{sup 10}B ratios.

  14. Stable isotope composition and volume of Early Archaean oceans

    DEFF Research Database (Denmark)

    Pope, Emily Catherine; Rosing, Minik Thorleif; Bird, Dennis K.

    Oxygen and hydrogen isotope compositions of seawater are controlled by volatile fluxes between mantle, lithospheric (oceanic and continental crust) and atmospheric reservoirs. Throughout geologic time oxygen was likely conserved within these Earth system reservoirs, but hydrogen was not, as it can...... escape to space [1]. Hydrogen isotope ratios of serpentinites from the ~3.8Ga Isua Supracrustal Belt in West Greenland are between -53 and -99‰; the highest values are in antigorite ± lizardite serpentinites from a low-strain lithologic domain where hydrothermal reaction of Archaean seawater with oceanic...... of continents present at that time), and the mass of Early Archaean oceans to ~109 to 126% of present day oceans. Oxygen isotope analyses from these Isua serpentinites (δ18O = +0.1 to 5.6‰ relative to VSMOW) indicate that early Archaean δ18OSEAWATER similar to modern oceans. Our observations suggest...

  15. Triple oxygen isotope composition of the Campi Flegrei magma systems

    Science.gov (United States)

    Iovine, Raffaella Silvia; Wörner, Gerhard; Pack, Andreas; Sengupta, Sukanya; Carmine Mazzeo, Fabio; Arienzo, Ilenia; D'Antonio, Massimo

    2017-04-01

    Sr-O isotope relationships in igneous rocks are a powerful tool to distinguish magma sources and quantify assimilation processes in magmatic rocks. Isotopic (87Sr/86Sr and 18O/16O-17O/16O) data have been acquired on whole rocks and separated minerals (feldspar, Fe-cpx, Mg-cpx, olivine phenocrysts) from pyroclastic products of the Campi Flegrei volcanic complex (Gulf of Naples, Southern Italy). Oxygen isotope ratios were measured by infrared laser fluorination using a Thermo MAT253 gas source isotope ratio mass spectrometer in dual inlet mode, on ˜2 mg of hand-picked phenocrysts. Variations in triple oxygen isotope ratios (17O/16O, 18O/16O) are expressed as the δ notation relative to VSMOW. Sr isotopic compositions were determined by thermal ionization mass spectrometry after standard cation-exchange methods on separated hand-picked phenocrysts (˜300 mg), and on whole rocks, in case of insufficient sample size to separate crystals. Sr-isotopes in Campi Flegrei minerals range from 0.707305 to 0.707605 and δ18O varies from 6.5 to 8.3‰ . Recalculated δ18Omelt values accordingly show a large range between 7.2 and 8.6‰ . Our data, compared with published δ18O-isotope data from other Italian volcanic centers (Alban Hills, Mts. Ernici, Ischia, Mt. Vesuvius, Aeolian Islands, Tuscany and Sardinia) and from subduction zones worldwide (Kamchatka, Lesser Antilles, Indonesia and Central Andean ignimbrites), show compositions that are very different from typical mantle values. Distinct trends and sources are recognized in our compilation from global data: (1) serpentinized mantle (Kamchatka), (2) sediment-enrichment in the mantle source (Indonesia, Lesser Antilles, Eolian arc), (3) assimilation of old radiogenic continental crust affecting magmas derived from sediment-modified mantle sources (Tuscany, Sardinia), (4) assimilation of lower crustal lithologies (Central Andes, Alban Hills, Mts. Ernici, Ischia). Sr-O-isotope values of Campi Flegrei and Vesuvius magmas

  16. Stable isotopic composition of bottled mineral waters from Romania

    Science.gov (United States)

    Bădăluţă, Carmen; Nagavciuc, Viorica; Perșoiu, Aurel

    2015-04-01

    Romania has a high potential of mineral waters resources, featuring one of the largest mineral resources at European and global level. In the last decade, due to increased in consumption of bottled water, numerous brands have appeared on the market, with equally numerous and variable sources of provenance. In this study we have analyzed the isotopic composition of bottled mineral waters from Romania in order to determine their source and authenticity. We have analysed 32 carbonated and 24 non-carbonated mineral waters from Romania. and the results were analysed in comparison with stable isotope data from precipitation and river waters. Generally, the isotopic values of the mineral waters follow those in precipitation; however, differences occur in former volcanic regions (due to deep circulation of meteoric waters and increased exchange with host rock and volcanic CO2), as well as in mountainous regions, where high-altitude recharge occurs.

  17. The carbon isotopic compositions of Non-methane Hydrocarbons in atmosphere

    Institute of Scientific and Technical Information of China (English)

    PENG Lin; ZHANG HuiMin; REN ZhaoFang; MU Ling; SHI RuiLiang; CHANG LiPing; LI Fan

    2009-01-01

    Carbon isotopic compositions of atmospheric Non-methane Hydrocarbons (NMHCs) in the urban areas of Taiyuan and Lanzhou in summer were reported and the sources of NMHCs are discussed.Carbon isotopic ratios (δ13C) of vehicle exhaust,coal-combustion exhaust,fuel volatiles and cooking exhaust were also measured with thermal desorption-gas chromatography-isotope ratio-mass spectrometry (TD-GC-IR-MS).δ13C values of NMHCs in the urban areas of Lanzhou and Taiyuan range from -32.3‰ to -22.3‰ and from -32.8‰ to -18.1‰.δ13C values of vehicle exhaust,coal-combustion exhaust,fuel volatiles and cooking exhaust are -32.5‰--21.7‰,-24.5‰--22.3‰,-32.5%--27.4‰ and -31.6‰--24.5‰,respectively.The data indicate that vehicle exhaust and cooking exhaust make a significant contribution to the atmospheric NMHCs.Therefore,to reduce emissions of vehicle exhaust and cook-ing exhaust is critical for controlling atmospheric NMHCs pollution in summer.

  18. The chromium isotope composition of reducing and oxic marine sediments

    Science.gov (United States)

    Gueguen, Bleuenn; Reinhard, Christopher T.; Algeo, Thomas J.; Peterson, Larry C.; Nielsen, Sune G.; Wang, Xiangli; Rowe, Harry; Planavsky, Noah J.

    2016-07-01

    The chromium (Cr) isotope composition of marine sediments has the potential to provide new insights into the evolution of Earth-surface redox conditions. There are significant but poorly constrained isotope fractionations associated with oxidative subaerial weathering and riverine transport, the major source of seawater Cr, and with partial Cr reduction during burial in marine sediments, the major sink for seawater Cr. A more comprehensive understanding of these processes is needed to establish global Cr isotope mass balance and to gauge the utility of Cr isotopes as a paleoredox proxy. For these purposes, we investigated the Cr isotope composition of reducing sediments from the upwelling zone of the Peru Margin and the deep Cariaco Basin. Chromium is present in marine sediments in both detrital and authigenic phases, and to estimate the isotopic composition of the authigenic fraction, we measured δ53Cr on a weakly acid-leached fraction in addition to the bulk sediment. In an effort to examine potential variability in the Cr isotope composition of the detrital fraction, we also measured δ53Cr on a variety of oxic marine sediments that contain minimal authigenic Cr. The average δ53Cr value of the oxic sediments examined here is -0.05 ± 0.10‰ (2σ, n = 25), which is within the range of δ53Cr values characteristic of the bulk silicate Earth. This implies that uncertainty in estimates of authigenic δ53Cr values based on bulk sediment analyses is mainly linked to estimation of the ratio of Cr in detrital versus authigenic phases, rather than to the Cr-isotopic composition of the detrital pool. Leaches of Cariaco Basin sediments have an average δ53Cr value of +0.38 ± 0.10‰ (2σ, n = 7), which shows no dependency on sample location within the basin and is close to that of Atlantic deepwater Cr (∼+0.5‰). This suggests that authigenic Cr in anoxic sediments may reliably reflect the first-order Cr isotope composition of deepwaters. For Peru Margin samples

  19. Biomass Conversion into Solid Composite Fuel for Bed-Combustion

    Directory of Open Access Journals (Sweden)

    Tabakaev Roman B.

    2015-01-01

    Full Text Available The purpose of this research is the conversion of different types of biomass into solid composite fuel. The subject of research is the heat conversion of biomass into solid composite fuel. The research object is the biomass of the Tomsk region (Russia: peat, waste wood, lake sapropel. Physical experiment of biomass conversion is used as method of research. The new experimental unit for thermal conversion of biomass into carbon residue, fuel gas and pyrolysis condensate is described. As a result of research such parameters are obtained: thermotechnical biomass characteristics, material balances and product characteristics of the heat-technology conversion. Different methods of obtaining solid composite fuel from the products of thermal technologies are considered. As a result, it is established: heat-technology provides efficient conversion of the wood chips and peat; conversion of the lake sapropel is inefficient since the solid composite fuel has the high ash content and net calorific value.

  20. Modeling the carbon isotope composition of bivalve shells (Invited)

    Science.gov (United States)

    Romanek, C.

    2010-12-01

    The stable carbon isotope composition of bivalve shells is a valuable archive of paleobiological and paleoenvironmental information. Previous work has shown that the carbon isotope composition of the shell is related to the carbon isotope composition of dissolved inorganic carbon (DIC) in the ambient water in which a bivalve lives, as well as metabolic carbon derived from bivalve respiration. The contribution of metabolic carbon varies among organisms, but it is generally thought to be relatively low (e.g., organism and high (>90%) in the shells from terrestrial organisms. Because metabolic carbon contains significantly more C-12 than DIC, negative excursions from the expected environmental (DIC) signal are interpreted to reflect an increased contribution of metabolic carbon in the shell. This observation contrasts sharply with modeled carbon isotope compositions for shell layers deposited from the inner extrapallial fluid (EPF). Previous studies have shown that growth lines within the inner shell layer of bivalves are produced during periods of anaerobiosis when acidic metabolic byproducts (e.g., succinic acid) are neutralized (or buffered) by shell dissolution. This requires the pH of EPF to decrease below ambient levels (~7.5) until a state of undersaturation is achieved that promotes shell dissolution. This condition may occur when aquatic bivalves are subjected to external stressors originating from ecological (predation) or environmental (exposure to atm; low dissolved oxygen; contaminant release) pressures; normal physiological processes will restore the pH of EPF when the pressure is removed. As a consequence of this process, a temporal window should also exist in EPF at relatively low pH where shell carbonate is deposited at a reduced saturation state and precipitation rate. For example, EPF chemistry should remain slightly supersaturated with respect to aragonite given a drop of one pH unit (6.5), but under closed conditions, equilibrium carbon isotope

  1. Uncertainty analysis of spent nuclear fuel isotopics and rod internal pressure

    Science.gov (United States)

    Bratton, Ryan N.

    The bias and uncertainty in fuel isotopic calculations for a well-defined radio- chemical assay benchmark are investigated with Sampler, the new sampling-based uncertainty quantification tool in the SCALE code system. Isotopic predictions are compared to measurements of fuel rod MKP109 of assembly D047 from the Calvert Cliffs Unit 1 core at three axial locations, representing a range of discharged fuel burnups. A methodology is developed which quantifies the significance of input parameter uncertainties and modeling decisions on isotopic prediction by compar- ing to isotopic measurement uncertainties. The SCALE Sampler model of the D047 assembly incorporates input parameter uncertainties for key input data such as multigroup cross sections, decay constants, fission product yields, the cladding thickness, and the power history for fuel rod MKP109. The effects of each set of input parameter uncertainty on the uncertainty of isotopic predictions have been quantified. In this work, isotopic prediction biases are identified and an investiga- tion into their sources is proposed; namely, biases have been identified for certain plutonium, europium, and gadolinium isotopes for all three axial locations. More- over, isotopic prediction uncertainty resulting from only nuclear data is found to be greatest for Eu-154, Gd-154, and Gd-160. The discharge rod internal pressure (RIP) and cladding hoop stress (CHS) distributions are quantified for Watts Bar Nuclear Unit 1 (WBN1) fuel rods by modeling core cycle design data, operation data (including modeling significant trips and downpowers), and as-built fuel enrichments and densities of each fuel rod in FRAPCON-3.5. A methodology is developed which tracks inter-cycle as- sembly movements and assembly batch fabrication information to build individual FRAPCON inputs for each considered WBN1 fuel rod. An alternate model for the amount of helium released from zirconium diboride (ZrB2) integral fuel burn- able absorber (IFBA) layers is

  2. MUICYCL and MUIFAP: models tracking minor uranium isotopes in the nuclear fuel cycle

    Energy Technology Data Exchange (ETDEWEB)

    Blum, S.R.; McLaren, R.A.

    1979-10-01

    Two computer programs have been written to provide information on the buildup of minor uranium isotopes in the nuclear fuel cycle. The Minor Uranium Isotope Cycle Program, MUICYCL, tracks fuel through a multiyear campaign cycle of enrichment, reactor burnup, reprocessing, enrichment, etc. MUICYCL facilities include preproduction stockpiles, U/sup 235/ escalation, and calculation of losses. The Minor Uranium Isotope Flowsheet Analyzer Program, MUIFAP, analyzes one minor isotope in one year of an enrichment operation. The formulation of the enrichment cascade, reactors, and reprocessing facility is presented. Input and output descriptions and sample cases are presented. The programs themselves are documented by short descriptions of each routine, flowcharts, definitions of common blocks and variables, and internal documentation. The programs are written in FORTRAN for use in batch mode.

  3. Alkali elemental and potassium isotopic compositions of Semarkona chondrules

    Science.gov (United States)

    Alexander, C.M. O'D.; Grossman, J.N.

    2005-01-01

    We report measurements of K isotope ratios in 28 Semarkona chondrules with a wide range of petrologic types and bulk compositions as well as the compositions of CPX-mesostasis pairs in 17 type I Semarkona chondrules, including two chondrules with radial alkali zonation and 19 type II chondrules. Despite the wide range in K/Al ratios, no systematic variations in K isotopic compositions were found. Semarkona chondrules do not record a simple history of Rayleigh-type loss of K. Experimentally determined evaporation rates suggest that considerable alkali evaporation would have occurred during chondrule formation. Nevertheless, based on Na CPX-mesostasis distribution coefficients, the alkali contents of the cores of most chondrules in Semarkona were probably established at the time of final crystallization. However, Na CPX-mesostasis distribution coefficients also show that alkali zonation in type I Semarkona chondrules was produced by entry of alkalis after solidification, probably during parent body alteration. This alkali metasomatism may have gone to completion in some chondrules. Our preferred explanation for the lack of systematic isotopic enrichments, even in alkali depleted type I chondrule cores, is that they exchanged with the ambient gas as they cooled. ?? The Meteoritical Society, 2005.

  4. Establishing Specifications for Low Enriched Uranium Fuel Operations Conducted Outside the High Flux Isotope Reactor Site

    Energy Technology Data Exchange (ETDEWEB)

    Pinkston, Daniel [ORNL; Primm, Trent [ORNL; Renfro, David G [ORNL; Sease, John D [ORNL

    2010-10-01

    The National Nuclear Security Administration (NNSA) has funded staff at Oak Ridge National Laboratory (ORNL) to study the conversion of the High Flux Isotope Reactor (HFIR) from the current, high enriched uranium fuel to low enriched uranium fuel. The LEU fuel form is a metal alloy that has never been used in HFIR or any HFIR-like reactor. This report provides documentation of a process for the creation of a fuel specification that will meet all applicable regulations and guidelines to which UT-Battelle, LLC (UTB) the operating contractor for ORNL - must adhere. This process will allow UTB to purchase LEU fuel for HFIR and be assured of the quality of the fuel being procured.

  5. Light and heavy element isotopic compositions of mainstream SiC grains.

    Energy Technology Data Exchange (ETDEWEB)

    Amari, S.; Clayton, R. N.; Davis, A. M.; Lewis, R. S.; Pellin, M. J.

    1999-02-03

    Although a variety of types of pre-solar SiC grains have been classified by their C, N, and Si isotopic composition, the majority of such grains are so-called mainstream grains and are believed to have come from asymptotic giant branch stars [1]. We have previously reported the Mo isotopic compositions of presolar SiC grains whose C, N, and Si isotopic compositions were not known [2]. Since most presolar SiC grains fall in the mainstream group, we assumed that these grains were mainstream. The excellent match of the Mo isotopic data with expectations for nucleosynthesis in AGB stars was consistent with this identification. In order to better understand the distribution of isotopic compositions in presolar grains, we have begun to measure heavy element isotopic compositions of presolar SiC grains of known C, N and Si isotopic composition.

  6. Clumped-isotope geochemistry of carbonates: A new tool for the reconstruction of temperature and oxygen isotope composition of seawater

    Energy Technology Data Exchange (ETDEWEB)

    Bernasconi, Stefano M., E-mail: Stefano.bernasconi@erdw.ethz.ch [Geological Institute, ETH Zuerich, Sonneggstrasse 5, 8092 Zuerich (Switzerland); Schmid, Thomas W.; Grauel, Anna-Lena [Geological Institute, ETH Zuerich, Sonneggstrasse 5, 8092 Zuerich (Switzerland); Mutterlose, Joerg [Institut fuer Geologie, Mineralogie und Geophysik, Ruhr Universitaet Bochum, Universitaetsstr. 150, 44801 Bochum (Germany)

    2011-06-15

    Highlights: > Clumped-isotope thermometry of carbonates is discussed. > Clumped isotopes of Belemnites show higher sea surface temperatures than commonly assumed for the lower Cretaceous. > The potential of clumped-isotope measurement on foraminifera is discussed. - Abstract: Clumped-isotope geochemistry deals with State of ordering of rare isotopes in molecules, in particular with their tendency to form bonds with other rare isotopes rather than with the most abundant ones. Among its possible applications, carbonate clumped-isotope thermometry is the one that has gained most attention because of the wide potential of applications in many disciplines of the earth sciences. In particular, it allows reconstructing the temperature of formation of carbonate minerals without knowledge of the isotopic composition of the water from which they were formed. In addition, the O isotope composition of the waters from which they were formed can be calculated using the {delta}{sup 18}O of the same carbonate sample. This feature offers new approaches in paleoclimatology for reconstructing past global geochemical cycles. In this contribution two applications of this method are presented. First the potential of a new analytical method of measurement of clumped isotopes on small samples of foraminifera, for high-resolution SST and seawater {delta}{sup 18}O reconstructions from marine sediments is shown. Furthermore the potential of clumped isotope analysis of belemnites, for reconstructing seawater {delta}{sup 18}O and temperatures in the Cretaceous is shown.

  7. Magnesium stable isotope composition of Earth's upper mantle

    Science.gov (United States)

    Handler, Monica R.; Baker, Joel A.; Schiller, Martin; Bennett, Vickie C.; Yaxley, Gregory M.

    2009-05-01

    The mantle is Earth's largest reservoir of Mg containing > 99% of Earth's Mg inventory. However, no consensus exists on the stable Mg isotope composition of the Earth's mantle or how variable it is and, in particular, whether the mantle has the same stable Mg isotope composition as chondrite meteorites. We have determined the Mg isotope composition of olivine from 22 mantle peridotites from eastern Australia, west Antarctica, Jordan, Yemen and southwest Greenland by pseudo-high-resolution MC-ICP-MS on Mg purified to > 99%. The samples include fertile lherzolites, depleted harzburgites and dunites, cryptically metasomatised ('dry') peridotites and modally metasomatised apatite ± amphibole-bearing harzburgites and wehrlites. Olivine from these samples of early Archaean through to Permian lithospheric mantle have δ25Mg DSM-3 = - 0.22 to - 0.08‰. These data indicate the bulk upper mantle as represented by peridotite olivine is homogeneous within current analytical uncertainties (external reproducibility ≤ ± 0.07‰ [2 sd]). We find no systematic δ25Mg variations with location, lithospheric age, peridotite fertility, or degree or nature of mantle metasomatism. Although pyroxene may have slightly heavier δ25Mg than coexisting olivine, any fractionation between mantle pyroxene and olivine is also within current analytical uncertainties with a mean Δ25Mg pyr-ol = +0.06 ± 0.10‰ (2 sd; n = 5). Our average mantle olivine δ25Mg DSM-3 = - 0.14 ± 0.07‰ and δ26Mg DSM-3 = - 0.27 ± 0.14‰ (2 sd) are indistinguishable from the average of data previously reported for terrestrial basalts, confirming that basalts have stable Mg isotope compositions representative of the mantle. Olivine from five pallasite meteorites have δ25Mg DSM-3 = - 0.16 to - 0.11‰ that are identical to terrestrial olivine and indistinguishable from the average δ25Mg previously reported for chondrites. These data provide no evidence for measurable heterogeneity in the stable Mg isotope

  8. The triple isotopic composition of oxygen in leaf water

    Science.gov (United States)

    Landais, A.; Barkan, E.; Yakir, D.; Luz, B.

    2006-08-01

    The isotopic composition of atmospheric O 2 depends on the rates of oxygen cycling in photosynthesis, respiration, photochemical reactions in the stratosphere and on δ17O and δ18O of ocean and leaf water. While most of the factors affecting δ17O and δ18O of air O 2 have been studied extensively in recent years, δ17O of leaf water—the substrate for all terrestrial photosynthesis—remained unknown. In order to understand the isotopic composition of atmospheric O 2 at present and in fossil air in ice cores, we studied leaf water in field experiments in Israel and in a European survey. We measured the difference in δ17O and δ18O between stem and leaf water, which is the result of isotope enrichment during transpiration. We calculated the slopes of the lines linking the isotopic compositions of stem and leaf water. The obtained slopes in ln( δ17O + 1) vs. ln( δ18O + 1) plots are characterized by very high precision (˜0.001) despite of relatively large differences between duplicates in both δ17O and δ18O (0.02-0.05‰). This is so because the errors in δ18O and δ17O are mass-dependent. The slope of the leaf transpiration process varied between 0.5111 ± 0.0013 and 0.5204 ± 0.0005, which is considerably smaller than the slope linking liquid water and vapor at equilibrium (0.529). We further found that the slope of the transpiration process decreases with atmospheric relative humidity ( h) as 0.522-0.008 × h, for h in the range 0.3-1. This slope is neither influenced by the plant species, nor by the environmental conditions where plants grow nor does it show strong variations along long leaves.

  9. Gamma spectrometry inspection of TRIGA MARK II fuel using caesium isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Karimzadeh, S., E-mail: sam.karimzadeh@ati.ac.a [Vienna University of Technology, Institute of Atomic and Subatomic Physics (ATI), Stadionallee 2, A-1020 Vienna (Austria); Khan, R.; Boeck, H. [Vienna University of Technology, Institute of Atomic and Subatomic Physics (ATI), Stadionallee 2, A-1020 Vienna (Austria)

    2011-01-15

    Research highlights: Cs isotopes are the best choices for the burn up determination of spent fuel. Gamma spectrometer calibration using MCNP5. Cs-ratio can be applied by relative calibration method. - Abstract: Gamma spectrometry is one of the common methods to inspect the spent fuel from research reactors. This method has been applied to in-pool measurements of the Spent Fuel Elements (SPEs) of the TRIGA Mark II research reactor. Due to mixed nature of the reactor core and complicated irradiation history of the fuel elements (FEs), the gamma spectrometry of the FE establishes improvements in the calculation and measurement of the SPE. In order to inspect the TRIGA SPE from dry storage and cooled fuel from the reactor pool, the selected spend fuels are scanned and measured using the fuel-scanning machine. Gamma spectrometry is performed by HPGe detector for spend fuel inspection and determination of the {sup 137}Cs activity and {sup 134}Cs/{sup 137}Cs ratio. In this work, the steps of the detector calibration and the use of the Monte Carlo radiation transport code (MCNP5) have been described. In addition, the fuel-scanning machine and the gamma spectrometer are modelled by MCNP5 to simulate the gamma transport from fuel to detector. It also simulate the gamma spectrometer calibration for the burn up determination of the spend fuel. The results from MCNP5 simulation are applied to spectroscopic measurements and compared with the theoretical predictions of the neutronics code ORIGEN2 in this research work.

  10. Corrigendum to "Coupled thermochemical, isotopic evolution and heat transfer simulations in highly irradiated UO2 nuclear fuel"

    Science.gov (United States)

    Piro, M. H. A.; Banfield, J.; Clarno, K.; Simunovic, S.; Besmann, T. M.; Lewis, B. J.; Thompson, W. T.

    2016-09-01

    Figs. 7-9 in "Coupled thermochemical, isotopic evolution and heat transfer simulations in highly irradiated UO2 nuclear fuel" [1] have a consistent error corresponding to the relative proportions of iodine. Reported concentrations of iodine in the original manuscript are approximately ten times higher than expected, and are comparable in atomic proportions to cesium. One would expect that the amount of cesium would be about one order of magnitude greater than iodine based on the difference in fission yields of 235U and 239Pu. A practical consequence of this error would affect the predicted quantity and chemical composition of iodine on the fuel surface, which is related to iodine-induced stress corrosion cracking [2].

  11. Corrosion of graphite composites in phosphoric acid fuel cells

    Science.gov (United States)

    Christner, L. G.; Dhar, H. P.; Farooque, M.; Kush, A. K.

    1986-01-01

    Polymers, polymer-graphite composites and different carbon materials are being considered for many of the fuel cell stack components. Exposure to concentrated phosphoric acid in the fuel cell environment and to high anodic potential results in corrosion. Relative corrosion rates of these materials, failure modes, plausible mechanisms of corrosion and methods for improvement of these materials are investigated.

  12. Plutonium isotopes in the atmosphere of Central Europe: Isotopic composition and time evolution vs. circulation factors.

    Science.gov (United States)

    Kierepko, Renata; Mietelski, Jerzy W; Ustrnul, Zbigniew; Anczkiewicz, Robert; Wershofen, Herbert; Holgye, Zoltan; Kapała, Jacek; Isajenko, Krzysztof

    2016-11-01

    This paper reports evidence of Pu isotopes in the lower part of the troposphere of Central Europe. The data were obtained based on atmospheric aerosol fraction samples collected from four places in three countries (participating in the informal European network known as the Ring of Five (Ro5)) forming a cell with a surface area of about 200,000km(2). We compared our original data sets from Krakow (Poland, 1990-2007) and Bialystok (Poland, 1991-2007) with the results from two other locations, Prague (Czech Republic; 1997-2004) and Braunschweig (Germany; 1990-2003) to find time evolution of the Pu isotopes. The levels of the activity concentration for (238)Pu and for ((239+240))Pu were estimated to be a few and some tens of nBqm(-3), respectively. However, we also noted some results were much higher (even about 70 times higher) than the average concentration of (238)Pu in the atmosphere. The achieved complex data sets were used to test a new approach to the problem of solving mixing isotopic traces from various sources (here up to three) in one sample. Results of our model, supported by mesoscale atmospheric circulation parameters, suggest that Pu from nuclear weapon accidents or tests and nuclear burnt-up fuel are present in the air.

  13. A method for determining the nitrogen isotopic composition of porphyrins.

    Science.gov (United States)

    Higgins, Meytal B; Robinson, Rebecca S; Casciotti, Karen L; McIlvin, Matthew R; Pearson, Ann

    2009-01-01

    We describe a new method for analysis of the nitrogen isotopic composition of sedimentary porphyrins. This method involves separation and purification of geoporphyrins from sediment samples using liquid chromatography and HPLC, oxidation of the nitrogen within porphyrin-enriched fractions using a two-step process, and isotopic analysis of the resulting nitrate using the denitrifier method. By analysis of these degradation products of chlorophylls, we are able to measure an isotopic signature that reflects the nitrogen utilized by primary producers. The high sensitivity of the denitrifier method allows measurement of small samples that contain low concentrations of porphyrins. Extraction of only 50 nmol of nitrogen (nmol N) allows the following five analyses to be made (each on approximately 10 nmol N): nitrogen concentration, an assessment of potential contamination by nonporphyrin N, and three replicate isotopic measurements. The measured values of delta15N have an average analytical precision of +/-0.5 per thousand (1sigma) and an average contribution from Rayleigh fractionation of 0.7 per thousand from incomplete oxidation of porphyrin N to nitrate. The overall method will enable high-resolution records of delta15N values to be obtained for geological and ecological applications.

  14. Fuel composition and secondary organic aerosol formation: gas-turbine exhaust and alternative aviation fuels.

    Science.gov (United States)

    Miracolo, Marissa A; Drozd, Greg T; Jathar, Shantanu H; Presto, Albert A; Lipsky, Eric M; Corporan, Edwin; Robinson, Allen L

    2012-08-07

    A series of smog chamber experiments were performed to investigate the effects of fuel composition on secondary particulate matter (PM) formation from dilute exhaust from a T63 gas-turbine engine. Tests were performed at idle and cruise loads with the engine fueled on conventional military jet fuel (JP-8), Fischer-Tropsch synthetic jet fuel (FT), and a 50/50 blend of the two fuels. Emissions were sampled into a portable smog chamber and exposed to sunlight or artificial UV light to initiate photo-oxidation. Similar to previous studies, neat FT fuel and a 50/50 FT/JP-8 blend reduced the primary particulate matter emissions compared to neat JP-8. After only one hour of photo-oxidation at typical atmospheric OH levels, the secondary PM production in dilute exhaust exceeded primary PM emissions, except when operating the engine at high load on FT fuel. Therefore, accounting for secondary PM production should be considered when assessing the contribution of gas-turbine engine emissions to ambient PM levels. FT fuel substantially reduced secondary PM formation in dilute exhaust compared to neat JP-8 at both idle and cruise loads. At idle load, the secondary PM formation was reduced by a factor of 20 with the use of neat FT fuel, and a factor of 2 with the use of the blend fuel. At cruise load, the use of FT fuel resulted in no measured formation of secondary PM. In every experiment, the secondary PM was dominated by organics with minor contributions from sulfate when the engine was operated on JP-8 fuel. At both loads, FT fuel produces less secondary organic aerosol than JP-8 because of differences in the composition of the fuels and the resultant emissions. This work indicates that fuel reformulation may be a viable strategy to reduce the contribution of emissions from combustion systems to secondary organic aerosol production and ultimately ambient PM levels.

  15. Analysis of Trace Hydrogen Isotopes in Fusion Fuel Cycle by High Precision Gas Chromatograph

    Institute of Scientific and Technical Information of China (English)

    YANG; Li-ling; YANG; Hong-guang; ZHAO; Wei-wei; HE; Chang-shui; LIU; Zhen-xing; ZHAN; Qin

    2013-01-01

    It is essential to analysis of hydrogen isotopes in the fuel cycle system of fusion reactors,gas chromatography(GC)was found to be an effectively analytical technique.Compared with conventional GC,the high-precision GC with a cryogenic column could achieve fairly good performance to reduce the retention time.

  16. Observation of the Isotopic Evolution of PWR Fuel Using an Antineutrino Detector

    CERN Document Server

    Bowden, N S; Dazeley, S; Svoboda, R; Misner, A; Palmer, T

    2008-01-01

    By operating an antineutrino detector of simple design during several fuel cycles, we have observed long term changes in antineutrino flux that result from the isotopic evolution of a commercial pressurized water reactor. Measurements made with simple antineutrino detectors of this kind offer an alternative means for verifying fissile inventories at reactors, as part of IAEA and other reactor safeguards regimes.

  17. Measuring the Effect of Fuel Chemical Structure on Particulate and Gaseous Emissions using Isotope Tracing

    Energy Technology Data Exchange (ETDEWEB)

    Buchholz, B A; Mueller, C J; Martin, G C; Upatnicks, A; Dibble, R W; Cheng, S

    2003-09-11

    Using accelerator mass spectrometry (AMS), a technique initially developed for radiocarbon dating and recently applied to internal combustion engines, carbon atoms within specific fuel molecules can be labeled and followed in particulate or gaseous emissions. In addition to examining the effect of fuel chemical structure on emissions, the specific source of carbon for PM can be identified if an isotope label exists in the appropriate fuel source. Existing work has focused on diesel engines, but the samples (soot collected on quartz filters or combustion gases captured in bombs or bags) are readily collected from large industrial combustors as well.

  18. A Stochastic Method for Estimating the Effect of Isotopic Uncertainties in Spent Nuclear Fuel

    Energy Technology Data Exchange (ETDEWEB)

    DeHart, M.D.

    2001-08-24

    This report describes a novel approach developed at the Oak Ridge National Laboratory (ORNL) for the estimation of the uncertainty in the prediction of the neutron multiplication factor for spent nuclear fuel. This technique focuses on burnup credit, where credit is taken in criticality safety analysis for the reduced reactivity of fuel irradiated in and discharged from a reactor. Validation methods for burnup credit have attempted to separate the uncertainty associated with isotopic prediction methods from that of criticality eigenvalue calculations. Biases and uncertainties obtained in each step are combined additively. This approach, while conservative, can be excessive because of a physical assumptions employed. This report describes a statistical approach based on Monte Carlo sampling to directly estimate the total uncertainty in eigenvalue calculations resulting from uncertainties in isotopic predictions. The results can also be used to demonstrate the relative conservatism and statistical confidence associated with the method of additively combining uncertainties. This report does not make definitive conclusions on the magnitude of biases and uncertainties associated with isotopic predictions in a burnup credit analysis. These terms will vary depending on system design and the set of isotopic measurements used as a basis for estimating isotopic variances. Instead, the report describes a method that can be applied with a given design and set of isotopic data for estimating design-specific biases and uncertainties.

  19. Tellurium isotope compositions of calcium-aluminum-rich inclusions

    Science.gov (United States)

    Fehr, M. A.; Rehkämper, M.; Halliday, A. N.; Hattendorf, B.; Günther, D.

    2009-08-01

    A method for the precise and accurate determination of the tellurium (Te) isotope compositions of calcium-aluminum-rich inclusions (CAIs) has been developed. The technique utilizes multiple-collector inductively coupled plasma-mass spectrometry (MC-ICPMS) with either Faraday detectors or a dual ion-counting system. The external reproducibility (2σ) for 126Te/125Te was ~15‰ and ~2‰ when 3 pg and 65 pg of Te were analyzed with the electron multipliers. Measurements performed on 200 pg of Te using Faraday detectors and time-resolved software displayed an external reproducibility of ~8‰ for 126Te/124Te, whereas 3 ng Te could be measured to a precision of about 0.6‰. Analyses of five CAIs from the Allende chondrite yielded Te concentrations that range from 12 to 537 ppb and the inclusions are therefore depleted in Te relative to bulk Allende by factors of about 2 to 86. The Sn/Te ratios of the CAIs are also fractionated compared to bulk Allende (which displays 124Sn/128Te ≍ 0.1) with 124Sn/128Te ratios of about 0.1 to 2.5. The Te isotope measurements for these refractory inclusions yielded no 126Te excesses from the decay of the short-lived radionuclide 126Sn (τ½ = 234,500 years) and the most precise analysis provided a ɛ126Te value of 1 ± 6 (ɛ126Te = 126Te/ 124Te normalized to 122Te/124Te = 0.53594 and reported relative to the JMC Te standard). Minor differences in the Te isotope composition of the CAIs relative to the terrestrial standard and bulk Allende hint at the presence of small deficits in r-process Te isotopes or excess of s-process Te, but these nucleosynthetic anomalies are barely resolvable given the analytical uncertainties. Hence, it is also conceivable that these effects reflect small unresolved analytical artifacts.

  20. Oxygen isotope composition of mafic magmas at Vesuvius

    Science.gov (United States)

    Dallai, L.; Cioni, R.; Boschi, C.; D'Oriano, C.

    2009-12-01

    The oxygen isotope composition of olivine and clinopyroxene from four plinian (AD 79 Pompeii, 3960 BP Avellino), subplinian (AD 472 Pollena) and violent strombolian (Middle Age activity) eruptions were measured to constrain the nature and evolution of the primary magmas of the last 4000 years of Mt. Vesuvius activity. A large set of mm-sized crystals was accurately separated from selected juvenile material of the four eruptions. Crystals were analyzed for their major and trace element compositions (EPMA, Laser Ablation ICP-MS), and for 18O/16O ratios. As oxygen isotope composition of uncontaminated mantle rocks on world-wide scale is well constrained (δ18Oolivine = 5.2 ± 0.3; δ18Ocpx = 5.6 ± 0.3 ‰), the measured values can be conveniently used to monitor the effects of assimilation/contamination of crustal rocks in the evolution of the primary magmas. Instead, typically uncontaminated mantle values are hardly recovered in Italian Quaternary magmas, mostly due to the widespread occurrence of crustal contamination of the primary magmas during their ascent to the surface (e.g. Alban Hills, Ernici Mts., and Aeolian Islands). Low δ18O values have been measured in olivine from Pompeii eruption (δ18Oolivine = 5.54 ± 0.03‰), whereas higher O-compositions are recorded in mafic minerals from pumices or scoria of the other three eruptions. Measured olivine and clinopyroxene share quite homogeneous chemical compositions (Olivine Fo 85-90 ; Diopside En 45-48, respectively), and represent phases crystallized in near primary mafic magmas, as also constrained by their trace element compositions. Data on melt inclusions hosted in crystals of these compositions have been largely collected in the past demonstrating that they crystallized from mafic melt, basaltic to tephritic in composition. Published data on volatile content of these melt inclusions reveal the coexistence of dissolved water and carbon dioxide, and a minimum trapping pressure around 200-300 MPa, suggesting

  1. Upward revision of global fossil fuel methane emissions based on isotope database.

    Science.gov (United States)

    Schwietzke, Stefan; Sherwood, Owen A; Bruhwiler, Lori M P; Miller, John B; Etiope, Giuseppe; Dlugokencky, Edward J; Michel, Sylvia Englund; Arling, Victoria A; Vaughn, Bruce H; White, James W C; Tans, Pieter P

    2016-10-06

    Methane has the second-largest global radiative forcing impact of anthropogenic greenhouse gases after carbon dioxide, but our understanding of the global atmospheric methane budget is incomplete. The global fossil fuel industry (production and usage of natural gas, oil and coal) is thought to contribute 15 to 22 per cent of methane emissions to the total atmospheric methane budget. However, questions remain regarding methane emission trends as a result of fossil fuel industrial activity and the contribution to total methane emissions of sources from the fossil fuel industry and from natural geological seepage, which are often co-located. Here we re-evaluate the global methane budget and the contribution of the fossil fuel industry to methane emissions based on long-term global methane and methane carbon isotope records. We compile the largest isotopic methane source signature database so far, including fossil fuel, microbial and biomass-burning methane emission sources. We find that total fossil fuel methane emissions (fossil fuel industry plus natural geological seepage) are not increasing over time, but are 60 to 110 per cent greater than current estimates owing to large revisions in isotope source signatures. We show that this is consistent with the observed global latitudinal methane gradient. After accounting for natural geological methane seepage, we find that methane emissions from natural gas, oil and coal production and their usage are 20 to 60 per cent greater than inventories. Our findings imply a greater potential for the fossil fuel industry to mitigate anthropogenic climate forcing, but we also find that methane emissions from natural gas as a fraction of production have declined from approximately 8 per cent to approximately 2 per cent over the past three decades.

  2. Upward revision of global fossil fuel methane emissions based on isotope database

    Science.gov (United States)

    Schwietzke, Stefan; Sherwood, Owen A.; Bruhwiler, Lori M. P.; Miller, John B.; Etiope, Giuseppe; Dlugokencky, Edward J.; Michel, Sylvia Englund; Arling, Victoria A.; Vaughn, Bruce H.; White, James W. C.; Tans, Pieter P.

    2016-10-01

    Methane has the second-largest global radiative forcing impact of anthropogenic greenhouse gases after carbon dioxide, but our understanding of the global atmospheric methane budget is incomplete. The global fossil fuel industry (production and usage of natural gas, oil and coal) is thought to contribute 15 to 22 per cent of methane emissions to the total atmospheric methane budget. However, questions remain regarding methane emission trends as a result of fossil fuel industrial activity and the contribution to total methane emissions of sources from the fossil fuel industry and from natural geological seepage, which are often co-located. Here we re-evaluate the global methane budget and the contribution of the fossil fuel industry to methane emissions based on long-term global methane and methane carbon isotope records. We compile the largest isotopic methane source signature database so far, including fossil fuel, microbial and biomass-burning methane emission sources. We find that total fossil fuel methane emissions (fossil fuel industry plus natural geological seepage) are not increasing over time, but are 60 to 110 per cent greater than current estimates owing to large revisions in isotope source signatures. We show that this is consistent with the observed global latitudinal methane gradient. After accounting for natural geological methane seepage, we find that methane emissions from natural gas, oil and coal production and their usage are 20 to 60 per cent greater than inventories. Our findings imply a greater potential for the fossil fuel industry to mitigate anthropogenic climate forcing, but we also find that methane emissions from natural gas as a fraction of production have declined from approximately 8 per cent to approximately 2 per cent over the past three decades.

  3. Isotopic Composition of Cosmic Rays:. Results from the Cosmic Ray Isotope Spectrometer on the Ace Spacecraft

    Science.gov (United States)

    Israel, M. H.

    Over the past seven years the Cosmic Ray Isotope Spectrometer (CRIS) on the ACE spacecraft has returned data with an unprecedented combination of excellent mass resolution and high statistics, describing the isotopic composition of elements from lithium through nickel in the energy interval ~ 50 to 500 MeV/nucleon. These data have demonstrated: * The time between nucleosynthesis and acceleration of the cosmic-ray nuclei is at least 105 years. The supernova in which nucleosynthesis takes place is thus not the same supernova that accelerates a heavy nucleus to cosmic-ray energy. * The mean confinement time of cosmic rays in the Galaxy is 15 Myr. * The isotopic composition of the cosmic-ray source is remarkably similar to that of solar system. The deviations that are observed, particularly at 22Ne and 58Fe, are consistent with a model in which the cosmic-ray source is OB associations in which the interstellar medium has solar-system composition enriched by roughly 20% admixture of ejecta from Wolf-Rayet stars and supernovae. * Cosmic-ray secondaries that decay only by electron capture provide direct evidence for energy loss of cosmic rays as they penetrate the solar system. This invited overview paper at ECRS 19 was largely the same as an invited paper presented a month earlier at the 8th Nuclei in the Cosmos Conference in Vancouver. The proceedings of that conference will be published shortly by Elsevier as a special edition of Nuclear Physics A. For further summary of results from CRIS, the reader is referred to URL and links on that page to CRIS and to Science News.

  4. Isotopic composition and origin of the precipitation in Northern Chile

    Energy Technology Data Exchange (ETDEWEB)

    Aravena, R. [Department of Earth Sciences, University of Waterloo, Waterloo (Canada); Suzuki, O. [Exploracion y Desarrollo de Recursos Hidricos, Santiago (Chile); Pena, H. [Direccion General de Aguas, Ministerio de Obras Publicas, Santiago (Chile); Pollastri, A. [Comision Chilena de Energia Nuclear, Santiago (Chile); Fuenzalida, H. [Departamento de Geofisica, Universidad of Chile, Santiago (Chile); Grilli, A. [Empresa Metropolitana de Obras Sanitarias, Santiago (Chile)

    1999-06-01

    A 3 a data set of isotopes in precipitation from northern Chile show a very distinct pattern, with {delta}{sup 18}O values ranging between -18 and -15per thousand at high altitude stations, compared to {delta}{sup 18}O values between -10 and -6per thousand at the lower altitude areas. The {sup 18}O-depleted values observed in the high altitude area, the Altiplano, are related to processes that affect the air masses that originated over the Atlantic, cross the Amazon Basin (continental effect), ascend the Andes (altitude effect) and precipitated (convective effect) in the Altiplano. It is postulated that a second source of moisture, associated with air masses from the Pacific, may contribute to the {sup 18}O-enriched values observed in the lower altitude areas. Similar isotopic patterns are documented in springs and groundwater indicating that the data presented in this paper are an accurate representation of the long term behavior isotopic composition of rain in northern Chile. (Copyright (c) 1999 Elsevier Science B.V., Amsterdam. All rights reserved.)

  5. On the isotopic composition of magmatic carbon in SNC meteorites

    Science.gov (United States)

    Wright, I. P.; Grady, M. M.; Pillinger, C. T.

    1992-01-01

    SNC meteorites are thought, from many lines of evidence, to come from Mars. A line of investigation which has been pursued in our laboratory over the years involves measurement of the stable isotopic composition of carbon, in its various forms, in SNC meteorites. In order to establish a firm basis for studying the isotopic systematics of carbon in the martian surface environment, it is first necessary to try and constrain the delta C-13 of bulk Mars. Taking all of the available information, it would seem that the delta C-13 of the Earth's mantle lies somewhere in the range of -5 to -7 percent. Preliminary assessment of magnetic carbon in SNC meteorites, would tend to suggest a delta C-13 of 20 to 30 percent, which is conspicuously different from that of the terrestrial mantle. It is not obvious why there should be such a difference between the two planets, although many explanations are possible. One of these possibilities, that previous delta C-13 measurements for magnetic carbon in SNC meteorites are in error to some degree, is being actively investigated. The most recent results seem to constrain the theta C-13 of the magnetic carbon in SNC meteorites to about -20 percent, which is not at odds with previous estimates. As such, it is considered that a detailed investigation of the carbon isotopic systematics of martian surface materials does have the necessary information with which to proceed.

  6. Stable carbon isotopic composition of gasolines determined by isotope ratio monitoring gas chromatography mass spectrometry

    Energy Technology Data Exchange (ETDEWEB)

    Smallwood, B.J.; Philp, R.P.; Allen, J.D. [University of Oklahoma, Norman, OK (United States). School of Geology and Geophysics

    2002-07-01

    A large number of underground gasoline storage facilities in the United States continuously leak gasoline into the subsurface, which makes gasoline a major groundwater contaminant. Gas chromatography (GC) and gas chromatography-mass spectrometry (GC-MS) are used currently to characterize contaminated groundwater and soils. Correlations of contaminants with suspected source(s) are extremely difficult by these techniques because many gasolines have similar hydrocarbon distributions. The present study applied the technique of isotope ratio monitoring gas chromatography-mass spectrometry (irmGC-MS) to 19 gasoline samples from different areas of the USA. This allows a much better correlation of gasoline contaminants to source. Data obtained indicate a wide range of {sup {delta}}{sup 13}C values for 16 ubiquitous compounds in the gasolines. The majority of samples could be distinguished from each other on the basis of {sup {delta}}{sup 13}C hydrocarbon composition. The oxygenated additive methyl tertiary butyl ether (MTBE) was present in ten of the gasolines analyzed, and had a relatively narrow range of {sup {delta}}{sup 13}C values (-30.4 to -28.3 per mille). Preliminary investigations were also made to determine the extent of carbon isotopic fractionation after simple water washing and evaporation experiments. Results indicate that the majority of compounds did not undergo significant carbon isotopic fractionation as a result of these processes. (author)

  7. Recent insights into intramolecular 13C isotope composition of biomolecules

    Science.gov (United States)

    Gilbert, A.; Yamada, K.; Julien, M.; Yoshida, N.; Remaud, G.; Robins, R.

    2016-12-01

    In 1961 Abelson & Hoering shown that the intramolecular 13C distribution in amino acids was not homogeneous, namely the carboxylic acid positions were 13C-enriched compared with the mean of the remaining C-atoms in the molecule [1]. Nearly 20 years later, Monson & Hayes were able to demonstrate that even and odd positions in acetogenic fatty acids also showed non-statistical 13C isotope distributions, and that the pattern varied depending on the organism [2]. It took a further decade for the intramolecular 13C distribution in the key metabolite, glucose, to be defined [3]. Although informative, much of this work was incomplete, a number of positions having to be deduced by difference. This limitation arose mainly due to the lack of techniques enabling the separation and quantification of 13C isotopomers of the target molecule. In the past decade, quantitative 13C NMR has been developed for the determination of the intramolecular isotope composition of a given molecule with a precision of 1‰ or better [4]. This breakthrough has made possible a comprehensive view of the determinants governing intramolecular isotope composition of biological molecules. In particular, it can be shown that intramolecular pattern in sugars is influenced by the C-assimilation pathway and by post-photosynthetic fractionation associated with carbohydrate metabolism [5]. In addition, analysis by NMR of the alkyl chain of acetogenic lipids (fatty acids, n-alkanes) shows an alternation between odd and even C-atom positions, as observed by Monson& Hayes [2], throughout the molecule [6]. Overall, it is becoming apparent that this pattern is influenced by two principal metabolic factors: (i) the 13C pattern extant in the starting compounds; (ii) isotope fractionation associated with the enzymes involved in the biosynthetic pathway. On the whole, the determination of intramolecular isotope patterns in biomolecules allows better insights into the conditions and pathways by which they are formed

  8. Isotope composition of bicarbonate carbon in bed waters of oil and gas deposits

    Energy Technology Data Exchange (ETDEWEB)

    Golyshev, S.I.; Cherepnin, A.V.; Ivanov, V.G.; Manylova, L.S.

    1981-01-01

    A study is made of the isotope composition of bicarbonate carbon in bed waters of the Jurassic water complex in southeast West Siberia. It has been established that waters of empty and transcontour structures have isotope composition of carbon 5/sup 0//oo, while in waters which contact the hydrocarbon formations, the isotope composition of carbon is lighter on the average by 5-8/sup 0//oo. The isotope composition of bicarbonate carbon in bed waters reflects both the conditions for primary sedimentation, and secondary processes associated with organic matter transformation.

  9. A thirty year record of the isotopic composition of atmospheric methane from North America

    Science.gov (United States)

    Rice, A. L.; Teama, D. G.; Roeger, F. H.; Butenhoff, C. L.; Khalil, A. K.

    2012-12-01

    Methane (CH4) is one of the most important greenhouse gases after water vapor and carbon dioxide. Its atmospheric concentration increased from 650 ppb during the preindustrial era to nearly 1800 ppb in the present day due to human activities such as rice cultivation, animal husbandry, biomass burning, and fossil fuel production and use. Since the 1980s, the long-term growth rate of atmospheric CH4 slowed dramatically consistent with a leveling off of CH4 sources with significant interannual variability over this period. One powerful tool to constrain changes in sources and sinks is the use of stable isotopes of atmospheric CH4 because of the distinct values of carbon isotope (δ13C) and hydrogen isotope (δD) ratios in CH4 sources and characteristic isotopic fractionation effects in sinks. Measurements of the long-term trend of the isotopic composition of CH4 can improve the constraint of changes to the CH4 budget from microbial sources (e.g., wetlands, ruminants, and rice agriculture, δ13C ~-60 ‰, δD ~-300‰), fossil sources (e.g. natural gas and coal mining, δ13C ~-40‰, δD ~-200‰), and biomass burning (δ13C ~-25‰, δD ~-100‰). In this work, we present measurements of δ13C and δD of atmospheric CH4 from a unique archive of more than 200 air samples collected at Cape Meares, Oregon (45.5°N, 124°W) from 1978 to 1998. The measurements from this archive indicate enrichments in both isotope tracers over this period which average 0.017 (±0.002) ‰yr-1 for δ13C and 0.68 (±0.04) ‰yr-1 for δD. Seasonal cycles in δ13C and δD are also evident with amplitudes of ~ 0.3 ‰ and ~ 4 ‰, respectively; maximum values are found May-July and minimum values September-December, consistent with previous results from the mid-latitude northern hemisphere. Combining our results with more recent timeseries since 1988 from Olympic Peninsula (WA, 48°N), Montana de Oro (CA, 35°N), and Niwot Ridge (CO, 40°N) provides a composite record of the isotopic

  10. Coupled thermochemical, isotopic evolution and heat transfer simulations in highly irradiated UO2 nuclear fuel

    Science.gov (United States)

    Piro, M. H. A.; Banfield, J.; Clarno, K. T.; Simunovic, S.; Besmann, T. M.; Lewis, B. J.; Thompson, W. T.

    2013-10-01

    Predictive capabilities for simulating irradiated nuclear fuel behavior are enhanced in the current work by coupling thermochemistry, isotopic evolution and heat transfer. Thermodynamic models that are incorporated into this framework not only predict the departure from stoichiometry of UO2, but also consider dissolved fission and activation products in the fluorite oxide phase, noble metal inclusions, secondary oxides including uranates, zirconates, molybdates and the gas phase. Thermochemical computations utilize the spatial and temporal evolution of the fission and activation product inventory in the pellet, which is typically neglected in nuclear fuel performance simulations. Isotopic computations encompass the depletion, decay and transmutation of more than 2000 isotopes that are calculated at every point in space and time. These computations take into consideration neutron flux depression and the increased production of fissile plutonium near the fuel pellet periphery (i.e., the so-called “rim effect”). Thermochemical and isotopic predictions are in very good agreement with reported experimental measurements of highly irradiated UO2 fuel with an average burnup of 102 GW d t(U)-1. Simulation results demonstrate that predictions are considerably enhanced when coupling thermochemical and isotopic computations in comparison to empirical correlations. Notice: This manuscript has been authored by UT-Battelle, LLC, under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes.

  11. Measuring the Effect of Fuel Structures and Blend Distribution on Diesel Emissions Using Isotope Tracing

    Energy Technology Data Exchange (ETDEWEB)

    Cheng, A S; Mueller, C J; Buchholz, B A; Dibble, R W

    2004-02-10

    Carbon atoms occupying specific positions within fuel molecules can be labeled and followed in emissions. Renewable bio-derived fuels possess a natural uniform carbon-14 ({sup 14}C) tracer several orders of magnitude above petroleum-derived fuels. These fuels can be used to specify sources of carbon in particulate matter (PM) or other emissions. Differences in emissions from variations in the distribution of a fuel component within a blend can also be measured. Using Accelerator Mass Spectrometry (AMS), we traced fuel components with biological {sup 14}C/C levels of 1 part in 10{sup 12} against a {sup 14}C-free petroleum background in PM and CO{sub 2}. Different carbon atoms in the ester structure of the diesel oxygenate dibutyl maleate displayed far different propensities to produce PM. Homogeneous cosolvent and heterogeneous emulsified ethanol-in-diesel blends produced significantly different PM despite having the same oxygen content in the fuel. Emulsified blends produced PM with significantly more volatile species. Although ethanol-derived carbon was less likely to produce PM than diesel fuel, it formed non-volatile structures when it resided in PM. The contribution of lubrication oil to PM was determined by measuring an isotopic difference between 100% bio-diesel and the PM it produced. Data produced by the experiments provides validation for combustion models.

  12. The chlorine isotopic composition of Martian meteorites 1: Chlorine isotope composition of Martian mantle and crustal reservoirs and their interactions

    Science.gov (United States)

    Williams, J. T.; Shearer, C. K.; Sharp, Z. D.; Burger, P. V.; McCubbin, F. M.; Santos, A. R.; Agee, C. B.; McKeegan, K. D.

    2016-11-01

    The Martian meteorites record a wide diversity of environments, processes, and ages. Much work has been done to decipher potential mantle sources for Martian magmas and their interactions with crustal and surface environments. Chlorine isotopes provide a unique opportunity to assess interactions between Martian mantle-derived magmas and the crust. We have measured the Cl-isotopic composition of 17 samples that span the range of known ages, Martian environments, and mantle reservoirs. The 37Cl of the Martian mantle, as represented by the olivine-phyric shergottites, NWA 2737 (chassignite), and Shergotty (basaltic shergottite), has a low value of approximately -3.8‰. This value is lower than that of all other planetary bodies measured thus far. The Martian crust, as represented by regolith breccia NWA 7034, is variably enriched in the heavy isotope of Cl. This enrichment is reflective of preferential loss of 35Cl to space. Most basaltic shergottites (less Shergotty), nakhlites, Chassigny, and Allan Hills 84001 lie on a continuum between the Martian mantle and crust. This intermediate range is explained by mechanical mixing through impact, fluid interaction, and assimilation-fractional crystallization.

  13. Continuous measurements of isotopic composition of water vapour on the East Antarctic Plateau

    Science.gov (United States)

    Casado, Mathieu; Landais, Amaelle; Masson-Delmotte, Valérie; Genthon, Christophe; Kerstel, Erik; Kassi, Samir; Arnaud, Laurent; Picard, Ghislain; Prie, Frederic; Cattani, Olivier; Steen-Larsen, Hans-Christian; Vignon, Etienne; Cermak, Peter

    2016-07-01

    Water stable isotopes in central Antarctic ice cores are critical to quantify past temperature changes. Accurate temperature reconstructions require one to understand the processes controlling surface snow isotopic composition. Isotopic fractionation processes occurring in the atmosphere and controlling snowfall isotopic composition are well understood theoretically and implemented in atmospheric models. However, post-deposition processes are poorly documented and understood. To quantitatively interpret the isotopic composition of water archived in ice cores, it is thus essential to study the continuum between surface water vapour, precipitation, surface snow and buried snow. Here, we target the isotopic composition of water vapour at Concordia Station, where the oldest EPICA Dome C ice cores have been retrieved. While snowfall and surface snow sampling is routinely performed, accurate measurements of surface water vapour are challenging in such cold and dry conditions. New developments in infrared spectroscopy enable now the measurement of isotopic composition in water vapour traces. Two infrared spectrometers have been deployed at Concordia, allowing continuous, in situ measurements for 1 month in December 2014-January 2015. Comparison of the results from infrared spectroscopy with laboratory measurements of discrete samples trapped using cryogenic sampling validates the relevance of the method to measure isotopic composition in dry conditions. We observe very large diurnal cycles in isotopic composition well correlated with temperature diurnal cycles. Identification of different behaviours of isotopic composition in the water vapour associated with turbulent or stratified regime indicates a strong impact of meteorological processes in local vapour/snow interaction. Even if the vapour isotopic composition seems to be, at least part of the time, at equilibrium with the local snow, the slope of δD against δ18O prevents us from identifying a unique origin leading

  14. Perchlorate in The Great Lakes: Distribution, Isotopic Composition and Origin

    Science.gov (United States)

    Poghosyan, A.; Sturchio, N. C.; Jackson, W. A.; Guan, Y.; Eiler, J. M.; Hatzinger, P. B.

    2013-12-01

    Concentrations, stable chlorine and oxygen isotopic compositions, and 36Cl abundances of perchlorate were investigated in the five Laurentian Great Lakes. Samples were collected during monitoring cruises in 2007 and 2008 of the U.S. EPA's RV Lake Guardian and in 2010 at the water supply intake of Marquette, MI on the southern shore of Lake Superior. Concentrations of perchlorate were measured by IC/MS/MS at 24 locations, including one or two depth profiles in each lake. Mean concentrations (μg/L) are: Superior, 0.06 × 0.01; Michigan, 0.10 × 0.01; Huron, 0.11 × 0.01; Erie, 0.08 × 0.01, and Ontario, 0.09 × 0.01. Concentration vs. depth is nearly constant in each lake, indicating well-mixed conditions. Perchlorate was extracted from near-surface water by passing 15,000 to 80,000 L of water through 1-L cartridges containing Purolite A530E bifunctional anion-exchange resin. In the laboratory, perchlorate was eluted from the resin, purified, and precipitated as a >99% pure crystalline phase. Milligram amounts were recovered from each lake. Chlorine and oxygen isotopic analyses were performed at Caltech using the Cameca 7f-GEO SIMS instrument, following validation of the SIMS method with analyses of USGS-37 and USGS-38 isotopic reference materials. Results indicate a relatively narrow range in δ37Cl values (+2.9 to +3.9 ‰) and a wider range in δ18O values (-4.0 to +4.1 ‰), with a general geographic trend of increasing δ18O from west to east. Oxygen-17 was measured at UIC using dual-inlet IRMS of O2 produced by decomposition of KClO4. Great Lakes perchlorate has mass-independent oxygen isotopic variations with positive Δ17O values (+1.6 ‰ to +2.7 ‰) divided into two distinct groups: Lake Superior (+2.7 ‰) and the other four lakes (~ +1.7 ‰). The isotopic data indicate that perchlorate is dominantly of natural origin, having stable isotopic compositions resembling those of perchlorate from pre-industrial groundwaters in the western USA. The 36Cl

  15. Burn-up characteristics of ADS system utilizing the fuel composition from MOX PWRs spent fuel

    Energy Technology Data Exchange (ETDEWEB)

    Marsodi E-mail: marsodi@batan.go.id; Lasman, K.A.S.; Nishihara, K. E-mail: nishi@omega.tokai.jaeri.go.jp; Osugi, T.; Tsujimoto, K.; Marsongkohadi; Su' ud, Z. E-mail: szaki@fi.itb.ac.id

    2002-12-01

    Burn-up characteristics of accelerator-driven system, ADS has been evaluated utilizing the fuel composition from MOX PWRs spent fuel. The system consists of a high intensity proton beam accelerator, spallation target, and sub-critical reactor core. The liquid lead-bismuth, Pb-Bi, as spallation target, was put in the center of the core region. The general approach was conducted throughout the nitride fuel that allows the utilities to choose the strategy for destroying or minimizing the most dangerous high level wastes in a fast neutron spectrum. The fuel introduced surrounding the target region was the same with the composition of MOX from 33 GWd/t PWRs spent-fuel with 5 year cooling and has been compared with the fuel composition from 45 and 60 GWd/t PWRs spent-fuel with the same cooling time. The basic characteristics of the system such as burn-up reactivity swing, power density, neutron fluxes distribution, and nuclides densities were obtained from the results of the neutronics and burn-up analyses using ATRAS computer code of the Japan Atomic Energy research Institute, JAERI.

  16. FY13 Summary Report on the Augmentation of the Spent Fuel Composition Dataset for Nuclear Forensics: SFCOMPO/NF

    Energy Technology Data Exchange (ETDEWEB)

    Brady Raap, Michaele C.; Lyons, Jennifer A.; Collins, Brian A.; Livingston, James V.

    2014-03-31

    This report documents the FY13 efforts to enhance a dataset of spent nuclear fuel isotopic composition data for use in developing intrinsic signatures for nuclear forensics. A review and collection of data from the open literature was performed in FY10. In FY11, the Spent Fuel COMPOsition (SFCOMPO) excel-based dataset for nuclear forensics (NF), SFCOMPO/NF was established and measured data for graphite production reactors, Boiling Water Reactors (BWRs) and Pressurized Water Reactors (PWRs) were added to the dataset and expanded to include a consistent set of data simulated by calculations. A test was performed to determine whether the SFCOMPO/NF dataset will be useful for the analysis and identification of reactor types from isotopic ratios observed in interdicted samples.

