Ice-condenser aerosol tests

International Nuclear Information System (INIS)

Ligotke, M.W.; Eschbach, E.J.; Winegardner, W.K.

1991-09-01

This report presents the results of an experimental investigation of aerosol particle transport and capture using a full-scale height and reduced-scale cross section test facility based on the design of the ice compartment of a pressurized water reactor (PWR) ice-condenser containment system. Results of 38 tests included thermal-hydraulic as well as aerosol particle data. Particle retention in the test section was greatly influenced by thermal-hydraulic and aerosol test parameters. Test-average decontamination factor (DF) ranged between 1.0 and 36 (retentions between ∼0 and 97.2%). The measured test-average particle retentions for tests without and with ice and steam ranged between DF = 1.0 and 2.2 and DF = 2.4 and 36, respectively. In order to apparent importance, parameters that caused particle retention in the test section in the presence of ice were steam mole fraction (SMF), noncondensible gas flow rate (residence time), particle solubility, and inlet particle size. Ice-basket section noncondensible flows greater than 0.1 m 3 /s resulted in stable thermal stratification whereas flows less than 0.1 m 3 /s resulted in thermal behavior termed meandering with frequent temperature crossovers between flow channels. 10 refs., 66 figs., 16 tabs

Elemental composition and oxidation of chamber organic aerosol

Directory of Open Access Journals (Sweden)

P. S. Chhabra

2011-09-01

Full Text Available Recently, graphical representations of aerosol mass spectrometer (AMS spectra and elemental composition have been developed to explain the oxidative and aging processes of secondary organic aerosol (SOA. It has been shown previously that oxygenated organic aerosol (OOA components from ambient and laboratory data fall within a triangular region in the f₄₄ vs. f₄₃ space, where f₄₄ and f₄₃ are the ratios of the organic signal at m/z 44 and 43 to the total organic signal in AMS spectra, respectively; we refer to this graphical representation as the "triangle plot." Alternatively, the Van Krevelen diagram has been used to describe the evolution of functional groups in SOA. In this study we investigate the variability of SOA formed in chamber experiments from twelve different precursors in both "triangle plot" and Van Krevelen domains. Spectral and elemental data from the high-resolution Aerodyne aerosol mass spectrometer are compared to offline species identification analysis and FTIR filter analysis to better understand the changes in functional and elemental composition inherent in SOA formation and aging. We find that SOA formed under high- and low-NO_x conditions occupy similar areas in the "triangle plot" and Van Krevelen diagram and that SOA generated from already oxidized precursors allows for the exploration of areas higher on the "triangle plot" not easily accessible with non-oxidized precursors. As SOA ages, it migrates toward the top of the triangle along a path largely dependent on the precursor identity, which suggests increasing organic acid content and decreasing mass spectral variability. The most oxidized SOA come from the photooxidation of methoxyphenol precursors which yielded SOA O/C ratios near unity. α-pinene ozonolysis and naphthalene photooxidation SOA systems have had the highest degree of mass closure in previous chemical characterization studies and also show the

Modeling organic aerosol from the oxidation of α-pinene in a Potential Aerosol Mass (PAM chamber

Directory of Open Access Journals (Sweden)

S. Chen

2013-05-01

Full Text Available A model has been developed to simulate the formation and evolution of secondary organic aerosol (SOA and was tested against data produced in a Potential Aerosol Mass (PAM flow reactor and a large environmental chamber. The model framework is based on the two-dimensional volatility basis set approach (2D-VBS, in which SOA oxidation products in the model are distributed on the 2-D space of effective saturation concentration (Ci* and oxygen-to-carbon ratio (O : C. The modeled organic aerosol mass concentrations (COA and O : C agree with laboratory measurements within estimated uncertainties. However, while both measured and modeled O : C increase with increasing OH exposure as expected, the increase of modeled O : C is rapid at low OH exposure and then slows as OH exposure increases while the increase of measured O : C is initially slow and then accelerates as OH exposure increases. A global sensitivity analysis indicates that modeled COA values are most sensitive to the assumed values for the number of Ci* bins, the heterogeneous OH reaction rate coefficient, and the yield of first-generation products. Modeled SOA O : C values are most sensitive to the assumed O : C of first-generation oxidation products, the number of Ci* bins, the heterogeneous OH reaction rate coefficient, and the number of O : C bins. All these sensitivities vary as a function of OH exposure. The sensitivity analysis indicates that the 2D-VBS model framework may require modifications to resolve discrepancies between modeled and measured O : C as a function of OH exposure.

Special aerosol sources for certification and test of aerosol radiometers

International Nuclear Information System (INIS)

Belkina, S.K.; Zalmanzon, Y.E.; Kuznetsov, Y.V.; Rizin, A.I.; Fertman, D.E.

1991-01-01

The results are presented of the development and practical application of new radionuclide source types (Special Aerosol Sources (SAS)), that meet the international standard recommendations, which are used for certification and test of aerosol radiometers (monitors) using model aerosols of plutonium-239, strontium-yttrium-90 or uranium of natural isotope composition and certified against Union of Soviet Socialist Republics USSR national radioactive aerosol standard or by means of a reference radiometer. The original technology for source production allows the particular features of sampling to be taken into account as well as geometry and conditions of radionuclides radiation registration in the sample for the given type of radiometer. (author)

Special aerosol sources for certification and test of aerosol radiometers

Energy Technology Data Exchange (ETDEWEB)

Belkina, S.K.; Zalmanzon, Y.E.; Kuznetsov, Y.V.; Rizin, A.I.; Fertman, D.E. (Union Research Institute of Instrumentation, Moscow (USSR))

1991-01-01

The results are presented of the development and practical application of new radionuclide source types (Special Aerosol Sources (SAS)), that meet the international standard recommendations, which are used for certification and test of aerosol radiometers (monitors) using model aerosols of plutonium-239, strontium-yttrium-90 or uranium of natural isotope composition and certified against Union of Soviet Socialist Republics USSR national radioactive aerosol standard or by means of a reference radiometer. The original technology for source production allows the particular features of sampling to be taken into account as well as geometry and conditions of radionuclides radiation registration in the sample for the given type of radiometer. (author).

Characteristics of agglomerates of sodium oxide aerosol particles: Task 7, topical report

International Nuclear Information System (INIS)

Gieseke, J.A.; Reed, L.D.; Jordan, H.; Lee, K.W.

1977-01-01

Accurate macroscopic predictions of aerosol population behavior within enclosed containments are known to depend strongly upon the microscopic characteristics of the individual aerosols. Also, coagulation rates due to mechanisms which produce relative motions between particles within the suspended aerosol are known to depend upon the cross sectional areas of the individual particles. Hence, it has been the primary concern of this study to examine experimentally the microscopic characteristics of sodium oxide aerosols produced in air. The results of these measurements can now be incorporated into the various macroscopic aerosol behavior prediction models

Environmental health hazards of e-cigarettes and their components: Oxidants and copper in e-cigarette aerosols

International Nuclear Information System (INIS)

Lerner, Chad A.; Sundar, Isaac K.; Watson, Richard M.; Elder, Alison; Jones, Ryan; Done, Douglas; Kurtzman, Rachel; Ossip, Deborah J.; Robinson, Risa; McIntosh, Scott; Rahman, Irfan

2015-01-01

To narrow the gap in our understanding of potential oxidative properties associated with Electronic Nicotine Delivery Systems (ENDS) i.e. e-cigarettes, we employed semi-quantitative methods to detect oxidant reactivity in disposable components of ENDS/e-cigarettes (batteries and cartomizers) using a fluorescein indicator. These components exhibit oxidants/reactive oxygen species reactivity similar to used conventional cigarette filters. Oxidants/reactive oxygen species reactivity in e-cigarette aerosols was also similar to oxidant reactivity in cigarette smoke. A cascade particle impactor allowed sieving of a range of particle size distributions between 0.450 and 2.02 μm in aerosols from an e-cigarette. Copper, being among these particles, is 6.1 times higher per puff than reported previously for conventional cigarette smoke. The detection of a potentially cytotoxic metal as well as oxidants from e-cigarette and its components raises concern regarding the safety of e-cigarettes use and the disposal of e-cigarette waste products into the environment. - Highlights: • E-cigarettes disposal is associated with environmental health hazard/pollution. • Oxidants associated with electronic cigarette components and aerosols. • Metal copper and nanoparticles detected in electronic cigarette aerosols. • Environmental disposal of e-cigarettes components must be regulated with guidelines. - An electronic cigarette with disposable cartomizer exhibits oxidant reactivity similar to conventional cigarettes and releases copper and other particles associated with its aerosols

A new oxidation flow reactor for measuring secondary aerosol formation of rapidly changing emission sources

Science.gov (United States)

Simonen, Pauli; Saukko, Erkka; Karjalainen, Panu; Timonen, Hilkka; Bloss, Matthew; Aakko-Saksa, Päivi; Rönkkö, Topi; Keskinen, Jorma; Dal Maso, Miikka

2017-04-01

Oxidation flow reactors (OFRs) or environmental chambers can be used to estimate secondary aerosol formation potential of different emission sources. Emissions from anthropogenic sources, such as vehicles, often vary on short timescales. For example, to identify the vehicle driving conditions that lead to high potential secondary aerosol emissions, rapid oxidation of exhaust is needed. However, the residence times in environmental chambers and in most oxidation flow reactors are too long to study these transient effects ( ˜ 100 s in flow reactors and several hours in environmental chambers). Here, we present a new oxidation flow reactor, TSAR (TUT Secondary Aerosol Reactor), which has a short residence time ( ˜ 40 s) and near-laminar flow conditions. These improvements are achieved by reducing the reactor radius and volume. This allows studying, for example, the effect of vehicle driving conditions on the secondary aerosol formation potential of the exhaust. We show that the flow pattern in TSAR is nearly laminar and particle losses are negligible. The secondary organic aerosol (SOA) produced in TSAR has a similar mass spectrum to the SOA produced in the state-of-the-art reactor, PAM (potential aerosol mass). Both reactors produce the same amount of mass, but TSAR has a higher time resolution. We also show that TSAR is capable of measuring the secondary aerosol formation potential of a vehicle during a transient driving cycle and that the fast response of TSAR reveals how different driving conditions affect the amount of formed secondary aerosol. Thus, TSAR can be used to study rapidly changing emission sources, especially the vehicular emissions during transient driving.

Physicochemical Characterization of Capstone Depleted Uranium Aerosols III: Morphologic and Chemical Oxide Analyses

International Nuclear Information System (INIS)

Krupka, Kenneth M.; Parkhurst, MaryAnn; Gold, Kenneth; Arey, Bruce W.; Jenson, Evan D.; Guilmette, Raymond A.

2009-01-01

The impact of depleted uranium (DU) penetrators against an armored target causes erosion and fragmentation of the penetrators, the extent of which is dependent on the thickness and material composition of the target. Vigorous oxidation of the DU particles and fragments creates an aerosol of DU oxide particles and DU particle agglomerations combined with target materials. Aerosols from the Capstone DU aerosol study, in which vehicles were perforated by DU penetrators, were evaluated for their oxidation states using X-ray diffraction (XRD) and particle morphologies using scanning electron microscopy/energy dispersive spectrometry (SEM/EDS). The oxidation state of a DU aerosol is important as it offers a clue to its solubility in lung fluids. The XRD analysis showed that the aerosols evaluated were a combination primarily of U3O8 (insoluble) and UO3 (relatively more soluble) phases, though intermediate phases resembling U4O9 and other oxides were prominent in some samples. Analysis of particle residues in the micrometer-size range by SEM/EDS provided microstructural information such as phase composition and distribution, fracture morphology, size distribution, and material homogeneity. Observations from SEM analysis show a wide variability in the shapes of the DU particles. Some of the larger particles appear to have been fractured (perhaps as a result of abrasion and comminution); others were spherical, occasionally with dendritic or lobed surface structures. Amorphous conglomerates containing metals other than uranium were also common, especially with the smallest particle sizes. A few samples seemed to contain small chunks of nearly pure uranium metal, which were verified by EDS to have a higher uranium content exceeding that expected for uranium oxides. Results of the XRD and SEM/EDS analyses were used in other studies described in this issue of The Journal of Health Physics to interpret the results of lung solubility studies and in selecting input parameters for

Effect of glutathione aerosol on oxidant-antioxidant imbalance in idiopathic pulmonary fibrosis.

Science.gov (United States)

Borok, Z; Buhl, R; Grimes, G J; Bokser, A D; Hubbard, R C; Holroyd, K J; Roum, J H; Czerski, D B; Cantin, A M; Crystal, R G

1991-07-27

Idiopathic pulmonary fibrosis (IPF) is characterised by alveolar inflammation, exaggerated release of oxidants, and subnormal concentrations of the antioxidant glutathione in respiratory epithelial lining fluid (ELF). Glutathione (600 mg twice daily for 3 days) was given by aerosol to 10 patients with IPF. Total ELF glutathione rose transiently, ELF oxidised glutathione concentrations increased, and there was a decrease in spontaneous superoxide anion release by alveolar macrophages. Thus, glutathione by aerosol could be a means of reversing the oxidant-antioxidant imbalance in IPF.

Study of the sodium oxide aerosol behavior in a containment building

International Nuclear Information System (INIS)

Fermandjian, Jean.

1982-01-01

Fast breeder reactor safety analysis needs validated models to predict the behavior of sodium oxide aerosols (released during hypothetical accidents) in the different reactor compartments and, in particular, to evaluate the quantity (and the size distribution) of the particles which can be released outside the containment building by taking into account the associated devices (ventilation, especially). In order to validate the computer models, experimental tests were performed by CEA/DSN (Atomic Energy Commission/Nuclear Safety Department) at Cadarache: sodium pool fire tests in a 400 m 3 concrete vessel (CASSANDRE tests) and in a 4.4 m 3 steel vessel (EMIS tests). Furthermore, we utilized the results of the experimental tests performed by our German colleagues of KFK/LAF (Kernforschungszentrum Karlsruhe/Laboratorium fuer Aerosolphysik und Filtertechnik): sodium pool fire tests in a 220 m 3 steel vessel (FAUNA tests). The application of the computer models to the experimental tests and to the reactor case allowed us: - to explain the differences observed between the results given by the codes ''with log-normal hypothesis'' (HAARM 3) and ''with finite difference'' (PARDISEKO 3B), - to define the limits of application of the codes ''with log-normal hypothesis'', - to determine the important parameters (characteristics of the aerosol source, form factors of the agglomerates and collision efficiency) and the important phenomena (turbulent coagulation, in particular) [fr

Plutonium-containing aerosols found within containment enclosures in industrial mixed-oxide reactor fuel fabrication

International Nuclear Information System (INIS)

Newton, G.J.; Yeh, H.C.; Stanley, J.A.

1977-01-01

Mixed oxide (PuO 2 and UO 2 ) nuclear reactor fuel pellets are fabricated within safety enclosures at Babcock and Wilcox's Park Township site near Apollo, PA. Forty-two sample runs of plutonium-containing aerosols were taken from within glove boxes during routine industrial operations. A small, seven-stage cascade impactor and the Lovelace Aerosol Particle Separator (LAPS) were used to determine aerodynamic size distribution and gross alpha aerosol concentration. Powder comminution and blending produced aerosols with lognormal size distributions characterized by activity median aerodynamic diameters (AMAD) of 1.89 +- 0.33 μm, sigma/sub g/ = 1.62 +- 0.09 and a gross alpha aerosol concentration range of 0.1 to 150 nCi/l. Slug pressing and grinding produced aerosols of AMAD = 3.08 +- 0.1 μm, sigma/sub g/ = 1.53 +- 0.01 and AMAD = 2.26 +- 0.16 μm, sigma/sub g/ = 1.68 +- 0.20, respectively. Gross alpha aerosol concentrations ranged from 3.4 to 450 nCi/l. Centerless grinding produced similar-sized aerosols but the gross alpha concentration ranged from 220 to 1690 nCi/l. In vitro solubility studies on selected LAPS samples in a lung fluid simulant indicate that plutonium mixed-oxide aerosols are more soluble than laboratory-produced plutonium aerosols

Analyses of CsI aerosol deposition in aerosol behavior tests in WIND project

International Nuclear Information System (INIS)

Kudo, Tamotsu; Shibazaki, Hiroaki; Hidaka, Akihide

1999-01-01

The aerosol deposition tests have been performed in WIND project at JAERI to characterize the aerosol behavior. The aerosol deposition tests named WAV1-D and WAV2-D were analyzed by aerosol behavior analysis codes, JAERI's ART and SNL's VICTORIA. The comparison calculation was performed for the confirmation of the analytical capabilities of the both codes and improvement of the models in ART. The deposition mass calculated by ART was larger than that by VICTORIA. This discrepancy is caused by differences in model for FP vapor condensation onto the wall surface. In the WAV2-D test, in which boric acid was placed on the floor area of the test section prior to the deposition phase to simulate the PWR primary coolant, there was a discrepancy in deposition mass between analytical results in both codes and experimental results. The discrepancy may be caused by existence of boric acid which is not considered in the codes. (author)

Characterization of aerosol photooxidation flow reactors: heterogeneous oxidation, secondary organic aerosol formation and cloud condensation nuclei activity measurements

Directory of Open Access Journals (Sweden)

A. T. Lambe

2011-03-01

Full Text Available Motivated by the need to develop instrumental techniques for characterizing organic aerosol aging, we report on the performance of the Toronto Photo-Oxidation Tube (TPOT and Potential Aerosol Mass (PAM flow tube reactors under a variety of experimental conditions. The PAM system was designed with lower surface-area-to-volume (SA/V ratio to minimize wall effects; the TPOT reactor was designed to study heterogeneous aerosol chemistry where wall loss can be independently measured. The following studies were performed: (1 transmission efficiency measurements for CO₂, SO₂, and bis(2-ethylhexyl sebacate (BES particles, (2 H₂SO₄ yield measurements from the oxidation of SO₂, (3 residence time distribution (RTD measurements for CO₂, SO₂, and BES particles, (4 aerosol mass spectra, O/C and H/C ratios, and cloud condensation nuclei (CCN activity measurements of BES particles exposed to OH radicals, and (5 aerosol mass spectra, O/C and H/C ratios, CCN activity, and yield measurements of secondary organic aerosol (SOA generated from gas-phase OH oxidation of m-xylene and α-pinene. OH exposures ranged from (2.0 ± 1.0 × 10¹⁰ to (1.8 ± 0.3 × 10¹² molec cm⁻³ s. Where applicable, data from the flow tube reactors are compared with published results from the Caltech smog chamber. The TPOT yielded narrower RTDs. However, its transmission efficiency for SO₂ was lower than that for the PAM. Transmission efficiency for BES and H₂SO₄ particles was size-dependent and was similar for the two flow tube designs. Oxidized BES particles had similar O/C and H/C ratios and CCN activity at OH exposures greater than 10¹¹ molec cm⁻³ s, but different CCN activity at lower OH exposures. The O/C ratio, H/C ratio, and yield of m-xylene and α-pinene SOA was strongly affected by reactor design and

Aerosol and Photo-Oxidant Processes in the Eastern Mediterranean

Czech Academy of Sciences Publication Activity Database

Lazaridis, M.; Spyridaki, A.; Solberg, S.; Smolík, Jiří; Ždímal, Vladimír; Eleftheriadis, K.; Aleksandropoulos, V.; Hov, O.; Georgopoulos, P. G.

2004-01-01

Roč. 4, - (2004), s. 5455-5514 ISSN 1680-7367 Grant - others:ENVK2(XE) 1999-00052 Institutional research plan: CEZ:AV0Z4072921 Keywords : aerosol * mesoscale modeling * photo-oxidant processes Subject RIV: CF - Physical ; Theoretical Chemistry

Intercomparison test of various aerosol measurement techniques

International Nuclear Information System (INIS)

Cherdron, W.; Hassa, C.; Jordan, S.

1984-01-01

At the suggestion of the CONT group (Containment Loading and Response), which is a subgroup of the Safety Working Group of the Fast Reactor Coordinating Committee, a group of experts undertook a comparison of the techniques of sodium aerosol measurement used in various laboratories in the EC. The following laboratories took part in the exercise: CEN-Mol (Belgium), CEA-Cadarache (France), CEA-Fontenay-aux-Roses (France), KfK-Karlsruhe (Federal Republic of Germany), ENEA-Bologna (Italy), and UKAEA-Winfrith (United Kingdom). The objective of the aerosol measurement workshop was to assess the applicability and reliability of specific aerosol measuring instruments. Measurements performed with equipment from the participating laboratories were evaluated using a standard procedure. This enabled an estimate of the accuracy of the experimental data to be provided for the verification of aerosol codes. Thus these results can be used as input for the physical modelling of aerosol behaviour, and the work reported here is a contribution to the definition of the radioactive source term for severe accidents in LMFBRs. The aerosol experts participating in the exercise agreed to concentrate on the techniques of measuring aerosol particle size distributions. The tests were performed at the FAUNA test facility using the aerosol loop. A sodium spray fire, which provides a continuous aerosol source of variable concentration, was produced under open-loop conditions in this facility. Although the primary objective of the workshop was to determine the particle size distributions of the aerosols, measurements of the sodium mass concentration were also made

Size-resolved mass concentrations of iron oxide aerosols and size-resolved number concentrations of iron oxide aerosols collected from King Air aircraft in Yellow Sea and East China Sea from 2013-02-14 to 2013-03-10 (NCEI Accession 0162201)

Data.gov (United States)

National Oceanic and Atmospheric Administration, Department of Commerce — This dataset contains size-resolved mass concentrations of iron oxide aerosols and size-resolved number concentrations of iron oxide aerosols, measured using the...

Physicochemical characterization of Capstone depleted uranium aerosols III: morphologic and chemical oxide analyses.

Science.gov (United States)

Krupka, Kenneth M; Parkhurst, Mary Ann; Gold, Kenneth; Arey, Bruce W; Jenson, Evan D; Guilmette, Raymond A

2009-03-01

The impact of depleted uranium (DU) penetrators against an armored target causes erosion and fragmentation of the penetrators, the extent of which is dependent on the thickness and material composition of the target. Vigorous oxidation of the DU particles and fragments creates an aerosol of DU oxide particles and DU particle agglomerations combined with target materials. Aerosols from the Capstone DU aerosol study, in which vehicles were perforated by DU penetrators, were evaluated for their oxidation states using x-ray diffraction (XRD), and particle morphologies were examined using scanning electron microscopy/energy dispersive spectroscopy (SEM/EDS). The oxidation state of a DU aerosol is important as it offers a clue to its solubility in lung fluids. The XRD analysis showed that the aerosols evaluated were a combination primarily of U3O8 (insoluble) and UO3 (relatively more soluble) phases, though intermediate phases resembling U4O9 and other oxides were prominent in some samples. Analysis of particle residues in the micrometer-size range by SEM/EDS provided microstructural information such as phase composition and distribution, fracture morphology, size distribution, and material homogeneity. Observations from SEM analysis show a wide variability in the shapes of the DU particles. Some of the larger particles were spherical, occasionally with dendritic or lobed surface structures. Others appear to have fractures that perhaps resulted from abrasion and comminution, or shear bands that developed from plastic deformation of the DU material. Amorphous conglomerates containing metals other than uranium were also common, especially with the smallest particle sizes. A few samples seemed to contain small bits of nearly pure uranium metal, which were verified by EDS to have a higher uranium content exceeding that expected for uranium oxides. Results of the XRD and SEM/EDS analyses were used in other studies described in this issue of Health Physics to interpret the

High formation of secondary organic aerosol from the photo-oxidation of toluene

Directory of Open Access Journals (Sweden)

L. Hildebrandt

2009-05-01

Full Text Available Toluene and other aromatics have long been viewed as the dominant anthropogenic secondary organic aerosol (SOA precursors, but the SOA mass yields from toluene reported in previous studies vary widely. Experiments conducted in the Carnegie Mellon University environmental chamber to study SOA formation from the photo-oxidation of toluene show significantly larger SOA production than parameterizations employed in current air-quality models. Aerosol mass yields depend on experimental conditions: yields are higher under higher UV intensity, under low-NO_x conditions and at lower temperatures. The extent of oxidation of the aerosol also varies with experimental conditions, consistent with ongoing, progressive photochemical aging of the toluene SOA. Measurements using a thermodenuder system suggest that the aerosol formed under high- and low-NO_x conditions is semi-volatile. These results suggest that SOA formation from toluene depends strongly on ambient conditions. An approximate parameterization is proposed for use in air-quality models until a more thorough treatment accounting for the dynamic nature of this system becomes available.

Containment aerosol behaviour simulation studies in the BARC nuclear aerosol test facility

International Nuclear Information System (INIS)

Mayya, Y.S.; Sapra, B.K.; Khan, Arshad; Sunny, Faby; Nair, R.N.; Raghunath, Radha; Tripathi, R.M.; Markandeya, S.G.; Puranik, V.D.; Ghosh, A.K.; Kushwaha, H.S.; Shreekumar, K.P.; Padmanabhan, P.V.A.; Murthy, P.S.S.; Venlataramani, N.

2005-02-01

A Nuclear Aerosol Test Facility (NATF) has been built and commissioned at Bhabha Atomic Research Centre to carry out simulation studies on the behaviour of aerosols released into the reactor containment under accident conditions. This report also discusses some new experimental techniques for estimation of density of metallic aggregates. The experimental studies have shown that the dynamic densities of aerosol aggregates are far lower than their material densities as expected by the well-known fractal theory of aggregates. In the context of codes, this has significant bearing in providing a mechanistic basis for the input density parameter used in estimating the aerosol evolution characteristics. The data generated under the quiescent and turbulent conditions and the information on aggregate densities are now being subjected to the validation of the aerosol behaviour codes. (author)

Charge distribution on plutonium-containing aerosols produced in mixed-oxide reactor fuel fabrication and the laboratory

International Nuclear Information System (INIS)

Yeh, H.C.; Newton, G.J.; Teague, S.V.

1976-01-01

The inhalation toxicity of potentially toxic aerosols may be affected by the electrostatic charge on the particles. Charge may influence the deposition site during inhalation and therefore its subsequent clearance and dose patterns. The electrostatic charge distributions on plutonium-containing aerosols were measured with a miniature, parallel plate, aerosol electrical mobility spectrometer. Two aerosols were studied: a laboratory-produced 238 PuO 2 aerosol (15.8 Ci/g) and a plutonium mixed-oxide aerosol (PU-MOX, natural UO 2 plus PuO 2 , 0.02 Ci/g) formed during industrial centerless grinding of mixed-oxide reactor fuel pellets. Plutonium-238 dioxide particles produced in the laboratory exhibited a small net positive charge within a few minutes after passing through a 85 Kr discharger due to alpha particle emission removal of valence electrons. PU-MOX aerosols produced during centerless grinding showed a charge distribution essentially in Boltzmann equilibrium. The gross alpha aerosol concentrations (960-1200 nCi/l) within the glove box were sufficient to provide high ion concentrations capable of discharging the charge induced by mechanical and/or nuclear decay processes

Pretest aerosol code comparisons for LWR aerosol containment tests LA1 and LA2

International Nuclear Information System (INIS)

Wright, A.L.; Wilson, J.H.; Arwood, P.C.

1986-01-01

The Light-Water-Reactor (LWR) Aerosol Containment Experiments (LACE) are being performed in Richland, Washington, at the Hanford Engineering Development Laboratory (HEDL) under the leadership of an international project board and the Electric Power Research Institute. These tests have two objectives: (1) to investigate, at large scale, the inherent aerosol retention behavior in LWR containments under simulated severe accident conditions, and (2) to provide an experimental data base for validating aerosol behavior and thermal-hydraulic computer codes. Aerosol computer-code comparison activities are being coordinated at the Oak Ridge National Laboratory. For each of the six LACE tests, ''pretest'' calculations (for code-to-code comparisons) and ''posttest'' calculations (for code-to-test data comparisons) are being performed. The overall goals of the comparison effort are (1) to provide code users with experience in applying their codes to LWR accident-sequence conditions and (2) to evaluate and improve the code models

Secondary organic aerosol from VOC mixtures in an oxidation flow reactor

Science.gov (United States)

Ahlberg, Erik; Falk, John; Eriksson, Axel; Holst, Thomas; Brune, William H.; Kristensson, Adam; Roldin, Pontus; Svenningsson, Birgitta

2017-07-01

The atmospheric organic aerosol is a tremendously complex system in terms of chemical content. Models generally treat the mixtures as ideal, something which has been questioned owing to model-measurement discrepancies. We used an oxidation flow reactor to produce secondary organic aerosol (SOA) mixtures containing oxidation products of biogenic (α-pinene, myrcene and isoprene) and anthropogenic (m-xylene) volatile organic compounds (VOCs). The resulting volume concentration and chemical composition was measured using a scanning mobility particle sizer (SMPS) and a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), respectively. The SOA mass yield of the mixtures was compared to a partitioning model constructed from single VOC experiments. The single VOC SOA mass yields with no wall-loss correction applied are comparable to previous experiments. In the mixtures containing myrcene a higher yield than expected was produced. We attribute this to an increased condensation sink, arising from myrcene producing a significantly higher number of nucleation particles compared to the other precursors. Isoprene did not produce much mass in single VOC experiments but contributed to the mass of the mixtures. The effect of high concentrations of isoprene on the OH exposure was found to be small, even at OH reactivities that previously have been reported to significantly suppress OH exposures in oxidation flow reactors. Furthermore, isoprene shifted the particle size distribution of mixtures towards larger sizes, which could be due to a change in oxidant dynamics inside the reactor.

Generation and oxidation of aerosol deposited PdAg nanoparticles

Science.gov (United States)

Blomberg, S.; Gustafson, J.; Martin, N. M.; Messing, M. E.; Deppert, K.; Liu, Z.; Chang, R.; Fernandes, V. R.; Borg, A.; Grönbeck, H.; Lundgren, E.

2013-10-01

PdAg nanoparticles with a diameter of 10 nm have been generated by an aerosol particle method, and supported on a silica substrate. By using a combination of X-ray Energy Dispersive Spectroscopy and X-ray Photoelectron Spectroscopy it is shown that the size distribution of the particles is narrow and that the two metals form an alloy with a mixture of 75% Pd and 25% Ag. Under oxidizing conditions, Pd is found to segregate to the surface and a thin PdO like oxide is formed similar to the surface oxide previously reported on extended PdAg and pure Pd surfaces.

LWR aerosol containment experiments (LACE) program and initial test results

International Nuclear Information System (INIS)

Muhlestein, L.D.; Hilliard, R.K.; Bloom, G.R.; McCormack, J.D.; Rahn, F.J.

1985-01-01

The LWR aerosol containment experiments (LACE) program is described. The LACE program is being performed at the Hanford Engineer Development Laboratory (operated by Westinghouse Hanford Company) and the initial tests are sponsored by EPRI. The objectives of the LACE program are: to demonstrate, at large-scale, inherent radioactive aerosol retention behavior for postulated high consequence LWR accident situations; and to provide a data base to be used for aerosol behavior . Test results from the first phase of the LACE program are presented and discussed. Three large-scale scoping tests, simulating a containment bypass accident sequence, demonstrated the extent of agglomeration and deposition of aerosols occurring in the pipe pathway and vented auxiliary building under realistic accident conditions. Parameters varied during the scoping tests were aerosol type and steam condensation

Summary of aerosol code-comparison results for LWR aerosol containment tests LA1, LA2, and LA3

International Nuclear Information System (INIS)

Wright, A.L.; Wilson, J.H.; Arwood, P.C.

1987-01-01

The light-water reactor (LWR) aerosol containment experiments (LACE) are being performed in Richland, Washington, at the Hanford Engineering Development Laboratory under the leadership of an international project board and the Electric Power Research Institute. These tests have two objectives: (1) to investigate, at large scale, the inherent aerosol retention behavior in LWR containments under simulated severe accident conditions, and (2) to provide an experimental data base for validating aerosol behavior and thermal-hydraulic computer codes. Aerosol computer-code comparison activities for the LACE tests are being coordinated at the Oak Ridge National Laboratory. For each of the six experiments, pretest calculations (for code-to-code comparisons) and blind post-test calculations (for code-to-test data comparisons) are being performed. This paper presents a summary of the pretest aerosol-code results for tests LA1, LA2, and LA3

Carbon oxidation state as a metric for describing the chemistry of atmospheric organic aerosol

Energy Technology Data Exchange (ETDEWEB)

Massachusetts Institute of Technology; Kroll, Jesse H.; Donahue, Neil M.; Jimenez, Jose L.; Kessler, Sean H.; Canagaratna, Manjula R.; Wilson, Kevin R.; Altieri, Katye E.; Mazzoleni, Lynn R.; Wozniak, Andrew S.; Bluhm, Hendrik; Mysak, Erin R.; Smith, Jared D.; Kolb, Charles E.; Worsnop, Douglas R.

2010-11-05

A detailed understanding of the sources, transformations, and fates of organic species in the environment is crucial because of the central roles that organics play in human health, biogeochemical cycles, and Earth's climate. However, such an understanding is hindered by the immense chemical complexity of environmental mixtures of organics; for example, atmospheric organic aerosol consists of at least thousands of individual compounds, all of which likely evolve chemically over their atmospheric lifetimes. Here we demonstrate the utility of describing organic aerosol (and other complex organic mixtures) in terms of average carbon oxidation state (OSC), a quantity that always increases with oxidation, and is readily measured using state-of-the-art analytical techniques. Field and laboratory measurements of OSC , using several such techniques, constrain the chemical properties of the organics and demonstrate that the formation and evolution of organic aerosol involves simultaneous changes to both carbon oxidation state and carbon number (nC).