  17. Spectroscopic metrology for isotope composition measurements and transfer standards

    Science.gov (United States)

    Anyangwe Nwaboh, Javis; Balslev-Harder, David; Kääriäinen, Teemu; Richmond, Craig; Manninen, Albert; Mohn, Joachim; Kiseleva, Maria; Petersen, Jan C.; Werhahn, Olav; Ebert, Volker

    2017-04-01

    The World Meteorological Organization (WMO) has identified greenhouse gases such as CO2, CH4 and N2O as critical for global climate monitoring. Other molecules such as CO that has an indirect effect of enhancing global warming are also monitored. WMO has stated compatibility goals for atmospheric concentration and isotope ratio measurements of these gases, e.g. 0.1 ppm for CO2 concentration measurements in the northern hemisphere and 0.01 ‰ for δ13C-CO2. For measurements of the concentration of greenhouse gases, gas analysers are typically calibrated with static gas standards e.g. traceable to the WMO scale or to the International System of Units (SI) through a national metrology institute. However, concentrations of target components, e.g. CO, in static gas standards have been observed to drift, and typically the gas matrix as well as the isotopic composition of the target component does not always reflect field gas composition, leading to deviations of the analyser response, even after calibration. The deviations are dependent on the measurement technique. To address this issue, part of the HIGHGAS (Metrology for high-impact greenhouse gases) project [1] focused on the development of optical transfer standards (OTSs) for greenhouse gases, e.g. CO2 and CO, potentially complementing gas standards. Isotope ratio mass spectrometry (IRMS) [2] is currently used to provide state-of-the-art high precision (in the 0.01 ‰ range) measurements for the isotopic composition of greenhouse gases. However, there is a need for field-deployable techniques such as optical isotope ratio spectroscopy (OIRS) that can be combined with metrological measurement methods. Within the HIGHGAS project, OIRS methods and procedures based on e.g. cavity enhanced spectroscopy (CES) and tunable diode laser absorption spectroscopy (TDLAS), matched to metrological principles have been established for the measurement of 13C/12C and 18O/16O ratios in CO2, 15N/14N ratios in N2O, and 13C/12C and 2H

  18. Evaluating Foraminifera as an Archive for Seawater Chromium Isotopic Composition

    Science.gov (United States)

    Wang, X.; Planavsky, N.; Hull, P. M.; Tripati, A.; Reinhard, C.; Zou, H.; Elder, L. E.; Henehan, M. J.

    2015-12-01

    In recent years there has been growing interest in using chromium isotopes (δ53Cr) as a proxy to investigate the redox evolution of Earth's ocean-atmosphere system throughout geological history. Potential archives for seawater δ53Cr that have been identified to date include iron formations and organic-rich siliciclastic sediments. However, these types of sediments are not common and they are discontinuous over geologic time. As a result, alternative types of archives are needed. Here we evaluate the utility of foraminifera tests as a recorder of seawater δ53Cr. Core-tops used were from different ocean basins. Mono-specific samples of Globigerinoides sacculifer, Orbulina universa, Pulleniatina obliquiloculata, Globoratalia crassula-crassaformis, Globoratalia truncatulinoides, and Globigerinella siphonifera were isolated to investigate inter-species isotope fractionation. Chromium concentrations were measured by isotope dilution method to be 0.1-0.3 μg/g. The δ53Cr values of these species range from 0.2‰ to 2.4‰, with an analytical uncertainty of 0.3‰ (95% confidence). Despite the high analytical uncertainty due to the extremely low levels of Cr present, there is still large detectable variation in foraminiferal δ53Cr values, which overlap presently available seawater values (Bonnand et al., 2013; Scheiderich et al., 2015). Possible explanations for such variations in foraminiferal δ53Cr values include heterogeneity of seawater δ53Cr in the modern oceans, and/or photobiochemical redox cycling of Cr in the surface oceans. Therefore, care should be taken when using foraminifera to reconstruct past seawater δ53Cr values. ReferencesBonnand, P., James, R., Parkinson, I., Connelly, D., Fairchild, I., 2013. The chromium isotopic composition of seawater and marine carbonates. Earth and Planetary Science Letters, 382: 10-20. Scheiderich, K., Amini, M., Holmden, C., Francois, R., 2015. Global variability of chromium isotopes in seawater demonstrated by Pacific

  19. Regional source identification of atmospheric aerosols in Beijing based on sulfur isotopic compositions

    Science.gov (United States)

    Lianfang, Wei; Pingqing, Fu; Xiaokun, Han; Qingjun, Guo; Yele, Sun; Zifa, Wang

    2016-04-01

    65 daily PM2.5 (aerosol particle with aerodynamic diameter less than 2.5 μm) samples were collected from an urban site in Beijing in four months representing the four seasons between September 2013 and July 2014. Inorganic ions, organic/elemental carbon and stable sulfur isotopes of sulfate aerosols were analyzed systematically. The "fingerprint" characteristics of the stable sulfur isotopic composition, together with trajectory clustering modeled by HYSPLIT-4 and potential source contribution function (PSCF), were employed for identifying potential regional sources. Results obviously exhibited the distinctive seasonality for various aerosol speciation associated with PM2.5 in Beijing with sulfate, nitrate, ammonium, organic matter, and element carbon being the dominant species. Elevated chloride associated with higher concentration of organics were found in autumn and winter, due to enhanced coal combustion emissions. The δ34S values of Beijing aerosol samples ranged from 2.94‰ to 10.2‰ with an average value of 6.18±1.87‰ indicating that the major sulfur source is direct fossil fuel burning-related emissions. Owning to a temperature-dependent fractionation and elevated biogenic sources of isotopically light sulfur in summer, the δ34S values had significant seasonal variations with a winter maximum ( 8.6‰)and a summer minimum ( 5.0‰). The results of trajectory clustering and the PSCF method demonstrated that higher concentrations of sulfate with lower sulfur isotope ratios ( 4.83‰) were associated with air masses from the south, southeast or east, whereas lower sulfate concentrations with higher δ34S values ( 6.69‰) when the air masses were mainly from north or northwest. These results suggested two main different kinds of regional coal combustion sources contributed to the pollution in Beijing.

  20. FBR core design with the composite fuel assembly

    Energy Technology Data Exchange (ETDEWEB)

    Cappiello, M.W.

    Although calculations are preliminary, overall feasibility of an FBR core design with the composite fuel assembly has been demonstrated. The advantaged over the heterogeneous design is that large variances in assembly mixed mean outlet temperatures are eliminated. Also, the effective enrichment of an assembly may easily be adjusted by varying the number of fertile pins per assembly, thus making it possible to flatten the core radial power profile. The use of the composite fuel assembly may in the future offer a significant alternative to heterogeneous FBR core design.

  1. Fuel options from microalgae with representative chemical compositions

    Energy Technology Data Exchange (ETDEWEB)

    Feinberg, D. A.

    1984-07-01

    Representative species of microalgae are examined with respect to their reported chemical compositions. Each species is analyzed under a variety of culture conditions, with the objective being to characterize an optimum mixture of fuel products (e.g., methane, ethanol, methylester) which should be produced by the particular species. Historically the emphasis has been on the entire algal cell mass. Using the reported chemical composition for the representative species under specific sets of growth conditions, some conclusions can be drawn about the preferred fuel product conversion routes that could be employed. 10 references, 7 figures, 12 tables.

  2. Isotopic composition of the ice cores obtained on the Western Plateau of the Mt Elbrus

    Directory of Open Access Journals (Sweden)

    A. V. Kozachek

    2015-01-01

    Full Text Available The results of the isotopic investigations of several ice cores obtained at the Western Plateau of Mt. Elbrus (the Caucasus are presented. There is a distinct seasonal cycle in the isotopic composition record in these cores. Mean annual and seasonal values of the isotopic composition and accumulation rate were reconstructed for 89 years (1924–2012. These values were compared with the available regional meteorological data and the atmospheric circulation characteristics. It was shown that in the summer season the isotopic composition reflects the local temperature while in winter it depends on the atmospheric circulation.

  3. Osmium Isotopic Composition of the Sumbar Cretaceous- Tertiary Boundary, Turkmenia

    Science.gov (United States)

    Meisel, T.; Krahenbuhl, U.; Nazarov, M. A.

    1992-07-01

    Turekian (1982) propagated the use of the osmium isotopic composition as a cosmic indicator for the origin of the high osmium (and iridium) layers at the K/T boundaries. He did not consider the osmium isotopic signature of the terrestrial mantle, which also has a chondritic evolution of the Re-Os system. Osmium cannot serve alone as an infallible indicator of the impact theory, but interesting results can be obtained from their investigation. Different K/T boundary section have been analyzed so far for ^187Os/^186Os. An overview of the values is presented in the table. Boundary Clay layer Os ratio Reference Stevns Klint fish clay 1.66 Luck and Turekian, 1983 Woodside Creek 1.12 Lichte et al., 1986 Raton Basin 1.23 Kraehenbuehl et al., 1988 Raton Basin (several) 1.15-1.23 Esser and Turekian, 1989 Sumbar (0-1 cm) 1.16 This work We obtained a complete marine section of the K/T boundary in southern Turkmenia (decribed by Alekseyev, 1988). It shows a very high Ir concentration (66 ppb) at the boundary layer and a remarkable Ir enrichment over crustal rocks continuing up to 30 cm above the boundary. Our aim of this investigation is to analyze several samples from above and below the boundary for the ^187Os/^186Os ratio to obtain a complete picture of the isotopic evolution of the section. We want to evaluate mixing of Os with chondritic ratios with Os from upper crustal rocks. Another goal is to investigate a mobilization of Os. So far only one sample has been analyzed with NTI-MS after fire assay digestion of the sample. The sample 0 to 1 cm has an ^187Os/^186Os ratio of 1.162 +- 13, which is quite low. We expect an even lower value for the boundary clay (0 cm) itself not taking into account a contribution of radiogenic osmium from the decay of terrestrial rhenium. This might put this K/T boundary section closest of all to the present day chondritic value (approx. 1.05). Further analysis will be presented at the meeting. References Alekseyev A. S., Nazarov M. A

  4. Triple sulfur isotope composition of Late Archean seawater sulfate

    Science.gov (United States)

    Paris, G.; Fischer, W. W.; Sessions, A. L.; Adkins, J. F.

    2013-12-01

    Multiple sulfur isotope ratios in Archean sedimentary rocks have provided powerful insights into the behavior of the ancient sulfur cycle, the redox state of fluid Earth, and the timing of the rise of atmospheric oxygen [1]. Most processes fractionate sulfur isotopes in proportion to their mass differences, but the Archean sulfur isotope record is marked by pronounced mass-independent fractionation (MIF, Δ33S≠0). The origin of these signatures has been traditionally interpreted as the result of photolysis of SO2 from short wavelength UV light, with positive Δ33S values recorded in pyrite and negative Δ33S values in sulfate-bearing phases [2]. This long-held hypothesis rests on observations of negative Δ33S from enigmatic barite occurrences from mixed volcanic sedimentary strata in Mesoarchean greenstone terrains. Despite forming the framework for understanding Archean sulfur cycle processes [3], it is largely untested [3]. It is largely untested. Consequently, the biggest challenge to our current understanding of the early sulfur cycle is a poor understanding of the isotopic composition of seawater sulfate. Sulfate evaporite minerals are absent from Archean strata and the sulfur isotope record is written entirely by measurements of pyrite. Carbonate associated sulfate (CAS) provides an important archive for assaying the isotopic composition of ancient seawater sulfate It has been exploited in many studies of Phanerozoic and Proterozoic sulfate but have been only marginally used thus far for Archean samples because of the extremely low concentration of CAS in limestones and dolomites from this era. We have developed a novel MC-ICP-MS approach to solve this problem [4]. This new method lowers the detection limit by up to three orders of magnitude for δ34S and Δ33S measurements, enabling to work on a few nmols of sulfate which represent only tens of mg of sample powders micromilled from specific carbonate textures. Two stratigraphic sections from the 2

  5. Australian atmospheric lead deposition reconstructed using lead concentrations and isotopic compositions of archival lichen and fungi.

    Science.gov (United States)

    Wu, Liqin; Taylor, Mark Patrick; Handley, Heather K; Wu, Michael

    2016-01-01

    Lead concentrations and their isotopic compositions were measured in lichen genera Cladonia and Usnea and fungi genus Trametes from the Greater Sydney region (New South Wales, Australia) that had been collected and archived over the past 120 years. The median lead contents were elevated in lichens and fungi prior to the introduction of leaded petrol (Cladonia 12.5 mg/kg; Usnea 15.6 mg/kg; Trametes 1.85 mg/kg) corresponding to early industrial development. During the use of leaded petrol for automobiles in Australia from 1932 to 2002, total median lead concentrations rose: Cladonia 18.8 mg/kg; Usnea 21.5 mg/kg; Trametes 4.3 mg/kg. Following the cessation of leaded petrol use, median total lead concentrations decreased sharply in the 2000s: Cladonia 4.8 mg/kg; Usnea 1.7 mg/kg. The lichen and fungi isotopic compositions reveal a significant decrease in (206)Pb/(207)Pb values from the end of 19th century to the 1970s. The following decades were characterised by lower allowable levels of lead additive in fuel and the introduction of unleaded petrol in 1985. The environmental response to these regulatory changes was that lichen and fungi (206)Pb/(207)Pb values increased, particularly from 1995 onwards. Although the lead isotope ratios of lichens continued to increase in the 2000s they do not return to pre-leaded petrol values. This demonstrates that historic leaded petrol emissions, inter alia other sources, remain a persistent source of anthropogenic contamination in the Greater Sydney region.

  6. Isotopic composition of sulfate accumulations, Northern Calcareous Alps, Austria

    Science.gov (United States)

    Bojar, Ana-Voica; Halas, Stanislaw; Bojar, Hans-Peter; Trembaczowski, Andrzej

    2015-04-01

    The Eastern Alps are characterised by the presence of three main tectonic units, such as the Lower, Middle and Upper Austroalpine, which overlie the Penninicum (Tollmann, 1977). The Upper Austroalpine unit consists of the Northern Calcareous Alps (NCA) overlying the Greywacke zone and corresponding to the Graz Paleozoic, Murau Paleozoic and the Gurktal Nappe. Evaporitic rocks are lacking in the later ones. The Northern Calcareous Alps are a detached fold and thrust belt. The sedimentation started in the Late Carboniferous or Early Permian, the age of the youngest sediments being Eocene. The NCA are divided into the Bajuvaric, Tirolic and Juvavic nappe complexes. The evaporitic Haselgebirge Formation occurs in connection with the Juvavic nappe complex at the base of the Tirolic units (Leitner et al., 2013). The Haselgebirge Formation consists mainly of salt, shales, gypsum and anhydrite and includes the oldest sediments of the NCA. The age of the Haselgebirge Formation, established by using spors and geochronological data, is Permian to Lower Triassic. For the Northern Calcareous Alps, the mineralogy of sulphate accumulations consists mainly of gypsum and anhydrite and subordonates of carbonates. The carbonates as magnesite, dolomite and calcite can be found either as singular crystals or as small accumulations within the hosting gypsum. Sulfides (sphalerite, galena, pyrite), sulfarsenides (enargite, baumhauerite) and native sulphur enrichments are known from several deposits (Kirchner, 1987; Postl, 1990). The investigated samples were selected from various gypsum and halite rich deposits of the Northern Calcareous Alps. A total of over 20 samples were investigated, and both oxygen and sulfur isotopic composition were determined for anhydrite, gyps, polyhalite, blödite and langbeinite. The sulfur isotopic values vary between 10.1 to 14 ‰ (CDT), with three values higher than 14 ‰. The Oxygen isotopic values show a range from 9 to 23 ‰ (SMOW). The sulfur

  7. Oxygen Isotopic Composition of Carbon Dioxide in the Middle Atmosphere

    Science.gov (United States)

    Liang, M.; Blake, G. A.; Lewis, B. R.; Yung, Y. L.

    2005-12-01

    The isotopic composition of long-lived trace gases provides a window into atmospheric transport and chemistry. Carbon dioxide is a particularly powerful tracer, because its abundance remains >100 ppmv in the mesosphere. Current models consider O3 as the main source of O(1D) in the mesosphere, but we note that the photolysis of 16O17O and 16O18O by solar Lyman-α radiation yields O(1D) 10-100 times more enriched in 17O and 18O than that from ozone photodissociation. We therefore incorporate both photochemical sources into stratospheric and mesospheric chemical transport models that quantitatively predict the unusual enhancement of 17O in CO2 from the middle atmosphere. New laboratory and atmospheric measurements are proposed to test our model and validate the use of CO2 isotopic fractionation as a tracer of atmospheric chemical and dynamical processes. Once fully understood the `anomalous' oxygen signature in CO2 can be used in turn to study biogeochemical cycles, in particular to constrain the gross carbon fluxes between the atmosphere and terrestrial biosphere.

  8. Volatile Concentrations and H-Isotope Composition of Unequilibrated Eucrites

    Science.gov (United States)

    Sarafian, Adam R.; Nielsen, Sune G.; Marschall, Horst R.; Gaetani, Glenn A.; Hauri, Erik H.; Righter, Kevin; Berger, Eve L.

    2017-01-01

    Eucrites are among the oldest and best studied asteroidal basalts (1). They represent magmatism that occurred on their parent asteroid, likely 4-Vesta, starting at 4563 Ma and continuing for approx. 30 Myr. Two hypotheses are debated for the genesis of eucrites, a magma ocean model (2), and a mantle partial melting model. In general, volatiles (H, C, F, Cl) have been ignored for eucrites and 4-Vesta, but solubility of wt% levels of H2O are possible at Vestan interior PT conditions. Targeted measurements on samples could aid our understanding considerably. Recent studies have found evidence of volatile elements in eucrites, but quantifying the abundance of volatiles remains problematic (6). Volatile elements have a disproportionately large effect on melt properties and phase stability, relative to their low abundance. The source of volatile elements can be elucidated by examining the hydrogen isotope ratio (D/H), as different H reservoirs have drastically different H isotope compositions. Recent studies of apatite in eucrites have shown that the D/H of 4-Vesta matches that of Earth and carbonaceous chondrites, however, the D/H of apatites may not represent the D/H of a primitive 4-Vesta melt due to the possibility of degassing prior to the crystallization of apatite. Therefore, the D/H of early crystallizing phases must be measured to determine if the D/H of 4-Vesta is equal to that of the Earth and carbonaceous chondrites.

  9. Silicon carbide composite for light water reactor fuel assembly applications

    Science.gov (United States)

    Yueh, Ken; Terrani, Kurt A.

    2014-05-01

    The feasibility of using SiCf-SiCm composites in light water reactor (LWR) fuel designs was evaluated. The evaluation was motivated by the desire to improve fuel performance under normal and accident conditions. The Fukushima accident once again highlighted the need for improved fuel materials that can maintain fuel integrity to higher temperatures for longer periods of time. The review identified many benefits as well as issues in using the material. Issues perceived as presenting the biggest challenges to the concept were identified to be flux gradient induced differential volumetric swelling, fragmentation and thermal shock resistance. The oxidation of silicon and its release into the coolant as silica has been identified as an issue because existing plant systems have limited ability for its removal. Detailed evaluation using available literature data and testing as part of this evaluation effort have eliminated most of the major concerns. The evaluation identified Boiling Water Reactor (BWR) channel, BWR fuel water tube, and Pressurized Water Reactor (PWR) guide tube as feasible applications for SiC composite. A program has been initiated to resolve some of the remaining issues and to generate physical property data to support the design of commercial fuel components.

  10. Silicon carbide composite for light water reactor fuel assembly applications

    Energy Technology Data Exchange (ETDEWEB)

    Yueh, Ken, E-mail: kyueh@epri.com [Fuel Reliability Program, EPRI, 1300 West WT Harris Blvd, Charlotte, NC 28262 (United States); Terrani, Kurt A., E-mail: terranika@ornl.gov [Fusion and Materials for Nuclear Systems Division, Oak Ridge National Laboratory, 1 Bethel Valley Rd. MS 6093, Oak Ridge, TN 37831 (United States)

    2014-05-01

    The feasibility of using SiC{sub f}–SiC{sub m} composites in light water reactor (LWR) fuel designs was evaluated. The evaluation was motivated by the desire to improve fuel performance under normal and accident conditions. The Fukushima accident once again highlighted the need for improved fuel materials that can maintain fuel integrity to higher temperatures for longer periods of time. The review identified many benefits as well as issues in using the material. Issues perceived as presenting the biggest challenges to the concept were identified to be flux gradient induced differential volumetric swelling, fragmentation and thermal shock resistance. The oxidation of silicon and its release into the coolant as silica has been identified as an issue because existing plant systems have limited ability for its removal. Detailed evaluation using available literature data and testing as part of this evaluation effort have eliminated most of the major concerns. The evaluation identified Boiling Water Reactor (BWR) channel, BWR fuel water tube, and Pressurized Water Reactor (PWR) guide tube as feasible applications for SiC composite. A program has been initiated to resolve some of the remaining issues and to generate physical property data to support the design of commercial fuel components.

  11. Isotopic composition and neutronics of the Okelobondo natural reactor

    Science.gov (United States)

    Palenik, Christopher Samuel

    The Oklo-Okelobondo and Bangombe uranium deposits, in Gabon, Africa host Earth's only known natural nuclear fission reactors. These 2 billion year old reactors represent a unique opportunity to study used nuclear fuel over geologic periods of time. The reactors in these deposits have been studied as a means by which to constrain the source term of fission product concentrations produced during reactor operation. The source term depends on the neutronic parameters, which include reactor operation duration, neutron flux and the neutron energy spectrum. Reactor operation has been modeled using a point-source computer simulation (Oak Ridge Isotope Generation and Depletion, ORIGEN, code) for a light water reactor. Model results have been constrained using secondary ionization mass spectroscopy (SIMS) isotopic measurements of the fission products Nd and Te, as well as U in uraninite from samples collected in the Okelobondo reactor zone. Based upon the constraints on the operating conditions, the pre-reactor concentrations of Nd (150 ppm +/- 75 ppm) and Te (<1 ppm) in uraninite were estimated. Related to the burnup measured in Okelobondo samples (0.7 to 13.8 GWd/MTU), the final fission product inventories of Nd (90 to 1200 ppm) and Te (10 to 110 ppm) were calculated. By the same means, the ranges of all other fission products and actinides produced during reactor operation were calculated as a function of burnup. These results provide a source term against which the present elemental and decay abundances at the fission reactor can be compared. Furthermore, they provide new insights into the extent to which a "fossil" nuclear reactor can be characterized on the basis of its isotopic signatures. In addition, results from the study of two other natural systems related to the radionuclide and fission product transport are included. A detailed mineralogical characterization of the uranyl mineralogy at the Bangombe uranium deposit in Gabon, Africa was completed to improve

  12. Nitrate isotopic composition and ancillary variables (land use, redox, excess N2, age, water isotopics) in California groundwater

    Science.gov (United States)

    Veale, Nathan; Moran, Jean; Visser, Ate; Singleton, Michael; Esser, Bradley

    2017-04-01

    Nitrate is a critical water quality issue in California, the United States and the world. Lawrence Livermore National Laboratory (LLNL) has compiled a large, unique database of California groundwater nitrate isotopic compositions (δ15N-NO3 and δ18O-NO3), acquired largely through more than a decade of coordination with the State of California Groundwater Ambient Monitoring and Assessment (GAMA) program. The water samples are predominantly from shallow aquifers accessed by domestic and monitoring wells. The database of >1,300 nitrate isotopic compositions includes a number of important ancillary parameters: DO, ORP and DOC (measured for 18% of samples); excess air and dissolved N2 (24%); water isotopic composition (δ18O-H2O and δD-H2O) (43%); and tritium/3He groundwater age (27%). Methods used at LLNL include sample preparation by the denitrifier method (for δ15N-NO3 and δ18O-NO3) and Isotope Ratio Mass Spectrometry with (δ15N-NO3 and δ18O-NO3 and δ18O-H2O and δD-H2O), Noble Gas Mass Spectrometry (NGMS; for excess air and groundwater age), and Membrane Inlet Mass Spectrometry (MIMS; for major dissolved gases and excess N2). Redox indicators (DO, ORP and DOC) in conjunction with excess N2, groundwater age, and nitrate isotopic composition are used to assess the presence or absence, and potentially the rate of, saturated-zone denitrification. Comparison of δ18O-NO3 to δ18O-H2O isotopic composition is used to distinguish synthetic nitrate from nitrification of reduced forms of nitrogen as a source of groundwater nitrate. Groundwater age is used to discern timing and temporal trends in groundwater nitrate isotopic composition. The relationship of nitrate isotopic composition to ancillary parameters (redox, excess N2, water isotopic composition and groundwater age) is explored, along with its relationship to well location, screened interval, and land use, with a focus on the extent of saturated-zone denitrification and the significance of synthetic nitrate as

  13. Stable isotope composition of atmospheric carbon monoxide. A modelling study

    Energy Technology Data Exchange (ETDEWEB)

    Gromov, Sergey S.

    2014-11-01

    This study aims at an improved understanding of the stable carbon and oxygen isotope composition of the carbon monoxide (CO) in the global atmosphere by means of numerical simulations. At first, a new kinetic chemistry tagging technique for the most complete parameterisation of isotope effects has been introduced into the Modular Earth Submodel System (MESSy) framework. Incorporated into the ECHAM/MESSy Atmospheric Chemistry (EMAC) general circulation model, an explicit treatment of the isotope effects on the global scale is now possible. The expanded model system has been applied to simulate the chemical system containing up to five isotopologues of all carbon- and oxygen-bearing species, which ultimately determine the δ{sup 13}C, δ{sup 18}O and Δ{sup 17}O isotopic signatures of atmospheric CO. As model input, a new stable isotope-inclusive emission inventory for the relevant trace gases has been compiled. The uncertainties of the emission estimates and of the resulting simulated mixing and isotope ratios have been analysed. The simulated CO mixing and stable isotope ratios have been compared to in-situ measurements from ground-based observatories and from the civil-aircraft-mounted CARIBIC-1 measurement platform. The systematically underestimated {sup 13}CO/{sup 12}CO ratios of earlier, simplified modelling studies can now be partly explained. The EMAC simulations do not support the inferences of those studies, which suggest for CO a reduced input of the highly depleted in {sup 13}C methane oxidation source. In particular, a high average yield of 0.94 CO per reacted methane (CH{sub 4}) molecule is simulated in the troposphere, to a large extent due to the competition between the deposition and convective transport processes affecting the CH{sub 4} to CO reaction chain intermediates. None of the other factors, assumed or disregarded in previous studies, however hypothesised to have the potential in enriching tropospheric CO in {sup 13}C, were found significant

  14. Nuclear magnetic resonance spectroscopic investigation of anode exhaust of direct methanol fuel cells without isotope enrichment

    Energy Technology Data Exchange (ETDEWEB)

    Byun, Young Seok; Hwang, Reo Yun; Han, Ochee [Western Seoul Center, Korea Basic Science Institute, Seoul (Korea, Republic of)

    2016-12-15

    Fuel cells are devices that electrochemically convert the chemical energy of fuels such as natural gas, gasoline, and methanol, into electricity. Fuel cells more efficiently use energy than internal combustion engines and do not produce undesirable pollutants, such as NO{sub x} ,SO{sub x} and particulates. Fuel cells can be distinguished from one another by their electrolytes. Among the various direct alcohol fuel cells, direct methanol fuel cells (DMFCs) have been developed most. However, DMFCs have several practical problems such as methanol crossove r from an anode to a cathode and slow methanol oxidation reaction rates. Therefore, understanding the electrochemical reaction mechanisms of DMFCs may provide clues to solve these problems, and various analytical methods have been employed to examine these mechanisms. We demonstrated that {sup 1}H and {sup 13}C NMR spectroscopy can be used for analyzing anode exhausts of DMFCs operated with methanol without any isotope enrichment. However, the low sensitivity of NMR spectroscopy hindered our efforts to detect minor reaction intermediates. Therefore, sensitivity enhancement techniques such as dynamic nuclear polarization (DNP) NMR methods and/or presaturation methods to increase the dynamic range of the proton spectra by pre-saturating large water signals, are expected to be useful to detect low-concentration species.

  15. Tooth enamel maturation reequilibrates oxygen isotope compositions and supports simple sampling methods

    Science.gov (United States)

    Trayler, Robin B.; Kohn, Matthew J.

    2017-02-01

    Oxygen isotope and major element zoning patterns of several disparate ungulate teeth were collected to evaluate the timing and geometry of enamel formation, records of isotope zoning, and tooth enamel sampling strategies. Isotopic zoning in mammalian tooth enamel encodes a sub-annual time series of isotopic variation of an animal's body water composition, with a damping factor that depends on the specifics of how enamel mineralizes. Enamel formation comprises two stages: precipitation of appositional enamel with a high CO3:PO4 ratio, followed by precipitation of maturational enamel with a lower CO3:PO4. If appositional and maturational enamel both contribute to isotope compositions (but with different CO3:PO4), and if isotope compositions vary seasonally, paired δ18O values from CO3 and PO4 profiles should show a spatial separation. CO3 isotope patterns should be shifted earlier seasonally than PO4 isotope patterns. Such paired profiles for new and published data show no resolvable shifts, i.e. CO3 and PO4 δ18O profiles show coincident maxima and minima. This coincidence suggests that enamel maturation reequilibrates appositional isotope compositions. If enamel maturation establishes enamel isotope compositions, the geometry of maturation, not apposition, should be considered when devising sampling protocols. X-ray maps of Ca zoning show that the majority of enamel (inner and middle layers) mineralizes heavily at a high angle to the external tooth surface and the enamel-dentine junction over length scales of 2-4 mm, while the outer enamel surface mineralizes more slowly. These data suggest that isotopic sampling strategies should parallel maturational geometry and focus on interior enamel to improve data fidelity. The magnitude of isotopic damping is also smaller than implied in previous studies, so tooth enamel zoning more closely reflects original body water isotopic variations than previously assumed.

  16. Isotopic and Elemental Composition of Roasted Coffee as a Guide to Authenticity and Origin.

    Science.gov (United States)

    Carter, James F; Yates, Hans S A; Tinggi, Ujang

    2015-06-24

    This study presents the stable isotopic and elemental compositions of single-origin, roasted coffees available to retail consumers. The δ(13)C, δ(15)N, and δ(18)O compositions were in agreement with those previously reported for green coffee beans. The δ(15)N composition was seen to be related to organic cultivation, reflected in both δ(2)H and δ(18)O compositions. The δ(13)C composition of extracted caffeine differed little from that of the bulk coffee. Stepwise discriminant analysis with jackknife tests, using isotopic and elemental data, provided up to 77% correct classification of regions of production. Samples from Africa and India were readily classified. The wide range in both isotopic and elemental compositions of samples from other regions, specifically Central/South America, resulted in poor discrimination between or within these regions. Simpler X-Y and geo-spatial plots of the isotopic data provided effective visual means to distinguish between coffees from different regions.

  17. Light element isotopic compositions of cometary matter returned by the STARDUST mission

    Energy Technology Data Exchange (ETDEWEB)

    McKeegan, K D; Aleon, J; Bradley, J; Brownlee, D; Busemann, H; Butterworth, A; Chaussidon, M; Fallon, S; Floss, C; Gilmour, J; Gounelle, M; Graham, G; Guan, Y; Heck, P R; Hoppe, P; Hutcheon, I D; Huth, J; Ishii, H; Ito, M; Jacobsen, S B; Kearsley, A; Leshin, L A; Liu, M; Lyon, I; Marhas, K; Marty, B; Matrajt, G; Meibom, A; Messenger, S; Mostefaoui, S; Nakamura-Messenger, K; Nittler, L; Palma, R; Pepin, R O; Papanastassiou, D A; Robert, F; Schlutter, D; Snead, C J; Stadermann, F J; Stroud, R; Tsou, P; Westphal, A; Young, E D; Ziegler, K; Zimmermann, L; Zinner, E

    2006-10-10

    Hydrogen, carbon, nitrogen, and oxygen isotopic compositions are heterogeneous among comet 81P/Wild2 particle fragments, however extreme isotopic anomalies are rare, indicating that the comet is not a pristine aggregate of presolar materials. Non-terrestrial nitrogen and neon isotope ratios suggest that indigenous organic matter and highly volatile materials were successfully collected. Except for a single circumstellar stardust grain, silicate and oxide minerals have oxygen isotopic compositions consistent with solar system origin. One refractory grain is {sup 16}O-enriched like refractory inclusions in meteorites, suggesting formation in the hot inner solar nebula and large-scale radial transport prior to comet accretion in the outer solar system.

  18. Composite materials for polymer electrolyte membrane microbial fuel cells.

    Science.gov (United States)

    Antolini, Ermete

    2015-07-15

    Recently, the feasibility of using composite metal-carbon, metal-polymer, polymer-carbon, polymer-polymer and carbon-carbon materials in microbial fuel cells (MFCs) has been investigated. These materials have been tested as MFC anode catalyst (microorganism) supports, cathode catalysts and membranes. These hybrid materials, possessing the properties of each component, or even with a synergistic effect, would present improved characteristics with respect to the bare components. In this paper we present an overview of the use of these composite materials in microbial fuel cells. The characteristics of the composite materials as well as their effect on MFC performance were compared with those of the individual component and/or the conventionally used materials.

  19. Modelling and interpreting the isotopic composition of water vapour in convective updrafts

    Directory of Open Access Journals (Sweden)

    M. Bolot

    2013-08-01

    Full Text Available The isotopic compositions of water vapour and its condensates have long been used as tracers of the global hydrological cycle, but may also be useful for understanding processes within individual convective clouds. We review here the representation of processes that alter water isotopic compositions during processing of air in convective updrafts and present a unified model for water vapour isotopic evolution within undiluted deep convective cores, with a special focus on the out-of-equilibrium conditions of mixed-phase zones where metastable liquid water and ice coexist. We use our model to show that a combination of water isotopologue measurements can constrain critical convective parameters, including degree of supersaturation, supercooled water content and glaciation temperature. Important isotopic processes in updrafts include kinetic effects that are a consequence of diffusive growth or decay of cloud particles within a supersaturated or subsaturated environment; isotopic re-equilibration between vapour and supercooled droplets, which buffers isotopic distillation; and differing mechanisms of glaciation (droplet freezing vs. the Wegener–Bergeron–Findeisen process. As all of these processes are related to updraft strength, particle size distribution and the retention of supercooled water, isotopic measurements can serve as a probe of in-cloud conditions of importance to convective processes. We study the sensitivity of the profile of water vapour isotopic composition to differing model assumptions and show how measurements of isotopic composition at cloud base and cloud top alone may be sufficient to retrieve key cloud parameters.

  20. Controls on the stable isotope compositions of travertine from hyperalkaline springs in Oman: Insights from clumped isotope measurements

    Science.gov (United States)

    Falk, E. S.; Guo, W.; Paukert, A. N.; Matter, J. M.; Mervine, E. M.; Kelemen, P. B.

    2016-11-01

    Carbonate formation at hyperalkaline springs is typical of serpentinization in peridotite massifs worldwide. These travertines have long been known to exhibit large variations in their carbon and oxygen isotope compositions, extending from apparent equilibrium values to highly depleted values. However, the exact causes of these variations are not well constrained. We analyzed a suite of well-characterized fresh carbonate precipitates and travertines associated with hyperalkaline springs in the peridotite section of the Samail ophiolite, Sultanate of Oman, and found their clumped isotope compositions vary systematically with formation environments. Based on these findings, we identified four main processes controlling the stable isotope compositions of these carbonates. These include hydroxylation of CO2, partial isotope equilibration of dissolved inorganic carbon, mixing between isotopically distinct carbonate end-members, and post-depositional recrystallization. Most notably, in fresh crystalline films on the surface of hyperalkaline springs and in some fresh carbonate precipitates from the bottom of hyperalkaline pools, we observed large enrichments in Δ47 (up to ∼0.2‰ above expected equilibrium values) which accompany depletions in δ18O and δ13C, yielding about 0.01‰ increase in Δ47 and 1.1‰ decrease in δ13C for every 1‰ decrease in δ18O, relative to expected equilibrium values. This disequilibrium trend, also reflected in preserved travertines ranging in age from modern to ∼40,000 years old, is interpreted to arise mainly from the isotope effects associated with the hydroxylation of CO2 in high-pH fluids and agrees with our first-order theoretical estimation. In addition, in some fresh carbonate precipitates from the bottom of hyperalkaline pools and in subsamples of one preserved travertine terrace, we observed additional enrichments in Δ47 at intermediate δ13C and δ18O, consistent with mixing between isotopically distinct carbonate end

  1. Solid oxide fuel cell having a glass composite seal

    Science.gov (United States)

    De Rose, Anthony J.; Mukerjee, Subhasish; Haltiner, Jr., Karl Jacob

    2013-04-16

    A solid oxide fuel cell stack having a plurality of cassettes and a glass composite seal disposed between the sealing surfaces of adjacent cassettes, thereby joining the cassettes and providing a hermetic seal therebetween. The glass composite seal includes an alkaline earth aluminosilicate (AEAS) glass disposed about a viscous glass such that the AEAS glass retains the viscous glass in a predetermined position between the first and second sealing surfaces. The AEAS glass provides geometric stability to the glass composite seal to maintain the proper distance between the adjacent cassettes while the viscous glass provides for a compliant and self-healing seal. The glass composite seal may include fibers, powders, and/or beads of zirconium oxide, aluminum oxide, yttria-stabilized zirconia (YSZ), or mixtures thereof, to enhance the desirable properties of the glass composite seal.

  2. Seasonality of Oxygen isotope composition in cow (Bos taurus) hair and its model interpretation

    Science.gov (United States)

    Chen, Guo; Schnyder, Hans; Auerswald, Karl

    2017-04-01

    Oxygen isotopes in animal and human tissues are expected to be good recorders of geographical origin and migration histories based on the isotopic relationship between hair oxygen and annual precipitation and the well-known spatial pattern of oxygen isotope composition in meteoric water. However, seasonal variation of oxygen isotope composition may diminish the origin information in the tissues. Here the seasonality of oxygen isotope composition in tail hair was investigated in a domestic suckler cow (Bos taurus) that underwent different ambient conditions, physiological states, and keeping and feeding strategies during five years. A detailed mechanistic model involving in ambient conditions, soil properties and animal physiology was built to explain this variation. The measured oxygen isotope composition in hair was significantly related (pwater in a regression analysis. Modelling suggested that this relation was only partly derived from the direct influence of feed moisture. Ambient conditions (temperature, moisture) did not only influence the isotopic signal of precipitation but also affected the animal itself (drinking water demand, transcutaneous vapor etc.). The clear temporal variation thus resulted from complex interactions with multiple influences. The twofold influence of ambient conditions via the feed and via the animal itself is advantageous for tracing the geographic origin because the oxygen isotope composition is then less influenced by variations in moisture uptake; however, it is unfavorable for indicating the production system, e.g. to distinguish between milk produced from fresh grass or from silage.

  3. Clumped Isotope Composition of Cold-Water Corals: A Role for Vital Effects?

    Science.gov (United States)

    Spooner, P.; Guo, W.; Robinson, L. F.

    2014-12-01

    Measurements on a set of cold-water corals (mainly Desmophyllum dianthus) have suggested that their clumped isotope composition could serve as a promising proxy for reconstructing paleocean temperatures. Such measurements have also offered support for certain isotope models of coral calcification. However, there are differences in the clumped isotope compositions between warm-water and cold-water corals, suggesting that different kinds of corals could have differences in their biocalcification processes. In order to understand the systematics of clumped isotope variations in cold-water corals more fully, we present clumped isotope data from a range of cold-water coral species from the tropical Atlantic and the Southern Ocean.Our samples were either collected live or recently dead (14C ages biocalcification may not apply equally well to all corals. Clumped isotope vital effects may be present in certain cold-water corals as they are in warm-water corals, complicating the use of this paleoclimate proxy.

  4. Micro-analytical uranium isotope and chemical investigations of zircon crystals from the Chernobyl “lava” and their nuclear fuel inclusions

    Energy Technology Data Exchange (ETDEWEB)

    Pöml, P., E-mail: Philipp.POEML@ec.europa.eu [European Commission, Joint Research Centre, Institute for Transuranium Elements, P.O. Box 2340, 76125 Karlsruhe (Germany); Burakov, B. [Laboratory of Applied Mineralogy and Radiogeochemistry, V.G. Khlopin Radium Institute, 28, 2-nd Murinskiy Ave., St. Petersburg 194021 (Russian Federation); Geisler, T. [Steinmann Institut für Geologie, Mineralogie und Paläontologie, University of Bonn, Poppelsdorfer Schloss, 53115 Bonn (Germany); Walker, C.T. [European Commission, Joint Research Centre, Institute for Transuranium Elements, P.O. Box 2340, 76125 Karlsruhe (Germany); Grange, M.L.; Nemchin, A.A. [Department of Applied Geology, Western Australian School of Mines, Curtin University, GPO Box U1987, Western Australia 6845 (Australia); Berndt, J. [Institut für Mineralogie, Westfälische Wilhelms-Universität, Corrensstraße 24, 48149 Münster (Germany); Fonseca, R.O.C. [Steinmann Institut für Geologie, Mineralogie und Paläontologie, University of Bonn, Poppelsdorfer Schloss, 53115 Bonn (Germany); Bottomley, P.D.W.; Hasnaoui, R. [European Commission, Joint Research Centre, Institute for Transuranium Elements, P.O. Box 2340, 76125 Karlsruhe (Germany)

    2013-08-15

    U isotope data measured on real fragments of the Chernobyl nuclear fuel included in zircon crystals crystallised from the Chernobyl “lava” are presented for the first time. The U isotope data show no anomalies and lie within the expected burnup values for the Chernobyl nuclear fuel. However, the U concentration, the U isotopic composition, and the Ti concentration in the host zircon vary significantly within single crystals as well as between single crystals. Our results indicate that during the time of melt activity temperature and melt composition likely varied considerably. New melt was formed progressively (and solidified) during the accident that reacted and mixed with pre-existing melt that never fully equilibrated. In such an environment zircon crystals crystallised at temperatures below 1250 °C, as estimated from thermodynamic considerations along with the observation that the centre of the investigated zircon crystal contains monoclinic ZrO{sub 2} inclusions. Since the zircon crystals crystallised before the silicate melt spread out into the reactor block basement, the flow of the melt into the basement must also have occurred at temperatures below 1250 °C.

  5. Irradiated Xenon Isotopic Ratio Measurement for Failed Fuel Detection and Location in Fast Reactor

    Science.gov (United States)

    Ito, Chikara; Iguchi, Tetsuo; Harano, Hideki

    2009-08-01

    The accuracy of xenon isotopic ratio burn-up calculations used for failed fuel identification was evaluated by an irradiation test of xenon tag gas samples in the Joyo test reactor. The experiment was carried out using pressurized steel capsules containing unique blend ratios of stable xenon tag gases in an on-line creep rupture experiment in Joyo. The tag gas samples were irradiated to total neutron fluences of 1.6 to 4.8 × 1026 n/m2. Laser resonance ionization mass spectrometry was used to analyze the cover gas containing released tag gas diluted to isotopic ratios of 100 to 102 ppb. The isotopic ratios of xenon tag gases after irradiation were calculated using the ORIGEN2 code. The neutron cross sections of xenon nuclides were based on the JENDL-3.3 library. These cross sections were collapsed into one group using the neutron spectra of Joyo. The comparison of measured and calculated xenon isotopic ratios provided C/E values that ranged from 0.92 to 1.10. The differences between calculation and measurement were considered to be mainly due to the measurement errors and the xenon nuclide cross section uncertainties.

  6. Hybrid Composites for LH2 Fuel Tank Structure

    Science.gov (United States)

    Grimsley, Brian W.; Cano, Roberto J.; Johnston, Norman J.; Loos, Alfred C.; McMahon, William M.

    2001-01-01

    The application of lightweight carbon fiber reinforced plastics (CFRP) as structure for cryogenic fuel tanks is critical to the success of the next generation of Reusable Launch Vehicles (RLV). The recent failure of the X-33 composite fuel tank occurred in part due to microcracking of the polymer matrix, which allowed cryogen to permeate through the inner skin to the honeycomb core. As part of an approach to solve these problems, NASA Langley Research Center (LaRC) and Marshall Space Flight Center (MSFC) are working to develop and investigate polymer films that will act as a barrier to the permeation of LH2 through the composite laminate. In this study two commercially available films and eleven novel LaRC films were tested in an existing cryogenics laboratory at MSFC to determine the permeance of argon at room temperature. Several of these films were introduced as a layer in the composite to form an interleaved, or hybrid, composite to determine the effects on permeability. In addition, the effects of the interleaved layer thickness, number, and location on the mechanical properties of the composite laminate were investigated. In this initial screening process, several of the films were found to exhibit lower permeability to argon than the composite panels tested.

  7. Dual-Carbon sources fuel the OCS deep-reef Community, a stable isotope investigation

    Science.gov (United States)

    Sulak, Kenneth J.; Berg, J.; Randall, Michael; Dennis, George D.; Brooks, R.A.

    2008-01-01

    The hypothesis that phytoplankton is the sole carbon source for the OCS deep-reef community (>60 m) was tested. Trophic structure for NE Gulf of Mexico deep reefs was analyzed via carbon and nitrogen stable isotopes. Carbon signatures for 114 entities (carbon sources, sediment, fishes, and invertebrates) supported surface phytoplankton as the primary fuel for the deep reef. However, a second carbon source, the macroalga Sargassum, with its epiphytic macroalgal associate, Cladophora liniformis, was also identified. Macroalgal carbon signatures were detected among 23 consumer entities. Most notably, macroalgae contributed 45 % of total carbon to the 13C isotopic spectrum of the particulate-feeding reef-crest gorgonian Nicella. The discontinuous spatial distribution of some sessile deep-reef invertebrates utilizing pelagic macroalgal carbon may be trophically tied to the contagious distribution of Sargassum biomass along major ocean surface features.

  8. Hydrogen and oxygen in brine shrimp chitin reflect environmental water and dietary isotopic composition

    Science.gov (United States)

    Nielson, Kristine E.; Bowen, Gabriel J.

    2010-03-01

    Hydrogen and oxygen isotope ratios of the common structural biopolymer chitin are a potential recorder of ecological and environmental information, but our understanding of the mechanisms of incorporation of H and O from environmental substrates into chitin is limited. We report the results of a set of experiments in which the isotopic compositions of environmental water and diet were varied independently in order to assess the contribution of these variables to the H and O isotopic composition of Artemia franciscana chitin. Hydrogen isotope ratios of chitin were strongly linearly correlated with both food and water, with approximately 26% of the hydrogen signal reflecting food and approximately 38% reflecting water. Oxygen isotopes were also strongly correlated with the isotopic composition of water and food, but whereas 69% of oxygen in chitin exchanged with environmental water, only 10% was derived from food. We propose that these observations reflect the position-specific, partial exchange of H and O atoms with brine shrimp body water during the processes of digestion and chitin biosynthesis. Comparison of culture experiments with a set of natural samples collected from the Great Salt Lake, UT in 2006 shows that, with some exceptions, oxygen isotope compositions of chitin track those of water, whereas hydrogen isotopes vary inversely with those of lake water. The different behavior of the two isotopic systems can be explained in terms of a dietary shift from allochthonous particulate matter with relatively higher δ 2H values in the early spring to autochthonous particulate matter with significantly lower δ 2H values in the late summer to autumn. These results suggest oxygen in chitin may be a valuable proxy for the oxygen isotopic composition of environmental water, whereas hydrogen isotope values from the same molecule may reveal ecological and biogeochemical changes within lakes.

  9. The iron isotope composition of enstatite meteorites: Implications for their origin and the metal/sulfide Fe isotopic fractionation factor

    Science.gov (United States)

    Wang, Kun; Savage, Paul S.; Moynier, Frédéric

    2014-10-01

    Despite their unusual chemical composition, it is often proposed that the enstatite chondrites represent a significant component of Earth’s building materials, based on their terrestrial similarity for numerous isotope systems. In order to investigate a possible genetic relationship between the Fe isotope composition of enstatite chondrites and the Earth, we have analyzed 22 samples from different subgroups of the enstatite meteorites, including EH and EL chondrites, aubrites (main group and Shallowater) and the Happy Canyon impact melt. We have also analyzed the Fe isotopic compositions of separated (magnetic and non-magnetic) phases from both enstatite chondrites and achondrites. On average, EH3-5 chondrites (δ56Fe = 0.003 ± 0.042‰; 2 standard deviation; n = 9; including previous literature data) as well as EL3 chondrites (δ56Fe = 0.030 ± 0.038‰; 2 SD; n = 2) have identical and homogeneous Fe isotopic compositions, indistinguishable from those of the carbonaceous chondrites and average terrestrial peridotite. In contrast, EL6 chondrites display a larger range of isotopic compositions (-0.180‰ < δ56Fe < 0.181‰; n = 11), a result of mixing between isotopically distinct mineral phases (metal, sulfide and silicate). The large Fe isotopic heterogeneity of EL6 is best explained by chemical/mineralogical fragmentation and brecciation during the complex impact history of the EL parent body. Enstatite achondrites (aubrites) also exhibit a relatively large range of Fe isotope compositions: all main group aubrites are enriched in the light Fe isotopes (δ56Fe = -0.170 ± 0.189‰; 2 SD; n = 6), while Shallowater is, isotopically, relatively heavy (δ56Fe = 0.045 ± 0.101‰; 2 SD; n = 4; number of chips). We take this variation to suggest that the main group aubrite parent body formed a discreet heavy Fe isotope-enriched core, whilst the Shallowater meteorite is most likely from a different parent body where core and silicate material remixed. This could be

  10. A continuous flow isotope ratio mass spectrometry method for high precision determination of dissolved gas ratios and isotopic composition

    DEFF Research Database (Denmark)

    Charoenpong, C. N.; Bristow, L. A.; Altabet, M. A.

    2014-01-01

    Dissolved gas ratios and isotopic compositions provide essential information about the biological and physical mechanisms influencing N-2, O-2, and Ar in aquatic systems. Current methods available are either limited by overall cost, labor-intensive sample collection and analysis, or insufficient ...

  11. Direct borohydride fuel cell using Ni-based composite anodes

    Energy Technology Data Exchange (ETDEWEB)

    Ma, Jia; Sahai, Yogeshwar; Buchheit, Rudolph G. [Department of Materials Science and Engineering, The Ohio State University, 2041 College Rd., Columbus, OH 43210 (United States)

    2010-08-01

    In this study, nickel-based composite anode catalysts consisting of Ni with either Pd on carbon or Pt on carbon (the ratio of Ni:Pd or Ni:Pt being 25:1) were prepared for use in direct borohydride fuel cells (DBFCs). Cathode catalysts used were 1 mg cm{sup -2} Pt/C or Pd electrodeposited on activated carbon cloth. The oxidants were oxygen, oxygen in air, or acidified hydrogen peroxide. Alkaline solution of sodium borohydride was used as fuel in the cell. High power performance has been achieved by DBFC using non-precious metal, Ni-based composite anodes with relatively low anodic loading (e.g., 270 mW cm{sup -2} for NaBH{sub 4}/O{sub 2} fuel cell at 60 C, 665 mW cm{sup -2} for NaBH{sub 4}/H{sub 2}O{sub 2} fuel cell at 60 C). Effects of temperature, oxidant, and anode catalyst loading on the DBFC performance were investigated. The cell was operated for about 100 h and its performance stability was recorded. (author)

  12. Near Surface CO2 Triple Oxygen Isotope Composition

    Directory of Open Access Journals (Sweden)

    Sasadhar Mahata

    2016-02-01

    Full Text Available The isotopic composition of carbon dioxide in the atmosphere is a powerful tool for constraining its sources and sinks. In particular, the 17O oxygen anomaly [Δ17O = 1000 × ln(1 + δ17O/1000 - 0.516 × 1000 × ln(1 + δ18O/1000], with a value > 0.5‰ produced in the middle atmosphere, provides an ideal tool for probing the exchange of carbon dioxide between the biosphere/hydrosphere and atmosphere. The biosphere/hydrosphere and anthropogenic emissions give values ≤ 0.3‰. Therefore, any anomaly in near surface CO2 would reflect the balance between stratospheric input and exchange with the aforementioned surface sources. We have analyzed Δ17O values of CO2 separated from air samples collected in Taipei, Taiwan, located in the western Pacific region. The obtained mean anomaly is 0.42 ± 0.14‰ (1-σ standard deviation, in good agreement with model prediction and a published decadal record. Apart from typically used δ13C and δ18O values, the Δ17O value could provide an additional tracer for constraining the carbon cycle.

  13. Determining the isotopic compositions of uranium and fission products in radioactive environmental microsamples using laser ablation ICP-MS with multiple ion counters.

    Science.gov (United States)

    Boulyga, Sergei F; Prohaska, Thomas

    2008-01-01

    microsamples varied in the range from 0.0073 (corresponding to the natural uranium isotopic composition) to 0.023 (corresponding to initial 235U enrichment in reactor fuel). An inverse correlation was observed between the 236U/238U and 235U/238U isotope ratios, except in the case of one sample with natural uranium. The heterogeneity of the uranium isotope composition is attributed to the different burn-up grades of uranium in the fuel rods from which the microsamples originated.

  14. Composite nuclear fuel fabrication methodology for gas fast reactors

    Science.gov (United States)

    Vasudevamurthy, Gokul

    An advanced fuel form for use in Gas Fast Reactors (GFR) was investigated. Criteria for the fuel includes operation at high temperature (˜1400°C) and high burnup (˜150 MWD/MTHM) with effective retention of fission products even during transient temperatures exceeding 1600°C. The GFR fuel is expected to contain up to 20% transuranics for a closed fuel cycle. Earlier evaluations of reference fuels for the GFR have included ceramic-ceramic (cercer) dispersion type composite fuels of mixed carbide or nitride microspheres coated with SiC in a SiC matrix. Studies have indicated that ZrC is a potential replacement for SiC on account of its higher melting point, increased fission product corrosion resistance and better chemical stability. The present work investigated natural uranium carbide microspheres in a ZrC matrix instead of SiC. Known issues of minor actinide volatility during traditional fabrication procedures necessitated the investigation of still high temperature but more rapid fabrication techniques to minimize these anticipated losses. In this regard, fabrication of ZrC matrix by combustion synthesis from zirconium and graphite powders was studied. Criteria were established to obtain sufficient matrix density with UC microsphere volume fractions up to 30%. Tests involving production of microspheres by spark erosion method (similar to electrodischarge machining) showed the inability of the method to produce UC microspheres in the desired range of 300 to 1200 mum. A rotating electrode device was developed using a minimum current of 80A and rotating at speeds up to 1500 rpm to fabricate microspheres between 355 and 1200 mum. Using the ZrC process knowledge, UC electrodes were fabricated and studied for use in the rotating electrode device to produce UC microspheres. Fabrication of the cercer composite form was studied using microsphere volume fractions of 10%, 20%, and 30%. The macrostructure of the composite and individual components at various stages were

  15. Monitoring the water vapor isotopic composition in the temperate North Atlantic

    Science.gov (United States)

    Sveinbjörnsdottir, Arny E.; Steen-Larsen, Hans Christian; Jonsson, Thorsteinn; Johnsen, Sigfus J.

    2013-04-01

    Water stable isotopes have during many decades been used as climate proxies and indicators for variations in the hydrological cycle. However we are to a great extent still using simple empirical relationships without any deeper theoretical understanding. In order to properly relate changes in the climate and hydrological cycle to changes in the observed stable water isotopic signal we must understand the underlying physical processes. Furthermore it is a challenge for General Climate Models to adequately represent the isotopes in the hydrological cycle because of lack of in-situ measurements of the atmospheric water-vapor composition in the source regions. During the fall of 2010 we installed an autonomous water vapor spectroscopy laser (from Los Gatos Research) in a lighthouse on the South Coast of Iceland (63.83 N 21.47W) with the plan to be operational for several years. The purpose of this installation was through monitoring of the water vapor isotopic composition to understand the physical processes governing the isotopic composition of the water vapor evaporated from the ocean as well as the processes of mixing between the free troposphere and marine boundary layer. Because of the remoteness of the monitoring site and simple topography we are able to isolate the 'fingerprint' on the isotopic signal in the water vapor from respectively the ocean and the interior highland leading to a near perfect case-study area. Using back-trajectories we find a strong influence of the origin of the air masses on the measured isotopic composition. The mixing of the marine-boundary layer is found to strongly influence the measured isotopic composition. The second order isotopic parameter, d-excess, is contrary to theory and previous observations found not to depend on the relative humidity. However we do find a good correlation between the d-excess and the measured isotopic composition. We speculate that the lack of correlation between d-excess and relative humidity can be

  16. Isotopic composition of Pb and Th in interplinian volcanics from Somma-Vesuvius volcano, Italy

    Science.gov (United States)

    Cortini, M.; Ayuso, R.A.; de Vivo, B.; Holden, P.; Somma, R.

    2004-01-01

    We present a detailed isotopic study of volcanic rocks emitted from Somma-Vesuvius volcano during three periods of interplinian activity: "Protohistoric" (3550 y B.P. to 79 A.D.), "Ancient Historic" (79 to 472 A.D.) and "Medieval" (472 to 1631 A.D.). Pb isotopic compositions of two acid leached fractions and whole rock residues of 37 whole rock samples (determined by Somma et al., 2001) show that each of the three interplinian periods is distinguished by small, systematic, and unique uranogenic and thorogenic Pb isotopic trends. This key and novel feature is compatible with the notion that the Pb isotopic data reflect small-scale source heterogeneity operating over relatively short periods of time. From this representative group of samples, a selected set of nine whole rocks were analysed for Th isotopes. 232Th/238U ratios in the source can be obtained independently from Pb and from Th isotopes. Those obtained from Pb isotopes represent source ratios, time-integrated over the whole age of the Earth; they range from 3.9 to 4.1. 232Th/238U obtained from Th isotopes are those of the present source. They are lower, and cluster around 3.5; this difference probably indicates recent U enrichment of the present source. The behaviour of Pb, as inferred by its isotopic ratios, is quite distinct from that of Sr and Nd isotopes: Pb isotope variations are not correlated to Sr or Nd isotope variations. The isotopic contrast is compatible with the idea that the isotopes were decoupled during magmatic production, evolution, and ascent through the crust. Thus, the Pb isotopes do not reflect the effects of the same processes as in the case of the Sr and Nd isotopes, or, as we also favor, they do not necessarily reflect the same source contributions into the magmas. Moreover, the Pb isotopic evolution of the interplinian rocks chiefly reflects mixing, driven by processes that are superimposed on, and independent of, other source contributions that determine the isotopic compositions

  17. Natural isotopic composition of nitrogen in suspended particulate matter in the Bay of Bengal

    Digital Repository Service at National Institute of Oceanography (India)

    Kumar, S.; Ramesh, R.; Bhosle, N.B.; Sardessai, S.; Sheshshayee, M.S.

    The first measurements of nitrogen isotopic composition (delta sup(15) N) in suspended particulate matter (SPM) of the surface Bay of Bengal (BOB) at 24 different locations during pre- (April-May 2003) and post- (September-October 2002) monsoon...

  18. Evolution of Organic Molecules in Space: Characterization and Isotope Composition of Experimental Analogues

    Science.gov (United States)

    Piani, L.; Tachibana, S.; Hama, T.; Endo, Y.; Fujita, K.; Nakatsubo, S.; Fukushi, H.; Mori, S.; Chigai, T.; Yurimoto, H.; Kouchi, A.

    2014-09-01

    Laboratory experiments are conducted to investigate the organic compound formation in molecular cloud conditions and its evolution through UV irradiation and heating. A particular attention is given to the isotope composition of the organic residue.