Fission product aerosol removal test by containment spray under accident management conditions (3)

International Nuclear Information System (INIS)

Watanabe, Atsushi; Nagasaka, Hideo; Yokobori, Seiichi; Akinaga, Makoto

2000-01-01

In order to demonstrate the effective FP aerosol removal by containment spray under Japanese AM conditions, two system integral tests and two separate effect tests were carried out using a full-height simulation test facility. In case of PWR LOCA, aerosol concentration in the upper containment vessel decreased even under low spray flow rate. In case of BWR LOCA with water injection into RPV, the aerosol concentration in the entire vessel also decreased rapidly after aerosol supply stopping. In both cases, the removal rate estimated from the NUREG-1465 was coincided with test results. The aerosol washing effect by spray was confirmed to be predominant by conducting suppression chamber isolation test. It turned out that the effect of aerosol solubility and density on aerosol removal by spray was quite small by conducting insoluble aerosol injection test. After the modification of aerosol removal model by the spray and hygroscopic aerosol model in original MELCOR 1.8.4, calculated aerosol concentration transient in the containment vessel agreed well with the test data. (author)

Laboratory studies of the chemical composition and cloud condensation nuclei (CCN activity of secondary organic aerosol (SOA and oxidized primary organic aerosol (OPOA

Directory of Open Access Journals (Sweden)

A. T. Lambe

2011-09-01

Full Text Available Secondary organic aerosol (SOA and oxidized primary organic aerosol (OPOA were produced in laboratory experiments from the oxidation of fourteen precursors representing atmospherically relevant biogenic and anthropogenic sources. The SOA and OPOA particles were generated via controlled exposure of precursors to OH radicals and/or O₃ in a Potential Aerosol Mass (PAM flow reactor over timescales equivalent to 1–20 days of atmospheric aging. Aerosol mass spectra of SOA and OPOA were measured with an Aerodyne aerosol mass spectrometer (AMS. The fraction of AMS signal at m/z = 43 and m/z = 44 (f₄₃, f₄₄, the hydrogen-to-carbon (H/C ratio, and the oxygen-to-carbon (O/C ratio of the SOA and OPOA were obtained, which are commonly used to characterize the level of oxidation of oxygenated organic aerosol (OOA. The results show that PAM-generated SOA and OPOA can reproduce and extend the observed f₄₄–f₄₃ composition beyond that of ambient OOA as measured by an AMS. Van Krevelen diagrams showing H/C ratio as a function of O/C ratio suggest an oxidation mechanism involving formation of carboxylic acids concurrent with fragmentation of carbon-carbon bonds. Cloud condensation nuclei (CCN activity of PAM-generated SOA and OPOA was measured as a function of OH exposure and characterized as a function of O/C ratio. CCN activity of the SOA and OPOA, which was characterized in the form of the hygroscopicity parameter κ_org, ranged from 8.4×10⁻⁴ to 0.28 over measured O/C ratios ranging from 0.05 to 1.42. This range of κ_org and O/C ratio is significantly wider than has been previously obtained. To first order, the κ_org-to-O/C relationship is well represented by a linear function of the form κ_org = (0.18±0.04 ×O/C + 0.03, suggesting that a simple, semi-empirical parameterization of OOA hygroscopicity and

High formation of secondary organic aerosol from the photo-oxidation of toluene

OpenAIRE

L. Hildebrandt; N. M. Donahue; S. N. Pandis

2009-01-01

Toluene and other aromatics have long been viewed as the dominant anthropogenic secondary organic aerosol (SOA) precursors, but the SOA mass yields from toluene reported in previous studies vary widely. Experiments conducted in the Carnegie Mellon University environmental chamber to study SOA formation from the photo-oxidation of toluene show significantly larger SOA production than parameterizations employed in current air-quality models. Aerosol mass yields depend on experimental co...

Aerosol composition, oxidation properties, and sources in Beijing: results from the 2014 Asia-Pacific Economic Cooperation summit study

Science.gov (United States)

Xu, W. Q.; Sun, Y. L.; Chen, C.; Du, W.; Han, T. T.; Wang, Q. Q.; Fu, P. Q.; Wang, Z. F.; Zhao, X. J.; Zhou, L. B.; Ji, D. S.; Wang, P. C.; Worsnop, D. R.

2015-12-01

The mitigation of air pollution in megacities remains a great challenge because of the complex sources and formation mechanisms of aerosol particles. The 2014 Asia-Pacific Economic Cooperation (APEC) summit in Beijing serves as a unique experiment to study the impacts of emission controls on aerosol composition, size distributions, and oxidation properties. Herein, a high-resolution time-of-flight aerosol mass spectrometer was deployed in urban Beijing for real-time measurements of size-resolved non-refractory submicron aerosol (NR-PM1) species from 14 October to 12 November 2014, along with a range of collocated measurements. The average (±σ) PM1 was 41.6 (±38.9) μg m-3 during APEC, which was decreased by 53 % compared with that before APEC. The aerosol composition showed substantial changes owing to emission controls during APEC. Secondary inorganic aerosol (SIA: sulfate + nitrate + ammonium) showed significant reductions of 62-69 %, whereas organics presented much smaller decreases (35 %). The results from the positive matrix factorization of organic aerosol (OA) indicated that highly oxidized secondary organic aerosol (SOA) showed decreases similar to those of SIA during APEC. However, primary organic aerosol (POA) from cooking, traffic, and biomass-burning sources were comparable to those before APEC, indicating the presence of strong local source emissions. The oxidation properties showed corresponding changes in response to OA composition. The average oxygen-to-carbon level during APEC was 0.36 (±0.10), which is lower than the 0.43 (±0.13) measured before APEC, demonstrating a decrease in the OA oxidation degree. The changes in size distributions of primary and secondary species varied during APEC. SIA and SOA showed significant reductions in large accumulation modes with peak diameters shifting from ~ 650 to 400 nm during APEC, whereas those of POA remained relatively unchanged. The changes in aerosol composition, size distributions, and oxidation

A Miniaturized Nickel Oxide Thermistor via Aerosol Jet Technology.

Science.gov (United States)

Wang, Chia; Hong, Guan-Yi; Li, Kuan-Ming; Young, Hong-Tsu

2017-11-12

In this study, a miniaturized thermistor sensor was produced using the Aerosol Jet printing process for temperature sensing applications. A nickel oxide nanoparticle ink with a large temperature coefficient of resistance was fabricated. The thermistor was printed with a circular NiO thin film in between the two parallel silver conductive tracks on a cutting tool insert. The printed thermistor, which has an adjustable dimension with a submillimeter scale, operates over a range of 30-250 °C sensitively (B value of ~4310 K) without hysteretic effects. Moreover, the thermistor may be printed on a 3D surface through the Aerosol Jet printing process, which has increased capability for wide temperature-sensing applications.

Sodium oxide aerosol behavior in a closed vessel. Comparison of computer modeling with aerosol experiments

International Nuclear Information System (INIS)

Fermandjian, Jean.

1979-08-01

Fast breeder reactor safety needs models validated to predict the behavior of sodium aerosols in the different reactor compartments during hypothetical sodium accident. Besides their chemical toxicity, the sodium aerosols are a transfer vector of radioactivity during a contaminated sodium fire. The purpose of this work is to validate models (HAARM 2 and PARDISEKO 3) with tests of sodium pool fires in a 400 m 3 concrete vessel in a confined atmosphere (CASSANDRE tests). The comparison between calculations and experimental results reveals that difficulties still exist, especially as to the selection of the values to be given to some input parameters (physical data of experimental origin, in particular the aerosols source function, the characteristics of the distribution of the emitted particles and the form factor of the agglomerated particles) [fr

Organic nitrate and secondary organic aerosol yield from NO3 oxidation of β-pinene evaluated using a gas-phase kinetics/aerosol partitioning model

Directory of Open Access Journals (Sweden)

H.-P. Dorn

2009-02-01

Full Text Available The yields of organic nitrates and of secondary organic aerosol (SOA particle formation were measured for the reaction NO3+β-pinene under dry and humid conditions in the atmosphere simulation chamber SAPHIR at Research Center Jülich. These experiments were conducted at low concentrations of NO3 (NO3+N2O5pvap~5×10−6 Torr (6.67×10−4 Pa, which constrains speculation about the oxidation mechanism and chemical identity of the organic nitrate. Once formed the SOA in this system continues to evolve, resulting in measurable aerosol volume decrease with time. The observations of high aerosol yield from NOx-dependent oxidation of monoterpenes provide an example of a significant anthropogenic source of SOA from biogenic hydrocarbon precursors. Estimates of the NO3+β-pinene SOA source strength for California and the globe indicate that NO3 reactions with monoterpenes are likely an important source (0.5–8% of the global total of organic aerosol on regional and global scales.

Aerosol generation by oxidation and combustion of plutonium and its compounds: literature survey

International Nuclear Information System (INIS)

Ballereau, P.

1987-09-01

Generation of aerosols by oxidation or combustion is one of the greatest risks due to plutonium. A review is made of the most interesting documents available on this topic. Following a brief study of plutonium oxydation conditions, characteristics of aerosols generated by accidents of fires involving metallic Pu and some of its compounds are assessed. Nuclear weapons are not included in this review [fr

The design of an aerosol test tunnel for occupational hygiene investigations

Science.gov (United States)

Blackford, D. B.; Heighington, K.

An aerosol test tunnel which provides large working sections is described and its performance evaluated. Air movement within the tunnel is achieved with a powerful D.C. motor and centrifugal fan. Test dusts are dispersed and injected into the tunnel by means of an aerosol generator. A unique divertor valve allows aerosol laden air to be either cleaned by a commercial pulse jet filtration unit or recycled around the tunnel to obtain a high aerosol concentration. The tunnel instrumentation is managed by a microcomputer which automatically controls the airspeed and aerosol concentration.

Simulated Field Trials Using an Indoor Aerosol Test Chamber

National Research Council Canada - National Science Library

Semler, D. D; Roth, A. P; Semler, K. A; Nolan, P. M

2004-01-01

.... In this method, the aerosol chamber control software manipulates circulation fan speeds, chamber vacuum and agent spray times to produce a simulated dynamic cloud within the aerosol test chamber...

Simulated Field Trials Using An Indoor Aerosol Test Chamber

National Research Council Canada - National Science Library

Semler, D. D; Roth, A. P; Semler, K. A; Nolan, P. M

2004-01-01

.... In this method, the aerosol chamber control software manipulates circulation fan speeds, chamber vacuum and agent spray times to produce a simulated dynamic cloud within the aerosol test chamber...

Research on aerosol formation, aerosol behaviour, aerosol filtration, aerosol measurement techniques and sodium fires at the Laboratory for Aerosol Physics and Filter Technology at the Nuclear Research Center Karlsruhe

Energy Technology Data Exchange (ETDEWEB)

Jordan, S; Schikarski, W; Schoeck, W [Gesellschaft fuer Kernforschung mbH, Karlsruhe (Germany)

1977-01-01

The behaviour of aerosols in LMFBR plant systems is of great importance for a number of problems, both normal operational and accident kind. This paper covers the following: aerosol modelling for LMFBR containment systems; aerosol size spectrometry by laser light scattering; experimental facilities and experimental results concerned with aerosol release under accident conditions; filtration of sodium oxide aerosols by multilayer sand bed filters.

Research on aerosol formation, aerosol behaviour, aerosol filtration, aerosol measurement techniques and sodium fires at the Laboratory for Aerosol Physics and Filter Technology at the Nuclear Research Center Karlsruhe

International Nuclear Information System (INIS)

Jordan, S.; Schikarski, W.; Schoeck, W.

1977-01-01

The behaviour of aerosols in LMFBR plant systems is of great importance for a number of problems, both normal operational and accident kind. This paper covers the following: aerosol modelling for LMFBR containment systems; aerosol size spectrometry by laser light scattering; experimental facilities and experimental results concerned with aerosol release under accident conditions; filtration of sodium oxide aerosols by multilayer sand bed filters

Determination of permeability of ultra-fine cupric oxide aerosol through military filters and protective filters

Science.gov (United States)

Kellnerová, E.; Večeřa, Z.; Kellner, J.; Zeman, T.; Navrátil, J.

2018-03-01

The paper evaluates the filtration and sorption efficiency of selected types of military combined filters and protective filters. The testing was carried out with the use of ultra-fine aerosol containing cupric oxide nanoparticles ranging in size from 7.6 nm to 299.6 nm. The measurements of nanoparticles were carried out using a scanning mobility particle sizer before and after the passage through the filter and a developed sampling device at the level of particle number concentration approximately 750000 particles·cm-3. The basic parameters of permeability of ultra-fine aerosol passing through the tested material were evaluated, in particular particle size, efficiency of nanoparticle capture by filter, permeability coefficient and overall filtration efficiency. Results indicate that the military filter and particle filters exhibited the highest aerosol permeability especially in the nanoparticle size range between 100–200 nm, while the MOF filters had the highest permeability in the range of 200 to 300 nm. The Filter Nuclear and the Health and Safety filter had 100% nanoparticle capture efficiency and were therefore the most effective. The obtained measurement results have shown that the filtration efficiency over the entire measured range of nanoparticles was sufficient; however, it was different for particular particle sizes.

Nuclear aerosol behaviour in LMFBR. Comparison of computer modelling with aerosol experiments

Energy Technology Data Exchange (ETDEWEB)

Fermandjian, J [DSN/Centre de Fontenay-aux-Roses, Fontenay-aux-Roses (France)

1979-03-01

For the purpose of studying the behaviour of the concentration of aerosols confined in a vessel, various models have been developed, especially in the United States: HAA 3B, HAARM 2 and HAARM 3 - in the Federal Republic of Germany: PARDISEKO 3 and PARDISEKO 3 B - in Japan: ABC 2 and ABC 3 - in the United Kingdom: AEROSIM and in the Netherlands: ETHERDEMO and MADCA. These codes were validated on the basis of tests conducted in vessels whose volumes varied between 0.022 and 850 m{sup 3}. The aerosols studied differed in nature (sodium oxide, fuel oxide, sodium oxide-fuel oxide, gold) and method of production (sodium pool fires, sodium spray fires, arc vaporization, exploding wire) in various atmospheres air, air with variable amounts of oxygen, and nitrogen. This comparison between calculation and experimental results reveals that difficulties still exist, especially as to the selection of the values to be given to some input parameters of the codes (physical data of experimental origin, in particular, the aerosol source function and the characteristics of the size distribution of the emitted particles). Furthermore, the importance of thermophoresis and convection currents has been proved: including the soaring effect in the ABC 3 code enables to fit the experiment. (author)

Nuclear aerosol behaviour in LMFBR. Comparison of computer modelling with aerosol experiments

International Nuclear Information System (INIS)

Fermandjian, J.

1979-01-01

For the purpose of studying the behaviour of the concentration of aerosols confined in a vessel, various models have been developed, especially in the United States: HAA 3B, HAARM 2 and HAARM 3 - in the Federal Republic of Germany: PARDISEKO 3 and PARDISEKO 3 B - in Japan: ABC 2 and ABC 3 - in the United Kingdom: AEROSIM and in the Netherlands: ETHERDEMO and MADCA. These codes were validated on the basis of tests conducted in vessels whose volumes varied between 0.022 and 850 m 3 . The aerosols studied differed in nature (sodium oxide, fuel oxide, sodium oxide-fuel oxide, gold) and method of production (sodium pool fires, sodium spray fires, arc vaporization, exploding wire) in various atmospheres air, air with variable amounts of oxygen, and nitrogen. This comparison between calculation and experimental results reveals that difficulties still exist, especially as to the selection of the values to be given to some input parameters of the codes (physical data of experimental origin, in particular, the aerosol source function and the characteristics of the size distribution of the emitted particles). Furthermore, the importance of thermophoresis and convection currents has been proved: including the soaring effect in the ABC 3 code enables to fit the experiment. (author)

Aerosol composition, oxidative properties, and sources in Beijing: results from the 2014 Asia-Pacific Economic Cooperation Summit study

Science.gov (United States)

Xu, W. Q.; Sun, Y. L.; Chen, C.; Du, W.; Han, T. T.; Wang, Q. Q.; Fu, P. Q.; Wang, Z. F.; Zhao, X. J.; Zhou, L. B.; Ji, D. S.; Wang, P. C.; Worsnop, D. R.

2015-08-01

The mitigation of air pollution in megacities remains a great challenge because of the complex sources and formation mechanisms of aerosol particles. The 2014 Asia- Pacific Economic Cooperation (APEC) summit in Beijing serves as a unique experiment to study the impacts of emission controls on aerosol composition, size distributions, and oxidative properties. Herein, a high-resolution time-of-flight aerosol mass spectrometer was deployed in urban Beijing for real-time measurements of size-resolved non-refractory submicron aerosol (NR-PM1) species from 14 October to 12 November 2014, along with a range of collocated measurements. The average (±σ) PM1 was 41.6 (±38.9) μg m-3 during APEC, which was decreased by 53 % compared with that before APEC. The aerosol composition showed substantial changes owing to emission controls during APEC. Secondary inorganic aerosols (SIA = sulfate + nitrate + ammonium) showed significant reductions of 62-69 %, whereas organics presented much smaller decreases (35 %). The results from the positive matrix factorization of organic aerosols (OA) indicated that highly oxidized secondary OA (SOA) showed decreases similar to those of SIA during APEC. However, primary OA (POA) from cooking, traffic, and biomass burning sources were comparable to those before APEC, indicating the presence of strong local source emissions. The oxidation properties showed corresponding changes in response to OA composition. The average oxygen-to-carbon level during APEC was 0.36 (±0.10), which is lower than the 0.43 (±0.13) measured before APEC, demonstrating a decrease in the OA oxidation degree. The changes in size distributions of primary and secondary species varied during APEC. SIA and SOA showed significant reductions in large accumulation modes with peak diameters shifting from ~ 650 to 400 nm during APEC, whereas those of POA remained relatively unchanged. The changes in aerosol composition, size distributions, and oxidation degrees during the aging

Late-occurring pulmonary pathologies following inhalation of mixed oxide (uranium + plutonium oxide) aerosol in the rat.

Science.gov (United States)

Griffiths, N M; Van der Meeren, A; Fritsch, P; Abram, M-C; Bernaudin, J-F; Poncy, J L

2010-09-01

Accidental exposure by inhalation to alpha-emitting particles from mixed oxide (MOX: uranium and plutonium oxide) fuels is a potential long-term health risk to workers in nuclear fuel fabrication plants. For MOX fuels, the risk of lung cancer development may be different from that assigned to individual components (plutonium, uranium) given different physico-chemical characteristics. The objective of this study was to investigate late effects in rat lungs following inhalation of MOX aerosols of similar particle size containing 2.5 or 7.1% plutonium. Conscious rats were exposed to MOX aerosols and kept for their entire lifespan. Different initial lung burdens (ILBs) were obtained using different amounts of MOX. Lung total alpha activity was determined by external counting and at autopsy for total lung dose calculation. Fixed lung tissue was used for anatomopathological, autoradiographical, and immunohistochemical analyses. Inhalation of MOX at ILBs ranging from 1-20 kBq resulted in lung pathologies (90% of rats) including fibrosis (70%) and malignant lung tumors (45%). High ILBs (4-20 kBq) resulted in reduced survival time (N = 102; p inhalation result in similar risk for development of lung tumors as compared with industrial plutonium oxide.

Large-Scale Spray Releases: Additional Aerosol Test Results

Energy Technology Data Exchange (ETDEWEB)

Daniel, Richard C.; Gauglitz, Phillip A.; Burns, Carolyn A.; Fountain, Matthew S.; Shimskey, Rick W.; Billing, Justin M.; Bontha, Jagannadha R.; Kurath, Dean E.; Jenks, Jeromy WJ; MacFarlan, Paul J.; Mahoney, Lenna A.

2013-08-01

One of the events postulated in the hazard analysis for the Waste Treatment and Immobilization Plant (WTP) and other U.S. Department of Energy (DOE) nuclear facilities is a breach in process piping that produces aerosols with droplet sizes in the respirable range. The current approach for predicting the size and concentration of aerosols produced in a spray leak event involves extrapolating from correlations reported in the literature. These correlations are based on results obtained from small engineered spray nozzles using pure liquids that behave as a Newtonian fluid. The narrow ranges of physical properties on which the correlations are based do not cover the wide range of slurries and viscous materials that will be processed in the WTP and in processing facilities across the DOE complex. To expand the data set upon which the WTP accident and safety analyses were based, an aerosol spray leak testing program was conducted by Pacific Northwest National Laboratory (PNNL). PNNL’s test program addressed two key technical areas to improve the WTP methodology (Larson and Allen 2010). The first technical area was to quantify the role of slurry particles in small breaches where slurry particles may plug the hole and prevent high-pressure sprays. The results from an effort to address this first technical area can be found in Mahoney et al. (2012a). The second technical area was to determine aerosol droplet size distribution and total droplet volume from prototypic breaches and fluids, including sprays from larger breaches and sprays of slurries for which literature data are mostly absent. To address the second technical area, the testing program collected aerosol generation data at two scales, commonly referred to as small-scale and large-scale testing. The small-scale testing and resultant data are described in Mahoney et al. (2012b), and the large-scale testing and resultant data are presented in Schonewill et al. (2012). In tests at both scales, simulants were used

Heterogeneous oxidation of saturated organic aerosols by hydroxyl radicals: uptake kinetics, condensed-phase products, and particle size change

Directory of Open Access Journals (Sweden)

I. J. George

2007-08-01

Full Text Available The kinetics and reaction mechanism for the heterogeneous oxidation of saturated organic aerosols by gas-phase OH radicals were investigated under NO_x-free conditions. The reaction of 150 nm diameter Bis(2-ethylhexyl sebacate (BES particles with OH was studied as a proxy for chemical aging of atmospheric aerosols containing saturated organic matter. An aerosol reactor flow tube combined with an Aerodyne time-of-flight aerosol mass spectrometer (ToF-AMS and scanning mobility particle sizer (SMPS was used to study this system. Hydroxyl radicals were produced by 254 nm photolysis of O₃ in the presence of water vapour. The kinetics of the heterogeneous oxidation of the BES particles was studied by monitoring the loss of a mass fragment of BES with the ToF-AMS as a function of OH exposure. We measured an initial OH uptake coefficient of γ₀=1.3 (±0.4, confirming that this reaction is highly efficient. The density of BES particles increased by up to 20% of the original BES particle density at the highest OH exposure studied, consistent with the particle becoming more oxidized. Electrospray ionization mass spectrometry analysis showed that the major particle-phase reaction products are multifunctional carbonyls and alcohols with higher molecular weights than the starting material. Volatilization of oxidation products accounted for a maximum of 17% decrease of the particle volume at the highest OH exposure studied. Tropospheric organic aerosols will become more oxidized from heterogeneous photochemical oxidation, which may affect not only their physical and chemical properties, but also their hygroscopicity and cloud nucleation activity.

In Vitro Tests for Aerosol Deposition. V: Using Realistic Testing to Estimate Variations in Aerosol Properties at the Trachea.

Science.gov (United States)

Wei, Xiangyin; Hindle, Michael; Delvadia, Renishkumar R; Byron, Peter R

2017-10-01

The dose and aerodynamic particle size distribution (APSD) of drug aerosols' exiting models of the mouth and throat (MT) during a realistic inhalation profile (IP) may be estimated in vitro and designated Total Lung Dose, TLD in vitro , and APSD TLDin vitro , respectively. These aerosol characteristics likely define the drug's regional distribution in the lung. A general method was evaluated to enable the simultaneous determination of TLD in vitro and APSD TLDin vitro for budesonide aerosols' exiting small, medium and large VCU-MT models. Following calibration of the modified next generation pharmaceutical impactor (NGI) at 140 L/min, variations in aerosol dose and size exiting MT were determined from Budelin ® Novolizer ® across the IPs reported by Newman et al., who assessed drug deposition from this inhaler by scintigraphy. Values for TLD in vitro from the test inhaler determined by the general method were found to be statistically comparable to those using a filter capture method. Using new stage cutoffs determined by calibration of the modified NGI at 140 L/min, APSD TLDin vitro profiles and mass median aerodynamic diameters at the MT exit (MMAD TLDin vitro ) were determined as functions of MT geometric size across Newman's IPs. The range of mean values (n ≥ 5) for TLD in vitro and MMAD TLDin vitro for this inhaler extended from 6.2 to 103.0 μg (3.1%-51.5% of label claim) and from 1.7 to 3.6 μm, respectively. The method enables reliable determination of TLD in vitro and APSD TLDin vitro for aerosols likely to enter the trachea of test subjects in the clinic. By simulating realistic IPs and testing in different MT models, the effects of major variables on TLD in vitro and APSD TLDin vitro may be studied using the general method described in this study.

The oxidation of SO2 by NO2(g) at the air-water interface of aquated aerosol: implications for the rapid onset of haze-aerosol events in China

Science.gov (United States)

Li, L.; Colussi, A. J.; Hoffmann, M. R.

2017-12-01

Aqueous phase chemistry plays a vital role in the global atmosphere. The importance of heterogeneous chemistry has been recently underscored by the severe haze-fog pollution episodes experienced in Chinese megacities. A key finding is that despite reduced photochemistry during the wintertime haze events, the oxidation of S(IV) into sulfate aerosol occurs rapidly in spite of the low levels of ozone and H2O2. Field observations suggest that NO2 could serve as a suitable oxidant of S(IV) during the events under neutral pH conditions. However, the haze aerosols are mostly acidic. Furthermore, the air-water interface is more acidic than bulk-phase aquated system according to our recent findings. This work investigates the chemistry taking place as NO2(g) collides with the surface of aqueous S(IV) microdroplets as a function of pH to closely simulate actual haze aerosol events under atmospheric conditions. The reaction between NO2(g) and HSO3- (aq) is studied in situ under ambient temperature and pressure via online electrospray ionization mass spectrometry. The aqueous aerosols containing HSO3- is generated using a microjet which is exposed to NO2(g) alternatively, while the composition of the 1 nm interfacial liquid layer of the aerosol is instantaneously measured. The ratio of HSO3- to HSO4- is observed to decrease with the concomitant appearance of a strong m/z 62 signal upon NO2(g) exposure. The appearance of m/z 62 indicates the formation of NO3- via the disproportionation of NO2 (2NO2(g) + H2O (l) ⇌ H++NO3-(aq) + HONO(aq)) and thus impacts the ion-ion interactions of NO3- on the ratio of HSO3- to HSO4- in the outermost interfacial layers. Parallel experiments with NO3-(aq) additions are conducted to quantify the impact of NO3- on the the ratio, in order to unravel the contribution of NO2 to the oxidation of S(IV). After accounting for the HNO3 effect, it is concluded: (1) most NO2(g) is converted into NO3- via anion-catalyzed hydrolytic disproportionation; (2

Small-Scale Spray Releases: Additional Aerosol Test Results

Energy Technology Data Exchange (ETDEWEB)

Schonewill, Philip P.; Gauglitz, Phillip A.; Kimura, Marcia L.; Brown, G. N.; Mahoney, Lenna A.; Tran, Diana N.; Burns, Carolyn A.; Kurath, Dean E.

2013-08-01

One of the events postulated in the hazard analysis at the Waste Treatment and Immobilization Plant (WTP) and other U.S. Department of Energy (DOE) nuclear facilities is a breach in process piping that produces aerosols with droplet sizes in the respirable range. The current approach for predicting the size and concentration of aerosols produced in a spray leak involves extrapolating from correlations reported in the literature. These correlations are based on results obtained from small engineered spray nozzles using pure liquids with Newtonian fluid behavior. The narrow ranges of physical properties on which the correlations are based do not cover the wide range of slurries and viscous materials that will be processed in the WTP and across processing facilities in the DOE complex. To expand the data set upon which the WTP accident and safety analyses were based, an aerosol spray leak testing program was conducted by Pacific Northwest National Laboratory (PNNL). PNNL’s test program addressed two key technical areas to improve the WTP methodology (Larson and Allen 2010). The first technical area was to quantify the role of slurry particles in small breaches where slurry particles may plug the hole and prevent high-pressure sprays. The results from an effort to address this first technical area can be found in Mahoney et al. (2012a). The second technical area was to determine aerosol droplet size distribution and total droplet volume from prototypic breaches and fluids, including sprays from larger breaches and sprays of slurries for which literature data are largely absent. To address the second technical area, the testing program collected aerosol generation data at two scales, commonly referred to as small-scale and large-scale. The small-scale testing and resultant data are described in Mahoney et al. (2012b) and the large-scale testing and resultant data are presented in Schonewill et al. (2012). In tests at both scales, simulants were used to mimic the

Results and code prediction comparisons of lithium-air reaction and aerosol behavior tests

International Nuclear Information System (INIS)

Jeppson, D.W.

1986-03-01

The Hanford Engineering Development Laboratory (HEDL) Fusion Safety Support Studies include evaluation of potential safety and environmental concerns associated with the use of liquid lithium as a breeder and coolant for fusion reactors. Potential mechanisms for volatilization and transport of radioactive metallic species associated with breeder materials are of particular interest. Liquid lithium pool-air reaction and aerosol behavior tests were conducted with lithium masses up to 100 kg within the 850-m 3 containment vessel in the Containment Systems Test Facility. Lithium-air reaction rates, aerosol generation rates, aerosol behavior and characterization, as well as containment atmosphere temperature and pressure responses were determined. Pool-air reaction and aerosol behavior test results were compared with computer code calculations for reaction rates, containment atmosphere response, and aerosol behavior. The volatility of potentially radioactive metallic species from a lithium pool-air reaction was measured. The response of various aerosol detectors to the aerosol generated was determined. Liquid lithium spray tests in air and in nitrogen atmospheres were conducted with lithium temperatures of about 427 0 and 650 0 C. Lithium reaction rates, containment atmosphere response, and aerosol generation and characterization were determined for these spray tests

Environmental Health Hazards of e-Cigarettes and their Components: Oxidants and Copper in e-cigarette aerosols

Science.gov (United States)

Lerner, Chad A.; Sundar, Isaac K.; Watson, Richard M.; Elder, Alison; Jones, Ryan; Done, Douglas; Kurtzman, Rachel; Ossip, Deborah J.; Robinson, Risa; McIntosh, Scott; Rahman, Irfan

2014-01-01

To narrow the gap in our understanding of potential oxidative properties associated with Electronic Nicotine Delivery systems (ENDS) i.e. e-cigarettes, we employed semi-quantitative methods to detect oxidant reactivity in disposable components of ENDS/e-cigarettes (batteries and cartomizers) using a fluorescein indicator. These components exhibit oxidants/reactive oxygen species reactivity similar to used conventional cigarette filters. Oxidants/reactive oxygen species reactivity in e-cigarette aerosols was also similar to oxidant reactivity in cigarette smoke. A cascade particle impactor allowed sieving of a range of particle size distributions between 0.450 and 2.02 μm in aerosols from an e-cigarette. Copper, being among these particles, is 6.1 times higher per puff than reported previously for conventional cigarette smoke. The detection of a potentially cytotoxic metal as well as oxidants from e-cigarette and its components raises concern regarding the safety of e-cigarettes use and the disposal of e-cigarette waste products into the environment. PMID:25577651

Compositional evolution of particle-phase reaction products and water in the heterogeneous OH oxidation of model aqueous organic aerosols

Directory of Open Access Journals (Sweden)

M. M. Chim

2017-12-01

Full Text Available Organic compounds present at or near the surface of aqueous droplets can be efficiently oxidized by gas-phase OH radicals, which alter the molecular distribution of the reaction products within the droplet. A change in aerosol composition affects the hygroscopicity and leads to a concomitant response in the equilibrium amount of particle-phase water. The variation in the aerosol water content affects the aerosol size and physicochemical properties, which in turn governs the oxidation kinetics and chemistry. To attain better knowledge of the compositional evolution of aqueous organic droplets during oxidation, this work investigates the heterogeneous OH-radical-initiated oxidation of aqueous methylsuccinic acid (C5H8O4 droplets, a model compound for small branched dicarboxylic acids found in atmospheric aerosols, at a high relative humidity of 85 % through experimental and modeling approaches. Aerosol mass spectra measured by a soft atmospheric pressure ionization source (Direct Analysis in Real Time, DART coupled with a high-resolution mass spectrometer reveal two major products: a five carbon atom (C5 hydroxyl functionalization product (C5H8O5 and a C4 fragmentation product (C4H6O3. These two products likely originate from the formation and subsequent reactions (intermolecular hydrogen abstraction and carbon–carbon bond scission of tertiary alkoxy radicals resulting from the OH abstraction occurring at the methyl-substituted carbon site. Based on the identification of the reaction products, a kinetic model of oxidation (a two-product model coupled with the Aerosol Inorganic–Organic Mixtures Functional groups Activity Coefficients (AIOMFAC model is built to simulate the size and compositional changes of aqueous methylsuccinic acid droplets during oxidation. Model results show that at the maximum OH exposure, the droplets become slightly more hygroscopic after oxidation, as the mass fraction of water is predicted to increase from

Development of Aerosol Scrubbing Test Loop for Containment Filtered Venting System

International Nuclear Information System (INIS)

Lee, Doo Yong; Jung, Woo Young; Lee, Hyun Chul; Lee, Jong Chan; Kim, Gyu Tae

2016-01-01

The scrubber tank is filled with scrubbing water with the chemical additives. The droplet separator based on a cyclone is installed above the scrubbing water pool to remove the large droplets that may clog a metal fiber filter installed at the upper section of the scrubber tank. The outlet piping is connected from the scrubber tank to the molecular sieve to chemically remove the gaseous iodine. The aerosol as a particle is physically captured in the scrubbing water pool passing through the scrubbing nozzle as well as the metal fiber filter. The gaseous iodine such as molecular iodine as well as organic iodide is chemically removed in the scrubbing water pool and molecular sieve. The thermal-hydraulic as well as scrubbing performance for the CFVS should be verified with the experiments. The experiment can be divided into the filtration component based experiment and whole system based one. In this paper, the aerosol scrubbing test loop developed to test the thermal-hydraulic and aerosol scrubbing performance of the scrubbing nozzle with the scrubbing water pool is introduced. The aerosol scrubbing test loop has been developed as a part of the Korean CFVS project. In this loop, the filtration components such as the scrubbing nozzle submerged in the scrubbing water pool as well as the cyclone as droplet separator can be tested under the CFVS operating conditions. The aerosol scrubbing performance of the filtration components including pool scrubbing behavior can be tested with the aerosol generation and feeding system and aerosol measurement system.

Development of Aerosol Scrubbing Test Loop for Containment Filtered Venting System

Energy Technology Data Exchange (ETDEWEB)

Lee, Doo Yong; Jung, Woo Young; Lee, Hyun Chul; Lee, Jong Chan; Kim, Gyu Tae [FNC Technology, Yongin (Korea, Republic of)

2016-05-15

The scrubber tank is filled with scrubbing water with the chemical additives. The droplet separator based on a cyclone is installed above the scrubbing water pool to remove the large droplets that may clog a metal fiber filter installed at the upper section of the scrubber tank. The outlet piping is connected from the scrubber tank to the molecular sieve to chemically remove the gaseous iodine. The aerosol as a particle is physically captured in the scrubbing water pool passing through the scrubbing nozzle as well as the metal fiber filter. The gaseous iodine such as molecular iodine as well as organic iodide is chemically removed in the scrubbing water pool and molecular sieve. The thermal-hydraulic as well as scrubbing performance for the CFVS should be verified with the experiments. The experiment can be divided into the filtration component based experiment and whole system based one. In this paper, the aerosol scrubbing test loop developed to test the thermal-hydraulic and aerosol scrubbing performance of the scrubbing nozzle with the scrubbing water pool is introduced. The aerosol scrubbing test loop has been developed as a part of the Korean CFVS project. In this loop, the filtration components such as the scrubbing nozzle submerged in the scrubbing water pool as well as the cyclone as droplet separator can be tested under the CFVS operating conditions. The aerosol scrubbing performance of the filtration components including pool scrubbing behavior can be tested with the aerosol generation and feeding system and aerosol measurement system.

LABORATORY EVALUATION OF A MICROFLUIDIC ELECTROCHEMICAL SENSOR FOR AEROSOL OXIDATIVE LOAD.

Science.gov (United States)

Koehler, Kirsten; Shapiro, Jeffrey; Sameenoi, Yupaporn; Henry, Charles; Volckens, John

2014-05-01

Human exposure to particulate matter (PM) air pollution is associated with human morbidity and mortality. The mechanisms by which PM impacts human health are unresolved, but evidence suggests that PM intake leads to cellular oxidative stress through the generation of reactive oxygen species (ROS). Therefore, reliable tools are needed for estimating the oxidant generating capacity, or oxidative load, of PM at high temporal resolution (minutes to hours). One of the most widely reported methods for assessing PM oxidative load is the dithiothreitol (DTT) assay. The traditional DTT assay utilizes filter-based PM collection in conjunction with chemical analysis to determine the oxidation rate of reduced DTT in solution with PM. However, the traditional DTT assay suffers from poor time resolution, loss of reactive species during sampling, and high limit of detection. Recently, a new DTT assay was developed that couples a Particle-Into-Liquid-Sampler with microfluidic-electrochemical detection. This 'on-line' system allows high temporal resolution monitoring of PM reactivity with improved detection limits. This study reports on a laboratory comparison of the traditional and on-line DTT approaches. An urban dust sample was aerosolized in a laboratory test chamber at three atmospherically-relevant concentrations. The on-line system gave a stronger correlation between DTT consumption rate and PM mass (R 2 = 0.69) than the traditional method (R 2 = 0.40) and increased precision at high temporal resolution, compared to the traditional method.

Aged organic aerosol in the Eastern Mediterranean: the Finokalia Aerosol Measurement Experiment – 2008

Directory of Open Access Journals (Sweden)

L. Hildebrandt

2010-05-01

Full Text Available Aged organic aerosol (OA was measured at a remote coastal site on the island of Crete, Greece during the Finokalia Aerosol Measurement Experiment-2008 (FAME-2008, which was part of the EUCAARI intensive campaign of May 2008. The site at Finokalia is influenced by air masses from different source regions, including long-range transport of pollution from continental Europe. A quadrupole aerosol mass spectrometer (Q-AMS was employed to measure the size-resolved chemical composition of non-refractory submicron aerosol (NR-PM₁, and to estimate the extent of oxidation of the organic aerosol. Factor analysis was used to gain insights into the processes and sources affecting the OA composition. The particles were internally mixed and liquid. The largest fraction of the dry NR-PM₁ sampled was ammonium sulfate and ammonium bisulfate, followed by organics and a small amount of nitrate. The variability in OA composition could be explained with two factors of oxygenated organic aerosol (OOA with differing extents of oxidation but similar volatility. Hydrocarbon-like organic aerosol (HOA was not detected. There was no statistically significant diurnal variation in the bulk composition of NR-PM₁ such as total sulfate or total organic aerosol concentrations. However, the OA composition exhibited statistically significant diurnal variation with more oxidized OA in the afternoon. The organic aerosol was highly oxidized, regardless of the source region. Total OA concentrations also varied little with source region, suggesting that local sources had only a small effect on OA concentrations measured at Finokalia. The aerosol was transported for about one day before arriving at the site, corresponding to an OH exposure of approximately 4×10¹¹ molecules cm⁻³ s. The constant extent of oxidation suggests that atmospheric aging results in a highly oxidized OA at these OH exposures, regardless of the aerosol source.

Mass yields of secondary organic aerosols from the oxidation of α-pinene and real plant emissions

Directory of Open Access Journals (Sweden)

J. N. Smith

2011-02-01

Full Text Available Biogenic volatile organic compounds (VOCs are a significant source of global secondary organic aerosol (SOA; however, quantifying their aerosol forming potential remains a challenge. This study presents smog chamber laboratory work, focusing on SOA formation via oxidation of the emissions of two dominant tree species from boreal forest area, Scots pine (Pinus sylvestris L. and Norway spruce (Picea abies, by hydroxyl radical (OH and ozone (O3. Oxidation of α-pinene was also studied as a reference system. Tetramethylethylene (TME and 2-butanol were added to control OH and O3 levels, thereby allowing SOA formation events to be categorized as resulting from either OH-dominated or O3-initiated chemistry. SOA mass yields from α-pinene are consistent with previous studies while the yields from the real plant emissions are generally lower than that from α-pinene, varying from 1.9% at an aerosol mass loading of 0.69 μg m−3 to 17.7% at 26.0 μg m−3. Mass yields from oxidation of real plant emissions are subject to the interactive effects of the molecular structures of plant emissions and their reaction chemistry with OH and O3, which lead to variations in condensable product volatility. SOA formation can be reproduced with a two-product gas-phase partitioning absorption model in spite of differences in the source of oxidant species and product volatility in the real plant emission experiments. Condensable products from OH-dominated chemistry showed a higher volatility than those from O3-initiated systems during aerosol growth stage. Particulate phase products became less volatile via aging process which continued after input gas-phase oxidants had been completely consumed.

Large-Scale Spray Releases: Initial Aerosol Test Results

Energy Technology Data Exchange (ETDEWEB)

Schonewill, Philip P.; Gauglitz, Phillip A.; Bontha, Jagannadha R.; Daniel, Richard C.; Kurath, Dean E.; Adkins, Harold E.; Billing, Justin M.; Burns, Carolyn A.; Davis, James M.; Enderlin, Carl W.; Fischer, Christopher M.; Jenks, Jeromy WJ; Lukins, Craig D.; MacFarlan, Paul J.; Shutthanandan, Janani I.; Smith, Dennese M.

2012-12-01

One of the events postulated in the hazard analysis at the Waste Treatment and Immobilization Plant (WTP) and other U.S. Department of Energy (DOE) nuclear facilities is a breach in process piping that produces aerosols with droplet sizes in the respirable range. The current approach for predicting the size and concentration of aerosols produced in a spray leak involves extrapolating from correlations reported in the literature. These correlations are based on results obtained from small engineered spray nozzles using pure liquids with Newtonian fluid behavior. The narrow ranges of physical properties on which the correlations are based do not cover the wide range of slurries and viscous materials that will be processed in the WTP and across processing facilities in the DOE complex. Two key technical areas were identified where testing results were needed to improve the technical basis by reducing the uncertainty due to extrapolating existing literature results. The first technical need was to quantify the role of slurry particles in small breaches where the slurry particles may plug and result in substantially reduced, or even negligible, respirable fraction formed by high-pressure sprays. The second technical need was to determine the aerosol droplet size distribution and volume from prototypic breaches and fluids, specifically including sprays from larger breaches with slurries where data from the literature are scarce. To address these technical areas, small- and large-scale test stands were constructed and operated with simulants to determine aerosol release fractions and generation rates from a range of breach sizes and geometries. The properties of the simulants represented the range of properties expected in the WTP process streams and included water, sodium salt solutions, slurries containing boehmite or gibbsite, and a hazardous chemical simulant. The effect of anti-foam agents was assessed with most of the simulants. Orifices included round holes and

Small-Scale Spray Releases: Initial Aerosol Test Results

Energy Technology Data Exchange (ETDEWEB)

Mahoney, Lenna A.; Gauglitz, Phillip A.; Kimura, Marcia L.; Brown, Garrett N.; Kurath, Dean E.; Buchmiller, William C.; Smith, Dennese M.; Blanchard, Jeremy; Song, Chen; Daniel, Richard C.; Wells, Beric E.; Tran, Diana N.; Burns, Carolyn A.

2013-05-29

One of the events postulated in the hazard analysis at the Waste Treatment and Immobilization Plant (WTP) and other U.S. Department of Energy (DOE) nuclear facilities is a breach in process piping that produces aerosols with droplet sizes in the respirable range. The current approach for predicting the size and concentration of aerosols produced in a spray leak involves extrapolating from correlations reported in the literature. These correlations are based on results obtained from small engineered spray nozzles using pure liquids with Newtonian fluid behavior. The narrow ranges of physical properties on which the correlations are based do not cover the wide range of slurries and viscous materials that will be processed in the WTP and across processing facilities in the DOE complex. Two key technical areas were identified where testing results were needed to improve the technical basis by reducing the uncertainty due to extrapolating existing literature results. The first technical need was to quantify the role of slurry particles in small breaches where the slurry particles may plug and result in substantially reduced, or even negligible, respirable fraction formed by high-pressure sprays. The second technical need was to determine the aerosol droplet size distribution and volume from prototypic breaches and fluids, specifically including sprays from larger breaches with slurries where data from the literature are scarce. To address these technical areas, small- and large-scale test stands were constructed and operated with simulants to determine aerosol release fractions and net generation rates from a range of breach sizes and geometries. The properties of the simulants represented the range of properties expected in the WTP process streams and included water, sodium salt solutions, slurries containing boehmite or gibbsite, and a hazardous chemical simulant. The effect of antifoam agents was assessed with most of the simulants. Orifices included round holes and

Small-Scale Spray Releases: Initial Aerosol Test Results

Energy Technology Data Exchange (ETDEWEB)

Mahoney, Lenna A.; Gauglitz, Phillip A.; Kimura, Marcia L.; Brown, Garrett N.; Kurath, Dean E.; Buchmiller, William C.; Smith, Dennese M.; Blanchard, Jeremy; Song, Chen; Daniel, Richard C.; Wells, Beric E.; Tran, Diana N.; Burns, Carolyn A.

2012-11-01

One of the events postulated in the hazard analysis at the Waste Treatment and Immobilization Plant (WTP) and other U.S. Department of Energy (DOE) nuclear facilities is a breach in process piping that produces aerosols with droplet sizes in the respirable range. The current approach for predicting the size and concentration of aerosols produced in a spray leak involves extrapolating from correlations reported in the literature. These correlations are based on results obtained from small engineered spray nozzles using pure liquids with Newtonian fluid behavior. The narrow ranges of physical properties on which the correlations are based do not cover the wide range of slurries and viscous materials that will be processed in the WTP and across processing facilities in the DOE complex. Two key technical areas were identified where testing results were needed to improve the technical basis by reducing the uncertainty due to extrapolating existing literature results. The first technical need was to quantify the role of slurry particles in small breaches where the slurry particles may plug and result in substantially reduced, or even negligible, respirable fraction formed by high-pressure sprays. The second technical need was to determine the aerosol droplet size distribution and volume from prototypic breaches and fluids, specifically including sprays from larger breaches with slurries where data from the literature are scarce. To address these technical areas, small- and large-scale test stands were constructed and operated with simulants to determine aerosol release fractions and generation rates from a range of breach sizes and geometries. The properties of the simulants represented the range of properties expected in the WTP process streams and included water, sodium salt solutions, slurries containing boehmite or gibbsite, and a hazardous chemical simulant. The effect of anti-foam agents was assessed with most of the simulants. Orifices included round holes and

Environmental health hazards of e-cigarettes and their components: Oxidants and copper in e-cigarette aerosols.

Science.gov (United States)

Lerner, Chad A; Sundar, Isaac K; Watson, Richard M; Elder, Alison; Jones, Ryan; Done, Douglas; Kurtzman, Rachel; Ossip, Deborah J; Robinson, Risa; McIntosh, Scott; Rahman, Irfan

2015-03-01

To narrow the gap in our understanding of potential oxidative properties associated with Electronic Nicotine Delivery Systems (ENDS) i.e. e-cigarettes, we employed semi-quantitative methods to detect oxidant reactivity in disposable components of ENDS/e-cigarettes (batteries and cartomizers) using a fluorescein indicator. These components exhibit oxidants/reactive oxygen species reactivity similar to used conventional cigarette filters. Oxidants/reactive oxygen species reactivity in e-cigarette aerosols was also similar to oxidant reactivity in cigarette smoke. A cascade particle impactor allowed sieving of a range of particle size distributions between 0.450 and 2.02 μm in aerosols from an e-cigarette. Copper, being among these particles, is 6.1 times higher per puff than reported previously for conventional cigarette smoke. The detection of a potentially cytotoxic metal as well as oxidants from e-cigarette and its components raises concern regarding the safety of e-cigarettes use and the disposal of e-cigarette waste products into the environment. Copyright © 2014 Elsevier Ltd. All rights reserved.

Reactive oxidation products promote secondary organic aerosol formation from green leaf volatiles

Directory of Open Access Journals (Sweden)

J. F. Hamilton

2009-06-01

Full Text Available Green leaf volatiles (GLVs are an important group of chemicals released by vegetation which have emission fluxes that can be significantly increased when plants are damaged or stressed. A series of simulation chamber experiments has been conducted at the European Photoreactor in Valencia, Spain, to investigate secondary organic aerosol (SOA formation from the atmospheric oxidation of the major GLVs cis-3-hexenylacetate and cis-3-hexen-1-ol. Liquid chromatography-ion trap mass spectrometry was used to identify chemical species present in the SOA. Cis-3-hexen-1-ol proved to be a more efficient SOA precursor due to the high reactivity of its first generation oxidation product, 3-hydroxypropanal, which can hydrate and undergo further reactions with other aldehydes resulting in SOA dominated by higher molecular weight oligomers. The lower SOA yields produced from cis-3-hexenylacetate are attributed to the acetate functionality, which inhibits oligomer formation in the particle phase. Based on observed SOA yields and best estimates of global emissions, these compounds may be calculated to be a substantial unidentified global source of SOA, contributing 1–5 TgC yr⁻¹, equivalent to around a third of that predicted from isoprene. Molecular characterization of the SOA, combined with organic mechanistic information, has provided evidence that the formation of organic aerosols from GLVs is closely related to the reactivity of their first generation atmospheric oxidation products, and indicates that this may be a simple parameter that could be used in assessing the aerosol formation potential for other unstudied organic compounds in the atmosphere.

Laboratory Measurements of Biomass Cook-stove Emissions Aged in an Oxidation Flow Reactor: Influence of Combustion and Aging Conditions on Aerosols

Science.gov (United States)

Grieshop, A. P.; Reece, S. M.; Sinha, A.; Wathore, R.

2016-12-01

Combustion in rudimentary and improved cook-stoves used by billions in developing countries can be a regionally dominant contributor to black carbon (BC), primary organic aerosols (POA) and precursors for secondary organic aerosol (SOA). Recent studies suggest that SOA formed during photo-oxidation of primary emissions from biomass burning may make important contribution to its atmospheric impacts. However, the extent to which stove type and operating conditions affect the amount, composition and characteristics of SOA formed from the aging of cookstoves emissions is still largely undetermined. Here we present results from experiments with a field portable oxidation flow reactor (F-OFR) designed to assess aging of cook-stove emissions in both laboratory and field settings. Laboratory tests results are used to compare the quantity and properties of fresh and aged emissions from a traditional open fire and twp alternative stove designs operated on the standard and alternate testing protocols. Diluted cookstove emissions were exposed to a range of oxidant concentrations in the F-OFR. Primary emissions were aged both on-line, to study the influence of combustion variability, and sampled from batched emissions in a smog chamber to examine different aging conditions. Data from real-time particle- and gas-phase instruments and integrated filter samples were collected up and down stream of the OFR. The properties of primary emissions vary strongly with stove type and combustion conditions (e.g. smoldering versus flaming). Experiments aging diluted biomass emissions from distinct phases of stove operation (smoldering and flaming) showed peak SOA production for both phases occurred between 3 and 6 equivalent days of aging with slightly greater production observed in flaming phase emissions. Changing combustion conditions had a stronger influence than aging on POA+SOA `emission factors'. Aerosol Chemical Speciation Monitor data show a substantial evolution of aerosol

Glutathione aerosol suppresses lung epithelial surface inflammatory cell-derived oxidants in cystic fibrosis.

Science.gov (United States)

Roum, J H; Borok, Z; McElvaney, N G; Grimes, G J; Bokser, A D; Buhl, R; Crystal, R G

1999-07-01

Cystic fibrosis (CF) is characterized by accumulation of activated neutrophils and macrophages on the respiratory epithelial surface (RES); these cells release toxic oxidants, which contribute to the marked epithelial derangements seen in CF. These deleterious consequences are magnified, since reduced glutathione (GSH), an antioxidant present in high concentrations in normal respiratory epithelial lining fluid (ELF), is deficient in CF ELF. To evaluate the feasibility of increasing ELF GSH levels and enhancing RES antioxidant protection, GSH aerosol was delivered (600 mg twice daily for 3 days) to seven patients with CF. ELF total, reduced, and oxidized GSH increased (P < 0.05, all compared with before GSH therapy), suggesting adequate RES delivery and utilization of GSH. Phorbol 12-myristate 13-acetate-stimulated superoxide anion (O2-.) release by ELF inflammatory cells decreased after GSH therapy (P < 0.002). This paralleled observations that GSH added in vitro to CF ELF inflammatory cells suppressed O2-. release (P < 0.001). No adverse effects were noted during treatment. Together, these observations demonstrate the feasibility of using GSH aerosol to restore RES oxidant-antioxidant balance in CF and support the rationale for further clinical evaluation.

Hygroscopicity of secondary organic aerosols formed by oxidation of cycloalkenes, monoterpenes, sesquiterpenes, and related compounds

Directory of Open Access Journals (Sweden)

V. Varutbangkul

2006-01-01

Full Text Available A series of experiments has been conducted in the Caltech indoor smog chamber facility to investigate the water uptake properties of aerosol formed by oxidation of various organic precursors. Secondary organic aerosol (SOA from simple and substituted cycloalkenes (C5-C8 is produced in dark ozonolysis experiments in a dry chamber (RH~5%. Biogenic SOA from monoterpenes, sesquiterpenes, and oxygenated terpenes is formed by photooxidation in a humid chamber (~50% RH. Using the hygroscopicity tandem differential mobility analyzer (HTDMA, we measure the diameter-based hygroscopic growth factor (GF of the SOA as a function of time and relative humidity. All SOA studied is found to be slightly hygroscopic, with smaller water uptake than that of typical inorganic aerosol substances. The aerosol water uptake increases with time early in the experiments for the cycloalkene SOA, but decreases with time for the sesquiterpene SOA. This behavior could indicate competing effects between the formation of more highly oxidized polar compounds (more hygroscopic, and formation of longer-chained oligomers (less hygroscopic. All SOA also exhibit a smooth water uptake with RH with no deliquescence or efflorescence. The water uptake curves are found to be fitted well with an empirical three-parameter functional form. The measured pure organic GF values at 85% RH are between 1.09–1.16 for SOA from ozonolysis of cycloalkenes, 1.01–1.04 for sesquiterpene photooxidation SOA, and 1.06–1.10 for the monoterpene and oxygenated terpene SOA. The GF of pure SOA (GForg in experiments in which inorganic seed aerosol is used is determined by assuming volume-weighted water uptake (Zdanovskii-Stokes-Robinson or 'ZSR' approach and using the size-resolved organic mass fraction measured by the Aerodyne Aerosol Mass Spectrometer. Knowing the water content associated with the inorganic fraction yields GForg values. However, for each precursor, the GForg values computed from different

X-ray fluorimetry in tests of the aerosol substances

International Nuclear Information System (INIS)

Walentek, A.; Cudny, W.; Marzec, J.; Pawlowski, Z.; Zaremba, K.

1992-01-01

Test results of aerosol samples from atmospheric air collected from membrane drains were presented. The ANFLU-2 analyzer constructed at the Warsaw Technical University were used for testing. (author). 3 figs, 1 tab

Organic aerosol formation during the atmospheric degradation of toluene.

Science.gov (United States)

Hurley, M D; Sokolov, O; Wallington, T J; Takekawa, H; Karasawa, M; Klotz, B; Barnes, I; Becker, K H

2001-04-01

Organic aerosol formation during the atmospheric oxidation of toluene was investigated using smog chamber systems. Toluene oxidation was initiated by the UV irradiation of either toluene/air/NOx or toluene/air/CH3ONO/NO mixtures. Aerosol formation was monitored using scanning mobility particle sizers and toluene loss was monitored by in-situ FTIR spectroscopy or GC-FID techniques. The experimental results show that the reaction of OH radicals, NO3 radicals and/or ozone with the first generation products of toluene oxidation are sources of organic aerosol during the atmospheric oxidation of toluene. The aerosol results fall into two groups, aerosol formed in the absence and presence of ozone. An analytical expression for aerosol formation is developed and values are obtained for the yield of the aerosol species. In the absence of ozone the aerosol yield, defined as aerosol formed per unit toluene consumed once a threshold for aerosol formation has been exceeded, is 0.075 +/- 0.004. In the presence of ozone the aerosol yield is 0.108 +/- 0.004. This work provides experimental evidence and a simple theory confirming the formation of aerosol from secondary reactions.

Secondary organic aerosol formation from in situ OH, O3, and NO3 oxidation of ambient forest air in an oxidation flow reactor

Science.gov (United States)

Palm, Brett B.; Campuzano-Jost, Pedro; Day, Douglas A.; Ortega, Amber M.; Fry, Juliane L.; Brown, Steven S.; Zarzana, Kyle J.; Dube, William; Wagner, Nicholas L.; Draper, Danielle C.; Kaser, Lisa; Jud, Werner; Karl, Thomas; Hansel, Armin; Gutiérrez-Montes, Cándido; Jimenez, Jose L.

2017-04-01

Ambient pine forest air was oxidized by OH, O3, or NO3 radicals using an oxidation flow reactor (OFR) during the BEACHON-RoMBAS (Bio-hydro-atmosphere interactions of Energy, Aerosols, Carbon, H2O, Organics and Nitrogen - Rocky Mountain Biogenic Aerosol Study) campaign to study biogenic secondary organic aerosol (SOA) formation and organic aerosol (OA) aging. A wide range of equivalent atmospheric photochemical ages was sampled, from hours up to days (for O3 and NO3) or weeks (for OH). Ambient air processed by the OFR was typically sampled every 20-30 min, in order to determine how the availability of SOA precursor gases in ambient air changed with diurnal and synoptic conditions, for each of the three oxidants. More SOA was formed during nighttime than daytime for all three oxidants, indicating that SOA precursor concentrations were higher at night. At all times of day, OH oxidation led to approximately 4 times more SOA formation than either O3 or NO3 oxidation. This is likely because O3 and NO3 will only react with gases containing C = C bonds (e.g., terpenes) to form SOA but will not react appreciably with many of their oxidation products or any species in the gas phase that lacks a C = C bond (e.g., pinonic acid, alkanes). In contrast, OH can continue to react with compounds that lack C = C bonds to produce SOA. Closure was achieved between the amount of SOA formed from O3 and NO3 oxidation in the OFR and the SOA predicted to form from measured concentrations of ambient monoterpenes and sesquiterpenes using published chamber yields. This is in contrast to previous work at this site (Palm et al., 2016), which has shown that a source of SOA from semi- and intermediate-volatility organic compounds (S/IVOCs) 3.4 times larger than the source from measured VOCs is needed to explain the measured SOA formation from OH oxidation. This work suggests that those S/IVOCs typically do not contain C = C bonds. O3 and NO3 oxidation produced SOA with elemental O : C and H : C

Nitrate radical oxidation of γ-terpinene: hydroxy nitrate, total organic nitrate, and secondary organic aerosol yields

Science.gov (United States)

Slade, Jonathan H.; de Perre, Chloé; Lee, Linda; Shepson, Paul B.

2017-07-01

Polyolefinic monoterpenes represent a potentially important but understudied source of organic nitrates (ONs) and secondary organic aerosol (SOA) following oxidation due to their high reactivity and propensity for multi-stage chemistry. Recent modeling work suggests that the oxidation of polyolefinic γ-terpinene can be the dominant source of nighttime ON in a mixed forest environment. However, the ON yields, aerosol partitioning behavior, and SOA yields from γ-terpinene oxidation by the nitrate radical (NO3), an important nighttime oxidant, have not been determined experimentally. In this work, we present a comprehensive experimental investigation of the total (gas + particle) ON, hydroxy nitrate, and SOA yields following γ-terpinene oxidation by NO3. Under dry conditions, the hydroxy nitrate yield = 4(+1/-3) %, total ON yield = 14(+3/-2) %, and SOA yield ≤ 10 % under atmospherically relevant particle mass loadings, similar to those for α-pinene + NO3. Using a chemical box model, we show that the measured concentrations of NO2 and γ-terpinene hydroxy nitrates can be reliably simulated from α-pinene + NO3 chemistry. This suggests that NO3 addition to either of the two internal double bonds of γ-terpinene primarily decomposes forming a relatively volatile keto-aldehyde, reconciling the small SOA yield observed here and for other internal olefinic terpenes. Based on aerosol partitioning analysis and identification of speciated particle-phase ON applying high-resolution liquid chromatography-mass spectrometry, we estimate that a significant fraction of the particle-phase ON has the hydroxy nitrate moiety. This work greatly contributes to our understanding of ON and SOA formation from polyolefin monoterpene oxidation, which could be important in the northern continental US and the Midwest, where polyolefinic monoterpene emissions are greatest.

Inhalation toxicology of industrial plutonium and uranium oxide aerosols I. Physical chemical characterization

International Nuclear Information System (INIS)

Eidson, A.F.; Mewhinney, J.A.

1978-01-01

In the fabrication of mixed plutonium and uranium oxide fuel, large quantities of dry powders are processed, causing dusty conditions in glove box enclosures. Inadvertent loss of glove box integrity or failure of air filter systems can lead to human inhalation exposure. Powdered samples and aerosol samples of these materials obtained during two fuel fabrication process steps have been obtained. A regimen of physical chemical tests of properties of these materials has been employed to identify physical chemical properties which may influence their biological behavior and dosimetry. Materials to be discussed are 750 deg. C heat-treated, mixed uranium and plutonium oxides obtained from the ball milling operation and 1750 deg. C heat-treated, mixed uranium and plutonium oxides obtained from the centerless grinding of fuel pellets. Results of x-ray diffraction studies have shown that the powder generated by the centerless grinding of fuel pellets is best described as a solid solution of UO x and PuO x consistent with its temperature history. In vitro dissolution studies of both mixed oxide materials indicate a generally similar dissolution rate for both materials. In one solvent, the material with the higher temperature history dissolves more rapidly. The x-ray diffraction and in vitro dissolution results as well as preliminary results of x-ray photoelectron spectroscopic analyses will be compared and the implications for the associated biological studies will be discussed. (author)

Aerosol Fragmentation Driven by Coupling of Acid-Base and Free-Radical Chemistry in the Heterogeneous Oxidation of Aqueous Citric Acid by OH Radicals.

Science.gov (United States)

Liu, Matthew J; Wiegel, Aaron A; Wilson, Kevin R; Houle, Frances A

2017-08-10

A key uncertainty in the heterogeneous oxidation of carboxylic acids by hydroxyl radicals (OH) in aqueous-phase aerosol is how the free-radical reaction pathways might be altered by acid-base chemistry. In particular, if acid-base reactions occur concurrently with acyloxy radical formation and unimolecular decomposition of alkoxy radicals, there is a possibility that differences in reaction pathways impact the partitioning of organic carbon between the gas and aqueous phases. To examine these questions, a kinetic model is developed for the OH-initiated oxidation of citric acid aerosol at high relative humidity. The reaction scheme, containing both free-radical and acid-base elementary reaction steps with physically validated rate coefficients, accurately predicts the experimentally observed molecular composition, particle size, and average elemental composition of the aerosol upon oxidation. The difference between the two reaction channels centers on the reactivity of carboxylic acid groups. Free-radical reactions mainly add functional groups to the carbon skeleton of neutral citric acid, because carboxylic acid moieties deactivate the unimolecular fragmentation of alkoxy radicals. In contrast, the conjugate carboxylate groups originating from acid-base equilibria activate both acyloxy radical formation and carbon-carbon bond scission of alkoxy radicals, leading to the formation of low molecular weight, highly oxidized products such as oxalic and mesoxalic acid. Subsequent hydration of carbonyl groups in the oxidized products increases the aerosol hygroscopicity and accelerates the substantial water uptake and volume growth that accompany oxidation. These results frame the oxidative lifecycle of atmospheric aerosol: it is governed by feedbacks between reactions that first increase the particle oxidation state, then eventually promote water uptake and acid-base chemistry. When coupled to free-radical reactions, acid-base channels lead to formation of low molecular

Experimental and modelling studies of iodine oxide formation and aerosol behaviour relevant to nuclear reactor accidents

International Nuclear Information System (INIS)

Dickinson, S.; Auvinen, A.; Ammar, Y.; Bosland, L.; Clément, B.; Funke, F.; Glowa, G.; Kärkelä, T.; Powers, D.A.; Tietze, S.; Weber, G.; Zhang, S.

2014-01-01

Highlights: • Radiolytic reactions can influence iodine volatility following a nuclear accident. • Kinetic models have been developed based on atmospheric chemistry studies. • Properties of iodine oxide aerosols produced by radiation have been measured. • Decomposition of iodine oxides by the action of heat or radiation has been observed. - Abstract: Plant assessments have shown that iodine contributes significantly to the source term for a range of accident scenarios. Iodine has a complex chemistry that determines its chemical form and, consequently, its volatility in the containment. If volatile iodine species are formed by reactions in the containment, they will be subject to radiolytic reactions in the atmosphere, resulting in the conversion of the gaseous species into involatile iodine oxides, which may deposit on surfaces or re-dissolve in water pools. The concentration of airborne iodine in the containment will, therefore, be determined by the balance between the reactions contributing to the formation and destruction of volatile species, as well as by the physico-chemical properties of the iodine oxide aerosols which will influence their longevity in the atmosphere. This paper summarises the work that has been done in the framework of the EC SARNET (Severe Accident Research Network) to develop a greater understanding of the reactions of gaseous iodine species in irradiated air/steam atmospheres, and the nature and behaviour of the reaction products. This work has mainly been focussed on investigating the nature and behaviour of iodine oxide aerosols, but earlier work by members of the SARNET group on gaseous reaction rates is also discussed to place the more recent work into context

Correlation of Secondary Organic Aerosol with Odd Oxygen in Mexico City

Energy Technology Data Exchange (ETDEWEB)

Herndon, Scott C.; Onasch, Timothy B.; Wood, Ezra C.; Kroll, Jesse H.; Canagaratna, M. R.; Jayne, John T.; Zavala, Miguel A.; Knighton, W. Berk; Mazzoleni, Claudio; Dubey, Manvendra K.; Ulbrich, Ingrid M.; Jimenez, Jose L.; Seila, Robert; de Gouw, Joost A.; de Foy, B.; Fast, Jerome D.; Molina, Luisa T.; Kolb, C. E.; Worsnop, Douglas R.

2008-08-05

Data collected from a mountain location within the Mexico City limits are used to demonstrate a correlation between secondary organic aerosol and odd-oxygen (O3 + NO2). Positive matrix factorization techniques are employed to separate organic aerosol components: hydrocarbon-like organic aerosol; oxidized-organic aerosol; and biomass burning organic aerosol. The measured hydrocarbon-like organic aerosol is correlated with urban CO (8±1) µg m-3 ppmv-1. The measured oxidized-organic aerosol is associated with photochemical oxidation products and correlates with odd-oxygen with an apparent slope of (70-120) µg m-3 ppmv-1. The dependence of the oxidized-organic aerosol to odd-oxygen correlation on the nature of the gas-phase hydrocarbon profile is discussed.

Isoprene oxidation by nitrate radical: alkyl nitrate and secondary organic aerosol yields

Directory of Open Access Journals (Sweden)

A. W. Rollins

2009-09-01

Full Text Available Alkyl nitrates and secondary organic aerosol (SOA produced during the oxidation of isoprene by nitrate radicals has been observed in the SAPHIR (Simulation of Atmospheric PHotochemistry In a large Reaction Chamber chamber. A 16 h dark experiment was conducted with temperatures at 289–301 K, and maximum concentrations of 11 ppb isoprene, 62.4 ppb O₃ and 31.1 ppb NO_x. We find the yield of nitrates is 70±8% from the isoprene + NO₃ reaction, and the yield for secondary dinitrates produced in the reaction of primary isoprene nitrates with NO₃ is 40±20%. We find an effective rate constant for reaction of NO₃ with the group of first generation oxidation products to be 7×10⁻¹⁴ molecule⁻¹ cm³ s⁻¹. At the low total organic aerosol concentration in the chamber (max=0.52 μg m⁻³ we observed a mass yield (ΔSOA mass/Δisoprene mass of 2% for the entire 16 h experiment. However a comparison of the timing of the observed SOA production to a box model simulation of first and second generation oxidation products shows that the yield from the first generation products was <0.7% while the further oxidation of the initial products leads to a yield of 14% (defined as ΔSOA/Δisoprene^2x where Δisoprene^2x is the mass of isoprene which reacted twice with NO₃. The SOA yield of 14% is consistent with equilibrium partitioning of highly functionalized C₅ products of isoprene oxidation.