  19. Carbon and hydrogen isotopic composition and generation pathway of biogenic gas in China

    Institute of Scientific and Technical Information of China (English)

    SHEN Ping; WANG Xiaofeng; XU Yin; SHI Baoguang; XU Yongchang

    2009-01-01

    The carbon and hydrogen isotopic composition of biogenic gas is of great importance for the study of its generation pathway and reservoiring characteristics. In this paper, the formation pathways and reservoiring characteristics of biogenic gas reservoirs in China are described in terms of the carbon and hydrogen isotopic compositions of 31 gas samples from 10 biogenic gas reservoirs. The study shows that the hydrogen isotopic compositions of these biogenic gas reservoirs can be divided into three intervals:δDCH4>-200‰,-250‰<δDCH4<-200‰ and δDCH4<-250‰. The forerunners believed that the main generation pathway of biogenic gas under the condition of continental fresh water is acetic fermentation. Our research results showed that the generation pathway of biogenic gas under the condition of marine facies is typical CO2- reduction, the biogenic gas has heavy hydrogen isotopic composition: its δDCH4 values are higher than -200‰; that the biogenic gas under the condition of continental facies also was generated by the same way, but its hydrogen isotopic composition is lighter than that of biogenetic gas generated under typical marine facies condition: -250‰<δDCH4<-200‰, the δDCH4 values may be related to the salinity of the water medium in ancient lakes. From the relevant data of the Qaidam Basin, it can be seen that the hydrogen isotopic composition of biogenic methane has the same variation trend with increasing salinity of water medium. There are biogenic gas reservoirs formed in transitional regions under the condition of continental facies. These gas reservoirs resulted from both CO2- reduction and acetic fermentation, the formation of which may be related to the non-variant salinity of ancient water medium and the relatively high geothermal gradient, as is the case encountered in the Baoshan Basin. The biogenic gas generating in these regions has light hydrogen isotopic composition: δDCH4<-250‰, and relatively heavy carbon isotopic

  20. Non-destructive measurement of carbonic anhydrase activity and the oxygen isotope composition of soil water

    Science.gov (United States)

    Jones, Sam; Sauze, Joana; Ogée, Jérôme; Wohl, Steven; Bosc, Alexandre; Wingate, Lisa

    2016-04-01

    Carbonic anhydrases are a group of metalloenzymes that catalyse the hydration of aqueous carbon dioxide (CO2). The expression of carbonic anhydrase by bacteria, archaea and eukarya has been linked to a variety of important biological processes including pH regulation, substrate supply and biomineralisation. As oxygen isotopes are exchanged between CO2 and water during hydration, the presence of carbonic anhydrase in plants and soil organisms also influences the oxygen isotope budget of atmospheric CO2. Leaf and soil water pools have distinct oxygen isotope compositions, owing to differences in pool sizes and evaporation rates, which are imparted on CO2during hydration. These differences in the isotopic signature of CO2 interacting with leaves and soil can be used to partition the contribution of photosynthesis and soil respiration to net terrestrial CO2 exchange. However, this relies on our knowledge of soil carbonic anhydrase activity and currently, the prevalence and function of these enzymes in soils is poorly understood. Isotopic approaches used to estimate soil carbonic anhydrase activity typically involve the inversion of models describing the oxygen isotope composition of CO2 fluxes to solve for the apparent, potentially catalysed, rate of oxygen exchange during hydration. This requires information about the composition of CO2 in isotopic equilibrium with soil water obtained from destructive, depth-resolved soil water sampling. This can represent a significant challenge in data collection given the considerable potential for spatial and temporal variability in the isotopic composition of soil water and limited a priori information with respect to the appropriate sampling resolution and depth. We investigated whether we could circumvent this requirement by constraining carbonic anhydrase activity and the composition of soil water in isotopic equilibrium with CO2 by solving simultaneously the mass balance for two soil CO2 steady states differing only in the

  1. Stable hydrogen isotope composition of n-alkanes in urban atmospheric aerosols in Taiyuan, China

    Science.gov (United States)

    Bai, Huiling; Li, Yinghui; Peng, Lin; Liu, Xiangkai; Liu, Xiaofeng; Song, Chongfang; Mu, Ling

    2017-03-01

    The hydrogen isotope compositions (δD) of n-alkanes associated with particulate matter with a diameter of ≤10 μm from Taiyuan, China, during heating and non-heating periods were measured via gas chromatography-isotope ratio mass spectrometry to reveal the spatial and temporal characteristics of five functional zones and to provide another constraint on atmospheric pollutants. The δD values of n-C16 to n-C31 during the heating and non-heating periods ranged from -235.9‰ to -119.8‰ and from -231.3‰ to -129.2‰, respectively, but these similar spans had different distribution features. During the heating period, the δD distributions between non-central heating and commercial districts were consistent, as were those between residential and industrial districts; the n-alkanes came from two or more types of emission sources. Coal soot might be the primary local emission source, but not the only source. During the non-heating period, the n-alkanes of n-C16 to n-C20 were more depleted in D with the increasing carbon number in all functional zones, but there was no rule for n-C21 to n-C31. Specifically, coal soot and vehicle exhaust might be the primary sources of n-alkanes for non-central heating districts in the heating and non-heating periods, respectively, according to the δD distribution of n-C18 to n-C22; gasoline vehicle exhaust might be an n-alkane source, and the hydrogen isotope fractionation effect during the condensation process should be a pollution mechanism for the commercial district during the heating period; the δD distribution difference of n-C16 to n-C18 between the two periods in the residential and industrial districts was consistent, which indicates a similar source of fossil fuel combustion and a similar isotope fractionation effect during the non-heating period.

  2. Spatiotemporal variation of stable isotopic composition in precipitation

    DEFF Research Database (Denmark)

    Müller, Sascha; Stumpp, Christine; Sørensen, Jens Havskov

    2017-01-01

    gradient and predominant westerly winds. Data showed the local meteoric water line for this region is expressed by the equation δ2H = 7.4δ18O + 5.4‰. A significant trend correlating enriched isotopic values to humidities around 70% during dry season and more depleted isotopic values to humidities around 90...

  3. Spatial gradients in the isotopic composition of paleoprecipitation for terrestrial climate and altimetry studies

    Science.gov (United States)

    Chamberlain, C. P.; Winnick, M.; Ibarra, D. E.; Caves, J. K.; Ritch, A. J.

    2016-12-01

    The oxygen and hydrogen isotopic composition of authigenic minerals in terrestrial sediments provides one of the critical measures of past climate change. Frequently, these measurements are made at single sites to determine how climate and/or topography have changed over specific time intervals of interest. We argue here that spatial gradients in the oxygen and hydrogen isotope of precipitation along specific storm tracks provide a more powerful method to determine changes in paleoclimate and paleotopography. We use a nondimensional isotopic vapor transport model coupled with a soil water isotope model to evaluate how moisture recycling and the relative role of eddy diffusion and advective transport of water vapor affect horizontal isotopic gradients on continents. Relatively large changes in the isotopic composition of precipitation can occur by changes in water balance and the transport mechanism of water vapor - certainly as high as can be induced by the uplift of major mountain belts and large changes in global/regional temperature. As an example, we point to Miocene to Recent oxygen isotopic records of paleo-mid latitude sediments that tend to increase with time, globally. We suggest that this increase in the oxygen isotope of precipitation is the result of increased aridity and the expansion of grasslands during the Miocene. Further, we suggest that many of the Miocene to Recent isotopic records collected in the mountainous regions of Central Asia, Western North America, and South America reflect changes in water balance that are, in part, independent of changes in surface topography.

  4. Long-term data set analysis of stable isotopic composition in German rivers

    Science.gov (United States)

    Reckerth, Anne; Stichler, Willibald; Schmidt, Axel; Stumpp, Christine

    2017-09-01

    Stable isotopes oxygen-18 (18O) and deuterium (2H) are commonly used to investigate hydrological processes in catchments. However, only a few isotope studies have been conducted on a large scale and rarely over long time periods. The objective of this study was to identify the spatial and seasonal variability of isotopic composition in river water and how it is affected by geographical and hydrological factors. The stable isotopic composition of river water has been measured in nine large river catchments in Germany for a time period of 12 years or 26 years. We conducted time series and correlation analyses to identify spatial and temporal patterns of the isotopic composition in the rivers. Further, we compared it to isotopic composition in local precipitation and catchments characteristics. In the majority of the rivers, the spatial and temporal patterns of precipitation were directly reflected in river water. The isotopic signals of the river water were time shifted and show attenuated amplitudes. Further deviations from isotopic compositions in local precipitation were observed in catchments with complex flow systems. These deviations were attributed to catchment processes and influences like evaporation, damming and storage. The seasonality of the isotopic composition was mainly determined by the discharge regimes of the rivers. We found correlations between isotopic long-term averages and catchment altitude as well as latitude and longitude, resulting in a northwest-southeast gradient. Furthermore, it was shown that long-term averages of d-excess were inversely related to flow length and catchment size, which indicates that evaporation enrichment has an impact on the isotopic composition even in catchments of humid climates. This study showed that isotopic composition in rivers can serve as a proxy for the local precipitation and can be utilized as an indicator for hydrological processes even in large river basins. In future, such long time series will help to

  5. Elemental and iron isotopic composition of aerosols collected in a parking structure.

    Science.gov (United States)

    Majestic, Brian J; Anbar, Ariel D; Herckes, Pierre

    2009-09-01

    The trace metal contents and iron isotope composition of size-resolved aerosols were determined in a parking structure in Tempe, AZ, USA. Particulate matter (PM)2.5 microm were collected. Several air toxics (e.g., arsenic, cadmium, and antimony) were enriched above the crustal average, implicating automobiles as an important source. Extremely high levels of fine copper (up to 1000 ng m(-3)) were also observed in the parking garage, likely from brake wear. The iron isotope composition of the aerosols were found to be +0.15+/-0.03 per thousand and +0.18+/-0.03 per thousand for the PM2.5 microm fractions, respectively. The similarity of isotope composition indicates a common source for each size fraction. To better understand the source of iron in the parking garage, the elemental composition in four brake pads (two semi-metallic and two ceramic), two tire tread samples, and two waste oil samples were determined. Striking differences in the metallic and ceramic brake pads were observed. The ceramic brake pads contained 10-20% copper by mass, while the metallic brake pads contained about 70% iron, with very little copper. Both waste oil samples contained significant amounts of calcium, phosphorous, and zinc, consistent with the composition of some engine oil additives. Differences in iron isotope composition were observed between the source materials; most notably between the tire tread (average=+0.02 per thousand) and the ceramic brake linings (average=+0.65 per thousand). Differences in isotopic composition were also observed between the metallic (average=+0.18 per thousand) and ceramic brake pads, implying that iron isotope composition may be used to resolve these sources. The iron isotope composition of the metallic brake pads was found to be identical to the aerosols, implying that brake dust is the dominant source of iron in a parking garage.

  6. The oxygen isotope composition of dissolved anthropogenic phosphates: a new tool for eutrophication research?

    Science.gov (United States)

    Gruau, Gérard; Legeas, Michèle; Riou, Christine; Gallacier, Eve; Martineau, François; Hénin, O

    2005-01-01

    High-precision oxygen isotope analyses were carried out on dissolved phosphate extracted from discharge waters from three wastewater treatment plants (WTP) located in western France, as well as on the different phosphate-based fertilizers applied by farmers in the same region. Measured delta(18)O values of phosphate from chemical fertilizers range from 19.6 to 23.1 per thousand, while those of phosphate from WTP discharge waters are more tightly grouped between 17.7 and 18.1 per thousand. The variability in delta(18)O values of phosphate fertilizers is attributed to oxygen isotope variations of the phosphorite deposits from which France's fertilizers are manufactured. The significance of the delta(18)O values of phosphate from WTP discharge waters is less straightforward. At present, it is not clear whether these values are primary isotopic compositions corresponding, e.g., to the oxygen isotope composition of phosphate builders included in detergents (delta(18)O(P)=17.9 per thousand), or represent secondary values reflecting biological recycling of the phosphate in equilibrium with ambient WTP water The restricted difference in isotopic composition obtained between phosphate from fertilizers and phosphate from WTP discharge waters (isotopic variability observed in both end-members (>/=1.5 per thousand), cast doubt about the possibility that the oxygen isotope composition could serve as a tracer for the source of anthropogenic phosphates in waters.

  7. Carbon and oxygen isotope compositions of the carbonate facies in the Vindhyan Supergroup, central India

    Indian Academy of Sciences (India)

    S Banerjee; S K Bhattacharya; S Sarkar

    2006-02-01

    The Vindhyan sedimentary succession in central India spans a wide time bracket from the Paleopro- terozoic to the Neoproterozoic period.Chronostratigraphic significance of stable carbon and oxygen isotope ratios of the carbonate phase in Vindhyan sediments has been discussed in some recent studies.However,the subtle controls of facies variation,depositional setting and post-depositional diagenesis on stable isotope compositions are not yet clearly understood.The Vindhyan Super- group hosts four carbonate units,exhibiting a wide variability in depositional processes and paleogeography.A detailed facies-specific carbon and oxygen isotope study of the carbonate units was undertaken by us to investigate the effect of these processes and to identify the least altered isotope values.It is seen that both carbon and oxygen isotope compositions have been affected by early meteoric water diagenesis.The effect of diagenetic alteration is,however,more pronounced in case of oxygen isotopes than carbon isotopes.Stable isotope compositions remained insensitive to facies only when sediments accumulated in a shallow shelf setting without being exposed.Major alteration of original isotope ratios was observed in case of shallow marine carbonates,which became exposed to meteoric fluids during early diagenetic stage.Duration of exposure possibly determined the magnitude of alteration and shift from the original values.Moreover,dolomitization is found to be accompanied by appreciable alteration of isotope compositions in some of the carbonates.The present study suggests that variations in sediment depositional settings,in particular the possibility of subaerial exposure,need to be considered while extracting chronostratigraphic signi ficance from 13C data.

  8. Variations in isotopic compositions of chlorine in evaporation-controlled salt lake brines of Qaidam Basin, China

    Digital Repository Service at National Institute of Oceanography (India)

    Xiao, Ying-kai; Liu, Wei-guo; Zhou, Y.M.; Wang, Yun-hui; Shirodkar, P.V.

    The variations in the isotopic compositions of chlorine in evaporation-controlled saline lake brines were determined by using an improved procedure for precise measurement of chlorine isotopes based on Cs sub(2) Cl sup(+) ion by thermal ionization...

  9. Oxygen isotopic composition of low-temperature authigenic clinoptilolite

    Science.gov (United States)

    Nähr, T.; Botz, R.; Bohrmann, G.; Schmidt, M.

    1998-08-01

    Oxygen isotope ratios were obtained from authigenic clinoptilolites from Barbados Accretionary Complex, Yamato Basin, and Exmouth Plateau sediments (ODP Sites 672, 797, and 762) in order to investigate the isotopic fractionation between clinoptilolite and pore water at early diagenetic stages and low temperatures. Dehydrated clinoptilolites display isotopic ratios for the zeolite framework ( δ18O f) that extend from +18.7‰ to +32.8‰ (vs. SMOW). In combination with associated pore water isotope data, the oxygen isotopic fractionation between clinoptilolite and pore fluids could be assessed in the temperature range from 25°C to 40°C. The resulting fractionation factors of 1.032 at 25°C and 1.027 at 40°C are in good agreement with the theoretically determined oxygen isotope fractionation between clinoptilolite and water. Calculations of isotopic temperatures illustrate that clinoptilolite formation occurred at relatively low temperatures of 17°C to 29°C in Barbados Ridge sediments and at 33°C to 62°C in the Yamato Basin. These data support a low-temperature origin of clinoptilolite and contradict the assumption that elevated temperatures are the main controlling factor for authigenic clinoptilolite formation. Increasing clinoptilolite δ18O f values with depth indicate that clinoptilolites which are now in the deeper parts of the zeolite-bearing intervals had either formed at lower temperatures (17-20°C) or under closed system conditions.

  10. Magnesium isotopic composition of the oceanic mantle and oceanic Mg cycling

    Science.gov (United States)

    Liu, Ping-Ping; Teng, Fang-Zhen; Dick, Henry J. B.; Zhou, Mei-Fu; Chung, Sun-Lin

    2017-06-01

    To constrain the Mg isotopic composition of the oceanic mantle, investigate Mg isotope fractionation of abyssal peridotites during seafloor alteration, and assess Mg budget in the oceans, a suite of 32 abyssal peridotite samples from the Gakkel Ridge and Southwest Indian Ridge (SWIR) was, for the first time, selected for high-precision Mg isotope analyses. Although most of these samples are extensively altered, largely by serpentinization and weathering, primary olivine, diopside and enstatite grains are preserved in some samples. Olivine grains from the least altered samples have δ26Mg varying from -0.30 to -0.12‰ (n = 7), whereas enstatite and diopside have δ26Mg varying from -0.27 to -0.16‰ (n = 7), and from -0.23 to -0.09‰ (n = 6), respectively. Whole-rock δ26Mg values range from -0.24 to 0.03‰ with an average of -0.12 ± 0.13‰ (2SD, n = 32). Strongly serpentinized peridotites have lower average δ26Mg values (δ26Mg = -0.19 ± 0.07‰, 2SD, n = 7) than weathering-dominated ones (δ26Mg = -0.10 ± 0.12‰, 2SD, n = 25). Calculated Mg isotopic compositions of fresh mantle peridotites vary from -0.29 to -0.13‰, beyond the previously reported range of the subcontinental lithospheric mantle (-0.25 ± 0.04‰) and the analytical uncertainty (±0.07‰, 2SD). Our study therefore indicates that the oceanic mantle may have similar but slightly heterogeneous Mg isotopic compositions to that of subcontinental lithospheric mantle. Secondary serpentinization does not fractionate Mg isotopes of abyssal peridotites, whereas low-T weathering and formation of clay can result in the enrichment of heavy Mg isotopes in abyssal peridotites. This study also demonstrates that fluid-rock interaction does not necessarily produce rocks with intermediate Mg isotopic compositions. Magnesium isotopes of the rocks thereafter are dependent on the secondary minerals formed. We also conclude that the release of light Mg isotopes into the ocean during alteration of abyssal

  11. Abyssal peridotites reveal the near-chondritic Fe isotopic composition of the Earth

    Science.gov (United States)

    Craddock, Paul R.; Warren, Jessica M.; Dauphas, Nicolas

    2013-03-01

    Terrestrial oceanic and continental basalts are enriched by approximately +0.1‰ in 56Fe/54Fe ratio relative to primitive, undifferentiated meteorites (chondrites). The δ56Fe values of terrestrial basalts are also distinct from those of basalts from Mars and asteroid Vesta, which have chondritic Fe isotopic compositions. The processes responsible for the isotopic enrichment of terrestrial basalts are debated, in part because the Fe isotopic composition of the mantle source of terrestrial basalts is unknown. Here we report Fe isotopic measurements of abyssal peridotites, which are the residues of limited melting at oceanic ridges and are thus the best proxies for the composition of the convective portion of the mantle. Our data show that abyssal peridotites have a mean δ56Fe value of +0.010±0.007‰ (relative to IRMM-014), which is indistinguishable from chondrites. After correcting this data for seafloor weathering and mantle melting, we estimate the average Fe isotopic composition of the terrestrial mantle to be δ56Fe=+0.025±0.025‰, which is also indistinguishable from chondrites, within current analytical precision. We determine that the maximum shift in δ56Fe for peridotite residues during partial mantle melting is 0.01‰. Our results argue against isotopic fractionation during core-mantle differentiation or iron vaporization during the Moon-forming giant impact, because both processes would yield a bulk mantle δ56Fe value that is non-chondritic. In addition, our results suggest that disproportionation of mantle Fe2+-Fe3+ in perovskite and Fe0 metal and segregation of metal to the core could not have been a driver for Fe isotopic fractionation in the silicate mantle. Instead, the different iron isotopic compositions of abyssal peridotites and MORBs support mounting evidence for iron isotopic fractionation of melts but not residues during the formation of oceanic and continental crust.

  12. Isotopic composition of Lake Agassiz-Ojibway water just prior to final drainage

    Science.gov (United States)

    Hillaire-Marcel, C.; Helie, J.; McKay, J.; Lalonde, A.

    2006-12-01

    Controversies persist with respect to the impact of the final drainage of Lake Agassiz-Ojibway on the thermohaline circulation of the North Atlantic, some 8.4 ka ago. The lack of response of planktic foraminifer isotope records, off Hudson Strait (i.e., at the outlet of the drainage channel) constitutes one of the most puzzling elements in this debate. However, data on the isotopic composition of drainage waters are needed to estimate the response of the 18-O-salinity relationship in NW Atlantic surface waters. In the literature, a large array of isotopic compositions have been suggested, notably for modeling experiment purposes. Scattered information about the isotopic composition of Lake Agassiz water does exist. It includes isotopic measurements of pore waters of lacustrine sediments [1], analyses of oxygen isotopes in cellulose from algal or plant remains [2], and stable isotope compositions of concretions from varves [3]. Whereas, relatively low oxygen isotope values (apx. -25 per mil vs. VSMOW) are inferred for Lake Agassiz waters during cold pulses of the deglaciation, most data suggest much higher values during the final stages of Lake Agassiz-Ojiway, just prior to its drainage. Calcareous concretions from Lake Ojibway varves (not necessarily contemporaneous to the lacustrine stage) yielded oxygen isotope compositions of about -10 per mil (vs. VPDB), suggesting values as high as -14 per mil (vs. VSMOW) for pore waters (assuming a 0-4 degrees C temperature range). Similar high values (as high as -8 per mil vs. VSMOW [1]) were also estimated from pore water analyses of contemporaneous Lake Agassiz sediments. Here, we used a core raised from Eastern Hudson Bay, off Great Whale River, to further document isotopic compositions of the lake waters prior to their drainage into the North Atlantic. The 7.40 m long core has an apx. 1.3 m-thick lacustrine layer at its base, including the drainage sub- layer. It is overlain by Tyrrell Sea clays. Scarce valves of Candona

  13. Low-Enriched Uranium Fuel Design with Two-Dimensional Grading for the High Flux Isotope Reactor

    Energy Technology Data Exchange (ETDEWEB)

    Ilas, Germina [ORNL; Primm, Trent [ORNL

    2011-05-01

    An engineering design study of the conversion of the High Flux Isotope Reactor (HFIR) from high-enriched uranium (HEU) to low-enriched uranium (LEU) fuel is ongoing at Oak Ridge National Laboratory. The computational models developed during fiscal year 2010 to search for an LEU fuel design that would meet the requirements for the conversion and the results obtained with these models are documented and discussed in this report. Estimates of relevant reactor performance parameters for the LEU fuel core are presented and compared with the corresponding data for the currently operating HEU fuel core. The results obtained indicate that the LEU fuel design would maintain the current performance of the HFIR with respect to the neutron flux to the central target region, reflector, and beam tube locations under the assumption that the operating power for the reactor fueled with LEU can be increased from the current value of 85 MW to 100 MW.

  14. Stable isotopic composition of perchlorate and nitrate accumulated in plants: Hydroponic experiments and field data

    Science.gov (United States)

    Estrada, Nubia Luz; Böhlke, John Karl; Sturchio, Neil C.; Gu, Baohua; Harvey, Greg; Burkey, Kent O.; Grantz, David A.; McGrath, Margaret T.; Anderson, Todd A.; Rao, Balaji; Sevanthi, Ritesh; Hatzinger, Paul B.; Jackson, W. Andrew

    2017-01-01

    Natural perchlorate (ClO4−) in soil and groundwater exhibits a wide range in stable isotopic compositions (δ37Cl, δ18O, and Δ17O), indicating that ClO4− may be formed through more than one pathway and/or undergoes post-depositional isotopic alteration. Plants are known to accumulate ClO4−, but little is known about their ability to alter its isotopic composition. We examined the potential for plants to alter the isotopic composition of ClO4− in hydroponic and field experiments conducted with snap beans (Phaseolus vulgaris L.). In hydroponic studies, anion ratios indicated that ClO4− was transported from solutions into plants similarly to NO3− but preferentially to Cl− (4-fold). The ClO4− isotopic compositions of initial ClO4− reagents, final growth solutions, and aqueous extracts from plant tissues were essentially indistinguishable, indicating no significant isotope effects during ClO4− uptake or accumulation. The ClO4− isotopic composition of field-grown snap beans was also consistent with that of ClO4− in varying proportions from irrigation water and precipitation. NO3− uptake had little or no effect on NO3− isotopic compositions in hydroponic solutions. However, a large fractionation effect with an apparent ε (15N/18O) ratio of 1.05 was observed between NO3− in hydroponic solutions and leaf extracts, consistent with partial NO3− reduction during assimilation within plant tissue. We also explored the feasibility of evaluating sources of ClO4− in commercial produce, as illustrated by spinach, for which the ClO4− isotopic composition was similar to that of indigenous natural ClO4−. Our results indicate that some types of plants can accumulate and (presumably) release ClO4− to soil and groundwater without altering its isotopic characteristics. Concentrations and isotopic compositions of ClO4−and NO3− in plants may be useful for determining sources of fertilizers and sources of ClO4− in their growth environments and

  15. Normal variations in the isotopic composition of metabolically relevant transition metals in human blood

    Science.gov (United States)

    Van Heghe, L.; Cloquet, C.; Vanhaecke, F.

    2012-04-01

    Cu, Fe and Zn are transition metals with great catalytic, structural and regulating importance in the human body. Hence, an aberrant metabolism of these elements can have serious implications on the health of a person. It is assumed that, due to differences in isotope fractionation, the isotopic composition of these elements in whole blood of patients can be different from that in blood of healthy subjects. Therefore, isotopic analysis of the element affected by the disease can be a promising approach for early diagnosis. A method for isotopic analysis of Cu, Fe and Zn in human whole blood was developed. The simultaneous chromatographic isolation of these elements and the conditions for isotope ratio measurement via multi-collector ICP - mass spectrometry (MC-ICP-MS) were optimized. So far, only whole blood of supposedly healthy volunteers (reference population) was analyzed. Results for Fe confirmed the known differences in isotopic composition between male and female blood. It is also shown that other parameters can have influence as well, e.g., the isotopic composition of Zn seems to be governed by the diet.

  16. The stable Cr isotopic compositions of chondrites and silicate planetary reservoirs

    Science.gov (United States)

    Schoenberg, Ronny; Merdian, Alexandra; Holmden, Chris; Kleinhanns, Ilka C.; Haßler, Kathrin; Wille, Martin; Reitter, Elmar

    2016-06-01

    The depletion of chromium in Earth's mantle (∼2700 ppm) in comparison to chondrites (∼4400 ppm) indicates significant incorporation of chromium into the core during our planet's metal-silicate differentiation, assuming that there was no significant escape of the moderately volatile element chromium during the accretionary phase of Earth. Stable Cr isotope compositions - expressed as the ‰-difference in 53Cr/52Cr from the terrestrial reference material SRM979 (δ53/52CrSRM979 values) - of planetary silicate reservoirs might thus yield information about the conditions of planetary metal segregation processes when compared to chondrites. The stable Cr isotopic compositions of 7 carbonaceous chondrites, 11 ordinary chondrites, 5 HED achondrites and 2 martian meteorites determined by a double spike MC-ICP-MS method are within uncertainties indistinguishable from each other and from the previously determined δ53/52CrSRM979 value of -0.124 ± 0.101‰ for the igneous silicate Earth. Extensive quality tests support the accuracy of the stable Cr isotope determinations of various meteorites and terrestrial silicates reported here. The uniformity in stable Cr isotope compositions of samples from planetary silicate mantles and undifferentiated meteorites indicates that metal-silicate differentiation of Earth, Mars and the HED parent body did not cause measurable stable Cr isotope fractionation between these two reservoirs. Our results also imply that the accretionary disc, at least in the inner solar system, was homogeneous in its stable Cr isotopic composition and that potential volatility loss of chromium during accretion of the terrestrial planets was not accompanied by measurable stable isotopic fractionation. Small but reproducible variations in δ53/52CrSRM979 values of terrestrial magmatic rocks point to natural stable Cr isotope variations within Earth's silicate reservoirs. Further and more detailed studies are required to investigate whether silicate

  17. The effect of small scale variablity in isotopic composition of precipitation on hydrograph separation results

    Science.gov (United States)

    Fischer, Benjamin; van Meerveld, Ilja; Seibert, Jan

    2016-04-01

    Understanding runoff processes is important for predictions of streamflow quantity and quality. The two-component isotope hydrograph separation (IHS) method is a valuable tool to study how catchments transform rainfall into runoff. IHS allows the stormflow hydrograph to be separated into rainfall (event water) and water that was stored in the catchment before the event (pre-event water). To be able to perform an IHS, water samples of baseflow (pre-event water) and stormflow are collected at the stream outlet. Rainfall is usually collected at one location by hand as an event total or sampled sequentially during the event. It is usually assumed that the spatial variability in rainfall and the isotopic composition of rainfall are negligible for small (area of 0.15, 0.23, and 0.7 km2). The isotopic composition of rainfall and streamflow were sampled for 10 different rain events (P: 5 mm intervals, Q: 12 to 51 samples per events). This dataset was used to perform a two-component isotope hydrograph separation. The results show that for some events the spatial variability in total rainfall, mean and maximum rainfall intensity and stable isotope composition of rainfall was high. There was no relation between the stable isotope composition of rainfall and the rainfall sum, rainfall intensity or altitude. The spatial variability of the isotopic composition of rainfall was for 4 out of the 10 events as large as the temporal variability in the isotopic composition. Different rainfall weighing methods resulted in different minimum pre-event water fractions in streamflow. For small events with a small mean temporal range in stable isotope composition of rainfall, the different rainfall weighing methods had little effect on the calculated minimum pre-event water fractions. However with increasing temporal variability in stable isotope composition of rainfall, the range in the minimum pre-event water fractions increased and therefore the choice of the rainfall weighing method

  18. Chromium isotope composition of reducing and anoxic sediments from the Peru Margin and Cariaco Basin

    Science.gov (United States)

    Gueguen, B.; Planavsky, N.; Wang, X.; Algeo, T. J.; Peterson, L. C.; Reinhard, C. T.

    2014-12-01

    Chromium isotope systematics in marine sediments are now being used as a new redox proxy of the modern and ancient Earth's surface. Chromium is primarily delivered to the oceans by riverine inputs through weathering of Cr(III)-rich minerals present in the continental crust and oxidation of insoluble Cr(III) to soluble Cr(VI) species. Since oxidation-reduction reactions fractionate Cr isotopes whereby oxidized Cr(VI) species are preferentially enriched in heavy Cr isotopes, the Cr isotope composition of marine sediments may be useful tracers of redox conditions at the Earth's surface through geological time. Chromium is quantitatively removed in organic-rich sediments where reducing conditions prevail and promote reduction of Cr(VI) to Cr(III), and thus, these sediments should capture the ambient seawater Cr isotope composition. However, the isotopic composition of modern organic-rich sediments is poorly documented so far, and this step is essential for further modeling the global oceanic Cr isotope mass balance and assessing the effects of sedimentation and post-depositional processes on the marine Cr isotopes archive. In this study, we have characterized modern marine organic-rich sediments for their Cr isotope composition (δ53/52Cr) from two different settings, the Peru margin upwelling zone and the anoxic Cariaco Basin (Venezuela). Chromium isotopes were measured on a MC-ICP-MS (Nu Plasma) using a double-spike correction method. The authigenic fraction of shallow samples from the Peru margin sedimentary sequence with a high Total Organic Carbon (TOC) content (>10 wt%) yield an average δ53/52Crauthigenic value of +0.67 ±0.05 ‰ (2sd). However, although this value is close to the seawater value (Atlantic Ocean) and to Cariaco basin sediments (~ +0.6 ‰), reducing sediments from the Peru margin are on average isotopically slightly heavier, especially in samples having a low authigenic fraction and a low TOC content (δ53/52Crauthigenic values up to +1.30

  19. Wet deposition at the base of Mt Everest: Seasonal evolution of the chemistry and isotopic composition

    Science.gov (United States)

    Balestrini, Raffaella; Delconte, Carlo A.; Sacchi, Elisa; Wilson, Alana M.; Williams, Mark W.; Cristofanelli, Paolo; Putero, Davide

    2016-12-01

    The chemistry of wet deposition was investigated during 2012-2014 at the Pyramid International Laboratory in the Upper Khumbu Valley, Nepal, at 5050 m a.s.l., within the Global Atmosphere Watch (GAW) programme. The main hydro-chemical species and stable isotopes of the water molecule were determined for monsoon rain (July-September) and snow samples (October-June). To evaluate the synoptic-scale variability of air masses reaching the measurement site, 5 day back-trajectories were computed for the sampling period. Ion concentrations in precipitation during the monsoon were low suggesting that they represent global regional background concentrations. The associations between ions suggested that the principal sources of chemical species were marine aerosols, rock and soil dust, and fossil fuel combustion. Most chemical species exhibited a pattern during the monsoon, with maxima at the beginning and at the end of the season, partially correlated with the precipitation amount. Snow samples exhibited significantly higher concentrations of chemical species, compared to the monsoon rainfall observations. Particularly during 2013, elevated concentrations of NO3-, SO42- and NH4+ were measured in the first winter snow event, and in May at the end of the pre-monsoon season. The analysis of large-scale circulation and wind regimes as well as atmospheric composition observations in the region indicates the transport of polluted air masses from the Himalayan foothills and Indian sub-continent up to the Himalaya region. During the summer monsoon onset period, the greater values of pollutants can be attributed to air-mass transport from the planetary boundary layer (PBL) of the Indo-Gangetic plains. Isotopic data confirm that during the monsoon period, precipitation occurred from water vapor that originated from the Indian Ocean and the Bay of Bengal; by contrast during the non-monsoon period, an isotopic signature of more continental origin appeared, indicating that the higher

  20. The stable isotopic composition of molecular hydrogen in the tropopause region probed by the CARIBIC aircraft

    Science.gov (United States)

    Batenburg, A. M.; Schuck, T. J.; Baker, A. K.; Zahn, A.; Brenninkmeijer, C. A. M.; Röckmann, T.

    2012-05-01

    More than 450 air samples that were collected in the upper troposphere - lower stratosphere (UTLS) region by the CARIBIC aircraft (Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container) have been analyzed for molecular hydrogen (H2) mixing ratios (χ(H2)) and H2 isotopic composition (deuterium content, δD). More than 120 of the analyzed samples contained air from the lowermost stratosphere (LMS). These show that χ(H2) does not vary appreciably with O3-derived height above the thermal tropopause (TP), whereas δD does increase with height. The isotope enrichment is caused by H2 production and destruction processes that enrich the stratospheric H2 reservoir in deuterium (D); the exact shapes of the profiles are mainly determined by mixing of stratospheric with tropospheric air. Tight negative correlations are found between δD and the mixing ratios of methane (χ(CH4)) and nitrous oxide (χ(N2O)), as a result of the relatively long lifetimes of these three species. The correlations are described by δD[‰]=-0.35 · χ(CH4)[ppb]+768 and δD[‰]=-1.90· χ(N2O)[ppb]+745. These correlations are similar to previously published results and likely hold globally for the LMS. Samples that were collected from the Indian subcontinent up to 40° N before, during and after the summer monsoon season show no significant seasonal change in χ(H2), but δD is up to 12.3‰ lower in the July, August and September monsoon samples. This δD decrease is correlated with the χ(CH4) increase in these samples. The significant correlation with χ(CH4) and the absence of a perceptible χ(H2) increase that accompanies the δD decrease indicates that microbial production of very D-depleted H2 in the wet season may contribute to this phenomenon. Some of the samples have very high χ(H2) and very low δD values, which indicates a pollution effect. Aircraft engine exhaust plumes are a suspected cause, since the effect mostly occurs in samples

  1. Process engineering of ceramic composite coatings for fuel cell systems

    Energy Technology Data Exchange (ETDEWEB)

    Li, G.; Kim, H.; Chen, M.; Yang, Q.; Troczynski, T. [British Columbia Univ., Vancouver, BC (Canada). Dept. of Metals and Materials Engineering

    2003-07-01

    Researchers at UBCeram at the Department of Metals and Materials Engineering at the University of British Columbia have developed a technology to chemically bond composite sol-gel (CB-CSG) coating onto metallic surfaces of complex or concave shapes. The process has been optimized for electrically resistive coatings and corrosion-resistant coatings. The CSG is sprayed onto metallic surfaces and is heat-treated at 300 degrees C to partially dehydrate the hydroxides. The CSG film is then chemically bonded through reaction of active alumina with metal phosphates, such as aluminium phosphate. A new chromate-free process is being developed to address the issue of coatings porosity. The electrodeposition technique involves polymer particles mixed with suspended fine alumina particles which are co-deposited by electrophoretic means or by electrocoagulation. The composite e-coatings have excellent mechanical properties and are being considered as a protective coating for various components of fuel cell systems. 9 refs., 7 figs.

  2. The isotopic composition of dissolved cadmium in the water column of the West Philippine Sea

    Directory of Open Access Journals (Sweden)

    Shun-Chung eYang

    2014-11-01

    Full Text Available The dissolved concentration and isotopic compositions of cadmium (Cd in the seawater of the West Philippine Sea were determined. In general, Cd isotopic composition in the water column decreased with depth, with ε114/110Cd (ε114/110Cd = [(114Cd/110Cdsample / (114Cd/110CdNIST 3108 - 1]×10000 ranging from +7.2 to +10.1 in the top 60 m, from +4.8 to +5.1 between 100 and 150 m, peaking at +8.2 at 200 m, decreasing from +4.5 to +3.3 from 400 to 1000 m, and remaining constant at +3.0 from 1000 m and deeper. Different to a Rayleigh fractionation model, the isotopic composition and log scale concentrations of Cd do not exhibit a linear relationship. However, from the deep water to thermocline, the variations in Cd concentration and ε114/110Cd are relevant to the variations of temperature and salinity, indicating that water mixing is the dominant processes determining the concentration and isotopic composition in the interval. At 200 m where North Pacific Tropic Water dominates the water mass, the elevated ε114/110Cd could be linked to the composition in the upper portions of the water mass. In the top 150 m, the ε114/110Cd varies similarly to the phytoplankton community structures, implying that Cd uptake by various phytoplankton species may be associated with the isotopic variation. However, the effects of atmospheric inputs to the ε114/110Cd in the surface water cannot be excluded. A box model calculation is used to constrain the contributions of various processes to the Cd isotopes of surface water, and the results indicate that the Cd concentration and isotopic composition in most of the water body of the region are controlled by physical mixing, while the effects of biological fractionation and atmospheric inputs are limited in the euphotic zone.

  3. The minor sulfur isotope composition of Cretaceous and Cenozoic seawater sulfate

    Science.gov (United States)

    Masterson, A. L.; Wing, Boswell A.; Paytan, Adina; Farquhar, James; Johnston, David T.

    2016-06-01

    The last 125 Myr capture major changes in the chemical composition of the ocean and associated geochemical and biogeochemical cycling. The sulfur isotopic composition of seawater sulfate, as proxied in marine barite, is one of the more perplexing geochemical records through this interval. Numerous analytical and geochemical modeling approaches have targeted this record. In this study we extend the empirical isotope record of seawater sulfate to therefore include the two minor sulfur isotopes, 33S and 36S. These data record a distribution of values around means of Δ33S and Δ36S of 0.043 ± 0.016‰ and -0.39 ± 0.15‰, which regardless of δ34S-based binning strategy is consistent with a signal population of values throughout this interval. We demonstrate with simple box modeling that substantial changes in pyrite burial and evaporite sulfate weathering can be accommodated within the range of our observed isotopic values.

  4. The atomic weight and isotopic composition of nitrogen and their variation in nature

    Energy Technology Data Exchange (ETDEWEB)

    Holden, N.E.

    1987-01-01

    Two stable isotopes of nitrogen exist in nature, /sup 14/N and /sup 15/N. The less abundant isotope, /sup 15/N, was discovered in 1929 by Naude, who studied the band spectra of nitric oxide, NO. However, the main source of a standard for this element is the air in the atmosphere, which is made up of approximately 78% N/sub 2/. Reviewed in this paper is the measurements of the isotopic composition in air and its variation around the world. Also investigated is the variation of the isotopic composition in the various compounds or sources of nitrogen compared to the value in air. Data on the atomic weight and non-terrestrial data for nitrogen is also reviewed.

  5. Solid oxide fuel cell composite cathodes based on perovskite and fluorite structures

    Science.gov (United States)

    Sadykov, Vladislav; Mezentseva, Natalia; Usoltsev, Vladimir; Sadovskaya, Ekaterina; Ishchenko, Arkady; Pavlova, Svetlana; Bespalko, Yulia; Kharlamova, Tamara; Zevak, Ekaterina; Salanov, Aleksei; Krieger, Tamara; Belyaev, Vladimir; Bobrenok, Oleg; Uvarov, Nikolai; Okhlupin, Yury; Smorygo, Oleg; Smirnova, Alevtina; Singh, Prabhakar; Vlasov, Aleksandr; Korobeynikov, Mikhail; Bryazgin, Aleksandr; Kalinin, Peter; Arzhannikov, Andrei

    This work presents the results related to the functionally graded fluorite (F)-perovskite (P) nanocomposite cathodes for IT SOFC. Nanocrystalline fluorites (GDC, ScCeSZ) and perovskites (LSrMn, LSrFNi) were synthesized by Pechini method. Nanocomposites were prepared by the ultrasonic dispersion of F and P powders in isopropanol with addition of polyvinyl butyral. Different techniques for deposition and sintering of functionally graded cathode materials were applied including traditional approaches as well as original methods, such as radiation-thermal sintering under electron beam or microwave radiation. Morphology, microstructure and elemental composition of nanocomposites was characterized by XRD and HRTEM/SEM with EDX. Even for dense composites, the sizes of perovskite and fluorite domains remain in the nanorange providing developed P-F interfaces. Oxygen isotope heteroexchange and conductivity/weight relaxation studies demonstrated that these interfaces provide a path for fast oxygen diffusion. The redistribution of the elements between P and F phases in nanocomposites occurs without formation of insulating zirconate phases. Button-size fuel cells with nanocomposite functionally graded cathodes, thin YSZ layers and anode Ni/YSZ cermet (either bulk or supported on Ni-Al foam substrates) were manufactured. For optimized composition and functionally graded design of P-F nanocomposite cathodes, a stable performance in the intermediate temperature range with maximum power density up to 0.5 W cm -2 at 700 °C in wet H 2/air feeds was demonstrated.

  6. On the isotopic composition of precipitation; Sur la composition isotopique des precipitations

    Energy Technology Data Exchange (ETDEWEB)

    Gonfiantini, R. [Paris-11 Univ., 91 - Orsay (France). Laboratoire d`Hydrologie et de Geochimie Isotopique

    1998-12-31

    The paper discusses some aspects of the isotopic composition (tritium and stable isotopes) of global precipitation which is being monitored since the late fifties through the network established by the International Atomic Energy Agency. Three quarters of the tritium formed during the atmospheric thermonuclear tests were released in the biennium 1961-1962. The successive five years of the test moratorium provide a unique information on the tritium transfer rate from the stratosphere to the troposphere. The tritium concentration decreased steadily, and the decrease rate appears to be greater at high latitude. This fact can possibly be explained by precipitation recycling by evapotranspiration, which is more important at low latitudes, and tritium concentration ratio between two successive years, is close to 0.68 {+-} 0.02, with the exception of the year 1965, when the tritium content dropped to 0.50 {+-} 0.02 with respect to the previous year. At latitudes between 30 and 60 deg C, the correlations between {delta}{sup 2}H and {delta}{sup 18}O show almost identical slopes in winter and summer precipitation, but different intercepts. The correlations are: {delta}{sup 2}H (8.36{+-}0.13) {delta}{sup 18}O+(14.2{+-}4.2) for January and {delta}{sup 2}H 8.33{+-}0.013) {delta}{sup 18}O+(8.2{+-}3.9) for July. This reflects a different seasonal deuterium excess (defined as d {delta}{sup 2}H - 8{delta}{sup 18}O), which has a mean value of 10.7{+-} 0.6 %0 in July, and a higher average value of 10.7 {+-} 0.6%0 in January and 5.8{+-} 0.5%0 in July, and a higher average value in stations with prevailing winter rains. Also, the slope becomes about 8 when summer and winter precipitation are considered all together. The altitude effect on the isotopic composition of precipitation on Mount Cameroon is re-examined. The model which best fits the data is based on the adiabatic condensation of the atmospheric vapour with a liquid/vapor ratio increasing from 0.15 at sea level to 0.45 at 4

  7. Natural variations in the rhenium isotopic composition of meteorites

    Science.gov (United States)

    Liu, R.; Hu, L.; Humayun, M.

    2017-03-01

    Rhenium is an important element with which to test hypotheses of isotope variation. Historically, it has been difficult to precisely correct the instrumental mass bias in thermal ionization mass spectrometry. We used W as an internal standard to correct mass bias on the MC-ICP-MS, and obtained the first precise δ187Re values ( ±0.02‰, 2SE) for iron meteorites and chondritic metal. Relative to metal from H chondrites, IVB irons are systematically higher in δ187Re by 0.14 ‰. δ187Re for other irons are similar to H chondritic metal, although some individual samples show significant isotope fractionation. Since 185Re has a high neutron capture cross section, the effect of galactic cosmic-ray (GCR) irradiation on δ187Re was examined using correlations with Pt isotopes. The pre-GCR irradiation δ187Re for IVB irons is lower, but the difference in δ187Re between IVB irons and other meteoritic metal remains. Nuclear volume-dependent fractionation for Re is about the right magnitude near the melting point of iron, but because of the refractory and compatible character of Re, a compelling explanation in terms of mass-dependent fractionation is elusive. The magnitude of a nucleosynthetic s-process deficit for Re estimated from Mo and Ru isotopes is essentially unresolvable. Since thermal processing reduced nucleosynthetic effects in Pd, it is conceivable that Re isotopic variations larger than those in Mo and Ru may be present in IVBs since Re is more refractory than Mo and Ru. Thus, the Re isotopic difference between IVBs and other irons or chondritic metal remains unexplained.

  8. Magmatic recharge buffers the isotopic compositions against crustal contamination in formation of continental flood basalts

    Science.gov (United States)

    Yu, Xun; Chen, Li-Hui; Zeng, Gang

    2017-07-01

    Isotopic compositions of continental flood basalts are essential to understand their genesis and to constrain the character of their mantle sources. Because of potential crustal contamination, it needs to be evaluated if and to which degree these basalts record original isotopic signals of their mantle sources and/or crustal signatures. This study examines the Sr, Nd, Hf, and Pb isotopic compositions of the late Cenozoic Xinchang-Shengzhou (XS) flood basalts, a small-scale continental flood basalt field in eastern China. The basalts show positive correlations between 87Sr/86Sr and 143Nd/144Nd, and negative correlations between 143Nd/144Nd and 176Hf/177Hf, which deviate from compositional arrays of crustal contamination and instead highlight variations in magmatic recharge intensity and mantle source compositions. The lava samples formed by high-volume magmatic recharge recorded signals of recycled sediments in the mantle source, which are characterized by moderate Ba/Th (91.9-106.5), excess 208Pb/204Pb relative to 206Pb/204Pb, and excess 176Hf/177Hf relative to 143Nd/144Nd. Thus, we propose that magmatic recharge buffers the original isotopic compositions of magmas against crustal contamination. Identifying and utilizing the isotope systematics of continental flood basalts generated by high volumes of magmatic recharge are thus crucial to trace their mantle sources.

  9. Synthesis and sintering of UN-UO2 fuel composites

    Science.gov (United States)

    Jaques, Brian J.; Watkins, Jennifer; Croteau, Joseph R.; Alanko, Gordon A.; Tyburska-Püschel, Beata; Meyer, Mitch; Xu, Peng; Lahoda, Edward J.; Butt, Darryl P.

    2015-11-01

    The design and development of an economical, accident tolerant fuel (ATF) for use in the current light water reactor (LWR) fleet is highly desirable for the future of nuclear power. Uranium mononitride has been identified as an alternative fuel with higher uranium density and thermal conductivity when compared to the benchmark, UO2, which could also provide significant economic benefits. However, UN by itself reacts with water at reactor operating temperatures. In order to reduce its reactivity, the addition of UO2 to UN has been suggested. In order to avoid carbon impurities, UN was synthesized from elemental uranium using a hydride-dehydride-nitride thermal synthesis route prior to mixing with up to 10 wt% UO2 in a planetary ball mill. UN and UN - UO2 composite pellets were sintered in Ar - (0-1 at%) N2 to study the effects of nitrogen concentration on the evolved phases and microstructure. UN and UN-UO2 composite pellets were also sintered in Ar - 100 ppm N2 to assess the effects of temperature (1700-2000 °C) on the final grain morphology and phase concentration.

  10. Variation in the terrestrial isotopic composition and atomic weight of argon

    Science.gov (United States)

    Böhlke, John Karl

    2014-01-01

    The isotopic composition and atomic weight of argon (Ar) are variable in terrestrial materials. Those variations are a source of uncertainty in the assignment of standard properties for Ar, but they provide useful information in many areas of science. Variations in the stable isotopic composition and atomic weight of Ar are caused by several different processes, including (1) isotope production from other elements by radioactive decay (radiogenic isotopes) or other nuclear transformations (e.g., nucleogenic isotopes), and (2) isotopic fractionation by physical-chemical processes such as diffusion or phase equilibria. Physical-chemical processes cause correlated mass-dependent variations in the Ar isotope-amount ratios (40Ar/36Ar, 38Ar/36Ar), whereas nuclear transformation processes cause non-mass-dependent variations. While atmospheric Ar can serve as an abundant and homogeneous isotopic reference, deviations from the atmospheric isotopic ratios in other Ar occurrences limit the precision with which a standard atomic weight can be given for Ar. Published data indicate variation of Ar atomic weights in normal terrestrial materials between about 39.7931 and 39.9624. The upper bound of this interval is given by the atomic mass of 40Ar, as some samples contain almost pure radiogenic 40Ar. The lower bound is derived from analyses of pitchblende (uranium mineral) containing large amounts of nucleogenic 36Ar and 38Ar. Within this interval, measurements of different isotope ratios (40Ar/36Ar or 38Ar/36Ar) at various levels of precision are widely used for studies in geochronology, water–rock interaction, atmospheric evolution, and other fields.

  11. Molybdenum isotopic composition of single silicon carbides from supernovae.

    Energy Technology Data Exchange (ETDEWEB)

    Amari, S.; Clayton, R. N.; Davis, A. M.; Lewis, R. S.; Pellin, M. J.

    1999-02-03

    Presolar silicon carbide grains form in a variety of types of stars, including asymptotic giant branch red giant stars and supernovae. The dominant mechanisms of heavy element nucleosynthesis, the s-process and r-process, are thought to occur in AGB stars and supernovae, respectively. We have previously reported that mainstream SiC grains have strong enrichments in the s-process isotopes of Sr, Zr and Mo. We report here the first measurements of Mo isotopes in X-type SiC grains, which have previously been identified as having formed from supernova ejecta.

  12. Is my C isotope excursion global, local, or both? Insights from the Mg and Ca isotopic composition of primary, diagenetic, and authigenic carbonates

    Science.gov (United States)

    Higgins, J. A.; Blättler, C. L.; Husson, J. M.

    2014-12-01

    The C isotopic composition of ancient limestones and dolomites is a widely used proxy for the global geochemical cycles of carbon and oxygen in the ocean-atmosphere system and a critical tool for chemostratigraphy in Precambrian rocks. Although relatively robust to diagenesis, the C isotopic composition of bulk carbonates can be reset when conditions favor high water-to-rock ratios or fluids with high C concentrations and distinct isotopic compositions. Authigenic carbonates and different pools of primary carbonate (e.g. calcite vs. aragonite) may also bias the C isotopic composition of bulk carbonates if they are both abundant and isotopically distinct. New approaches to quantifying contributions from diagenesis, authigenesis, and mixing of primary carbonates to the C isotopic composition of bulk sedimentary carbonates are needed. Here we present preliminary Mg and Ca isotope data sets of primary, diagenetic, and authigenic carbonates, both modern and ancient. We show that recrystallization, dolomitization, and authigenesis produce Mg and Ca isotope fingerprints that may be used to identify and characterize these processes in ancient carbonate sediments.

  13. Potential of using stable nitrogen isotope ratio measurements to resolve fuel and thermal NOx in coal combustion

    Energy Technology Data Exchange (ETDEWEB)

    Chenggong Sun; Janos Lakatos; Colin E. Snape; Tony Fallick [University of Nottingham, Nottingham (United Kingdom). School of Chemical, Environmental and Mining Engineering (SChEME)

    2003-07-01

    In order to examine the potential of applying isotopic analysis to apportion NOx formation from different mechanisms, stable nitrogen isotope ratio measurements have been conducted on a number of thermal/prompt (diesel) and actual (coal) PF NO samples generated from a 1MW test facility at Powergen (UK), together with measurements on a range of pyrolysis and combustion chars obtained from a drop-tube reactor. A highly effective nitrogen-free sorbent, derived from white sugar with Mn as promoter, has been developed using an innovative procedure. This adsorbent has facilitated, for the first time, the determination of {delta}{sup 15}N values without background corrections. The isotopic data indicate that the thermal/prompt NOx collected during start-up with diesel as fuel has a {delta}{sup 15}N of close to 6.5(per thousand) compared to +15(per thousand) for the actual PF sample analysed. Thus, differences of up to ca. 20(per thousand) have been found to exist between thermal and PF fuel (char) NOx isotopic values. This augurs very well for the further development of the approach in order to help quantify the extent of thermal/prompt NOx formation in PF combustion. Measurements on chars have indicated that the extent of isotopic fractionation that occurs between coal-N and NOx from char is related to the reactivity of coals. Further, it would appear that much of the isotopic fractionation that occurs between coal nitrogen and fuel NO arises in the formation of char, although further fractionation can be inferred to occur during char combustion. In contrast, a lesser degree of isotopic fractionation is associated with the formation of thermal NO (ca. 6(per thousand)), atmospheric nitrogen having a value of 0(per thousand). 4 refs., 6 tabs.

  14. Potassium Isotopic Compositions of NIST Potassium Standards and 40Ar/39Ar Mineral Standards

    Science.gov (United States)

    Morgan, Leah; Tappa, Mike; Ellam, Rob; Mark, Darren; Higgins, John; Simon, Justin I.

    2013-01-01

    Knowledge of the isotopic ratios of standards, spikes, and reference materials is fundamental to the accuracy of many geochronological methods. For example, the 238U/235U ratio relevant to U-Pb geochronology was recently re-determined [1] and shown to differ significantly from the previously accepted value employed during age determinations. These underlying values are fundamental to accurate age calculations in many isotopic systems, and uncertainty in these values can represent a significant (and often unrecognized) portion of the uncertainty budget for determined ages. The potassium isotopic composition of mineral standards, or neutron flux monitors, is a critical, but often overlooked component in the calculation of K-Ar and 40Ar/39Ar ages. It is currently assumed that all terrestrial materials have abundances indistinguishable from that of NIST SRM 985 [2]; this is apparently a reasonable assumption at the 0.25per mille level (1s) [3]. The 40Ar/39Ar method further relies on the assumption that standards and samples (including primary and secondary standards) have indistinguishable 40K/39K values. We will present data establishing the potassium isotopic compositions of NIST isotopic K SRM 985, elemental K SRM 999b, and 40Ar/39Ar biotite mineral standard GA1550 (sample MD-2). Stable isotopic compositions (41K/39K) were measured by the peak shoulder method with high resolution MC-ICP-MS (Thermo Scientific NEPTUNE Plus), using the accepted value of NIST isotopic SRM 985 [2] for fractionation [4] corrections [5]. 40K abundances were measured by TIMS (Thermo Scientific TRITON), using 41K/39K values from ICP-MS measurements (or, for SRM 985, values from [2]) for internal fractionation corrections. Collectively these data represent an important step towards a metrologically traceable calibration of 40K concentrations in primary 40Ar/39Ar mineral standards and improve uncertainties by ca. an order of magnitude in the potassium isotopic compositions of standards.

  15. About the possibility of creating a continuous range of standards with different isotopic composition of carbon

    Directory of Open Access Journals (Sweden)

    S. A. Sadykov

    2014-01-01

    Full Text Available It is established that the carbon isotopic composition in the formation of calcium carbonate is changed depending on the magnetic field strength. The formation of calcium carbonate occurred due to the interaction of calcium hydroxide with atmospheric carbon dioxide. The profile of isotopic relations13C/12C of the newly formed calcium carbonate is approximated by the equation of the parabola for certain values of tension solenoidal magnetic field. The possibility of creating standards with a continuous series of values of the content of carbon stable isotopes based on the data suggested.

  16. The isotopic composition of dissolved inorganic nitrogen in hydrothermal vent fluids

    Science.gov (United States)

    Lehmann, M. F.; Bourbonnais, A.; Butterfield, D. A.

    2006-12-01

    Hydrothermal vent systems at mid-ocean ridges are sites with rapid rates of biomass production, sustained by chemolithoautotrophic bacteria at the base of the vent community food chains. The exact metabolic pathways, in particular those that involve nitrogen (N), and the rates at which the metabolic reactions take place are poorly constrained. In previous studies, very low 15N/14N ratios have been attributed to strong N isotope fractionation during chemosynthetic assimilation of ammonium. However, actual data on the N isotopic composition of dissolved inorganic N in vent systems, which could provide coherent information on the sources of N during chemolithoautotrophic biosynthesis, do not exist. Furthermore, the fate of hydrothermally discharged ammonium as well as that of nitrate that is mixed in from the ocean water column have not been the focus of much attention. As a consequence, little is known about N-cycle reactions within hydrothermal vent systems. We will present nitrate isotope (15N/14N and 18O/16O) data from various sites at Axial Volcano on the Juan de Fuca ridge. Their integration with nitrate concentration data suggests non-conservative behavior of nitrate along temperature gradients. Highest N and O isotope ratios (7.6 permil and 21.0 permil, respectively) are found in average diffuse fluids (17°C). Elevated N and O isotope ratios were associated with decreased nitrate concentrations and indicate a nitrate consuming process that fractionates both N and O isotopes. The ratio of 15N versus 18O enrichment in residual nitrate is, however, not consistent with previous reports on nitrate N versus O isotope fractionation during denitrification in the suboxic ocean water column, implying anomalous N and O isotope fractionation during denitrification in hydrothermal vent fluids and/or the presence of additional microbially mediated N transformations that affect the N and O isotope composition of the nitrate pool in the Axial hydrothermal vent system in a

  17. Zirconium isotope constraints on the composition of Theia and current Moon-forming theories

    Science.gov (United States)

    Akram, W.; Schönbächler, M.

    2016-09-01

    The giant impact theory is the most widely recognized formation scenario of the Earth's Moon. Giant impact models based on dynamical simulations predict that the Moon acquired a significant amount of impactor (Theia) material, which is challenging to reconcile with geochemical data for O, Si, Cr, Ti and W isotopes in the Earth and Moon. Three new giant impact scenarios have been proposed to account for this discrepancy - hit-and-run impact, impact with a fast-spinning protoEarth and massive impactors - each one reducing the proportion of the impactor in the Moon compared to the original canonical giant impact model. The validity of each theory and their different dynamical varieties are evaluated here using an integrated approach that considers new high-precision Zr isotope measurements of lunar rocks, and quantitative geochemical modelling of the isotopic composition of the impactor Theia. All analysed lunar samples (whole-rock, ilmenite and pyroxene separates) display identical Zr isotope compositions to that of the Earth within the uncertainty of 13 ppm for 96Zr/90Zr (2σ weighted average). This 13 ppm upper limit is used to infer the most extreme isotopic composition that Theia could have possessed, relative to the Earth, for each of the proposed giant impact theories. The calculated Theian composition is compared with the Zr isotope compositions of different solar system materials in order to constrain the source region of the impactor. As a first order approximation, we show that all considered models (including the canonical) are plausible, alleviating the initial requirement for the new giant impact models. Albeit, the canonical and hit-and-run models are the most restrictive, suggesting that the impactor originated from a region close to the Earth. The fast-spinning protoEarth and massive impactor models are more relaxed and increase the allowed impactor distance from the Earth. Similar calculations carried out for O, Cr, Ti and Si isotope data support

  18. Water transport in protoplanetary disks and the hydrogen isotopic composition of chondrites

    CERN Document Server

    Jacquet, Emmanuel

    2013-01-01

    The D/H ratios of carbonaceous chondrites, believed to reflect that of water in the inner early solar system, are intermediate between the protosolar value and that of most comets. The isotopic composition of cometary water has been accounted for by several models where the isotopic composition of water vapor evolved by isotopic exchange with hydrogen gas in the protoplanetary disk. However, the position and the wide variations of the distribution of D/H ratios in carbonaceous chondrites have yet to be explained. In this paper, we assume that the D/H composition of cometary ice was achieved in the disk building phase and model the further isotopic evolution of water in the inner disk in the classical T Tauri stage. Reaction kinetics compel isotopic exchange between water and hydrogen gas to stop at $\\sim$500 K, but equilibrated water can be transported to the snow line (and beyond) via turbulent diffusion and consequently mix with isotopically comet-like water. Under certain simplifying assumptions, we calcul...

  19. Neutronic and thermal analysis of composite fuel for potential deployment in fast reactors

    Energy Technology Data Exchange (ETDEWEB)

    Abou Jaoude, Abdalla; Thomas, Colin; Erickson, Anna, E-mail: erickson@gatech.edu

    2016-07-15

    Highlights: • Neutronic and heat transfer performance of composite fuels on the macro-scale. • Methodology to guide flexible fuel design using high fidelity simulation tools. • Viability of composite fuels for ultra-high burnup fast reactor deployment. - Abstract: Composite fuels are promising candidates for high-burnup fast reactors because of their accommodation of swelling, limited fuel-cladding interactions and flexibility in design. While a proof-of-concept fuel consisting of granules of U-alloys and PuO{sub 2} dispersed within a porous zirconium matrix was successfully manufactured and irradiated, its neutronic and thermal performance remains to be optimized as compared to currently utilized fuels. MCNP6, COMSOL and a sphere packing algorithm were employed to perform the analysis. We found that both the theoretical maximum burnup reached and the temperature profiles are comparable to that of the currently considered alternative fuel. The results are promising and do not indicate any substantial limitation to the deployment of composite fuel. The fuel type merits further research, including full-core simulations. The methodology followed herein also provides a basis for screening different material compositions and guiding materials selection in composite fuels.

  20. A REFINED LOOK AT THE IRON ISOTOPE COMPOSITION OF THE MOON

    Science.gov (United States)

    Poitrasson, F.; Zambardi, T.; Magna, T.; Neal, C. R.

    2009-12-01

    It is difficult to estimate the bulk chemical and isotopic properties of planets, especially for the Moon for which our sampling is far more limited than for the Earth. As a result, there is currently a debate on the bulk Fe isotope composition of the Moon: Whereas in a first study we proposed that the bulk lunar Fe isotope composition (δ57Fe ~0.2‰) was twice as heavy as that of the Earth (δ57Fe ~0.1‰) relative to chondrites (δ57Fe ~0‰), normalized to IRMM-14, others proposed that there is no difference between Earth and Moon. This question is of crucial importance because the first case may track the Moon-forming giant interplanetary impact, whereas the alternative situation may also result from a very high pressure metal-silicate fractionation during the Earth’s core formation, assuming that the Moon subsequently inherited the Earth Fe isotope composition. To reassess this question, we analyzed a suite of 18 mare basalts (both high- and low-Ti) by MC-ICP-MS using the nickel doping technique developed at LMTG. Combined with our previous measurements of lunar rocks, we obtained a mean δ57Fe of 0.138±0.035‰ (2SE, n=11) for low-Ti basalts, 0.269±0.026‰ (2SE, n=16) for high-Ti ones and 0.177±0.036‰ (2SE, n=6) for highland rocks. T-tests confirm that averages of low- and high-Ti basalts are significantly different at the 95% confidence level. Similarly, t-tests indicate that highland rocks are significantly different from high-Ti basalts, but not from low-Ti ones. These new data therefore confirm suggestion from previous groups that low- and high-Ti basalts contain distinct Fe isotope signatures. This shows that on the Moon, high temperature processes can significantly change the Fe isotope composition of bulk mafic rocks at the planetary scale. This cannot result from simple equilibrium magmatic fractionation or assimilation of ilmenite given its Fe isotope fractionation factor, however. We conclude that another process, yet to be identified, is

  1. Low-Enriched Uranium Fuel Conversion Activities for the High Flux Isotope Reactor, Annual Report for FY 2011

    Energy Technology Data Exchange (ETDEWEB)

    Renfro, David G [ORNL; Cook, David Howard [ORNL; Freels, James D [ORNL; Griffin, Frederick P [ORNL; Ilas, Germina [ORNL; Sease, John D [ORNL; Chandler, David [ORNL

    2012-03-01

    This report describes progress made during FY11 in ORNL activities to support converting the High Flux Isotope Reactor (HFIR) from high-enriched uranium (HEU) fuel to low-enriched uranium (LEU) fuel. Conversion from HEU to LEU will require a change in fuel form from uranium oxide to a uranium-molybdenum (UMo) alloy. With both radial and axial contouring of the fuel foil and an increase in reactor power to 100 MW, calculations indicate that the HFIR can be operated with LEU fuel with no degradation in performance to users from the current levels achieved with HEU fuel. Studies are continuing to demonstrate that the fuel thermal safety margins can be preserved following conversion. Studies are also continuing to update other aspects of the reactor steady state operation and accident response for the effects of fuel conversion. Technical input has been provided to Oregon State University in support of their hydraulic testing program. The HFIR conversion schedule was revised and provided to the GTRI program. In addition to HFIR conversion activities, technical support was provided directly to the Fuel Fabrication Capability program manager.

  2. Thallium-isotopic compositions of euxinic sediments as a proxy for global manganese-oxide burial

    Science.gov (United States)

    Owens, Jeremy D.; Nielsen, Sune G.; Horner, Tristan J.; Ostrander, Chadlin M.; Peterson, Larry C.

    2017-09-01

    Thallium (Tl) isotopes are a new and potentially powerful paleoredox proxy that may track bottom water oxygen conditions based on the global burial flux of manganese oxides. Thallium has a residence time of ∼20 thousand years, which is longer than the ocean mixing time, and it has been inferred that modern oxic seawater is conservative with respect to both concentration and isotopes. Marine sources of Tl have nearly identical isotopic values. Therefore, the Tl sinks, adsorption onto manganese oxides and low temperature oceanic crust alteration (the dominant seawater output), are the primary controls of the seawater isotopic composition. For relatively short-term, ∼million years, redox events it is reasonable to assume that the dominant mechanism that alters the Tl isotopic composition of seawater is associated with manganese oxide burial because large variability in low temperature ocean crust alteration is controlled by long-term, multi-million years, average ocean crust production rates. This study presents new Tl isotope data for an open ocean transect in the South Atlantic, and depth transects for two euxinic basins (anoxic and free sulfide in the water column), the Cariaco Basin and Black Sea. The Tl isotopic signature of open ocean seawater in the South Atlantic was found to be homogeneous with ε205Tl = -6.0 ± 0.3 (±2 SD, n = 41) while oxic waters from Cariaco and the Black Sea are -5.6 and -2.2, respectively. Combined with existing data from the Pacific and Arctic Oceans, our Atlantic data establish the conservatism of Tl isotopes in the global ocean. In contrast, partially- and predominantly-restricted basins reveal Tl isotope differences that vary between open-ocean (-6) and continental material (-2) ε205Tl, scaling with the degree of restriction. Regardless of the differences between basins, Tl is quantitatively removed from their euxinic waters below the chemocline. The burial of Tl in euxinic sediments is estimated to be an order of magnitude

  3. The oxygen isotopic composition of the Sun inferred from captured solar wind.

    Science.gov (United States)

    McKeegan, K D; Kallio, A P A; Heber, V S; Jarzebinski, G; Mao, P H; Coath, C D; Kunihiro, T; Wiens, R C; Nordholt, J E; Moses, R W; Reisenfeld, D B; Jurewicz, A J G; Burnett, D S

    2011-06-24

    All planetary materials sampled thus far vary in their relative abundance of the major isotope of oxygen, (16)O, such that it has not been possible to define a primordial solar system composition. We measured the oxygen isotopic composition of solar wind captured and returned to Earth by NASA's Genesis mission. Our results demonstrate that the Sun is highly enriched in (16)O relative to the Earth, Moon, Mars, and bulk meteorites. Because the solar photosphere preserves the average isotopic composition of the solar system for elements heavier than lithium, we conclude that essentially all rocky materials in the inner solar system were enriched in (17)O and (18)O, relative to (16)O, by ~7%, probably via non-mass-dependent chemistry before accretion of the first planetesimals.

  4. Zinc isotope fractionation during mantle melting and constraints on the Zn isotope composition of Earth's upper mantle

    Science.gov (United States)

    Wang, Ze-Zhou; Liu, Sheng-Ao; Liu, Jingao; Huang, Jian; Xiao, Yan; Chu, Zhu-Yin; Zhao, Xin-Miao; Tang, Limei

    2017-02-01

    compositions of MORB. Therefore, preferential melting of spinel in the peridotites may account for the Zn isotopic difference between spinel peridotites and basalts. By contrast, the absence of Zn isotope fractionation between silicate minerals suggests that Zn isotopes are not significantly fractionated during partial melting of spinel-free garnet-facies mantle. If the studied non-metasomatized peridotites represent the refractory upper mantle, mass balance calculation shows that the depleted MORB mantle (DMM) has a δ66Zn value of +0.20 ± 0.05‰ (2SD), which is lighter than the primitive upper mantle (PUM) estimated in previous studies (+0.28 ± 0.05‰, 2SD, Chen et al., 2013b; +0.30 ± 0.07‰, 2SD, Doucet et al., 2016). This indicates that the Earth's upper mantle has a heterogeneous Zn isotopic composition vertically, which is probably due to shallow mantle melting processes.

  5. Variation in the Carbon Isotope Compositions of Phytoliths Across a Climate Gradient

    Science.gov (United States)

    Webb, E. A.; Longstaffe, F. J.

    2008-12-01

    The carbon isotope composition of plant organic matter within a single species may vary in response to changes in temperature, relative humidity, precipitation amount, altitude, nutrient availability, light levels and amount of canopy. All of these factors affect the rate of carbon assimilation during photosynthesis. Silica phytoliths, which form in the cells and intercellular spaces of terrestrial plants, occlude some of the plant's organic matrix. Carbon sequestered in phytoliths is protected from decay and may therefore be preserved in soils after most other plant material has decomposed. The carbon isotope composition of phytoliths may therefore have potential as an archive of climatic conditions during soil accumulation. In this study, the carbon isotope compositions of modern plant tissues and their phytoliths are compared for the C4 grass species Calamovilfa longifolia across the climate gradient of the North American prairies. The carbon isotope compositions of C. longifolia tissues ranged from -15 to -10 permil, with lower values being most typical of leaf tissues and with greater variability occurring in samples from lower latitudes. Carbonaceous compounds occluded in the phytoliths, by comparison, were depleted of carbon-13 by 5 to 15 permil relative to the tissues from the same plant. Understanding the causes of this offset, which is significantly larger and more variable than reported in previous studies, is necessary before the full potential of the carbon-isotope phytolith proxy can be realized.

  6. SIMSISH technique does not alter the apparent isotopic composition of bacterial cells.

    Directory of Open Access Journals (Sweden)

    Olivier Chapleur

    Full Text Available In order to identify the function of uncultured microorganisms in their environment, the SIMSISH method, combining in situ hybridization (ISH and nanoscale secondary ion mass spectrometry (nanoSIMS imaging, has been proposed to determine the quantitative uptake of specific labelled substrates by uncultured microbes at the single cell level. This technique requires the hybridization of rRNA targeted halogenated DNA probes on fixed and permeabilized microorganisms. Exogenous atoms are introduced into cells and endogenous atoms removed during the experimental procedures. Consequently differences between the original and the apparent isotopic composition of cells may occur. In the present study, the influence of the experimental procedures of SIMSISH on the isotopic composition of carbon in E. coli cells was evaluated with nanoSIMS and compared to elemental analyser-isotopic ratio mass spectrometer (EA-IRMS measurements. Our results show that fixation and hybridization have a very limited, reproducible and homogeneous influence on the isotopic composition of cells. Thereby, the SIMSISH procedure minimizes the contamination of the sample by exogenous atoms, thus providing a means to detect the phylogenetic identity and to measure precisely the carbon isotopic composition at the single cell level. This technique was successfully applied to a complex sample with double bromine - iodine labelling targeting a large group of bacteria and a specific archaea to evaluate their specific (13C uptake during labelled methanol anaerobic degradation.

  7. SIMSISH technique does not alter the apparent isotopic composition of bacterial cells.

    Science.gov (United States)

    Chapleur, Olivier; Wu, Ting-Di; Guerquin-Kern, Jean-Luc; Mazéas, Laurent; Bouchez, Théodore

    2013-01-01

    In order to identify the function of uncultured microorganisms in their environment, the SIMSISH method, combining in situ hybridization (ISH) and nanoscale secondary ion mass spectrometry (nanoSIMS) imaging, has been proposed to determine the quantitative uptake of specific labelled substrates by uncultured microbes at the single cell level. This technique requires the hybridization of rRNA targeted halogenated DNA probes on fixed and permeabilized microorganisms. Exogenous atoms are introduced into cells and endogenous atoms removed during the experimental procedures. Consequently differences between the original and the apparent isotopic composition of cells may occur. In the present study, the influence of the experimental procedures of SIMSISH on the isotopic composition of carbon in E. coli cells was evaluated with nanoSIMS and compared to elemental analyser-isotopic ratio mass spectrometer (EA-IRMS) measurements. Our results show that fixation and hybridization have a very limited, reproducible and homogeneous influence on the isotopic composition of cells. Thereby, the SIMSISH procedure minimizes the contamination of the sample by exogenous atoms, thus providing a means to detect the phylogenetic identity and to measure precisely the carbon isotopic composition at the single cell level. This technique was successfully applied to a complex sample with double bromine - iodine labelling targeting a large group of bacteria and a specific archaea to evaluate their specific (13)C uptake during labelled methanol anaerobic degradation.

  8. Spurious and functional correlates of the isotopic composition of a generalist across a tropical rainforest landscape

    Directory of Open Access Journals (Sweden)

    Poirson Evan K

    2009-11-01

    Full Text Available Abstract Background The isotopic composition of generalist consumers may be expected to vary in space as a consequence of spatial heterogeneity in isotope ratios, the abundance of resources, and competition. We aim to account for the spatial variation in the carbon and nitrogen isotopic composition of a generalized predatory species across a 500 ha. tropical rain forest landscape. We test competing models to account for relative influence of resources and competitors to the carbon and nitrogen isotopic enrichment of gypsy ants (Aphaenogaster araneoides, taking into account site-specific differences in baseline isotope ratios. Results We found that 75% of the variance in the fraction of 15N in the tissue of A. araneoides was accounted by one environmental parameter, the concentration of soil phosphorus. After taking into account landscape-scale variation in baseline resources, the most parsimonious model indicated that colony growth and leaf litter biomass accounted for nearly all of the variance in the δ15N discrimination factor, whereas the δ13C discrimination factor was most parsimoniously associated with colony size and the rate of leaf litter decomposition. There was no indication that competitor density or diversity accounted for spatial differences in the isotopic composition of gypsy ants. Conclusion Across a 500 ha. landscape, soil phosphorus accounted for spatial variation in baseline nitrogen isotope ratios. The δ15N discrimination factor of a higher order consumer in this food web was structured by bottom-up influences - the quantity and decomposition rate of leaf litter. Stable isotope studies on the trophic biology of consumers may benefit from explicit spatial design to account for edaphic properties that alter the baseline at fine spatial grains.

  9. The isotopic composition of methane in the stratosphere: high-altitude balloon sample measurements

    Directory of Open Access Journals (Sweden)

    T. Röckmann

    2011-12-01

    Full Text Available The isotopic composition of stratospheric methane has been determined on a large suite of air samples from stratospheric balloon flights covering subtropical to polar latitudes and a time period of 16 yr. 154 samples were analyzed for δ13C and 119 samples for δD, increasing the previously published dataset for balloon borne samples by an order of magnitude, and more than doubling the total available stratospheric data (including aircraft samples published to date. The samples also cover a large range in mixing ratio from tropospheric values near 1800 ppb down to only 250 ppb, and the strong isotope fractionation processes accordingly increase the isotopic composition up to δ13C = −14‰ and δD = +190‰, the largest enrichments observed for atmospheric CH4 so far. When analyzing and comparing kinetic isotope effects (KIEs derived from single balloon profiles, it is necessary to take into account the residence time in the stratosphere in combination with the observed mixing ratio and isotope trends in the troposphere, and the range of isotope values covered by the individual profile. The isotopic composition of CH4 in the stratosphere is affected by both chemical and dynamical processes. This severely hampers interpretation of the data in terms of the relative fractions of the three important sink mechanisms (reaction with OH, O(1D and Cl. It is shown that a formal sink partitioning using the measured data severely underestimates the fraction removed by OH, which is likely due to the insensitivity of the measurements to the kinetic fractionation in the lower stratosphere. Full quantitative interpretation of the CH4 isotope data in terms of the three sink reactions requires a global model.

  10. Carbon and oxygen isotopic composition of coal and carbon dioxide derived from laboratory coal combustion: A preliminary study

    Science.gov (United States)

    Warwick, Peter; Ruppert, Leslie F.

    2016-01-01

    The concentration of carbon dioxide (CO2) in the atmosphere has dramatically increased from the start of the industrial revolution in the mid-1700s to present levels exceeding 400 ppm. Carbon dioxide derived from fossil fuel combustion is a greenhouse gas and a major contributor to on-going climate change. Carbon and oxygen stable isotope geochemistry is a useful tool to help model and predict the contributions of anthropogenic sources of CO2 in the global carbon cycle. Surprisingly few studies have addressed the carbon and oxygen isotopic composition of CO2 derived from coal combustion. The goal of this study is to document the relationships between the carbon and oxygen isotope signatures of coal and signatures of the CO2 produced from laboratory coal combustion in atmospheric conditions.Six coal samples were selected that represent various geologic ages (Carboniferous to Tertiary) and coal ranks (lignite to bituminous). Duplicate splits of the six coal samples were ignited and partially combusted in the laboratory at atmospheric conditions. The resulting coal-combustion gases were collected and the molecular composition of the collected gases and isotopic analyses of δ13C of CO2, δ13C of CH4, and δ18O of CO2 were analysed by a commercial laboratory. Splits (~ 1 g) of the un-combusted dried ground coal samples were analyzed for δ13C and δ18O by the U.S. Geological Survey Reston Stable Isotope Laboratory.The major findings of this preliminary work indicate that the isotopic signatures of δ13C (relative to the Vienna Pee Dee Belemnite scale, VPDB) of CO2 resulting from coal combustion are similar to the δ13CVPDB signature of the bulk coal (− 28.46 to − 23.86 ‰) and are not similar to atmospheric δ13CVPDB of CO2 (~ − 8 ‰, see http://www.esrl.noaa.gov/gmd/outreach/isotopes/c13tellsus.html). The δ18O values of bulk coal are strongly correlated to the coal dry ash yields and appear to have little or no influence on the δ18O values of CO2

  11. Hydrogen isotope composition of mantle-derived mica megacryst from ion micro probe analysis

    Institute of Scientific and Technical Information of China (English)

    夏群科; 陈道公; 支霞臣

    1999-01-01

    The hydrogen isotope composition of a mantle-derived mica megacryst from Cenozoic basanite from NUshan, Anhui Province has been determined by ion micro probe. The results demonstrate that δD and water content of the megacryst were heterogeneous on the micro scale, which resulted from reaction with meteoric water after being brought to the surface. The primary δD of mica megacrysts was about-23‰, suggesting the recycled crustal materials in its source. By combining these values with those of other researchers, it is believed that the hydrogen isotope composition of the mantle is heterogeneous at least on the large scale.

  12. Optimization of fuels from waste composition with application of genetic algorithm.

    Science.gov (United States)

    Małgorzata, Wzorek

    2014-05-01

    The objective of this article is to elaborate a method to optimize the composition of the fuels from sewage sludge (PBS fuel - fuel based on sewage sludge and coal slime, PBM fuel - fuel based on sewage sludge and meat and bone meal, PBT fuel - fuel based on sewage sludge and sawdust). As a tool for an optimization procedure, the use of a genetic algorithm is proposed. The optimization task involves the maximization of mass fraction of sewage sludge in a fuel developed on the basis of quality-based criteria for the use as an alternative fuel used by the cement industry. The selection criteria of fuels composition concerned such parameters as: calorific value, content of chlorine, sulphur and heavy metals. Mathematical descriptions of fuel compositions and general forms of the genetic algorithm, as well as the obtained optimization results are presented. The results of this study indicate that the proposed genetic algorithm offers an optimization tool, which could be useful in the determination of the composition of fuels that are produced from waste.

  13. Sulfur isotopic composition of modern seafloor hydrothermal sediment and its geological significance

    Institute of Scientific and Technical Information of China (English)

    曾志刚; 李军; 蒋富清; 秦蕴珊; 翟世奎

    2002-01-01

    A total of 1 264 sulfur isotopic values for modem seafloor hydrothermel sediments from different hydrothermal fidds have been collected. On this basis, combining our sulfur isotpic data for surface hydrothermal sediments from the Jade hydrohtermal field in the Okinawa Trough and the TAG hydrothermal field in the Mid-Atlantic Ridge, respectively, and comparing the sulfur isotopic compositions and analyzing their sources of sulfur in seafloor hydrothermal sediments from different geologic-tectonic setting, the results show that: ( 1 ) sulfur isotopic values of sulfides and sulfates in modern seafloor hydrothermal sediments are concentrated in a narrow range, δ34S values of sulfides vary from l × 10-3 to 9 × 10- 3, with a mean of 4.5 × 10- 3 ( n = 1 042), δ34S values of sulfates vary from 19 × 10- 3 to 24× 10-3, with a mean of 21.3× 10-3 (n =217); (2) comparing the sulfur isotopic compositions of hydrothermal sediments from the sediment-hosted hydrothermal fields, the range of sulfur isotopic values for hydrothermal sediments from the sediment-free hydrothermal fields is narrow relatively; (3) the differences of sulfur isotopic compositions in sulfides from different hydrothermal fields show the differences in the sources of sulfur. The sulfur of hydrothermal sulfides in the sediment-free mid-ocean ridges is mainly from mid-ocean ridge basalt, and partially from the reduced seawater sulfate, and it is the result of partially reduced seawater sulfate mixed with basaltic sulfur. In the sediment-hosted nid-ocean ridges and the back-arc basins, the volcanics, the sediments and the organic matters also can offer their sulfur for forming hydrothermal sulfides; (4) the variations of sulfur isotopic compositions and the different sources of sulfur for hydrothermal sediments may be attributed to the various physical-chemical characteristics of hydrothermal fluids, the magmatic evolution and the different geologic-tectonic settings of seafloor hydrothermal systems.

  14. New insights to the use of ethanol in automotive fuels: a stable isotopic tracer for fossil- and bio-fuel combustion inputs to the atmosphere.

    Science.gov (United States)

    Giebel, Brian M; Swart, Peter K; Riemer, Daniel D

    2011-08-01

    Ethanol is currently receiving increased attention because of its use as a biofuel or fuel additive and because of its influence on air quality. We used stable isotopic ratio measurements of (13)C/(12)C in ethanol emitted from vehicles and a small group of tropical plants to establish ethanol's δ(13)C end-member signatures. Ethanol emitted in exhaust is distinctly different from that emitted by tropical plants and can serve as a unique stable isotopic tracer for transportation-related inputs to the atmosphere. Ethanol's unique isotopic signature in fuel is related to corn, a C4 plant and the primary source of ethanol in the U.S. We estimated a kinetic isotope effect (KIE) for ethanol's oxidative loss in the atmosphere and used previous assumptions with respect to the fractionation that may occur during wet and dry deposition. A small number of interpretive model calculations were used for source apportionment of ethanol and to understand the associated effects resulting from atmospheric removal. The models incorporated our end-member signatures and ambient measurements of ethanol, known or estimated source strengths and removal magnitudes, and estimated KIEs associated with atmospheric removal processes for ethanol. We compared transportation-related ethanol signatures to those from biogenic sources and used a set of ambient measurements to apportion each source contribution in Miami, Florida-a moderately polluted, but well ventilated urban location.

  15. The effect of phosphomonoesterases on the oxygen isotope composition of phosphate

    Science.gov (United States)

    von Sperber, Christian; Kries, Hajo; Tamburini, Federica; Bernasconi, Stefano M.; Frossard, Emmanuel

    2014-01-01

    Plants and microorganisms under phosphorus (P) stress release extracellular phosphatases as a strategy to acquire inorganic phosphate (Pi). These enzymes catalyze the hydrolysis of phosphoesters leading to a release of Pi. During the enzymatic hydrolysis an isotopic fractionation (ε) occurs leaving an imprint on the oxygen isotope composition of the released Pi which might be used to trace phosphorus in the environment. Therefore, enzymatic assays with acid phosphatases from wheat germ and potato tuber and alkaline phosphatase from Escherichia coli were prepared in order to determine the oxygen isotope fractionation caused by these enzymes. Adenosine 5‧ monophosphate and glycerol phosphate were used as substrates. The oxygen isotope fractionation caused by acid phosphatases is 20-30‰ smaller than for alkaline phosphatases, resulting in a difference of 5-7.5‰ in δ18O of Pi depending on the enzyme. We attribute the enzyme dependence of the isotopic fractionation to distinct reaction mechanisms of the two types of phosphatases. The observed difference is large enough to distinguish between the two enzymatic processes in environmental samples. These findings show that the oxygen isotope composition of Pi can be used to trace different enzymatic processes, offering an analytical tool that might contribute to a better understanding of the P-cycle in the environment.

  16. Isotopic analyses and calculation by use of JENDL-3.2 for high burn-up UO{sub 2} and MOX spent fuels

    Energy Technology Data Exchange (ETDEWEB)

    Sasahara, Akihiro; Matsumura, Tetsuo [Central Research Inst. of Electric Power Industry, Komae, Tokyo (Japan). Komae Research Lab.; Nicolaou, G.; Betti, M.; Walker, C.T.

    1997-03-01

    The post irradiation examinations (PIE) were carried out for high burn-up UO{sub 2} spent fuel (3.8%U235, average burn-up:60GWd/t) and mixed oxide (MOX) spent fuel (5.07%Pu, average burn-up:45GWd/t). The PIE includes, (a) isotopic analysis, (b) electron probe microanalysis (EPMA) in pellet cross section and so on. The results of isotopic analyses and EPMA were compared with ORIGEN2/82 and VIM-BURN calculation results. In VIM-BURN calculation, the nuclear data of actinides were proceeded from new data file, JENDL-3.2. The sensitivities of power history and moderator density to nuclides composition were investigated by VIM-BURN calculation and consequently power history mainly effected on Am241 and Am242m and moderator density effected on fissile nuclides. From EPMA results of U and Pu distribution in pellet, VIM-BURN calculation showed reasonable distribution in pellet cross section. (author)

  17. Carbon isotope composition of latex does not reflect temporal variations of photosynthetic carbon isotope discrimination in rubber trees (Hevea brasiliensis).

    Science.gov (United States)

    Kanpanon, Nicha; Kasemsap, Poonpipope; Thaler, Philippe; Kositsup, Boonthida; Gay, Frédéric; Lacote, Régis; Epron, Daniel

    2015-11-01

    Latex, the cytoplasm of laticiferous cells localized in the inner bark of rubber trees (Hevea brasiliensis Müll. Arg.), is collected by tapping the bark. Following tapping, latex flows out of the trunk and is regenerated, whereas in untapped trees, there is no natural exudation. It is still unknown whether the carbohydrates used for latex regeneration in tapped trees is coming from recent photosynthates or from stored carbohydrates, and in the former case, it is expected that latex carbon isotope composition of tapped trees will vary seasonally, whereas latex isotope composition of untapped trees will be more stable. Temporal variations of carbon isotope composition of trunk latex (δ(13)C-L), leaf soluble compounds (δ(13)C-S) and bulk leaf material (δ(13)C-B) collected from tapped and untapped 20-year-old trees were compared. A marked difference in δ(13)C-L was observed between tapped and untapped trees whatever the season. Trunk latex from tapped trees was more depleted (1.6‰ on average) with more variable δ(13)C values than those of untapped trees. δ(13)C-L was higher and more stable across seasons than δ(13)C-S and δ(13)C-B, with a maximum seasonal difference of 0.7‰ for tapped trees and 0.3‰ for untapped trees. δ(13)C-B was lower in tapped than in untapped trees, increasing from August (middle of the rainy season) to April (end of the dry season). Differences in δ(13)C-L and δ(13)C-B between tapped and untapped trees indicated that tapping affects the metabolism of both laticiferous cells and leaves. The lack of correlation between δ(13)C-L and δ(13)C-S suggests that recent photosynthates are mixed in the large pool of stored carbohydrates that are involved in latex regeneration after tapping.

  18. Coupled isotopes of plant wax and hemicellulose markers record information on relative humidity and isotopic composition of precipitation

    Directory of Open Access Journals (Sweden)

    M. Tuthorn

    2015-02-01

    Full Text Available The δ2H isotopic composition of leaf waxes is used increasingly for paleohydrological and -climate reconstructions. However, it is challenging to disentangle past changes in the isotopic composition of precipitation and changes in evapotranspirative enrichment of leaf water. We analyzed δ2H on n-alkanes and fatty acids in topsoils along a climate transect in Argentina, for which we had previously measured δ18O on plant-derived sugars. Our results indicate that leaf wax biomarker δ2H values (δ2Hlipids primarily reflect δ2Hsource water (precipitation, but are modulated by evapotranspirative enrichment. A mechanistic model is able to produce the main trends in δ2Hlipids along the transect, but seems to slightly underestimate evapotranspirative enrichment in arid regions and overestimate it in grass-dominated ecosystems. Furthermore, the (i coupling of the δ2Hlipid and δ18Osugar biomarker results and (ii application of biosynthetic fractionation factors allows calculating the δ2H-δ18O isotopic composition of leaf water along the transect. This also yields the deuterium excess (d excess of leaf water, which mainly reflects evapotranspirative enrichment, and can be used to model relative air humidity (RH. The high correlation of modeled (reconstructed based on biomarker results and measured RH, as well as the good agreement between modeled and actual δ2H and δ18O of precipitation along the transect lends support to the coupled δ2Hlipid and δ18Osugar biomarker approach for future paleoclimate research.

  19. Molybdenum Isotopic Composition of the Archean Mantle As Inferred from Studies of Komatiites

    Science.gov (United States)

    Greber, N. D.; Puchtel, I. S.; Nagler, T. F.; Mezger, K.

    2014-12-01

    Molybdenum isotopic composition has been shown to be a powerful tool in studies of planetary processes, e.g. estimating core formation temperatures [1,2]. However, Mo isotope compositions of terrestrial reservoirs are not well constrained. In order to better constrain the Mo isotopic composition of the early Earth's mantle, komatiites from four locations were analyzed for their Mo concentrations and isotopic compositions. Komatiites are particularly appropriate for this type of study because they formed by high degrees of partial melting of the mantle leading to a complete base metal sulfide removal from the residual mantle and the production of sulfur-undersaturated melts and thus a quantitative removal of Mo from the source into the melt. All samples, except for two strongly altered specimens specifically chosen to study the effects of secondary alteration, are very fresh having preserved most of their primary mineralogy. The Mo concentrations in komatiites range from 10 to 120 ng/g. Fresh komatiites have lighter δ98Mo (NIST SRM 3134 = 0.25‰, [3]) than altered samples. The estimated primary Mo isotope compositions of the studied komatiite melts range from 0.02 ± 0.16‰ to 0.19 ± 0.14‰ and are therefore indistinguishable within analytical uncertainty (2SD) from published values for chondritic meteorites (0.09 ± 0.04 ‰; 2SD; [2]) and lighter than the proposed average for Earth's continental crust (0.3 to 0.4‰ [4]). All data combined, although overlapping in errors, show a consistent trend of lighter δ98Mo and lower Mo concentrations in more melt-depleted mantle sources, indicating incompatible behaviour of Mo and preferential mobilization of heavy Mo isotopes during mantle melting. [1] Hin et al. (2013) EPSL, 379 [2] Burkhardt et al. (2014) EPSL, 391 [3] Nägler, et al. (2014) GGR, 38. [4] Voegelin et al. (2014) Lithos, 190-191.

  20. Diesel Surrogate Fuels for Engine Testing and Chemical-Kinetic Modeling: Compositions and Properties

    Science.gov (United States)

    Mueller, Charles J.; Cannella, William J.; Bays, J. Timothy; Bruno, Thomas J.; DeFabio, Kathy; Dettman, Heather D.; Gieleciak, Rafal M.; Huber, Marcia L.; Kweon, Chol-Bum; McConnell, Steven S.; Pitz, William J.; Ratcliff, Matthew A.

    2016-01-01

    The primary objectives of this work were to formulate, blend, and characterize a set of four ultralow-sulfur diesel surrogate fuels in quantities sufficient to enable their study in single-cylinder-engine and combustion-vessel experiments. The surrogate fuels feature increasing levels of compositional accuracy (i.e., increasing exactness in matching hydrocarbon structural characteristics) relative to the single target diesel fuel upon which the surrogate fuels are based. This approach was taken to assist in determining the minimum level of surrogate-fuel compositional accuracy that is required to adequately emulate the performance characteristics of the target fuel under different combustion modes. For each of the four surrogate fuels, an approximately 30 L batch was blended, and a number of the physical and chemical properties were measured. This work documents the surrogate-fuel creation process and the results of the property measurements. PMID:27330248

  1. Lead isotope studies of the Guerrero composite terrane, west-central Mexico: implications for ore genesis

    Science.gov (United States)

    Potra, Adriana; Macfarlane, Andrew W.

    2014-01-01

    New thermal ionization mass spectrometry and multi-collector inductively coupled plasma mass spectrometry Pb isotope analyses of three Cenozoic ores from the La Verde porphyry copper deposit located in the Zihuatanejo-Huetamo subterrane of the Guerrero composite terrane are presented and the metal sources are evaluated. Lead isotope ratios of 3 Cenozoic ores from the El Malacate and La Esmeralda porphyry copper deposits located in the Zihuatanejo-Huetamo subterrane and of 14 ores from the Zimapan and La Negra skarn deposits from the adjoining Sierra Madre terrane are also presented to look for systematic differences in the lead isotope trends and ore metal sources among the proposed exotic tectonostratigraphic terranes of southern Mexico. Comparison among the isotopic signatures of ores from the Sierra Madre terrane and distinct subterranes of the Guerrero terrane supports the idea that there is no direct correlation between the distinct suspect terranes of Mexico and the isotopic signatures of the associated Cenozoic ores. Rather, these Pb isotope patterns are interpreted to reflect increasing crustal contribution to mantle-derived magmas as the arc advanced eastward onto a progressively thicker continental crust. The lead isotope trend observed in Cenozoic ores is not recognized in the ores from Mesozoic volcanogenic massive sulfide and sedimentary exhalative deposits. The Mesozoic ores formed prior to the amalgamation of the Guerrero composite terrane to the continental margin, which took place during the Late Cretaceous, in intraoceanic island arc and intracontinental marginal basin settings, while the Tertiary deposits formed after this event in a continental arc setting. Lead isotope ratios of the Mesozoic and Cenozoic ores appear to reflect these differences in tectonic setting of ore formation. Most Pb isotope values of ores from the La Verde deposit (206Pb/204Pb = 18.674-18.719) are less radiogenic than those of the host igneous rocks, but plot within the

  2. Unexpected variations in the triple oxygen isotope composition of stratospheric carbon dioxide.

    Science.gov (United States)

    Wiegel, Aaron A; Cole, Amanda S; Hoag, Katherine J; Atlas, Elliot L; Schauffler, Sue M; Boering, Kristie A

    2013-10-29

    We report observations of stratospheric CO2 that reveal surprisingly large anomalous enrichments in (17)O that vary systematically with latitude, altitude, and season. The triple isotope slopes reached 1.95 ± 0.05(1σ) in the middle stratosphere and 2.22 ± 0.07 in the Arctic vortex versus 1.71 ± 0.03 from previous observations and a remarkable factor of 4 larger than the mass-dependent value of 0.52. Kinetics modeling of laboratory measurements of photochemical ozone-CO2 isotope exchange demonstrates that non-mass-dependent isotope effects in ozone formation alone quantitatively account for the (17)O anomaly in CO2 in the laboratory, resolving long-standing discrepancies between models and laboratory measurements. Model sensitivities to hypothetical mass-dependent isotope effects in reactions involving O3, O((1)D), or CO2 and to an empirically derived temperature dependence of the anomalous kinetic isotope effects in ozone formation then provide a conceptual framework for understanding the differences in the isotopic composition and the triple isotope slopes between the laboratory and the stratosphere and between different regions of the stratosphere. This understanding in turn provides a firmer foundation for the diverse biogeochemical and paleoclimate applications of (17)O anomalies in tropospheric CO2, O2, mineral sulfates, and fossil bones and teeth, which all derive from stratospheric CO2.

  3. Isotopic composition of Murchison organic compounds: Intramolecular carbon isotope fractionation of acetic acid. Simulation studies of cosmochemical organic syntheses

    Science.gov (United States)

    Yuen, G. U.; Cronin, J. R.; Blair, N. E.; Desmarais, D. J.; Chang, S.

    1991-01-01

    Recently, in our laboratories, samples of Murchison acetic acid were decarboxylated successfully and the carbon isotopic composition was measured for the methane released by this procedure. These analyses showed significant differences in C-13/C-12 ratios for the methyl and carboxyl carbons of the acetic acid molecule, strongly suggesting that more than one carbon source may be involved in the synthesis of the Murchison organic compounds. On the basis of this finding, laboratory model systems simulating cosmochemical synthesis are being studied, especially those processes capable of involving two or more starting carbon sources.

  4. Nafion®/H-ZSM-5 composite membranes with superior performance for direct methanol fuel cells

    NARCIS (Netherlands)

    Yildirim, Mustafa Hakan; Curos, Anna Roca; Motuzas, Julius; Julbe, Anne; Stamatialis, Dimitrios; Wessling, Matthias

    2009-01-01

    Solution cast composite direct methanol fuel cell membranes (DEZ) based on DE2020 Nafion® dispersion and in-house prepared H-ZSM-5 zeolites with different Si/Al ratios were prepared and thoroughly characterized for direct methanol fuel cell (DMFC) applications. All composite membranes have indeed l

  5. EXPERIMENTAL ASSESSMENT OF INFLUENCE OF COMPOSITE FUEL ON DIESEL OPERATION IN IDLE MODE

    OpenAIRE

    Godina, E.; Ukhanov, A.

    2014-01-01

    Unfavorable condition of the diesel engine is a separate idle mode, which is characterized by incomplete combustion, wasteful fuel consumption and increased emissions of harmful substances into the atmosphere. To evaluate the feasibility of using radish oil (RadishO) as the biological component of the diesel composite fuel (DCF) the experimental studies of tractor diesel engine D-243 at idle were conducted and the degree of the effect of different composition of radish and mineral fuel on eco...

  6. In situ observations of the isotopic composition of methane at the Cabauw tall tower site

    Science.gov (United States)

    Röckmann, Thomas; Eyer, Simon; van der Veen, Carina; Popa, Maria E.; Tuzson, Béla; Monteil, Guillaume; Houweling, Sander; Harris, Eliza; Brunner, Dominik; Fischer, Hubertus; Zazzeri, Giulia; Lowry, David; Nisbet, Euan G.; Brand, Willi A.; Necki, Jaroslav M.; Emmenegger, Lukas; Mohn, Joachim

    2016-08-01

    High-precision analyses of the isotopic composition of methane in ambient air can potentially be used to discriminate between different source categories. Due to the complexity of isotope ratio measurements, such analyses have generally been performed in the laboratory on air samples collected in the field. This poses a limitation on the temporal resolution at which the isotopic composition can be monitored with reasonable logistical effort. Here we present the performance of a dual isotope ratio mass spectrometric system (IRMS) and a quantum cascade laser absorption spectroscopy (QCLAS)-based technique for in situ analysis of the isotopic composition of methane under field conditions. Both systems were deployed at the Cabauw Experimental Site for Atmospheric Research (CESAR) in the Netherlands and performed in situ, high-frequency (approx. hourly) measurements for a period of more than 5 months. The IRMS and QCLAS instruments were in excellent agreement with a slight systematic offset of (+0.25 ± 0.04) ‰ for δ13C and (-4.3 ± 0.4) ‰ for δD. This was corrected for, yielding a combined dataset with more than 2500 measurements of both δ13C and δD. The high-precision and high-temporal-resolution dataset not only reveals the overwhelming contribution of isotopically depleted agricultural CH4 emissions from ruminants at the Cabauw site but also allows the identification of specific events with elevated contributions from more enriched sources such as natural gas and landfills. The final dataset was compared to model calculations using the global model TM5 and the mesoscale model FLEXPART-COSMO. The results of both models agree better with the measurements when the TNO-MACC emission inventory is used in the models than when the EDGAR inventory is used. This suggests that high-resolution isotope measurements have the potential to further constrain the methane budget when they are performed at multiple sites that are representative for the entire European domain.

  7. Method of producing exfoliated graphite composite compositions for fuel cell flow field plates

    Energy Technology Data Exchange (ETDEWEB)

    Zhamu, Aruna; Shi, Jinjun; Guo, Jiusheng; Jang, Bor Z

    2014-04-08

    A method of producing an electrically conductive composite composition, which is particularly useful for fuel cell bipolar plate applications. The method comprises: (a) providing a supply of expandable graphite powder; (b) providing a supply of a non-expandable powder component comprising a binder or matrix material; (c) blending the expandable graphite with the non-expandable powder component to form a powder mixture wherein the non-expandable powder component is in the amount of between 3% and 60% by weight based on the total weight of the powder mixture; (d) exposing the powder mixture to a temperature sufficient for exfoliating the expandable graphite to obtain a compressible mixture comprising expanded graphite worms and the non-expandable component; (e) compressing the compressible mixture at a pressure within the range of from about 5 psi to about 50,000 psi in predetermined directions into predetermined forms of cohered graphite composite compact; and (f) treating the so-formed cohered graphite composite to activate the binder or matrix material thereby promoting adhesion within the compact to produce the desired composite composition. Preferably, the non-expandable powder component further comprises an isotropy-promoting agent such as non-expandable graphite particles. Further preferably, step (e) comprises compressing the mixture in at least two directions. The method leads to composite plates with exceptionally high thickness-direction electrical conductivity.

  8. Method of producing exfoliated graphite composite compositions for fuel cell flow field plates

    Science.gov (United States)

    Zhamu, Aruna; Shi, Jinjun; Guo, Jiusheng; Jang, Bor Z

    2014-04-08

    A method of producing an electrically conductive composite composition, which is particularly useful for fuel cell bipolar plate applications. The method comprises: (a) providing a supply of expandable graphite powder; (b) providing a supply of a non-expandable powder component comprising a binder or matrix material; (c) blending the expandable graphite with the non-expandable powder component to form a powder mixture wherein the non-expandable powder component is in the amount of between 3% and 60% by weight based on the total weight of the powder mixture; (d) exposing the powder mixture to a temperature sufficient for exfoliating the expandable graphite to obtain a compressible mixture comprising expanded graphite worms and the non-expandable component; (e) compressing the compressible mixture at a pressure within the range of from about 5 psi to about 50,000 psi in predetermined directions into predetermined forms of cohered graphite composite compact; and (f) treating the so-formed cohered graphite composite to activate the binder or matrix material thereby promoting adhesion within the compact to produce the desired composite composition. Preferably, the non-expandable powder component further comprises an isotropy-promoting agent such as non-expandable graphite particles. Further preferably, step (e) comprises compressing the mixture in at least two directions. The method leads to composite plates with exceptionally high thickness-direction electrical conductivity.

  9. Multiple sulfur isotope composition of oxidized Samoan melts and the implications of a sulfur isotope 'mantle array' in chemical geodynamics

    Science.gov (United States)

    Labidi, J.; Cartigny, P.; Jackson, M. G.

    2015-05-01

    To better address how subducted protoliths drive the Earth's mantle sulfur isotope heterogeneity, we report new data for sulfur (S) and copper (Cu) abundances, S speciation and multiple S isotopic compositions (32S, 33S, 34S, 36S) in 15 fresh submarine basaltic glasses from the Samoan archipelago, which defines the enriched-mantle-2 (EM2) endmember. Bulk S abundances vary between 835 and 2279 ppm. About 17 ± 11% of sulfur is oxidized (S6+) but displays no consistent trend with bulk S abundance or any other geochemical tracer. The S isotope composition of both dissolved sulfide and sulfate yield homogeneous Δ33S and Δ36S values, within error of Canyon Diablo Troilite (CDT). In contrast, δ34S values are variable, ranging between +0.11 and +2.79‰ (±0.12‰ 1σ) for reduced sulfur, whereas oxidized sulfur values vary between +4.19 and +9.71‰ (±0.80‰, 1σ). Importantly, δ34S of the reduced S pool correlates with the 87Sr/86Sr ratios of the glasses, in a manner similar to that previously reported for South-Atlantic MORB, extending the trend to δ34S values up to + 2.79 ± 0.04 ‰, the highest value reported for undegassed oceanic basalts. As for EM-1 basalts from the South Atlantic ridge, the linear δ34S-87Sr/86Sr trend requires the EM-2 endmember to be relatively S-rich, and only sediments can account for these isotopic characteristics. While many authors argue that both the EM-1 and EM-2 mantle components record subduction of various protoliths (e.g. upper or lower continental crust, lithospheric mantle versus intra-metasomatized mantle, or others), it is proposed here that they primarily reflect sediment recycling. Their distinct Pb isotope variation can be accounted for by varying the proportion of S-poor recycled oceanic crust in the source of mantle plumes.

  10. Isotopic composition analysis and age dating of uranium samples by high resolution gamma ray spectrometry

    Science.gov (United States)

    Apostol, A. I.; Pantelica, A.; Sima, O.; Fugaru, V.

    2016-09-01

    Non-destructive methods were applied to determine the isotopic composition and the time elapsed since last chemical purification of nine uranium samples. The applied methods are based on measuring gamma and X radiations of uranium samples by high resolution low energy gamma spectrometric system with planar high purity germanium detector and low background gamma spectrometric system with coaxial high purity germanium detector. The "Multigroup γ-ray Analysis Method for Uranium" (MGAU) code was used for the precise determination of samples' isotopic composition. The age of the samples was determined from the isotopic ratio 214Bi/234U. This ratio was calculated from the analyzed spectra of each uranium sample, using relative detection efficiency. Special attention is paid to the coincidence summing corrections that have to be taken into account when performing this type of analysis. In addition, an alternative approach for the age determination using full energy peak efficiencies obtained by Monte Carlo simulations with the GESPECOR code is described.

  11. Isotopic Composition of Xenon in Petroleum from the Shell Bullwinkle Field

    Indian Academy of Sciences (India)

    J Nuzzo*; M Hyman; M W Rowe; Mnraoz; R L Palma; J Westrich

    2000-03-01

    We have measured the abundance and isotopic composition of xenon in petroleum samples from the Shell Bullwinkle Field off the coast of Louisiana. We used an oxidation and purification procedure designed to insure complete extraction and clean up of xenon from the petroleum. The xenon isotopic composition was found to be similar to the atmospheric value for one petroleum sample. While the results of the second sample suggest possible enrichment of the heavier isotopes, the errors associated with these excesses preclude a definitive statement to that effect. No monoisotopic enrichment in 129Xe was detected in either sample, the presence of which might have allowed us to deduce the petroleum age. Our results represent only the second xenon measurement from petroleum, and the concentrations are within the range of values published in the earlier report.

  12. Isotope composition and volume of Earth´s early oceans

    DEFF Research Database (Denmark)

    Pope, Emily Catherine; Bird, Dennis K.; Rosing, Minik Thorleif

    2012-01-01

    Oxygen and hydrogen isotope compositions of Earth´s seawater are controlled by volatile fluxes among mantle, lithospheric (oceanic and continental crust), and atmospheric reservoirs. Throughout geologic time the oxygen mass budget was likely conserved within these Earth system reservoirs......, but hydrogen´s was not, as it can escape to space. Isotopic properties of serpentine from the approximately 3.8 Ga Isua Supracrustal Belt in West Greenland are used to characterize hydrogen and oxygen isotope compositions of ancient seawater. Archaean oceans were depleted in deuterium [expressed as Î...... in Earth´s oceans. Our calculations predict that the oceans of early Earth were up to 26% more voluminous, and atmospheric CH4 and CO2 concentrations determined from limits on hydrogen escape to space are consistent with clement conditions on Archaean Earth....

  13. Abnormal composition of carbon isotopes in underground alkaline waters of Kuzbass

    Science.gov (United States)

    Shvartsev, S. L.; Lepokurova, O. E.; Ponomarchuk, V. A.; Domrocheva, E. V.; Sizikov, D. A.

    2016-08-01

    The first data on abnormally high δ13C values in hydrocarbonates (HCO 3 - ) dissolved in underground waters of coal deposits of Kuzbass (up to +30.9‰) are reported. It is shown that such an unusual isotope composition of waters results from the long, strictly directed interaction in the water-rock-gas-organic material system occurring under the conditions of hindered water exchange. Extensive fractionation of C isotopes is the result of the evolution of the water-rock-gas-coal system after penetration of infiltration waters into the coal deposits and their long interaction with all these components, rather than metamorphism of organic material upon its transformation into coal. With respect to such an approach, the isotope composition of dissolved C may indicate the duration of the evolution in the water-rock-gas-organic material system.

  14. Isotopic composition of carbon and oxygen of carbonates of oil and gas-bearing deposits of Western Siberia

    Energy Technology Data Exchange (ETDEWEB)

    Golyshev, S.I.; Cherepnin, A.V.; Rozhnev, A.N.

    1981-01-01

    There is measured the isotopic composition of carbon and oxygen in 129 samples of carbonates and carbonate cements of oil and gas-bearing Paleozoic and Mezozoic deposits of Western Siberia. The isotopic composition of samples of marine deposits varies from -1.2 to +6.1% for carbon and from 19.8 to 29.1% for oxygen and has a mean isotopic composition of 1.9 to 24.8%. Catagenetic processes lead to lightening of the isotopic composition of secondary carbonate on the average by 5% for carbon and 9% for oxygen. The most intense lightening of isotopic composition is observed in samples disposed near oil and gas deposits.

  15. Isotope variations of dissolved Zn in the Rio Grande watershed, USA: The role of adsorption on Zn isotope composition

    Science.gov (United States)

    Szynkiewicz, Anna; Borrok, David M.

    2016-01-01

    In order to better understand the factors influencing zinc (Zn) isotope composition in hydrological systems, we analyzed the δ66Zn of dissolved Zn in the streams and groundwater of the Upper and Middle Rio Grande watershed in Colorado and New Mexico, United States. The stream water samples have a wider variation of δ66Zn (-0.57 to + 0.41 ‰ relative to the JMC 3-0749-Lyon standard) than groundwater samples (-0.13 to + 0.12 ‰) and than samples from streams that are in close proximity to abandoned mining sites (+0.24 to + 0.40 ‰). Regional changes of bedrock geology, from primarily igneous rocks to primarily sedimentary rocks, have no resolvable effect on the δ66Zn of aqueous samples. Instead, an increase in water pH from 7.5 to 8.5 corresponds to a considerable decrease in the δ66Zn of dissolved Zn (R2 = - 0.37, p = 0.003, n = 22). Consequently, we link the observed Zn isotope variations to the process of adsorption of Zn onto suspended sediment and bedrock minerals (average Δ66Znadsorbed-dissolved = + 0.31 ‰). Our results are in good agreement with previous experimental and empirical studies suggesting that Zn adsorption leads to a residual dissolved pool enriched in light Zn isotopes. Given that anthropogenic Zn sources can also be responsible for lowering of δ66Zn, and may overlap with the pH/adsorption effect on δ66Zn, the latter needs to be carefully considered in future studies to differentiate between natural and anthropogenic factors influencing Zn isotopes in this and other aquatic systems.

  16. Calcium isotopic compositions as tracers of vegetation activity in boreal permafrost ecosystems (Kulingdakan watershed, Central Siberia)

    Science.gov (United States)

    Bagard, M.; Schmitt, A.; Chabaux, F. J.; Viers, J.; Pokrovsky, O. S.; Prokushkin, A. S.; Stille, P.; Dupré, B.

    2010-12-01

    In this work, we propose to investigate the geochemical potential of calcium isotopic fractionations in a forested boreal watershed to trace the impact of vegetation activity. This is the first study carried out in a geographical area characterized by deep and continuous permafrost. For this survey, we measured Ca and Sr isotopic compositions in the different compartments (stream waters, soil solutions, precipitations, rock, soils and soil leachates, vegetation) of a 4,100 ha Siberian watershed, the Kulingdakan watershed (Putorana Plateau, Central Siberia). Our results show that the activity of the vegetation is the only process that fractionates significantly calcium isotopes within the watershed. Indeed, Ca uptake by plants and its subsequent storage in larch tree organs favours 40Ca relatively to 44Ca. Vegetation decomposition releases light δ44/40Ca that affects calcium isotopic compositions of soil solution and soil exchangeable fractions. However, this biological impact is significant only for the South-facing slope of the watershed. Indeed, soil pools from the North-facing slope present no imprint of organic matter degradation in their δ44/40Ca signatures. Furthermore, the major difference between South- and North- facing slopes lies in the importance of the vegetation and its decomposition rate. Thus, we propose that in boreal permafrost areas with limited runoff, the available stock of biomass is critical to induce or not a significant vegetation impact on the calcium isotopic compositions in the soil-water system. As a consequence, the study of preserved calcium isotopic compositions in paleosoil exchangeable phases might bring relevant information on the evolution of biological activity at the watershed scale.

  17. Stable water isotopic composition of the Antarctic subglacial Lake Vostok: implications for understanding the lake's hydrology.

    Science.gov (United States)

    Ekaykin, Alexey A; Lipenkov, Vladimir Y; Kozachek, Anna V; Vladimirova, Diana O

    2016-01-01

    We estimated the stable isotopic composition of water from the subglacial Lake Vostok using two different sets of samples: (1) water frozen on the drill bit immediately after the first lake unsealing and (2) water frozen in the borehole after the unsealing and re-drilled one year later. The most reliable values of the water isotopic composition are: -59.0 ± 0.3 ‰ for oxygen-18, -455 ± 1 ‰ for deuterium and 17 ± 1 ‰ for d-excess. This result is also confirmed by the modelling of isotopic transformations in the water which froze in the borehole, and by a laboratory experiment simulating this process. A comparison of the newly obtained water isotopic composition with that of the lake ice (-56.2 ‰ for oxygen-18, -442.4 ‰ for deuterium and 7.2 ‰ for d-excess) leads to the conclusion that the lake ice is very likely formed in isotopic equilibrium with water. In turn, this means that ice is formed by a slow freezing without formation of frazil ice crystals and/or water pockets. This conclusion agrees well with the observed physical and chemical properties of the lake's accreted ice. However, our estimate of the water's isotopic composition is only valid for the upper water layer and may not be representative for the deeper layers of the lake, so further investigations are required.

  18. The carbon isotope composition of atmospheric CO 2 in Paris

    Science.gov (United States)

    Widory, David; Javoy, Marc

    2003-10-01

    One characteristic of air pollution in the urban environment is high CO 2 concentrations resulting from human activities. Determining the relative contributions of the different CO 2 sources can be addressed simply and elegantly by combining isotope and concentration measurements. Using this approach on atmospheric CO 2 samples collected in Paris, its suburbs and the open country provides fairly accurate conclusions. Our results show that air pollution within the first few metres above ground results basically from binary mixtures among which road traffic is the main contributor and, in particular, vehicles using unleaded gasoline (˜90% of the total). Heating sources, which account for 50% of the CO 2 input below the atmospheric inversion level, and vehicles using diesel contribute very little. Human respiration has a recognisable signature at street level under certain circumstances. The combined isotope and concentration analysis provides a sensitive tracer of local variations, even detecting the occasional prevalence of human respiration and the onset of actions in which natural gas is burnt. It also detects surprising inlets of 'clean air' (CO 2-wise) in the very centre of the city.

  19. The isotopic composition of methane in polar ice cores

    Science.gov (United States)

    Craig, H.; Chou, C. C.; Welhan, J. A.; Stevens, C. M.; Engelkemeir, A.

    1988-01-01

    Air bubbles in polar ice cores indicate that about 300 years ago the atmospheric mixing ratio of methane began to increase rapidly. Today the mixing ratio is about 1.7 parts per million by volume, and, having doubled once in the past several hundred years, it will double again in the next 60 years if current rates continue. Carbon isotope ratios in methane up to 350 years in age have been measured with as little as 25 kilograms of polar ice recovered in 4-meter-long ice-core segments. The data show that: (1) in situ microbiology or chemistry has not altered the ice-core methane concentrations, and (2) that the carbon-13 to carbon-12 ratio of atmospheric CH4 in ice from 100 years and 300 years ago was about 2 per mil lower than at present. Atmospheric methane has a rich spectrum of isotopic sources: the ice-core data indicate that anthropogenic burning of the earth's biomass is the principal cause of the recent C-13H4 enrichment, although other factors may also contribute.

  20. Diet control on carbon isotopic composition of land snail shell carbonate

    Institute of Scientific and Technical Information of China (English)

    LIU ZongXiu; GU ZhaoYan; WU NaiQin; XU Bing

    2007-01-01

    Carbon isotope compositions for both the carbonate shells and soft bodies (organic tissue) of living land snails collected mostly from the Loess Plateau, China have been measured. The result shows that δ13C values range from -13.1‰ to -4.3‰ for the aragonite shell samples and from -26.8‰ to -18.0‰ for the soft body samples. Although the shells are enriched in 13C relative to the bodies averagely by 14.2(±0.8)‰, the shell δ13Ca values are closely correlated to the body δ13Corg values, expressed as δ13Ca = 1.021 δ13Corg + 14.38 (R = 0.965; N = 31). This relationship indicates that δ13Ca is primarily a function of the isotopic composition of the snail diets since previous studies have proved that the snail body is the same as their food in carbon isotope composition. In other words, carbon isotope compo-sition of the carbonate shell can be used as a proxy to estimate the dietary 13C abundance of the land snails. The data also support that the 13C enrichment of the carbonate shells results mainly from the equilibrium fractionations between the metabolic CO2, HCO3- in the hemolymph and shell aragonite, and partially from kinetic fractionations when snail shells form during their activity.

  1. The atomic weight and isotopic composition of boron and their variation in nature

    Energy Technology Data Exchange (ETDEWEB)

    Holden, N.E.

    1993-08-01

    The boron isotopic composition and atomic weight value and their variation in nature are reviewed. Questions are raised about the previously recommended value and the uncertainty for the atomic weight. The problem of what constitutes an acceptable range for normal material and what should then be considered geologically exceptional is discussed. Recent measurements make some previous decisions in need of re-evaluation.

  2. Impact of metabolism and growth phase on the hydrogen isotopic composition of microbial fatty acids

    NARCIS (Netherlands)

    Heinzelmann, S.M.; Villanueva, L.; Sinke-Schoen, D.; Sinninghe Damsté, J.S.; Schouten, S.; Van der Meer, M.T.J.

    2015-01-01

    Microorganisms are involved in all elemental cycles and therefore it is important to study their metabolism in the natural environment. A recent technique to investigate this is the hydrogen isotopic composition of microbial fatty acids, i.e., heterotrophic microorganisms produce fatty acids enriche

  3. Interpretation of groundwater origin in the Velenje coal mine on the basis of isotope composition

    Directory of Open Access Journals (Sweden)

    Janko Urbanc

    2002-12-01

    Full Text Available The aim of the investigation was to determine the isotopic properties of cave waters from the Velenje coal mine and define the recharge areas of individual aquifers. With regard to the oxygen isotope composition, groundwater in the Velenje coal mine can beclassified into three types. Typical d18O values of the first type are around -9 ‰ and are found in surface waters in the vicinity of the mine, therefore it is supposed that these waters are recharged locally. The second type is represented mainly by waters from thelower part of the pliocene aquifer. The average oxygen composition of these waters is about -11 ‰. This isotope composition is considerably different from the isotope composition of recent waters from the mine’s vicinity, which leads to the conclusion that these are older, fossile waters. These waters also have a very high degree of mineralization and consequently conductivity. Waters of the third type have average δ18O values around -10 ‰ and originate mainly from triassic dolomites. These waters could be a mixture of recentand old waters, but it is also possible that they flow into the coal mine from the higher areas of Paški Kozjak.

  4. Soil moisture effects on the carbon isotope composition of soil respiration

    Science.gov (United States)

    Claire L. Phillips; Nick Nickerson; David Risk; Zachary E. Kayler; Chris Andersen; Alan Mix; Barbara J. Bond

    2010-01-01

    The carbon isotopic composition (δ13C) of recently assimilated plant carbon is known to depend on water-stress, caused either by low soil moisture or by low atmospheric humidity. Air humidity has also been shown to correlate with the δ13C of soil respiration, which suggests indirectly that recently fixed photosynthates...

  5. Single-molecule fluorescence autocorrelation experiments on pentacene : The dependence of intersystem crossing on isotopic composition

    NARCIS (Netherlands)

    Brouwer, A.C.J.; Köhler, J.; Oijen, A.M. van; Groenen, E.J.J.; Schmidt, J.

    1999-01-01

    Single pentacene molecules containing 13C or 1H in a pentacene-d14 doped p-terphenyl crystal have been studied by fluorescence autocorrelation. The triplet dynamics has been analyzed and a systematic dependence of the S1→T1 intersystem crossing rate on isotopic composition was found. This variation

  6. Validation of spent nuclear fuel nuclide composition data using percentage differences and detailed analysis

    Energy Technology Data Exchange (ETDEWEB)

    Kim, Man Cheol [Chung-Ang Univ., Seoul (Korea, Republic of). School of Energy Systems Engineering

    2017-06-15

    Nuclide composition data of spent nuclear fuels are important in many nuclear engineering applications. In reactor physics, nuclear reactor design requires the nuclide composition and the corresponding cross sections. In analyzing the radiological health effects of a severe accident on the public and the environment, the nuclide composition in the reactor inventory is among the important input data. Nuclide composition data need to be provided to analyze the possible environmental effects of a spent nuclear fuel repository. They will also be the basis for identifying the origin of unidentified spent nuclear fuels or radioactive materials.

  7. New approach to global barium cycle understanding: barium isotopic composition of marine carbonates and seawater.

    Science.gov (United States)

    Pretet, Chloé; Nägler, Thomas F.; Reynaud, Stéphanie; de Lange, Gert J.; Turpin, Mélanie; Immenhauser, Adrian; Böttcher, Michael E.; Samankassou, Elias

    2013-04-01

    In this communication we present the Ba isotope fractionation (delta137/134Ba) study on marine carbonates and seawater, initiated to gain a first order view of the marine Ba isotope cycle. A special focus is the question whether the nutrient type distribution of Ba in the water column, as well as different Ba sources, are reflected in Ba isotope ratios of carbonate archives. The approach ultimately aims to provide an improved Ba based paleonutrient proxy. The data set is composed of carbonates (micrites and limestone standard), coral skeleton and seawater (IAPSO standard and Mediterranean seawater). Part of the corals were cultured in monitored environments (CSM, Monaco) others originate from natural environments (shallow and warm water corals from the Bahamas/Florida and cold water corals from the Norwegian shelf). The analytical procedure includes the application of a 130Ba/135Ba double spike, a cation exchange column followed by isotope measurements on a Nu Instruments Multicollector ICP-MS. The Ba fractionation of the samples is compared to a Ba nitrate standard solution and a standard natural limestone BSC-CRM 393 (0.05 ± 0.04 ‰, 2SEM). No isotopic fractionation has been observed in the limestone standard and micrites (N=8) (-0.01 ± 0.04 ‰, 2SEM) compared to the Ba nitrate standard. On the contrary, coral skeletons show a significant positive fractionation (mean = 0.4 ± 0.05 ‰, 2 SEM). No significant difference was found between different cultured coral species. Thus no species-specific fractionation is identified within the same environmental conditions. Diagenetic influence on Ba isotopic composition was further tested on 5 natural samples with varying calcite to aragonite ratios (0 to 0.3). No significant effect was observed. Moreover, the Ba isotope composition seems independant from the Ba concentration in the studied coral skeleton, within our measurement resolution. Seawater isotopic composition (-0.05 ± 0.07 ‰, 2SD) is lighter than coral

  8. The Cl Isotope Composition of the Moon as evidence for an Anhydrous Mantle (Invited)

    Science.gov (United States)

    Sharp, Z. D.; Shearer, C., Jr.; McKeegan, K. D.; Barnes, J.; Wang, Y.

    2010-12-01

    The chlorine isotope composition of primitive terrestrial basalts and carbonaceous chondrites cover a narrow range centered around 0‰ with a total variation of ± 0.5‰. In contrast, the chlorine isotope composition of bulk samples and in situ ion microprobe analyses of lunar basalts and glasses cover a range of 25‰. Three possibilities were considered to explain the large spread: 1) initial isotopic heterogeneities, 2) devolatilization from solar wind/micrometeorite bombardment, 3) degassing under anhydrous conditions. The first of these possibilities is rejected because the Moon went through an magma ocean stage which would have homogenized any isotopic heterogeneities. To examine surface effects, we chose samples that have extremely different degrees of surface exposure. We find no correlation between the Cl isotope composition and surface exposure. We also conducted a laboratory experiment in which a thin film of NaCl was bombarded with a proton source for 24 hours with no change in Cl isotope composition. The third possibility is that the fractionation is explained by the anhydrous character of the Moon. On Earth, the volatiling Cl species is HCl. HCl is known to preferentially incorporate 37Cl relative to 35Cl due to the high bond strength of the molecule. This is offset by the higher translational velocity of H35Cl, so that overall, there is very little Cl isotope fractionation during degassing. We propose that lunar basalts were anhydrous and the volatile Cl species were metal chlorides, such as ZnCl2, NaCl, FeCl2, etc. The bond strength of metal chlorides and Cl dissolved in a basalt are similar, so that fractionation is caused mainly by volatilization, with the light isotopologue preferentially lost to the vapor phase. This idea is supported by the consistent lower Cl isotope ratios of water soluble salt fraction (~10 ‰ lower) and the lowest lunar Cl isotope values close to those of bulk Earth. The H content of lunar magmas must have been lower

  9. Oxygen and nitrogen isotopic composition of nitrate in commercial fertilizers, nitric acid, and reagent salts.

    Science.gov (United States)

    Michalski, Greg; Kolanowski, Michelle; Riha, Krystin M

    2015-01-01

    Nitrate is a key component of synthetic fertilizers that can be beneficial to crop production in agro-ecosystems, but can also cause damage to natural ecosystems if it is exported in large amounts. Stable isotopes, both oxygen and nitrogen, have been used to trace the sources and fate of nitrate in various ecosystems. However, the oxygen isotope composition of synthetic and organic nitrates is poorly constrained. Here, we present a study on the N and O isotope composition of nitrate-based fertilizers. The δ(15)N values of synthetic and natural nitrates were 0 ± 2 ‰ similar to the air N2 from which they are derived. The δ(18)O values of synthetic nitrates were 23 ± 3 ‰, similar to air O2, and natural nitrate fertilizer δ(18)O values (55 ± 5 ‰) were similar to those observed in atmospheric nitrate. The Δ(17)O values of synthetic fertilizer nitrate were approximately zero following a mass-dependent isotope relationship, while natural nitrate fertilizers had Δ(17)O values of 18 ± 2 ‰ similar to nitrate produced photochemically in the atmosphere. These narrow ranges of values can be used to assess the amount of nitrate arising from fertilizers in mixed systems where more than one nitrate source exists (soil, rivers, and lakes) using simple isotope mixing models.