Secondary organic aerosol in the global aerosol – chemical transport model Oslo CTM2

Directory of Open Access Journals (Sweden)

I. S. A. Isaksen

2007-11-01

Full Text Available The global chemical transport model Oslo CTM2 has been extended to include the formation, transport and deposition of secondary organic aerosol (SOA. Precursor hydrocarbons which are oxidised to form condensible species include both biogenic species such as terpenes and isoprene, as well as species emitted predominantly by anthropogenic activities (toluene, m-xylene, methylbenzene and other aromatics. A model simulation for 2004 gives an annual global SOA production of approximately 55 Tg. Of this total, 2.5 Tg is found to consist of the oxidation products of anthropogenically emitted hydrocarbons, and about 15 Tg is formed by the oxidation products of isoprene. The global production of SOA is increased to about 69 Tg yr−1 by allowing semi-volatile species to partition to ammonium sulphate aerosol. This brings modelled organic aerosol values closer to those observed, however observations in Europe remain significantly underestimated. Allowing SOA to partition into ammonium sulphate aerosol increases the contribution of anthropogenic SOA from about 4.5% to 9.4% of the total production. Total modelled organic aerosol (OA values are found to represent a lower fraction of the measured values in winter (when primary organic aerosol (POA is the dominant OA component than in summer, which may be an indication that estimates of POA emissions are too low. Additionally, for measurement stations where the summer OA values are higher than in winter, the model generally underestimates the increase in summertime OA. In order to correctly model the observed increase in OA in summer, additional SOA sources or formation mechanisms may be necessary. The importance of NO3 as an oxidant of SOA precursors is found to vary regionally, causing up to 50%–60% of the total amount of SOA near the surface in polluted regions and less than 25% in more remote areas, if the yield of condensible oxidation products for β-pinene is used for NO3 oxidation of all terpenes

Comparison of physical chemical properties of powders and respirable aerosols of industrial mixed uranium and plutonium oxide fuels

International Nuclear Information System (INIS)

Eidson, A.F.

1982-01-01

Studies were performed to characterize physical and chemical properties which may be important in determining the metabolism of accidentally released, inhaled aerosols of industrial mixed uranium and plutonium oxide fuels and to compare the properties of bulk powders and the respirable fraction they include. X-ray diffraction measurements showed that analysis of mixed-oxide powders from four process steps served to characterize their respirable fractions. IR spectroscopy was useful as a method to detect organic binders that were not observed by X-ray diffraction methods. Both X-ray diffraction and IR spectroscopy methods can be used in combination to identify the sources of a complex aerosol that might be released from more than one fabrication step. Isotopic distributions in powders and aerosols showed that information important for radiation dose to tissue calculations or Pu lung burden estimates can be obtained by analysis of powders. (U.K.)

Laboratory investigation of photochemical oxidation of organic aerosol from wood fires 2: analysis of aerosol mass spectrometer data

Directory of Open Access Journals (Sweden)

A. P. Grieshop

2009-03-01

Full Text Available Experiments were conducted to investigate the effects of photo-oxidation on organic aerosol (OA in dilute wood smoke by exposing emissions from soft- and hard-wood fires to UV light in a smog chamber. This paper focuses on changes in OA composition measured using a unit-mass-resolution quadrupole Aerosol Mass Spectrometer (AMS. The results highlight how photochemical processing can lead to considerable evolution of the mass, volatility and level of oxygenation of biomass-burning OA. Photochemical oxidation produced substantial new OA, more than doubling the OA mass after a few hours of aging under typical summertime conditions. Aging also decreased the volatility of the OA and made it progressively more oxygenated. The results also illustrate strengths of, and challenges with, using AMS data for source apportionment analysis. For example, the mass spectra of fresh and aged BBOA are distinct from fresh motor-vehicle emissions. The mass spectra of the secondary OA produced from aging wood smoke are very similar to those of the oxygenated OA (OOA that dominates ambient AMS datasets, further reinforcing the connection between OOA and OA formed from photo-chemistry. In addition, aged wood smoke spectra are similar to those from OA created by photo-oxidizing dilute diesel exhaust. This demonstrates that the OOA observed in the atmosphere can be produced by photochemical aging of dilute emissions from different types of combustion systems operating on fuels with modern or fossil carbon. Since OOA is frequently the dominant component of ambient OA, the similarity of spectra of aged emissions from different sources represents an important challenge for AMS-based source apportionment studies.

Dissolution of uranium oxide materials in simulated lung fluid

International Nuclear Information System (INIS)

Scripsick, R.C.; Soderholm, S.C.

1985-01-01

Depleted uranium (DU) oxide aerosols prepared in the laboratory and collected in the field were tested to characterize their dissolution in simulated lung fluid and to determine how dissolution is affected by aerosol preparation. DU, a by-product of the uranium fuel cycle, has been selected by the US military for use in several types of munitions. During development, manufacture, testing, and use of these munitions, opportunities exist for inhalation exposure to various (usually oxide) aerosol forms of DU. The hazard potential associated with such exposures is closely related to the chemical form, the size of the DU aerosol material, and its dissolution properties. Five DU sample materials produced by exposing uranium alloy penetrators to certain controlled oxidation atmospheres were studied (oxidation temperatures ranged from 500 to 900 0 C). In addition, two DU sample materials collected in the field were provided by the US Air Force. All sample materials were generated as aerosols and the respirable fraction was separated and collected. Data suggest that under some conditions a rapidly dissolving U 3 O 8 fraction may be formed concurrent with the production of UO 2

Experimental Characterization and Hygroscopicity Determination of Secondary Aerosol from D5 Cyclic Siloxane Oxidation

Science.gov (United States)

Stanier, C. O.; Janechek, N. J.; Bryngelson, N.; Marek, R. F.; Lersch, T.; Bunker, K.; Casuccio, G.; Brune, W. H.; Hornbuckle, K. C.

2017-12-01

Cyclic volatile methyl siloxanes are anthropogenic chemicals present in personal care products such as antiperspirants and lotions. These are volatile chemicals that are readily released into the atmosphere by product use. Due to their emission and relatively slow kinetics of their major transformation pathway, reaction with hydroxyl radicals (OH), these compounds are present in high concentrations in indoor environments and widespread in outdoor environments. Cyclic siloxane reaction with OH can lead to secondary organic aerosols, and due to the widespread prevalence of the parent compounds, may be an important source of ambient aerosols. Atmospheric aerosols have important influences to the climate by affecting the radiative balance and by serving as cloud condensation nuclei (CCN) which influence clouds. While the parent compounds have been well-studied, the oxidation products have received much less attention, with almost no ambient measurements or experimental physical property data. We report physical properties of aerosols generated by reacting the cyclic siloxane D5 with OH using a Potential Aerosol Mass (PAM) photochemical chamber. The particles were characterized by SMPS, imaging and elemental analysis using both Transmission Electron Microscopy and Scanning Transmission Electron Microscopy equipped with Energy Dispersive X-ray Spectroscopy systems (TEM-EDS and STEM-EDS), volatility measurements using Volatility Tandem Differential Mobility Analyzer (V-TDMA), and hygroscopicity measurements to determine CCN potential using a Droplet Measurement Technologies Cloud Condensation Nuclei Counter (DMT-CCN). Aerosol yield sensitivity to D5 and OH concentrations, residence time, and seed aerosols were analyzed. TEM-EDS and STEM-EDS analysis show spherical particle morphology with elemental composition consistent with aerosols derived from cyclic siloxane sources. Measured aerosol yields were 20-50% with typical aerosol concentrations 300,000 particles cm-3, up to

A perspective on SOA generated in aerosol water from glyoxal and methylglyoxal and its impacts on climate-relevant aerosol properties

Science.gov (United States)

Sareen, N.; McNeill, V. F.

2011-12-01

. These compounds included (hemi)acetals, aldol condensation products, and oligomeric species up to 759 amu. Since these products are vulnerable to oxidants such as O3 and OH in the atmosphere, kinetic studies were conducted to study their affect upon exposure to O3 and OH. Custom-designed flow tube reactors were coupled with the Aerosol-CIMS to monitor aerosol composition, and consequently this data was used to determine reactive uptake coefficients (γO3~10-8 and γOH~ 10-6). Additionally, the lifetime of these SOA species in the atmosphere can be estimated and if these time scales are sufficiently long, they may affect aerosol optical properties. The effect of oxidation on the optical properties is also currently being tested by collecting aerosol particles before and after oxidation on a quartz window and testing changes in absorption using the UV-Vis spectrophotometer. The results of all these studies will be integrated to understand the role of methylglyoxal as a SOA precursor and the effect on various aerosol properties, and this will be used as a model system to predict the fate of similar organics in the atmosphere.

Test equipment used for radiation protection type testing of aerosol filters at the National Board of Nuclear Safety and Radiation Protection (SAAS)

International Nuclear Information System (INIS)

Ullmann, W.; Przyborowski, S.

1977-01-01

Following a description of the overall design of test equipment developed in the SAAS for radiation protection type testing of aerosol filters, the most important physical and technical details concerning the preparation and measurement of test aerosols as well as the sampling procedure upstream and downstream of the filter to the tested, are comprehensively discussed. Furthermore, experiences gained during several years with different devices for mixing and diluting the aerosols are reported. (author)

Secondary organic aerosol production from pinanediol, a semi-volatile surrogate for first-generation oxidation products of monoterpenes

Science.gov (United States)

Ye, Penglin; Zhao, Yunliang; Chuang, Wayne K.; Robinson, Allen L.; Donahue, Neil M.

2018-05-01

We have investigated the production of secondary organic aerosol (SOA) from pinanediol (PD), a precursor chosen as a semi-volatile surrogate for first-generation oxidation products of monoterpenes. Observations at the CLOUD facility at CERN have shown that oxidation of organic compounds such as PD can be an important contributor to new-particle formation. Here we focus on SOA mass yields and chemical composition from PD photo-oxidation in the CMU smog chamber. To determine the SOA mass yields from this semi-volatile precursor, we had to address partitioning of both the PD and its oxidation products to the chamber walls. After correcting for these losses, we found OA loading dependent SOA mass yields from PD oxidation that ranged between 0.1 and 0.9 for SOA concentrations between 0.02 and 20 µg m-3, these mass yields are 2-3 times larger than typical of much more volatile monoterpenes. The average carbon oxidation state measured with an aerosol mass spectrometer was around -0.7. We modeled the chamber data using a dynamical two-dimensional volatility basis set and found that a significant fraction of the SOA comprises low-volatility organic compounds that could drive new-particle formation and growth, which is consistent with the CLOUD observations.

The composition of aerosols generated during a severe reactor accident: Experimental results from the Power Burst Facility Severe Fuel Damage Test 1-4

International Nuclear Information System (INIS)

Petti, D.A.; Hobbins, R.R.; Hagrman, D.L.

1994-01-01

Experimental results on fission product and aerosol release during the Power Burst Facility Severe Fuel Damages (SFD) Test 1-4 are examined to determine the composition of aerosols that would be generated during a severe reactor accident. The SFD 1-4 measured aerosol contained significant quantities of volatile fission products (VFPs) (cesium, iodine, tellurium), control materials (silver and cadmium), and structural materials (tin), indicating that fission product release, vaporization of control material, and release of tin from oxidized Zircaloy were all important aerosol sources. On average the aerosol composition is between one-quarter and one-half VFPs (especially cesium), with the remainder being control material (especially cadmium), and structural material (especially tin). Source term computer codes like CORSOR-M tend to overpredict the release of structural and control rod material relative to fission products by a factor of between 2 and 15 because the models do not account for relocation of molten control, fuel, and structural material during the degradation process, which tends to reduce the aerosol source. The results indicate that the aerosol generation in a severe reactor accident is intimately linked to the core degradation process. They recommend that these results be used to improve the models in source term computer codes

Identification of secondary aerosol precursors emitted by an aircraft turbofan

Science.gov (United States)

Kılıç, Doğuşhan; El Haddad, Imad; Brem, Benjamin T.; Bruns, Emily; Bozetti, Carlo; Corbin, Joel; Durdina, Lukas; Huang, Ru-Jin; Jiang, Jianhui; Klein, Felix; Lavi, Avi; Pieber, Simone M.; Rindlisbacher, Theo; Rudich, Yinon; Slowik, Jay G.; Wang, Jing; Baltensperger, Urs; Prévôt, Andre S. H.

2018-05-01

Oxidative processing of aircraft turbine-engine exhausts was studied using a potential aerosol mass (PAM) chamber at different engine loads corresponding to typical flight operations. Measurements were conducted at an engine test cell. Organic gases (OGs) and particle emissions pre- and post-PAM were measured. A suite of instruments, including a proton-transfer-reaction mass spectrometer (PTR-MS) for OGs, a multigas analyzer for CO, CO2, NOx, and an aerosol mass spectrometer (AMS) for nonrefractory particulate matter (NR-PM1) were used. Total aerosol mass was dominated by secondary aerosol formation, which was approximately 2 orders of magnitude higher than the primary aerosol. The chemical composition of both gaseous and particle emissions were also monitored at different engine loads and were thrust-dependent. At idling load (thrust 2.5-7 %), more than 90 % of the secondary particle mass was organic and could mostly be explained by the oxidation of gaseous aromatic species, e.g., benzene; toluene; xylenes; tri-, tetra-, and pentamethyl-benzene; and naphthalene. The oxygenated-aromatics, e.g., phenol, furans, were also included in this aromatic fraction and their oxidation could alone explain up to 25 % of the secondary organic particle mass at idling loads. The organic fraction decreased with thrust level, while the inorganic fraction increased. At an approximated cruise load sulfates comprised 85 % of the total secondary particle mass.

Description of test facilities bound to the research on sodium aerosols - some significant results

Energy Technology Data Exchange (ETDEWEB)

Dolias, M; Lafon, A; Vidard, M; Schaller, K H [DRNR/STRS - Centre de Cadarache, Saint-Paul-lez-Durance (France)

1977-01-01

This communication is dedicated to the description of the CEA (French Atomic Energy Authority) testing located at CADARACHE and which are utilized for the study of sodium aerosols behavior. These testing loops are necessary for studying the operating of equipment such as filters, sodium vapour traps, condensers and separators. It is also possible to study the effect of characteristics parameters on formation, coagulation and carrying away of sodium aerosols in the cover gas. Sodium aerosols deposits in a vertical annular space configuration with a cold area in its upper part are also studied. Some significant results emphasize the importance of operating conditions on the formation of aerosols. (author)

SUBMERGED GRAVEL SCRUBBER DEMONSTRATION AS A PASSIVE AIR CLEANER FOR CONTAINMENT VENTING AND PURGING WITH SODIUM AEROSOLS -- CSTF TESTS AC7 - AC10

Energy Technology Data Exchange (ETDEWEB)

HILLIARD, R K.; MCCORMACK, J D.; POSTMA, A K.

1981-11-01

Four large-scale air cleaning tests (AC7 - AC10) were performed in the Containment Systems Test Facility (CS'lF) to demonstrate the performance of a Submerged Gravel Scrubber for cleaning the effluent gas from a vented and purged breeder reactor containment vessel. The test article, comprised of a Submerged Gravel Scrubber (SGS) followed by a high efficiency fiber demister, had a design gas flow rate of 0.47 m{sup 3}/s (1000 ft{sup 3}/min) at a pressure drop of 9.0 kPa (36 in. H{sub 2}O). The test aerosol was sodium oxide, sodium hydroxide, or sodium carbonate generated in the 850-m{sup 3} CSTF vessel by continuously spraying sodium into the air-filled vessel while adding steam or carbon dioxide. Approximately 4500 kg (10,000 lb) of sodium was sprayed over a total period of 100 h during the tests. The SGS/Demister system was shown to be highly efficient (removing ~99.98% of the entering sodium aerosol mass), had a high mass loading capacity, and operated in a passive manner, with no electrical requirement. Models for predicting aerosol capture, gas cooling, and pressure drop are developed and compared with experimental results.

Secondary organic aerosol formation from in-use motor vehicle emissions using a potential aerosol mass reactor.

Science.gov (United States)

Tkacik, Daniel S; Lambe, Andrew T; Jathar, Shantanu; Li, Xiang; Presto, Albert A; Zhao, Yunliang; Blake, Donald; Meinardi, Simone; Jayne, John T; Croteau, Philip L; Robinson, Allen L

2014-10-07

Secondary organic aerosol (SOA) formation from in-use vehicle emissions was investigated using a potential aerosol mass (PAM) flow reactor deployed in a highway tunnel in Pittsburgh, Pennsylvania. Experiments consisted of passing exhaust-dominated tunnel air through a PAM reactor over integrated hydroxyl radical (OH) exposures ranging from ∼ 0.3 to 9.3 days of equivalent atmospheric oxidation. Experiments were performed during heavy traffic periods when the fleet was at least 80% light-duty gasoline vehicles on a fuel-consumption basis. The peak SOA production occurred after 2-3 days of equivalent atmospheric oxidation. Additional OH exposure decreased the SOA production presumably due to a shift from functionalization to fragmentation dominated reaction mechanisms. Photo-oxidation also produced substantial ammonium nitrate, often exceeding the mass of SOA. Analysis with an SOA model highlight that unspeciated organics (i.e., unresolved complex mixture) are a very important class of precursors and that multigenerational processing of both gases and particles is important at longer time scales. The chemical evolution of the organic aerosol inside the PAM reactor appears to be similar to that observed in the atmosphere. The mass spectrum of the unoxidized primary organic aerosol closely resembles ambient hydrocarbon-like organic aerosol (HOA). After aging the exhaust equivalent to a few hours of atmospheric oxidation, the organic aerosol most closely resembles semivolatile oxygenated organic aerosol (SV-OOA) and then low-volatility organic aerosol (LV-OOA) at higher OH exposures. Scaling the data suggests that mobile sources contribute ∼ 2.9 ± 1.6 Tg SOA yr(-1) in the United States, which is a factor of 6 greater than all mobile source particulate matter emissions reported by the National Emissions Inventory. This highlights the important contribution of SOA formation from vehicle exhaust to ambient particulate matter concentrations in urban areas.

An exploratory study of alkali sulfate aerosol formation during biomass combustion

DEFF Research Database (Denmark)

Løj, Lusi Hindiyarti; Frandsen, Flemming; Livbjerg, Hans

2008-01-01

mechanism. The modeling predictions are compared to data from laboratory experiments and entrained flow reactor experiments available in the literature. The analysis support that alkali sulfate aerosols are formed from homogeneous nucleation following a series of steps occurring in the gas phase. The rate......It is still in discussion to what extent alkali sulfate aerosols in biomass combustion are formed in the gas phase by a homogeneous mechanism or involve heterogeneous or catalyzed reactions. The present study investigates sulfate aerosol formation based on calculations with a detailed gas phase......-limiting step may be the oxidation of sulfite to sulfate, rather than the oxidation of SO2 to SO3 proposed previously. Even though the proposed model is consistent with experimental observations, experiments in a rigorously homogeneous system are called for to test its validity....

Sodium oxide aerosol filtration

International Nuclear Information System (INIS)

Duverger de Cuy, G.

1979-01-01

In the scope of the sodium aerosol trapping research effort by the CEA/DSN, the retention capacity and yield were measured for very high efficiency fiberglass filters and several types of prefilters (cyclone agglomerator, fabric prefilters, water scrubbers). (author)

Sodium oxide aerosol filtration

Energy Technology Data Exchange (ETDEWEB)

Duverger de Cuy, G [DSN/SESTR, Centre de Cadarache, Saint-Paul-lez-Durance (France)

1979-03-01

In the scope of the sodium aerosol trapping research effort by the CEA/DSN, the retention capacity and yield were measured for very high efficiency fiberglass filters and several types of prefilters (cyclone agglomerator, fabric prefilters, water scrubbers). (author)

Solubility of plutonium dioxide aerosols, in vitro

International Nuclear Information System (INIS)

Newton, G.J.; Kanapilly, G.M.

1976-01-01

Solubility of plutonium aerosols is an important parameter in establishing risk estimates for industrial workers who might accidentally inhale these materials and in evaluating environmental health impacts associated with Pu. In vitro solubility of industrial plutonium aerosols in a simulated lung fluid is compared to similar studies with ultrafine aerosols from laser ignition of delta phase plutonium metal and laboratory-produced spherical particles of 238 PuO 2 and 239 PuO 2 . Although relatively insoluble, industrial plutonium-mixed oxide aerosols were much more soluble than laboratory-produced plutonium dioxide particles. Chain agglomerate aerosols from laser ignition of metallic Pu indicated in vitro dissolution half-times of 10 and 50 days for activity median aerodynamic diameter (AMAD) of 0.7 and 2.3 μm, respectively. Plutonium-containing mixed oxide aerosols indicated dissolution half-times of 40 to 500 days for particles formed by industrial powder comminution and blending. Centerless grinding of fuel pellets yielded plutonium-containing aerosols with dissolution half-times of 1200 to 8000 days. All mixed oxide particles were in the size range 1.0 μm to 2.5 μm AMAD

Aerosol Delivery for Amendment Distribution in Contaminated Vadose Zones

Science.gov (United States)

Hall, R. J.; Murdoch, L.; Riha, B.; Looney, B.

2011-12-01

aqueous and oil deposition are assumed to occur due to surface interactions, and susceptibility to evaporation of aqueous aerosols. Distal salt accumulation during salt water aerosol tests suggests that solid salt forms as salt water aerosols evaporate. The solid salt aerosols are less likely to deposit, so they travel further than aqueous aerosols. A numerical model was calibrated using results from lab-scale tests. The calibrated model was then used to simulate field-scale aerosol injection. Results from field-scale simulations suggest that effective radii of influence on the scale of 8-10 meters could be achieved in partially saturated sand. The aerosol delivery process appears to be capable distributing oil amendments over considerable volumes of formation at concentrations appropriate for remediation purposes. Thus far, evaporation has limited liquid accumulation observed when distributing aqueous aerosols, however, results from salt water experiments suggest that injection of solid phase aerosols can effectively distribute water soluble amendments (electron donor, pH buffer, oxidants, etc.). Utilization of aerosol delivery could considerably expand treatment options for contaminated vadose zones at a wide variety of sites.

Nitrate radicals and biogenic volatile organic compounds: oxidation, mechanisms, and organic aerosol

Energy Technology Data Exchange (ETDEWEB)

Ng, Nga Lee; Brown, Steven S.; Archibald, Alexander T.; Atlas, Elliot; Cohen, Ronald C.; Crowley, John N.; Day, Douglas A.; Donahue, Neil M.; Fry, Juliane L.; Fuchs, Hendrik; Griffin, Robert J.; Guzman, Marcelo I.; Herrmann, Hartmut; Hodzic, Alma; Iinuma, Yoshiteru; Jimenez, José L.; Kiendler-Scharr, Astrid; Lee, Ben H.; Luecken, Deborah J.; Mao, Jingqiu; McLaren, Robert; Mutzel, Anke; Osthoff, Hans D.; Ouyang, Bin; Picquet-Varrault, Benedicte; Platt, Ulrich; Pye, Havala O. T.; Rudich, Yinon; Schwantes, Rebecca H.; Shiraiwa, Manabu; Stutz, Jochen; Thornton, Joel A.; Tilgner, Andreas; Williams, Brent J.; Zaveri, Rahul A.

2017-01-01

Oxidation of biogenic volatile organic compounds (BVOC) by the nitrate radical (NO₃) represents one of the important interactions between anthropogenic emissions related to combustion and natural emissions from the biosphere. This interaction has been recognized for more than 3 decades, during which time a large body of research has emerged from laboratory, field, and modeling studies. NO₃-BVOC reactions influence air quality, climate and visibility through regional and global budgets for reactive nitrogen (particularly organic nitrates), ozone, and organic aerosol. Despite its long history of research and the significance of this topic in atmospheric chemistry, a number of important uncertainties remain. These include an incomplete understanding of the rates, mechanisms, and organic aerosol yields for NO₃-BVOC reactions, lack of constraints on the role of heterogeneous oxidative processes associated with the NO₃ radical, the difficulty of characterizing the spatial distributions of BVOC and NO₃ within the poorly mixed nocturnal atmosphere, and the challenge of constructing appropriate boundary layer schemes and non-photochemical mechanisms for use in state-of-the-art chemical transport and chemistry–climate models.

This review is the result of a workshop of the same title held at the Georgia Institute of Technology in June 2015. The first half of the review summarizes the current literature on NO₃-BVOC chemistry, with a particular focus on recent advances in instrumentation and models, and in organic nitrate and secondary organic aerosol (SOA) formation chemistry. Building on this current understanding, the second half of the review outlines impacts of NO₃-BVOC chemistry on air quality and climate, and suggests critical research needs to better constrain this interaction to improve the predictive capabilities of atmospheric models.

Performance Testing of Tracer Gas and Tracer Aerosol Detectors for use in Radionuclide NESHAP Compliance Testing

Energy Technology Data Exchange (ETDEWEB)

Fuehne, David Patrick [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Lattin, Rebecca Renee [Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

2017-06-28

The Rad-NESHAP program, part of the Air Quality Compliance team of LANL’s Compliance Programs group (EPC-CP), and the Radiation Instrumentation & Calibration team, part of the Radiation Protection Services group (RP-SVS), frequently partner on issues relating to characterizing air flow streams. This memo documents the most recent example of this partnership, involving performance testing of sulfur hexafluoride detectors for use in stack gas mixing tests. Additionally, members of the Rad-NESHAP program performed a functional trending test on a pair of optical particle counters, comparing results from a non-calibrated instrument to a calibrated instrument. Prior to commissioning a new stack sampling system, the ANSI Standard for stack sampling requires that the stack sample location must meet several criteria, including uniformity of tracer gas and aerosol mixing in the air stream. For these mix tests, tracer media (sulfur hexafluoride gas or liquid oil aerosol particles) are injected into the stack air stream and the resulting air concentrations are measured across the plane of the stack at the proposed sampling location. The coefficient of variation of these media concentrations must be under 20% when evaluated over the central 2/3 area of the stack or duct. The instruments which measure these air concentrations must be tested prior to the stack tests in order to ensure their linear response to varying air concentrations of either tracer gas or tracer aerosol. The instruments used in tracer gas and aerosol mix testing cannot be calibrated by the LANL Standards and Calibration Laboratory, so they would normally be sent off-site for factory calibration by the vendor. Operational requirements can prevent formal factory calibration of some instruments after they have been used in hazardous settings, e.g., within a radiological facility with potential airborne contamination. The performance tests described in this document are intended to demonstrate the reliable

Aerosol Scrubbing Performance Test for Self-Priming Scrubbing Nozzle Submerged in Water Pool

Energy Technology Data Exchange (ETDEWEB)

Lee, Doo Yong; Jung, Woo Young; Lee, Hyun Chul; Lee, Jong Chan; Kim, Gyu Tae; Song, Yong Jae [FNC Technology Co., Yongin (Korea, Republic of)

2016-10-15

A scrubbing nozzle is one of the key components for a wet scrubber process based Containment Filtered Venting System (CFVS). As a part of a development of Korean CFVS, a self-priming scrubbing nozzle shown in Fig. 1 has been developed based on the well-known venturi scrubber concept. The thermal-hydraulic performances such as the pressure drop across the nozzle, water suction behavior and droplet generation inside throat have been tested in the non-submerged condition as well as submerged condition. The self-priming scrubbing nozzle used for the wet scrubber based CFVS has been developed, which is submerged in the water pool. When there is gas flow at the inlet of the nozzle, the pool water is passively sucked from the water suction slit. The fine droplets generated inside the throat capture the aerosol particles and is discharged into the water pool. In the water pool, the pool scrubbing happens. The aerosol scrubbing performance tests for the developed self-priming scrubbing nozzle has been conducted under the operational conditions such as different aerosol sizes, different carrier gas steam fractions, different, different pool water level and nozzle inlet pressure. The major findings are as follows. (1) Aerosol scrubbing efficiency increases with the increase of the aerosol size. (2) Aerosol scrubbing efficiency increases with the increase of the carrier gas steam fraction. (3) Aerosol scrubbing.

Aerosol Scrubbing Performance Test for Self-Priming Scrubbing Nozzle Submerged in Water Pool

International Nuclear Information System (INIS)

Lee, Doo Yong; Jung, Woo Young; Lee, Hyun Chul; Lee, Jong Chan; Kim, Gyu Tae; Song, Yong Jae

2016-01-01

A scrubbing nozzle is one of the key components for a wet scrubber process based Containment Filtered Venting System (CFVS). As a part of a development of Korean CFVS, a self-priming scrubbing nozzle shown in Fig. 1 has been developed based on the well-known venturi scrubber concept. The thermal-hydraulic performances such as the pressure drop across the nozzle, water suction behavior and droplet generation inside throat have been tested in the non-submerged condition as well as submerged condition. The self-priming scrubbing nozzle used for the wet scrubber based CFVS has been developed, which is submerged in the water pool. When there is gas flow at the inlet of the nozzle, the pool water is passively sucked from the water suction slit. The fine droplets generated inside the throat capture the aerosol particles and is discharged into the water pool. In the water pool, the pool scrubbing happens. The aerosol scrubbing performance tests for the developed self-priming scrubbing nozzle has been conducted under the operational conditions such as different aerosol sizes, different carrier gas steam fractions, different, different pool water level and nozzle inlet pressure. The major findings are as follows. (1) Aerosol scrubbing efficiency increases with the increase of the aerosol size. (2) Aerosol scrubbing efficiency increases with the increase of the carrier gas steam fraction. (3) Aerosol scrubbing

E-cigarette aerosols induce lower oxidative stress in vitro when compared to tobacco smoke.

Science.gov (United States)

Taylor, Mark; Carr, Tony; Oke, Oluwatobiloba; Jaunky, Tomasz; Breheny, Damien; Lowe, Frazer; Gaça, Marianna

2016-07-01

Tobacco smoking is a risk factor for various diseases. The underlying cellular mechanisms are not fully characterized, but include oxidative stress, apoptosis, and necrosis. Electronic-cigarettes (e-cigarettes) have emerged as an alternative to and a possible means to reduce harm from tobacco smoking. E-cigarette vapor contains significantly lower levels of toxicants than cigarette smoke, but standardized methods to assess cellular responses to exposure are not well established. We investigated whether an in vitro model of the airway epithelium (human bronchial epithelial cells) and commercially available assays could differentiate cellular stress responses to aqueous aerosol extracts (AqE) generated from cigarette smoke and e-cigarette aerosols. After exposure to AqE concentrations of 0.063-0.500 puffs/mL, we measured the intracellular glutathione ratio (GSH:GSSG), intracellular generation of oxidant species, and activation of the nuclear factor erythroid-related factor 2 (Nrf2)-controlled antioxidant response elements (ARE) to characterize oxidative stress. Apoptotic and necrotic responses were characterized by increases in caspase 3/7 activity and reductions in viable cell protease activities. Concentration-dependent responses indicative of oxidative stress were obtained for all endpoints following exposure to cigarette smoke AqE: intracellular generation of oxidant species increased by up to 83%, GSH:GSSG reduced by 98.6% and transcriptional activation of ARE increased by up to 335%. Caspase 3/7 activity was increased by up to 37% and the viable cell population declined by up to 76%. No cellular stress responses were detected following exposure to e-cigarette AqE. The methods used were suitably sensitive to be employed for comparative studies of tobacco and nicotine products.

Adsorption and revaporisation studies of thin iodine oxide and CsI aerosol deposits from containment surface materials in LWRs

Energy Technology Data Exchange (ETDEWEB)

Tietze, S.; Foreman, M.; Ekberg, C. [Chalmers Univ. of Technology, Goeteborg (Sweden); Kaerkelae, T.; Auvinen, A.; Tapper, U.; Jokiniemi, J. [VTT Technical Research Centre of Finland, Espoo (Finland)

2013-07-15

During a severe nuclear accident released fission and radiolysis products can react with each other to form new species which might contribute to the volatile source term. Iodine will be released from UO2 fuel mainly in form as CsI aerosol particles and elemental iodine. Elemental iodine can react in gaseous phase with ozone to form solid iodine oxide aerosol particles (IOx). Within the AIAS-2 (Adsorption of Iodine Aerosols on Surfaces) project the interactions of IOx and CsI aerosols with common containment surface materials was investigated. Common surface materials in Swedish and Finnish LWRs are Teknopox Aqua V A paint films and metal surfaces such as Cu, Zn, Al and SS. Non-radioactive and {sup 131}I labelled aerosols were produced from a KI solution and ozone with a new facility designed and built at VTT Technical Research Centre of Finland. CsI aerosols were produced from a CsI solution with the same facility. A monolayer of the aerosols was deposited on the surfaces. The deposits were analysed with microscopic and spectroscopic measurement techniques to identify the chemical form of the deposits on the surfaces to identify if a chemical conversion on the different surface materials had occured. The revaporisation behaviour of the deposited aerosol particles from the different surface materials was studied under the influence of heat, humidity and gamma irradiation at Chalmers University of Technology, Sweden. Studies on the effects of humidity were performed using the FOMICAG facility, while heat and irradiation experiments were performed in a thermostated heating block and with a gammacell 22 with a dose rate of 14 kGy/h. The revaporisation losses were measured using a HPGe detector. The decomposition effect of the radiolysis product carbon monoxide was tested on IOx aerosols deposited on a glass fibre filter. Iodine oxide particles were produced at 50 deg. C, 100 deg. C and 120 deg. C and deposited on filter samples in order to study the chemical

Adsorption and revaporisation studies of thin iodine oxide and CsI aerosol deposits from containment surface materials in LWRs

International Nuclear Information System (INIS)

Tietze, S.; Foreman, M.; Ekberg, C.; Kaerkelae, T.; Auvinen, A.; Tapper, U.; Jokiniemi, J.

2013-07-01

During a severe nuclear accident released fission and radiolysis products can react with each other to form new species which might contribute to the volatile source term. Iodine will be released from UO2 fuel mainly in form as CsI aerosol particles and elemental iodine. Elemental iodine can react in gaseous phase with ozone to form solid iodine oxide aerosol particles (IOx). Within the AIAS-2 (Adsorption of Iodine Aerosols on Surfaces) project the interactions of IOx and CsI aerosols with common containment surface materials was investigated. Common surface materials in Swedish and Finnish LWRs are Teknopox Aqua V A paint films and metal surfaces such as Cu, Zn, Al and SS. Non-radioactive and 131 I labelled aerosols were produced from a KI solution and ozone with a new facility designed and built at VTT Technical Research Centre of Finland. CsI aerosols were produced from a CsI solution with the same facility. A monolayer of the aerosols was deposited on the surfaces. The deposits were analysed with microscopic and spectroscopic measurement techniques to identify the chemical form of the deposits on the surfaces to identify if a chemical conversion on the different surface materials had occured. The revaporisation behaviour of the deposited aerosol particles from the different surface materials was studied under the influence of heat, humidity and gamma irradiation at Chalmers University of Technology, Sweden. Studies on the effects of humidity were performed using the FOMICAG facility, while heat and irradiation experiments were performed in a thermostated heating block and with a gammacell 22 with a dose rate of 14 kGy/h. The revaporisation losses were measured using a HPGe detector. The decomposition effect of the radiolysis product carbon monoxide was tested on IOx aerosols deposited on a glass fibre filter. Iodine oxide particles were produced at 50 deg. C, 100 deg. C and 120 deg. C and deposited on filter samples in order to study the chemical speciation of

Secondary organic aerosols over oceans via oxidation of isoprene and monoterpenes from Arctic to Antarctic.

Science.gov (United States)

Hu, Qi-Hou; Xie, Zhou-Qing; Wang, Xin-Ming; Kang, Hui; He, Quan-Fu; Zhang, Pengfei

2013-01-01

Isoprene and monoterpenes are important precursors of secondary organic aerosols (SOA) in continents. However, their contributions to aerosols over oceans are still inconclusive. Here we analyzed SOA tracers from isoprene and monoterpenes in aerosol samples collected over oceans during the Chinese Arctic and Antarctic Research Expeditions. Combined with literature reports elsewhere, we found that the dominant tracers are the oxidation products of isoprene. The concentrations of tracers varied considerably. The mean average values were approximately one order of magnitude higher in the Northern Hemisphere than in the Southern Hemisphere. High values were generally observed in coastal regions. This phenomenon was ascribed to the outflow influence from continental sources. High levels of isoprene could emit from oceans and consequently have a significant impact on marine SOA as inferred from isoprene SOA during phytoplankton blooms, which may abruptly increase up to 95 ng/m³ in the boundary layer over remote oceans.

Chemical composition and characteristics of ambient aerosols and rainwater residues during Indian summer monsoon: Insight from aerosol mass spectrometry

Science.gov (United States)

Chakraborty, Abhishek; Gupta, Tarun; Tripathi, Sachchida N.

2016-07-01

Real time composition of non-refractory submicron aerosol (NR-PM1) is measured via Aerosol mass spectrometer (AMS) for the first time during Indian summer monsoon at Kanpur, a polluted urban location located at the heart of Indo Gangetic Plain (IGP). Submicron aerosols are found to be dominated by organics followed by nitrate. Source apportionment of organic aerosols (OA) via positive matrix factorization (PMF) revealed several types of secondary/oxidized and primary organic aerosols. On average, OA are completely dominated by oxidized OA with a very little contribution from biomass burning OA. During rain events, PM1 concentration is decreased almost by 60%, but its composition remains nearly the same. Oxidized OA showed slightly more decrease than primary OAs, probably due to their higher hygroscopicity. The presence of organo nitrates (ON) is also detected in ambient aerosols. Apart from real-time sampling, collected fog and rainwater samples were also analyzed via AMS in offline mode and in the ICP-OES (Inductively coupled plasma - Optical emission spectrometry) for elements. The presence of sea salt, organo nitrates and sulfates has been observed. Rainwater residues are also dominated by organics but their O/C ratios are 15-20% lower than the observed values for ambient OA. Alkali metals such as Ca, Na, K are found to be most abundant in the rainwater followed by Zn. Rainwater residues are also found to be much less oxidized than the aerosols present inside the fog water, indicating presence of less oxidized organics. These findings indicate that rain can act as an effective scavenger of different types of pollutants even for submicron particle range. Rainwater residues also contain organo sulfates which indicate that some portion of the dissolved aerosols has undergone aqueous processing, possibly inside the cloud. Highly oxidized and possibly hygroscopic OA during monsoon period compared to other seasons (winter, post monsoon), indicates that they can act

LMFBR source term experiments in the Fuel Aerosol Simulant Test (FAST) facility

International Nuclear Information System (INIS)

Petrykowski, J.C.; Longest, A.W.

1985-01-01

The transport of uranium dioxide (UO 2 ) aerosol through liquid sodium was studied in a series of ten experiments in the Fuel Aerosol Simulant Test (FAST) facility at Oak Ridge National Laboratory (ORNL). The experiments were designed to provide a mechanistic basis for evaluating the radiological source term associated with a postulated, energetic core disruptive accident (CDA) in a liquid metal fast breeder reactor (LMFBR). Aerosol was generated by capacitor discharge vaporization of UO 2 pellets which were submerged in a sodium pool under an argon cover gas. Measurements of the pool and cover gas pressures were used to study the transport of aerosol contained by vapor bubbles within the pool. Samples of cover gas were filtered to determine the quantity of aerosol released from the pool. The depth at which the aerosol was generated was found to be the most critical parameter affecting release. The largest release was observed in the baseline experiment where the sample was vaporized above the sodium pool. In the nine ''undersodium'' experiments aerosol was generated beneath the surface of the pool at depths varying from 30 to 1060 mm. The mass of aerosol released from the pool was found to be a very small fraction of the original specimen. It appears that the bulk of aerosol was contained by bubbles which collapsed within the pool. 18 refs., 11 figs., 4 tabs

Identification of secondary aerosol precursors emitted by an aircraft turbofan

Directory of Open Access Journals (Sweden)

D. Kılıç

2018-05-01

Full Text Available Oxidative processing of aircraft turbine-engine exhausts was studied using a potential aerosol mass (PAM chamber at different engine loads corresponding to typical flight operations. Measurements were conducted at an engine test cell. Organic gases (OGs and particle emissions pre- and post-PAM were measured. A suite of instruments, including a proton-transfer-reaction mass spectrometer (PTR-MS for OGs, a multigas analyzer for CO, CO2, NOx, and an aerosol mass spectrometer (AMS for nonrefractory particulate matter (NR-PM1 were used. Total aerosol mass was dominated by secondary aerosol formation, which was approximately 2 orders of magnitude higher than the primary aerosol. The chemical composition of both gaseous and particle emissions were also monitored at different engine loads and were thrust-dependent. At idling load (thrust 2.5–7 %, more than 90 % of the secondary particle mass was organic and could mostly be explained by the oxidation of gaseous aromatic species, e.g., benzene; toluene; xylenes; tri-, tetra-, and pentamethyl-benzene; and naphthalene. The oxygenated-aromatics, e.g., phenol, furans, were also included in this aromatic fraction and their oxidation could alone explain up to 25 % of the secondary organic particle mass at idling loads. The organic fraction decreased with thrust level, while the inorganic fraction increased. At an approximated cruise load sulfates comprised 85 % of the total secondary particle mass.

Mathematical modelling of the kinetics of aerosol oxidation of sulfur dioxide upon electron-beam purification of power-plant flue gases from nitrogen and sulfur oxides

International Nuclear Information System (INIS)

Gerasimov, G.Ya.; Gerasimova, T.S.; Fadeev, S.A.

1996-01-01

A kinetic model of SO 2 oxidation in flue gases, irradiated with accelerated electron flux is proposed. The model comprises an optimized mechanism of gas phase radiation chemical oxidation of NO and SO 2 , kinetics circuit of SO 2 and NH 3 thermal interaction, kinetic models of volumetric condensation of water and sulfuric acid vapors and liquid-phase oxidation of SO 2 in aerosol drops, produced in the course of volumetric condensation. Calculation results are in a satisfactory agreement with experimental data. (author)

A high-flow humidograph for testing the water uptake by ambient aerosol

Energy Technology Data Exchange (ETDEWEB)

Ten Brink, H.M.; Khlystov, A.; Kos, G.P.A. [ECN Fuels Conversion and Environment, Petten (Netherlands); Tuch, T. [Institut of Medical Data Management, Biometrics and Epidemiology, Ludwig-Maximilian University, Muenich (Germany); Roth, C.; Kreyling, W. [Institute for Inhalation Biology, GSF National Research Center for Environment and Health, Neuherberg/Muenich (Germany)

1999-10-01

A scanning humidograph, with an air flow rate of 0.5 m{sup 3} s{sup -1} was built to investigate the uptake of water and its effect on sizing, collection and light-scattering of ambient aerosol. The performance of the system was assessed with laboratory particles of ammonium nitrate, ammonium sulfate and sodium chloride which are the major hygroscopic components of ambient aerosol. The increase in size at the deliquescence points, which ideally is a stepwise function of relative humidity, occurs over a range of 3% RH units. This is shown to be an optimum value in a system of such large dimensions. Because of the strong temperature increase of the vapor pressure of ammonium nitrate, its evaporative loss was investigated as a function of heating/drying temperature. The loss of pure test aerosol, with a mass distribution similar to that in the ambient atmosphere, was found to be acceptable for drying temperatures of up to 40C. The sizing of deliquesced aerosol by LAS-X monitors was tested and found to be a complex function of RH. In Berner low pressure impactors growth of hygroscopic aerosol was not observed, not even at an RH approaching saturation. 21 refs.

Fractionation of sulfur isotopes during heterogeneous oxidation of SO2 on sea salt aerosol: a new tool to investigate non-sea salt sulfate production in the marine boundary layer

Science.gov (United States)

Harris, E.; Sinha, B.; Hoppe, P.; Foley, S.; Borrmann, S.

2012-05-01

The oxidation of SO2 to sulfate on sea salt aerosols in the marine environment is highly important because of its effect on the size distribution of sulfate and the potential for new particle nucleation from H2SO4 (g). However, models of the sulfur cycle are not currently able to account for the complex relationship between particle size, alkalinity, oxidation pathway and rate - which is critical as SO2 oxidation by O3 and Cl catalysis are limited by aerosol alkalinity, whereas oxidation by hypohalous acids and transition metal ions can continue at low pH once alkalinity is titrated. We have measured 34S/32S fractionation factors for SO2 oxidation in sea salt, pure water and NaOCl aerosol, as well as the pH dependency of fractionation. Oxidation of SO2 by NaOCl aerosol was extremely efficient, with a reactive uptake coefficient of ≈0.5, and produced sulfate that was enriched in 32S with αOCl = 0.9882±0.0036 at 19 °C. Oxidation on sea salt aerosol was much less efficient than on NaOCl aerosol, suggesting alkalinity was already exhausted on the short timescale of the experiments. Measurements at pH = 2.1 and 7.2 were used to calculate fractionation factors for each step from SO2(g) → multiple steps → SOOCl2-. Oxidation on sea salt aerosol resulted in a lower fractionation factor than expected for oxidation of SO32- by O3 (αseasalt = 1.0124±0.0017 at 19 °C). Comparison of the lower fractionation during oxidation on sea salt aerosol to the fractionation factor for high pH oxidation shows HOCl contributed 29% of S(IV) oxidation on sea salt in the short experimental timescale, highlighting the potential importance of hypohalous acids in the marine environment. The sulfur isotope fractionation factors measured in this study allow differentiation between the alkalinity-limited pathways - oxidation by O3 and by Cl catalysis (α34 = 1.0163±0.0018 at 19 °C in pure water or 1.0199±0.0024 at pH = 7.2) - which favour the heavy isotope, and the alkalinity non

Fractionation of sulfur isotopes during heterogeneous oxidation of SO2 on sea salt aerosol: a new tool to investigate non-sea salt sulfate production in the marine boundary layer

Directory of Open Access Journals (Sweden)

S. Borrmann

2012-05-01

Full Text Available The oxidation of SO2 to sulfate on sea salt aerosols in the marine environment is highly important because of its effect on the size distribution of sulfate and the potential for new particle nucleation from H2SO4 (g. However, models of the sulfur cycle are not currently able to account for the complex relationship between particle size, alkalinity, oxidation pathway and rate – which is critical as SO2 oxidation by O3 and Cl catalysis are limited by aerosol alkalinity, whereas oxidation by hypohalous acids and transition metal ions can continue at low pH once alkalinity is titrated. We have measured 34S/32S fractionation factors for SO2 oxidation in sea salt, pure water and NaOCl aerosol, as well as the pH dependency of fractionation. Oxidation of SO2 by NaOCl aerosol was extremely efficient, with a reactive uptake coefficient of ≈0.5, and produced sulfate that was enriched in 32S with αOCl = 0.9882±0.0036 at 19 °C. Oxidation on sea salt aerosol was much less efficient than on NaOCl aerosol, suggesting alkalinity was already exhausted on the short timescale of the experiments. Measurements at pH = 2.1 and 7.2 were used to calculate fractionation factors for each step from SO2(g → multiple steps → SOOCl2−. Oxidation on sea salt aerosol resulted in a lower fractionation factor than expected for oxidation of SO32− by O3 (αseasalt = 1.0124±0.0017 at 19 °C. Comparison of the lower fractionation during oxidation on sea salt aerosol to the fractionation factor for high pH oxidation shows HOCl contributed 29% of S(IV oxidation on sea salt in the short experimental timescale, highlighting the potential importance of hypohalous acids in the marine environment. The sulfur isotope fractionation factors measured in this study allow differentiation between the alkalinity-limited pathways – oxidation by O3 and by Cl catalysis (α34 = 1.0163±0.0018 at 19 °C in pure water or 1.0199±0.0024 at pH = 7.2 – which favour the heavy isotope, and

Photo-oxidation products of α-pinene in coarse, fine and ultrafine aerosol: A new high sensitive HPLC-MS/MS method

Science.gov (United States)

Feltracco, Matteo; Barbaro, Elena; Contini, Daniele; Zangrando, Roberta; Toscano, Giuseppa; Battistel, Dario; Barbante, Carlo; Gambaro, Andrea

2018-05-01

Oxidation products of α-pinene represent a fraction of organic matter in the environmental aerosol. α-pinene is one of most abundant monoterpenes released in the atmosphere by plants, located typically in boreal, temperate and tropical forests. This primary compound reacts with atmospheric oxidants, such as O3, O2, OH radicals and NOx, through the major tropospheric degradation pathway for many monoterpenes under typical atmospheric condition. Although several studies identified a series of by-products deriving from the α-pinene photo-oxidation in the atmosphere, such as pinic and cis-pinonic acid, the knowledge of the mechanism of this process is partially still lacking. Thus, the investigation of the distribution of these acids in the different size aerosol particles provides additional information on this regard. The aim of this study is twofold. First, we aim to improve the existing analytical methods for the determination of pinic and cis-pinonic acid in aerosol samples, especially in terms of analytical sensitivity and limits of detection (LOD) and quantification (LOQ). We even attempted to increase the knowledge of the α-pinene photo-oxidation processes by analysing, for the first time, the particle-size distribution up to nanoparticle level of pinic and cis-pinonic acid. The analysis of aerosol samples was carried out via high-performance liquid chromatography coupled to a triple quadrupole mass spectrometer. The instrumental LOD values of cis-pinonic and pinic acid are 1.6 and 1.2 ng L-1 while LOQ values are 5.4 and 4.1 ng L-1, respectively. Samples were collected by MOUDI II™ cascade impactor with twelve cut-sizes, from March to May 2016 in the urban area of Mestre-Venice (Italy). The range concentrations in the aerosol samples were from 0.1 to 0.9 ng m-3 for cis-pinonic acid and from 0.1 to 0.8 ng m-3 for pinic acid.

Oxidative potential of secondary organic aerosols produced from photooxidation of different hydrocarbons using outdoor chamber under ambient sunlight

Science.gov (United States)

Jiang, Huanhuan; Jang, Myoseon; Sabo-Attwood, Tara; Robinson, Sarah E.

2016-04-01

The oxidative potential of various secondary organic aerosols (SOA) was measured using dithiothreitol (DTT) assay to understand how organic aerosols react with cellular materials. SOA was produced via the photooxidation of four different hydrocarbons (toluene, 1,3,5-trimethylbenzene, isoprene and α-pinene) in the presence of NOx using a large outdoor photochemical smog chamber. The DTT consumption rate was normalized by the aerosol mass, which is expressed as DTTmass. Toluene SOA and isoprene SOA yielded higher DTTmass than 1,3,5-trimethylbenzene SOA or α-pinene SOA. In order to discover the correlation between the molecular structure and oxidative potential, the DTT responses of selected model compounds were also measured. Among them, conjugated aldehydes, quinones, and H2O2 showed considerable DTT response. To investigate the correlation between DTT response and cell responses in vitro, the expression of biological markers, i.e. IL-6, IL-8, and HMOX-1 were studied using small airway epithelial cells. Higher cellular expression of IL-8 was observed with toluene SOA exposure compared to 1,3,5-trimethylbenzene SOA exposure, which aligned with the results from DTT assay. Our study also suggests that within the urban atmosphere, the contribution of toluene SOA and isoprene SOA to the oxidative potential of ambient SOA will be more significant than that of α-pinene SOA.

Calibration of aerosol radiometers. Special aerosol sources

International Nuclear Information System (INIS)

Belkina, S.K.; Zalmanzon, Yu.E.; Kuznetsov, Yu.V.; Fertman, D.E.

1988-01-01

Problems of calibration of artificial aerosol radiometry and information-measurement systems of radiometer radiation control, in particular, are considered. Special aerosol source is suggested, which permits to perform certification and testing of aerosol channels of the systems in situ without the dismantling

Secondary organic aerosol formation from ambient air in an oxidation flow reactor in central Amazonia

Science.gov (United States)

Palm, Brett B.; de Sá, Suzane S.; Day, Douglas A.; Campuzano-Jost, Pedro; Hu, Weiwei; Seco, Roger; Sjostedt, Steven J.; Park, Jeong-Hoo; Guenther, Alex B.; Kim, Saewung; Brito, Joel; Wurm, Florian; Artaxo, Paulo; Thalman, Ryan; Wang, Jian; Yee, Lindsay D.; Wernis, Rebecca; Isaacman-VanWertz, Gabriel; Goldstein, Allen H.; Liu, Yingjun; Springston, Stephen R.; Souza, Rodrigo; Newburn, Matt K.; Lizabeth Alexander, M.; Martin, Scot T.; Jimenez, Jose L.

2018-01-01

Secondary organic aerosol (SOA) formation from ambient air was studied using an oxidation flow reactor (OFR) coupled to an aerosol mass spectrometer (AMS) during both the wet and dry seasons at the Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5) field campaign. Measurements were made at two sites downwind of the city of Manaus, Brazil. Ambient air was oxidized in the OFR using variable concentrations of either OH or O3, over ranges from hours to days (O3) or weeks (OH) of equivalent atmospheric aging. The amount of SOA formed in the OFR ranged from 0 to as much as 10 µg m-3, depending on the amount of SOA precursor gases in ambient air. Typically, more SOA was formed during nighttime than daytime, and more from OH than from O3 oxidation. SOA yields of individual organic precursors under OFR conditions were measured by standard addition into ambient air and were confirmed to be consistent with published environmental chamber-derived SOA yields. Positive matrix factorization of organic aerosol (OA) after OH oxidation showed formation of typical oxidized OA factors and a loss of primary OA factors as OH aging increased. After OH oxidation in the OFR, the hygroscopicity of the OA increased with increasing elemental O : C up to O : C ˜ 1.0, and then decreased as O : C increased further. Possible reasons for this decrease are discussed. The measured SOA formation was compared to the amount predicted from the concentrations of measured ambient SOA precursors and their SOA yields. While measured ambient precursors were sufficient to explain the amount of SOA formed from O3, they could only explain 10-50 % of the SOA formed from OH. This is consistent with previous OFR studies, which showed that typically unmeasured semivolatile and intermediate volatility gases (that tend to lack C = C bonds) are present in ambient air and can explain such additional SOA formation. To investigate the sources of the unmeasured SOA-forming gases during this campaign

Intercontinental transport of aerosols and photochemical oxidants from Asia and its consequences

International Nuclear Information System (INIS)

Wuebbles, Donald J.; Lei, Hang; Lin, Jintai

2007-01-01

The intercontinental transport of aerosols and photochemical oxidants from Asia is a crucial issue for air quality concerns in countries downwind of the significant emissions and concentrations of pollutants occurring in this important region of the world. Since the lifetimes of some important pollutants are long enough to be transported over long distance in the troposphere, regional control strategies for air pollution in downwind countries might be ineffective without considering the effects of long-range transport of pollutants from Asia. Field campaigns provide strong evidence for the intercontinental transport of Asian pollutants. They, together with ground-based observations and model simulations, show that the air quality over parts of North America is being affected by the pollutants transported from Asia. This paper examines the current understanding of the intercontinental transport of gases and aerosols from Asia and resulting effects on air quality, and on the regional and global climate system. - Air quality over parts of North America is being affected by pollutants transported from Asia

Aerosol studies

International Nuclear Information System (INIS)

Cristy, G.A.; Fish, M.E.

1978-01-01

As part of the continuing studies of the effects of very severe reactor accidents, an effort was made to develop, test, and improve simple, effective, and inexpensive methods by which the average citizen, using only materials readily available, could protect his residence, himself, and his family from injury by toxic aerosols. The methods for protection against radioactive aerosols should be equally effective against a clandestine biological attack by terrorists. The results of the tests to date are limited to showing that spores of the harmless bacterium, bacillus globegii (BG), can be used as a simulant for the radioactive aerosols. An aerosol generator of Lauterbach type was developed which will produce an essentially monodisperse aerosol at the rate of 10 9 spores/min. Analytical techniques have been established which give reproducible results. Preliminary field tests have been conducted to check out the components of the system. Preliminary tests of protective devices, such as ordinary vacuum sweepers, have given protection factors of over 1000

Field and Laboratory Studies of Atmospheric Organic Aerosol

Science.gov (United States)

Coggon, Matthew Mitchell

This thesis is the culmination of field and laboratory studies aimed at assessing processes that affect the composition and distribution of atmospheric organic aerosol. An emphasis is placed on measurements conducted using compact and high-resolution Aerodyne Aerosol Mass Spectrometers (AMS). The first three chapters summarize results from aircraft campaigns designed to evaluate anthropogenic and biogenic impacts on marine aerosol and clouds off the coast of California. Subsequent chapters describe laboratory studies intended to evaluate gas and particle-phase mechanisms of organic aerosol oxidation. The 2013 Nucleation in California Experiment (NiCE) was a campaign designed to study environments impacted by nucleated and/or freshly formed aerosol particles. Terrestrial biogenic aerosol with > 85% organic mass was observed to reside in the free troposphere above marine stratocumulus. This biogenic organic aerosol (BOA) originated from the Northwestern United States and was transported to the marine atmosphere during periodic cloud-clearing events. Spectra recorded by a cloud condensation nuclei counter demonstrated that BOA is CCN active. BOA enhancements at latitudes north of San Francisco, CA coincided with enhanced cloud water concentrations of organic species such as acetate and formate. Airborne measurements conducted during the 2011 Eastern Pacific Emitted Aerosol Cloud Experiment (E-PEACE) were aimed at evaluating the contribution of ship emissions to the properties of marine aerosol and clouds off the coast of central California. In one study, analysis of organic aerosol mass spectra during periods of enhanced shipping activity yielded unique tracers indicative of cloud-processed ship emissions (m/z 42 and 99). The variation of their organic fraction (f42 and f 99) was found to coincide with periods of heavy (f 42 > 0.15; f99 > 0.04), moderate (0.05 controlled organic plume emitted from the R/V Point Sur. Under sunny conditions, nucleated particles composed

Estimation of Uncertainty in Aerosol Concentration Measured by Aerosol Sampling System

Energy Technology Data Exchange (ETDEWEB)

Lee, Jong Chan; Song, Yong Jae; Jung, Woo Young; Lee, Hyun Chul; Kim, Gyu Tae; Lee, Doo Yong [FNC Technology Co., Yongin (Korea, Republic of)

2016-10-15

FNC Technology Co., Ltd has been developed test facilities for the aerosol generation, mixing, sampling and measurement under high pressure and high temperature conditions. The aerosol generation system is connected to the aerosol mixing system which injects SiO{sub 2}/ethanol mixture. In the sampling system, glass fiber membrane filter has been used to measure average mass concentration. Based on the experimental results using main carrier gas of steam and air mixture, the uncertainty estimation of the sampled aerosol concentration was performed by applying Gaussian error propagation law. FNC Technology Co., Ltd. has been developed the experimental facilities for the aerosol measurement under high pressure and high temperature. The purpose of the tests is to develop commercial test module for aerosol generation, mixing and sampling system applicable to environmental industry and safety related system in nuclear power plant. For the uncertainty calculation of aerosol concentration, the value of the sampled aerosol concentration is not measured directly, but must be calculated from other quantities. The uncertainty of the sampled aerosol concentration is a function of flow rates of air and steam, sampled mass, sampling time, condensed steam mass and its absolute errors. These variables propagate to the combination of variables in the function. Using operating parameters and its single errors from the aerosol test cases performed at FNC, the uncertainty of aerosol concentration evaluated by Gaussian error propagation law is less than 1%. The results of uncertainty estimation in the aerosol sampling system will be utilized for the system performance data.

PHEBUS on-line aerosol monitor development test program

International Nuclear Information System (INIS)

Sprenger, M.H.; Pentecost, C.G.

1992-03-01

EG ampersand G Idaho, Inc. developed an on-line aerosol monitor (OLAM) for the French PHEBUS Fission Product Project. Part of the development was to manufacture and test an OLAM prototype. This report presents the results of the testing which determined the mechanical integrity of the monitor at operating temperature and pressure and performed a preliminary test of the optical system. A series of twenty different tests was conducted during the prototype testing sequence. Since no leaks were detected, the OLAM demonstrated that it could provide a pressure boundary at required test conditions. The optical and electrical system also proved its integrity by exceeding the design requirement of less than 105 optical signal drift during an actual two-hour test sequence

Development and calibration of an on-line aerosol monitor for PHEBUS test FPT1

International Nuclear Information System (INIS)

O'Brien, J.E.; Carmack, W.J.; Sprenger, M.H.; Thurston, G.C.; Hunt, J.L.

1994-10-01

An on-line aerosol monitor (OLAM2) has been developed and tested for PHEBUS test FPT1. OLAM2 utilizes new detachable fiber optic cables and sapphire light pipes for light transmission between the OLAM and the electronics. This light transmission system was tested and found to provide better signal-to-noise performance than was achieved with the continuous fibers used for test FPT0. An additional advantage of the detachable fiber/light pipe system is ease of installation. Aerosol testing (OLAM calibration) was performed in order to verify adequate signal-to-noise performance of the new fiber optic system over the specified operating conditions and to check the quantitative light attenuation measurements against theoretical predictions. Results of the testing indicated that light extinction measurements obtained during Phebus tests could be used to estimate aerosol volume concentrations, if diamond window fouling can be avoided. OLAM2 was also subjected to a proof pressure test and a long-term thermal stability test. These tests verified the mechanical and thermal integrity of the OLAM within design specifications. Long-term output signal stability was also verified with the system maintained at design temperature and half-design pressure

Relationship between chemical composition and oxidative potential of secondary organic aerosol from polycyclic aromatic hydrocarbons

Science.gov (United States)

Wang, Shunyao; Ye, Jianhuai; Soong, Ronald; Wu, Bing; Yu, Legeng; Simpson, André J.; Chan, Arthur W. H.

2018-03-01

Owing to the complex nature and dynamic behaviors of secondary organic aerosol (SOA), its ability to cause oxidative stress (known as oxidative potential, or OP) and adverse health outcomes remains poorly understood. In this work, we probed the linkages between the chemical composition of SOA and its OP, and investigated impacts from various SOA evolution pathways, including atmospheric oligomerization, heterogeneous oxidation, and mixing with metal. SOA formed from photooxidation of the two most common polycyclic aromatic hydrocarbons (naphthalene and phenanthrene) were studied as model systems. OP was evaluated using the dithiothreitol (DTT) assay. The oligomer-rich fraction separated by liquid chromatography dominates DTT activity in both SOA systems (52 ± 10 % for naphthalene SOA (NSOA), and 56 ± 5 % for phenanthrene SOA (PSOA)). Heterogeneous ozonolysis of NSOA was found to enhance its OP, which is consistent with the trend observed in selected individual oxidation products. DTT activities from redox-active organic compounds and metals were found to be not additive. When mixing with highly redox-active metal (Cu), OP of the mixture decreased significantly for 1,2-naphthoquinone (42 ± 7 %), 2,3-dihydroxynaphthalene (35 ± 1 %), NSOA (50 ± 6 %), and PSOA (43 ± 4 %). Evidence from proton nuclear magnetic resonance (1H NMR) spectroscopy illustrates that such OP reduction upon mixing can be ascribed to metal-organic binding interactions. Our results highlight the role of aerosol chemical composition under atmospheric aging processes in determining the OP of SOA, which is needed for more accurate and explicit prediction of the toxicological impacts from particulate matter.

The inhalation of insoluble iron oxide particles in the sub-micron ranges. Part II - Plutonium-237 labelled aerosols

International Nuclear Information System (INIS)

Waite, D.A.; Ramsden, D.

1971-10-01

The results of a series of inhalation studies using iron oxide particles in the size range 0.1 to 0.3 um (count median diameter) are described. In this series the aerosols were labelled with plutonium 237. In vivo detection, excretion analysis and crude location studies were obtainable and the results compared to the earlier studies using chromium 51 labelled aerosols. Plutonium 237 can be considered as a simulator for plutonium 239 and attempts are made to extrapolate the results to the problem of the estimation of plutonium 239 in the human lung. (author)

Secondary organic aerosol formation from ambient air in an oxidation flow reactor in central Amazonia

Directory of Open Access Journals (Sweden)

B. B. Palm

2018-01-01

Full Text Available Secondary organic aerosol (SOA formation from ambient air was studied using an oxidation flow reactor (OFR coupled to an aerosol mass spectrometer (AMS during both the wet and dry seasons at the Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5 field campaign. Measurements were made at two sites downwind of the city of Manaus, Brazil. Ambient air was oxidized in the OFR using variable concentrations of either OH or O3, over ranges from hours to days (O3 or weeks (OH of equivalent atmospheric aging. The amount of SOA formed in the OFR ranged from 0 to as much as 10 µg m−3, depending on the amount of SOA precursor gases in ambient air. Typically, more SOA was formed during nighttime than daytime, and more from OH than from O3 oxidation. SOA yields of individual organic precursors under OFR conditions were measured by standard addition into ambient air and were confirmed to be consistent with published environmental chamber-derived SOA yields. Positive matrix factorization of organic aerosol (OA after OH oxidation showed formation of typical oxidized OA factors and a loss of primary OA factors as OH aging increased. After OH oxidation in the OFR, the hygroscopicity of the OA increased with increasing elemental O : C up to O : C ∼ 1.0, and then decreased as O : C increased further. Possible reasons for this decrease are discussed. The measured SOA formation was compared to the amount predicted from the concentrations of measured ambient SOA precursors and their SOA yields. While measured ambient precursors were sufficient to explain the amount of SOA formed from O3, they could only explain 10–50 % of the SOA formed from OH. This is consistent with previous OFR studies, which showed that typically unmeasured semivolatile and intermediate volatility gases (that tend to lack C = C bonds are present in ambient air and can explain such additional SOA formation. To investigate the sources of the

Characterization of selenium in ambient aerosols and primary emission sources.

Science.gov (United States)

De Santiago, Arlette; Longo, Amelia F; Ingall, Ellery D; Diaz, Julia M; King, Laura E; Lai, Barry; Weber, Rodney J; Russell, Armistead G; Oakes, Michelle

2014-08-19

Atmospheric selenium (Se) in aerosols was investigated using X-ray absorption near-edge structure (XANES) spectroscopy and X-ray fluorescence (XRF) microscopy. These techniques were used to determine the oxidation state and elemental associations of Se in common primary emission sources and ambient aerosols collected from the greater Atlanta area. In the majority of ambient aerosol and primary emission source samples, the spectroscopic patterns as well as the absence of elemental correlations suggest Se is in an elemental, organic, or oxide form. XRF microscopy revealed numerous Se-rich particles, or hotspots, accounting on average for ∼16% of the total Se in ambient aerosols. Hotspots contained primarily Se(0)/Se(-II). However, larger, bulk spectroscopic characterizations revealed Se(IV) as the dominant oxidation state in ambient aerosol, followed by Se(0)/Se(-II) and Se(VI). Se(IV) was the only observed oxidation state in gasoline, diesel, and coal fly ash, while biomass burning contained a combination of Se(0)/Se(-II) and Se(IV). Although the majority of Se in aerosols was in the most toxic form, the Se concentration is well below the California Environmental Protection Agency chronic exposure limit (∼20000 ng/m(3)).

Characterization of urban aerosol using aerosol mass spectrometry and proton nuclear magnetic resonance spectroscopy

Science.gov (United States)

Cleveland, M. J.; Ziemba, L. D.; Griffin, R. J.; Dibb, J. E.; Anderson, C. H.; Lefer, B.; Rappenglück, B.

2012-07-01

Particulate matter was measured during August and September of 2006 in Houston as part of the Texas Air Quality Study II Radical and Aerosol Measurement Project. Aerosol size and composition were determined using an Aerodyne quadrupole aerosol mass spectrometer. Aerosol was dominated by sulfate (4.1 ± 2.6 μg m-3) and organic material (5.5 ± 4.0 μg m-3), with contributions of organic material from both primary (˜32%) and secondary (˜68%) sources. Secondary organic aerosol appears to be formed locally. In addition, 29 aerosol filter samples were analyzed using proton nuclear magnetic resonance (1H NMR) spectroscopy to determine relative concentrations of organic functional groups. Houston aerosols are less oxidized than those observed elsewhere, with smaller relative contributions of carbon-oxygen double bonds. These particles do not fit 1H NMR source apportionment fingerprints for identification of secondary, marine, and biomass burning organic aerosol, suggesting that a new fingerprint for highly urbanized and industrially influenced locations be established.

Enhanced Iron Solubility at Low pH in Global Aerosols

Directory of Open Access Journals (Sweden)

Ellery D. Ingall

2018-05-01

Full Text Available The composition and oxidation state of aerosol iron were examined using synchrotron-based iron near-edge X-ray absorption spectroscopy. By combining synchrotron-based techniques with water leachate analysis, impacts of oxidation state and mineralogy on aerosol iron solubility were assessed for samples taken from multiple locations in the Southern and the Atlantic Oceans; and also from Noida (India, Bermuda, and the Eastern Mediterranean (Crete. These sampling locations capture iron-containing aerosols from different source regions with varying marine, mineral dust, and anthropogenic influences. Across all locations, pH had the dominating influence on aerosol iron solubility. When aerosol samples were approximately neutral pH, iron solubility was on average 3.4%; when samples were below pH 4, the iron solubility increased to 35%. This observed aerosol iron solubility profile is consistent with thermodynamic predictions for the solubility of Fe(III oxides, the major iron containing phase in the aerosol samples. Source regions and transport paths were also important factors affecting iron solubility, as samples originating from or passing over populated regions tended to contain more soluble iron. Although the acidity appears to affect aerosol iron solubility globally, a direct relationship for all samples is confounded by factors such as anthropogenic influence, aerosol buffer capacity, mineralogy and physical processes.