  10. Impacts of microbial community composition on isotope fractionation during reductive dechlorination of tetrachloroethylene.

    Science.gov (United States)

    Dong, Yiran; Butler, Elizabeth C; Philp, R Paul; Krumholz, Lee R

    2011-04-01

    Isotope fractionation has been used with increasing frequency as a tool to quantify degradation of chlorinated aliphatic pollutants in the environment. The objective of this research was to determine if the electron donor present in enrichment cultures prepared from uncontaminated sediments influenced the extent of isotope fractionation of tetrachloroethylene (PCE), either directly, or through its influence on microbial community composition. Two PCE-degrading enrichment cultures were prepared from Duck Pond (DP) sediment and were incubated with formate (DPF) or H(2) (DPH) as electron donor. DPF and DPH were significantly different in both product distribution and extent of isotope fractionation. Chemical and isotope analyses indicated that electron donors did not directly affect the product distribution or the extent of isotope fractionation for PCE reductive dechlorination. Instead, restriction fragment length polymorphism (RFLP) and sequence analysis of the 16S rRNA clone libraries of DPF and DPH identified distinct microbial communities in each enrichment culture, suggesting that differences in microbial communities were responsible for distinct product distributions and isotope fractionation between the two cultures. A dominant species identified only in DPH was closely related to known dehalogenating species (Sulfurospirillum multivorans and Sulfurospirillum halorespirans) and may be responsible for PCE degradation in DPH. Our study suggests that different dechlorinators exist at the same site and can be preferentially stimulated by different electron donors, especially over the long-term (i.e., years), typical of in-situ ground water remediation.

  11. Evaluation of Isotopic Measurements and Burn-up Value of Sample GU3 of ARIANE Project

    Energy Technology Data Exchange (ETDEWEB)

    Tore, C.; Rodriguez Rivada, A.

    2014-07-01

    Estimation of the burn-up value of irradiated fuel and its isotopic composition are important for criticality analysis, spent fuel management and source term estimation. The practical way to estimate the irradiated fuel composition and burn.up value is calculation with validated code and nuclear data. Such validation of the neutronic codes and nuclear data requires the benchmarking with measured values. (Author)

  12. Sedimentary nitrate reduction and its effect on the N-isotopic composition of oceanic nitrate

    Science.gov (United States)

    Lehmann, M. F.; Sigman, D. M.; McCorkle, D. C.

    2005-12-01

    A prerequisite for assessing denitrification fluxes in a specific environment using water column nitrate N isotope ratios is the knowledge of the expressed N isotope effects of water column and/or benthic denitrification in this environment. Here, we aim at assessing the effects of benthic nitrogen cycling on the N isotopic composition of the oceanic nitrate pool in deep-sea sediments, which are believed to harbour a large portion of the global benthic denitrification. We report 15N/14N ratios of pore water nitrate in pelagic sediments from the deep Bering Sea, where benthic nitrate reduction has previously been identified as a significant sink of fixed nitrogen. Porewater profiles from multicores indicate strong 15N enrichment in porewater nitrate at all stations, as one goes deeper in the sediments and nitrate concentrations decrease (δ15N generally reached 25-35‰). Our data are consistent with variable biological isotope effect (ɛ) for dissimilatory nitrate reduction ranging between 13 to 30 ‰. A one-dimensional diffusion-reaction model including organic matter degradation, nitrification, and denitrification indicates that, although denitrification leads to a pore water nitrate pool that is enriched in 15N, N isotope fractionation is poorly expressed at the scale of sediment-water nitrate exchange, independent of whether sediments are a net sink or a net source of nitrate. The apparent nitrate isotope effect of sedimentary denitrification on nitrate in overlying waters is generally below 2‰, as a result of diffusive transport limitation into, and within, the sediments and/or the production of light nitrate during nitrification. Thus, our data suggest that the low expressed isotope effect of benthic denitrification observed previously in reactive shelf sediments also applies to deep-sea sediments. However, where ammonium fluxes out of the sediments, it is enriched in 15-N, and may ultimately lead to an N-isotopic enrichment of the water-column nitrate

  13. Influence of sea ice cover on evaporation and water vapour isotopic composition in the Arctic

    Science.gov (United States)

    Bonne, Jean-Louis; Werner, Martin; Meyer, Hanno; Kipfstuhl, Sepp; Rabe, Benjamin; Behrens, Melanie; Schönicke, Lutz; Steen-Larsen, Hans Christian

    2017-04-01

    Since July 2015, water stable isotopes (HDO and H218O) have been measured at two Arctic facilities: during the summer on board of the research vessel Polarstern, and year-round at the Siberian coastal site of Samoylov, situated in the Lena delta (N 72°22', E 126°29'), close to the Laptev Sea. In both places, the isotopic composition of water vapour is analysed continuously in surface air. Additional isotopic measurements are performed on a daily basis in ocean surface water samples taken on Polarstern and on an event basis from precipitation sampled in Samoylov. The two Polarstern summer campaigns cover a large region of the western Artic Ocean, including a one-month campaign in the central and eastern Arctic crossing the North Pole in September 2015, with very cold conditions (up to -20°C). Combining ocean and atmospheric observations from Polarstern allows an evaluation of local surface water evaporation and its isotopic fingerprint relative to the oceanic and meteorological conditions as well as the partial sea ice cover. In the central and eastern Arctic, a large area of complete sea ice cover also revealed a strong impact on the advected moisture above the ice cap under very cold conditions. A first year of Siberian observations at Samoylov depicted a large seasonal variability, with extremely dry and isotopically depleted winter values. Contrasted seasonal isotopic regimes might be utilized for identifying moisture sources changes in the region, such as ocean surface closure by sea ice, or freezing of the Lena River. Besides documenting the present meteorology and changes in the Arctic, our measurements will contribute to a better interpretation of regional paleoclimate records based on water isotopes and to the evaluation of climate models in the Arctic. A first model-data comparison of our measurements with simulation results by the isotope-enabled atmospheric general circulation model ECHAM5-wiso have revealed relevant model biases in the Arctic realm.

  14. Regulation of Isotopic Composition of Water - way of Improvement of Cosmonauts Drinking Water Functional Properties

    Science.gov (United States)

    Kulikova, Ekaterina; Utina, Dina; Vorozhtsova, Svetlana; Severyuhin, Yuri; Abrosimova, Anna; Sinyak, Yuri; Ivanov, Alexander

    The problem in providing drinking water to cosmonauts is solved - at this moment there is a task to improve the functional properties of the water. One of the perspectives of this trend is the use of light isotopic water. The animal studies have shown that long-term consumption of water with a depletion of deuterium and oxygen heavy isotopes accelerates the rise of mass non-irradiated mice, the phase fluctuations reducing or increasing hematological parameters were having adaptive nature. These fluctuations didn’t overcome values beyond the physiological norm of this type of animal. It is established that the therapeutic use of light isotopic water with 35 - 90 ppm in deuterium increases the survival of irradiated mice by an average of 30%, contributes to the preservation of irradiated animals body weight. Treatment of acute radiation sickness with light isotopic water stimulates hematopoietic recovery. At the same time, keeping mice drinking light isotopic water for 7 - 8 days before the irradiation (from 4 to 8.5 Gr) has no effect on the level of radio resistance. Longer keeping mice on light isotopic water, for 14 -21 days - reduction in life expectancy, animal mass, bone marrow cellularity and the level of white blood cells in irradiated animals is noted. It was established that keeping mice on light isotopic water for 14 days before exposure in experimental animals causes an increase in the mitotic index and the frequency of formation of aberrant mitosis after 24 hours of Co(60) gamma radiation in doses of 1 , 2, and 4 Gr. Thus, it is clear that the regulation of the isotopic composition of drinking water - way to improve its functional properties.

  15. The influence of traffic and wood combustion on the stable isotopic composition of carbon monoxide

    Directory of Open Access Journals (Sweden)

    M. Saurer

    2009-05-01

    Full Text Available Carbon monoxide in the atmosphere is originating from various combustion and oxidation processes. Recently, the proportion of CO resulting from the combustion of wood for domestic heating may have increased due to political measures promoting this renewable energy source. Here, we used the stable isotope composition of CO (δ13C and δ18O for the characterization of different CO sources in Switzerland, along with other indicators for traffic and wood combustion (NOx-concentration, aerosol light absorption at different wavelengths. We assessed diurnal variations of the isotopic composition of CO at 3 sites during winter: a village site dominated by domestic heating, a site close to a motorway and a rural site. The isotope ratios of wood combustion emissions were studied at a test facility, indicating significantly lower δ18O of CO from wood combustion compared to traffic emissions. At the village and the motorway site, we observed very pronounced diurnal δ18O-variations of CO with an amplitude of up to 8‰. Solving the isotope mass balance equation for three distinct sources (wood combustion, traffic, clean background air resulted in diurnal patterns consistent with other indicators for wood burning and traffic. The average night-time contribution of wood-burning to total CO was 70% at the village site, 49% at the motorway site and 29% at the rural site based on the isotope mass balance. The results, however, depend strongly on the pure source isotope values, which are not very well known. We therefore additionally applied a combined CO/NOx-isotope model for verification. Here, we separated the CO emissions into different sources based on distinct CO/NOx emissions ratios for wood combustion and traffic, and inserted this information in the isotope mass balance equation. Accordingly, a highly significant agreement between measured and calculated δ18

  16. Isotopic Composition of Gaseous Elemental Mercury (Hg0) at Various Sites in Japan

    Science.gov (United States)

    Yamakawa, A.; Moriya, K.; Yoshinaga, J.

    2015-12-01

    Mercury (Hg) is a toxic heavy metal, which exists in various chemical forms in the environmental system. In the atmosphere, Hg exists in three forms (Hg0(g), Hg+2(g), and Hg(p)). Hg0(g) is the dominant species of atmospheric Hg, accounting for >95% of the total Hg in the atmosphere. Because Hg0(g) is highly volatile and has limited solubility in water, it cannot be easily removed by wet or dry deposition processes. Therefore, the residence time of Hg0(g) in the atmosphere is relatively long (1 to 2 years), allowing long-range transport from mercury emission source(s). Conversely, Hg+2(g) and Hg(p) are effectively removed from the atmosphere through wet and dry depositions. The determination of mercury source attribution using quantitative data is challenging because Hg0(g) may be deposited on an area upon oxidation to Hg+2(g) and associated with aerosols and particulates to form Hg(p) while the global cycling of Hg0(g). Over the last decade, the development of analytical methods of highly precise Hg isotopic measurements demonstrated mass-dependent fractionation (MDF) and mass-independent fractionation (MIF) of Hg isotopes in environmental samples. For instance, MDF of Hg isotopes is thought to occur during various natural and industrial Hg transformations. MIF of Hg isotopes is observed during abiotic reduction, photochemical and non-photochemical, and physical and chemical processes. Such processes lead to differences in the Hg isotopic composition of different emission sources, both natural and anthropogenic, and atmospheric processes (i.e., transportation, oxidation/reduction, deposition, and reemission). Therefore, Hg isotopic compositions could be used to trace the sources and processes of atmospheric Hg. For securing the reliability and accuracy of atmospheric Hg isotope data, the methods of collection, pretreatment, and isotopic measurement for Hg0(g) were developed to obtain high recovery yield of samples with no Hg isotopic fractionation during each

  17. Chemical and Oxygen Isotopic Composition of Roman and Late Antique Glass from Northern Greece

    Directory of Open Access Journals (Sweden)

    Alberta Silvestri

    2017-01-01

    Full Text Available The present paper emphasizes the importance of measuring the oxygen isotopic and chemical compositions of ancient glass, in order to constrain some features such as age, raw materials, and production technologies and to identify the “fingerprint” of local productions. In this context, thirty-nine Roman and late Antique glass samples and eight chert samples from northern Greece were selected and analysed for their oxygen isotopic and chemical compositions. Results show that the majority of glass samples are produced using natron as flux and have δ18O values of about 15.5‰, plus or minus a few tenths of one per mil, suggesting that raw materials probably come from Levantine area. Four samples are heavily enriched in 18O, and their chemical composition clearly shows that they were made with soda plant ash as flux. Isotopic and chemical data of Greek chert samples support the hypothesis of local production of the above samples. About half of the glass samples have chemical compositions, which allow their age to be constrained to the late Antique period. For the remaining glass, similarities with literature compositional groups are reported and discussed.

  18. A non-terrestrial 16O-rich isotopic composition for the protosolar nebula.

    Science.gov (United States)

    Hashizume, Ko; Chaussidon, Marc

    2005-03-31

    The discovery in primitive components of meteorites of large oxygen isotopic variations that could not be attributed to mass-dependent fractionation effects has raised a fundamental question: what is the composition of the protosolar gas from which the host grains formed? This composition is probably preserved in the outer layers of the Sun, but the resolution of astronomical spectroscopic measurements is still too poor to be useful for comparison with planetary material. Here we report a precise determination of the oxygen isotopic composition of the solar wind from particles implanted in the outer hundreds of nanometres of metallic grains in the lunar regolith. These layers of the grains are enriched in 16O by >20 +/- 4 per thousand relative to the Earth, Mars and bulk meteorites, which implies the existence in the solar accretion disk of reactions--as yet unknown--that were able to change the 17O/16O and 18O/16O ratios in a way that was not dependent strictly on the mass of the isotope. Photochemical self-shielding of the CO gas irradiated by ultraviolet light may be one of these key processes, because it depends on the abundance of the isotopes, rather than their masses.

  19. The specific carbon isotopic compositions of branched and cyclic hydrocarbons from Fushun oil shale

    Institute of Scientific and Technical Information of China (English)

    DUAN Yi; WU Baoxiang; ZHENG Guodong; ZHANG Hui; ZHENG Chaoyang

    2004-01-01

    Various branched and cyclic hydrocarbons are isolated from the Fushun oil shale and their carbon isotopes are determined. The analytical results show that the branched and cyclic hydrocarbons are fully separated from n-alkanes by 5 A Molecular-sieve adduction using long time and cold solvent. The branched and cyclic hydrocarbon fraction obtained by this method is able to satisfy the analytic requests of GC-IRMS. The carbon isotopic compositions of these branched and cyclic hydrocarbons obtained from the sample indicate that they are derived from photoautotrophic algae, chemoautotrophic bacteria (-3.4‰ --39.0‰) and methanotrophic bacteria (-38.4‰--46.3‰). However the long-chain 2-methyl-branched alkanes indicate that their carbon isotopic compositions reflect biological origin from higher plants. The carbon isotopic composition of C30 4-methyl sterane (-22.1‰) is the heaviest in all studied ste- ranes, showing that the carbon source or growth condition for its precursor, dinoflagellate, may be different from that of regular steranes. The variation trend of δ13C values between isomers of hopanes shows that 13C-enriched precursors take precedence in process of their epimerization. Methanotrophic hopanes presented reveal the processes of strong transformation of organic matter and cycling of organic carbon in the water column and early diagenesis of oil shale.

  20. Stable carbon isotope composition of monoterpanes in essential oils and crude oils

    Institute of Scientific and Technical Information of China (English)

    2010-01-01

    Twenty-five monoterpanes from six types of essential oils and hydrogenated turpentine oil have been identified and their stable carbon isotope composition determined.Monoterpanes in essential oils sourced from terrestrial higher plants display a δ13C value in the range of-34‰-26‰,and mostly between-29‰ and-27‰.The δ13C value of any single monoterpane is very consistent in different essential oils.Acyclic monoterpanes show closer isotope composition between-28.6‰ and-26.2‰,with an average value of-27.7‰.In contrast,the isotope composition of cyclic monoterpanes is more scattered with an average value of-28.6‰.Isotopic fractionation with 13C enrichment has been observed during both artificial and geological hydrogenation of monoterpenoids to monoterpanes,and this is more obvious for the acyclic monoterpenoids.In addition to higher plants,acyclic monoterpane 2,6-dimethylheptane in crude oil can also be originated from other organic inputs.

  1. Preservation of Earth-forming events in the tungsten isotopic composition of modern flood basalts

    Science.gov (United States)

    Rizo, Hanika; Walker, Richard J.; Carlson, Richard W.; Horan, Mary F.; Mukhopadhyay, Sujoy; Manthos, Vicky; Francis, Don; Jackson, Matthew G.

    2016-05-01

    How much of Earth's compositional variation dates to processes that occurred during planet formation remains an unanswered question. High-precision tungsten isotopic data from rocks from two large igneous provinces, the North Atlantic Igneous Province and the Ontong Java Plateau, reveal preservation to the Phanerozoic of tungsten isotopic heterogeneities in the mantle. These heterogeneities, caused by the decay of hafnium-182 in mantle domains with high hafnium/tungsten ratios, were created during the first ~50 million years of solar system history, indicating that portions of the mantle that formed during Earth’s primary accretionary period have survived to the present.

  2. The Oxygen Isotopic Composition of MIL 090001: A CR2 Chondrite with Abundant Refractory Inclusions

    Science.gov (United States)

    Keller, Lindsay P.; McKeegan, K. D.; Sharp, Z. D.

    2012-01-01

    MIL 090001 is a large (>6 kg) carbonaceous chondrite that was classified as a member of the CV reduced subgroup (CVred) that was recovered during the 2009-2010 ANSMET field season [1]. Based on the abundance of refractory inclusions and the extent of aqueous alteration, Keller [2] suggested a CV2 classification. Here we report additional mineralogical and petrographic data for MIL 090001, its whole-rock oxygen isotopic composition and ion microprobe analyses of individual phases. The whole rock oxygen isotopic analyses show that MIL 090001 should be classified as a CR chondrite.

  3. On the iron isotope composition of Mars and volatile depletion in the terrestrial planets

    Science.gov (United States)

    Sossi, Paolo A.; Nebel, Oliver; Anand, Mahesh; Poitrasson, Franck

    2016-09-01

    Iron is the most abundant multivalent element in planetary reservoirs, meaning its isotope composition (expressed as δ57Fe) may record signatures of processes that occurred during the formation and subsequent differentiation of the terrestrial planets. Chondritic meteorites, putative constituents of the planets and remnants of undifferentiated inner solar system bodies, have δ57Fe ≈ 0 ‰; an isotopic signature shared with the Martian Shergottite-Nakhlite-Chassignite (SNC) suite of meteorites. The silicate Earth and Moon, as represented by basaltic rocks, are distinctly heavier, δ57Fe ≈ + 0.1 ‰. However, some authors have recently argued, on the basis of iron isotope measurements of abyssal peridotites, that the composition of the Earth's mantle is δ57Fe = + 0.04 ± 0.04 ‰, indistinguishable from the mean Martian value. To provide a more robust estimate for Mars, we present new high-precision iron isotope data on 17 SNC meteorites and 5 mineral separates. We find that the iron isotope compositions of Martian meteorites reflect igneous processes, with nakhlites and evolved shergottites displaying heavier δ57Fe (+ 0.05 ± 0.03 ‰), whereas MgO-rich rocks are lighter (δ57Fe ≈ - 0.01 ± 0.02 ‰). These systematics are controlled by the fractionation of olivine and pyroxene, attested to by the lighter isotope composition of pyroxene compared to whole rock nakhlites. Extrapolation of the δ57Fe SNC liquid line of descent to a putative Martian mantle yields a δ57Fe value lighter than its terrestrial counterpart, but indistinguishable from chondrites. Iron isotopes in planetary basalts of the inner solar system correlate positively with Fe/Mn and silicon isotopes. While Mars and IV-Vesta are undepleted in iron and accordingly have chondritic δ57Fe, the Earth experienced volatile depletion at low (1300 K) temperatures, likely at an early stage in the solar nebula, whereas additional post-nebular Fe loss is possible for the Moon and angrites.

  4. The stable isotopic composition of molecular hydrogen in the tropopause region probed by the CARIBIC aircraft

    Directory of Open Access Journals (Sweden)

    A. M. Batenburg

    2012-05-01

    Full Text Available More than 450 air samples that were collected in the upper troposphere – lower stratosphere (UTLS region by the CARIBIC aircraft (Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container have been analyzed for molecular hydrogen (H2 mixing ratios (χ(H2 and H2 isotopic composition (deuterium content, δD.

    More than 120 of the analyzed samples contained air from the lowermost stratosphere (LMS. These show that χ(H2 does not vary appreciably with O3-derived height above the thermal tropopause (TP, whereas δD does increase with height. The isotope enrichment is caused by H2 production and destruction processes that enrich the stratospheric H2 reservoir in deuterium (D; the exact shapes of the profiles are mainly determined by mixing of stratospheric with tropospheric air. Tight negative correlations are found between δD and the mixing ratios of methane (χ(CH4 and nitrous oxide (χ(N2O, as a result of the relatively long lifetimes of these three species. The correlations are described by δD[‰]=−0.35 · χ(CH4[ppb]+768 and δD[‰]=−1.90· χ(N2O[ppb]+745. These correlations are similar to previously published results and likely hold globally for the LMS.

    Samples that were collected from the Indian subcontinent up to 40° N before, during and after the summer monsoon season show no significant seasonal change in χ(H2, but δD is up to 12.3‰ lower in the July, August and September monsoon samples. This δD decrease is correlated with the χ(CH4 increase in these samples. The significant correlation with χ(CH4 and the absence of a perceptible χ(H2 increase that accompanies the δD decrease indicates that microbial production of

  5. A Record of Oceanic Lithium Isotope Composition for the Last 7Ma

    Science.gov (United States)

    Marriott, C. S.; Henderson, G. M.

    2003-12-01

    Continental weathering plays an important role in global climate change but has proved difficult to reconstruct for the past. New geological tools with which to assess the past rate and style of weathering are therefore urgently required. One such tool is Li isotope fractionation. Recent studies [1,2] have shown preferential release of 7Li into the aqueous phase and retention/adsorption of 6Li during weathering processes such as partial dissolution and secondary mineral formation. Lithium behaves conservatively in the oceans, with a residence time of ˜1Ma, so that a history of ocean Li isotope composition provides information about the average rate and style of global continental weathering on long timescales. The incorporation of lithium as a trace element in marine carbonates enables the construction of a record of oceanic Li-isotopic variation and is the focus of this work. Carbonate Li-isotope compositions are lighter than seawater by ˜8 per mil, but this fractionation is not temperature dependent. This has been demonstrated by measurement of Li isotopes in inorganically precipitated calcites (5-30° C) [3], in coralline aragonite (25-30° C) [3] and in benthic foraminifera Uvigerina (7-23° C). This lack of T-dependent fractionation suggests that the variation in the isotope composition of planktonic foraminifera will solely reflect changes in oceanic Li isotope composition, which in turn is strongly influence by changes in continental weathering. ODP site 758, located on the Ninetyeast Ridge in the Indian Ocean (5° N, 90° E; 2925m), was sampled at 2m intervals, over a depth corresponding to the last 7Ma, to produce 55 samples with a temporal resolution of approximately 130Ka. Site 758 is previously well studied with an existing chronology and high resolution Sr, O and Nd isotope data. Individual foram species in the core top were first investigated to assess inter-species fractionation effects. Down core lithium isotope variation was examined by

  6. Filled glass composites for sealing of solid oxide fuel cells.

    Energy Technology Data Exchange (ETDEWEB)

    Tandon, Rajan; Widgeon, Scarlett Joyce; Garino, Terry J.; Brochu, Mathieu; Gauntt, Bryan D.; Corral, Erica L.; Loehman, Ronald E.

    2009-04-01

    Glasses filled with ceramic or metallic powders have been developed for use as seals for solid oxide fuel cells (SOFC's) as part of the U.S. Department of Energy's Solid State Energy Conversion Alliance (SECA) Program. The composites of glass (alkaline earth-alumina-borate) and powders ({approx}20 vol% of yttria-stabilized zirconia or silver) were shown to form seals with SOFC materials at or below 900 C. The type and amount of powder were adjusted to optimize thermal expansion to match the SOFC materials and viscosity. Wetting studies indicated good wetting was achieved on the micro-scale and reaction studies indicated that the degree of reaction between the filled glasses and SOFC materials, including spinel-coated 441 stainless steel, at 750 C is acceptable. A test rig was developed for measuring strengths of seals cycled between room temperature and typical SOFC operating temperatures. Our measurements showed that many of the 410 SS to 410 SS seals, made using silver-filled glass composites, were hermetic at 0.2 MPa (2 atm.) of pressure and that seals that leaked could be resealed by briefly heating them to 900 C. Seal strength measurements at elevated temperature (up to 950 C), measured using a second apparatus that we developed, indicated that seals maintained 0.02 MPa (0.2 atm.) overpressures for 30 min at 750 C with no leakage. Finally, the volatility of the borate component of sealing glasses under SOFC operational conditions was studied using weight loss measurements and found by extrapolation to be less than 5% for the projected SOFC lifetime.

  7. Temperature and Oxygen Isotope Composition of The Ediacaran Ocean: Constraints From Clumped Isotope Carbonate Thermometry

    Science.gov (United States)

    Bonifacie, M.; Eiler, J. M.; Fike, D. A.

    2008-12-01

    The temperature and chemical variations of the early oceans on Earth are highly debated, particularly for periods associated with significant evolutionary change and/or extinction. The temperature of past oceans has been estimated based on conventional carbonate-water and/or silicate-water stable oxygen isotope thermometry. Precambrian carbonates and silicates both exhibit a long-term secular trend of increasing δ18O values with decreasing age. This trend has been used to support two opposite - though related - interpretations: the Earth's oceans gradually cooled over the course of the Proterozoic eon, from a maximum of ~ 60-90°C at ~ 2.5Ga (and were, on average, relatively warm during much of the Paleozoic era) [1]. This interpretation has been supported by Si-isotope proxies and the thermal tolerances of proteins in various classes of microbial organisms [2-3]. Alternatively, the δ18O value of the oceans has gradually increased through time [4-5], and mean Earth surface temperatures varied over a narrow range similar to modern conditions. In other terms, one either assumes an ocean of constant δ18O and infers that climate varied dramatically, or vise versa. Finally, it is possible that post- depositional processes (e.g., diagenesis, burial metamorphism, weathering) has modified the δ18O values of all or most Precambrian sedimentary carbonates and silicates, overprinting any paleoclimatic variations. Carbonate 'clumped isotope' thermometry provides a new way to independently test these hypotheses because it allows one to determine the apparent growth temperatures of carbonate minerals based on their abundances of 13C-18O bonds, as reflected by the 'Δ47' value of CO2 extracted by phosphoric acid digestion [6]. This method is thermodynamically based and independent of the δ18O of water from which the carbonate grew. We will report the initial results of measurements of 'Δ47 for a suite of carbonates from the Sultanate of Oman. This Ediacaran age (~ 635 to

  8. Change of Sm-Nd isotope composition during weathering of till

    Science.gov (United States)

    Öhlander, Björn; Ingri, Johan; Land, Magnus; Schöberg, Hans

    2000-03-01

    Weathering of till in northern Sweden results in the formation of well-developed spodosols. The till is dominated by 1.9-1.8 Ga granitic material. The REE are among the elements most strongly depleted during weathering, and the loss of REE from the E-horizon decreases as the atomic number increases. To study if weathering leads to a change of the Nd isotope composition, we have analysed the Nd isotopic composition of the various horizons including living plants and humus of two profiles of weathered till (typic haplocryods) in northern Sweden. As much as between 65.6 and 75.3% of the Sm and Nd in the fraction has been lost from the E-horizon, and between 32.5 and 54.7% from the B-horizon. Nd has been lost to a slightly greater extent than Sm. The two C-horizon samples have ɛ Nd(0) values of -22.1 and -23.2. Corresponding E-horizon values are -18.1 and -20.2. The B-horizon values are intermediate between the values of the E and C horizons. It is concluded that the weathering leads to a change in the Sm/Nd ratio resulting in a change of the Sm-Nd isotope composition. The plant and humus samples deviate even more from the unweathered till. For one station the results could be interpreted as if the Sm and Nd taken up by the plants had similar isotope characteristics as the amounts of these elements released by weathering in the E-horizon. For the other station it is probable that the Nd isotope composition of the organic samples is dominated by Nd released by till weathering which, however, is mixed with another Nd-source, possibly an airborne component. The explanation to the change of isotope compostion in the till is that a larger proportion of the Nd released by weathering is released from minerals with a lower Sm/Nd ratio than the bulk soil, compared with the amount released from minerals with a higher Sm/Nd ratio. Although the various REE-carrying minerals had the same initial Nd isotopic composition, 1.8-1.9 Ga of decay of 147Sm to 143Nd has resulted in a

  9. Predicting the Isotopic Composition of Subduction-Filtered Subducted Oceanic Crust and Sediment

    Science.gov (United States)

    White, W. M.

    2010-12-01

    The chemical and isotopic character of mantle plumes, which produce oceanic island volcanoes, are widely thought to reflect the presence of recycled oceanic crust and sediment. Isotopic systematics suggest the “cycle time” for this process is 1 Ga or longer, but it should be possible to use a simple mass balance approach to discern how the presently operating subduction zone filter affects the ratios of radioactive parent to radiogenic daughter isotopes. Simple uniformitarian assumptions can then be used to predict the present isotopic composition of anciently subducted lithosphere. Our underlying assumption in deciphering the subduction zone filter is that the flux of an element into the deep mantle is simply equal to the flux of element into the subduction zone less the flux of that element into subduction zone magmas. The former is readily calculated from published data. The latter can be calculated by estimating parental magma compositions, arc accretion rates, and the assumption that arc magma compositions differ from MORB only because of material derived from subducting crust and sediment. Using this approach for 8 intra-oceanic subduction zones, we find 73% of Th and Pb, 79% of U, 80% of Rb and Sr, 93% of Nd and 98% of Sm survive the subduction zone filter. The subduction zone filter systematically increases Sm/Nd ratios in all subduction zones, but the effect is small, with a weighted mean increase of 1.5%. The effect of subduction is to decrease the Sm/Nd of the mantle, but only slightly. The effect of subduction is to increase the Rb/Sr of the mantle, but the subduction zone filter does not have a systematic effect on Rb/Sr ratios: it significantly increases in Rb/Sr in 3 subduction zones and significantly decreases it in one; the weighted mean shows no significant change. The effect of the subduction zone filter on U/Pb is also not systematic. U/Pb ratios in the mantle fluxes are bimodal, with values equal to or lower than the bulk Earth value in 4

  10. Determining the isotopic compositions of uranium and fission products in radioactive environmental microsamples using laser ablation ICP-MS with multiple ion counters

    Energy Technology Data Exchange (ETDEWEB)

    Boulyga, Sergei F.; Prohaska, Thomas [University of Natural Resources and Applied Life Sciences, Department of Chemistry, Division of Analytical Chemistry-VIRIS Laboratory, Vienna (Austria)

    2008-01-15

    published results from the bulk analysis of contaminated samples originating from the vicinity of Chernobyl. Thus, the {sup 235}U/{sup 238}U ratios measured in ten microsamples varied in the range from 0.0073 (corresponding to the natural uranium isotopic composition) to 0.023 (corresponding to initial {sup 235}U enrichment in reactor fuel). An inverse correlation was observed between the {sup 236}U/{sup 238}U and {sup 235}U/{sup 238}U isotope ratios, except in the case of one sample with natural uranium. The heterogeneity of the uranium isotope composition is attributed to the different burn-up grades of uranium in the fuel rods from which the microsamples originated. (orig.)

  11. Stable isotope and chemical compositions of European and Australasian ciders as a guide to authenticity.

    Science.gov (United States)

    Carter, James F; Yates, Hans S A; Tinggi, Ujang

    2015-01-28

    This paper presents a data set derived from the analysis of bottled and canned ciders that may be used for comparison with suspected counterfeit or substitute products. Isotopic analysis of the solid residues from ciders (predominantly sugar) provided a means to determine the addition of C4 plant sugars. The added sugars were found to comprise cane sugar, high-fructose corn syrup, glucose, or combinations. The majority of ciders from Australia and New Zealand were found to contain significant amounts of added sugar, which provided a limited means to distinguish these ciders from European ciders. The hydrogen and oxygen isotopic compositions of the whole ciders (predominantly water) were shown to be controlled by two factors, the water available to the parent plant and evaporation. Analysis of data derived from both isotopic and chemical analysis of ciders provided a means to discriminate between regions and countries of manufacture.

  12. Modelling the regional climate and isotopic composition of Svalbard precipitation using REMOiso

    DEFF Research Database (Denmark)

    Divine..[], D.V.; Sjolte, Jesper; Isaksson, E.;

    2011-01-01

    Simulations of a regional (approx. 50 km resolution) circulation model REMOiso with embedded stable water isotope module covering the period 1958-2001 are compared with the two instrumental climate and four isotope series (d18O) from western Svalbard. We examine the data from ice cores drilled...... on Svalbard ice caps in 1997 (Lomonosovfonna, 1250 m asl) and 2005 (Holtedahlfonna, 1150 m asl) and the GNIP series from Ny-angstrom lesund and Isfjord Radio. The surface air temperature (SAT) and precipitation data from Longyearbyen and Ny-angstrom lesund are used to assess the skill of the model...... in reproducing the local climate. The model successfully captures the climate variations on the daily to multidecadal times scales although it tends to systematically underestimate the winter SAT. Analysis suggests that REMOiso performs better at simulating isotope compositions of precipitation in the winter...

  13. Carbon isotope composition of low molecular weight hydrocarbons and monocarboxylic acids from Murchison meteorite

    Science.gov (United States)

    Yuen, G.; Blair, N.; Des Marais, D. J.; Chang, S.

    1984-01-01

    Carbon isotopic compositions have been measured for individual hydrocarbons and monocarboxylic acids from the Murchison meteorite, a C2 carbonaceous chondrite which fell in Australia in 1969. With few exceptions, notably benzene, the volatile products are substantially isotopically heavier than their terrestrial counterparts, signifying their extraterrestrial origin. For both classes of compounds, the ratio of C-13 to C-12 decreases with increasing carbon number in a roughly parallel manner, and each carboxylic acid exhibits a higher isotopic ratio than the hydrocarbon containing the same number of carbon atoms. These trends are consistent with the kinetically controlled synthesis of higher homologues from lower ones. The results suggest the possibility that the production mechanisms for hydrocarbons and carboxylic acids may be similar, and impose constraints on the identity of the reactant species.

  14. Absolute isotopic composition and atomic weight of neodymium using thermal ionization mass spectrometry.

    Science.gov (United States)

    Zhao, Motian; Zhou, Tao; Wang, Jun; Lu, Hai; Fang, Xiang; Guo, Chunhua; Li, Qiuli; Li, Chaofeng

    2005-01-01

    Synthetic mixtures prepared gravimetrically from highly enriched isotopes of neodymium in the form of oxides of well-defined purity were used to calibrate a thermal ionization mass spectrometer. A new error analysis was applied to calculate the final uncertainty of the atomic weight value. Measurements on natural neodymium samples yielded an absolute isotopic composition of 27.153(19) atomic percent (at.%) 142Nd, 12.173(18) at.% 143Nd, 23.798(12) at.% 144Nd, 8.293(7) at.% 145Nd, 17.189(17) at.% 146Nd, 5.756(8) at.% 148Nd, and 5.638(9) at.% 150Nd, and the atomic weight of neodymium as 144.2415(13), with uncertainties given on the basis of 95% confidence limits. No isotopic fractionation was found in terrestrial neodymium materials.

  15. Stable isotope study of a new chondrichthyan fauna (Kimmeridgian, Porrentruy, Swiss Jura): an unusual freshwater-influenced isotopic composition for the hybodont shark Asteracanthus

    Science.gov (United States)

    Leuzinger, L.; Kocsis, L.; Billon-Bruyat, J.-P.; Spezzaferri, S.; Vennemann, T.

    2015-12-01

    Chondrichthyan teeth (sharks, rays, and chimaeras) are mineralized in isotopic equilibrium with the surrounding water, and parameters such as water temperature and salinity can be inferred from the oxygen isotopic composition (δ18Op) of their bioapatite. We analysed a new chondrichthyan assemblage, as well as teeth from bony fish (Pycnodontiformes). All specimens are from Kimmeridgian coastal marine deposits of the Swiss Jura (vicinity of Porrentruy, Ajoie district, NW Switzerland). While the overall faunal composition and the isotopic composition of bony fish are generally consistent with marine conditions, unusually low δ18Op values were measured for the hybodont shark Asteracanthus. These values are also lower compared to previously published data from older European Jurassic localities. Additional analyses on material from Solothurn (Kimmeridgian, NW Switzerland) also have comparable, low-18O isotopic compositions for Asteracanthus. The data are hence interpreted to represent a so far unique, freshwater-influenced isotopic composition for this shark that is classically considered a marine genus. While reproduction in freshwater or brackish realms is established for other hybodonts, a similar behaviour for Asteracanthus is proposed here. Regular excursions into lower salinity waters can be linked to the age of the deposits and correspond to an ecological adaptation, most likely driven by the Kimmeridgian transgression and by the competition of the hybodont shark Asteracanthus with the rapidly diversifying neoselachians (modern sharks).

  16. Stable isotope study of a new chondrichthyan fauna (Kimmeridgian, Porrentruy, Swiss Jura: an unusual freshwater-influenced isotopic composition for the hybodont shark Asteracanthus

    Directory of Open Access Journals (Sweden)

    L. Leuzinger

    2015-08-01

    Full Text Available Chondrichthyan teeth (sharks, rays and chimaeras are mineralised in isotopic equilibrium with the surrounding water, and parameters such as water temperature and salinity can be inferred from the oxygen isotopic composition (δ18Op of their bioapatite. We analysed a new chondrichthyan assemblage, as well as teeth from bony fish (Pycnodontiformes. All specimens are from Kimmeridgian coastal marine deposits of the Swiss Jura (vicinity of Porrentruy, Ajoie district, NW Switzerland. While the overall faunal composition and the isotopic composition of bony fish are consistent with marine conditions, unusually low δ18Op values were measured for the hybodont shark Asteracanthus. These values are also lower compared to previously published data from older European Jurassic localities. Additional analyses on material from Solothurn (Kimmeridgian, NW Switzerland also have comparable, low-18O isotopic compositions for Asteracanthus. The data are hence interpreted to represent a so far unique, freshwater-influenced isotopic composition for this shark that is classically considered as a marine genus. While reproduction in freshwater or brackish realms is established for other hybodonts, a similar behaviour for Asteracanthus is proposed here. Regular excursions into lower salinity waters can be linked to the age of the deposits and correspond to an ecological adaptation, most likely driven by the Kimmeridgian transgression and by the competition of the primitive shark Asteracanthus with the rapidly diversifying neoselachians (modern sharks.

  17. Experimental assessment of environmental influences on the stable isotopic composition of Daphnia pulicaria and their ephippia

    Science.gov (United States)

    Schilder, J.; Tellenbach, C.; Möst, M.; Spaak, P.; van Hardenbroek, M.; Wooller, M. J.; Heiri, O.

    2015-02-01

    The stable isotopic composition of fossil resting eggs (ephippia) of Daphnia spp. is being used to reconstruct past environmental conditions in lake ecosystems. However, the underlying assumption that the stable isotopic composition of the ephippia reflects the stable isotopic composition of the parent Daphnia, of their diet and of the environmental water have yet to be confirmed in a controlled experimental setting. We performed experiments with Daphnia pulicaria cultures, which included a control treatment conducted at 12 °C in filtered lake water and with a diet of fresh algae, and three treatments in which we manipulated the stable carbon isotopic composition (δ13C value) of the algae, stable oxygen isotopic composition (δ18O value) of the water, and the water temperature, respectively. The stable nitrogen isotopic composition (δ15N value) of the algae was similar for all treatments. At 12 °C, differences in algal δ13C values and in δ18O values of water are reflected in those of Daphnia. The differences between ephippia and Daphnia stable isotope ratios were similar in the different treatments (δ13C: + 0.2 ± 0.4‰ (SD); δ15N: -1.6 ± 0.4‰; δ18O: -0.9 ± 0.4‰) indicating that changes in dietary δ13C and δ18O values of water are passed on to these fossilizing structures. A higher water temperature (20 °C) resulted in lower δ13C values in Daphnia and ephippia than in the other treatments with the same food source and in a minor change in the difference between δ13C values of ephippia and Daphnia (to -1.3 ± 0.3‰). This may have been due to microbial processes or increased algal respiration rates in the experimental containers, which may not affect Daphnia in natural environments. There was no significant difference in the offset between δ18O and δ15N values of ephippia and Daphnia between the 12 °C and 20 °C treatments, but the δ18O values of Daphnia and ephippia were on average 1.2‰ lower at 20 °C compared with 12 °C. We conclude

  18. Lead isotopic compositions of common arsenical pesticides used in New England

    Science.gov (United States)

    Ayuso, Robert; Foley, Nora; Robinson, Gilpin; Wandless, Gregory; Dillingham, Jeremy

    2004-01-01

    The three most important arsenical pesticides and herbicides that were extensively used on apple, blueberry, and potato crops in New England from mid-1800s to recent times are lead arsenate, calcium arsenate, and sodium arsenate. Lead arsenate was probably the most heavily used of the arsenical pesticides until it was banned in 1988. Other metal-arsenic pesticides were also used but in lesser amounts. A recent report identified areas in New England where arsenical pesticides were used extensively (Robinson and Ayuso, 2004). On the basis of factor analysis of metal concentrations in stream sediment samples, a positive correlation with pesticide use was shown in regions having stream sediment sample populations that contained concentrations of high arsenic and lead. Lead isotope compositions of stream sediments from areas with heavy use of the pesticides could not be entirely explained by lead originating from rock sulfides and their weathering products. An industrial lead contribution (mostly from atmospheric deposition of lead) was suggested in general to explain the lead isotopic distributions of the stream sediments that could not be accounted for by the natural lead in the environment. We concluded that when agricultural land previously contaminated with arsenical pesticides is urbanized, pesticide residues in the soils and stream sediments could be released into the groundwater. No lead isotopic data characterizing the compositions of pesticides were available for comparison. We have determined the lead isotopic compositions of commonly used pesticides in New England, such as lead arsenate, sodium metaarsenite, and calcium arsenate, in order to assist in future isotopic comparisons and to better establish anthropogenic sources of Pb and As. New data are also presented for copper acetoarsenite (or Paris green), methyl arsonic acid and methane arsonic acid, as well as for arsanilic acid, all of which are used as feed additives to promote swine and poultry growth

  19. Soil Drying Effects on the Carbon Isotope Composition of Soil Respiration

    Science.gov (United States)

    Phillips, C. L.; Nickerson, N.; Risk, D.; Kayler, Z. E.; Rugh, W.; Mix, A. C.; Bond, B. J.

    2008-12-01

    Stable isotopes are used widely as a tool for determining sources of carbon (C) fluxes in ecosystem C studies. Environmental factors that change over time, such as moisture, can create dynamic changes in the isotopic composition of C assimilated by plants, and offers a unique opportunity to distinguish fast- responding plant C from slower-responding soil C pools, which under steady-state conditions may be too similar isotopically to partition. Monitoring the isotopic composition of soil respiration over a period of changing moisture conditions is potentially a useful approach for characterizing plant contributions to soil respiration. But this partitioning hinges on the assumption that any change in the isotopic signature of soil respiration is solely due to recent photosynthetic discrimination, and that post-photosynthetic processes, such as microbial respiration, do not discriminate as moisture decreases. The purpose of the present study is to test the assumption that δ13CO2 from microbial respiration remains static as soil dries. We conducted a series of greenhouse experiments employing different techniques to isolate microbial respiration from root respiration. The first involves removing roots from soil, and showed that when roots are present, respiration from dry soil is enriched in 13C relative to moist soil, but when roots are absent, respiration is isotopically similar from moist and dry soils. This indicates that rhizospheric respiration changes isotopically with moisture whereas soil microbial respiration does not. In contrast, a second experiment in which soil columns without plants were monitored as they dried, showed respiration from very dry soil to be enriched by 8‰ relative to moist soil. However, simulations with an isotopologue-based soil gas diffusion model demonstrate that at least a portion of the apparent enrichment is due to non-steady state gas transport processes. Careful sampling methodologies which prevent or account for non

  20. REE characteristics and Pb, Sr and Nd isotopic compositions of steel plant emissions.

    Science.gov (United States)

    Geagea, M Lahd; Stille, P; Millet, M; Perrone, Th

    2007-02-01

    A comprehensive Pb-Sr-Nd isotope and REE tracer study of atmospheric trace metal pollution by a steel plant situated to the north of the urban communities of Strasbourg (France) and Kehl (Germany) has been performed using tree barks as biomonitors. The 206Pb/207Pb and 208Pb/207Pb isotopic ratios of the steel plant's filter dust are similar to values found in dust of waste incinerators. The 87Sr/86Sr ratio is similar to present-day ratios of Phanerozoic or Precambrian granitic rocks. The 143Nd/144Nd isotopic composition is very low and corresponds to an (Nd) value of -17.5. Such a low value is characteristic of old Precambrian granitic rocks and banded iron formations. Thus, this low (Nd) value might point to the origin of the iron necessary for the steel production. The fact, that this isotopic composition does not occur in crustal rocks of Western Central Europe makes the Nd isotope ratio a powerful tool to trace steel plants atmospheric emissions. The rare earth element (REE) distribution pattern of the steel plant's filter dust shows very specific fractionations like La and Nd enrichments which are traceable in tree barks over a distance of 4 km. The Pb, Sr and Nd isotope ratios not only enable the steel plant's emissions to be traced in a north-easterly direction, along the principal wind pathway but also enables the interference of this emission at 4 km NE from the steel plant with another atmospheric component originating from the Strasbourg Rhine harbour to be identified.

  1. Detection of phosphohydrolytic enzyme activity through the oxygen isotope composition of dissolved phosphate

    Science.gov (United States)

    Colman, A. S.

    2016-02-01

    Phosphohydrolytic enzymes play an important role in phosphorus remineralization. As they release phosphate (Pi) from various organophosphorus compounds, these enzymes facilitate the transfer of oxygen atoms from water to the phosphoryl moieties. Most such enzymatic reactions impart a significant isotopic fractionation to the oxygen transferred. If this reaction occurs within a cell, then the resultant oxygen isotope signal is overprinted by continued recycling of the Pi. However, if this reaction occurs extracellularly, then the isotopic signal will be preserved until the Pi is transported back into a cell. Thus, the oxygen isotope composition of Pi (δ18Op) in an aquatic ecosystem can serve as a useful indicator of the mechanisms by which P is remineralized. We develop a time-dependent model illustrating the sensitivity of the δ18O of dissolved phosphate to various modes of P remineralization. The model is informed by cell lysis experiments that reveal the relative proportions of P­i that are directly liberated from cytosol vs. regenerated from co-liberated dissolved organic phosphorus compounds via extracellular hydrolysis. By incorporating both cellular uptake and release fluxes of P, we show that the degree of isotopic disequilibrium in an aquatic ecosystem can be a strong indicator of P remineralization mode. Apparent oxygen isotope equilibrium between Pi and water arises in this model as a steady-state scenario in which fractionation upon cellular uptake of Pi counterbalances the hydrolytic source flux of disequilibrated Pi. Low and high rates of extracellular phosphohydrolase activity are shown to produce steady-state δ18Op values that are respectively above or below thermodynamic equilibrium compositions.

  2. Diamond growth history from in situ measurement of Pb and S isotopic compositions of sulfide inclusions

    Science.gov (United States)

    Rudnick, Roberta L.; Eldridge, C. Stewart; Bulanova, Galina P.

    1993-01-01

    In a continuing effort to understand crust-mantle dynamics, we have determined the S and Pb isotopic compositions of mantle sulfides encapsulated within diamonds from under the Siberian craton and compared these results to those of previously investigated African counterparts. Because diamond inclusions are isolated from exchange with surrounding mantle, they may preserve the history of diamond growth and act as direct tracers of the origins of mantle materials. Study of these inclusions may thus offer the best chance of recognizing global-scale interaction between Earth's crust and mantle. Although δ34S values of the Siberian sulfides do not deviate significantly from the mantle value of 0‰ ± 3‰, Pb isotopic compositions are highly variable. Pb isotopic compositions of sulfides from peridotitic suite diamonds generally plot near the terrestrial Pb growth curve, with model ages ranging between 0 and 2 Ga, whereas sulfides from eclogitic suite diamonds have radiogenic compositions, plotting beyond the growth curve. These results, which are similar to those for sulfides in African diamonds, suggest that the sulfides from eclogitic suite diamonds were derived from a source with an unusually high U/Pb ratio and may indicate a common process (such as subduction of crystal materials into the mantle) operating beneath Africa and Siberia. The absence of extremely radiogenic Pb in sulfides from eclogite xenoliths suggests that the radiogenic material from which eclogitic suite diamonds grew was a transient feature of the mantle, associated with diamond growth. The ultimate origin of this high U/Pb signature, however, remains enigmatic. Large variations in Pb isotopic composition of sulfides from different zones in a single peridotitic suite diamond document (1) crystallization of the diamond's core near 2.0 Ga, (2) growth of its outer zone in an environment with a high U/Pb ratio similar to the growth environment of eclogitic suite diamonds, and (3) growth of the

  3. Isotope composition of winter precipitation and snow cover in the foothills of the Altai

    Directory of Open Access Journals (Sweden)

    N. S. Malygina

    2017-01-01

    Full Text Available Over the past three decades, several general circulation models of the atmosphere and ocean (atmospheric and oceanic general circulation models  – GCMs have been improved by modeling the hydrological cycle with the use of isotopologues (isotopes of water HDO and H2 18O. Input parameters for the GCM models taking into account changes in the isotope composition of atmospheric precipitation were, above all, the results obtained by the network GNIP – Global Network of Isotopes in Precipitation. At different times, on the vast territory of Russia there were only about 40 simultaneously functioning stations where the sampling of atmospheric precipitation was performed. In this study we present the results of the isotope composition of samples taken on the foothills of the Altai during two winter seasons of 2014/15 and 2015/16. Values of the isotope composition of precipitation changed in a wide range and their maximum fluctuations were 25, 202 and 18‰ for δ18О, dexc and δD, respectively. The weighted-mean values of δ18О and δD of the precipitation analyzed for the above two seasons were close to each other (−21.1 and −158.1‰ for the first season and −21.1 and −161.9‰ for the second one, while dexc values differed significantly. The comparison of the results of isotope analysis of the snow cover integral samples with the corresponding in the time interval the weighted-mean values of precipitation showed high consistency. However, despite the similarity of values of δ18О and δD, calculated for precipitation and snow cover, and the results, interpolated in IsoMAP (from data of the GNIP stations for 1960–2010, the dexc values were close to mean annual values of IsoMAP for only the second winter season. According to the trajectory analysis (the HYSPLIT model, the revealed differences between both, the seasons, and the long-term average values of IsoMAP, were associated with a change of main regions where the air masses

  4. Hf isotopic compositions of the standard zircons for U-Pb dating

    Institute of Scientific and Technical Information of China (English)

    XU Ping; WU Fuyuan; XIE Liewen; YANG Yueheng

    2004-01-01

    Using the newly published Yb isotopic abundances and the mass bias relationship between Yb and Hf, we carried out an analysis of Hf isotopes in the standard zircon 91500 by means of 193 nm laser attached to Neptune multi-collector ICP-MS (LA-MC-ICPMS). The obtained Hf isotopic data, in either in situ or line scan modes, are not only identical for different spot sizes, but also are consistent with previously published results obtained on TIMS or other MC-ICPMS machines within errors. This indicates that it is possible to obtain reliable 176Hf/177Hf isotopic ratios for zircon in either in situ or line scan conditions on LA-MC-ICPMS machine, and the applied procedures in our study for elemental interfering correction are appropriate for the purpose of acquiring satisfactory accuracy for Hf isotope analyses. The Hf isotopic compositions of four zircon standards in high spatial resolution U-Pb dating, 91500, CZ3,CN92-1 and TEMORA, are measured, respectively. The obtained 176Hf/177Hf ratios are 0.282316+4 (n = 34, 2σ) for 91500, 0.281704±6 (n = 16, 2σ) for CZ3, 0.282200±6 (n = 20,2σ-) for CN92-1 and 0.282684±14 (n = 24, 2σ) for TEMORA,respectively, with 176Lu/177Hf ratios of ~0.00031, 0.000036,0.00083 and 0.00127. Zircons 91500 and CZ3 show narrower variations in 176Hf/177Hf and 176Lu/177Hf ratios than those of zircons CN92-1 and TEMORA, and thus are appropriate standards for the Hf isotope analysis.

  5. Controlling Factors of the Stable Isotope Composition in the Precipitation of Islamabad, Pakistan

    Directory of Open Access Journals (Sweden)

    Shakir Hussain

    2015-01-01

    Full Text Available Significant temporal variations in δ18O and deuterium isotopes were found in the rainfall water of Islamabad, Pakistan, over a 15-year period (1992–2006. The data were obtained from the International Atomic Energy Agency/Global Network of Isotopes in Precipitation (IAEA/GNIP database, and statistical correlations were investigated. In particular, this study provides the first detailed analysis of GNIP data for Islamabad. Both dry (1999-2000 and wet years (1994, 1997, and 2000 were chosen to investigate the correlations between precipitation amount, vapor flux, and temperature. We observed obvious differences between the dry and wet years and among seasons as well. Long-term features in the isotope composition agreed with the global meteorological water line, whereas short-term values followed rainfall amounts; that is, a total of 72% of the precipitation’s isotopic signature was dependent on the rainfall amount, and temperature controlled 73% of the isotopic features during October to May. The lower d-excess values were attributed to conditions during the spring season and a secondary evaporation boost during dry years; precipitation originating from the Mediterranean Sea showed high d-excess values. Overall, the results of this study contribute to the understanding of precipitation variations and their association with water vapor transport over Islamabad, Pakistan.

  6. Neoproterozoic variations in the C-isotopic composition of seawater: stratigraphic and biogeochemical implications.

    Science.gov (United States)

    Kaufman, A J; Knoll, A H

    1995-01-01

    The recent proliferation of stratigraphic studies of delta 13C variation in carbonates and organic C in later Neoproterozoic and basal Cambrian successions (approximately 850-530 Ma) indicates a strong oscillating trend in the C-isotopic composition of surface seawater. Alone, this trend does not adequately characterize discrete intervals in Neoproterozoic time. However, integrated with the vectorial signals provided by fossils and Sr-isotopic variations, C isotope chemostratigraphy facilitates the interbasinal correlation of later Neoproterozoic successions. Results of these studies are evaluated in terms of four stratigraphic intervals: (1) the Precambrian/Cambrian boundary, (2) the post-Varanger terminal Proterozoic, (3) the late Cryogenian, and (4) the early Cryogenian. Where biostratigraphic or radiometric data constrain the age of Neoproterozoic sedimentary sequences, secular variations in C and Sr isotopes can provide a level of stratigraphic resolution exceeding that provided by fossils alone. Isotopic data place strong constraints on the chemical evolution of seawater, linking it to major tectonic and paleoclimatic events. They also provide a biogeochemical framework for the understanding of the initial radiation of macroscopic metazoans, which is associated stratigraphically, and perhaps causally, with a global increase in the burial of organic C and a concomitant rise of atmospheric O2.

  7. Anthropogenic Pb input into Bohai Bay, China: Evidence from stable Pb isotopic compositions in sediments

    Science.gov (United States)

    Hu, Ningjing; Huang, Peng

    2016-04-01

    Anthropogenic Pb input into Bohai Bay, China: Evidence from stable Pb isotopic compositions in sediments Hu Ning-jinga, Huang Pengb,, Liu Ji-huaa, a First Institute of Oceanography, State Oceanic Administration, Qingdao 266061, China b Institute of Oceanology, Chinese Academy of Sciences, Qingdao 266071, China To investigate the source of Pb within Bohai Bay, Pb concentrations and Pb isotopic compositions (204Pb, 206Pb, 207Pb, and 208Pb) of surface sediments in this area were determined. The Pb concentration in this bay varied widely from 6.9 to 39.2 μg/g (average: 21.8 ± 7.8 μg/g), and the Pb isotopic compositions ranged from 0.8338 to 0.8864 (average: 2.0997 ± 0.0180) for 208Pb/206Pb and from 2.0797 to 2.1531 (average: 0.8477 ± 0.0135) for 207Pb/206Pb, presenting in three distinct clusters. The Pb isotopic ratios of sediments from the northeastern (NE zone) and northwestern (NW zone) coastal areas were significantly influenced by anthropogenic sources such as coal combustion and automobile emission. In sediments from the central and southern Bohai Bay (C-S zone); however, Pb mainly originated from the Yellow River catchment, as a result of lithogenic sediment (from rock weathering) accumulation. The Pb isotopic ratios further indicate that, apart from riverine inputs, the neighboring large-scale ports and aerosols significantly contributed to the anthropogenic Pb contained in these sediments. Pb contamination in the Haihe and Luanhe river mouths as well as in the regions near ports is also suggested from anthropogenic enrichment factors. As cities and ports continue to develop around Bohai Bay, a long-term extensive sewage monitoring program is highly recommended.

  8. Stable chromium isotopic composition of meteorites and metal-silicate experiments: Implications for fractionation during core formation

    Science.gov (United States)

    Bonnand, P.; Williams, H. M.; Parkinson, I. J.; Wood, B. J.; Halliday, A. N.

    2016-02-01

    We present new mass independent and mass dependent Cr isotope compositions for meteorites measured by double spike thermal ionisation mass spectrometry. Small differences in both mass independent 53Cr and 54Cr relative to the Bulk Silicate Earth are reported and are very similar to previously published values. Carbonaceous chondrites are characterised by an excess in 54Cr compared to ordinary and enstatite chondrites which make mass independent Cr isotopes a useful tool for distinguishing between meteoritic groups. Mass dependent stable Cr isotope compositions for the same samples are also reported. Carbonaceous and ordinary chondrites are identical within uncertainty with average δ53 Cr values of - 0.118 ± 0.040 ‰ and - 0.143 ± 0.074 ‰ respectively. The heaviest isotope compositions are recorded by an enstatite chondrite and a CO carbonaceous chondrite, both of which have relatively reduced chemical compositions implying some stable Cr isotope fractionation related to redox processes in the circumstellar disk. The average δ53 Cr values for chondrites are within error of the estimate for the Bulk Silicate Earth (BSE) also determined by double spiking. The lack of isotopic difference between chondritic material and the BSE provides evidence that Cr isotopes were not fractionated during core formation on Earth. A series of high-pressure experiments was also carried out to investigate stable Cr isotope fractionation between metal and silicate and no demonstrable fractionation was observed, consistent with our meteorites data. Mass dependent Cr isotope data for achondrites suggest that Cr isotopes are fractionated during magmatic differentiation and therefore further work is required to constrain the Cr isotopic compositions of the mantles of Vesta and Mars.

  9. Reconstructing Cambro-Ordovician Seawater Composition using Clumped Isotope Paleothermometry on Calcitic and Phosphatic Brachiopods

    Science.gov (United States)

    Bergmann, K.; Robles, M.; Finnegan, S.; Hughes, N. C.; Eiler, J. M.; Fischer, W. W.

    2012-12-01

    A secular increase in δ18O values of marine fossils through early Phanerozoic time raises questions about the evolution of climate and the water cycle. This pattern suggests two end-member hypotheses 1) surface temperatures during early Paleozoic time were very warm, in excess of 40°C (tropical MAT), or 2) the isotopic composition of seawater increased by up to 7-8‰. It has been difficult to evaluate these hypotheses because the δ18O composition of fossils depends on both temperature and the δ18O of water. Furthermore, primary isotopic signatures can be overprinted by diagenetic processes that modify geological materials. This too could explain the decrease in δ18O values of marine fossils with age. Carbonate clumped isotope thermometry can constrain this problem by providing an independent measure of crystallization temperature and, when paired with classical δ18O paleothermometry, can determine the isotopic composition of the fluid the mineral last equilibrated with. Combined with traditional tools, this method has the potential to untangle primary isotopic signatures from diagenetic signals. We measured the isotopic ordering of CO3 groups (Δ47) substituted into the phosphate lattice of phosphatic brachiopods in Cambrian strata. Phosphatic fossils are generally less soluble than carbonates in surface and diagenetic environments, and so are hypothesized to provide a more robust record of primary growth conditions. They also provide an archive prior to the rise of thick shelled calcitic fossils during the Ordovician Radiation. Additionally, measurements of the δ18O of the CO3 groups can be compared with the δ18O of PO4 groups to test whether their mutual fractionation is consistent with primary growth and the apparent temperature recorded by carbonate clumped isotope measurements. We are constructing a phosphatic brachiopod calibration for carbonate clumped isotope thermometry, and Δ47 values of CO2 extracted from modern phosphatic brachiopods suggest

  10. Pb Isotope Compositions of Shibaqinghao Gold Deposit in Central Inner Mongolia, China

    Institute of Scientific and Technical Information of China (English)

    ZHANG Hongying; LIANG Yibo

    2002-01-01

    There are two types of gold ore in Shibaqinghao gold deposit, a mylonite ore and a quartz - vein ore. Pb isotope compositions for mylonite ore are characterized by lower Pb isotope ratios ranging from 16.63 to 17.45 (206Pb/204Pb), 15.31 to15.48 (207Pb/204pb), 36.52 to 38.85 (208Pb/204Pb). They are scattered very close to a model curve of the mantle evolution. These ratios suggest that gold in the mylonite ore might be derived from the country rocks, which originated directly in the upper mantle. Pb isotope compositions for quartz - vein ore are characterized by higher Pb isotope ratios ranging from 18.23 to 19.74 (206Pb/204Pb), 15.69 to 15.89 (207Pb/204Pb), 38.64 to 40. 13 (208Pb/204Pb). They are scattered very close to a model curve of the upper crustal evolution. These facts indicate that the gold in the quartz - vein ore might be related to some granitic magma generated in the crust.