Processing of Unsaturated Organic Acid Aerosols by Ozone

Science.gov (United States)

Aloisio, S.; Donaldson, D. J.; Eliason, T. L.; Cziczo, D.; Vaida, V.

2002-05-01

We present results of in-situ studies of the oxidative "processing" of organic aerosols composed of unsaturated organic compounds. Aerosol samples of 2-octenoic acid and undecylenic acid were exposed to approx. 10 mbar ozone in a room temperature, atmospheric pressure flow tube reactor. In-situ spectroscopic probing of the reaction mixture, as well as GC-MS analysis of the flow tube effluent, shows evidence of efficient oxidation of double bonds in the organic species, with production of gas-phase and aerosol phase ozonolysis products.

Finish-Kazakhstan cooperation on an aerosols sampling - testing of a new methods for nuclear monitoring improvement

International Nuclear Information System (INIS)

Tarvajnen, M.; Akhmetov, M.A.; Ptitskaya, L.D.; Osintsev, A.Yu.; Zhantikin, T.M.; Eligbaeva, G.

2001-01-01

The aerosols sampling is the powerful method of air radioactivity monitoring both the natural and artificial origin. Up to the today the IAEA does not engage of aerosols sampling study. To study of possibility of this method examination for radiation monitoring - the state authorities of Finland and the Republic of Kazakhstan - Department of Radiation and Nuclear Safety (Stuck) and Kazakhstan Atomic Energy Committee - jointly carried out the field tests in Kazakhstan. The test was began in the Kurchatov in April 2000 - at the desire of IAEA working team on Iraq - close to former Semipalatinsk test site and was ended in Astana in August of 2001. The main aim of the field test was study of possibility and appropriateness of concept and technology of aerosols sampling developed for the complete condition of environment. In the paper the role of participating sides in the field test and main results and conclusions are discussed as well. The gained experience will allow developing the method aerosols sampling for IAEA international safeguard measures strengthening application

Ozonolysis and Subsequent Photolysis of unsaturated organic molecules: Model Systems for Photochemical Aging of Organic Aerosol Particles

Science.gov (United States)

Park, J.; Gomez, A. L.; Walser, M. L.; Lin, A.; Nizkorodov, S. A.

2005-12-01

Chemical and photochemical aging of organic species adsorbed on aerosol particle surfaces is believed to have a significant effect on cloud condensation properties of atmospheric aerosols. Ozone initiated oxidation reactions of thin films of undecylenic acid and alkene-terminated self assembled monolayers (SAMs) on SiO2 surface were investigated using a combination of spectroscopic and mass spectrometric techniques. Photolysis of the oxidized film in the tropospheric actinic region (λ>290 nm) readily produces formaldehyde and formic acid as gas-phase products. Photodissociation action spectra of the oxidized film suggest that organic peroxides are responsible for the enhanced photochemical activity. The presence of peroxides in the oxidized sample was confirmed by mass-spectrometric analysis and by an iodometric test. Significant polymerization resulting from secondary reactions of Criegee radicals during ozonolysis of the film is also observed. The reaction mechanism and its implications for photochemical aging of atmospheric aerosol particles will be discussed.

Relative importance of nitrate and sulfate aerosol production mechanisms in urban atmospheres

International Nuclear Information System (INIS)

Middleton, P.; Kiang, C.S.

1979-01-01

The relative importance of the various sulfate and nitrate aerosol production mechanisms is calculated for different atmospheric conditions. The calculation scheme used to determine the rates of nitrate and sulfate production, based on the concept that vapor transfer to the aerosols and nitrate and sulfate formation within the aerosols are coupled kinetic processes, considers sulfate formation by ozone and hydrogen peroxide oxidation and catalytic oxidation in the presence of soot, iron and manganese of sulfite solutions and sulfuric acid condensation and nitrate formation by the liquid-phase oxidation of dissolved nitrogen oxides for different initial gas concentrations and particle compositions and sizes. It is found that sulfate production is higher under daytime conditions, primarily proceeding by mechanisms involving sulfuric acid and hydrogen peroxide, while at night oxidation processes on the surface of the aerosol film are more important. Nitrate tends to decrease nighttime sulfate production due to an increase in aerosol acidity and nitrate production is found to be higher under nighttime conditions and in the winter

Indium oxide deposition on glass by aerosol pyrolysis (Pyrosol (R) process)

International Nuclear Information System (INIS)

Blandenet, G.; Lagarde, Y.; Spitz, J.

1975-01-01

The pyrosol (R) process involves the pyrolysis of an aerosol generated by ultrasonic nebulisation from a solution of organic or inorganic compounds. This technique was used to deposit transparent n-conducting indium oxide films on glass. The electrical and optical properties of these films were studied as a function of the deposition temperature and doping (using tin or fluorine). A deposition temperature of 480 deg C and a Sn/In ratio of about 5% gave the best results. In this case, the transmission in the visible range was 92%, the infrared reflection 84% and the electrical resistivity 1.7x10 -4 ohm.cm [fr

Flame generation of sodium chloride aerosol for filter testing

International Nuclear Information System (INIS)

Edwards, J.; Kinnear, D.I.

1975-01-01

A generator for sodium chloride aerosol is described, which when used in conjunction with a sensitive portable sodium flame detector unit, will permit the in-place testing of large filter installations having air throughputs up to about 80,000 m 3 /h, at penetrations down to at least 0.005 percent. (U.S.)

Development and first application of an Aerosol Collection Module (ACM) for quasi online compound specific aerosol measurements

Science.gov (United States)

Hohaus, Thorsten; Kiendler-Scharr, Astrid; Trimborn, Dagmar; Jayne, John; Wahner, Andreas; Worsnop, Doug

2010-05-01

Atmospheric aerosols influence climate and human health on regional and global scales (IPCC, 2007). In many environments organics are a major fraction of the aerosol influencing its properties. Due to the huge variety of organic compounds present in atmospheric aerosol current measurement techniques are far from providing a full speciation of organic aerosol (Hallquist et al., 2009). The development of new techniques for compound specific measurements with high time resolution is a timely issue in organic aerosol research. Here we present first laboratory characterisations of an aerosol collection module (ACM) which was developed to allow for the sampling and transfer of atmospheric PM1 aerosol. The system consists of an aerodynamic lens system focussing particles on a beam. This beam is directed to a 3.4 mm in diameter surface which is cooled to -30 °C with liquid nitrogen. After collection the aerosol sample can be evaporated from the surface by heating it to up to 270 °C. The sample is transferred through a 60cm long line with a carrier gas. In order to test the ACM for linearity and sensitivity we combined it with a GC-MS system. The tests were performed with octadecane aerosol. The octadecane mass as measured with the ACM-GC-MS was compared versus the mass as calculated from SMPS derived total volume. The data correlate well (R2 0.99, slope of linear fit 1.1) indicating 100 % collection efficiency. From 150 °C to 270 °C no effect of desorption temperature on transfer efficiency could be observed. The ACM-GC-MS system was proven to be linear over the mass range 2-100 ng and has a detection limit of ~ 2 ng. First experiments applying the ACM-GC-MS system were conducted at the Jülich Aerosol Chamber. Secondary organic aerosol (SOA) was formed from ozonolysis of 600 ppbv of b-pinene. The major oxidation product nopinone was detected in the aerosol and could be shown to decrease from 2 % of the total aerosol to 0.5 % of the aerosol over the 48 hours of

Assessing the impact of anthropogenic pollution on isoprene-derived secondary organic aerosol formation in PM2.5 collected from the Birmingham, Alabama, ground site during the 2013 Southern Oxidant and Aerosol Study

Directory of Open Access Journals (Sweden)

W. Rattanavaraha

2016-04-01

Full Text Available In the southeastern US, substantial emissions of isoprene from deciduous trees undergo atmospheric oxidation to form secondary organic aerosol (SOA that contributes to fine particulate matter (PM2.5. Laboratory studies have revealed that anthropogenic pollutants, such as sulfur dioxide (SO2, oxides of nitrogen (NOx, and aerosol acidity, can enhance SOA formation from the hydroxyl radical (OH-initiated oxidation of isoprene; however, the mechanisms by which specific pollutants enhance isoprene SOA in ambient PM2.5 remain unclear. As one aspect of an investigation to examine how anthropogenic pollutants influence isoprene-derived SOA formation, high-volume PM2.5 filter samples were collected at the Birmingham, Alabama (BHM, ground site during the 2013 Southern Oxidant and Aerosol Study (SOAS. Sample extracts were analyzed by gas chromatography–electron ionization-mass spectrometry (GC/EI-MS with prior trimethylsilylation and ultra performance liquid chromatography coupled to electrospray ionization high-resolution quadrupole time-of-flight mass spectrometry (UPLC/ESI-HR-QTOFMS to identify known isoprene SOA tracers. Tracers quantified using both surrogate and authentic standards were compared with collocated gas- and particle-phase data as well as meteorological data provided by the Southeastern Aerosol Research and Characterization (SEARCH network to assess the impact of anthropogenic pollution on isoprene-derived SOA formation. Results of this study reveal that isoprene-derived SOA tracers contribute a substantial mass fraction of organic matter (OM ( ∼  7 to  ∼  20 %. Isoprene-derived SOA tracers correlated with sulfate (SO42− (r2 = 0.34, n = 117 but not with NOx. Moderate correlations between methacrylic acid epoxide and hydroxymethyl-methyl-α-lactone (together abbreviated MAE/HMML-derived SOA tracers with nitrate radical production (P[NO3] (r2 = 0.57, n = 40 were observed during nighttime, suggesting a

DSMC multicomponent aerosol dynamics: Sampling algorithms and aerosol processes

Science.gov (United States)

Palaniswaamy, Geethpriya

The post-accident nuclear reactor primary and containment environments can be characterized by high temperatures and pressures, and fission products and nuclear aerosols. These aerosols evolve via natural transport processes as well as under the influence of engineered safety features. These aerosols can be hazardous and may pose risk to the public if released into the environment. Computations of their evolution, movement and distribution involve the study of various processes such as coagulation, deposition, condensation, etc., and are influenced by factors such as particle shape, charge, radioactivity and spatial inhomogeneity. These many factors make the numerical study of nuclear aerosol evolution computationally very complicated. The focus of this research is on the use of the Direct Simulation Monte Carlo (DSMC) technique to elucidate the role of various phenomena that influence the nuclear aerosol evolution. In this research, several aerosol processes such as coagulation, deposition, condensation, and source reinforcement are explored for a multi-component, aerosol dynamics problem in a spatially homogeneous medium. Among the various sampling algorithms explored the Metropolis sampling algorithm was found to be effective and fast. Several test problems and test cases are simulated using the DSMC technique. The DSMC results obtained are verified against the analytical and sectional results for appropriate test problems. Results show that the assumption of a single mean density is not appropriate due to the complicated effect of component densities on the aerosol processes. The methods developed and the insights gained will also be helpful in future research on the challenges associated with the description of fission product and aerosol releases.

Dissolution of LMFBR fuel-sodium aerosols

International Nuclear Information System (INIS)

Allen, M.D.; Moss, O.R.

1979-01-01

Plutonium dioxide, normally insoluble in biological fluids, becomes much more soluble when mixed with sodium as the aerosol is formed. Sodium-fuel aerosols are approximately 20 times less soluble in simulated lung fluid than in distilled water. Solubility of sodium-fuel aerosols increases when Na 2 CO 3 are added to the distilled-water dissolution fluid. Mixed-oxide fuel aerosols without sodium present are relatively insoluble in distilled water, simulated lung fluid, and distilled water with Na 2 CO 3 and NaHCO 3 added

Filter-based Aerosol Measurement Experiments using Spherical Aerosol Particles under High Temperature and High Pressure

Energy Technology Data Exchange (ETDEWEB)

Lee, Jong Chan; Jung, Woo Young; Lee, Hyun Chul; Lee, Doo Young [FNC TECH., Yongin (Korea, Republic of)

2016-05-15

Optical Particle Counter (OPC) is used to provide real-time measurement of aerosol concentration and size distribution. Glass fiber membrane filter also be used to measure average mass concentration. Three tests (MTA-1, 2 and 3) have been conducted to study thermal-hydraulic effect, a filtering tendency at given SiO{sub 2} particles. Based on the experimental results, the experiment will be carried out further with a main carrier gas of steam and different aerosol size. The test results will provide representative behavior of the aerosols under various conditions. The aim of the tests, MTA 1, 2 and 3, are to be able to 1) establish the test manuals for aerosol generation, mixing, sampling and measurement system, which defines aerosol preparation, calibration, operating and evaluation method under high pressure and high temperature 2) develop commercial aerosol test modules applicable to the thermal power plant, environmental industry, automobile exhaust gas, chemical plant, HVAC system including nuclear power plant. Based on the test results, sampled aerosol particles in the filter indicate that important parameters affecting aerosol behavior aerosols are 1) system temperature to keep above a evaporation temperature of ethanol and 2) aerosol losses due to the settling by ethanol liquid droplet.

Secondary organic aerosol formation and composition from the photo-oxidation of methyl chavicol (estragole)

Science.gov (United States)

Pereira, K. L.; Hamilton, J. F.; Rickard, A. R.; Bloss, W. J.; Alam, M. S.; Camredon, M.; Muñoz, A.; Vázquez, M.; Borrás, E.; Ródenas, M.

2014-06-01

The increasing demand for palm oil for uses in biofuel and food products is leading to rapid expansion of oil palm agriculture. Methyl chavicol (also known as estragole and 1-allyl-4-methoxybenzene) is an oxygenated biogenic volatile organic compound (VOC) that was recently identified as the main floral emission from an oil palm plantation in Malaysian Borneo. The emissions of methyl chavicol observed may impact regional atmospheric chemistry, but little is known of its ability to form secondary organic aerosol (SOA). The photo-oxidation of methyl chavicol was investigated at the European Photoreactor chamber as a part of the atmospheric chemistry of methyl chavicol (ATMECH) project. Aerosol samples were collected using a particle into liquid sampler (PILS) and analysed offline using an extensive range of instruments including; high-performance liquid chromatography mass spectrometry (HPLC-ITMS), high-performance liquid chromatography quadrupole time-of-flight mass spectrometry (HPLC-QTOFMS) and Fourier transform ion cyclotron resonance mass spectrometry (FTICR-MS). The SOA yield was determined as 18 and 29% for an initial VOC mixing ratio of 212 and 460 ppbv (parts per billion by volume) respectively; using a VOC:NOx ratio of ~5:1. In total, 59 SOA compounds were observed and the structures of 10 compounds have been identified using high-resolution tandem mass spectrometry. The addition of hydroxyl and/or nitro-functional groups to the aromatic ring appears to be an important mechanistic pathway for aerosol formation. This results in the formation of compounds with both low volatility and high O:C ratios, where functionalisation rather than fragmentation is mainly observed as a result of the stability of the ring. The SOA species observed can be characterised as semi-volatile to low-volatility oxygenated organic aerosol (SVOOA and LVOOA) components and therefore may be important in aerosol formation and growth.

Impact of OH Heterogenous Oxidation on the Evolution of Brown Carbon Aerosol Optical Properties

Science.gov (United States)

Schnitzler, E.; Abbatt, J.

2017-12-01

The effects of varying relative humidity (RH) on the evolution of brown carbon (BrC) optical properties induced by heterogeneous OH oxidation were investigated in a series of photooxidation chamber experiments. A BrC surrogate was generated from aqueous 1,3-dihydroxybenzene (10 mM) and H2O2 (10 mM) exposed to >300 nm radiation, atomized, passed through a series of trace gas denuders, and injected into the chamber, which was conditioned to about 10 or 60% RH. Following aerosol injection, H2O2 was continuously bubbled into the chamber; an hour later, the chamber was irradiated with black-lights (UV-B) to produce OH. Before irradiation, aerosol absorption and scattering at 405 nm, measured using a photoacoustic spectrometer, decreased due only to deposition and dilution, and single scattering albedo (SSA) was relatively steady. In the presence of gas-phase OH, absorption first increased, despite continued particle losses, and SSA decreased. Subsequently, absorption decreased faster than scattering, and SSA increased uniformly. At 60% RH, colour enhancement, likely associated with functionalization, was greatest after only minutes of reaction. In contrast, at 10% RH, peak colour enhancement occurred after about two hours of reaction, indicating that the decrease in RH and the attendant increase in particle viscosity significantly impeded heterogeneous OH oxidation of the BrC surrogate.

DTPA therapy of lung contaminations: testing a self contained aerosol generator

International Nuclear Information System (INIS)

Ducousso, R.; Pasquier, C.

1975-01-01

It has been shown how much the effectiveness of DTPA therapy of respiratory contamination decreased when the delay of administration of the product increased. Moreover, the effectiveness of local administration of the chelating agent as aerosol has been widely recognized. Owing to both the therapeutic urgency and the local administration, an individual pocket apparatus allowing emergency DTPA inhalation, on the spot of the accident was tried. A turbo-inhalator sold for the administration of an anti-asthmatic powder was tested, using DTPA powder inhaled by a volunteer previously contaminated by a 140 LaCl 3 aerosol [fr

OH-initiated Aging of Biomass Burning Aerosol during FIREX

Science.gov (United States)

Lim, C. Y.; Hagan, D. H.; Cappa, C. D.; Kroll, J. H.; Coggon, M.; Koss, A.; Sekimoto, K.; De Gouw, J. A.; Warneke, C.

2017-12-01

Biomass burning emissions represent a major source of fine particulate matter to the atmosphere, and this source will likely become increasingly important in the future due to changes in the Earth's climate. Understanding the effects that increased fire emissions have on both air quality and climate requires understanding the composition of the particles emitted, since chemical and physical composition directly impact important particle properties such as absorptivity, toxicity, and cloud condensation nuclei activity. However, the composition of biomass burning particles in the atmosphere is dynamic, as the particles are subject to the condensation of low-volatility vapors and reaction with oxidants such as the hydroxyl radical (OH) during transport. Here we present a series of laboratory chamber experiments on the OH-initiated aging of biomass burning aerosol performed at the Fire Sciences Laboratory in Missoula, MT as part of the Fire Influences on Regional and Global Environments Experiment (FIREX) campaign. We describe the evolution of biomass burning aerosol produced from a variety of fuels operating the chamber in both particle-only and gas + particle mode, focusing on changes to the organic composition. In particle-only mode, gas-phase biomass burning emissions are removed before oxidation to focus on heterogeneous oxidation, while gas + particle mode includes both heterogeneous oxidation and condensation of oxidized volatile organic compounds onto the particles (secondary organic aerosol formation). Variability in fuels and burning conditions lead to differences in aerosol loading and secondary aerosol production, but in all cases aging results in a significant and rapid increases in the carbon oxidation state of the particles.

Size distributions of aerosols produced from substitute materials by the Laskin cold DOP aerosol generator

International Nuclear Information System (INIS)

Hinds, W.; Macher, J.; First, M.W.

1981-01-01

Test aerosols of di(2-ethylhexyl)phthalate (DOP) produced by Laskin nozzle aerosol generators are widely used for in-place filter testing and respirator fit testing. Concern for the health effects of this material has led to a search for substitute materials for test aerosols. Aerosols were generated with a Laskin generator and diluted 6000-fold with clean air. Size distributions were measured for DOP, di(2-ethylhexyl)sebecate, polyethylene glycol, mineral oil, and corn oil aerosols with a PMS ASAS-X optical particle counter. Distributions were slightly bimodal with count median diameters from 0.22 to 0.30 μm. Size distributions varied little with aerosol material, operating pressure, or liquid level. Mineral oil and corn oil gave the best agreement with the DOP size distribution

Development and testing of an aerosol-stratus cloud parameterization scheme for middle and high latitudes

Energy Technology Data Exchange (ETDEWEB)

Olsson, P.Q.; Meyers, M.P.; Kreidenweis, S.; Cotton, W.R. [Colorado State Univ., Fort Collins, CO (United States)

1996-04-01

The aim of this new project is to develop an aerosol/cloud microphysics parameterization of mixed-phase stratus and boundary layer clouds. Our approach is to create, test, and implement a bulk-microphysics/aerosol model using data from Atmospheric Radiation Measurement (ARM) Cloud and Radiation Testbed (CART) sites and large-eddy simulation (LES) explicit bin-resolving aerosol/microphysics models. The primary objectives of this work are twofold. First, we need the prediction of number concentrations of activated aerosol which are transferred to the droplet spectrum, so that the aerosol population directly affects the cloud formation and microphysics. Second, we plan to couple the aerosol model to the gas and aqueous-chemistry module that will drive the aerosol formation and growth. We begin by exploring the feasibility of performing cloud-resolving simulations of Arctic stratus clouds over the North Slope CART site. These simulations using Colorado State University`s regional atmospheric modeling system (RAMS) will be useful in designing the structure of the cloud-resolving model and in interpreting data acquired at the North Slope site.

Aerosol detection efficiency in inductively coupled plasma mass spectrometry

Science.gov (United States)

Hubbard, Joshua A.; Zigmond, Joseph A.

2016-05-01

An electrostatic size classification technique was used to segregate particles of known composition prior to being injected into an inductively coupled plasma mass spectrometer (ICP-MS). Size-segregated particles were counted with a condensation nuclei counter as well as sampled with an ICP-MS. By injecting particles of known size, composition, and aerosol concentration into the ICP-MS, efficiencies of the order of magnitude aerosol detection were calculated, and the particle size dependencies for volatile and refractory species were quantified. Similar to laser ablation ICP-MS, aerosol detection efficiency was defined as the rate at which atoms were detected in the ICP-MS normalized by the rate at which atoms were injected in the form of particles. This method adds valuable insight into the development of technologies like laser ablation ICP-MS where aerosol particles (of relatively unknown size and gas concentration) are generated during ablation and then transported into the plasma of an ICP-MS. In this study, we characterized aerosol detection efficiencies of volatile species gold and silver along with refractory species aluminum oxide, cerium oxide, and yttrium oxide. Aerosols were generated with electrical mobility diameters ranging from 100 to 1000 nm. In general, it was observed that refractory species had lower aerosol detection efficiencies than volatile species, and there were strong dependencies on particle size and plasma torch residence time. Volatile species showed a distinct transition point at which aerosol detection efficiency began decreasing with increasing particle size. This critical diameter indicated the largest particle size for which complete particle detection should be expected and agreed with theories published in other works. Aerosol detection efficiencies also displayed power law dependencies on particle size. Aerosol detection efficiencies ranged from 10- 5 to 10- 11. Free molecular heat and mass transfer theory was applied, but

Probing functional groups at the gas-aerosol interface using heterogeneous titration reactions: a tool for predicting aerosol health effects?

Science.gov (United States)

Setyan, Ari; Sauvain, Jean-Jacques; Guillemin, Michel; Riediker, Michael; Demirdjian, Benjamin; Rossi, Michel J

2010-12-17

The complex chemical and physical nature of combustion and secondary organic aerosols (SOAs) in general precludes the complete characterization of both bulk and interfacial components. The bulk composition reveals the history of the growth process and therefore the source region, whereas the interface controls--to a large extent--the interaction with gases, biological membranes, and solid supports. We summarize the development of a soft interrogation technique, using heterogeneous chemistry, for the interfacial functional groups of selected probe gases [N(CH(3))(3), NH(2)OH, CF(3)COOH, HCl, O(3), NO(2)] of different reactivity. The technique reveals the identity and density of surface functional groups. Examples include acidic and basic sites, olefinic and polycyclic aromatic hydrocarbon (PAH) sites, and partially and completely oxidized surface sites. We report on the surface composition and oxidation states of laboratory-generated aerosols and of aerosols sampled in several bus depots. In the latter case, the biomarker 8-hydroxy-2'-deoxyguanosine, signaling oxidative stress caused by aerosol exposure, was isolated. The increase in biomarker levels over a working day is correlated with the surface density N(i)(O3) of olefinic and/or PAH sites obtained from O(3) uptakes as well as with the initial uptake coefficient, γ(0), of five probe gases used in the field. This correlation with γ(0) suggests the idea of competing pathways occurring at the interface of the aerosol particles between the generation of reactive oxygen species (ROS) responsible for oxidative stress and cellular antioxidants.

Local transport of vertically- and horizontally-emitted sodium oxide aerosols

International Nuclear Information System (INIS)

Fields, D.E.; Miller, C.W.; Cooper, A.C.

1986-01-01

Liquid-metal cooled breeder reactors are expected to use large quantities of sodium or sodium-potassium alloy, and evaluation of the possible consequences of a liquid-metal fire, henceforth referred to as a sodium fire, is an important consideration. Of particular interest is the sodium aerosol concentration at the air intake ports that are used for reactor cooling, and which might suffer restricted flow under high aerosol concentrations. We have devised and applied a methodology for estimating the concentration of aerosols released vertically and horizontally from building surfaces and monitored at other building surface points. We have used this methodology to make calculations that indicate the time-development of aerosol build-up, and the maximum aerosol concentrations, at air intake ports. Building wake effects, momentum-driven plume rise, and density-driven plume rise are considered

Local transport of vertically and horizontally emitted sodium oxide aerosols

International Nuclear Information System (INIS)

Fields, D.E.; Miller, C.W.; Cooper, A.C.

1986-01-01

Liquid-metal-cooled breeder reactors are expected to use large quantities of sodium or sodium-potassium alloy, and evaluation of the possible consequences of a liquid-metal fire, henceforth referred to as a sodium fire, is an important consideration. Of particular interest is the sodium aerosol concentration at the air intake ports that are used for reactor cooling, and which might suffer restricted flow under high aerosol concentrations. The authors have devised and applied a methodology for estimating the concentration of aerosols released vertically and horizontally from building surfaces and monitored at other building surface points. This methodology has been used to make calculations that indicate the time development of aerosol buildup, and the maximum aerosol concentration, at air intake ports. Building wake effects, momentum-driven plume rise, and density-driven plume rise are considered

Factor analysis of combined organic and inorganic aerosol mass spectra from high resolution aerosol mass spectrometer measurements

Directory of Open Access Journals (Sweden)

Y. L. Sun

2012-09-01

Full Text Available Positive matrix factorization (PMF was applied to the merged high resolution mass spectra of organic and inorganic aerosols from aerosol mass spectrometer (AMS measurements to investigate the sources and evolution processes of submicron aerosols in New York City in summer 2009. This new approach is able to study the distribution of organic and inorganic species in different types of aerosols, the acidity of organic aerosol (OA factors, and the fragment ion patterns related to photochemical processing. In this study, PMF analysis of the unified AMS spectral matrix resolved 8 factors. The hydrocarbon-like OA (HOA and cooking OA (COA factors contain negligible amounts of inorganic species. The two factors that are primarily ammonium sulfate (SO₄-OA and ammonium nitrate (NO₃-OA, respectively, are overall neutralized. Among all OA factors the organic fraction of SO₄-OA shows the highest degree of oxidation (O/C = 0.69. Two semi-volatile oxygenated OA (OOA factors, i.e., a less oxidized (LO-OOA and a more oxidized (MO-OOA, were also identified. MO-OOA represents local photochemical products with a diurnal profile exhibiting a pronounced noon peak, consistent with those of formaldehyde (HCHO and O_x(= O₃ + NO₂. The NO⁺/NO₂⁺ ion ratio in MO-OOA is much higher than that in NO₃-OA and in pure ammonium nitrate, indicating the formation of organic nitrates. The nitrogen-enriched OA (NOA factor contains ~25% of acidic inorganic salts, suggesting the formation of secondary OA via acid-base reactions of amines. The size distributions of OA factors derived from the size-resolved mass spectra show distinct diurnal evolving behaviors but overall a progressing evolution from smaller to larger particle mode as the oxidation degree of OA increases. Our results demonstrate that PMF analysis of the unified aerosol mass spectral matrix which contains both

Monoterpene oxidation in an oxidative flow reactor: SOA yields and the relationship between bulk gas-phase properties and organic aerosol growth

Science.gov (United States)

Friedman, B.; Link, M.; Farmer, D.

2016-12-01

We use an oxidative flow reactor (OFR) to determine the secondary organic aerosol (SOA) yields of five monoterpenes (alpha-pinene, beta-pinene, limonene, sabinene, and terpinolene) at a range of OH exposures. These OH exposures correspond to aging timescales of a few hours to seven days. We further determine how SOA yields of beta-pinene and alpha-pinene vary as a function of seed particle type (organic vs. inorganic) and seed particle mass concentration. We hypothesize that the monoterpene structure largely accounts for the observed variance in SOA yields for the different monoterpenes. We also use high-resolution time-of-flight chemical ionization mass spectrometry to calculate the bulk gas-phase properties (O:C and H:C) of the monoterpene oxidation systems as a function of oxidant concentrations. Bulk gas-phase properties can be compared to the SOA yields to assess the capability of the precursor gas-phase species to inform the SOA yields of each monoterpene oxidation system. We find that the extent of oxygenated precursor gas-phase species corresponds to SOA yield.

A new method for in-situ filter testing using pulses of aerosol and photometric detection with computer control

International Nuclear Information System (INIS)

Marshall, P.R.C.; Bosley, R.B.

1993-01-01

This paper describes a new technique, developed at the Harwell Laboratory, for the in-situ testing of High Efficiency Particulate Air (HEPA) filters using multiple pulses of test aerosol. The pulse test apparatus consists of a modified forward light scattering photometer coupled to a portable micro-computer fitted with an external data acquisition and control card. The micro-computer switches an aerosol generator on and off via an external relay driver unit. Using this apparatus the filter bank is challenged by a small number of equal length, constant concentration, pulses of aerosol at timed intervals. The aerosol concentration data upstream of the filter bank is logged, to disk, by the computer. The process is then repeated for the downstream concentration with the photometer gain increased to give maximum sensitivity. The collected data is analysed using a computer spread-sheet package; the recorded aerosol pulses are combined, integrated and the background data subtracted; the downstream data is then divided by the upstream pulse data to give the filter penetration. Using this technique the sensitivity of the in-situ filter test has been greatly improved, penetrations approaching 10 -5 % can now be measured, allowing HEPA filters mounted in series to be successfully tested. In addition, filter loading is reduced considerably

Effects of SO2 oxidation on ambient aerosol growth in water and ethanol vapours

Directory of Open Access Journals (Sweden)

T. Petäjä

2005-01-01

Full Text Available Hygroscopicity (i.e. water vapour affinity of atmospheric aerosol particles is one of the key factors in defining their impacts on climate. Condensation of sulphuric acid onto less hygroscopic particles is expected to increase their hygrocopicity and hence their cloud condensation nuclei formation potential. In this study, differences in the hygroscopic and ethanol uptake properties of ultrafine aerosol particles in the Arctic air masses with a different exposure to anthropogenic sulfur pollution were examined. The main discovery was that Aitken mode particles having been exposed to polluted air were more hygroscopic and less soluble to ethanol than after transport in clean air. This aging process was attributed to sulphur dioxide oxidation and subsequent condensation during the transport of these particle to our measurement site. The hygroscopicity of nucleation mode aerosol particles, on the other hand, was approximately the same in all the cases, being indicative of a relatively similar chemical composition despite the differences in air mass transport routes. These particles had also been produced closer to the observation site typically 3–8 h prior to sampling. Apparently, these particles did not have an opportunity to accumulate sulphuric acid on their way to the site, but instead their chemical composition (hygroscopicity and ethanol solubility resembled that of particles produced in the local or semi-regional ambient conditions.

A global perspective on aerosol from low-volatility organic compounds

Directory of Open Access Journals (Sweden)

H. O. T. Pye

2010-05-01

Full Text Available Global production of organic aerosol from primary emissions of semivolatile (SVOCs and intermediate (IVOCs volatility organic compounds is estimated using the global chemical transport model, GEOS-Chem. SVOC oxidation is predicted to be a larger global source of net aerosol production than oxidation of traditional parent hydrocarbons (terpenes, isoprene, and aromatics. Using a prescribed rate constant and reduction in volatility for atmospheric oxidation, the yield of aerosol from SVOCs is predicted to be about 75% on a global, annually-averaged basis. For IVOCs, the use of a naphthalene-like surrogate with different high-NO_x and low-NO_x parameterizations produces a global aerosol yield of about 30%, or roughly 5 Tg/yr of aerosol. Estimates of the total global organic aerosol source presented here range between 60 and 100 Tg/yr. This range reflects uncertainty in the parameters for SVOC volatility, SVOC oxidation, SVOC emissions, and IVOC emissions, as well as wet deposition. The highest estimates result if SVOC emissions are significantly underestimated (by more than a factor of 2 or if wet deposition of the gas-phase semivolatile species is less effective than previous estimates. A significant increase in SVOC emissions, a reduction of the volatility of the SVOC emissions, or an increase in the enthalpy of vaporization of the organic aerosol all lead to an appreciable reduction of prediction/measurement discrepancy. In addition, if current primary organic aerosol (POA inventories capture only about one-half of the SVOC emission and the Henrys Law coefficient for oxidized semivolatiles is on the order of 10³ M/atm, a global estimate of OA production is not inconsistent with the top-down estimate of 140 Tg/yr by (Goldstein and Galbally, 2007. Additional information is needed to constrain the emissions and treatment of SVOCs and IVOCs, which have traditionally not been included in models.

Heterogeneous Oxidation of Atmospheric Organic Aerosol: Kinetics of Changes to the Amount and Oxidation State of Particle-Phase Organic Carbon.

Science.gov (United States)

Kroll, Jesse H; Lim, Christopher Y; Kessler, Sean H; Wilson, Kevin R

2015-11-05

Atmospheric oxidation reactions are known to affect the chemical composition of organic aerosol (OA) particles over timescales of several days, but the details of such oxidative aging reactions are poorly understood. In this study we examine the rates and products of a key class of aging reaction, the heterogeneous oxidation of particle-phase organic species by the gas-phase hydroxyl radical (OH). We compile and reanalyze a number of previous studies from our laboratories involving the oxidation of single-component organic particles. All kinetic and product data are described on a common basis, enabling a straightforward comparison among different chemical systems and experimental conditions. Oxidation chemistry is described in terms of changes to key ensemble properties of the OA, rather than to its detailed molecular composition, focusing on two quantities in particular, the amount and the oxidation state of the particle-phase carbon. Heterogeneous oxidation increases the oxidation state of particulate carbon, with the rate of increase determined by the detailed chemical mechanism. At the same time, the amount of particle-phase carbon decreases with oxidation, due to fragmentation (C-C scission) reactions that form small, volatile products that escape to the gas phase. In contrast to the oxidation state increase, the rate of carbon loss is nearly uniform among most systems studied. Extrapolation of these results to atmospheric conditions indicates that heterogeneous oxidation can have a substantial effect on the amount and composition of atmospheric OA over timescales of several days, a prediction that is broadly in line with available measurements of OA evolution over such long timescales. In particular, 3-13% of particle-phase carbon is lost to the gas phase after one week of heterogeneous oxidation. Our results indicate that oxidative aging represents an important sink for particulate organic carbon, and more generally that fragmentation reactions play a major

Cobalt-60 oxide aerosols: methods of production and short-term retention and distribution kinetics in the beagle dog

International Nuclear Information System (INIS)

Barnes, J.E.; Kanapilly, G.M.; Newton, G.J.