  11. Lead isotope and trace element composition of urban soils in Mongolia

    Science.gov (United States)

    Tserenpil, Sh.; Sapkota, A.; Liu, C.-Q.; Peng, J.-H.; Liu, B.; Segebade, P. Chr.

    2016-08-01

    Lead (Pb) pollution in and around Ulaanbaatar is of national concern, given that the Mongolian capital is home to nearly half of the country's entire population. By comparison, Mongolian countryside is a pristine environment because of its sparse population and low industrial activity. The concentration of Pb in urban soils (average of 39.1 mg kg-1) was twice the values found (average 18.6 mg kg-1) in background territories (i.e., Mongolian rural sites). Furthermore, Pb contamination was examined by using Pb stable isotopic composition, and covariance of Pb isotopic ratios showed two groups between rural and urban soils as pristine and disturbed sites. The 206Pb/207Pb ratio, the most prominent fingerprint for Pb pollution, was 1.163-1.185 for the urban whereas values for rural soils (1.186-1.207) were analogue to the regional Pb isotopic signatures. Local coal sources and their combustion products, one of the potential Pb pollution sources in Ulaanbaatar, have significant radiogenic properties in terms of Pb isotopic composition and revealed an average of 1.25 for 206Pb/207Pb and 19.551 for 206Pb/204Pb ratios. Thus, contributions from coal firing activity to Pb pollution lower than it was assumed, and smaller range of these values measured in urban soils may be attributed to the mixing of less radiogenic Pb as a constituent of the leaded gasolines.

  12. Elemental and isotopic fingerprint of Argentinean wheat. Matching soil, water, and crop composition to differentiate provenance.

    Science.gov (United States)

    Podio, Natalia S; Baroni, María V; Badini, Raúl G; Inga, Marcela; Ostera, Héctor A; Cagnoni, Mariana; Gautier, Eduardo A; García, Pilar Peral; Hoogewerff, Jurian; Wunderlin, Daniel A

    2013-04-24

    The aim of this study was to investigate if elemental and isotopic signatures of Argentinean wheat can be used to develop a reliable fingerprint to assess its geographical provenance. For this pilot study we used wheat cultivated at three different regions (Buenos Aires, Córdoba, and Entre Ríos), together with matching soil and water. Elemental composition was determined by ICP-MS. δ(13)C and δ(15)N were measured by isotopic ratio mass spectrometry, while (87)Sr/(86)Sr ratio was determined using thermal ionization mass spectrometry. Wheat samples from three sampling sites were differentiated by the combination of 11 key variables (K/Rb, Ca/Sr, Ba, (87)Sr/(86)Sr, Co, Mo, Zn, Mn, Eu, δ(13)C, and Na), demonstrating differences among the three studied regions. The application of generalized Procrustes analysis showed 99.2% consensus between cultivation soil, irrigation water, and wheat samples, in addition to clear differences between studied areas. Furthermore, canonical correlation analysis showed significant correlation between the elemental and isotopic profiles of wheat and those corresponding to both soil and water (r(2) = 0.97, p wheat samples using different statistical methods, showing that wheat elemental and isotopic compositions are mainly related to soil and irrigation water characteristics of the site of growth.

  13. Spacial and temporal variation of H and O isotopic compositions of the Xijiang Rivers System

    Science.gov (United States)

    Han, G.

    2015-12-01

    Pin Lv1, Fushan Li2, Yang Tang2 School of Water Resources and Environment, China University of Geosciences (Beijing), Beijing 10083, China The State Laboratory of Environmental Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang 550002, China The H and O isotope compositions in the Xijiang River water was investigated on the sample collected from the mainstream and main tributaries in Aug. 2014 and in Jan. 2015. Large variation ranges were observed for δD with (-35.3‰ to -77.1‰ in summer, -31.3‰ to -76.6‰ in winter) andδ18O (-4.8‰ to -10.3‰ in summer, -4.5‰ to -10.3‰ in winter). From the river head to the river mouth, the H and O isotope compositions of the river water collected in the high-discharge and low-discharge period display always a similar variation pattern. On the basis of isotopic composition of river water, the Xijiang River may be separated by three subbasins including the upper basin, the middle basin and the lower basin. The upper reached river water contains relatively low values of δD and δ18O. The values of δD and δ18O in the middle reaches are quite variable because of the middle basin severely disturbed through water impoundments. The lower reaches river water contains high values of δD and δ18O. The differences of δD and δ18O compositions between various tributaries and its effect to the δD and δ18O of the mainstream reflects also the constraint of the meteoric water to the Xijiang River. Evaporation has also important effect to the H and O isotope compositions of the Xijiang River, and it is found that evaporation can also raise the δD and δ18O values of the water during the dry season. Our investigation indicates that the H and O isotope tracing method can play a key role in studying the interaction between river water and other waters, such as the meteoric water, underground water, and lake water. The combination of proper H and O isotope study with conventional meteoric and

  14. Hydrogen isotope composition of leaf wax n-alkanes in Arabidopsis lines with different transpiration rates

    Science.gov (United States)

    Pedentchouk, N.; Lawson, T.; Eley, Y.; McAusland, L.

    2012-04-01

    Stable isotopic compositions of oxygen and hydrogen are used widely to investigate modern and ancient water cycles. The D/H composition of organic compounds derived from terrestrial plants has recently attracted significant attention as a proxy for palaeohydrology. However, the role of various plant physiological and biochemical factors in controlling the D/H signature of leaf wax lipids in extant plants remains unclear. The focus of this study is to investigate the effect of plant transpiration on the D/H composition of n-alkanes in terrestrial plants. This experiment includes 4 varieties of Arabidopsis thaliana that differ with respect to stomatal density and stomatal geometry. All 4 varieties were grown indoors under identical temperature, relative humidity, light and watering regimes and then sampled for leaf wax and leaf water stable isotopic measurements. During growth, stomatal conductance to carbon dioxide and water vapour were also determined. We found that the plants varied significantly in terms of their transpiration rates. Transpiration rates were significantly higher in Arabidopsis ost1 and ost1-1 varieties (2.4 and 3.2 mmol m-2 s-1, respectively) than in Arabidopsis RbohD and Col-0 (1.5 and 1.4). However, hydrogen isotope measurements of n-alkanes extracted from leaf waxes revealed a very different pattern. Varieties ost1, ost1-1, and RbohD have very similar deltaD values of n-C29 alkane (-125, -128, and -127 per mil), whereas the deltaD value of Col-0 is more negative (-137 per mil). The initial results of this work suggest that plant transpiration is decoupled from the D/H composition of n-alkanes. In other words, physical processes that affect water vapour movement between the plant and its environment apparently cannot account for the stable hydrogen isotope composition of organic compounds that comprise leaf waxes. Additional, perhaps biochemical, processes that affect hydrogen isotope fractionation during photosynthesis might need to be invoked

  15. Fabrication procedures for manufacturing High Flux Isotope Reactor fuel elements - 2

    Energy Technology Data Exchange (ETDEWEB)

    Knight, R.W.; Morin, R.A.

    1999-12-01

    The original fabrication procedures written in 1968 delineated the manufacturing procedures at that time. Since 1968, there have been a number of procedural changes. This rewrite of the fabrication procedures incorporates these changes. The entire fuel core of this reactor is made up of two fuel elements. Each element consists of one annular array of fuel plates. These annuli are identified as the inner and outer fuel elements, since one fits inside the other. The inner element consists of 171 identical fuel plates, and the outer element contains 369 identical fuel plates differing slightly from those in the inner element. Both sets of fuel plates contain U{sub 3}O{sub 8} powder as the fuel, dispersed in an aluminum powder matrix and clad with aluminum. Procedures for manufacturing and inspection of the fuel elements are described and illustrated.

  16. Stocking rate and fuels reduction effects on beef cattle diet composition and quality

    Science.gov (United States)

    Abe Clark; Tim DelCurto; Martin Vavra; Brian L. Dick

    2013-01-01

    An experiment was conducted to evaluate the influence of forest fuels reduction on diet quality, botanical composition, relative preference, and foraging efficiency of beef cattle grazing at different stocking rates. A split plot factorial design was used, with whole plots (3 ha) being fuel reduced or no treatment (control), and split plots (1 ha) within whole plots...

  17. Atmospheric control on isotopic composition and d-excess in water vapor over ocean surface

    Science.gov (United States)

    Fan, Naixin

    For decades, stable isotopes of water have been used as proxies to infer the variation of the hydrological cycle. However, it is still not clear how various atmospheric processes quantitatively control kinetic fractionation during evaporation over the ocean. Understanding kinetic fractionation is important in that the interpretation of the isotopic composition record preserved in ice cores and precipitation relies in part on the isotopic information at the moisture source. In addition, the isotopic composition of vapor contains information about variation of atmospheric processes such as turbulence and change in moisture source region which is useful for studying meteorological processes and climate change. In this study the isotopic composition of water vapor in the marine boundary layer (MBL) over the ocean was investigated using a combination of a newly developed marine boundary layer (MBL) model and observational data. The new model has a more realistic MBL structure than previous models and includes new features such as vertical advection of air and diffusion coefficients that vary continuously in the vertical direction. A robust linear relationship between deltaD and delta18O was found in observational oceanic water vapor data and the model can well capture the characteristics of this relationship. The individual role of atmospheric processes or variables on deltaD, delta18O and d-excess was quantitatively investigated and an overview of the combined effect of all the meteorological processes is provided. In particular, we emphasize that the properties of subsiding air (such as its mixing ratio and isotopic values) are crucial to the isotopic composition of surface water vapor. Relative humidity has been used to represent the moisture deficit that drives evaporative isotopic fluxes, however, we argue that it has serious limitations in explaining d-excess variation as latitude varies. We introduce a new quantity Gd=SST-Td, the difference between the sea

  18. Multidisciplinary Simulation of Graphite-Composite and Cermet Fuel Elements for NTP Point of Departure Designs

    Science.gov (United States)

    Stewart, Mark E.; Schnitzler, Bruce G.

    2015-01-01

    This paper compares the expected performance of two Nuclear Thermal Propulsion fuel types. High fidelity, fluid/thermal/structural + neutronic simulations help predict the performance of graphite-composite and cermet fuel types from point of departure engine designs from the Nuclear Thermal Propulsion project. Materials and nuclear reactivity issues are reviewed for each fuel type. Thermal/structural simulations predict thermal stresses in the fuel and thermal expansion mis-match stresses in the coatings. Fluid/thermal/structural/neutronic simulations provide predictions for full fuel elements. Although NTP engines will utilize many existing chemical engine components and technologies, nuclear fuel elements are a less developed engine component and introduce design uncertainty. Consequently, these fuel element simulations provide important insights into NTP engine performance.

  19. Advanced Composite Bipolar Plate for Unitized Regenerative Fuel Cell/Electrolyzer Systems Project

    Data.gov (United States)

    National Aeronautics and Space Administration — Development of an advanced composite bipolar plate is proposed for a unitized regenerative fuel cell and electrolyzer system that operates on pure feed streams...

  20. Modelling the isotopic composition of snow using backward trajectories : a particular precipitation event in Dronning Maud Land, Antarctica

    NARCIS (Netherlands)

    Helsen, MM; Van de Wal, RSW; Van den Broeke, MR; Kerstel, ERT; Masson-Delmotte, [No Value; Meijer, HAJ; Reijmer, CH; Scheele, MP; Jacka, J

    2004-01-01

    We consider a specific accumulation event that occurred in January 2002 in western Dronning Maud Land, Antarctica. Snow samples were obtained a few days after accumulation. We combine meteorological analyses and isotopic modelling to describe the isotopic composition of moisture during transport. Ba

  1. The effects of growth phase and salinity on the hydrogen isotopic composition of alkenones produced by coastal haptophyte algae

    NARCIS (Netherlands)

    Chivall, D.; M'Boule, D.; Sinke-Schoen, D.; Sinninghe Damsté, J.S.; Schouten, S.; van der Meer, M.T.J.

    2014-01-01

    The isotopic fractionation of hydrogen during the biosynthesis of alkenones produced by marine haptophyte algae has been shown to depend on salinity and, as such, the hydrogen isotopic composition of alkenones is emerging as a palaeosalinity proxy. The relationship between fractionation and salinity

  2. Situation of sewage input reflected by nitrogen isotopic composition in a sediment core of Hongfeng Lake

    Institute of Scientific and Technical Information of China (English)

    2006-01-01

    Nitrogen in Hongfeng South Lake water mainly comes from sewage with high N concentrations from Pingba Chemical Fertilizer Plant (PCFP). Studies on the sediment core HF010427 sampled in the lake showed that the upward increase of nitrogen isotopic composition of sedimentary organic nitrogen (δ15Norg) accorded with the trend of industrial total production (TP) of PCFC. On the contrary, diagenesis will theoretically cause an upward decrease of δ15Norg. Because no treatment of sewage water was carried out, TP corresponds with sewage emission, indicating that sedimentary δ15Norg can reflect well the total trend of sewage input. The very similar profile shape between nitrogen isotopic composition of sedimentary absorbed ammonium (δ15NH4+absorbed) and TP of PCFP suggests that δ15NH4+absorbed can be used to reconstruct more detailed situation of sewage input. The study has a reference to history investigation of sewage input.

  3. A rapid method for determination of the isotopic composition of uranium samples by alpha spectrometry

    Energy Technology Data Exchange (ETDEWEB)

    Martin Sanchez, A.; Tome, F.V.; Diaz Bejarano, J.; Jurado Vargas, M. (Dept. de Fisica, Univ. Extremadura, Badajoz (Spain))

    1992-03-01

    A simple method of analyzing alpha spectra from natural and enriched or depleted uranium samples is developed. The procedure is non-iterative, and takes into consideration low-energy tail and branching-ratio corrections to accurately calculate the area corresponding to each uranium isotope ({sup 234}U, {sup 235}U, {sup 236}U, {sup 238}U) in the spectrum, and then the isotopic composition of the sample. A BASIC computer program, called ENURA, has been developed to perform all the necessary calculations to give the results together with their uncertainties. Several samples were prepared with different uranium concentrations made from standard solutions with known compositions, and the method was checked against the experimental measurements from these samples. Other series of uranium spectra were theoretically constructed using a given line shape in order to cover the required range of enriched or depleted uranium. (orig.).

  4. Isotopic compositions and probable origins of organic molecules in the Eocene Messel shale

    Science.gov (United States)

    Hayes, J. M.; Takigiku, Ray; Ocampo, Ruben; Callot, Enry J.; Albrecht, Pierre

    1987-01-01

    It is shown here that the carbon isotopic compositions of biomarkers from the Eocene Messel shale, accumulated 47 + or - 2 million years ago in anaerobic waters at the bottom of a lake, allow identification of specific sources for some materials and reconstruction of carbon flows within the lake and its sediments. The C-13 content of organic matter synthesized by lacustrine primary producers can be estimated from the observed C-13 content of the geoporphyrins derived from their chlorophylls. Total organic material in the shale is depleted in C-13 by six parts per thousand relative to that input. This difference cannot be explained by selective loss of components enriched in C-13, nor, as shown by isotopic compositions of other biomarkers, by inputs from land plants surrounding the lake or from methanogenic bacteria.

  5. Accurate measurement of neodymium isotopic composition using Neptune MC-ICP-MS

    Institute of Scientific and Technical Information of China (English)

    Yueheng YANG; Hongfu ZHANG; Liewen XIE; Fuyuan WU

    2008-01-01

    This paper reports the measurement of the Neodymium isotopic composition by Neptune Multiple Collector Inductively Coupled Plasma Mass Spectrometry (MC-ICP-MS) over the last two years. Although there is concomitant Cerium in the chemical separation process, this has no significant influence on the Neodymium analysis. As for the sample containing small amounts of Samarium (Sm/Nd<0.04), direct calibration for isobaric interference and mass discrimina-tion by the exponential law can be obtained by assuming that Samarium mass discrimination is the same as that of Neodymium. Geological samples after traditional chemi-cal separation were measured by Neptune MC-ICP-MS and Thermal Ionization Mass Spectrometry (TIMS) respectively. The results show that Neptune MC-ICP-MS can measure Neodymium isotopic composition as precisely the TIMS does and is even more effective and less time-consuming than the TIMS Method.

  6. Experimental assessment of environmental influences on the stable isotopic composition of Daphnia pulicaria and their ephippia

    Directory of Open Access Journals (Sweden)

    J. Schilder

    2015-02-01

    δ15N values of ephippia and Daphnia between the 12 °C and 20 °C treatments, but the δ18O values of Daphnia and ephippia were on average 1.2‰ lower at 20 °C compared with 12 °C. We conclude that the stable isotopic composition of Daphnia ephippia provides information on that of the parent Daphnia and of the food and water they were exposed to, with small offsets between Daphnia and ephippia relative to variations in Daphnia stable isotopic composition reported from downcore studies. However, our experiments also indicate that temperature may have a minor influence on the δ13C, δ15N and δ18O values of Daphnia body tissue and ephippia. This aspect deserves attention in further controlled experiments.

  7. Thorium utilisation in a small long-life HTR. Part III: Composite-rod fuel blocks

    Energy Technology Data Exchange (ETDEWEB)

    Verrue, Jacques, E-mail: jacques.verrue@polytechnique.org [Delft University of Technology, Reactor Institute Delft, Mekelweg 15, 2629 JB Delft (Netherlands); École Polytechnique (Member of ParisTech), 91128 Palaiseau Cedex (France); Ding, Ming, E-mail: dingm2005@gmail.com [Delft University of Technology, Reactor Institute Delft, Mekelweg 15, 2629 JB Delft (Netherlands); Harbin Engineering University, Nantong Street 145, 150001 Harbin (China); Kloosterman, Jan Leen, E-mail: j.l.kloosterman@tudelft.nl [Delft University of Technology, Reactor Institute Delft, Mekelweg 15, 2629 JB Delft (Netherlands)

    2014-02-15

    Highlights: • Composite-rod fuel blocks are proposed for a small block-type HTR. • An axial separation of fuel compacts is the most important feature. • Three patterns are presented to analyse the effects of the spatial distribution. • The spatial distribution has a large influence on the neutron spectrum. • Composite-rod fuel blocks reach a reactivity swing less than 4%. - Abstract: The U-Battery is a small long-life high temperature gas-cooled reactor (HTR) with power of 20 MWth. In order to increase its lifetime and diminish its reactivity swing, the concept of composite-rod fuel blocks with uranium and thorium was investigated. Composite-rod fuel blocks feature a specific axial separation between UO{sub 2} and ThO{sub 2} compacts in fuel rods. The design parameters, investigated by SCALE 6, include the number and spatial distribution of fuel compacts within the rods, the enrichment of uranium, the radii of fuel kernels and fuel compacts, and the packing fractions of uranium and thorium TRISO particles. The analysis shows that a lower moderation ratio and a larger inventory of heavy metals results in a lower reactivity swing. The optimal atomic carbon-to-heavy metal ratio depends on the mass fraction of U-235 and is commonly in the 160–200 range. The spatial distribution of the fuel compacts within the fuel rods has a large influence on the energy spectrum in each fuel compact and thus on the beginning-of-life reactivity and the reactivity swing. At end-of-life, the differences caused by the spatial distribution of the fuel compacts are smaller due to the fissions of U-233 in the ThO{sub 2} fuel compacts. This phenomenon enables to design fuel blocks with a very low reactivity swing, down to less than 4% in a 10-year lifetime. Among three types of thorium fuelled U-Battery blocks, the composite-rod fuel block achieves the highest end-of-life reactivity and the lowest reactivity swing.

  8. Where Did the Ureilite Parent Body Accrete? Constraints from Chemical and Isotopic Compositions

    Science.gov (United States)

    Goodrich, Cyrena; O'Brien, David P.

    2014-11-01

    Almahata Sitta and other polymict ureilites contain a remarkable diversity of materials, including EH, EL, OC, R- and CB chondrites, in addition to the dominant ureilitic material [1]. These materials represent at least 6 different parent asteroids and a wide range of chemical and isotopic environments in the early Solar System. To understand the origin of this diversity it is critical to know where (heliocentric distance) the ureilite parent body (UPB) accreted. The chemical and isotopic compositions of ureilite precursors (inferred from the compositions of ureilites) can provide clues. Lithophile element ratios such as Si/Mg and Mn/Mg [2,3], and deficits in neutron-rich Cr, Ti and Ni isotopes [3], indicate that ureilite precursors were similar to ordinary or enstatite chondrites (OC or EC), not carbonaceous chondrites (CC). In contrast, high carbon contents, carbon isotopes and oxygen isotopes suggest a genetic link to CC. This poses a conundrum considering the variation of asteroid types, which suggests that EC and OC dominate the inner asteroid belt and CC the outer belt. However, the CC-like oxygen isotopes of ureilites strongly suggest the effects of parent-body aqueous alteration [4,5], which clearly implies that the UPB accreted beyond the ice line. Lithophile element properties of ureilites compared with chondrites may not be a reliable indicator of location of accretion, because lithophile elements in chondrites are sited mainly in chondrules and the UPB accreted before most chondrules formed [6]. Ureilite Cr, Ti and Ni isotopes may indicate late introduction of the neutron rich isotopes of these elements to the CC-formation region [7]. We conclude that the UPB accreted in the outer belt, like CC. The UPB or one of its offspring must have migrated to the inner belt to acquire OC, EC and R-chondrite materials.[1] Horstmann M. & Bischoff A. [2014] Chemie der Erde 74, 149.[2] Goodrich C. [1999] MAPS 34, 109.[3] Warren P. [2011] GCA 46, 53.[4] Young E. [1999

  9. Mineralogy and Oxygen Isotope Compositions of an Unusual Hibonite-Perovskite Refractory Inclusion from Allende

    Science.gov (United States)

    Keller, L. P.; Snead, C.; Rahman, Z.; McKeegan, K. D.

    2012-01-01

    Hibonite-rich Ca- and Al-rich inclusions (CAIs) are among the earliest formed solids that condensed in the early nebula. We discovered an unusual refractory inclusion from the Allende CV3 chondrite (SHAL) containing an approx 500 micron long single crystal of hibonite and co-existing coarse-grained perovskite. The mineralogy and petrography of SHAL show strong similarities to some FUN inclusions, especially HAL. Here we report on the mineralogy, petrography, mineral chemistry and oxygen isotopic compositions in SHAL.

  10. U and Th Concentration and Isotopic Composition of Hydrothermal Fluids at the Lost City Hydrothermal Field

    Science.gov (United States)

    Ludwig, K. A.; Shen, C.; Cheng, H.; Edwards, R.; Kelley, D. S.; Butterfield, D. A.

    2006-12-01

    Uranium and Th concentration and isotopic composition of hydrothermal fluids at the Lost City Hydrothermal Field (LCHF) were determined using multi-collector inductively coupled plasma mass spectrometry (MC-ICP- MS). The LCHF is an off-axis, serpentinite-hosted hydrothermal system located at 30°N near the Mid- Atlantic Ridge. Carbonate chimneys reaching 60 m in height vent alkaline (pH~10), calcium-rich fluids at 40- 91°C and the towers are home to dense microbial communities. Vent fluid and seawater U and Th concentration and isotopic composition data provide critical information for constraining U-Th chimney ages. The increased sensitivity (1-2%) of MC-ICP-MS combined with an Aridus nebulization system allows the precise measurement of small quantities of sample (~150 ml) with low concentrations (ICP-MS techniques to measure the U and Th concentration and isotopic composition (234U, 238U, 230Th, and 232Th) of eight hydrothermal fluid samples. Endmember fluids with ~1mmol/kg Mg have ~0.02 ng/g U, confirming that end-member fluids contain near-zero values of both Mg and U. Thorium concentrations of fluids are close to deep seawater values. U and Th isotopic compositions are reported at the permil level. These data may provide new insights into the role of serpentinite-hosted hydrothermal systems in the budgets of U and Th in the ocean. Techniques presented in this study may be applied to other hydrothermal and seep environments.

  11. An assessment of upper mantle heterogeneity based on abyssal peridotite isotopic compositions

    Science.gov (United States)

    Warren, J. M.; Shimizu, N.; Sakaguchi, C.; Dick, H. J. B.; Nakamura, E.

    2009-12-01

    Abyssal peridotites, the depleted solid residues of ocean ridge melting, are the most direct samples available to assess upper oceanic mantle composition. We present detailed isotope and trace element analyses of pyroxene mineral separates from Southwest Indian Ridge abyssal peridotites and pyroxenites in order to constrain the size and length scale of mantle heterogeneity. Our results demonstrate that the mantle can be highly heterogeneous to account adequately for the complexities of ancient and recent melting processes.

  12. Catalytic Surface Promotion of Composite Cathodes in Protonic Ceramic Fuel Cells

    DEFF Research Database (Denmark)

    Solis, Cecilia; Navarrete, Laura; Bozza, Francesco;

    2015-01-01

    Composite cathodes based on an electronic conductor and a protonic conductor show advantages for protonic ceramic fuel cells. In this work, the performance of a La5.5WO11.25-δ/ La0.8Sr0.2MnO3+δ (LWO/LSM) composite cathode in a fuel cell based on an LWO protonic conducting electrolyte is shown and...

  13. Spatial variability in the isotopic composition of rainfall in a small headwater catchment and its effect on hydrograph separation

    Science.gov (United States)

    Fischer, Benjamin M. C.; van Meerveld, H. J. (Ilja); Seibert, Jan

    2017-04-01

    Isotope hydrograph separation (IHS) is a valuable tool to study runoff generation processes. To perform an IHS, samples of baseflow (pre-event water) and streamflow are taken at the catchment outlet. For rainfall (event water) either a bulk sample is collected or it is sampled sequentially during the event. For small headwater catchment studies, event water samples are usually taken at only one sampling location in or near the catchment because the spatial variability in the isotopic composition of rainfall is assumed to be small. However, few studies have tested this assumption. In this study, we investigated the spatiotemporal variability in the isotopic composition of rainfall and its effects on IHS results using detailed measurements from a small pre-alpine headwater catchment in Switzerland. Rainfall was sampled sequentially at eight locations across the 4.3 km2 Zwäckentobel catchment and stream water was collected in three subcatchments (0.15, 0.23, and 0.70 km2) during ten events. The spatial variability in rainfall amount, average and maximum rainfall intensity and the isotopic composition of rainfall was different for each event. There was no significant relation between the isotopic composition of rainfall and total rainfall amount, rainfall intensity or elevation. For eight of the ten studied events the temporal variability in the isotopic composition of rainfall was larger than the spatial variability in the rainfall isotopic composition. The isotope hydrograph separation results, using only one rain sampler, varied considerably depending on which rain sampler was used to represent the isotopic composition of event water. The calculated minimum pre-event water contributions differed up to 60%. The differences were particularly large for events with a large spatial variability in the isotopic composition of rainfall and a small difference between the event and pre-event water isotopic composition. Our results demonstrate that even in small catchments

  14. Investigating the source, transport, and isotope composition of water vapor in the planetary boundary layer

    Science.gov (United States)

    Griffis, Timothy J.; Wood, Jeffrey D.; Baker, John M.; Lee, Xuhui; Xiao, Ke; Chen, Zichong; Welp, Lisa R.; Schultz, Natalie M.; Gorski, Galen; Chen, Ming; Nieber, John

    2016-04-01

    Increasing atmospheric humidity and convective precipitation over land provide evidence of intensification of the hydrologic cycle - an expected response to surface warming. The extent to which terrestrial ecosystems modulate these hydrologic factors is important to understand feedbacks in the climate system. We measured the oxygen and hydrogen isotope composition of water vapor at a very tall tower (185 m) in the upper Midwest, United States, to diagnose the sources, transport, and fractionation of water vapor in the planetary boundary layer (PBL) over a 3-year period (2010 to 2012). These measurements represent the first set of annual water vapor isotope observations for this region. Several simple isotope models and cross-wavelet analyses were used to assess the importance of the Rayleigh distillation process, evaporation, and PBL entrainment processes on the isotope composition of water vapor. The vapor isotope composition at this tall tower site showed a large seasonal amplitude (mean monthly δ18Ov ranged from -40.2 to -15.9 ‰ and δ2Hv ranged from -278.7 to -113.0 ‰) and followed the familiar Rayleigh distillation relation with water vapor mixing ratio when considering the entire hourly data set. However, this relation was strongly modulated by evaporation and PBL entrainment processes at timescales ranging from hours to several days. The wavelet coherence spectra indicate that the oxygen isotope ratio and the deuterium excess (dv) of water vapor are sensitive to synoptic and PBL processes. According to the phase of the coherence analyses, we show that evaporation often leads changes in dv, confirming that it is a potential tracer of regional evaporation. Isotope mixing models indicate that on average about 31 % of the growing season PBL water vapor is derived from regional evaporation. However, isoforcing calculations and mixing model analyses for high PBL water vapor mixing ratio events ( > 25 mmol mol-1) indicate that regional evaporation can account

  15. Computer Simulations of Composite Electrodes in Solid-Oxide Fuel-Cells

    Energy Technology Data Exchange (ETDEWEB)

    Sunde, Svein

    1999-07-01

    Fuel cells are devices for converting the combined chemical (free) energy of fuels and oxygen (air) directly to electrical energy without relying on the dynamic action of steam heated by reacting fuel-oxygen mixtures, like in steam turbines, or of the reacting gas mixtures themselves, like in gas turbines. The basic rationale for fuel cells is their high efficiencies as compared to indirect-conversion methods. Fuel cells are currently being considered for a number of applications, among them de-centralised power supply. Fuel cells come in five basic types and are usually classified according to the type of electrolyte used, which in turn to a significant degree limits the options for anode and cathode materials. The solid-oxide fuel-cell (SOFC) , with which this thesis is concerned, is thus named after its oxide electrolyte, typically the oxide-ion conducting material yttria-stabilised zirconia (YSZ). While the cathode of an SOFC is often uniform in chemical composition (or at least intended to be), various problems of delamination, cracking etc. associated with the use of metallic anode electrocatalysts led to the development of composite SOFC anodes. Porous anodes consisting of Ni and YSZ particles in roughly 50/50 wt-% mixtures are now almost standard with any SOFC-development programme. The designer of composite SOFC electrodes is faced with at least three, interrelated questions: (1) What will be the optimum microstructure and composition of the composite electrode? (2) If the structure changes during operation, as is often observed, what will be the consequences for the internal losses in the cell? (3) How do we interpret electrochemical and conductivity measurements with regard to structure and composition? It is the primary purpose of this thesis to provide a framework for modelling the electrochemical and transport properties of composite electrodes for SOFC, and to arrive at some new insights that cannot be offered by experiment alone. Emphasis is put on

  16. Li Isotopic Composition and Concentration of the Upper Continental Crust: New Insights from Desert Loess

    Science.gov (United States)

    Sauzeat, L.; Rudnick, R. L.; Chauvel, C.

    2014-12-01

    The isotopic composition of lithium (δ7Li) is recognized to be an excellent proxy of near-surface fluid-rock reactions during weathering. Using Li as a tracer of these processes however requires constraints on the average Li composition of terrestrial reservoirs, in particular that of the upper continental crust. To date, only one value for the average δ7Li value of the upper continental crust, derived from periglacial loess, shales, and granites is available in the literature (7δLi = 0 ± 4 (2σ), Teng et al., 2004). Several values exist for the average [Li] of the upper crust, but they differ by more than 30%. We measured the Li isotopic composition of about 30 desert and periglacial loess (unweathered windblown sediments) from several parts of the world (Europe, Argentina, China and Tajikistan). We demonstrate that desert loess, which is more homogeneous and representative of larger portions of the Earth's surface, provides a better proxy for the average composition of the upper continental crust compared to periglacial loess. The Li isotopic compositions and concentrations of desert loess are controlled by eolian sorting, which can be quantified as a binary isotopic mixing between a weathered fine-grained end-member and an unweathered coarse-grained end-member. Using correlations between Li isotopic compositions, Li concentrations and trace element concentrations in desert loess, we estimate new average values for the upper continental crust: 1 ± 2 (2σ); [Li] = 35.3 ± 4.6 (2σ) ppm. This δ7Li value is slightly higher than that previously published in Teng et al. (2004), but overlaps within uncertainty, whereas the [Li] is identical to that of Teng et al. (2004: 35 ± 11, 2σ); both new estimates have lower uncertainty. Our new estimate of [Li], along with that of Teng et al. (2004), are higher than all previous estimates for the upper continental crust, raising the question as to whether the average concentrations of other mobile alkali metals such as

  17. Temporal variations in lead concentrations and isotopic composition in the Southern California Bight

    Energy Technology Data Exchange (ETDEWEB)

    Sanudo-Wilhelmy, S.A.; Flegal, A.R. (Univ. of California, Santa Cruz, CA (United States))

    1994-08-01

    Lead concentrations in surface waters of the Southern California Bight appear to have decreased threefold (from >170 to <60 pM) since they were initially measured by Clair Patterson and his associates in the 1970s. The decrease parallels a threefold decline in anthropogenic inputs of industrial lead to the bight over the past two decades. Moreover, mass balance calculations indicate that the primary source of lead to the bight now is upwelling. This is evidenced by the isotopic compositions of surface waters in the bight, which are most characteristic of Asian industrial lead aerosols (0.4793 [le] [sup 206]Pb/[sup 208]Pb [le] 0.4833) deposited in oceanic waters of the North Pacific. While the decrease in surface water lead concentrations in the bight reflects the reduction in industrial lead emissions from the United States, the isotopic compositions of surface waters in the southern reach of the bight reflect a concurrent increase in industrial lead emissions from Mexico (0.4852 [le] [sup 206]Pb/[sup 208]Pb [le] 0.4877). The isotopic composition ([sup 208]Pb/[sup 207]Pb [approximately] 2.427) of elevated lead concentrations of surface waters in San Diego Bay indicate that lead is being remobilized from contaminated sediments within that bay.

  18. Analysis of maximum allowable fragment heights during dissolution of high flux isotope reactor fuel in an h-canyon dissolver

    Energy Technology Data Exchange (ETDEWEB)

    Daniel, G. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Rudisill, T. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)

    2017-07-17

    As part of the Spent Nuclear Fuel (SNF) processing campaign, H-Canyon is planning to begin dissolving High Flux Isotope Reactor (HFIR) fuel in late FY17 or early FY18. Each HFIR fuel core contains inner and outer fuel elements which were fabricated from uranium oxide (U3O8) dispersed in a continuous Al phase using traditional powder metallurgy techniques. Fuels fabricated in this manner, like other SNF’s processed in H-Canyon, dissolve by the same general mechanisms with similar gas generation rates and the production of H2. The HFIR fuel cores will be dissolved using a flowsheet developed by the Savannah River National Laboratory (SRNL) in either the 6.4D or 6.1D dissolver using a unique insert. Multiple cores will be charged to the same dissolver solution maximizing the concentration of dissolved Al. The recovered U will be down-blended into low-enriched U for subsequent use as commercial reactor fuel. During the development of the HFIR fuel dissolution flowsheet, the cycle time for the initial core was estimated at 28 to 40 h. Once the cycle is complete, H-Canyon personnel will open the dissolver and probe the HFIR insert wells to determine the height of any fuel fragments which did not dissolve. Before the next core can be charged to the dissolver, an analysis of the potential for H2 gas generation must show that the combined surface area of the fuel fragments and the subsequent core will not generate H2 concentrations in the dissolver offgas which exceeds 60% of the lower flammability limit (LFL) of H2 at 200 °C. The objective of this study is to identify the maximum fuel fragment height as a function of the Al concentration in the dissolving solution which will provide criteria for charging successive HFIR cores to an H-Canyon dissolver.

  19. Stable carbon and radiocarbon isotope compositions of particle size fractions to determine origins of sedimentary organic matter in an estuary

    NARCIS (Netherlands)

    Megens, L; van der Plicht, J; de Leeuw, JW; Smedes, F; Altabet, M.

    2002-01-01

    Stable and radioactive carbon isotopic compositions of particle size fractions of a surface sediment from the Ems-Dollard estuary vary considerably with particle size. The organic material in the fine fractions (

  20. Stable carbon and radiocarbon isotope compositions of particle size fractions to determine origins of sedimentary organic matter in an estuary

    NARCIS (Netherlands)

    Megens, L; van der Plicht, J; de Leeuw, JW; Smedes, F; Altabet, M.

    2002-01-01

    Stable and radioactive carbon isotopic compositions of particle size fractions of a surface sediment from the Ems-Dollard estuary vary considerably with particle size. The organic material in the fine fractions (

  1. Limitations of the isotopic composition of nitrates as a tracer of their origin

    Science.gov (United States)

    Kloppmann, Wolfram; Mayer, Bernhard; Otero, Neus; Sebilo, Mathieu; Gooddy, Daren; Lapworth, Dan; Surridge, Ben; Petelet Giraud, Emmanuelle; Flehoc, Christine; Baran, Nicole

    2017-04-01

    Nitrogen and oxygen isotopes are traditionally considered and frequently used as tracers of nitrate sources in watersheds used for drinking water production. The enrichment of synthetic nitrate-containing fertilizers in 18O due to the contribution of atmospheric oxygen in the production process confers a specific isotopic fingerprint to mineral fertilizers. In spite of the still widespread use on nitrate-containing synthetic fertilizers, their characteristic N and O isotope signatures are rarely unambiguously observed in nitrate-contaminated groundwater. We postulate, in line with Mengis et al. (2001), that fertilizer-derived nitrate is not directly and rapidly transferred to groundwater but rather retained in the soil-plant system as organic N and then mineralized and re-oxidized (termed the mineralization-immobilization turnover, MIT) thereby re-setting the oxygen isotope composition of nitrate and also changing its N isotope ratios. We show examples from watersheds on diverse alluvial/clastic and carbonate aquifers in eastern and northern France where, in spite of the use of mineral fertilizers, evidenced also through other isotopic tracers (boron isotopes), both N and O-isotope ratios are very homogeneous and compatible with nitrification of ammonium where 2/3 of oxygen is derived from soil water and 1/3 from atmospheric O2. These field data are corroborated by lysimeter data from Canada. Even if in areas where ammonium is derived from chemical fertilizers, N values still tend to be lower than in areas where ammonium is derived from manure/sewage, this is clearly a limitation to the dual isotope method (N, O) for nitrate source identification, but has important implications for the nitrogen mobility and residence time in soils amended with synthetic fertilizers (Sebilo et al., 2013). Mengis M., Walther U., Bernasconi S. M., Wehrli B. (2001) Limitations of Using δ18O for the Source Identification of Nitrate in Agricultural Soils. Environmental Science

  2. Triple oxygen isotopic composition of the high-3He/4He mantle

    Science.gov (United States)

    Starkey, N. A.; Jackson, C. R. M.; Greenwood, R. C.; Parman, S.; Franchi, I. A.; Jackson, M.; Fitton, J. G.; Stuart, F. M.; Kurz, M.; Larsen, L. M.

    2016-03-01

    Measurements of Xe isotope ratios in ocean island basalts (OIB) suggest that Earth's mantle accreted heterogeneously, and that compositional remnants of accretion are sampled by modern, high-3He/4He OIB associated with the Icelandic and Samoan plumes. If so, the high-3He/4He source may also have a distinct oxygen isotopic composition from the rest of the mantle. Here, we test if the major elements of the high-3He/4He source preserve any evidence of heterogeneous accretion using measurements of three oxygen isotopes on olivine from a variety of high-3He/4He OIB locations. To high precision, the Δ17O value of high-3He/4He olivines from Hawaii, Pitcairn, Baffin Island and Samoa, are indistinguishable from bulk mantle olivine (Δ17OBulk Mantle - Δ17OHigh 3He/4He olivine = -0.002 ± 0.004 (2 × SEM)‰). Thus, there is no resolvable oxygen isotope evidence for heterogeneous accretion in the high-3He/4He source. Modelling of mixing processes indicates that if an early-forming, oxygen-isotope distinct mantle did exist, either the anomaly was extremely small, or the anomaly was homogenised away by later mantle convection. The δ18O values of olivine with the highest 3He/4He ratios from a variety of OIB locations have a relatively uniform composition (∼5‰). This composition is intermediate to values associated with the depleted MORB mantle and the average mantle. Similarly, δ18O values of olivine from high-3He/4He OIB correlate with radiogenic isotope ratios of He, Sr, and Nd. Combined, this suggests that magmatic oxygen is sourced from the same mantle as other, more incompatible elements and that the intermediate δ18O value is a feature of the high-3He/4He mantle source. The processes responsible for the δ18O signature of high-3He/4He mantle are not certain, but δ18O-87Sr/86Sr correlations indicate that it may be connected to a predominance of a HIMU-like (high U/Pb) component or other moderate δ18O components recycled into the high-3He/4He source.

  3. Tracking nitrous oxide emission processes at a suburban site with semicontinuous, in situ measurements of isotopic composition

    Science.gov (United States)

    Harris, Eliza; Henne, Stephan; Hüglin, Christoph; Zellweger, Christoph; Tuzson, Béla; Ibraim, Erkan; Emmenegger, Lukas; Mohn, Joachim

    2017-02-01

    The isotopic composition of atmospheric nitrous oxide (N2O) was measured semicontinuously, at ˜35 min frequency in intermittent periods of 1-6 days over one and a half years, using preconcentration coupled to a quantum cascade laser spectrometer at the suburban site of Dübendorf, Switzerland. The achieved measurement repeatability was 0.08‰, 0.11‰, and 0.10‰ for δ18O, site preference, and δ15Nbulk respectively, which is better than or equal to standard flask sampling-based isotope ratio mass spectrometry performance. The observed mean diurnal cycle reflected the buildup of N2O from isotopically light sources on an isotopically heavy tropospheric background. The measurements were used to determine the source isotopic composition, which varied significantly compared to chemical and meteorological parameters monitored at the site. FLEXPART-COSMO transport modeling in combination with modified Emissions Database for Global Atmospheric Research inventory emissions was used to model N2O mole fractions at the site. Additionally, isotopic signatures were estimated for different source categories using literature data and used to simulate N2O isotopic composition over the measurement period. The model was able to capture variability in N2O mole fraction well, but simulations of isotopic composition showed little agreement with observations. In particular, measured source isotopic composition exhibited one magnitude larger variability than simulated, clearly indicating that the range of isotopic source signatures estimated from literature significantly underestimates true variability of source signatures. Source δ18O signature was found to be the most sensitive tracer for urban/industry versus agricultural N2O. δ15Nbulk and site preference may provide more insight into microbial and chemical emission processes than partitioning of anthropogenic source categories.

  4. Isotopic composition for source identification of mercury in atmospheric fine particles

    Science.gov (United States)

    Huang, Qiang; Chen, Jiubin; Huang, Weilin; Fu, Pingqing; Guinot, Benjamin; Feng, Xinbin; Shang, Lihai; Wang, Zhuhong; Wang, Zhongwei; Yuan, Shengliu; Cai, Hongming; Wei, Lianfang; Yu, Ben

    2016-09-01

    The usefulness of mercury (Hg) isotopes for tracing the sources and pathways of Hg (and its vectors) in atmospheric fine particles (PM2.5) is uncertain. Here, we measured Hg isotopic compositions in 30 potential source materials and 23 PM2.5 samples collected in four seasons from the megacity Beijing (China) and combined the seasonal variation in both mass-dependent fractionation (represented by the ratio 202Hg / 198Hg, δ202Hg) and mass-independent fractionation of isotopes with odd and even mass numbers (represented by Δ199Hg and Δ200Hg, respectively) with geochemical parameters and meteorological data to identify the sources of PM2.5-Hg and possible atmospheric particulate Hg transformation. All PM2.5 samples were highly enriched in Hg and other heavy metals and displayed wide ranges of both δ202Hg (-2.18 to 0.51 ‰) and Δ199Hg (-0.53 to 0.57 ‰), as well as small positive Δ200Hg (0.02 to 0.17 ‰). The results indicated that the seasonal variation in Hg isotopic composition (and elemental concentrations) was likely derived from variable contributions from anthropogenic sources, with continuous input due to industrial activities (e.g., smelting, cement production and coal combustion) in all seasons, whereas coal combustion dominated in winter and biomass burning mainly found in autumn. The more positive Δ199Hg of PM2.5-Hg in spring and early summer was likely derived from long-range-transported Hg that had undergone extensive photochemical reduction. The study demonstrated that Hg isotopes may be potentially used for tracing the sources of particulate Hg and its vectors in the atmosphere.

  5. Probing the homogeneity of the isotopic composition and molar mass of the ‘Avogadro’-crystal

    Science.gov (United States)

    Pramann, Axel; Lee, Kyoung-Seok; Noordmann, Janine; Rienitz, Olaf

    2015-12-01

    Improved measurements on silicon crystal samples highly enriched in the 28Si isotope (known as ‘Si28’ or AVO28 crystal material) have been carried out at PTB to investigate local isotopic variations in the original crystal. This material was used for the determination of the Avogadro constant NA and therefore plays an important role in the upcoming redefinition of the SI units kilogram and mole, using fundamental constants. Subsamples of the original crystal have been extensively studied over the past few years at the National Research Council (NRC, Canada), the National Metrology Institute of Japan (NMIJ, Japan), the National Institute of Standards and Technology (NIST, USA), the National Institute of Metrology (NIM, People’s Republic of China), and multiple times at PTB. In this study, four to five discrete, but adjacent samples were taken from three distinct axial positions of the crystal to obtain a more systematic and comprehensive understanding of the distribution of the isotopic composition and molar mass throughout the crystal. Moreover, improved state-of-the-art techniques in the experimental measurements as well as the evaluation approach and the determination of the calibration factors were utilized. The average molar mass of the measured samples is M  =  27.976 970 12(12) g mol-1 with a relative combined uncertainty uc,rel(M)  =  4.4 ×10-9. This value is in astounding agreement with the values of single samples measured and published by NIST, NMIJ, and PTB. With respect to the associated uncertainties, no significant variations in the molar mass and the isotopic composition as a function of the sample position in the boule were observed and thus could not be traced back to an inherent property of the crystal. This means that the crystal is not only ‘homogeneous’ with respect to molar mass but also has predominantly homogeneous distribution of the three stable Si isotopes.

  6. The bulk isotopic composition of hydrocarbons in subaerial volcanic-hydrothermal emissions from different tectonic settings

    Science.gov (United States)

    Fiebig, J.; Tassi, F.; Vaselli, O.; Viveiros, M. F.; Silva, C.; Lopez, T. M.; D'Alessandro, W.; Stefansson, A.

    2015-12-01

    Assuming that methane and its higher chain homologues derive from a common source, carbon isotope patterns have been applied as a criterion to identify occurrences of abiogenic hydrocarbons. Based on these, it has been postulated that abiogenic hydrocarbon production occurs within several (ultra)mafic environments. More evolved volcanic-hydrothermal systems may also provide all the prerequisites necessary for abiogenic hydrocarbon production, such as availability of inorganic CO2, hydrogen and heat. We have investigated the chemical and isotopic composition of n-alkanes contained within subaerial hydrothermal discharges emitted from a range of hot spot, subduction and rift-related volcanoes to determine the origin of hydrocarbons in these systems. Amongst these are Nisyros (Greece), Vesuvio, Campi Flegrei, Ischia, Pantelleria and Vulcano (all Italy), Mt. Mageik and Trident (USA), Copahue (Argentina), Teide (Spain), Furnas and Fogo (Portugal). The carbon isotopic composition of methane emitted from these sites varies from -65 to -8‰ , whereas δ13C of ethane and propane exhibit a much narrower variation from -17‰ to -31‰. Methane that occurs most enriched in 13C is also characterized by relatively positive δD values ranging up to -80‰. Carbon isotope reversals between methane and ethane are only observed for locations exhibiting δ13C-CH4 values > -20‰, such as Teide, Pantelleria, Trident and Furnas. At Furnas, δ13C-CH4 varies by 50‰ within a relatively short distance of <50m between two vents, whereas δ13C-C2H6 varies by less than 2‰ only. For some of the investigated locations apparent carbon isotopic temperatures between methane and CO2 are in agreement with those derived from gas concentration geothermometers. At these locations methane, however seems to be in disequilibrium with ethane and propane. These findings imply that methane on the one hand and the C2+ hydrocarbons on the other hand often might derive from distinct sources.

  7. Sulfur isotopic composition and source identification of atmospheric environment in central Zhejiang,China

    Institute of Scientific and Technical Information of China (English)

    2010-01-01

    Sulfur dioxide and sulfate aerosols in the atmosphere are significant factors leading to acidification of the atmospheric environment and worsening the pollution of acid deposition. Because of the "fingerprint" characteristics of the stable sulfur isotopic composition, sulfur isotope has been widely adopted in environmental researches concerning sulfur cycle and source identification. In this study, the atmospheric environment of Jinhua City, central Zhejiang Province, was continuously monitored, and the sulfur isotopic composition of SO2 and sulfate aerosols in the atmosphere was analyzed. The results indicate that the variation of δ34S values for SO2 ranges from 1.0‰ to 7.5‰, and annual average is 4.7‰±2.3‰, whereas that of sulfate aerosols ranges from 6.4‰ to 9.8‰,and annual average is 8.1‰±1.0‰. The δ 34S values for SO2 have significant seasonal variations, which are 7.0‰ in winter and 3.3‰ in summer. These variations cannot be attributed to a single factor, and we suggest a temperature-dependent isotope equilibrium fractionation and elevated biogenic sulfur emissions of isotopically light S in summer may be the main controlling mechanisms. Furthermore, we also discuss the δ 34S model of atmospheric SO2 oxidation to form sulfate, and suggest that heterogeneous oxidation dominates in the oxidation reactions of atmospheric SO2 in the central Zhejiang Province. We further suggest that the relative humidity in the atmosphere plays an important role in the oxidation mechanism of atmospheric SO2.

  8. Cerium-modified doped strontium titanate compositions for solid oxide fuel cell anodes and electrodes for other electrochemical devices

    Science.gov (United States)

    Marina, Olga A [Richland, WA; Stevenson, Jeffry W [Richland, WA

    2010-03-02

    The present invention provides novel compositions that find advantageous use in making electrodes for electrochemical cells and electrochemical devices such as solid oxide fuel cells, electrolyzers, sensors, pumps and the like, the compositions comprising cerium-modified doped strontium titanate. The invention also provides novel methods for making and using anode material compositions and solid oxide fuel cells and solid oxide fuel cell assemblies having anodes comprising the compositions.

  9. Copper-substituted perovskite compositions for solid oxide fuel cell cathodes and oxygen reduction electrodes in other electrochemical devices

    Science.gov (United States)

    Rieke, Peter C.; Coffey, Gregory W.; Pederson, Larry R.; Marina, Olga A.; Hardy, John S.; Singh, Prabhaker; Thomsen, Edwin C.

    2010-07-20

    The present invention provides novel compositions that find advantageous use in making electrodes for electrochemical cells. Also provided are electrochemical devices that include active oxygen reduction electrodes, such as solid oxide fuel cells, sensors, pumps and the like. The compositions comprises a copper-substituted ferrite perovskite material. The invention also provides novel methods for making and using the electrode compositions and solid oxide fuel cells and solid oxide fuel cell assemblies having cathodes comprising the compositions.

  10. Determination of optimum electrolyte composition for molten carbonate fuel cells

    Energy Technology Data Exchange (ETDEWEB)

    Yuh, C.Y.; Pigeaud, A.

    1987-01-01

    The goal of this program is the development of a molten carbonate fuel cell (MCFC) anode which is more tolerant of sulfur contaminants in the fuel than the current state-of-the-art nickel-based anode structures. This program addresses two different but related aspects of the sulfur contamination problem. The primary aspect is concerned with the development of a sulfur tolerant electrocatalyst for the fuel oxidation reaction. A secondary issue is the development of a sulfur tolerant water-gas-shift reaction catalyst and an investigation of potential steam reforming catalysts which also have some sulfur tolerant capabilities. These two aspects are being addressed as two separate tasks.

  11. Proof of Concept Simulations of the Multi-Isotope Process Monitor: An Online, Nondestructive, Near-Real-Time Safeguards Monitor for Nuclear Fuel Reprocessing Facilities

    Energy Technology Data Exchange (ETDEWEB)

    Orton, Christopher R.; Fraga, Carlos G.; Christensen, Richard; Schwantes, Jon M.

    2011-02-11

    The International Atomic Energy Agency (IAEA) will require the development of advanced technologies to effectively safeguard nuclear material at increasingly large-scale nuclear recycling facilities. Ideally, the envisioned technologies would be capable of nondestructive, near-real-time, autonomous process monitoring. This paper describes recent results from model simulations designed to test the Multi-Isotope Process (MIP) monitor, a novel approach to safeguarding reprocessing plants. The MIP monitor combines the detection of intrinsic gamma ray signatures emitted from process solutions with multivariate analysis to detect off-normal conditions in process streams nondestructively and in near-real-time. Three computer models including ORIGEN-ARP, AMUSE, and SYNTH were used in series to predict spent nuclear fuel composition, estimate element partitioning during separation, and simulate spectra from product and raffinate streams using a variety of gamma detectors, respectively. Simulations were generated for fuel with various irradiation histories and under a variety of plant operating conditions. Principal component analysis (PCA) was applied to the simulated gamma spectra to investigate pattern variations as a function of acid concentration, burnup, and cooling time. Hierarchical cluster analysis (HCA) and partial least squares (PLS) were also used in the analysis. The MIP monitor was found to be sensitive to induced variations of several operating parameters including distinguishing ±2.5% variation from normal process acid concentrations. The ability of PLS to predict burnup levels from simulated spectra was also demonstrated to be within 3.5% of measured values.

  12. Proof of concept simulations of the Multi-Isotope Process monitor: An online, nondestructive, near-real-time safeguards monitor for nuclear fuel reprocessing facilities

    Science.gov (United States)

    Orton, Christopher R.; Fraga, Carlos G.; Christensen, Richard N.; Schwantes, Jon M.

    2011-02-01

    The International Atomic Energy Agency will require the development of advanced technologies to effectively safeguard nuclear material at increasingly large-scale nuclear recycling facilities. Ideally, the envisioned technologies would be capable of nondestructive, near-real-time, autonomous process monitoring. This paper describes recent results from model simulations designed to test the Multi-Isotope Process (MIP) monitor, a novel addition to a safeguards system for reprocessing facilities. The MIP monitor combines the detection of intrinsic gamma ray signatures emitted from process solutions with multivariate analysis to detect off-normal conditions in process streams nondestructively and in near-real-time. Three computer models including ORIGEN-ARP, AMUSE, and SYNTH were used in series to predict spent nuclear fuel composition, estimate element partitioning during separation, and simulate spectra from product and raffinate streams using a variety of gamma detectors, respectively. Simulations were generated for fuel with various irradiation histories and under a variety of plant operating conditions. Principal component analysis was applied to the simulated gamma spectra to investigate pattern variations as a function of acid concentration, burnup, and cooling time. Hierarchical cluster analysis and partial least squares (PLS) were also used in the analysis. The MIP monitor was found to be sensitive to induced variations of several operating parameters including distinguishing ±2.5% variation from normal process acid concentrations. The ability of PLS to predict burnup levels from simulated spectra was also demonstrated to be within 3.5% of measured values.

  13. Assessing the ability of isotope-enabled General Circulation Models to simulate the variability of Iceland water vapor isotopic composition

    Science.gov (United States)

    Erla Sveinbjornsdottir, Arny; Steen-Larsen, Hans Christian; Jonsson, Thorsteinn; Ritter, Francois; Riser, Camilla; Messon-Delmotte, Valerie; Bonne, Jean Louis; Dahl-Jensen, Dorthe

    2014-05-01

    During the fall of 2010 we installed an autonomous water vapor spectroscopy laser (Los Gatos Research analyzer) in a lighthouse on the Southwest coast of Iceland (63.83°N, 21.47°W). Despite initial significant problems with volcanic ash, high wind, and attack of sea gulls, the system has been continuously operational since the end of 2011 with limited down time. The system automatically performs calibration every 2 hours, which results in high accuracy and precision allowing for analysis of the second order parameter, d-excess, in the water vapor. We find a strong linear relationship between d-excess and local relative humidity (RH) when normalized to SST. The observed slope of approximately -45 o/oo/% is similar to theoretical predictions by Merlivat and Jouzel [1979] for smooth surface, but the calculated intercept is significant lower than predicted. Despite this good linear agreement with theoretical calculations, mismatches arise between the simulated seasonal cycle of water vapour isotopic composition using LMDZiso GCM nudged to large-scale winds from atmospheric analyses, and our data. The GCM is not able to capture seasonal variations in local RH, nor seasonal variations in d-excess. Based on daily data, the performance of LMDZiso to resolve day-to-day variability is measured based on the strength of the correlation coefficient between observations and model outputs. This correlation coefficient reaches ~0.8 for surface absolute humidity, but decreases to ~0.6 for δD and ~0.45 d-excess. Moreover, the magnitude of day-to-day humidity variations is also underestimated by LMDZiso, which can explain the underestimated magnitude of isotopic depletion. Finally, the simulated and observed d-excess vs. RH has similar slopes. We conclude that the under-estimation of d-excess variability may partly arise from the poor performance of the humidity simulations.

  14. VARIATIONS IN ISOTOPIC COMPOSITIONS OF CHLORINE IN EVAPORATION-CONTROLLED SALT LAKE BRINES OF QAIDAM BASIN,CHINA

    Institute of Scientific and Technical Information of China (English)

    2000-01-01

    The variations in the isotopic compositions of chlorine in evaporation-controlled saline lake brines were determined by using an improved procedure for precise measurement of chlorine isotopes based on Cs2Cl+ ion by thermal ionization mass spectrometry. The results showed that variation in δ37Cl values in these evaporation-controlled brines are attributable to evaporation of brine accompanied by the deposition of saline minerals. The isotopic fractionation of chlorine between the deposited saline mineral and the co-existing brine caused the variation of δ37Cl values in the brine. In general the isotopic fractionation of chlorine in nature indicates enrichment of 37Cl in the solid phase relative to 35Cl. The reverse isotopic fractionation of chlorine in which 35Cl is enriched in the solid phase, was observed to some extent during quick deposition under laboratory conditions as well as in nature. The mechanism of isotopic fractionation of chlorine during evaporation deposition was studied.

  15. Measurement of position-specific 13C isotopic composition of propane at the nanomole level

    Science.gov (United States)

    Gilbert, Alexis; Yamada, Keita; Suda, Konomi; Ueno, Yuichiro; Yoshida, Naohiro

    2016-03-01

    We have developed a novel method for analyzing intramolecular carbon isotopic distribution of propane as a potential new tracer of its origin. The method is based on on-line pyrolysis of propane followed by analysis of carbon isotope ratios of the pyrolytic products methane, ethylene and ethane. Using propane samples spiked with 13C at the terminal methyl carbon, we characterize the origin of the pyrolytic fragments. We show that the exchange between C-atoms during the pyrolytic process is negligible, and thus that relative intramolecular isotope composition can be calculated. Preliminary data from 3 samples show that site-preference (SP) values, defined as the difference of δ13C values between terminal and sub-terminal C-atom positions of propane, range from -1.8‰ to -12.9‰. In addition, SP value obtained using our method for a thermogenic natural gas sample is consistent with that expected from theoretical models of thermal cracking, suggesting that the isotope fractionation associated with propane pyrolysis is negligible. The method will provide novel insights into the characterization of the origin of propane and will help better understand the biogeochemistry of natural gas deposits.

  16. Laboratory and Field Measurements of the Nitrogen Isotopic Composition of NOx

    Science.gov (United States)

    Fibiger, D. L.; Miller, D. J.; Dahal, B. R.; Lew, A. F.; Peltier, R.; Hastings, M. G.

    2014-12-01

    The nitrogen isotopic composition of nitrogen oxides (NOx = NO + NO2) has been measured from several NOx emissions sources in prior studies. These measurements have utilized a variety of methods for collecting the NOx as nitrate or nitrite for isotopic analysis, but none of these methods have been verified for complete conversion of NOx. Less than 100% conversion can result in isotopic fractionations. We present a method for accurately measuring the nitrogen isotopic composition of NOx using a .25 M KMnO4 and 0.5 M NaOH solution. Based on laboratory tests, this technique has been found to collect all NOx passed through under a variety of conditions (e.g., air flow rate, NOx concentration, temperature, humidity), allowing for diagnosis of δ15N-NOx without correction for fractionation. The precision across the entire analytic technique is 1.5‰. This active collection method is advantageous for collecting NOx over short time scales in environments with highly variable NOx sources and concentrations. The major drawback of the NaOH/KMnO4 method is a significant nitrate background found in the KMnO4, but this background is consistent and can be easily accounted for. We aim to use this method to provide more robust constraints on the isotopic signatures of NOx emissions from different sources. Initial results will be presented from lab- and field-based collections of NOx emissions. Emissions from a diesel engine were measured in a laboratory smog chamber and yielded δ15N values with a mean of -18.0‰ (n = 5, 1σ = 0.97‰). Measurements of δ15N-NOx were also made on a rooftop between two highways in Providence, RI. The values ranged from -7.7 to -0.63‰ for different time periods sampled, with excellent reproducibility in side-by-side collections. Additionally, the NaOH/KMnO4 was deployed in a laboratory study of biomass burning (FLAME4) to analyze the nitrogen isotopic composition of NOx produced from the burning of variety of materials (e.g. trees, agricultural

  17. Uranium isotope composition of a laterite profile during extreme weathering of basalt in Guangdong, South China

    Science.gov (United States)

    Huang, J.; Zhou, Z.; Gong, Y.; Lundstrom, C.; Huang, F.