1976-01-01

Cobalt-60 has been used extensively in nuclear applications and has been considered for use in nuclear auxiliary power devices. The most common chemical form used is the oxide. This study of the retention and distribution of two differnt exoides of cobalt when administered by inhalation was conducted to assess the potential inhalation hazard associated with its use. Cobaltosic oxide (Co 3 O 4 ) was formed by passing a cobalt nitrate aerosol through a heating column at 850 0 C before delivery to the dog. Cobaltous oxide (CoO) was formed by raising the heating column temperature to 1400 0 C. Three beagle dogs were exposed to 60 Co 3 O 4 and sacrificed singly at 8, 64 and 128 days. Three beagle dogs were exposed to 60 CoO and sacrificed at 8, 16 and 64 days after exposure. Whole-body retention patterns showed that 60 CoO left the body with a shorter effective half-life than 60 Co 3 O 4 . The concentration of 60 Co detected in the blood was at least an order of magnitude higher in the dogs exposed to 60 CoO than in the dogs exposed to 60 Co 3 O 4 . Cobalt-60 translocated from the lung accumulated predominantly in the kidney, liver, skeleton and cartilagenous structures such as the trachea. Higher concentrations were reached earlier in the dogs exposed to 60 CoO. After early fecal excretion of material deposited in the upper respiratory tract, excretion was greatest via the urine. The higher solubility of the 60 CoO formed at 1400 0 C relative to 60 Co 3 O 4 formed at 850 0 C is noteworthy considering that generally aerosols formed at higher temperatures are more insoluble than aerosols formed at lower temperatures. (author)

Field characterization of plutonium aerosols in mixed-oxide fuel fabrication

International Nuclear Information System (INIS)

Newton, G.J.; Teague, S.V.; Yeh, H.C.

1976-01-01

Nuclear reactor fuel pellets of PuO 2 and UO 2 are fabricated within safety enclosures at Babcock and Wilcox's Parker Township Site near Apolla, Pa. Nineteen sample runs were taken from within glove boxes of aerosols formed during powder comminution and blending. Eight sampling runs were also taken of a centerless grinding operation during routine industrial operations. A small seven-stage cascade impactor and the Lovelace Aerosol Particle Separator (LAPS) were used to determine aerodynamic size distribution and gross alpha aerosol concentrations. The potential toxicity of inhaled plutonium originating in the nuclear fuel cycle following accidental releases of these aerosols and possible inhalation by industrial workers is considered

Analyses of CsI aerosol deposition tests in WIND project with ART and VICTORIA codes

International Nuclear Information System (INIS)

Yuchi, Y.; Shibazaki, H.; Kudo, T.

2000-01-01

Deposition behavior of cesium iodide (CsI) was analyzed with ART and VICTORIA-92 codes for a test of the aerosol re-vaporization test series performed in WIND project at JAERI. In the test analyzed, CsI aerosol was injected into piping of test section where metaboric acid (HBO 2 ) was placed in advance on the floor area. It was confirmed in the present analysis that similar results on the CsI deposition were obtained between ART and VICTORIA when influences of chemical interactions were negligibly small. The analysis with VICTORIA agreed satisfactorily with the test results in analytical cases that cesium metaborate (CsBO 2 ) was injected into the test section instead of CsI to simulate the pre-existence of HBO 2 effect. (author)

In-cloud oxidation of SO2 as deduced from trace elements in aerosol and precipitation

International Nuclear Information System (INIS)

Heaton, R.; Rahn, K.A.

1985-01-01

During the past year, the authors have developed and begun to apply a sampling and analytical technique for precipitation which can measure nearly as many elements (30-40) as in the parent aerosol. Rain is collected in a polyethylene bag mounted directly under a simple polyethylene funnel. Typically, up to 500 ml are accumulated; sampling begins only after the rain has started. Snow is scooped into the same kind of bag during or shortly after the event; up to 500 ml are accumulated by repeated sampling and melting in the laboratory. The bags are sealed, frozen overnight, then opened and freeze-dried until all the ice has disappeared. The bag and its contents are then analyzed by instrumental neutron activation at the Rhode Island Nuclear Science Center. Sulfate is determined from a small aliquot of the precipitation removed before it is frozen. For comparison, aerosol samples taken before, during, and after the event are analyzed similarly. The principal goal of this research is to develop procedures for applying the University of Rhode Island's regional elemental tracer system, originally to use the patter of trace elements in precipitation to determine the fraction of the sulfate which has been produced by in-cloud oxidation of SO 2 , as opposed to direct scavenging of sulfate from aerosol

Diffusive deposition of aerosols in Phebus containment during FPT-2 test

International Nuclear Information System (INIS)

Kontautas, A.; Urbonavicius, E.

2012-01-01

At present the lumped-parameter codes is the main tool to investigate the complex response of the containment of Nuclear Power Plant in case of an accident. Continuous development and validation of the codes is required to perform realistic investigation of the processes that determine the possible source term of radioactive products to the environment. Validation of the codes is based on the comparison of the calculated results with the measurements performed in experimental facilities. The most extensive experimental program to investigate fission product release from the molten fuel, transport through the cooling circuit and deposition in the containment is performed in PHEBUS test facility. Test FPT-2 performed in this facility is considered for analysis of processes taking place in containment. Earlier performed investigations using COCOSYS code showed that the code could be successfully used for analysis of thermal-hydraulic processes and deposition of aerosols, but there was also noticed that diffusive deposition on the vertical walls does not fit well with the measured results. In the CPA module of ASTEC code there is implemented different model for diffusive deposition, therefore the PHEBUS containment model was transferred from COCOSYS code to ASTEC-CPA to investigate the influence of the diffusive deposition modelling. Analysis was performed using PHEBUS containment model of 16 nodes. The calculated thermal-hydraulic parameters are in good agreement with measured results, which gives basis for realistic simulation of aerosol transport and deposition processes. Performed investigations showed that diffusive deposition model has influence on the aerosol deposition distribution on different surfaces in the test facility. (authors)

Experimental determination of the partitioning coefficient and volatility of important BVOC oxidation products using the Aerosol Collection Module (ACM) coupled to a PTR-ToF-MS

Science.gov (United States)

Gkatzelis, G.; Hohaus, T.; Tillmann, R.; Schmitt, S. H.; Yu, Z.; Schlag, P.; Wegener, R.; Kaminski, M.; Kiendler-Scharr, A.

2015-12-01

Atmospheric aerosol can alter the Earth's radiative budget and global climate but can also affect human health. A dominant contributor to the submicrometer particulate matter (PM) is organic aerosol (OA). OA can be either directly emitted through e.g. combustion processes (primary OA) or formed through the oxidation of organic gases (secondary organic aerosol, SOA). A detailed understanding of SOA formation is of importance as it constitutes a major contribution to the total OA. The partitioning between the gas and particle phase as well as the volatility of individual components of SOA is yet poorly understood adding uncertainties and thus complicating climate modelling. In this work, a new experimental methodology was used for compound-specific analysis of organic aerosol. The Aerosol Collection Module (ACM) is a newly developed instrument that deploys an aerodynamic lens to separate the gas and particle phase of an aerosol. The particle phase is directed to a cooled sampling surface. After collection particles are thermally desorbed and transferred to a detector for further analysis. In the present work, the ACM was coupled to a Proton Transfer Reaction-Time of Flight-Mass Spectrometer (PTR-ToF-MS) to detect and quantify organic compounds partitioning between the gas and particle phase. This experimental approach was used in a set of experiments at the atmosphere simulation chamber SAPHIR to investigate SOA formation. Ozone oxidation with subsequent photochemical aging of β-pinene, limonene and real plant emissions from Pinus sylvestris (Scots pine) were studied. Simultaneous measurement of the gas and particle phase using the ACM-PTR-ToF-MS allows to report partitioning coefficients of important BVOC oxidation products. Additionally, volatility trends and changes of the SOA with photochemical aging are investigated and compared for all systems studied.

Black carbon aerosol mixing state, organic aerosols and aerosol optical properties over the UK

Science.gov (United States)

McMeeking, G. R.; Morgan, W. T.; Flynn, M.; Highwood, E. J.; Turnbull, K.; Haywood, J.; Coe, H.

2011-05-01

Black carbon (BC) aerosols absorb sunlight thereby leading to a positive radiative forcing and a warming of climate and can also impact human health through their impact on the respiratory system. The state of mixing of BC with other aerosol species, particularly the degree of internal/external mixing, has been highlighted as a major uncertainty in assessing its radiative forcing and hence its climate impact, but few in situ observations of mixing state exist. We present airborne single particle soot photometer (SP2) measurements of refractory BC (rBC) mass concentrations and mixing state coupled with aerosol composition and optical properties measured in urban plumes and regional pollution over the UK. All data were obtained using instrumentation flown on the UK's BAe-146-301 large Atmospheric Research Aircraft (ARA) operated by the Facility for Airborne Atmospheric Measurements (FAAM). We measured sub-micron aerosol composition using an aerosol mass spectrometer (AMS) and used positive matrix factorization to separate hydrocarbon-like (HOA) and oxygenated organic aerosols (OOA). We found a higher number fraction of thickly coated rBC particles in air masses with large OOA relative to HOA, higher ozone-to-nitrogen oxides (NOx) ratios and large concentrations of total sub-micron aerosol mass relative to rBC mass concentrations. The more ozone- and OOA-rich air masses were associated with transport from continental Europe, while plumes from UK cities had higher HOA and NOx and fewer thickly coated rBC particles. We did not observe any significant change in the rBC mass absorption efficiency calculated from rBC mass and light absorption coefficients measured by a particle soot absorption photometer despite observing significant changes in aerosol composition and rBC mixing state. The contributions of light scattering and absorption to total extinction (quantified by the single scattering albedo; SSA) did change for different air masses, with lower SSA observed in

An SOA model for toluene oxidation in the presence of inorganic aerosols.

Science.gov (United States)

Cao, Gang; Jang, Myoseon

2010-01-15

A predictive model for secondary organic aerosol (SOA) formation including both partitioning and heterogeneous reactions is explored for the SOA produced from the oxidation of toluene in the presence of inorganic seed aerosols. The predictive SOA model comprises the explicit gas-phase chemistry of toluene, gas-particle partitioning, and heterogeneous chemistry. The resulting products from the explicit gas phase chemistry are lumped into several classes of chemical species based on their vapor pressure and reactivity for heterogeneous reactions. Both the gas-particle partitioning coefficient and the heterogeneous reaction rate constant of each lumped gas-phase product are theoretically determined using group contribution and molecular structure-reactivity. In the SOA model, the predictive SOA mass is decoupled into partitioning (OM(P)) and heterogeneous aerosol production (OM(H)). OM(P) is estimated from the SOA partitioning model developed by Schell et al. (J. Geophys. Res. 2001, 106, 28275-28293 ) that has been used in a regional air quality model (CMAQ 4.7). OM(H) is predicted from the heterogeneous SOA model developed by Jang et al. (Environ. Sci. Technol. 2006, 40, 3013-3022 ). The SOA model is evaluated using a number of the experimental SOA data that are generated in a 2 m(3) indoor Teflon film chamber under various experimental conditions (e.g., humidity, inorganic seed compositions, NO(x) concentrations). The SOA model reasonably predicts not only the gas-phase chemistry, such as the ozone formation, the conversion of NO to NO(2), and the toluene decay, but also the SOA production. The model predicted that the OM(H) fraction of the total toluene SOA mass increases as NO(x) concentrations decrease: 0.73-0.83 at low NO(x) levels and 0.17-0.47 at middle and high NO(x) levels for SOA experiments with high initial toluene concentrations. Our study also finds a significant increase in the OM(H) mass fraction in the SOA generated with low initial toluene

Speciation of Fe in ambient aerosol and cloudwater

Energy Technology Data Exchange (ETDEWEB)

Siefert, Ronald Lyn [California Inst. of Technology (CalTech), Pasadena, CA (United States)

1996-08-15

Atmospheric iron (Fe) is thought to play an important role in cloudwater chemistry (e.g., S(IV) oxidation, oxidant production, etc.), and is also an important source of Fe to certain regions of the worlds oceans where Fe is believed to be a rate-limiting nutrient for primary productivity. This thesis focuses on understanding the chemistry, speciation and abundance of Fe in cloudwater and aerosol in the troposphere, through observations of Fe speciation in the cloudwater and aerosol samples collected over the continental United States and the Arabian Sea. Different chemical species of atmospheric Fe were measured in aerosol and cloudwater samples to help assess the role of Fe in cloudwater chemistry.

Aerosolization and Atmospheric Transformation of Engineered Nanoparticles

Science.gov (United States)

Tiwari, Andrea J.

While research on the environmental impacts of engineered nanoparticles (ENPs) is growing, the potential for them to be chemically transformed in the atmosphere has been largely ignored. The overall objective of this work was to assess the atmospheric transformation of carbonaceous nanoparticles (CNPs). The research focuses on C60 fullerene because it is an important member of the carbonaceous nanoparticle (CNP) family and is used in a wide variety of applications. The first specific objective was to review the potential of atmospheric transformations to alter the environmental impacts of CNPs. We described atmospheric processes that were likely to physically or chemically alter aerosolized CNPs and demonstrated their relevance to CNP behavior and toxicity in the aqueous and terrestrial environment. In order to investigate the transformations of CNP aerosols under controlled conditions, we developed an aerosolization technique that produces nano-scale aerosols without using solvents, which can alter the surface chemistry of the aerosols. We demonstrated the technique with carbonaceous (C60) and metal oxide (TiO2, CeO2) nanoparticle powders. All resulting aerosols exhibited unimodal size distributions and mode particle diameters below 100 nm. We used the new aerosolization technique to investigate the reaction between aerosolized C60 and atmospherically realistic levels of ozone (O3) in terms of reaction products, reaction rate, and oxidative stress potential. We identified C60O, C60O2, and C60O3 as products of the C60-O3 reaction. We demonstrated that the oxidative stress potential of C 60 may be enhanced by exposure to O3. We found the pseudo-first order reaction rate to be 9 x 10-6 to 2 x 10 -5 s-1, which is several orders of magnitude lower than the rate for several PAH species under comparable conditions. This research has demonstrated that a thorough understanding of atmospheric chemistry of ENPs is critical for accurate prediction of their environmental

Chemical, physical, and optical evolution of biomass burning aerosols: a case study

Science.gov (United States)

Adler, G.; Flores, J. M.; Abo Riziq, A.; Borrmann, S.; Rudich, Y.

2011-02-01

In-situ chemical composition measurements of ambient aerosols have been used for characterizing the evolution of submicron aerosols from a large anthropogenic biomass burning (BB) event in Israel. A high resolution Time of Flight Aerosol Mass Spectrometer (HR-RES-TOF-AMS) was used to follow the chemical evolution of BB aerosols during a night-long, extensive nationwide wood burning event and during the following day. While these types of extensive BB events are not common in this region, burning of agricultural waste is a common practice. The aging process of the BB aerosols was followed through their chemical, physical and optical properties. Mass spectrometric analysis of the aerosol organic component showed that aerosol aging is characterized by shifting from less oxidized fresh BB aerosols to more oxidized aerosols. Evidence for aerosol aging during the day following the BB event was indicated by an increase in the organic mass, its oxidation state, the total aerosol concentration, and a shift in the modal particle diameter. The effective broadband refractive index (EBRI) was derived using a white light optical particle counter (WELAS). The average EBRI for a mixed population of aerosols dominated by open fires was m = 1.53(±0.03) + 0.07i(±0.03), during the smoldering phase of the fires we found the EBRI to be m = 1.54(±0.01) + 0.04i(±0.01) compared to m = 1.49(±0.01) + 0.02i(±0.01) of the aged aerosols during the following day. This change indicates a decrease in the overall aerosol absorption and scattering. Elevated levels of particulate Polycyclic Aromatic Hydrocarbons (PAHs) were detected during the entire event, which suggest possible implications for human health during such extensive event.

SECONDARY ORGANIC AEROSOL FORMATION FROM THE OXIDATION OF AROMATIC HYDROCARBONS IN THE PRESENCE OF DRY SUBMICRON AMMONIUM SULFATE AEROSOL

Science.gov (United States)

A laboratory study was conducted to examine formation of secondary organic aerosols. A smog chamber system was developed for studying gas-aerosol interactions in a dynamic flow reactor. These experiments were conducted to investigate the fate of gas and aerosol phase compounds ...

Performance of multiple HEPA filters against plutonium aerosols

International Nuclear Information System (INIS)

Gonzales, M.; Elder, J.; Ettinger, H.

1975-01-01

Performance of multiple stages of High Efficiency Particulate Air (HEPA) filters against aerosols similar to those produced by plutonium processing facilities has been verified as part of an experimental program. A system of three HEPA filters in series was tested against 238 PuO 2 aerosol concentrations as high as 3.3 x 10 10 d/s-m 3 . An air nebulization aerosol generation system, using ball milled plutonium oxide suspended in water, provided test aerosols with size characteristics similar to those defined by a field sampling program at several different AEC plutonium processing facilities. Aerosols have been produced ranging from 0.22 μm activity median aerodynamic diameter (amad) to 1.6 μm amad. The smaller size distributions yield 10 to 30 percent of the total activity in the less than 0.22 μm size range allowing efficiency measurement as a function of size for the first two HEPA filters in series. The low level of activity on the sampler downstream of the third HEPA filter (approximately 0.01 c/s) precludes aerosol size characterization downstream of this filter. For the first two HEPA filters, overall efficiency, and efficiency as a function of size, exceeds 99.98 percent including the <0.12 μm and the 0.12 to 0.22 μm size intervals. Efficiency of the third HEPA filter is somewhat lower with an overall average efficiency of 99.8 percent and an apparent minimum efficiency of 99.5 percent. This apparently lower efficiency is an artifact due to the low level of activity on the sampler downstream of HEPA No. 3 and the variations due to counting statistics. Recent runs with higher concentrations, thereby improving statistical variations, show efficiencies well within minimum requirements. (U.S.)

Current status of sodium fire and aerosol research in Japan

International Nuclear Information System (INIS)

Himeno, Yoshiaki

1989-01-01

State-of-the-art of the research and development related to sodium fire and aerosol behaviour is presented. This paper covers the Japanese work on sodium leak, leak detector, sodium oxidation and combustion, sodium aerosol release, fire mitigation, reliabilities of the electrical instruments and the reactor components under the sodium aerosols suspended atmosphere, aerosol plugging in a leak path, and the computer codes are presented. (author)

The composition and variability of atmospheric aerosol over Southeast Asia during 2008

Directory of Open Access Journals (Sweden)

W. Trivitayanurak

2012-01-01

Full Text Available We use a nested version of the GEOS-Chem global 3-D chemistry transport model to better understand the composition and variation of aerosol over Borneo and the broader Southeast Asian region in conjunction with aircraft and satellite observations. Our focus on Southeast Asia reflects the importance of this region as a source of reactive organic gases and aerosols from natural forests, biomass burning, and food and fuel crops. We particularly focus on July 2008 when the UK BAe-146 research aircraft was deployed over northern Malaysian Borneo as part of the ACES/OP3 measurement campaign. During July 2008 we find using the model that Borneo (defined as Borneo Island and the surrounding Indonesian islands was a net exporter of primary organic aerosol (42 kT and black carbon aerosol (11 kT. We find only 13% of volatile organic compound oxidation products partition to secondary organic aerosol (SOA, with Borneo being a net exporter of SOA (15 kT. SOA represents approximately 19% of the total organic aerosol over the region. Sulphate is mainly from aqueous-phase oxidation (68%, with smaller contributions from gas-phase oxidation (15% and advection into the regions (14%. We find that there is a large source of sea salt, as expected, but this largely deposits within the region; we find that dust aerosol plays only a relatively small role in the aerosol burden. In contrast to coincident surface measurements over Northern Borneo that find a pristine environment with evidence for substantial biogenic SOA formation we find that the free troposphere is influenced by biomass burning aerosol transported from the northwest of the Island and further afield. We find several transport events during July 2008 over Borneo associated with elevated aerosol concentrations, none of which coincide with the aircraft flights. We use MODIS aerosol optical depths (AOD data and the model to put the July campaign into a longer temporal perspective. We find that Borneo is where

The composition and variability of atmospheric aerosol over Southeast Asia during 2008

Science.gov (United States)

Trivitayanurak, W.; Palmer, P. I.; Barkley, M. P.; Robinson, N. H.; Coe, H.; Oram, D. E.

2012-01-01

We use a nested version of the GEOS-Chem global 3-D chemistry transport model to better understand the composition and variation of aerosol over Borneo and the broader Southeast Asian region in conjunction with aircraft and satellite observations. Our focus on Southeast Asia reflects the importance of this region as a source of reactive organic gases and aerosols from natural forests, biomass burning, and food and fuel crops. We particularly focus on July 2008 when the UK BAe-146 research aircraft was deployed over northern Malaysian Borneo as part of the ACES/OP3 measurement campaign. During July 2008 we find using the model that Borneo (defined as Borneo Island and the surrounding Indonesian islands) was a net exporter of primary organic aerosol (42 kT) and black carbon aerosol (11 kT). We find only 13% of volatile organic compound oxidation products partition to secondary organic aerosol (SOA), with Borneo being a net exporter of SOA (15 kT). SOA represents approximately 19% of the total organic aerosol over the region. Sulphate is mainly from aqueous-phase oxidation (68%), with smaller contributions from gas-phase oxidation (15%) and advection into the regions (14%). We find that there is a large source of sea salt, as expected, but this largely deposits within the region; we find that dust aerosol plays only a relatively small role in the aerosol burden. In contrast to coincident surface measurements over Northern Borneo that find a pristine environment with evidence for substantial biogenic SOA formation we find that the free troposphere is influenced by biomass burning aerosol transported from the northwest of the Island and further afield. We find several transport events during July 2008 over Borneo associated with elevated aerosol concentrations, none of which coincide with the aircraft flights. We use MODIS aerosol optical depths (AOD) data and the model to put the July campaign into a longer temporal perspective. We find that Borneo is where the model

Black carbon aerosol mixing state, organic aerosols and aerosol optical properties over the United Kingdom

Science.gov (United States)

McMeeking, G. R.; Morgan, W. T.; Flynn, M.; Highwood, E. J.; Turnbull, K.; Haywood, J.; Coe, H.

2011-09-01

Black carbon (BC) aerosols absorb sunlight thereby leading to a positive radiative forcing and a warming of climate and can also impact human health through their impact on the respiratory system. The state of mixing of BC with other aerosol species, particularly the degree of internal/external mixing, has been highlighted as a major uncertainty in assessing its radiative forcing and hence its climate impact, but few in situ observations of mixing state exist. We present airborne single particle soot photometer (SP2) measurements of refractory BC (rBC) mass concentrations and mixing state coupled with aerosol composition and optical properties measured in urban plumes and regional pollution over the United Kingdom. All data were obtained using instrumentation flown on the UK's BAe-146-301 large Atmospheric Research Aircraft (ARA) operated by the Facility for Airborne Atmospheric Measurements (FAAM). We measured sub-micron aerosol composition using an aerosol mass spectrometer (AMS) and used positive matrix factorization to separate hydrocarbon-like (HOA) and oxygenated organic aerosols (OOA). We found a higher number fraction of thickly coated rBC particles in air masses with large OOA relative to HOA, higher ozone-to-nitrogen oxides (NOx) ratios and large concentrations of total sub-micron aerosol mass relative to rBC mass concentrations. The more ozone- and OOA-rich air masses were associated with transport from continental Europe, while plumes from UK cities had higher HOA and NOx and fewer thickly coated rBC particles. We did not observe any significant change in the rBC mass absorption efficiency calculated from rBC mass and light absorption coefficients measured by a particle soot absorption photometer despite observing significant changes in aerosol composition and rBC mixing state. The contributions of light scattering and absorption to total extinction (quantified by the single scattering albedo; SSA) did change for different air masses, with lower SSA

Black carbon aerosol mixing state, organic aerosols and aerosol optical properties over the United Kingdom

Directory of Open Access Journals (Sweden)

G. R. McMeeking

2011-09-01

Full Text Available Black carbon (BC aerosols absorb sunlight thereby leading to a positive radiative forcing and a warming of climate and can also impact human health through their impact on the respiratory system. The state of mixing of BC with other aerosol species, particularly the degree of internal/external mixing, has been highlighted as a major uncertainty in assessing its radiative forcing and hence its climate impact, but few in situ observations of mixing state exist. We present airborne single particle soot photometer (SP2 measurements of refractory BC (rBC mass concentrations and mixing state coupled with aerosol composition and optical properties measured in urban plumes and regional pollution over the United Kingdom. All data were obtained using instrumentation flown on the UK's BAe-146-301 large Atmospheric Research Aircraft (ARA operated by the Facility for Airborne Atmospheric Measurements (FAAM. We measured sub-micron aerosol composition using an aerosol mass spectrometer (AMS and used positive matrix factorization to separate hydrocarbon-like (HOA and oxygenated organic aerosols (OOA. We found a higher number fraction of thickly coated rBC particles in air masses with large OOA relative to HOA, higher ozone-to-nitrogen oxides (NO_x ratios and large concentrations of total sub-micron aerosol mass relative to rBC mass concentrations. The more ozone- and OOA-rich air masses were associated with transport from continental Europe, while plumes from UK cities had higher HOA and NO_x and fewer thickly coated rBC particles. We did not observe any significant change in the rBC mass absorption efficiency calculated from rBC mass and light absorption coefficients measured by a particle soot absorption photometer despite observing significant changes in aerosol composition and rBC mixing state. The contributions of light scattering and absorption to total extinction (quantified by the single scattering albedo; SSA did change for

Extreme testing of undiluted e-cigarette aerosol in vitro using an Ames air-agar-interface technique.

Science.gov (United States)

Thorne, D; Hollings, M; Seymour, A; Adamson, J; Dalrymple, A; Ballantyne, M; Gaca, M

2018-04-01

There is a growing consensus that e-cigarettes hold the potential for reducing the harm associated with cigarette smoking. Recently published studies have reported in vitro testing of e-cigarettes, demonstrating reduced toxicological and biological effects. Few studies however have reported the use of e-cigarettes under extreme testing conditions. To assess the full mutagenic potential of a commercially available electronic-cigarette (Vype ePen), this study investigated the delivery of aerosol under extreme conditions, using a scaled-down 35 mm plate Ames bacterial reverse mutagenicity assay. S. typhimurium strains TA98, TA100, TA97, TA104 and E. coli WP2 uvrA pKM101 with or without metabolic activation (S9), were employed. Using a modified Vitrocell VC 10 exposure system 0, 180, 360, 540, 720 or 900 puffs of undiluted e-cigarette aerosol was generated and delivered to bacterial cultures aligned to reported human consumption data. The results demonstrate that no mutagenic activity was observed in any strain under any test condition even when exposed to 900 puffs of undiluted e-cigarette aerosols +/- S9. Positive control responses were observed in all strains +/- S9. Nicotine assessments demonstrated an increased and consistent aerosol delivery, with calculated maximum doses of ∼1 mg/mL delivery of nicotine. These data demonstrate the validity of this unique testing approach and adds further information to the growing weight of evidence that e-cigarettes offer substantially reduced exposure when compared to conventional cigarette smoke. For future in vitro assessments of next generation tobacco and nicotine products, the generation, delivery and testing of undiluted aerosols can now be considered. Copyright © 2018 The Authors. Published by Elsevier B.V. All rights reserved.

Current Status of Aerosol Generation and Measurement Facilities for the Verification Test of Containment Filtered Venting System in KAERI

Energy Technology Data Exchange (ETDEWEB)

Kim, Sung Il; An, Sang Mo; Ha, Kwang Soon; Kim, Hwan Yeol [KAERI, Daejeon (Korea, Republic of)

2016-05-15

In this study, the design of aerosol generation and measurement systems are explained and present circumstances are also described. In addition, the aerosol test plan is shown. Containment Filtered Venting System (FCVS) is one of the safety features to reduce the amount of released fission product into the environment by depressurizing the containment. Since Chernobyl accident, the regulatory agency in several countries in Europe such as France, Germany, Sweden, etc. have been demanded the installation of the CFVS. Moreover, the feasibility study on the CFVS was also performed in U.S. After the Fukushima accident, there is a need to improve a containment venting or installation of depressurizing facility in Korea. As a part of a Ministry of Trade, Industry and Energy (MOTIE) project, KAERI has been conducted the integrated performance verification test of CFVS. As a part of the test, aerosol generation system and measurement systems were designed to simulate the fission products behavior. To perform the integrated verification test of CFVS, aerosol generation and measurement system was designed and manufactured. The component operating condition is determined to consider the severe accident condition. The test will be performed in normal conditions at first, and will be conducted under severe condition, high pressure and high temperature. Undesirable difficulties which disturb the elaborate test are expected, such as thermophoresis on the pipe, vapor condensation on aerosol, etc.

Atmospheric oxidation of isoprene and 1,3-Butadiene: influence of aerosol acidity and Relative humidity on secondary organic aerosol

Science.gov (United States)

The effects of acidic seed aerosols on the formation of secondary organic aerosol (SOA)have been examined in a number of previous studies, several of which have observed strong linear correlations between the aerosol acidity (measured as nmol H+ per m3 air s...

Fungal spores overwhelm biogenic organic aerosols in a midlatitudinal forest

Directory of Open Access Journals (Sweden)

C. Zhu

2016-06-01

Full Text Available Both primary biological aerosol particles (PBAPs and oxidation products of biogenic volatile organic compounds (BVOCs contribute significantly to organic aerosols (OAs in forested regions. However, little is known about their relative importance in diurnal timescales. Here, we report biomarkers of PBAP and secondary organic aerosols (SOAs for their diurnal variability in a temperate coniferous forest in Wakayama, Japan. Tracers of fungal spores, trehalose, arabitol and mannitol, showed significantly higher levels in nighttime than daytime (p < 0.05, resulting from the nocturnal sporulation under near-saturated relative humidity. On the contrary, BVOC oxidation products showed higher levels in daytime than nighttime, indicating substantial photochemical SOA formation. Using tracer-based methods, we estimated that fungal spores account for 45 % of organic carbon (OC in nighttime and 22 % in daytime, whereas BVOC oxidation products account for 15 and 19 %, respectively. To our knowledge, we present for the first time highly time-resolved results that fungal spores overwhelmed BVOC oxidation products in contributing to OA especially in nighttime. This study emphasizes the importance of both PBAPs and SOAs in forming forest organic aerosols.

The hygroscopicity parameter (κ) of ambient organic aerosol at a field site subject to biogenic and anthropogenic influences: relationship to degree of aerosol oxidation

Science.gov (United States)

Chang, R. Y.-W.; Slowik, J. G.; Shantz, N. C.; Vlasenko, A.; Liggio, J.; Sjostedt, S. J.; Leaitch, W. R.; Abbatt, J. P. D.

2010-06-01

Cloud condensation nuclei (CCN) concentrations were measured at Egbert, a rural site in Ontario, Canada during the spring of 2007. The CCN concentrations were compared to values predicted from the aerosol chemical composition and size distribution using κ-Köhler theory, with the specific goal of this work being to determine the hygroscopic parameter (κ) of the oxygenated organic component of the aerosol, assuming that oxygenation drives the hygroscopicity for the entire organic fraction of the aerosol. The hygroscopicity of the oxygenated fraction of the organic component, as determined by an Aerodyne aerosol mass spectrometer (AMS), was characterised by two methods. First, positive matrix factorization (PMF) was used to separate oxygenated and unoxygenated organic aerosol factors. By assuming that the unoxygenated factor is completely non-hygroscopic and by varying κ of the oxygenated factor so that the predicted and measured CCN concentrations are internally consistent and in good agreement, κ of the oxygenated organic factor was found to be 0.22±0.04 for the suite of measurements made during this five-week campaign. In a second, equivalent approach, we continue to assume that the unoxygenated component of the aerosol, with a mole ratio of atomic oxygen to atomic carbon (O/C) ≈ 0, is completely non-hygroscopic, and we postulate a simple linear relationship between κorg and O/C. Under these assumptions, the κ of the entire organic component for bulk aerosols measured by the AMS can be parameterised as κorg=(0.29±0.05)·(O/C), for the range of O/C observed in this study (0.3 to 0.6). These results are averaged over our five-week study at one location using only the AMS for composition analysis. Empirically, our measurements are consistent with κorg generally increasing with increasing particle oxygenation, but high uncertainties preclude us from testing this hypothesis. Lastly, we examine select periods of different aerosol composition, corresponding

Effect of relative humidity on growth of sodium oxide aerosols

International Nuclear Information System (INIS)

Sundarajan, A.R.; Mitragotri, D.S.; Mukunda Rao, S.R.