    2015-12-01

    Rock weathering and soil formation in the critical zone are important for material cycle from the solid Earth to superficial system. Laterite is a major type of soil in South China forming at hot-humid climate, which has strong effect on the global uranium cycle. Uranium is closely related to the environmental redox condition because U is stable at U(Ⅳ) in anoxic condition and U(Ⅵ) as soluble uranyl ion (UO22+) under oxic circumstance. In order to understand the behavior of U isotopes during crust weathering, here we report uranium isotopic compositions of soil and base rock samples from a laterite profile originated from extreme weathering of basalt in Guangdong, South China. The uranium isotopic data were measured on a Nu Plasma MC-ICP-MS at the University of Illinois at Urbana-Champaign using the double spike method. The δ238U of BCR-1 is -0.29±0.03‰ (relative to the international standard CRM-112A), corresponding to a 238U/235U ratio of 137.911±0.004. Our result of BCR-1 agrees with previous analyses (e.g., -0.28‰ in Weyer et al. 2008) [1]. U contents of the laterite profile decrease from 1.9 ppm to 0.9 ppm with depth, and peak at 160 - 170 cm (2.3 ppm), much higher than the U content of base rocks (~0.5 ppm). In contrary, U/Th of laterites is lower than that of base rock (0.27) except the peak at the depth of 160-170 cm (0.38), indicating significant U loss during weathering. Notably, U isotope compositions of soils show a small variation from -0.38 to -0.28‰, consistent with the base rock within analytical error (0.05‰ to 0.08‰, 2sd). Such small variation can be explained by a "rind effect" (Wang et al., 2015) [2], by which U(Ⅳ) can be completely oxidized to U(VI) layer by layer during basalt weathering by dissolved oxygen. Therefore, our study indicates that U loss during basalt weathering at the hot-humid climate does not change U isotope composition of superficial water system. [1] Weyer S. et al. (2008) Natural fractionation of 238U/235

  18. Space and Time Distribution of Pu Isotopes inside The First Experimental Fuel Pin Designed for PWR and Manufactured in Indonesia

    Science.gov (United States)

    Suwardi; Setiawan, J.; Susilo, J.

    2017-01-01

    The first short fuel pin containing natural UO2 pellet in Zry4 cladding has been prepared and planned to be tested in power ramp irradiation. An irradiation test should be designed to allow an experiment can be performed safely and giving maximum results of many performance aspects of design and manufacturing. Performance analysis to the fuel specimen shows that the specimen is not match to be used for power ramp testing. Enlargement by 0.20 mm of pellet diameter has been proposed. The present work is evaluation of modified design for important aspect of isotopic Pu distribution during irradiation test, because generated Pu isotopes in natural UO2 fuel, contribute more power relative to the contribution by enriched UO2 fuel. The axial profile of neutrons flux have been chosen from both experimental measurement and model calculation. The parameters of ramp power has been obtained from statistical experiment data. A simplified and typical base-load commercial PHWR profile of LHR history has been chosen, to determine the minimum irradiation time before ramp test can be performed. The data design and Mat pro XI materials properties models have been chosen. The axial profile of neutrons flux has been accommodated by 5 slices of discrete pin. The Pu distribution of slice-4 with highest power rate has been chosen to be evaluated. The radial discretion of pellet and cladding and numerical parameter have been used the default best practice of TU. The results shows that Pu 239 increased rapidly. The maximum burn up of slice 4 at upper the median slice, it reached nearly 90% of maximum value at about 6000 h with peak of 0.8%a Pu/HM at 22000 h, which is higher than initial U 235. Each 240, 241 and 240 Pu grows slower and ends up to 0.4, 0.2 and 0.18 % respectively. This results can be used for verification of other aspect of fuel behavior in the modeling results and also can be used as guide and comparison to the future post irradiation examination for Pu isotopes distribution.

  19. Stable isotope composition of land snail body water and its relation to environmental waters and shell carbonate

    Science.gov (United States)

    Goodfriend, Glenn A.; Magaritz, Mordeckai; Gat, Joel R.

    1989-12-01

    Day-to-day and within-day (diel) variations in δD and δ18O of the body water of the land snail, Theba pisana, were studied at a site in the southern coastal plain of Israel. Three phases of variation, which relate to isotopic changes in atmospheric water vapor, were distinguished: 1) on rain days, snail water becomes isotopically depleted approximately in the direction of the rain isotope values, but always less depleted in D as is atmospheric water vapor; 2) during the 1-3 days following a rain, the snail water becomes isotopically enriched along a line with slope persists until the next rain event. The isotopic variations can be explained by isotopic equilibration with atmospheric water vapor and/or uptake of dew derived therefrom. During the winter, when the snails are active, there is only very minor enrichment in 18O relative to equilibrium with water vapor or dew, apparently as a result of metabolic activity. But this enrichment becomes pronounced after long periods of inactivity. Within-day variation in body water isotopic composition is minor on non-rain days. Shell carbonate is enriched in 18O by ca. 1-2%. relative to equilibrium with body water. In most regions, the isotopic composition of atmospheric water vapor (or dew) is a direct function of that of rain. Because the isotopic composition of snail body water is related to that of atmospheric water vapor and the isotopic composition of shell carbonate in turn is related to that of body water, land snail shell carbonate 18O should provide a reliable indication of rainfall 18O. However, local environmental conditions and the ecological properties of the snail species must be taken into account.

  20. Isotope- and tracer-based measurements of fossil fuel and biospheric carbon dioxide in Paris during winter 2010

    Science.gov (United States)

    Lopez, M.; Schmidt, M.; Delmotte, M.; Colomb, A.; Gros, V.; Janssen, C.; Lehman, S. J.; Mondelain, D.; Perrussel, O.; Ramonet, M.; Xueref-Remy, I.; Bousquet, P.

    2013-01-01

    Measurements of the mole fraction of the CO2 and its isotopes were performed in Paris during the MEGAPOLI winter campaign (January-February 2010). Radiocarbon (14CO2) measurements were used to identify the relative contributions of 77% CO2 from fossil fuel consumption (CO2ff from liquid and gas combustion) and 23% from biospheric CO2 (CO2 from the use of biofuels and from human and plant respiration: CO2bio). These percentages correspond to average mole fractions of 26.4 ppm and 8.2 ppm for CO2ff and CO2bio, respectively. The 13CO2 analysis indicated that gas and liquid fuel contributed 70% and 30%, respectively, of the CO2 emission from fossil fuel use. Continuous measurements of CO and NOx and the ratios CO/CO2ff and NOx/CO2ff derived from radiocarbon measurements during four days make it possible to estimate the fossil fuel CO2 contribution over the entire campaign. The ratios CO/CO2ff and NOx/CO2ff are functions of air mass origin and exhibited daily ranges of 7.9 to 14.5 ppb ppm-1 and 1.1 to 4.3 ppb ppm-1, respectively. These ratios are sufficiently consistent with different emission inventories given the uncertainties of the different approaches.

  1. The isotope composition of inorganic germanium in seawater and deep sea sponges

    Science.gov (United States)

    Guillermic, Maxence; Lalonde, Stefan V.; Hendry, Katharine R.; Rouxel, Olivier J.

    2017-09-01

    Although dissolved concentrations of germanium (Ge) and silicon (Si) in modern seawater are tightly correlated, uncertainties still exist in the modern marine Ge cycle. Germanium stable isotope systematics in marine systems should provide additional constraints on marine Ge sources and sinks, however the low concentration of Ge in seawater presents an analytical challenge for isotopic measurement. Here, we present a new method of pre-concentration of inorganic Ge from seawater which was applied to measure three Ge isotope profiles in the Southern Ocean and deep seawater from the Atlantic and Pacific Oceans. Germanium isotopic measurements were performed on Ge amounts as low as 2.6 ng using a double-spike approach and a hydride generation system coupled to a MC-ICP-MS. Germanium was co-precipitated with iron hydroxide and then purified through anion-exchange chromatography. Results for the deep (i.e. >1000 m depth) Pacific Ocean off Hawaii (nearby Loihi Seamount) and the deep Atlantic off Bermuda (BATS station) showed nearly identical δ74/70Ge values at 3.19 ± 0.31‰ (2SD, n = 9) and 2.93 ± 0.10‰ (2SD, n = 2), respectively. Vertical distributions of Ge concentration and isotope composition in the deep Southern Ocean for water depth > 1300 m yielded an average δ74/70Ge = 3.13 ± 0.25‰ (2SD, n = 14) and Ge/Si = 0.80 ± 0.09 μmol/mol (2SD, n = 12). Significant variations in δ74/70Ge, from 2.62 to 3.71‰, were measured in the first 1000 m in one station of the Southern Ocean near Sars Seamount in the Drake Passage, with the heaviest values measured in surface waters. Isotope fractionation by diatoms during opal biomineralization may explain the enrichment in heavy isotopes for both Ge and Si in surface seawater. However, examination of both oceanographic parameters and δ74/70Ge values suggest also that water mass mixing and potential contribution of shelf-derived Ge also could contribute to the variations. Combining these results with new Ge isotope data

  2. Noble gas abundances and isotopic compositions in mantle-derived xenoliths,NE China

    Institute of Scientific and Technical Information of China (English)

    2002-01-01

    Following the researches of helium isotopic compositions in mantle-derived xenoliths in eastern China,this study reported noble gas abundances and isotopic compositions of mantle-derived xenoliths from Kuandian of Liaoning Province, Huinan of Jilin Province and Hannuoba of Hebei Province. Compared with the middle ocean ridge basalt (MORB) and other continental areas, mantle-derived xenoliths in NE China are characterized by slightly low noble gas abundances, 3He/4He equivalent to or lower than that of MORB, 40Ar/36Ar lower than that of MORB, 38Ar/36Ar and Ne-Kr-Xe isotopic ratios equivalent to those of atmosphere. These results indicate the heterogeneity of subcontinentai lithospheric mantle beneath northeastern China, that is, a MORB reservoir-like mantle beneath Kuandian and an enriched/metasomatized mantle beneath Huinan. Low 40Ar/36Ar ratios in the three studied areas may imply that a subducted atmospheric component has been preserved in the subcontinental lithospheric mantle.``

  3. The relationship between carbon and oxygen isotopic composition characteristics of carbonates in loess sediments and paleoclimate

    Institute of Scientific and Technical Information of China (English)

    李春园; 王先彬; 文启彬; 邵波

    1995-01-01

    Based on the carbon and oxygen isotopic compositions of carbonates in loess sediments meas-ured by the methods of stepwise heating and phosphoric acid decomposition from five pieces of samples ofpaleosol,loess and eolian sand,respectively,the distributive characteristics in different temperature steps andthe fractionation mechanisms of carbon and oxygen isotope and their relation to the paleoclirnate are discussed.The preliminary results show that,by means of stepwise heating,different carbon and oxygen isotopiccompositions are obtained in different temperature steps and carbon and oxygen isotopic compositions ofpaleosol,loess and eolian sand are in a different distributive pattern in the range of studied temperaturesteps.The results also show that the δ13C ratios in 700-800℃ are more sensitive tracers of paleoclimatethan those measured by the method of phosphoric acid decomposition.The susceptibility to climatic changesof δ18O ratios analysed by the method of phosphoric acid decomposition is higher than those analysed by themethod of stepwise heating,but the δ18O ratios measured by these two methods do not effectively reflect cli-matic changes.

  4. Tracing the secular evolution of the UCC using the iron isotope composition of ancient glacial diamictites

    Science.gov (United States)

    Liu, X. M.; Gaschnig, R. M.; Rudnick, R. L.; Hazen, R. M.; Shahar, A.

    2015-12-01

    Iron is the fourth most abundant element in the continental crust and influences global climate and biogeochemical cycles in the ocean1. Continental inputs, including river waters, sediments and atmospheric dust are dominant sources (>95%) of iron into the ocean2. Therefore, understanding how continental inputs may have changed through time is important in understanding the secular evolution of the marine Fe cycle. We analysed the Fe isotopic composition of twenty-four glacial diamictite composites, upper continental crust (UCC) proxies, with ages ranging from the Mesoarchean to the Paleozoic eras to characterize the secular evolution of the UCC. The diamictites all have elevated chemical index of alteration (CIA) and other characteristics of weathered regolith (e.g., strong depletion in soluble elements such as Sr), which they inherited from their upper crustal source region3. δ56Fe in the diamictite composites range from -0.59 to +0.23‰, however, most diamictites cluster with an average δ56Fe of 0.11± 0.20 (2s), overlapping juvenile continental material such as island arc basalts (IABs), which show a narrow range in δ56Fe from -0.04 to +0.14 ‰4. There is no obvious correlation between δ56Fe of the glacial diamictites and the CIA, except that the diamictite with the lowest δ56Fe at -0.59 ‰ also has the highest CIA = 89 (the Paleoproterozoic Makganyene Fm.). The data suggest that the Fe isotope compositions in the upper continental crust did not vary throughout Earth history. Interestingly, chemical weathering and sedimentary transport likely play only a minor role in producing Fe isotope variations in the upper continental crust. Anoxic weathering pre-GOE (Great Oxidation Event) does not seem to generate different Fe isotopic signatures from the post-GOE oxidative weathering environment in the upper continental crust. Therefore, large Fe isotopic fractionations observed in various marine sedimentary records are likely due to other processes occurring

  5. Mineral composition control on inter-mineral iron isotopic fractionation in granitoids

    Science.gov (United States)

    Wu, Hongjie; He, Yongsheng; Bao, Leier; Zhu, Chuanwei; Li, Shuguang

    2017-02-01

    This study reports elemental and iron isotopic compositions of feldspar and its coexisting minerals from four Dabie I-type granitoids to evaluate the factors that control inter-mineral Fe isotopic fractionation in granitoids. The order of heavy iron isotope enrichment is feldspar > pyrite > magnetite > biotite ≈ hornblende. Feldspar has heavier iron isotopic compositions than its co-existing magnetite (Δ56Feplagioclase-magnetite = +0.376‰ to +1.084‰, Δ56Fealkali-feldspar-magnetite = +0.516‰ to +0.846‰), which can be attributed to its high Fe3+/Fetot ratio and low coordination number (tetrahedrally-coordinated) of Fe3+. Δ56Femagnetite-biotite of coexisting magnetite and biotite ranges from 0.090‰ to 0.246‰. Based on homogeneous major and iron isotopic compositions of mineral replicates, the inter-mineral fractionation in this study should reflect equilibrium fractionation. The large variations of inter-mineral fractionation among feldspar, magnetite and biotite cannot be simply explained by temperature variation, but strongly depend on mineral compositions. The Δ56Feplagioclase-magnetite and Δ56Fealkali-feldspar-magnetite are positively correlated with albite mode in plagioclase and orthoclase mode in alkali-feldspar, respectively. This could be explained by different Fe-O bond strength in feldspar due to different Fe3+/∑Fe or different crystal parameters. The Δ56Femagnetite-biotite increases with decreasing Fe3+/∑Febiotite and increasing mole (Na + K)/Mgbiotite, indicating a decrease of β factor in low Fe3+/∑Fe and high (Na + K)/Mg biotite. High-silica leucosomes from Dabie migmatites with a feldspar accumulation petrogenesis have higher δ56Fe values (δ56Fe = 0.42-0.567‰) than leucosome that represents pristine partial melt (δ56Fe = 0.117 ± 0.016‰), indicating that accumulation of feldspar could account for high δ56Fe values of these rocks. High δ56Fe values are also predicted for other igneous rocks that are mainly composed of

  6. Hydrogen isotopic composition of the Martian mantle inferred from the newest Martian meteorite fall, Tissint

    Science.gov (United States)

    Mane, P.; Hervig, R.; Wadhwa, M.; Garvie, L. A. J.; Balta, J. B.; McSween, H. Y.

    2016-11-01

    The hydrogen isotopic composition of planetary reservoirs can provide key constraints on the origin and history of water on planets. The sources of water and the hydrological evolution of Mars may be inferred from the hydrogen isotopic compositions of mineral phases in Martian meteorites, which are currently the only samples of Mars available for Earth-based laboratory investigations. Previous studies have shown that δD values in minerals in the Martian meteorites span a large range of -250 to +6000‰. The highest hydrogen isotope ratios likely represent a Martian atmospheric component: either interaction with a reservoir in equilibrium with the Martian atmosphere (such as crustal water), or direct incorporation of the Martian atmosphere due to shock processes. The lowest δD values may represent those of the Martian mantle, but it has also been suggested that these values may represent terrestrial contamination in Martian meteorites. Here we report the hydrogen isotopic compositions and water contents of a variety of phases (merrillites, maskelynites, olivines, and an olivine-hosted melt inclusion) in Tissint, the latest Martian meteorite fall that was minimally exposed to the terrestrial environment. We compared traditional sample preparation techniques with anhydrous sample preparation methods, to evaluate their effects on hydrogen isotopes, and find that for severely shocked meteorites like Tissint, the traditional sample preparation techniques increase water content and alter the D/H ratios toward more terrestrial-like values. In the anhydrously prepared Tissint sample, we see a large range of δD values, most likely resulting from a combination of processes including magmatic degassing, secondary alteration by crustal fluids, shock-related fractionation, and implantation of Martian atmosphere. Based on these data, our best estimate of the δD value for the Martian depleted mantle is -116 ± 94‰, which is the lowest value measured in a phase in the

  7. Gas Compositions and He-C Isotopic Ratios of Fumarolic Samples from Negros Island, Central Philippines

    Science.gov (United States)

    Lee, Hsiao-Fen; Yang, Tsanyao Frank; Faith Lan, Tefang; Chen, Yue-Gau; Sincioco, Jaime S.; Solidum, Renato U., Jr.

    2010-05-01

    Four volcanoes that are distributed in the Negros Island, Central Philippines, include Kanlaon Volcano which is considered as one of the most active volcanoes in Philippines. All of these volcanoes are related to subduction system of Negros trench and form the Negros volcanic arc. Besides Kanlaon, from north to south, the volcanoes in Negros Island are Silay Volcano, Mandalagan Volcano and Cuernos de Negros Volcano. Although there is no eruption record of these three volcanoes in last 10,000 years, due to the ongoing solfataric/fumarolic activities, the Philippine Institute of Volcanology and Seismology (PHIVOLCS) classifies these as 'potentially active' volcanoes. It means that there is still a considerable threat and risk of eruption. Fumarolic gas samples and bubbling gas samples of hot spring were collected in February 2007 and April 2008 to compare the compositions with others in the world. We analyzed the gas composition, carbon isotopes of CO2, and helium isotopes of these samples. The results of these samples show a similar composition as those of low-temperature fumaroles in other parts of the world, i.e., temperature 1. H2O is the major species of these gas samples, and CO2 is the dominant component after de-watering. Minor components include H2S, N2 and CH4. The gas composition of most of these samples falls in the range of affinity with convergent plate gases associated with groundwater based on the plot of N2-He-Ar diagram. The high 3He/4He ratios indicate a mantle-derived degassing source in origin, i.e., magma chambers could still exist beneath these volcanoes. Helium isotopes ratios show a decreasing trend from north to south, such distribution could be due to more crustal contamination caused by the collision event which happened in the northern part of the island. The carbon isotopic values of CO2 are far less negative than the values from a magma source. There are other carbon sources of CO2, most likely a thick sequence of limestone formation in

  8. Chemical and Isotope Compositions of Neogene Hippopotamidae Teeth From Lake Albert (Uganda): Implications for Environmental Change

    Science.gov (United States)

    Brugmann, G. E.; Brachert, T. C.; Ssemmanda, I.; Mertz, D. F.

    2008-12-01

    The Neogene was a period of long-term global cooling and increasing climatic variability on astronomical time scales. Lake systems strongly depend on rainfall patterns and size or geographical distribution of river networks. To unravel environmental change and watershed dynamics in the western branch of the East African Rift (Lake Albert, Uganda) during the Late Neogene, we use proxy data (trace elements, O, C and Sr isotopes) from Hippopotamidae teeth. Laser ablation ICPMS profiles in enamel measured from the outside rim towards the dentin show an asymmetric trace element distribution in that the concentrations continuously decrease by up to 5 orders of magnitude within a distance of about 1 mm until a minimum is reached (migration pathways and palaeoenvironmental changes. On geological time scales δ13C compositions reflect a transition from pure C3 browsers (-11 per mil PDB) at 5 to 6 Ma towards C4 dominated grazers (0 per mil PDB) at 2.0 to 2.5 Ma. The oxygen stable isotope (δ18O) composition of enamel rises from 26 per mil at 5 to 6 Ma to a maximum of 32 per mil SMOW at 2.3 Ma. Increasing δ18O values suggest enhanced evaporation of the lake due to rising aridity. This is in agreement with a synchronous spread of C4 vegetation in the reach of Hippopotamid populations. The Sr isotopic composition of enamel displays a large variation and 87Sr/86Sr is 0.714 about 5 Ma ago, reaches a maximum of 0.717 at about 2.3 Ma and decreases from there on to about 0.708. Thus, Sr and O isotopic compositions correlate with each other on the geological time scale. This is plausible if the Sr isotopic composition of Hippopotamid enamel dominantly reflects the changes of the water chemistry of the lake, and is therefore a powerful tool for tracing ancient hydrological networks. The large variation of the Sr isotope composition can be explained if the lake is fed by different sources: water draining Cenozoic volcanic terrains have low 87Sr/86Sr (~ 0.704), whereas Proterozoic

  9. Chlorine isotopic compositions of deep saline fluids in Ibusuki coastal geothermal region, Japan : using B–Cl isotopes to interpret fluid sources

    NARCIS (Netherlands)

    Musashi, Masaaki; Oi, Takao; Kreulen, Rob

    2015-01-01

    We report chlorine stable isotopic compositions (δ37Cl, expressed in ‰ relative to the standard mean ocean chloride) as well as δ2H and δ18O values of deep saline fluids taken at eight drill-holes reaching from 73 to 780 m below sea level in the Ibusuki coastal geothermal region, Japan. Analytical r

  10. Molecular and carbon isotopic compositions of gas inclusions of deep carbonate rocks in the Tarim Basin

    Institute of Scientific and Technical Information of China (English)

    ZHOU Shixin; WANG Xianbin; MENG Zifang; LI Yuan; Paul Farrimond; LI Liwu; DUAN Yi

    2004-01-01

    Gaseous components of gas inclusions in deep carbonate rocks (>5700 m) from the Tacan 1 well were analyzed by online mass spectrometry by means of either the stepwise heating technique or vacuum electromagnetism crushing. The carbon isotopic compositions of gases released by vacuum electromagnetism crushing were also measured. Although the molecular compositions of gas inclusions show differences between the two methods, the overall characteristics are that gas inclusions mainly contain CO2, whilst hydrocarbon gases, such as CH4, C2H6 and C3H8, are less abundant. The content of CO is higher in the stepwise heating experiment than that in the method of vacuum electromagnetism crushing, and there are only minor amounts of N2, H2 and O2 in gas inclusions. Methane δ13C values of gas inclusions in Lower Ordovician and Upper Cambrian rocks (from 5713.7 to 6422 m; -52‰-63‰) are similar to those of bacterial methane, but their chemical compositions do not exhibit the dry character in comparison with biogenic gases. These characteristics of deep gas inclusions may be related to the migration fractionation. Some deep natural gases with light carbon isotopic characteristics in the Tazhong Uplift may have a similar origin. The δ13C1 values of gas inclusions in Lower Cambrian rocks (7117-7124 m) are heavier (-39‰), consistent with highly mature natural gases. Carbon isotopic compositions of CO2 in the gas inclusions of deep carbonate rocks are similar (from -4‰ to -13‰) to those of deep natural gases, indicating predominantly an inorganic origin.

  11. Carbon nanotubes based nafion composite membranes for fuel cell applications

    CSIR Research Space (South Africa)

    Cele, NP

    2009-01-01

    Full Text Available surface oxidation as well as functionalisation in composite membranes was investigated by focussing on three aspects: thermo-mechanical stability, thermal degradation and proton conductivity. The oCNTs-containing Nafion composite membrane exhibited...

  12. Oxygen isotopic compositions of zircons from pyroxenite of Daoshichong, Dabieshan: Implications for crust-mantle interaction

    Institute of Scientific and Technical Information of China (English)

    2002-01-01

    Oxygen isotopic compositions of zircons from pyroxenite (~145 Ma) of Daoshichong, Dabieshan have been measured by an ion microprobe. Both within the single grain and among different grains, oxygen isotopic ratios are homogeneous, δ 18O = (7.66‰±0.46)‰ (1 SD, 1 σ = 0.10, n = 22). High δ 18O values indicate that the mantle-derived parent magma of Daoshichong pyroxenite have undergone interaction with crustal materials. Combing with other geochemical constraints, the way of crust-mantle interaction is suggested to be source mixing other than crustal contamination. The time interval between crust-mantle interaction and formation of the parent magma of Daoshichong pyroxenite is less than several million years. The crustal component involving in crust-mantle interaction is mafic lower crust, and the parent magma of pyroxenite possibly contain large proportion (>37%) of such lower crust.

  13. Mass-independent isotopic compositions in terrestrial and extraterrestrial solids and their applications.

    Science.gov (United States)

    Thiemens, M H; Savarino, J; Farquhar, J; Bao, H

    2001-08-01

    In 1983, Thiemens and Heidenreich reported the first chemically produced mass-independent isotope effect. This work has been shown to have a wide range of applications, including atmospheric chemistry, solar system evolution, and chemical physics. This work has recently been reviewed (Weston, R. E. Chem. Rev. 1999, 99, 2115-2136; Thiemens, M. H. Science 1999, 283, 341-345). In this Account, observations of mass-independent isotopic compositions in terrestrial and Martian solids are reviewed. A wide range of applications, including formation and transport of aerosols in the present atmosphere, chemistry of ancient atmospheres and oceans, history and coupling of the atmosphere-surface in the Antarctic dry valleys, origin and evolution of oxygen in the Earth's earliest environment, and the chemistry of the atmosphere and surface of Mars, are discussed.

  14. Isotopic Details of the Spent Catawba-1 MOX Fuel Rods at ORNL

    Energy Technology Data Exchange (ETDEWEB)

    Ellis, Ronald James [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

    2015-04-01

    The United States Department of Energy funded Shaw/AREVA MOX Services LLC to fabricate four MOX Lead Test Assemblies (LTA) from weapons-grade plutonium. A total of four MOX LTAs (including MX03) were irradiated in the Catawba Nuclear Station (Unit 1) Catawba-1 PWR which operated at a total thermal power of 3411 MWt and had a core with 193 total fuel assemblies. The MOX LTAs were irradiated along with Duke Energy s irradiation of eight Westinghouse Next Generation Fuel (NGF) LEU LTAs (ref.1) and the remaining 181 LEU fuel assemblies. The MX03 LTA was irradiated in the Catawba-1 PWR core (refs.2,3) during cycles C-16 and C-17. C-16 began on June 5, 2005, and ended on November 11, 2006, after 499 effective full power days (EFPDs). C-17 started on December 29, 2006, (after a shutdown of 48 days) and continued for 485 EFPDs. The MX03 and three other MOX LTAs (and other fuel assemblies) were discharged at the end of C-17 on May 3, 2008. The design of the MOX LTAs was based on the (Framatome ANP, Inc.) Mark-BW/MOX1 17 17 fuel assembly design (refs. 4,5,6) for use in Westinghouse PWRs, but with MOX fuel rods with three Pu loading ranges: the nominal Pu loadings are 4.94 wt%, 3.30 wt%, and 2.40 wt%, respectively, for high, medium, and low Pu content. The Mark-BW/MOX1 (MOX LTA) fuel assembly design is the same as the Advanced Mark-BW fuel assembly design but with the LEU fuel rods replaced by MOX fuel rods (ref. 5). The fabrication of the fuel pellets and fuel rods for the MOX LTAs was performed at the Cadarache facility in France, with the fabrication of the LTAs performed at the MELOX facility, also in France.

  15. Assessment of dissolved Pb concentration and isotopic composition in surface waters of the modern global ocean

    Science.gov (United States)

    Pinedo-Gonzalez, P.; West, A. J.; Sanudo-Wilhelmy, S. A.

    2015-12-01

    Lead (Pb) produced by human activities, mainly from leaded gasoline combustion and high-temperature industries, dominates Pb in our present-day oceans. Previous studies have shown that surface ocean Pb concentrations and isotope ratios have varied in time and space, reflecting the changes in the amount of inputs and sources of anthropogenic Pb. However, data on surface ocean Pb is quite limited, especially for some basins like the Indian Ocean. In the present study, Pb concentrations and stable isotopes (208, 207, and 206) have been analyzed in surface water samples (3m depth) collected during the Malaspina Circumnavigation Expedition, 2010. Our results are compared with data from the literature to i) evaluate the changing status of metal contamination in surface waters of the global ocean over the last 30 years, and ii) propose potential sources of modern Pb to the oceans. Our results show that Pb concentrations in surface waters of the North Atlantic Ocean have decreased ~ 40% since 1975, attributable to the phase-out of leaded gasoline in North America. This result is corroborated by stable Pb isotope measurements. Furthermore, the isotopic gradient observed in surface waters of the studied transects in the north tropical and subtropical Atlantic Ocean can be attributed to simple mixing of European and African aerosols and Saharan Holocene loess. Results from an understudied transect in the Southern Indian Ocean give an indication of the source region of Pb delivered to this region. Although comparison with literature data is limited, mixing of Australian ores and African and Australian coals could potentially explain the measured Pb isotope composition. This study provides an opportunity to build on the work of previous oceanographic campaigns, enabling us to assess the impact of anthropogenic Pb inputs to the ocean and the relative importance of various Pb sources, providing new insights into the transport and fate of Pb in the oceans.

  16. Triple oxygen isotope composition of leaf waters in Mpala, central Kenya

    Science.gov (United States)

    Li, Shuning; Levin, Naomi E.; Soderberg, Keir; Dennis, Kate J.; Caylor, Kelly K.

    2017-06-01

    Variations in triple oxygen isotopes have been used in studies of atmospheric photochemistry, global productivity and increasingly in studies of hydroclimate. Understanding the distribution of triple oxygen isotopes in plant waters is critical to studying the fluxes of oxygen isotopes between the atmosphere and hydrosphere, in which plants play an important role. In this paper we report triple oxygen isotope data for stem and leaf waters from Mpala, Kenya and explore how Δ17 O, the deviation from an expected relationship between 17O /16O and 18O /16O ratios, in plant waters vary with respect to relative humidity and deuterium excess (d-excess). We observe significant variation in Δ17 O among waters in leaves and stems from a single plant (up to 0.16‰ range in Δ17 O in leaf water in a plant over the course of a signal day), which correlates to changes in relative humidity. A steady state model for evaporation in leaf water reproduces the majority of variation in Δ17 O and d-excess we observed in leaf waters, except for samples that were collected in the morning, when relative humidity is high and the degree of fractionation in the system is minimal. The data and the steady state model indicate that the slope, λtransp, that links δ17 O and δ18 O values of stem and leaf waters and characterizes the fractionation during transpiration, is strongly influenced by the isotopic composition of ambient vapor when relative humidity is high. We observe a strong, positive relationship between d-excess and Δ17 O, with a slope 2.2 ± 0.2 per meg ‰-1, which is consistent with the observed relationship in tropical rainfall and in water in an evaporating open pan. The strong linear relationship between d-excess and Δ17 O should be typical for any process involving evaporation or any other fractionation that is governed by kinetic effects.

  17. Isotopic composition of dissolved iron in the Equatorial Pacific and the Southern oceans

    Science.gov (United States)

    Radic, A.; Lacan, F.; Jeandel, C.; Poitrasson, F.; Sarthou, G.

    2009-12-01

    Iron is a fundamental element linking ocean biogeochemistry and climate. Iron isotopes are a very promising tool for the study of the iron oceanic cycle, notably for tracing its sources to the ocean and/or for studying its speciation. Several studies reports iron isotopic data in the marine environment: in plankton tows, pore waters, aerosols, seafloor or marginal seas (Bergquist and Boyle, 2006; Severmann et al., 2006; De Jong et al., 2007). To link these isotopic data together and to fully study the iron isotope marine cycle, we need to document the central reservoir in the marine environment : dissolved iron in seawater, espacially in High Nutrient Low Chlorophyll (NHLC) areas. So far there are very few comunicated data of dissolved iron isotopic composition in the open ocean (Rouxel, 2008; Lacan et al., 2008; John and Andkins, 2009;). Here, the first profiles in HNLC areas will be presented : 2 full-depth profiles in the Equatorial Pacific Ocean (EUCFe 2006), 2 full-depth profiles in the Atlantic sector of the Southern Ocean (Bonus-GoodHope 2008) and some data from the Kerguelen area (Southern Ocean, KEOPS 2005). δ56Fe values range from -0.7‰ to more than 1.0‰. All the samples from the Equatorial Pacific Ocean display positive values (heavy iron) whereas samples from the Sourthern Ocean display rather negative values (light iron), especially around 450 m deepth. These results will be discussed in terms of iron sources to ocean. Potential applications of this new tracer for studying internal oceanic processes, such as biological uptake, will be discussed.

  18. Mercury Stable Isotopic Composition of Monomethylmercury in Estuarine Sediments and Pure Cultures of Mercury Methylating Bacteria

    Science.gov (United States)

    Janssen, S.; Johnson, M. W.; Barkay, T.; Blum, J. D.; Reinfelder, J. R.

    2014-12-01

    Tracking monomethylmercury (MeHg) from its source in soils and sediments through various environmental compartments and transformations is critical to understanding its accumulation in aquatic and terrestrial food webs. Advances in the field of mercury (Hg) stable isotopes have allowed for the tracking of discrete Hg sources and the examination of photochemical and bacterial transformations. Despite analytical advances, measuring the Hg stable isotopic signature of MeHg in environmental samples or laboratory experiments remains challenging due to difficulties in the quantitative separation of MeHg from complex matrices with high concentrations of inorganic Hg. To address these challenges, we have developed a MeHg isolation method for sediments and bacterial cultures which involves separation by gas chromatography. The MeHg eluting from the GC is passed through a pyrolysis column and purged onto a gold amalgam trap which is then desorbed into a final oxidizing solution. A MeHg reference standard carried through our separation process retained its isotopic composition within 0.02 ‰ for δ202Hg, and for native estuarine sediments, MeHg recoveries were 80% to 100%. For sediment samples from the Hackensack and Passaic Rivers (New Jersey, USA), δ202Hg values for MeHg varied from -1.2 to +0.58 ‰ (relative to SRM 3133) and for individual samples were significantly different from that of total Hg (-0.38 ± 0.06 ‰). No mass independent fractionation was observed in MeHg or total Hg from these sediments. Pure cultures of Geobacter sulfurreducens, grown under fermentative conditions showed preferential enrichment of lighter isotopes (lower δ202Hg) during Hg methylation. The Hg stable isotope signatures of MeHg in sediments and laboratory methylation experiments will be discussed in the context of the formation and degradation of MeHg in the environment and the bioaccumulation of MeHg in estuarine food webs.

  19. Carbon isotopic composition of fossil leaves from the Early Cretaceous sediments of western India

    Indian Academy of Sciences (India)

    S Chakraborty; B N Jana; S K Bhattacharya; I Robertson

    2011-08-01

    Stable carbon isotope analysis of fossil leaves from the Bhuj Formation, western India was carried out to infer the prevailing environmental conditions. Compression fossil leaves such as Pachypteris indica, Otozamite kachchhensis, Brachyphyllum royii and Dictyozamites sp. were recovered from three sedimentary successions of the Bhuj Formation, Early Cretaceous in age. A chronology was established based on faunal assemblage and palyno-stratigraphy and further constrained by carbon isotope stratigraphy. The three sampling sites were the Karawadi river bank near Dharesi; the Chawad river bank near Mathal; and the Pur river section near Trambau village in Gujarat. The Dharesi sample was also analyzed to investigate intra-leaf 13C variability. The mean 13C of the leaf was −24.6 ± 0.4‰ which implied negligible systematic change along the leaf axis. The Mathal sample was fragmented in nature and showed considerable variation in carbon isotopic composition. The Trambau sample considered to be the oldest, dating to the middle of Aptian (ca. 116 Ma), shows the most depleted value in 13C among all of them. The overall 13C trend ranging from mid Aptian (ca. 116 Ma) to early Albian (ca. 110 Ma) shows a progressive increase in 13C from −26.8 to −20.5‰. Based on these measurements the carbon isotopic composition of atmospheric carbon dioxide of the Aptian–Albian period is estimated to be between −7.4 and −1.7‰. The ratio of the partial pressure of carbon dioxide in leaf to that of the ambient atmosphere calculated based on a model is estimated to be similar to that of the modern plants. This indicates that the Early-Cretaceous plants adapted to the prevailing high carbon dioxide regime by increasing their photosynthetic uptake.

  20. Altitude effect on leaf wax carbon isotopic composition in humid tropical forests

    Science.gov (United States)

    Wu, Mong Sin; Feakins, Sarah J.; Martin, Roberta E.; Shenkin, Alexander; Bentley, Lisa Patrick; Blonder, Benjamin; Salinas, Norma; Asner, Gregory P.; Malhi, Yadvinder

    2017-06-01

    The carbon isotopic composition of plant leaf wax biomarkers is commonly used to reconstruct paleoenvironmental conditions. Adding to the limited calibration information available for modern tropical forests, we analyzed plant leaf and leaf wax carbon isotopic compositions in forest canopy trees across a highly biodiverse, 3.3 km elevation gradient on the eastern flank of the Andes Mountains. We sampled the dominant tree species and assessed their relative abundance in each tree community. In total, 405 sunlit canopy leaves were sampled across 129 species and nine forest plots along the elevation profile for bulk leaf and leaf wax n-alkane (C27-C33) concentration and carbon isotopic analyses (δ13C); a subset (76 individuals, 29 species, five forest plots) were additionally analyzed for n-alkanoic acid (C22-C32) concentrations and δ13C. δ13C values display trends of +0.87 ± 0.16‰ km-1 (95% CI, r2 = 0.96, p families, suggesting the biochemical response to environment is robust to taxonomic turnover. We calculate fractionations and compare to adiabatic gradients, environmental variables, leaf wax n-alkane concentrations, and sun/shade position to assess factors influencing foliar chemical response. For the 4 km forested elevation range of the Andes, 4-6‰ higher δ13C values are expected for upland versus lowland C3 plant bulk leaves and their n-alkyl lipids, and we expect this pattern to be a systematic feature of very wet tropical montane environments. This elevation dependency of δ13C values should inform interpretations of sedimentary archives, as 13C-enriched values may derive from C4 grasses, petrogenic inputs or upland C3 plants. Finally, we outline the potential for leaf wax carbon isotopes to trace biomarker sourcing within catchments and for paleoaltimetry.

  1. Optimisation of composite metallic fuel for minor actinide transmutation in an accelerator-driven system

    Science.gov (United States)

    Uyttenhove, W.; Sobolev, V.; Maschek, W.

    2011-09-01

    A potential option for neutralization of minor actinides (MA) accumulated in spent nuclear fuel of light water reactors (LWRs) is their transmutation in dedicated accelerator-driven systems (ADS). A promising fuel candidate dedicated to MA transmutation is a CERMET composite with Mo metal matrix and (Pu, Np, Am, Cm)O 2-x fuel particles. Results of optimisation studies of the CERMET fuel targeting to increasing the MA transmutation efficiency of the EFIT (European Facility for Industrial Transmutation) core are presented. In the adopted strategy of MA burning the plutonium (Pu) balance of the core is minimized, allowing a reduction in the reactivity swing and the peak power form-factor deviation and an extension of the cycle duration. The MA/Pu ratio is used as a variable for the fuel optimisation studies. The efficiency of MA transmutation is close to the foreseen theoretical value of 42 kg TW -1 h -1 when level of Pu in the actinide mixture is about 40 wt.%. The obtained results are compared with the reference case of the EFIT core loaded with the composite CERCER fuel, where fuel particles are incorporated in a ceramic magnesia matrix. The results of this study offer additional information for the EFIT fuel selection.

  2. Conceptual Process for the Manufacture of Low-Enriched Uranium/Molybdenum Fuel for the High Flux Isotope Reactor

    Energy Technology Data Exchange (ETDEWEB)

    Sease, J.D.; Primm, R.T. III; Miller, J.H.

    2007-09-30

    The U.S. nonproliferation policy 'to minimize, and to the extent possible, eliminate the use of HEU in civil nuclear programs throughout the world' has resulted in the conversion (or scheduled conversion) of many of the U.S. research reactors from high-enriched uranium (HEU) to low-enriched uranium (LEU). A foil fuel appears to offer the best option for using a LEU fuel in the High Flux Isotope Reactor (HFIR) without degrading the performance of the reactor. The purpose of this document is to outline a proposed conceptual fabrication process flow sheet for a new, foil-type, 19.75%-enriched fuel for HFIR. The preparation of the flow sheet allows a better understanding of the costs of infrastructure modifications, operating costs, and implementation schedule issues associated with the fabrication of LEU fuel for HFIR. Preparation of a reference flow sheet is one of the first planning steps needed in the development of a new manufacturing capacity for low enriched fuels for U.S. research and test reactors. The flow sheet can be used to develop a work breakdown structure (WBS), a critical path schedule, and identify development needs. The reference flow sheet presented in this report is specifically for production of LEU foil fuel for the HFIR. The need for an overall reference flow sheet for production of fuel for all High Performance Research Reactors (HPRR) has been identified by the national program office. This report could provide a starting point for the development of such a reference flow sheet for a foil-based fuel for all HPRRs. The reference flow sheet presented is based on processes currently being developed by the national program for the LEU foil fuel when available, processes used historically in the manufacture of other nuclear fuels and materials, and processes used in other manufacturing industries producing a product configuration similar to the form required in manufacturing a foil fuel. The processes in the reference flow sheet are

  3. Carbon elemental and isotopic composition in mantle xenoliths from Spain: Insights on sources and petrogenetic processes

    Science.gov (United States)

    Bianchini, G.; Natali, C.

    2017-02-01

    The carbon elemental concentration (C wt%) and isotopic (δ13C ‰) composition of mantle xenoliths from the Tallante and Calatrava volcanic occurrences (in South-East and Central Spain, respectively) have been investigated to identify carbon sources and processes occurring in distinct geodynamic settings of the Iberian Peninsula. The peridotitic mantle xenoliths from Calatrava show elemental C ranging from 0.11 to 2.87 wt% which is coupled with a continuous isotopic variation from very negative values (δ13C - 26.1‰) to typical mantle values (δ13C - 5.9‰). On the other hand, the Tallante mantle xenolith suite displays lower C contents (0.06-0.15 wt%) showing a tighter variation with 13C-depleted values ranging between - 20.1 and - 23.7‰; higher elemental C up to 0.41 wt% displaying distinctly less negative isotopic values (δ13C between - 13.8 and - 11.9‰) have been recorded in veins crosscutting Tallante peridotites, plausibly representing the product of metasomatic reactions. The data from the two investigated xenolith suites invariably display a good correlation between elemental and isotopic composition, suggesting a mantle origin for carbon and Rayleigh-type fractionation as the process responsible for the observed C-δ13C variation. However, the correlation between the carbon isotopic data with other isotopic tracers (e.g. 87Sr/86Sr, 3He/4He) used to identify distinct mantle components and metasomatic reactions, indicates systematic differences between the two xenolith suites suggesting that beneath the Betic Cordillera (where Tallante is located) the deep C-cycle involves recycling, via subduction preceding/accompanying continental collision, of crustal components back in the mantle. Coherently, geochemical trends observed in the Tallante xenoliths seem to be influenced by metasomatic agents generated by melting of crustal lithologies that according to the analysis of a metasedimentary xenolith can contain C up to 1.2 wt% having δ13C of ca. - 18

  4. Preservation of Primary Carbonate Clumped Isotope Compositions: Insights from Fossil Brachiopod Calcite

    Science.gov (United States)

    Henkes, G. A.; Perez-Huerta, A.; Grossman, E. L.; Passey, B. H.

    2016-12-01

    Invertebrate fossils, mainly mollusks and brachiopods, are keystone recorders of primary elemental and isotopic compositions of ancient oceans. Certifying these biominerals as robust archives has been the focus of decades of study, the results of which have established petrographic and geochemical diagenetic screening tests for identifying ostensibly pristine fossils. Despite this fact, the oxygen isotope (δ18O) thermometer `water problem'—the unknown seawater δ18O over most of Earth's history—has restricted shell δ18O paleothermometry. Carbonate clumped isotopes are a promising solution, but the study of preservation of primary compositions is in relative infancy. Analyses of brachiopod shells have confirmed that while petrographic and geochemical tests effectively screen for `open-system' exchange, they do not completely address `closed-system' exchange. Elevated clumped isotope temperatures (T(Δ47)) without signs for recrystallization have been attributed to solid-state C-O bond reordering, which re-equilibrate the 13C-18O bonds that are the basis of the thermometer at elevated burial temperatures. Currently there are no a priori methods for identifying geologic samples that have been affected by bond reordering. An alternative approach is to employ experimentally validated kinetic models to test whether a sample has passed through burial conditions—temperatures >100°C for timescales <108 years—that would've activated reordering. New and existing experimental data on reordering reaction kinetics confirm that the rate constants are virtually identical for an optical spar and brachiopod and crinoid fossils, suggesting uniform behavior across calcite morphologies during heating. Yet questions remain over distinguishing marginal clumped isotope reordering from cryptic recrystallization in natural samples. To this end, we are exploring electron backscatter diffraction as an additional test for confirming isotopic preservation over geologic timescales

  5. Fuel Composition Analysis of Endothermically Heated JP-8 Fuel for Use in a Pulse Detonation Engine

    Science.gov (United States)

    2008-06-01

    0.15 0.14 0.03 0.11 0.07 0.12 0.13 0.14 0.14 Methyl -cyclohexane * 3.38 0.13 0.25 0.30 0.37 0.38 0.18 0.31 0.26 0.31 0.28 0.32 0.33 Ethyl -cyclopentane...FUEL FOR USE IN A PULSE DETONATION ENGINE I. Introduction Motivation JP-8 is the predominant kerosene fuel currently used in the United States Air...Thermal Decomposition The fuel of choice for this research is JP-8 for many practical reasons. JP-8 is the predominant kerosene fuel currently used

  6. Isotopic composition and identification of the origins of individuals buried in a Neolithic collective grave at Bronocice (southern Poland).

    Science.gov (United States)

    Szostek, K; Haduch, E; Stepańczak, B; Kruk, J; Szczepanek, A; Pawlyta, J; Głąb, H; Milisauskas, S

    2014-04-01

    The oxygen present in a human organism comes from numerous sources, but the major factor that causes variation in the isotopic composition of this element in a tissue is available drinking water. The isotopic ratio of oxygen in an organism's tissue, including that found in bones and teeth, reflects the isotopic oxygen composition typical for the area where a given individual developed and lived. Of particular interest with regard to this issue were a series of skeletons from the multiple grave discovered at the Funnel Beaker-Baden settlement at Bronocice (southern Poland). The question therefore arose whether the specimens buried in this grave were part of the local community. The oxygen isotope level was established using apatite isolated from bones or teeth. A femur and root dentine samples taken from permanent teeth were subjected to oxygen isotope analysis. The oxygen isotope level of the site was established on the basis of local water precipitation and measurements taken from the oxygen isotope concentration in apatite samples isolated from the bones of animals co-occurring with the studied human group. It has been found that the oxygen isotope levels in the bones and dentine of almost all the analysed specimens from the excavated site at Bronocice were within the established range for the area's environment, providing evidence for their local origin. Thus, it can be assumed that the analysed group inhabiting the macrosettlement at Bronocice during the Funnel Beaker phase of the Baden culture was most probably of local origin.

  7. Effect of composition on the polarization and ohmic resistances of LSM/YSZ composite cathodes in solid oxide fuel cell

    Indian Academy of Sciences (India)

    B SHRI PRAKASH; S SENTHIL KUMAR; S T ARUNA

    2017-06-01

    La0.8Sr0.2MnO$_3$−$\\delta$ (LSM)/8 mol% yttria-stabilized ZrO$_2$ (YSZ) (LSM/YSZ) composite cathodes with varying composition are studied for both polarization and ohmic resistance by electrochemical impedance spectroscopy. It was found that total resistance and polarization resistance are lowest for the composite with 60 wt% of LSM (LSM60/YSZ40). However, the ohmic resistance was highest for the same composition and amounted to 60% of the total resistance value. Compositional dependence of resistances has been explained based on the variations of the triple phase boundaries and width of the O$_2$−ion migration path with the composition of the electrode. Based on the observed area specific ohmic resistance values for the composite cathodes, it is proposed to verify the advantages of LSM/YSZ over LSM cathode in anode-supported solidoxide fuel cell with thin electrolyte.

  8. Advanced Thermally Stable Coal-Derived Jet Fuels Compositional Factors Affecting Thermal Degradation of Jet Fuels

    Science.gov (United States)

    1992-12-01

    Hou, R.M. Copenhaver Fuel Science Program Department of Materials Science & Engineering The Pennsylvania State University 209 Academic Projects...AMMM, M. Sobbilif Y. LU. L N% R.M. Cap..kavw 7. PERFORMING ORGANIZATION NAME(S) AND ADORESS(ES) .. PERFORMING ORGANIZATION Fuel Science Program REPORT...NUMBER Department of Materials Science & Engineering The Pennsylvania State University 209 Academic Projects Builiding University Park, PA 16802 9

  9. The precise measurement of Tl isotopic compositions by MC-ICPMS: Application to the analysis of geological materials and meteorites

    Energy Technology Data Exchange (ETDEWEB)

    Rehkaemper, M. [Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Geological Sciences]|[Univ. Muenster (Germany). Zentrallabor fuer Geochronologie; Halliday, A.N. [Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Geological Sciences]|[ETH Zuerich (Switzerland). Inst. for Isotope Geology and Mineral Resources

    1999-03-01

    The precision of Tl isotopic measurements by thermal ionization mass spectrometry (TIMS) is severely limited by the fact that Tl possesses only two naturally occurring isotopes, such that there is no invariant isotope ratio that can be used to correct for instrumental mass discrimination. In this paper the authors describe new chemical and mass spectrometric techniques for the determination of Tl isotopic compositions at a level of precision hitherto unattained. Thallium is first separated from the geological matrix using a two-stage anion-exchange procedure. Thallium isotopic compositions are then determined by multiple-collector inductively coupled plasma-mass spectrometry with correction for mass discrimination using the known isotopic composition of Pb that is admixed to the sample solutions. With these procedures they achieve a precision of 0.01--0.02% for Tl isotope ratio measurements in geological samples and this is a factor of {ge}3--4 better than the best published results by TIMS. Results are discussed for five terrestrial samples and for the C3V chondrite Allende.

  10. Sulfur Isotopic Compositions of Submicrometer SiC Grains from the Murchison Meteorite

    Science.gov (United States)

    Xu, Yuchen; Zinner, Ernst; Gallino, Roberto; Heger, Alexander; Pignatari, Marco; Lin, Yangting

    2015-02-01

    We report C, Si, N, S, Mg-Al, and Ca-Ti isotopic compositions of presolar silicon carbide (SiC) grains from the SiC-rich KJE size fraction (0.5-0.8 μm) of the Murchison meteorite. One thousand one hundred thirteen SiC grains were identified based on their C and Si isotopic ratios. Mainstream, AB, C, X, Y, and Z subtypes of SiC, and X-type silicon nitride (Si3N4) account for 81.4%, 5.7%, 0.1%, 1.5%, 5.8%, 4.9%, and 0.4%, respectively. Twenty-five grains with unusual Si isotopic ratios, including one C grain, 16 X grains, 1 Y grain, 5 Z grains, and 2 X-type Si3N4 grains were selected for N, S, Mg-Al, and Ca-Ti isotopic analysis. The C grain is highly enriched in 29Si and 30Si (δ29Si = 1345‰ ± 19‰, δ30Si = 1272‰ ± 19‰). It has a huge 32S excess, larger than any seen before, and larger than that predicted for the Si/S supernova (SN) zone, providing evidence against the elemental fractionation model by Hoppe et al. Two SN models investigated here present a more satisfying explanation in terms of a radiogenic origin of 32S from the decay of short-lived 32Si (τ1/2 = 153 yr). Silicon-32 as well as 29Si and 30Si can be produced in SNe by short neutron bursts; evidence for initial 44Ti (τ1/2 = 60 yr) in the C grain is additional evidence for an SN origin. The X grains have marginal 32S excesses, much smaller than expected from their large 28Si excesses. Similarly, the Y and Z grains do not show the S-isotopic anomalies expected from their large Si isotopic anomalies. Low intrinsic S contents and contamination with isotopically normal S are the most likely explanations.

  11. SULFUR ISOTOPIC COMPOSITIONS OF SUBMICROMETER SiC GRAINS FROM THE MURCHISON METEORITE

    Energy Technology Data Exchange (ETDEWEB)

    Xu, Yuchen [Institute of Geochemistry, Chinese Academy of Sciences, Guiyang 550002 (China); Zinner, Ernst [Laboratory for Space Sciences and Physics Department, Washington University, St. Louis, MO 63130 (United States); Gallino, Roberto [Dipartimento di Fisica, Università di Torino, I-10125 Torino (Italy); Heger, Alexander [Monash Centre for Astrophysics, School of Mathematical Sciences, Monash University, Vic 3800 (Australia); Pignatari, Marco [Department of Physics, University of Basel, CH-4056 Basel (Switzerland); Lin, Yangting, E-mail: xuyuchen@mail.iggcas.ac.cn [Key Laboratory of Earth' s Deep Interior, Institute of Geology and Geophysics, Chinese Academy of Sciences, Beijing 100029 (China)

    2015-02-01

    We report C, Si, N, S, Mg-Al, and Ca-Ti isotopic compositions of presolar silicon carbide (SiC) grains from the SiC-rich KJE size fraction (0.5-0.8 μm) of the Murchison meteorite. One thousand one hundred thirteen SiC grains were identified based on their C and Si isotopic ratios. Mainstream, AB, C, X, Y, and Z subtypes of SiC, and X-type silicon nitride (Si{sub 3}N{sub 4}) account for 81.4%, 5.7%, 0.1%, 1.5%, 5.8%, 4.9%, and 0.4%, respectively. Twenty-five grains with unusual Si isotopic ratios, including one C grain, 16 X grains, 1 Y grain, 5 Z grains, and 2 X-type Si{sub 3}N{sub 4} grains were selected for N, S, Mg-Al, and Ca-Ti isotopic analysis. The C grain is highly enriched in {sup 29}Si and {sup 30}Si (δ{sup 29}Si = 1345‰ ± 19‰, δ{sup 30}Si = 1272‰ ± 19‰). It has a huge {sup 32}S excess, larger than any seen before, and larger than that predicted for the Si/S supernova (SN) zone, providing evidence against the elemental fractionation model by Hoppe et al. Two SN models investigated here present a more satisfying explanation in terms of a radiogenic origin of {sup 32}S from the decay of short-lived {sup 32}Si (τ{sub 1/2} = 153 yr). Silicon-32 as well as {sup 29}Si and {sup 30}Si can be produced in SNe by short neutron bursts; evidence for initial {sup 44}Ti (τ{sub 1/2} = 60 yr) in the C grain is additional evidence for an SN origin. The X grains have marginal {sup 32}S excesses, much smaller than expected from their large {sup 28}Si excesses. Similarly, the Y and Z grains do not show the S-isotopic anomalies expected from their large Si isotopic anomalies. Low intrinsic S contents and contamination with isotopically normal S are the most likely explanations.

  12. Using ORIGEN2 to Predict Nuclear Reactor Fuel Compositions.

    Science.gov (United States)

    1988-03-01

    transitions, alpha decay , spontaneous fission, and delayed neutron decay (3) the recoverable heat per decay for each radioactive parent (4) the isotopic...21 BWR, 27.5 GWd/MTIHM................................................. 21 CANDU , 7.5 GWd/MTIHM...22 CANDU , 20.9 GWd/MTIHM............................................ 23 Aii MW"I wEMV 6 r1w Page LMvFBR - Core, 100 GWd/MTIHM

  13. Determination of uranium isotopic composition and 236U content of soil samples and hot particles using inductively coupled plasma mass spectrometry.

    Science.gov (United States)

    Boulyga, S F; Becker, J S

    2001-07-01

    As a result of the accident at the Chernobyl nuclear power plant (NPP) the environment was contaminated with spent nuclear fuel. The 236U isotope was used in this study to monitor the spent uranium from nuclear fallout in soil samples collected in the vicinity of the Chernobyl NPP. Nuclear track radiography was applied for the identification and extraction of hot radioactive particles from soil samples. A rapid and sensitive analytical procedure was developed for uranium isotopic ratio measurement in environmental samples based on double-focusing inductively coupled plasma mass spectrometry (DF-ICP-MS) with a MicroMist nebulizer and a direct injection high-efficiency nebulizer (DIHEN). The performance of the DF-ICP-MS with a quartz DIHEN and plasma shielded torch was studied. Overall detection efficiencies of 4 x 10(-4) and 10(-3) counts per atom were achieved for 238U in DF-ICP-QMS with the MicroMist nebulizer and DIHEN, respectively. The rate of formation of uranium hydride ions UH+/U+ was 1.2 x 10(-4) and 1.4 x 10(-4), respectively. The precision of short-term measurements of uranium isotopic ratios (n = 5) in 1 microg L(-1) NBS U-020 standard solution was 0.11% (238U/235U) and 1.4% (236U/238U) using a MicroMist nebulizer and 0.25% (235U/238U) and 1.9% (236U/P38U) using a DIHEN. The isotopic composition of all investigated Chernobyl soil samples differed from those of natural uranium; i.e. in these samples the 236U/238U ratio ranged from 10(-5) to 10(-3). Results obtained with ICP-MS, alpha- and gamma-spectrometry showed differences in the migration properties of spent uranium, plutonium, and americium. The isotopic ratio of uranium was also measured in hot particles extracted from soil samples.

  14. Osmium Isotopic Composition of the K/T Boundary Sediments from Sumbar: A Progress Report

    Science.gov (United States)

    Meisel, T.; Krahenbuhl, U.; Nazarov, M. A.

    1993-07-01

    Osmium isotope measurements have been performed on the boundary clay at different Cretaceous-Tertiary boundary (KTB) sites [1-5] since [6] suggested that Os isotopes are an indicator of an extraterrestrial component. The debate over "impact vs. volcanic" could not be resolved, but an isotope ratio close to chondritic could be demonstrated. The study of the distribution of iridium in the stratigraphy of the KTB cannot distinguish the contribution of chondritic and/or terrestrial Ir respectively, whereas the Os isotopes allow us to better constrain a mixing model. The ^187Os/^186Os ratio of the continental crust and chondritic reservoirs differ by at least 10-30 times. Assuming certain parameters, we should be able to calculate the proportion of the reservoirs making up the sediments of the KTB section. We studied a complete section of the KTB of Sumbar, Turkmenistan [7], for its Os isotopic composition. In the section 0-30 cm above the boundary clay, the ^187Os/^186Os ratio increases from 1.15 to 1.47, whereas the Ir concentration decreases from 66 to 1.4 ng/g or 66 to 4.7 ng/g on a carbonate-free basis respectively. Calculations show that the chondritic component makes up 9% at the boundary layer and decreases down to 0.6% at +30 cm. The data cannot be simply explained by varying admixtures of a chondritic component to a sediment of constant Os concentration and isotopic signature. To explain the Os ratios completely it is necessary to consider a mixture of four components (extraterrestrial, ejecta material, local terrigeneous, and carbonacous sediments) with certain assumptions: (1) The extraterrestrial source is chondritic in its Os and Re content and has an initial Os isotope ratio of 1.12 at 65 Ma (time of impact), which is above the average for normal chondrites but is within the range measured so far (e.g., Murray). (2) The ejecta material has a higher Os concentration (0.2 ng/g) than the sediments and is only present in the first 5 cm of the sequence above

  15. The summer 2012 Greenland heat wave: monitoring water vapour isotopic composition along an atmospheric river event

    Science.gov (United States)

    Bonne, Jean-Louis; Steen-Larsen, Hans Christian; Masson-Delmotte, Valérie; Sodemann, Harald; Lacour, Jean-Lionel; Risi, Camille; Werner, Martin; Clerbaux, Cathy; Fettweis, Xavier

    2014-05-01

    In July 2012, an extreme warm event occurred in Greenland, leading to surface melt over almost all the ice sheet. This event was recorded in the isotopic composition of water vapour measured by the IASI satellite along the transport pathway and at two sites where continuous in situ surface vapour isotopic measurements were conducted, situated at a coastal station of South Greenland (Ivittuut) and further North on top of the ice sheet (NEEM, NW Greenland). These observations allowed us to monitor the isotopic composition of the air mass at different stages of its advection towards Greenland, which can inform on processes along this trajectory, such as cloud properties and moisture sources. In addition, two simulations of this event, using the atmospheric general circulation models LMDZiso and ECHAM5wiso equipped with water stable isotopes and nudged towards large scale wind fields, are investigated. Furthermore, a regional high-resolution model was used to study the moisture transport to Greenland during this event using tagged water tracers of the North Atlantic ocean and coastal land evaporation. Using moisture source diagnostic based on the Lagrangian particle dispersion model Flexpart, we show that this 2012 heat wave event corresponds to moisture sources located over the subtropical Atlantic Ocean, where intense evaporation was caused by dry air masses associated with the US intense summer drought. This moisture was then advected northward along a narrow band, due to a very stationary surface cyclone southwest of Greenland, reached southern Greenland and Ivittuut coastal station on July 9th, travelled along the west coast of Greenland, continued eastwards above the ice sheet and arrived above the NEEM deep drilling camp on July 11th. Surface isotopic observations during the event show larger variations at NEEM than in Ivittuut, strongly reducing the isotopic and deuterium excess latitudinal gradient usually observed between South and North Greenland. This

  16. Neutron multiplication method for measuring the amount of fissile isotopes in the spent fuel

    Energy Technology Data Exchange (ETDEWEB)

    Chwaszczewski, S.; Pytel, K. [Institute of Atomic Energy, 05-400 Otwock-Swierk (Poland); Abou-Zaid, A.A. [Atomic Energy Authority, 13759 Cairo (Egypt)

    2001-07-01

    A nondestructive assay method for determination the amount of fissile materials content along the vertical axis of irradiated fuel is presented. The method, called neutron multiplication method, can be realized as passive measurement technique and the active one. The Monte Carlo code has been used for the neutron transport simulation and optimization of the measuring equipment geometry. On the basis of these results, a preliminary experimental stand for MARIA reactor fuel investigation has been designed and the measurements have been performed for the fresh fuel and the fuel mock-up. Based upon both numerical and experimental simulations, an ultimate measuring stand has been designed and the measurements for MARIA spent fuel assemblies as well as for the fresh fuel and mock-up of the fuel have been carried out. The results showed that the active neutron technique does not provide sufficient resolution of the distribution of the amount of fissile materials. But rather can be applied for measurement of the absolute value. The passive one can be used to restore the distribution of the bum-up and the amount of fissile materials along the axial length of the spent fuel assembly. (author)

  17. Mineralogy of the mid-ocean-ridge basalt source from neodymium isotopic composition of abyssal peridotites.

    Science.gov (United States)

    Salters, Vincent J M; Dick, Henry J B

    2002-07-04

    Inferring the melting process at mid-ocean ridges, and the physical conditions under which melting takes place, usually relies on the assumption of compositional similarity between all mid-ocean-ridge basalt sources. Models of mantle melting therefore tend to be restricted to those that consider the presence of only one lithology in the mantle, peridotite. Evidence from xenoliths and peridotite massifs show that after peridotite, pyroxenite and eclogite are the most abundant rock types in the mantle. But at mid-ocean ridges, where most of the melting takes place, and in ophiolites, pyroxenite is rarely found. Here we present neodymium isotopic compositions of abyssal peridotites to investigate whether peridotite can indeed be the sole source for mid-ocean-ridge basalts. By comparing the isotopic compositions of basalts and peridotites at two segments of the southwest Indian ridge, we show that a component other than peridotite is required to explain the low end of the (143)Nd/(144)Nd variations of the basalts. This component is likely to have a lower melting temperature than peridotite, such as pyroxenite or eclogite, which could explain why it is not observed at mid-ocean ridges.

  18. Tracing changes in atmospheric sources of lead contamination using lead isotopic compositions in Australian red wine.

    Science.gov (United States)

    Kristensen, Louise Jane; Taylor, Mark Patrick; Evans, Andrew James

    2016-07-01

    Air quality data detailing changes to atmospheric composition from Australia's leaded petrol consumption is spatially and temporally limited. In order to address this data gap, wine was investigated as a potential proxy for atmospheric lead conditions. Wine spanning sixty years was collected from two wine regions proximal to the South Australian capital city, Adelaide, and analysed for lead concentration and lead and strontium isotopic composition for source apportionment. Maximum wine lead concentrations (328 μg/L) occur prior to the lead-in-air monitoring in South Australia in the later 1970s. Wine lead concentrations mirror available lead-in-air measurements and show a declining trend reflecting parallel reductions in leaded petrol emissions. Lead from petrol dominated the lead in wine ((206)Pb/(207)Pb: 1.086; (208)Pb/(207)Pb: 2.360) until the introduction of unleaded petrol, which resulted in a shift in the wine lead isotopic composition closer to vineyard soil ((206)Pb/(207)Pb: 1.137; (208)Pb/(207)Pb: 2.421). Current mining activities or vinification processes appear to have no impact with recent wine samples containing less than 4 μg/L of lead. This study demonstrates wine can be used to chronicle changes in environmental lead emissions and is an effective proxy for atmospherically sourced depositions of lead in the absence of air quality data.

  19. Comparison of neutron cross sections for selected fission products and isotopic composition analyses with burnup

    Energy Technology Data Exchange (ETDEWEB)

    Kim, D. H.; Gil, C. S.; Kim, J. D.; Jang, J. H.; Lee, Y. D. [KAERI, Taejon (Korea)

    2003-10-01

    The neutron absorption cross sections for 18 fission products evaluated within the framework of the KAERI-BNL international collaboration have been compared with the ENDF/B-VI release 7. Also, the influence of the new evaluations on isotopic compositions of the fission products as a function of burnup has been analyzed through the OECD/NEA burnup credit criticality benchmarks (Phase 1B) and the LWR/Pu recycling benchmarks. These calculations were performed by WIMSD-5B with the 69 group libraries prepared from three evaluated nuclear data libraries: ENDF/B-VI.7, ENDF/B-VI.8 including new evaluations in resonance region covering thermal region, and ENDF/B-VII expected including those in upper resonance region up to 20 MeV. For Xe-131, the composition calculated with ENDF/B-VI.8 shows maximum difference of 4.78% compared to ENDF/B-VI.7. However, the isotopic compositions of all fission products calculated with ENDF/B-VII shows no differences compared to ENDF/B-VI.7.

  20. Comparisons of Neutron Cross Sections and Isotopic Composition Calculations for Fission-Product Evaluations

    Science.gov (United States)

    Kim, Do Heon; Gil, Choong-Sup; Chang, Jonghwa; Lee, Yong-Deok

    2005-05-01

    The neutron absorption cross sections for 18 fission products evaluated within the framework of the KAERI (Korea Atomic Energy Research Institute)-BNL (Brookhaven National Laboratory) international collaboration have been compared with ENDF/B-VI.7. Also, the influence of the new evaluations on the isotopic composition calculations of the fission products has been estimated through the OECD/NEA burnup credit criticality benchmarks (Phase 1B) and the LWR/Pu recycling benchmarks. These calculations were performed by WIMSD-5B with the 69-group libraries prepared from three evaluated nuclear data libraries: ENDF/B-VI.7, ENDF/B-VI.8 including the new evaluations in the resonance region covering the thermal region, and the expected ENDF/B-VII including those in the upper resonance region up to 20 MeV. For Xe-131, the composition calculated with ENDF/B-VI.8 shows a maximum difference of 5.02% compared to ENDF/B-VI.7. However, the isotopic compositions of all the fission products calculated with the expected ENDF/B-VII show no differences when compared to ENDF/B-VI.7 for the thermal reactor benchmark cases.

  1. A method for in situ monitoring of the isotope composition of tree xylem water using laser spectroscopy.

    Science.gov (United States)

    Volkmann, Till H M; Kühnhammer, Kathrin; Herbstritt, Barbara; Gessler, Arthur; Weiler, Markus

    2016-09-01

    Field studies analyzing the stable isotope composition of xylem water are providing important information on ecosystem water relations. However, the capacity of stable isotopes to characterize the functioning of plants in their environment has not been fully explored because of methodological constraints on the extent and resolution at which samples could be collected and analysed. Here, we introduce an in situ method offering the potential to continuously monitor the stable isotope composition of tree xylem water via its vapour phase using a commercial laser-based isotope analyser and compact microporous probes installed into the xylem. Our technique enables efficient high-frequency measurement with intervals of only a few minutes per sample while eliminating the need for costly and cumbersome destructive collection of plant material and laboratory-based processing. We present field observations of xylem water hydrogen and oxygen isotope compositions obtained over several days including a labelled irrigation event and compare them against results from concurrent destructive sampling with cryogenic distillation and mass spectrometric analysis. The data demonstrate that temporal changes as well as spatial patterns of integration in xylem water isotope composition can be resolved through direct measurement. The new technique can therefore present a valuable tool to study the hydraulic architecture and water utilization of trees.

  2. Observations of molecular hydrogen mixing ratio and stable isotopic composition at the Cabauw tall tower in the Netherlands

    Science.gov (United States)

    Batenburg, A. M.; Popa, M. E.; Vermeulen, A. T.; van den Bulk, W. C. M.; Jongejan, P. A. C.; Fisher, R. E.; Lowry, D.; Nisbet, E. G.; Röckmann, T.

    2016-12-01

    Measurements of the stable isotopic composition (δD(H2) or δD) of atmospheric molecular hydrogen (H2) are a useful addition to mixing ratio (χ(H2)) measurements for understanding the atmospheric H2 cycle. δD datasets published so far consist mostly of observations at background locations. We complement these with observations from the Cabauw tall tower at the CESAR site, situated in a densely populated region of the Netherlands. Our measurements show a large anthropogenic influence on the local H2 cycle, with frequently occurring pollution events that are characterized by χ(H2) values that reach up to ≈1 ppm and low δD values. An isotopic source signature analysis yields an apparent source signature below -400‰, which is much more D-depleted than the fossil fuel combustion source signature commonly used in H2 budget studies. Two diurnal cycles that were sampled at a suburban site near London also show a more D-depleted source signature (≈-340‰), though not as extremely depleted as at Cabauw. The source signature of the Northwest European vehicle fleet may have shifted to somewhat lower values due to changes in vehicle technology and driving conditions. Even so, the surprisingly depleted apparent source signature at Cabauw requires additional explanation; microbial H2 production seems the most likely cause. The Cabauw tower site also allowed us to sample vertical profiles. We found no decrease in χ(H2) at lower sampling levels (20 and 60 m) with respect to higher sampling levels (120 and 200 m). There was a significant shift to lower median δD values at the lower levels. This confirms the limited role of soil uptake around Cabauw, and again points to microbial H2 production during an extended growing season, as well as to possible differences in average fossil fuel combustion source signature between the different footprint areas of the sampling levels. So, although knowledge of the background cycle of H2 has improved over the last decade, surprising

  3. Viscous sealing glass compositions for solid oxide fuel cells

    Energy Technology Data Exchange (ETDEWEB)

    Kim, Cheol Woon; Brow, Richard K.

    2016-12-27

    A sealant for forming a seal between at least two solid oxide fuel cell components wherein the sealant comprises a glass material comprising B.sub.2O.sub.3 as a principal glass former, BaO, and other components and wherein the glass material is substantially alkali-free and contains less than 30% crystalline material.

  4. Measurements of Fission Cross Sections for the Isotopes relevant to the Thorium Fuel Cycle

    CERN Multimedia

    2002-01-01

    The present concern about a sustainable energy supply is characterised by a considerable uncertainty: the green house effect and foreseeable limits in fossil fuel resources on the one hand, the concern about the environmental impact of nuclear fission energy and the long term fusion research on the other hand, have led to the consideration of a variety of advanced strategies for the nuclear fuel cycle and related nuclear energy systems. The present research directories concern such strategies as the extension of the life span of presently operating reactors, the increase of the fuel burn-up, the plutonium recycling, and in particular the incineration of actinides and long-Lived fission products, the accelerator driven systems (ADS), like the "Energy Amplifier" (EA) concept of C. Rubbia, and the possible use of the Thorium fuel cycle. The detailed feasibility study and safety assessment of these strategies requires the accurate knowledge of neutron nuclear reaction data. Both, higher fuel burn-up and especiall...

  5. Pore-water isotopic compositions and unsaturated-zone flow, Yucca Mountain, Nevada

    Energy Technology Data Exchange (ETDEWEB)

    Yang, In C.

    2001-04-29

    Isotopic compositions of core-water samples from boreholes USW SD-6 and USW WT-24 indicate that recent water has been introduced at depth. Tritium, carbon, oxygen, and deuterium isotopic compositions all support younger water at depth in the two boreholes. Peaks in tritium concentrations in pore-water samples, indicating younger water than the other samples, observed near the basal vitrophyre of the Topopah Spring Tuff and at the bottom of the CHF and the top of the PP in both boreholes SD-6 and WT-24. Larger {sup 14}C activities in two pore-water samples from WT-24 at the bottom of the CHF and the top of the PP indicate younger water than in other samples from WT-24. More positive {delta}{sup 18}O and {delta}D values indicate younger water in samples of pore water at the bottom of the CHF in boreholes SD-6 and WT-24. The isotopic compositions indicating younger water at depth in boreholes SD-6 and WT-24 occur at the basal vitrophyre zone of the Topopah Spring Tuff and the bottom of the CHF/upper part of the PP, probably from lateral preferential flow through connected fractures (fast-flow paths). The source of the young water at borehole WT-24 probably was recharge from The Prow to the north, which then flowed laterally southward through the highly fractured TSw. The source of the young water at borehole SD-6 probably was water flow from the Solitario Canyon fault to the west, which then flowed laterally through the TSw and CHF.

  6. Isotopic composition of inorganic mercury and methylmercury downstream of a historical gold mining region

    Science.gov (United States)

    Donovan, Patrick M.; Blum, Joel D.; Singer, Michael B.; Marvin-DiPasquale, Mark C.; Tsui, Martin T.K.

    2016-01-01

    We measured total mercury (THg) and monomethyl mercury (MMHg) concentrations and mercury (Hg) isotopic compositions in sediment and aquatic organisms from the Yuba River (California, USA) to identify Hg sources and biogeochemical transformations downstream of a historical gold mining region. Sediment THg concentrations and δ202Hg decreased from the upper Yuba Fan to the lower Yuba Fan and the Feather River. These results are consistent with the release of Hg during gold mining followed by downstream mixing and dilution. The Hg isotopic composition of Yuba Fan sediment (δ202Hg = −0.38 ± 0.17‰ and Δ199Hg = 0.04 ± 0.03‰; mean ± 1 SD, n = 7) provides a fingerprint of inorganic Hg (IHg) that could be methylated locally or after transport downstream. The isotopic composition of MMHg in the Yuba River food web was estimated using biota with a range of %MMHg (the percent of THg present as MMHg) and compared to IHg in sediment, algae, and the food web. The estimated δ202Hg of MMHg prior to photodegradation (−1.29 to −1.07‰) was lower than that of IHg and we suggest this is due to mass-dependent fractionation (MDF) of up to −0.9‰ between IHg and MMHg. This result is in contrast to net positive MDF (+0.4 to +0.8‰) previously observed in lakes, estuaries, coastal oceans, and forests. We hypothesize that this unique relationship could be due to differences in the extent or pathway of biotic MMHg degradation in stream environments.

  7. Measurement of the Carbon Isotopic Composition of Methane Using Helicoidal Laser Eigenstates

    Science.gov (United States)

    Jacob, D.; Le Floch, A.; Bretenaker, F.; Guenot, P.

    1996-06-01

    The spatially generalized Jones matrix formalism is used to design a laser cavity to make intracavity measurements of the carbon isotopic composition of methane. the method is based on a double optical lever effect for helicoidally polarized eigenstates, permitting to measure successively the ^{12}CH_4 and ^{13}CH_4 concentrations. To choose the probed isotope, one simply tunes the frequency of the laser by Zeeman effect. The experiment exhibits a good agreement with the predictions and permits to measure the ^{13}CH4/^{12}CH_4 composition ratio of methane with an uncertainty of the order of ± 0.07% for a sample containing only 6× 10^{-9} mole of methane. On utilise le formalisme des matrices de Jones généralisées spatialement pour concevoir une cavité laser permettant la mesure intra-cavité de la composition isotopique du carbone présent dans le méthane. La méthode est fondée sur une double application de l'effet de levier optique pour les états propres hélicoïdaux, permettant de mesurer successivement les concentrations de ^{12}CH_4 et de ^{13}CH_4. Pour passer d'un isotope à l'autre, on ajuste simplement la fréquence du laser par effet Zeeman. L'expérience est en bon accord avec les prédictions et permet d'effectuer la mesure du rapport isotopique ^{13}CH4/^{12}CH_4 avec une fourchette d'incertitude de ± 0,07% pour des échantillons de gaz ne contenant que 6× 10^{-9} mole de méthane.

  8. Isotopic Composition of Inorganic Mercury and Methylmercury Downstream of a Historical Gold Mining Region.

    Science.gov (United States)

    Donovan, Patrick M; Blum, Joel D; Singer, Michael Bliss; Marvin-DiPasquale, Mark; Tsui, Martin T K

    2016-02-16

    We measured total mercury (THg) and monomethyl mercury (MMHg) concentrations and mercury (Hg) isotopic compositions in sediment and aquatic organisms from the Yuba River (California, USA) to identify Hg sources and biogeochemical transformations downstream of a historical gold mining region. Sediment THg concentrations and δ(202)Hg decreased from the upper Yuba Fan to the lower Yuba Fan and the Feather River. These results are consistent with the release of Hg during gold mining followed by downstream mixing and dilution. The Hg isotopic composition of Yuba Fan sediment (δ(202)Hg = -0.38 ± 0.17‰ and Δ(199)Hg = 0.04 ± 0.03‰; mean ± 1 SD, n = 7) provides a fingerprint of inorganic Hg (IHg) that could be methylated locally or after transport downstream. The isotopic composition of MMHg in the Yuba River food web was estimated using biota with a range of %MMHg (the percent of THg present as MMHg) and compared to IHg in sediment, algae, and the food web. The estimated δ(202)Hg of MMHg prior to photodegradation (-1.29 to -1.07‰) was lower than that of IHg and we suggest this is due to mass-dependent fractionation (MDF) of up to -0.9‰ between IHg and MMHg. This result is in contrast to net positive MDF (+0.4 to +0.8‰) previously observed in lakes, estuaries, coastal oceans, and forests. We hypothesize that this unique relationship could be due to differences in the extent or pathway of biotic MMHg degradation in stream environments.

  9. C4 plant isotopic composition (delta13C) evidence for urban CO2 pollution in the city of Cotonou, Benin (West Africa).

    Science.gov (United States)

    Kèlomé, Nelly C; Lévêque, Jean; Andreux, Francis; Milloux, Marie-Jeanne; Oyédé, Lucien-Marc

    2006-08-01

    The carbon isotopic composition (delta13C) of plants can reveal the isotopic carbon content of the atmosphere in which they develop. The delta13C values of air and plants depend on the amount of atmospheric fossil fuel CO2, which is chiefly emitted in urban areas. A new indicator of CO2 pollution is tested using the delta13C variation in a C4 grass: Eleusine indica. A range of about 4 per thousand delta units was observed at different sites in Cotonou, the largest city in the Republic of Benin. The highest delta13C values, from -12 per thousand to -14 per thousand, were found in low traffic zones; low delta13C values, from -14 per thousand to -16 per thousand, were found in high traffic zones. The amount of fossil fuel carbon assimilated by plants represented about 20% of the total plant carbon content. An overall decrease in plant delta13C values was observed over a four-year monitoring period. This decrease was correlated with increasing vehicle traffic. The delta13C dataset and the corresponding geographical database were used to map and define zones of high and low 13C-depleted CO2 emissions in urban and sub-urban areas. The spatial distribution follows dominant wind directions, with the lowest emission zones found in the southwest of Cotonou. High CO2 emissions occurred in the north, the east and the center, providing evidence of intense anthropogenic activity related to industry and transportation.

  10. Box-modeling of bone and tooth phosphate oxygen isotope compositions as a function of environmental and physiological parameters.

    Science.gov (United States)

    Langlois, C; Simon, L; Lécuyer, Ch

    2003-12-01

    A time-dependent box model is developed to calculate oxygen isotope compositions of bone phosphate as a function of environmental and physiological parameters. Input and output oxygen fluxes related to body water and bone reservoirs are scaled to the body mass. The oxygen fluxes are evaluated by stoichiometric scaling to the calcium accretion and resorption rates, assuming a pure hydroxylapatite composition for the bone and tooth mineral. The model shows how the diet composition, body mass, ambient relative humidity and temperature may control the oxygen isotope composition of bone phosphate. The model also computes how bones and teeth record short-term variations in relative humidity, air temperature and delta18O of drinking water, depending on body mass. The documented diversity of oxygen isotope fractionation equations for vertebrates is accounted for by our model when for each specimen the physiological and diet parameters are adjusted in the living range of environmental conditions.

  11. Sulfur isotope composition of metasomatised mantle xenoliths from the Bultfontein kimberlite (Kimberley, South Africa): Contribution from subducted sediments and the effect of sulfide alteration on S isotope systematics

    Science.gov (United States)

    Giuliani, Andrea; Fiorentini, Marco L.; Martin, Laure A. J.; Farquhar, James; Phillips, David; Griffin, William L.; LaFlamme, Crystal

    2016-07-01

    Sulfur isotopes are a powerful geochemical tracer in high-temperature processes, but have rarely been applied to the study of mantle metasomatism. In addition, there are very limited S isotope data on sub-continental lithospheric mantle (SCLM) material. For cratonic regions, these data are restricted to sulfide inclusions in diamonds. To provide new constraints on the S isotope composition of the SCLM and on the source(s) of mantle metasomatic fluids beneath the diamondiferous Kimberley region (South Africa), we investigated the S isotope systematics of five metasomatised mantle xenoliths from the Bultfontein kimberlite. Pentlandite and chalcopyrite in these xenoliths were analysed by in situ secondary-ion mass spectrometry (SIMS), with bulk-rock material measured by gas source isotope ratio mass spectrometry techniques. Based on previous studies, the xenoliths experienced different types of metasomatism to one another at distinct times (∼180 and ∼90-80 Ma). Contained pentlandite grains show variable alteration to heazlewoodite (i.e. Ni sulfide) + magnetite. The in situ S isotope analyses of pentlandite exhibit a relatively restricted range between -5.9 and - 1.4 ‰δ34 S (compared to VCDT), with no statistically meaningful differences between samples. Chalcopyrite only occurs in one sample and shows δ34 S values between -5.4 and - 1.0 ‰. The bulk-rock Ssulfide isotope analyses vary between -3.4 and + 0.8 ‰δ34 S. Importantly, the only sample hosting dominantly fresh sulfides shows a bulk-rock δ34 S value consistent with the mean value for the sulfides, whereas the other samples exhibit higher bulk 34S/32S ratios. The differences between bulk-rock and average in situδ34 S values are directly correlated with the degree of sulfide alteration. This evidence indicates that the elevated 34S/32S ratios in the bulk samples are not due to the introduction of heavy S (commonly as sulfates) and are best explained by isotopic fractionation coupled with the removal

  12. Modelling the Oceanic Nd Isotopic Composition With a North Atlantic Eddy Permitting Model

    Science.gov (United States)

    Peronne, S.; Treguier, A.; Arsouze, T.; Dutay, J.; Lacan, F.; Jeandel, C.

    2006-12-01

    The oceanic water masses differ by their temperatures, salinity, but also a number of geochemical tracers characterized by their weak concentrations and their ability to quantify oceanic processes (mixing, scavenging rates etc). Among these tracers, the Nd isotopic composition (hereafter epsilon-Nd) is a (quasi) conservative tracer of water mass mixing in the ocean interior, far from any lithogenic inputs. It has been recently established that exchange of Nd at the oceanic margins could be the dominant process controlling both its concentration and isotopic composition distribution in the ocean. This was demonstrated using in situ measurements and budget calculations and has recently been confirmed by a low resolution (2°) modeling approach (Arsouze et al., 2006). However, the currents flowing on the ocean margins are not correctly represented in coarse ocean models. It is the case in the North Atlantic ocean, which is of particular interest since i) it is the area of deep water formation and ii) these deep waters are characterized by the most negative epsilon-Nd values of the world ocean, which are used as "imprint" of the present and past thermohaline circulation. It is therefore essential to understand how these water masses acquire their epsilon-Nd signature. We propose here the first results of the modeling of oceanic Nd isotopic composition at eddy-permitting resolution, with the North Atlantic 0.25° version of the NEMO model used for the DRAKKAR European project. A 150 years off-line experiment and a shorter on-line experiment are performed. Simulated Nd distributions are compared to the present-day data base, vertical profiles, and the results of the low resolution model (in the North Atlantic). The eddy permitting model generally provides improved results, provided a high enough exchange rate is imposed in the deep ocean. Deficiencies of the simulated distribution in the Nordic Seas and the subpolar gyre are explained by errors in the input function on

  13. The Oxygen Isotope Composition of Dark Inclusions in HEDs, Ordinary and Carbonaceous Chondrites

    Science.gov (United States)

    Greenwood, R. C.; Zolensky, M. E.; Buchanan, P. C.; Franchi, I. A.

    2015-01-01

    Dark inclusions (DIs) are lithic fragments that form a volumetrically small, but important, component in carbonaceous chondrites. Carbonaceous clasts similar to DIs are also found in some ordinary chondrites and HEDs. DIs are of particular interest because they provide a record of nebular and planetary processes distinct from that of their host meteorite. DIs may be representative of the material that delivered water and other volatiles to early Earth as a late veneer. Here we focus on the oxygen isotopic composition of DIs in a variety of settings with the aim of understanding their formational history and relationship to the enclosing host meteorite.

  14. The Oxygen Isotopic Composition of Water in the Inner Solar System

    OpenAIRE

    Nunn, Morgan

    2015-01-01

    Where there is water, there can be life. Improving our understanding of how life, as we know it, arose uniquely in our solar system on Earth depends critically on our understanding of the history of water in the solar system. Better characterizing the sources of water to the Earth-Moon system is crucial in constraining this history and motivated the experiments described in this dissertation.The oxygen isotopic composition of water in lunar samples in addition to meteorites from Mars and seve...

  15. Re-Os isotopic composition of the Dongling ⅢCD iron meteorite

    Institute of Scientific and Technical Information of China (English)

    2001-01-01

    Re,Os concentrations and Os isotopic compositions of the Dongling ⅢCD iron meteorite were determined by N-TIMS technique. The result was compared with that of the other irons and chondrites. The Re and Os concentrations of the Dongling iron meteorite were plotted on the trends of the group ⅢA and ⅣA irons. The Pt-Os relation of the Dongling iron meteorite is similar to that of the group ⅡA irons. That suggests a higher fractionation for the Dongling iron meteorite.

  16. Isotopic composition of ground waters from Kufra (Lybia) as indicator for ground water formation

    Energy Technology Data Exchange (ETDEWEB)

    Swailem, F.M.; Hamza, M.S.; Aly, A.I.M. (Middle Eastern Regional Radioisotope Centre for the Arab Countries, Cairo (Egypt))

    1984-02-01

    The results of the isotopic composition of shallow and deep ground waters from the Kufra region indicate the fossil origin of these waters and that they are not recharged under the present climatic conditions. The virtual absence of tritium and the radiocarbon ages of these waters show that they were formed mainly in the past pluvial periods. Deuterium and oxygen-18 data indicate that the ground waters were recharged under cooler climatic conditions. These results may explain the origin of the large amounts of ground water which existed in the region.

  17. Recovery of protactinium from molten fluoride nuclear fuel compositions

    Science.gov (United States)

    Baes, C.F. Jr.; Bamberger, C.; Ross, R.G.

    1973-12-25

    A method is provided for separating protactinium from a molten fluonlde salt composition consisting essentially of at least one alkali and alkaline earth metal fluoride and at least one soluble fluoride of uranium or thorium which comprises oxidizing the protactinium in said composition to the + 5 oxidation state and contacting said composition with an oxide selected from the group consisting of an alkali metal oxide, an alkaline earth oxide, thorium oxide, and uranium oxide, and thereafter isolating the resultant insoluble protactinium oxide product from said composition. (Official Gazette)

  18. Uranium isotopic data in uraninite spent fuel from the Bangombe natural nuclear reactor (Gabon) and its surroundings

    Science.gov (United States)

    Fernandez-Diaz; Quejido; Crespo; Perez del Villar L; Martin-Sanchez; Lozano

    2000-07-01

    In the framework of the "Oklo-Natural Analogue Phase II" Project, uraninite from the Bangombe natural reactor and samples from its host rock were analyzed to determine their uranium isotopic composition by thermal ionisation mass spectrometry, inductively coupled plasma mass spectrometry and alpha spectrometry. There were several objectives for this work: (i) to validate the 235U/238U isotopic ratios obtained by these techniques; (ii) to test the use of the 235U/238U ratio of uraninite as a tracer of migration/retention processes of uranium from the source term to the far field; (iii) to evaluate the most recent migration/retention processes of uranium in the system by U-series disequilibrium.

  19. Uranium isotopic data in uraninite spent fuel from the Bangombe natural nuclear reactor (Gabon) and its surroundings

    Energy Technology Data Exchange (ETDEWEB)

    Fernandez-Diaz, M.; Quejido, A.J.; Crespo, M.T.; Villar, L.P. del; Martin-Sanchez, A. E-mail: ams@unex.es; Lozano, J.C

    2000-07-15

    In the framework of the 'Oklo-Natural Analogue Phase II' Project, uraninite from the Bangombe natural reactor and samples from its host rock were analyzed to determine their uranium isotopic composition by thermal ionisation mass spectrometry, inductively coupled plasma mass spectrometry and alpha spectrometry. There were several objectives for this work: (i) to validate the {sup 235}U/{sup 238}U isotopic ratios obtained by these techniques; (ii) to test the use of the {sup 235}U/{sup 238}U ratio of uraninite as a tracer of migration/retention processes of uranium from the source term to the far field; (iii) to evaluate the most recent migration/retention processes of uranium in the system by U-series disequilibrium.

  20. Determination of Sectional Constancy of Organic Coal-Water Fuel Compositions

    Directory of Open Access Journals (Sweden)

    Dmitrienko Margarita A.

    2016-01-01

    Full Text Available To use widespreadly the waste of coals and oils processing in the great and the small-scale power generation, the key parameter, which is sectional constancy of promising organic coal-water fuels (OCWF, was studied. The compo-sitions of OCWF from brown and bituminous coals, filter cakes, used motor, turbine and dielectrical oils, water-oil emul-sion and special wetting agent (plasticizer were investigated. Two modes of preparation were considered. They are with homogenizer and cavitator. It was established that the constancy did not exceed 5–7 days for the compositions of OCWF with brown coals, and 12–15 days for that compositions with bituminous coals and filter cakes. The injection of used oils in a composition of OCWF led to increase in viscosity of fuel compositions and their sectional constancy.

  1. Abnormal lithium isotope composition from the ancient lithospheric mantle beneath the North China Craton.

    Science.gov (United States)

    Tang, Yan-Jie; Zhang, Hong-Fu; Deloule, Etienne; Su, Ben-Xun; Ying, Ji-Feng; Santosh, M; Xiao, Yan

    2014-03-04

    Lithium elemental and isotopic compositions of olivines in peridotite xenoliths from Hebi in the North China Craton provide direct evidence for the highly variable δ(7)Li in Archean lithospheric mantle. The δ(7)Li in the cores of olivines from the Hebi high-Mg# peridotites (Fo > 91) show extreme variation from -27 to +21, in marked deviation from the δ(7)Li range of fresh MORB (+1.6 to +5.6) although the Li abundances of the olivines are within the range of normal mantle (1-2 ppm). The Li abundances and δ(7)Li characteristics of the Hebi olivines could not have been produced by recent diffusive-driven isotopic fractionation of Li and therefore the δ(7)Li in the cores of these olivines record the isotopic signature of the subcontinental lithospheric mantle. Our data demonstrate that abnormal δ(7)Li may be preserved in the ancient lithospheric mantle as observed in our study from the central North China Craton, which suggest that the subcontinental lithospheric mantle has experienced modification of fluid/melt derived from recycled oceanic crust.

  2. Isotopic compositions of strontium in river water of Guizhou karst areas, China

    Institute of Scientific and Technical Information of China (English)

    韩贵琳; 刘丛强

    2001-01-01

    We have carried out a study on the variation of strontium isotope composition of river waters, Wujiang and Yuangjiang River, in karst areas of Guizhou Province, China. The results obtained permit us to characterize the geochemistry of the river draining karst terrain and obtain a better understanding of main controls of catchment geology, chemical weathering of different rocks, and evaluate impact of human activities on the environment. The isotopic ratios of dissolved Sr in all rivers are between 87Sr/86Sr =0.7077 and 0.7110, totally lower than the weighted average of 87Sr/86Sr =0.7119 for the world large rivers. The Wujiang River waters have Sr concentrations from 1.0 to 6.1 μmol/L, while the Yuanjiang River waters have much lower Sr concentrations ranging from 0.28 to 1.3 μmol/L. Most of the river waters from the Wujiang river are characterized by low Ca/Sr and Mg/Sr, and 87Sr/86Sr ratios, in which a majority of river waters are of 87Sr/86Sr ratios lower than the average Sr isotope ratio (87Sr/86Sr

  3. Changing compositions in the Iceland plume; Isotopic and elemental constraints from the Paleogene Faroe flood basalts

    DEFF Research Database (Denmark)

    Søager, Nina; Holm, Paul Martin

    2011-01-01

    -type component similar in geochemistry to the Icelandic Öræfajökull lavas. This component is believed to be recycled pelagic sediments in the plume but it can alternatively be a local crustal or lithospheric mantle component. The enriched Faroe high-Ti lavas erupted inland from the rift have isotopic......Elemental and Sr, Nd, Hf and high precision Pb isotopic data are presented from 59 low-Ti and high-Ti lavas from the syn-break up part of the Faroe Flood Basalt Province. The depleted MORB-like low-Ti lavas erupted in the rift zone between the Faroe Islands and central East Greenland around...... the time of break up of the North Atlantic have isotopic end-member compositions different from the depleted Iceland lavas. We suggest that the main low-Ti mantle component is NAEM (North Atlantic End-Member (Ellam and Stuart, 2000, J. Petrol. 41, 919) and that the 207Pb/204Pb value of the component should...

  4. Continuous monitoring of summer surface water vapor isotopic composition above the Greenland Ice Sheet

    Directory of Open Access Journals (Sweden)

    H. C. Steen-Larsen

    2013-05-01

    Full Text Available We present here surface water vapor isotopic measurements conducted from June to August 2010 at the NEEM (North Greenland Eemian Drilling Project camp, NW Greenland (77.45° N, 51.05° W, 2484 m a.s.l.. Measurements were conducted at 9 different heights from 0.1 m to 13.5 m above the snow surface using two different types of cavity-enhanced near-infrared absorption spectroscopy analyzers. For each instrument specific protocols were developed for calibration and drift corrections. The inter-comparison of corrected results from different instruments reveals excellent reproducibility, stability, and precision with a standard deviations of ~ 0.23‰ for δ18O and ~ 1.4‰ for δD. Diurnal and intraseasonal variations show strong relationships between changes in local surface humidity and water vapor isotopic composition, and with local and synoptic weather conditions. This variability probably results from the interplay between local moisture fluxes, linked with firn–air exchanges, boundary layer dynamics, and large-scale moisture advection. Particularly remarkable are several episodes characterized by high (> 40‰ surface water vapor deuterium excess. Air mass back-trajectory calculations from atmospheric analyses and water tagging in the LMDZiso (Laboratory of Meteorology Dynamics Zoom-isotopic atmospheric model reveal that these events are associated with predominant Arctic air mass origin. The analysis suggests that high deuterium excess levels are a result of strong kinetic fractionation during evaporation at the sea-ice margin.

  5. Interactive Evolution of Multiple Water-Ice Reservoirs on Mars: Insights from Hydrogen Isotope Compositions

    CERN Document Server

    Kurokawa, Hiroyuki; Sato, Masahiko

    2015-01-01

    Remote sensing data from orbiter missions have proposed that ground ice may currently exist on Mars, although the volume is still uncertain. Recent analyses of Martian meteorites have suggested that the water reservoirs have at least three distinct hydrogen isotope compositions (D/H ratios): primordial and high D/H ratios, which are approximately the same and six times that of ocean water on Earth, respectively, and a newly identified intermediate D/H ratio, which is approximately two to three times higher than that in ocean water on Earth. We calculate the evolution of the D/H ratios and the volumes of the water reservoirs on Mars by modeling the exchange of hydrogen isotopes between multiple water reservoirs and the atmospheric escape. The D/H ratio is slightly higher in the topmost thin surface-ice layer than that in the atmosphere because of isotopic fractionation by sublimation, whereas the water-ice reservoir just below the exchangeable topmost surface layer retains the intermediate D/H signature found ...

  6. Interpreting bryophyte stable carbon isotope composition: Plants as temporal and spatial climate recorders

    Science.gov (United States)

    Royles, Jessica; Horwath, Aline B.; Griffiths, Howard

    2014-04-01

    are unable to control tissue water content although physiological adaptations allow growth in a wide range of habitats. Carbon isotope signals in two mosses (Syntrichia ruralis and Chorisodontium aciphyllum) and two liverworts (Conocephalum conicum and Marchantia polymorpha), whether instantaneous (real time, Δ13C), or organic matter (as δ13COM), provide an assimilation-weighted summary of bryophyte environmental adaptations. In mosses, δ13COM is within the measured range of Δ13C values, which suggests that other proxies, such as compound-specific organic signals, will be representative of historical photosynthetic and growth conditions. The liverworts were photosynthetically active over a wider range of relative water contents (RWC) than the mosses. There was a consistent 5‰ offset between Δ13C values in C. conicum and M. polymorpha, suggestive of greater diffusion limitation in the latter. Analysis of a C. aciphyllum moss-peat core showed the isotopic composition over the past 200 years reflects recent anthropogenic CO2 emissions. Once corrected for source-CO2 inputs, the seasonally integrated Δ13COM between 1350 and 2000 A.D. varied by 1.5‰ compared with potential range of the 12‰ measured experimentally, demonstrating the relatively narrow range of conditions under which the majority of net assimilation takes place. Carbon isotope discrimination also varies spatially, with a 4‰ shift in epiphytic bryophyte organic matter found between lowland Amazonia and upper montane tropical cloud forest in the Peruvian Andes, associated with increased diffusion limitation.

  7. Characterizing the oxygen isotopic composition of phosphate sources to aquatic ecosystems.

    Science.gov (United States)

    Young, Megan B; McLaughlin, Karen; Kendall, Carol; Stringfellow, William; Rollog, Mark; Elsbury, Katy; Donald, Elizabeth; Paytan, Adina

    2009-07-15

    The oxygen isotopic composition of dissolved inorganic phosphate (delta18Op) in many aquatic ecosystems is not in isotopic equilibrium with ambient water and, therefore, may reflect the source delta18Op. Identification of phosphate sources to water bodies is critical for designing best management practices for phosphate load reduction to control eutrophication. In order for delta18Op to be a useful tool for source tracking, the delta18Op of phosphate sources must be distinguishable from one another; however, the delta18Op of potential sources has not been well characterized. We measured the delta18Op of a variety of known phosphate sources, including fertilizers, semiprocessed phosphorite ore, particulate aerosols, detergents, leachates of vegetation, soil, animal feces, and wastewater treatment plant effluent. We found a considerable range of delta18Op, values (from +8.4 to +24.9 per thousand) for the various sources, and statistically significant differences were found between several of the source types. delta18Op measured in three different fresh water systems was generally not in equilibrium with ambient water. Although there is overlap in delta18Op values among the groups of samples, our results indicate that some sources are isotopically distinct and delta18Op can be used for identifying phosphate sources to aquatic systems.

  8. Effect of Fuel Composition on the Response of an Acoustically Forced Flat Flame

    Science.gov (United States)

    Gorski, Jan

    Interest in alternative fuels for power generation is growing, yet these fuels bring new challenges to gas turbine design and operation. Among these challenges are combustor operability issues, highlighted by problems with combustion instabilities. For this thesis, a fundamental study of the effects of fuel composition on combustion dynamics was undertaken. An acoustically forced flat flame burner was constructed, allowing measurement of the flame transfer function (FTF) relating acoustic perturbations to heat release rate fluctuations in the flame. Tests were done using methane, along with simulated syngas and biogas fuel mixtures over a variety of operating conditions. Large variations in methane concentration had a significant impact on the FTF, while variations in the hydrogen to carbon monoxide ratio did not impact the FTF in fuel mixtures of equal parts methane and syngas. The Strouhal number was found to be an important parameter in predicting phase response independent of the fuel type. Flame liftoff distance and fuel composition were the key parameters determining the peak FTF magnitude. A hypothesis on the role of the non-adiabatic nature of the flat flame and thermal-diffusive effects on the trends in peak FTF magnitude is presented and discussed.

  9. Fuel effects on the stability of turbulent flames with compositionally inhomogeneous inlets

    KAUST Repository

    Guiberti, T. F.

    2016-10-11

    This paper reports an analysis of the influence of fuels on the stabilization of turbulent piloted jet flames with inhomogeneous inlets. The burner is identical to that used earlier by the Sydney Group and employs two concentric tubes within the pilot stream. The inner tube, carrying fuel, can be recessed, leading to a varying degree of inhomogeneity in mixing with the outer air stream. Three fuels are tested: dimethyl ether (DME), liquefied petroleum gas (LPG), and compressed natural gas (CNG). It is found that improvement in flame stability at the optimal compositional inhomogeneity is highest for CNG and lowest for DME. Three possible reasons for this different enhancement in stability are investigated: mixing patterns, pilot effects, and fuel chemistry. Numerical simulations realized in the injection tube highlight similarities and differences in the mixing patterns for all three fuels and demonstrate that mixing cannot explain the different stability gains. Changing the heat release rates from the pilot affects the three fuels in similar ways and this also implies that the pilot stream is unlikely to be responsible for the observed differences. Fuel reactivity is identified as a key factor in enhancing stability at some optimal compositional inhomogeneity. This is confirmed by inference from joint images of PLIF-OH and PLIF-CHO, collected at a repetition rate of 10kHz in turbulent flames of DME, and from one-dimensional calculations of laminar flames using detailed chemistry for DME, CNG, and LPG.

  10. Nitrogen and oxygen isotopic composition of N sub(2)O from suboxic waters of the eastern tropical North Pacific and the Arabian Sea - measurement by continuous-flow isotope-ratio monitoring

    Digital Repository Service at National Institute of Oceanography (India)

    Yoshinari, T.; Altabet, M.A.; Naqvi, S.W.A.; Codispoti, L.; Jayakumar, D.A.; Kuhland, M.; Devol, A.

    and of the dual stable isotopic composition of N sub(2)O in the eastern tropical North Pacific (ETNP) and the Arabian Sea. The stable isotopic composition of N sub(2)O was determined by a new method that required only 80-100 nmol of N sub(2)O per sample analysis...

  11. Isotopic composition of low-latitude paleoprecipitation during the Early Cretaceous

    Science.gov (United States)

    Suarez, M.B.; Gonzalez, Luis A.; Ludvigson, Greg A.; Vega, F.J.; Alvarado-Ortega, J.

    2009-01-01

    The response of the hydrologic cycle in global greenhouse conditions is important to our understanding of future climate change and to the calibration of global climate models. Past greenhouse conditions, such as those of the Cretaceous, can be used to provide empirical data with which to evaluate climate models. Recent empirical studies have utilized pedogenic carbonates to estimate the isotopic composition of meteoric waters and calculate precipitation rates for the AptianAlbian. These studies were limited to data from mid(35??N) to high (75??N) paleolatitudes, and thus future improvements in accuracy will require more estimates of meteoric water compositions from numerous localities around the globe. This study provides data for tropical latitudes (18.5??N paleolatitude) from the Tlayua Formation, Puebla, Mexico. In addition, the study confirms a shallow nearshore depositional environment for the Tlayua Formation. Petrographic observations of fenestral fabrics, gypsum crystal molds, stromatolitic structures, and pedogenic matrix birefringence fabric support the interpretation that the strata represent deposition in a tidal flat environment. Carbonate isotopic data from limestones of the Tlayua Formation provide evidence of early meteoric diagenesis in the form of meteoric calcite lines. These trends in ??18O versus ??13C were used to calculate the mean ??18O value of meteoric water, which is estimated at -5.46 ?? 0.56??? (Vienna Standard Mean Ocean Water [VSMOW]). Positive linear covariant trends in oxygen and carbon isotopic values from some horizons were used to estimate evaporative losses of vadose groundwater from tropical exposure surfaces during the Albian, and the resulting values range from 8% to 12%. However, the presence of evaporative mineral molds indicates more extensive evaporation. The added tropical data improve latitudinal coverage of paleoprecipitation ??18O estimates. The data presented here imply that earlier isotope mass balance models most

  12. Isotopic Composition of Boron Secondary Ions as a Function of Ion-Beam Fluence.

    Science.gov (United States)

    Baumel, Laurie Michelle

    The experiment performed in this work isolates and examines the effects of mass on the composition of the sputtered flux from a multi-component target. Chemical complexities are minimized by measuring sputtered ions from a target consisting only of two isotopes of one element. In this case, chemical effects as well as inter-atomic potentials are assumed to be identical for all constituents moving within the target, thus simplifying the target kinematics. Since any non-stoichiometry in the sputtered material should be caused only by the effects of mass on the kinetics in the target, measuring the sputtered material and comparing various analytical predictions with the experimental results leads to a better understanding of mass effects in these targets. 100-keV argon and neon were used to sputter an elemental target comprising the two naturally occurring isotopes of boron. The resulting secondary ions were examined with an electrostatic quadrupole mass analyzer. At low beam fluences (~1 times 20^{15} ions/cm ^2) a light-isotope secondary ion enhancement is observed relative to the steady-state secondary ion yields collected at higher beam fluences ( ~5 times 10 ^{17} ions/cm^2 ). The steady-state ion yields are representative of the bulk composition of the target. The enhancement (46.1perthous for Ne^+ irradiation and 51.8perthous for Ar^+ irradiation) is large compared to the predictions of analytical theories and is determined to be independent of variations in surface potential, chemical effects, and surface impurities. This effect is consistent with an explanation based on an energy and momentum asymmetry in the collision cascade. The asymmetry was caused by an extra collision mechanism which allowed light particles to backscatter 180^circ (towards the target surface) from underlying heavier target particles whereas the reverse process can not occur. When irradiated with projectiles heavier than the target constituents, the heavier target particles had a higher

  13. Calcium isotopic composition of mantle xenoliths and minerals from Eastern China

    Science.gov (United States)

    Kang, Jin-Ting; Zhu, Hong-Li; Liu, Yu-Fei; Liu, Fang; Wu, Fei; Hao, Yan-Tao; Zhi, Xia-Chen; Zhang, Zhao-Feng; Huang, Fang

    2016-02-01

    This study presents calcium isotope data for co-existing clinopyroxenes (cpx), orthopyroxenes (opx), and olivine (ol) in mantle xenoliths to investigate Ca isotopic fractionation in the upper mantle. δ44/40Ca (δ44/40Ca (‰) = (44Ca/40Ca)SAMPLE/(44Ca/40Ca)SRM915a - 1) in opx varies from 0.95 ± 0.05‰ to 1.82 ± 0.01‰ and cpx from 0.71 ± 0.06‰ to 1.03 ± 0.12‰ (2se). δ44/40Ca in ol (P-15) is 1.16 ± 0.08‰, identical to δ44/40Ca of the co-existing opx (1.12 ± 0.09‰, 2se). The Δ44/40Caopx-cpx (Δ44/40Caopx-cpx = δ44/40Caopx-δ44/40Cacpx) shows a large variation ranging from -0.01‰ to 1.11‰ and it dramatically increases with decreasing of Ca/Mg (atomic ratio) in opx. These observations may reflect the effect of opx composition on the inter-mineral equilibrium fractionation of Ca isotopes, consistent with the theoretical prediction by first-principles theory calculations (Feng et al., 2014). Furthermore, Δ44/40Caopx-cpx decreases when temperature slightly increases from 1196 to 1267 K. However, the magnitude of such inter-mineral isotopic fractionation (1.12‰) is not consistent with the value calculated by the well-known correlation between inter-mineral isotope fractionation factors and 1/T2 (Urey, 1947). Instead, it may reflect the temperature control on crystal chemistry of opx (i.e., Ca content), which further affects Δ44/40Caopx-cpx. The calculated δ44/40Ca of bulk peridotites and pyroxenites range from 0.76 ± 0.06‰ to 1.04 ± 0.12‰ (2se). Notably, δ44/40Ca of bulk peridotites are positively correlated with CaO and negatively with MgO content. Such correlations can be explained by mixing between a fertile mantle end-member and a depleted one with low δ44/40Ca, indicating that Ca isotopes could be a useful tool in studying mantle evolution.

  14. The Effect of Phytase on the Oxygen Isotope Composition of Phosphate

    Science.gov (United States)

    von Sperber, C.; Tamburini, F.; Bernasconi, S. M.; Frossard, E.

    2013-12-01

    Plants and microorganisms under phosphorus (P) stress release extracellular phosphatases as a strategy to acquire inorganic phosphate (Pi) (1-2). These enzymes catalyze the hydrolysis of phosphoesters leading to a release of Pi. The enzymatic hydrolysis leads, via a nucleophilic attack, to the incorporation of one oxygen atom from the water into the newly formed Pi molecule. During the incorporation, an isotopic fractionation occurs, which might be used to identify the origin of Pi in the environment (3-6). While the effect of phosphomonoesterases and phosphodiesterases on the oxygen isotope composition of phosphate has been examined, there are, so far, no studies dealing with the effect of phytases (4-6). Phytases catalyze the hydrolysis of myo-inositol-hexakis-phosphate (IP6), which is an important component of organic P in many ecosystems (7). Enzymatic assays with phytase from wheat germ and Aspergillus niger were prepared under sterile and temperature controlled conditions in order to determine the effect of phytases on the oxygen isotope composition of phosphate, which has been liberated from IP6 via enzymatic hydrolysis. Assays with phytase from wheat germ lead to a turnover of the substrate close to 100%, while assays with phytase from Aspergillus niger lead to a turnover of the substrate close to 80%. In the case of the assays with phytase from wheat germ, our results indicate that one sixth of the total 24 oxygen which are associated to the phosphates in IP6 are exchanged with oxygen from water. From this we conclude that the incorporation of one oxygen atom from water occurs only at four phosphate molecules of IP6, while two phosphate molecules do not experience an incorporation of oxygen. This suggests that during the enzymatic hydrolysis, four P-O bonds and two C-O bonds are broken. Provided that, the isotopic fractionation can be calculated with an isotopic mass balance resulting in -8.4‰ (×3.6 SD). This is a value very similar to those reported

  15. The Boron Isotopic Composition of Elephant Dung: Inputs to the Global Boron Budget

    Science.gov (United States)

    Williams, L. B.; Hervig, R. L.

    2011-12-01

    A survey of boron in kerogen showed isotopically light δ11B values (0 to -50%) that are distinctly different from most mineral and natural water B reservoirs. Diagenesis releases this isotopically light B into pore fluids when hydrocarbons are generated, thus enriching oilfield brines in 10B. This observation suggests that borated biomolecules (BM) are primarily tetrahedral favoring 10B, whereas 11B is preferred in trigonal coordination. Plants, with optimal concentrations up to 100ppm, contribute more B than animal remains to sediment. Elephants are one of the largest herbivores on earth, consuming 200 - 250 kg of plant material/day and producing 50 kg of manure/day. They are inefficient at digestion, thus the manure contains >50% undigested plant material. Dung samples are therefore ideal for studying the δ11B of both the food input and digested output of a significant B supply to sedimentary systems. Horse and rabbit manure were studied for comparison to evaluate B isotope variations in the food supply and potential vital effects on the output. B-content and isotopic composition of dung plant material and digested fractions were measured in the solid state by secondary ion mass spectrometry. The digests were rinsed in 1.8% mannitol, a B-complexing agent, to remove surface adsorbed-B, then air dried and Au-coated for charge compensation. Results showed that the elephant diet contains 3-13 ppm B, with an average δ11B of -20 ± 0.8% (1σ), while rabbit food had 88 ppm B with a δ11B of -50 ± 1.3 %. The digested fraction of the elephant dung contains 4-10ppm B with average δ11B values of -12 ± 1.2%. In comparison, horse manure with 11-21 ppm B has a δ11B of -10.7 ± 0.5% and rabbit manure contains 2-3 ppm B with a δ11B of -8.8 ± 1%. Boron isotope compositions of these manures are indistinguishable (within error). Clearly plant material is a major contributor of isotopically light B to sediments. The herbivores studied fractionate their total B intake in

  16. In situ oxygen isotope compositions in olivines of different types of cosmic spherules: An assessment of relationships to chondritic particles

    Digital Repository Service at National Institute of Oceanography (India)

    Rudraswami, N.G.; ShyamPrasad, M.; Jones, R.H.; Nagashima, K.

    et al., 2015a). The micrometeorites that have entered Earth’s atmosphere at high zenith angle and low velocity are interesting because their petrologic and isotopic characteristics are largely preserved thereby providing constraints on the parent... et al., 2012). Oxygen isotope studies complemented by mineralogical compositions are vital to unravel the complexity involved in distinguishing the known components of micrometeorites and their parent bodies. For carbonaceous chondrites...

  17. Stable chromium isotopic composition of meteorites and metal-silicate experiments:Implications for fractionation during core formation

    OpenAIRE

    Bonnand, P; WILLIAMS, H. M.; Parkinson, I. J.; Wood, B.J.; Halliday, A. N.

    2016-01-01

    We present new mass independent and mass dependent Cr isotope compositions for meteorites measured by double spike thermal ionisation mass spectrometry. Small differences in both mass independent 53Cr and 54Cr relative to the Bulk Silicate Earth are reported and are very similar to previously published values. Carbonaceous chondrites are characterised by an excess in 54Cr compared to ordinary and enstatite chondrites which make mass independent Cr isotopes a useful tool for distinguishing bet...

  18. Composite Bipolar Plate for Unitized Fuel Cell/Electrolyzer Systems

    Science.gov (United States)

    Mittelsteadt, Cortney K.; Braff, William

    2009-01-01

    In a substantial improvement over present alkaline systems, an advanced hybrid bipolar plate for a unitized fuel cell/electrolyzer has been developed. This design, which operates on pure feed streams (H2/O2 and water, respectively) consists of a porous metallic foil filled with a polymer that has very high water transport properties. Combined with a second metallic plate, the pore-filled metallic plates form a bipolar plate with an empty cavity in the center.

  19. Stable isotope composition of bulk and secondary carbonates from the Quaternary loess-paleosol sequence in Sutto, Hungary

    DEFF Research Database (Denmark)

    Koeniger, Paul; Barta, Gabriella; Thiel, Christine

    2014-01-01

    , and microscale secondary (authigenic) carbonates (calcified root cells, carbonate coatings, hypocoatings, and earthworm biospheroids) and concretions at 10 cm resolution were analysed to interpret stable isotope variations. Isotope values of bulk samples were in the range of 2.6 parts per thousand to -13.9 parts......, secondary carbonates showed more depleted values than bulk samples. Calcified root cells have the most depleted isotope composition with mean values of -16.0 parts per thousand and -11.8 parts per thousand for delta C-13 and 8180, respectively. Results indicate that loess and paleosol secondary carbonates...

  20. The Nitrogen and Oxygen Isotope Composition of Porewater Nitrate from Bering Sea Sediments

    Science.gov (United States)

    Lehmann, M. F.; Sigman, D. M.; McCorkle, D. C.; Berelson, W. M.; Brunelle, B. G.; Hoffmann, S. S.

    2002-12-01

    We have measured the δ15N and δ18O of nitrate from sediment pore waters and the water column of the Bering Sea basin. The first high-resolution sediment porewater profile (with pore waters extracted by whole-core squeezing) shows an increase in nitrate δ15N and δ18O with depth in the sediment column (by 26‰ and 20‰ , respectively) as the nitrate concentration decreases from 45 to 0.5 μM, due to denitrification at depth. However, the nitrate δ15N and δ18O values in the shallow zone of nitrification are equal to or slightly lower than those of bottom water, suggesting that the deep denitrification does not greatly alter the isotopic composition of the nitrate in the shallowest porewaters or, in turn, in the bottom water. These results appear to be consistent with results from ex situ incubation and in situ benthic chamber experiments by ourselves and other investigators (Brandes et al., 1997), which show that loss of nitrate due to sedimentary denitrification is not accompanied by an isotopic effect on the nitrate of the overlying water. Measurements conducted during the GEOSECS and WOCE programs revealed the existence of a sizable deficit of remineralized nitrate in the deep Bering Sea, but water-column denitrification is not a likely mechanism for nitrate loss, since oxygen concentrations found in Bering Sea waters are too high (> 15 μM) to allow for bacterial nitrate reduction. Our water column measurements indicate that the nitrate deficit in the deep Bering Sea is not associated with nitrate isotopic enrichment. Together, our sediment and water column nitrate isotope analyses provide strong support for the earlier hypothesis that the deep Bering Sea nitrate deficit is due to sedimentary denitrification. J. A. Brandes and A. H. Devol, Geochim. Cosmochim. Acta, 61(9), 1793-1801 (1997).

  1. Compositional impact of acidification and warming on Fucus vesiculosus: First biogeochemical and stable isotope results from coastal benthocosm experiments

    Science.gov (United States)

    Winde, Vera; Al-Janabi, Balsam; Sokol, Steffani; Buchholz, Björn; Escher, Peter; Voss, Maren; Schneider, Bernd; Wahl, Martin; Böttcher, Michael E.

    2014-05-01

    In the frame of the German BIOACID II project, the separate and combined effects of warming and acidification on the elemental and stable isotope composition of Fucus vesiculosus are investigated by means of benthic mesocosm experiments in brackish waters of the Baltic Sea. We aim for a calibration of the composition of Fucus in response to single and combined temperature and pCO2 elevation. Benthocosm experiments are carried out in the Kiel Fjord with a fully crossed array of 2 globally importnant stressors: an increase in temperature and an increase in atmospheric CO2 partial pressure. The experiments run for almost 3 months per season (winter, spring, summer, autumn). There are analyses from the experiments of the aquatic chemistry (TA, pH, salinity, carbon isotope composition of DIC, main and trace elements and nutrients) as well as the composition of the Fucus vesiculosus organic tissues (C-N-S-P contents, and C and N stable isotope composition, as well as major and trace elements). The composition of the aqueous solution in the mesocosms was recovered two times a week and for the Fucus tissue at the start and the end of the experiments. In addition several 24h cycles were followed in high temporal resolution to characterize the community response to diurnal light cycles. It was found, that seasonal variations in the composition of the input solutions (brackish water from the Kiel Fjord) were reflected by changes in the experiments with short time delay. The changes in the aquatic chemistry of the mesocosms, however, were strongly superimposed for most parameters during daytime by biological activity. The response of the communities to light conditions was clearly observed during the 24h-campaigns, when alternating phases of net respiration and photosynthesis were creating strong variations in the dissolved carbonate system. These variations were accompanied by significant changes in the carbon isotope composition of DIC. The atmosphere of some experimental

  2. A kinetic chemistry tagging technique and its application to modelling the stable isotopic composition of atmospheric trace gases

    Directory of Open Access Journals (Sweden)

    S. Gromov

    2010-02-01

    Full Text Available Isotope composition, in many cases, holds unique information on sources, chemical modification and sinks of atmospheric trace gases. Vital to the interpretation and use of an increasing number of isotope analyses is appropriate modelling. However, the exact implementation of isotopic information is a challenge, and often studies use simplifications which limit their applicability. Here we confer a thorough isotopic extension to MECCA, a comprehensive kinetic chemistry sub-model. To this end, we devise a generic tagging technique for the kinetic chemistry mechanisms implemented as the sub-submodel MECCA-TAG. The technique constitutes a diagnostic tool that can benefit the investigation of various aspects of kinetic chemistry schemes; at the same time, the designed numerical optimisation reduces the computational effort while keeping important details unaffected. We further focus specifically on the modelling of stable isotopic composition, including the required extensions of the approach. The results of MECCA-TAG are evaluated against the reference sub-submodel MECCA-DBL, which is implicitly full-detailed, but necessarily is sub-optimal in practical applications due to its high computational demands. Furthermore, we evaluate the elaborate carbon and oxygen isotopic mechanism by simulating the multi-isotope composition of CO and other trace gases in the CAABA/MECCA box-model. The mechanism realistically simulates the oxygen isotope composition of key species resulting from the interchange with ozone and main atmospheric reservoirs, as well as the carbon isotope signature transfer. The model adequately reproduces the isotope chemistry features for CO under the limitation of the modelling domain. In particular, the mass-independently fractionated (MIF composition of CO due to reactions of ozone with unsaturated hydrocarbons (a source effect versus its intrinsic MIF enrichment induced in the removal reaction via oxidation by OH is assessed. As for

  3. A kinetic chemistry tagging technique and its application to modelling the stable isotopic composition of atmospheric trace gases

    Directory of Open Access Journals (Sweden)

    S. Gromov

    2010-08-01

    Full Text Available Isotope composition, in many cases, holds unique information on the sources, chemical modification and sinks of atmospheric trace gases. Vital to the interpretation and use of an increasing number of isotope analyses is appropriate modelling. However, the exact implementation of isotopic information in chemistry-climate models is a challenge, and often studies use simplifications which limit their applicability. Here we implement a thorough isotopic extension in MECCA, a comprehensive kinetic chemistry sub-model. To this end, we devise a generic tagging technique for the kinetic chemistry mechanisms implemented as the sub-submodel MECCA-TAG. The technique is diagnostic and numerically efficient and supports the investigation of various aspects of kinetic chemistry schemes. We focus specifically on the application to the modelling of stable isotopic composition. The results of MECCA-TAG are evaluated against the reference sub-submodel MECCA-DBL, which is implicitly full-detailed, but computationally expensive and thus sub-optimal in practical applications. Furthermore, we evaluate the elaborate carbon and oxygen isotopic mechanism by simulating the multi-isotope composition of CO and other trace gases in the CAABA/MECCA box-model. The mechanism realistically simulates the oxygen isotope composition of key species, as well as the carbon isotope signature transfer. The model adequately reproduces the isotope chemistry features for CO, taking into account the limits of the modelling domain. In particular, the mass-independently fractionated (MIF composition of CO due to reactions of ozone with unsaturated hydrocarbons (a source effect versus its intrinsic MIF enrichment induced in the removal reaction via oxidation by OH is assessed. The simulated ozone source effect was up to +1‰ in Δ17O(CO. The versatile modelling framework we employ (the Modular Earth Submodel System, MESSy opens the way for implementation of the novel detailed

  4. Chemical and isotopic composition of secondary organic aerosol generated by α-pinene ozonolysis

    Science.gov (United States)

    Meusinger, Carl; Dusek, Ulrike; King, Stephanie M.; Holzinger, Rupert; Rosenørn, Thomas; Sperlich, Peter; Julien, Maxime; Remaud, Gerald S.; Bilde, Merete; Röckmann, Thomas; Johnson, Matthew S.

    2017-05-01

    Secondary organic aerosol (SOA) plays a central role in air pollution and climate. However, the description of the sources and mechanisms leading to SOA is elusive despite decades of research. While stable isotope analysis is increasingly used to constrain sources of ambient aerosol, in many cases it is difficult to apply because neither the isotopic composition of aerosol precursors nor the fractionation of aerosol forming processes is well characterised. In this paper, SOA formation from ozonolysis of α-pinene - an important precursor and perhaps the best-known model system used in laboratory studies - was investigated using position-dependent and average determinations of 13C in α-pinene and advanced analysis of reaction products using thermal-desorption proton-transfer-reaction mass spectrometry (PTR-MS). The total carbon (TC) isotopic composition δ13C of the initial α-pinene was measured, and the δ13C of the specific carbon atom sites was determined using position-specific isotope analysis (PSIA). The PSIA analysis showed variations at individual positions from -6.9 to +10. 5 ‰ relative to the bulk composition. SOA was formed from α-pinene and ozone in a constant-flow chamber under dark, dry, and low