1982-01-01

Behavior of aerosol resulting from sodium fires in a closed vessel is investigated and the changes in the particle size distribution of the aerosol due to coagulation and humidity have been studied. The initial mass concentration is in the range of 80 -- 500 mg/m 3 and the relative humidity is varied between 50 to 98%. The initial size of the released aerosol is found to be 0.9 μm. Equilibrium diameters of particles growing in humid air have been computed for various humidity levels using water activity of sodium hydroxide. Both theoretical and experimental results have yielded growth ratios of about 3 at about 95% relative humidity. It is recommended that the computer codes dealing with aerosol coagulation behavior in reactor containment should include an appropriate humidity-growth function. (author)

Formation of secondary organic aerosol from isoprene oxidation over Europe

Directory of Open Access Journals (Sweden)

M. Karl

2009-09-01

Full Text Available The role of isoprene as a precursor to secondary organic aerosol (SOA over Europe is studied with the two-way nested global chemistry transport model TM5. The inclusion of the formation of SOA from isoprene oxidation in our model almost doubles the atmospheric burden of SOA over Europe compared to SOA formation from terpenes and aromatics. The reference simulation, which considers SOA formation from isoprene, terpenes and aromatics, predicts a yearly European production rate of 1.0 Tg SOA yr⁻¹ and an annual averaged atmospheric burden of about 50 Gg SOA over Europe. A fraction of 35% of the SOA produced in the boundary layer over Europe is transported to higher altitudes or to other world regions. Summertime measurements of organic matter (OM during the extensive EMEP OC/EC campaign 2002/2003 are better reproduced when SOA formation from isoprene is taken into account, reflecting also the strong seasonality of isoprene and other biogenic volatile organic compounds (BVOC emissions from vegetation. However, during winter, our model strongly underestimates OM, likely caused by missing wood burning in the emission inventories. Uncertainties in the parameterisation of isoprene SOA formation have been investigated. Maximum SOA production is found for irreversible sticking (non-equilibrium partitioning of condensable vapours on particles, with tropospheric SOA production over Europe increased by a factor of 4 in summer compared to the reference case. Completely neglecting SOA formation from isoprene results in the lowest estimate (0.51 Tg SOA yr⁻¹. The amount and the nature of the absorbing matter are shown to be another key uncertainty when predicting SOA levels. Consequently, smog chamber experiments on SOA formation should be performed with different types of seed aerosols and without seed aerosols in order to derive an improved treatment of the absorption of SOA in the models. Consideration of a number of recent insights

Automated aerosol sampling and analysis for the Comprehensive Test Ban Treaty

International Nuclear Information System (INIS)

Miley, H.S.; Bowyer, S.M.; Hubbard, C.W.; McKinnon, A.D.; Perkins, R.W.; Thompson, R.C.; Warner, R.A.

1998-01-01

Detecting nuclear debris from a nuclear weapon exploded in or substantially vented to the Earth's atmosphere constitutes the most certain indication that a violation of the Comprehensive Test Ban Treaty has occurred. For this reason, a radionuclide portion of the International Monitoring System is being designed and implemented. The IMS will monitor aerosols and gaseous xenon isotopes to detect atmospheric and underground tests, respectively. An automated system, the Radionuclide Aerosol Sampler/Analyzer (RASA), has been developed at Pacific Northwest National Laboratory to meet CTBT aerosol measurement requirements. This is achieved by the use of a novel sampling apparatus, a high-resolution germanium detector, and very sophisticated software. This system draws a large volume of air (∼ 20,000 m 3 /day), performs automated gamma-ray spectral measurements (MDC( 140 Ba) 3 ), and communicates this and other data to a central data facility. Automated systems offer the added benefit of rigid controls, easily implemented QA/QC procedures, and centralized depot maintenance and operation. Other types of automated communication include pull or push transmission of State-Of-Health data, commands, and configuration data. In addition, a graphical user interface, Telnet, and other interactive communications are supported over ordinary phone or network lines. This system has been the subject of a USAF commercialization effort to meet US CTBT monitoring commitments. It will also be available to other CTBT signatories and the monitoring community for various governmental, environmental, or commercial needs. The current status of the commercialization is discussed

Secondary organic aerosol formation from primary aliphatic amines with NO3 radical

Science.gov (United States)

Malloy, Q. G. J.; Qi, Li; Warren, B.; Cocker, D. R., III; Erupe, M. E.; Silva, P. J.

2009-03-01

Primary aliphatic amines are an important class of nitrogen containing compounds emitted from automobiles, waste treatment facilities and agricultural animal operations. A series of experiments conducted at the UC-Riverside/CE-CERT Environmental Chamber is presented in which oxidation of methylamine, ethylamine, propylamine, and butylamine with O3 and NO3 have been investigated. Very little aerosol formation is observed in the presence of O3 only. However, after addition of NO, and by extension NO3, large aerosol mass yields (~44% for butylamine) are seen. Aerosol generated was determined to be organic in nature due to the small fraction of NO and NO2 in the total signal (tested) as detected by an aerosol mass spectrometer (AMS). We propose a reaction mechanism between carbonyl containing species and the parent amine leading to formation of particulate imine products. These findings can have significant impacts on rural communities with elevated nighttime PM loadings, when significant levels of NO3 exist.

Secondary organic aerosol formation from primary aliphatic amines with NO3 radical

Directory of Open Access Journals (Sweden)

P. J. Silva

2009-03-01

Full Text Available Primary aliphatic amines are an important class of nitrogen containing compounds emitted from automobiles, waste treatment facilities and agricultural animal operations. A series of experiments conducted at the UC-Riverside/CE-CERT Environmental Chamber is presented in which oxidation of methylamine, ethylamine, propylamine, and butylamine with O3 and NO3 have been investigated. Very little aerosol formation is observed in the presence of O3 only. However, after addition of NO, and by extension NO3, large aerosol mass yields (~44% for butylamine are seen. Aerosol generated was determined to be organic in nature due to the small fraction of NO and NO2 in the total signal (<1% for all amines tested as detected by an aerosol mass spectrometer (AMS. We propose a reaction mechanism between carbonyl containing species and the parent amine leading to formation of particulate imine products. These findings can have significant impacts on rural communities with elevated nighttime PM loadings, when significant levels of NO3 exist.

Atmospheric oxidation of 1,3-butadiene: characterization of gas and aerosol reaction products and implications for PM2.5

Science.gov (United States)

Jaoui, M.; Lewandowski, M.; Docherty, K.; Offenberg, J. H.; Kleindienst, T. E.

2014-12-01

examined. The contribution of SOA products from 13BD oxidation to ambient PM2.5 was investigated by analyzing a series of ambient PM2.5 samples collected in several locations around the United States. In addition to the occurrence of several organic compounds in field and laboratory samples, glyceric acid, d-threitol, erythritol, erythrose, and threonic acid were found to originate only from the oxidation of 13BD based on our previous experiments involving chamber oxidation of a series of hydrocarbons. Initial attempts have been made to quantify the concentrations of these compounds. The average concentrations of these compounds in ambient PM2.5 samples from the California Research at the Nexus of Air Quality and Climate Change (CalNex) study ranged from 0 to approximately 14.1 ng m-3. The occurrence of several other compounds in both laboratory and field samples suggests that SOA originating from 13BD oxidation could contribute to the ambient aerosol mainly in areas with high 13BD emission rates.

Cloud condensation nuclei activity of aliphatic amine secondary aerosol

Science.gov (United States)

Aliphatic amines can form secondary aerosol via oxidation with atmospheric radicals (e.g. hydroxyl radical and nitrate radical). The resulting particle composition can contain both secondary organic aerosol (SOA) and inorganic salts. The fraction of organic to inorganic materials in the particulate ...

Organic Aerosols in the Presence of CO{sub 2} in the Early Earth and Exoplanets: UV–Vis Refractive Indices of Oxidized Tholins

Energy Technology Data Exchange (ETDEWEB)

Gavilan, Lisseth; Carrasco, Nathalie; Vettier, Ludovic [LATMOS, Université Versailles St Quentin, UPMC Université Paris 06, CNRS, 11 blvd d’Alembert, F-78280 Guyancourt (France); Broch, Laurent [LCP-A2MC, Institut Jean Barriol, Université de Lorraine, Metz (France); Fleury, Benjamin, E-mail: lisseth.gavilan@latmos.ipsl.fr [Jet Propulsion Laboratory, California Institute of Technology, Pasadena, CA 91109 (United States)

2017-10-10

In this experimental study we investigate the role of atmospheric CO{sub 2} on the optical properties of organic photochemical aerosols. To this end, we add CO{sub 2} to a N{sub 2}:CH{sub 4} gas mixture used in a plasma typically used for Titan studies. We produce organic thin films (tholins) in plasmas where the CO{sub 2}/CH{sub 4} ratio is increased from 0 to 4. We measure these films via spectrometric ellipsometry and apply a Tauc–Lorentz model, used for optically transparent materials, to obtain the thickness of the thin film, its optical band gap, and the refractive indices in the UV–visible (270–600 nm). All samples present a significant absorption band in the UV. According to the Tauc–Lorentz model, as the CO{sub 2}/CH{sub 4} ratio is quadrupled, the position of the UV band is shifted from ∼177 nm to 264 nm while its strength is quadrupled. Consequently, we infer that oxidized organic aerosols absorb more efficiently at longer UV wavelengths than reduced aerosols. Our laboratory wavelength-tabulated UV–vis refractive indices provide new constraints to atmospheric models of the early Earth and Earth-like exoplanets including photochemical hazes formed under increasingly oxidizing conditions.

Test Concept for Advanced Oxidation Techniques

DEFF Research Database (Denmark)

Bennedsen, Lars Rønn; Søgaard, Erik Gydesen; Mortensen, Lars

advanced on-site oxidation tests. The remediation techniques included are electrochemical oxidation, photochemical/photocatalytic oxidation, ozone, hydrogen peroxide, permanganate, and persulfate among others. A versatile construction of the mobile test unit makes it possible to combine different...

Chemical and physical transformations of organic aerosol from the photo-oxidation of open biomass burning emissions in an environmental chamber

Science.gov (United States)

C. J. Hennigan; M. A. Miracolo; G. J. Engelhart; A. A. May; A. A. Presto; T. Lee; A. P. Sullivan; G. R. McMeeking; H. Coe; C. E. Wold; W.-M. Hao; J. B. Gilman; W. C. Kuster; J. de Gouw; B. A. Schichtel; J. L. Collett; S. M. Kreidenweis; A. L. Robinson

2011-01-01

Smog chamber experiments were conducted to investigate the chemical and physical transformations of organic aerosol (OA) during photo-oxidation of open biomass burning emissions. The experiments were carried out at the US Forest Service Fire Science Laboratory as part of the third Fire Lab at Missoula Experiment (FLAME III). We investigated emissions from 12 different...

40 CFR 53.59 - Aerosol transport test for Class I equivalent method samplers.

Science.gov (United States)

2010-07-01

... through which sample air is flowing during performance of this test. (3) A no-flow filter is a sample filter through which no sample air is intended to flow during performance of this test. (4) A channel is... a device or means to allow or cause the aerosol to be routed to one of several channels. (c...

Aerosol Chemical Composition and its Effects on Cloud-Aerosol Interactions during the 2007 CHAPS Experiment

Science.gov (United States)

Lee, Y.; Alexander, L.; Newburn, M.; Jayne, J.; Hubbe, J.; Springston, S.; Senum, G.; Andrews, B.; Ogren, J.; Kleinman, L.; Daum, P.; Berg, L.; Berkowitz, C.

2007-12-01

Chemical composition of submicron aerosol particles was determined using an Aerodyne Time-of-Flight Aerosol Mass Spectrometer (AMS) outfitted on the DOE G-1 aircraft during the Cumulus Humilis Aerosol Processing Study (CHAPS) conducted in Oklahoma City area in June 2007. The primary objective of CHAPS was to investigate the effects of urban emissions on cloud aerosol interactions as a function of processing of the emissions. Aerosol composition was typically determined at three different altitudes: below, in, and above cloud, in both upwind and downwind regions of the urban area. Aerosols were sampled from an isokinetic inlet with an upper size cut-off of ~1.5 micrometer. During cloud passages, the AMS also sampled particles that were dried from cloud droplets collected using a counter-flow virtual impactor (CVI) sampler. The aerosol mass concentrations were typically below 10 microgram per cubic meter, and were dominated by organics and sulfate. Ammonium was often less than required for complete neutralization of sulfate. Aerosol nitrate levels were very low. We noted that nitrate levels were significantly enhanced in cloud droplets compared to aerosols, most likely resulting from dissolution of gaseous nitric acid. Organic to sulfate ratios appeared to be lower in cloud droplets than in aerosols, suggesting cloud condensation nuclei properties of aerosol particles might be affected by loading and nature of the organic components in aerosols. In-cloud formation of sulfate was considered unimportant because of the very low SO2 concentration in the region. A detailed examination of the sources of the aerosol organic components (based on hydrocarbons determined using a proton transfer reaction mass spectrometer) and their effects on cloud formation as a function of atmospheric processing (based on the degree of oxidation of the organic components) will be presented.

Glyoxal contribution to aerosols over Los Angeles

Science.gov (United States)

Balcerak, Ernie

2012-01-01

Laboratory and field studies have indicated that glyoxal (chemical formula OCHCHO), an atmospheric oxidation product of isoprene and aromatic compounds, may contribute to secondary organic aerosols in the atmosphere, which can block sunlight and affect atmospheric chemistry. Some aerosols are primary aerosols, emitted directly into the atmosphere, while others are secondary, formed through chemical reactions in the atmosphere. Washenfelder et al. describe in situ glyoxal measurements from Pasadena, Calif., near Los Angeles, made during summer 2010. They used three different methods to calculate the contribution of glyoxal to secondary atmospheric aerosol and found that it is responsible for 0-0.2 microgram per cubic meter, or 0-4%, of the secondary organic aerosol mass. The researchers also compared their results to those of a previous study that calculated the glyoxal contribution to aerosol for Mexico City. Mexico City had higher levels of organic aerosol mass from glyoxal. They suggest that the lower contribution of glyoxal to aerosol concentrations for Los Angeles may be due to differences in the composition or water content of the aerosols above the two cities. (Journal of Geophysical Research-Atmospheres, doi:10.1029/2011JD016314, 2011)

VUV photoionization aerosol mass spectrometric study on the iodine oxide particles formed from O3-initiated photooxidation of diiodomethane (CH2I2)

Czech Academy of Sciences Publication Activity Database

Wei, N.; Hu, Ch.; Zhou, S.; Ma, Q.; Mikuška, Pavel; Večeřa, Zbyněk; Gai, Y.; Lin, X.; Gu, X.; Zhao, W.; Fang, B.; Zhang, W.; Chen, J.; Liu, F.; Shan, X.; Sheng, L.

2017-01-01

Roč. 7, č. 89 (2017), s. 56779-56787 ISSN 2046-2069 Institutional support: RVO:68081715 Keywords : iodine oxide particles * photooxidation * aerosol mass spectrometer Subject RIV: CB - Analytical Chemistry, Separation OBOR OECD: Analytical chemistry Impact factor: 3.108, year: 2016

Aerosol in the containment

International Nuclear Information System (INIS)

Lanza, S.; Mariotti, P.

1986-01-01

The US program LACE (LWR Aerosol Containment Experiments), in which Italy participates together with several European countries, Canada and Japan, aims at evaluating by means of a large scale experimental activity at HEDL the retention in the pipings and primary container of the radioactive aerosol released following severe accidents in light water reactors. At the same time these experiences will make available data through which the codes used to analyse the behaviour of the aerosol in the containment and to verify whether by means of the codes of thermohydraulic computation it is possible to evaluate with sufficient accuracy variable influencing the aerosol behaviour, can be validated. This report shows and compares the results obtained by the participants in the LACE program with the aerosol containment codes NAVA 5 and CONTAIN for the pre-test computations of the test LA 1, in which an accident called containment by pass is simulated

Frequency analysis of pulmonary tumors occurrence at the rat after exposure to actinide oxide aerosols. Risk factors identification by comparing NpO2 and PuO2

International Nuclear Information System (INIS)

Dudoignon, N.

2001-07-01

Inhalation of actinide oxide particles is potentially one route of contamination of workers, which might induce pulmonary tumours due to aerosol generation during nuclear fuel fabrication process. Dose-effect relationships for lung tumour induction have been well established from epidemiological and experimental studies. However, they do not take into account specific parameters of exposure. The aim of this study was to compare cancer incidence among groups of rats exposed either to NpO 2 or to PuO 2 , two actinide oxides with different specific activity, but with similar aerosol granulometry. During the rat life-span, lung tumour development could occur and the individual follow-up allowed the determination of lung dose at death. Although aerosol particle sizes were similar, the mean number of particles per unit of activity was 2400 times higher for NpO 2 as compared to PuO 2 . This range of variation appeared higher than the variation of specific activity (450). Initial distribution of aerosol was then much more homogeneous for neptunium. In the range of initial lung deposits studied, the only physiological changes observed concerned lung clearance and rat life- span after exposure to the highest levels of Np activity. Pathological examination performed at death showed that carcinogenic power of neptunium was 2 to 3 times higher than that of plutonium. Dose-effect relationships appeared linear and when compared to previous studies, showed an increase of lung cancer risk as the specific activity of the inhaled actinide oxide decreases. The range of risk variation can reach a factor of 10, revealing that the consideration of lung dose at death solely might not be sufficient for an accurate estimate of risk and that specific parameters of exposure, such as nature and granulometry of aerosols, should also be taken into account. (author)

The clearance of Pu and Am from the respiratory system of rodents after the inhalation of oxide aerosols of these actinides either alone or in combination with other metals

International Nuclear Information System (INIS)

Stather, J.W.; James, A.C.; Brightwell, J.; Rodwell, P.

1979-01-01

In this series of studies in rodents the lung clearance and tissue distribution of both plutonium and americium have been measured following their inhalation as mixed actinide oxides either alone or in combination with other metals. The aerosols used were materials to which workers in the nuclear industry may be occupationally exposed or which could be generated in the event of an accident in a reactor core or fuel fabrication plant. The studies showed that, at least for some PuO 2 aerosols, the lung model currently being used by ICRP for estimating tissue doses from inhaled actinides may overestimate, by about a factor of ten, the amount of plutonium translocated to the blood. The presence of oxides of other metals can, however, appreciably influence the clearance of plutonium from the lung. While in some mixtures plutonium dioxide behaves as an insoluble (Class Y) compound and in others as a soluble (Class W) compound, it may also have transportability characteristics between these two extremes. Americium-241 behaves as a soluble (Class W) compound when inhaled as the oxide. However, if it is present in trace quantities in mixed-oxide aerosols its behaviour depends upon that of the materials present in greatest mass. (author)

Products of BVOC oxidation: ozone and organic aerosols

Science.gov (United States)

Wildt, Jürgen; Andres, Stefanie; Carriero, Giulia; Ehn, Mikael; Fares, Silvano; Hoffmann, Thorsten; Hacker, Lina; Kiendler-Scharr, Astrid; Kleist, Einhard; Paoletti, Elena; Pullinen, Iida; Rohrer, Franz; Rudich, Yinon; Springer, Monika; Tillmann, Ralf; Wahner, Andreas; Wu, Cheng; Mentel, Thomas

2015-04-01

Biogenic Volatile Organic Compounds (BVOC) are important precursors in photochemical O3 and secondary organic aerosol (SOA) formation. We conducted a series of laboratory experiments with OH-induced oxidation of monoterpenes to elucidate pathways and efficiencies of O3 and SOA formation. At high NOx conditions ([BVOC] / [NOx] monoterpene mixes emitted from different plant species we observed increasing ozone formation with increasing [NOX]. Between 2 and 3 O3-molecules were formed from 1 monoterpene when ozone formation was BVOC limited. Under such high NOX conditions, new particle formation was suppressed. Increasing [BVOC] / [NOX] ratios caused increasing efficiency of new particle formation indicating that peroxy radicals are the key intermediates in both, photochemical ozone- and new particle formation. The classical chemistry of peroxy radicals is well established (e.g. Master Chemical Mechanism). Peroxy radicals are produced by addition of molecular oxygen to the alkyl radical formed after OH attack at the BVOC. They either react with NO which leads to ozone formation or they react with other peroxy radicals and form chemically stable products (hydroperoxides, alkoholes and ketones). Much less knowledge exists on such reactions for Highly Oxidized Peroxy Radicals, (HOPR). Such HOPR were observed during ozonolysis of several volatiles and, in case of monoterpenes as precursors, they can contain more than 12 Oxygen atoms (Mentel et al., 2015). Although the OH-initiated formation of HOPR is yet not fully understood, their basic gas phase reactions seem to follow classical photochemical rules. In reactions with NO they can act as precursor for O3 and in reactions with other HOPR or with classical less oxidized peroxy radicals they can form highly oxidized stable products and alkoxy radicals. In addition, HOPR-HOPR reactions lead to the formation of dimers that, in case of monoterpenes as reactants, consist of a skeleton with 20 carbon atoms. These dimers seem to

Analysis of the heat and mass transfer processes of a UO2 bubble in sodium for the Fuel Aerosol Simulant Test (FAST)

International Nuclear Information System (INIS)

Tobias, M.L.

1979-01-01

The anticipated behavior of uranium oxide vapor bubbles produced by the capacitor discharge vaporization (CDV) method in the Fuel Aerosol Simulant Test (FAST) Facility is discussed on the basis of relatively simple physical models. Results of calculations for the rate of bubble rise and for heat and mass transfer rates are presented. Parametric studies indicate that future analysis efforts should emphasize the diffusion condensation process and the loss of heat from the bubble by radiation. Transfer of heat in the surrounding sodium is rapid enough that simplified models should be adequate. No important effects were noted in connection with bubble depth, initial quantity of UO 2 , or initial superheat

Quantitative characterization of colloidal assembly of graphene oxide-silver nanoparticle hybrids using aerosol differential mobility-coupled mass analyses.

Science.gov (United States)

Nguyen, Thai Phuong; Chang, Wei-Chang; Lai, Yen-Chih; Hsiao, Ta-Chih; Tsai, De-Hao

2017-10-01

In this work, we develop an aerosol-based, time-resolved ion mobility-coupled mass characterization method to investigate colloidal assembly of graphene oxide (GO)-silver nanoparticle (AgNP) hybrid nanostructure on a quantitative basis. Transmission electron microscopy (TEM) and zeta potential (ZP) analysis were used to provide visual information and elemental-based particle size distributions, respectively. Results clearly show a successful controlled assembly of GO-AgNP by electrostatic-directed heterogeneous aggregation between GO and bovine serum albumin (BSA)-functionalized AgNP under an acidic environment. Additionally, physical size, mass, and conformation (i.e., number of AgNP per nanohybrid) of GO-AgNP were shown to be proportional to the number concentration ratio of AgNP to GO (R) and the selected electrical mobility diameter. An analysis of colloidal stability of GO-AgNP indicates that the stability increased with its absolute ZP, which was dependent on R and environmental pH. The work presented here provides a proof of concept for systematically synthesizing hybrid colloidal nanomaterials through the tuning of surface chemistry in aqueous phase with the ability in quantitative characterization. Graphical Abstract Colloidal assembly of graphene oxide-silver nanoparticle hybrids characterized by aerosol differential mobility-coupled mass analyses.

2-D model of global aerosol transport

Energy Technology Data Exchange (ETDEWEB)

Rehkopf, J; Newiger, M; Grassl, H

1984-01-01

The distribution of aerosol particles in the troposphere is described. Starting with long term mean seasonal flow and diffusivities as well as temperature, cloud distribution (six cloud classes), relative humidity and OH radical concentration, the steady state concentration of aerosol particles and SO/sub 2/ are calculated in a two-dimensional global (height and latitude) model. The following sources and sinks for particles are handled: direct emission, gas-to-particle conversion from SO/sub 2/, coagulation, rainout, washout, gravitational settling, and dry deposition. The sinks considered for sulphur emissions are dry deposition, washout, rainout, gasphase oxidation, and aqueous phase oxidation. Model tests with the water vapour cycle show a good agreement between measured and calculated zonal mean precipitation distribution. The steady state concentration distribution for natural emissions reached after 10 weeks model time, may be described by a mean exponent ..cap alpha.. = 3.2 near the surface assuming a modified Junge distribution and an increased value, ..cap alpha.. = 3.7, for the combined natural and man-made emission. The maximum ground level concentrations are 2000 and 10,000 particules cm/sup -3/ for natural and natural plus man-made emissions, respectively. The resulting distribution of sulphur dioxide agrees satisfactorily with measurements given by several authors. 37 references, 4 figures.

Overview of the Capstone Depleted Uranium Study of Aerosols from Impact with Armored Vehicles: Test Setup and Aerosol Generation, Characterization, and Application in Assessing Dose and Risk

International Nuclear Information System (INIS)

Parkhurst, MaryAnn; Guilmette, Raymond A.

2009-01-01

The Capstone Depleted Uranium (DU) Aerosol Characterization and Risk Assessment Study was conducted to generate data about DU aerosols generated during the perforation of armored combat vehicles with large-caliber DU penetrators, and to apply the data in assessments of human health risks to personnel exposed to these aerosols, primarily through inhalation, during the 1991 Gulf War or in future military operations. The Capstone study consisted of two components: (1) generating, sampling and characterizing DU aerosols by firing at and perforating combat vehicles and (2) applying the source-term quantities and characteristics of the aerosols to the evaluation of doses and risks. This paper reviews the background of the study including the bases for the study, previous reviews of DU particles and health assessments from DU used by the U.S. military, the objectives of the study components, the participants and oversight teams, and the types of exposures it was intended to evaluate. It then discusses exposure scenarios used in the dose and risk assessment and provides an overview of how the field tests and dose and risk assessments were conducted

Aerosol filtration with metallic fibrous filters

International Nuclear Information System (INIS)

Klein, M.; Goossens, W.R.A.

1983-01-01

The filtration efficiency of stainless steel fibrous filters (BEKIPOR porous mats and sintered webs) is determined using submicronic monodisperse polystyrene aerosols. Lasers spectrometers are used for the aerosol measurements. The parameters varied are the fiber diameter, the number of layers, the aerosol diameter and the superficial velocity. Two selected types of filters are tested with polydisperse methylene blue aerosols to determine the effect of bed loading on the filter performance and to test washing techniques for the regeneration of the filter

Measuring aerosols generated inside armoured vehicles perforated by depleted uranium ammunition

International Nuclear Information System (INIS)

Parkhurst, M.A.

2003-01-01

In response to questions raised after the Gulf War about the health significance of exposure to depleted uranium (DU), the US Department of Defense initiated a study designed to provide an improved scientific basis for assessment of possible health effects on soldiers in vehicles struck by these munitions. As part of this study, a series of DU penetrators were fired at an Abrams tank and a Bradley fighting vehicle, and the aerosols generated by vehicle perforation were collected and characterised. A robust sampling system was designed to collect aerosols in this difficult environment and monitor continuously the sampler flow rates. The aerosol samplers selected for these tests included filter cassettes, cascade impactors, a five-stage cyclone and a moving filter. Sampler redundancy was an integral part of the sampling system to offset losses from fragment damage. Wipe surveys and deposition trays collected removable deposited particulate matter. Interior aerosols were analysed for uranium concentration and particle size distribution as a function of time. They were also analysed for uranium oxide phases, particle morphology and dissolution in vitro. These data, currently under independent peer review, will provide input for future prospective and retrospective dose and health risk assessments of inhaled or ingested DU aerosols. This paper briefly discusses the target vehicles, firing trajectories, aerosol samplers and instrumentation control systems, and the types of analyses conducted on the samples. (author)

Atmo-metabolomics: a new measurement approach for investigating aerosol composition and ecosystem functioning.

Science.gov (United States)

Rivas-Ubach, A.; Liu, Y.; Sardans, J.; Tfaily, M. M.; Kim, Y. M.; Bourrianne, E.; Paša-Tolić, L.; Penuelas, J.; Guenther, A. B.

2016-12-01

Aerosols play crucial roles in the processes controlling the composition of the atmosphere and the functioning of ecosystems. Gaining a deeper understanding of the chemical composition of aerosols is one of the major challenges for atmospheric and climate scientists and is beginning to be recognized as important for ecological research. Better comprehension of aerosol chemistry can potentially provide valuable information on atmospheric processes such as oxidation of organics and the production of cloud condensation nuclei as well as provide an approximation of the general status of an ecosystem through the measurement of certain stress biomarkers. In this study, we describe an efficient aerosol sampling method, the metabolite extraction and the analytical procedures for the chemical characterization of aerosols, namely, the atmo-metabolome. We used mass spectrometry (MS) coupled to liquid chromatography (LC-MS), gas chromatography (GC-MS) and Fourier transform ion cyclotron resonance (FT-ICR-MS) to characterize the atmo-metabolome of two marked seasons; spring and summer. Our sampling and extraction methods demonstrated to be suitable for aerosol chemical characterization with any of the analytical platforms used in this study. The atmo-metabolome between spring and summer showed overall statistically differences. We identified several metabolites that can be attributed to pollen and other plant-related aerosols. Spring aerosols exhibit higher concentrations of metabolites linked to higher plant activity while summer samples had higher concentrations of metabolites that may reflect certain oxidative stresses in primary producers. Moreover, the elemental composition of aerosols showed clear different between seasons. Summer aerosols were generally higher in molecular weight and with higher O/C ratios, indicating higher oxidation levels and condensation of compounds relative to spring. Our method represents an advanced approach for characterizing the composition of

Capstone Depleted Uranium Aerosols: Generation and Characterization

Energy Technology Data Exchange (ETDEWEB)

Parkhurst, MaryAnn; Szrom, Fran; Guilmette, Ray; Holmes, Tom; Cheng, Yung-Sung; Kenoyer, Judson L.; Collins, John W.; Sanderson, T. Ellory; Fliszar, Richard W.; Gold, Kenneth; Beckman, John C.; Long, Julie

2004-10-19

In a study designed to provide an improved scientific basis for assessing possible health effects from inhaling depleted uranium (DU) aerosols, a series of DU penetrators was fired at an Abrams tank and a Bradley fighting vehicle. A robust sampling system was designed to collect aerosols in this difficult environment and continuously monitor the sampler flow rates. Aerosols collected were analyzed for uranium concentration and particle size distribution as a function of time. They were also analyzed for uranium oxide phases, particle morphology, and dissolution in vitro. The resulting data provide input useful in human health risk assessments.

Exchanges in boundary layer and low troposphere and consequences on pollution of Fos-Berre-Marseille area (ESCOMPTE experiment); Les aerosols: emissions, formation d'aerosols organiques secondaires, transport longue distance. Zoom sur les aerosols carbones en Europe

Energy Technology Data Exchange (ETDEWEB)

Guillaume, B

2006-01-15

There are two types of 'carbonaceous aerosols': 'black carbon' (BC) and 'organic carbon'(OC). BC is directly emitted in the atmosphere while OC is either directly emitted (primary OC, OCp) or secondarily formed through oxidation processes in the atmosphere (secondary organic aerosols, SOA). Complexity of carbonaceous aerosols is still poorly represented in existing aerosol models and uncertainties appear mainly both in their emission inventories and in their complex atmospheric evolution (transport, gas-particle interactions, dry/wet deposition), making difficult the estimation of their radiative impact. In this framework, I developed during my PhD at Laboratoire d'Aerologie, a new approach to deal with this complexity, with implementation of both a new carbonaceous aerosol emission inventory and a new aerosol modelling tool at global scale. My work is divided in 5 different tasks: - better characterisation of BC and OCp emissions, achieved through the development of a new emission inventory from fossil fuel and biofuel combustion sources (industrial, domestic and mobile sources). This inventory provides BC and OCp emissions for Europe at 25 km * 25 km resolution for the years 1990, 1995, 2000, 2005 and 2010, with two additional regional zooms: on France, at 10 km * 10 km resolution for the years 2000 and 2010 with improved road traffic, and in Marseille region (Escompte campaign, 1999,-2001) at 1 km * 1 km resolution for the year 1999; - better modelling of carbonaceous aerosol complex atmospheric evolution, through coupling of a global scale gas transport/chemistry model (TM4) with an aerosol module (ORISAM) featuring size-distributed aerosols (on 8 diameter sections from 40 nm to 10 {mu}m) organic/inorganic chemical composition and explicit treatment of SOA formation; - simulations with this new aerosol model ORISAM-TM4 and model/measurements comparisons to study BC and OC long-range transport; - sensitivity tests on SOA

International standard problem ISP37: VANAM M3 - A Multi compartment aerosol depletion test with hygroscopic aerosol material: comparison report

International Nuclear Information System (INIS)

Firnhaber, M.; Kanzleiter, T.F.; Schwarz, S.; Weber, G.

1996-12-01

This paper presents the results and assessment of the 'open' ISP37, which deals with the containment thermal-hydraulics and aerosol behavior during an unmitigated severe LWR accident with core melt-down and steam and aerosol release into the containment. Representatives of 22 organizations participated to the ISP37 using the codes CONTAIN, FIPLOC, MELCOR, RALOC, FUMO, MACRES, REMOVAL etc. The containment and aerosol behavior experiment VANAM M3 was selected as experimental comparison basis. The main phenomena investigated are the thermal behavior of a multi-compartment containment, e.g. pressure, temperature and the distribution and depletion of a soluble aerosol. The ISP37 has demonstrated that the codes used could calculate the thermal-hydraulic containment behavior in general with sufficient accuracy. But with respect to the needs of aerosol behavior analysis the accuracies, both analytical and experimental as well, for specific thermal-hydraulic variables should be improved. Although large progress has been made in the simulation of aerosol behavior in multi-compartment geometries the calculated local aerosol concentrations scatter widely. However, the aerosol source term to the environment is overestimated in general. The largest uncertainty concerning the aerosol results is caused by a limited number of thermal hydraulic variables like relative humidity, volume condensation rate and atmospheric flow rate. In some codes also a solubility model is missing

Source term experiments project (STEP): aerosol characterization system

International Nuclear Information System (INIS)

Schlenger, B.J.; Dunn, P.F.

1985-01-01

A series of four experiments is being conducted at Argonne National Laboratory's TREAT Reactor. They have been designed to provide some of the necessary data regarding magnitude and release rates of fission products from degraded fuel pins, physical and chemical characteristics of released fission products, and aerosol formation and transport phenomena. These are in-pile experiments, whereby the test fuel is heated by neutron induced fission and subsequent clad oxidation in steam environments that simulate as closely as practical predicted reactor accident conditions. The test sequences cover a range of pressure and fuel heatup rate, and include the effect of Ag/In/Cd control rod material

Laboratory Experiments and Modeling for Interpreting Field Studies of Secondary Organic Aerosol Formation Using an Oxidation Flow Reactor

Energy Technology Data Exchange (ETDEWEB)

Jimenez, Jose-Luis [Univ. of Colorado, Boulder, CO (United States)

2016-02-01

This grant was originally funded for deployment of a suite of aerosol instrumentation by our group in collaboration with other research groups and DOE/ARM to the Ganges Valley in India (GVAX) to study aerosols sources and processing. Much of the first year of this grant was focused on preparations for GVAX. That campaign was cancelled due to political reasons and with the consultation with our program manager, the research of this grant was refocused to study the applications of oxidation flow reactors (OFRs) for investigating secondary organic aerosol (SOA) formation and organic aerosol (OA) processing in the field and laboratory through a series of laboratory and modeling studies. We developed a gas-phase photochemical model of an OFR which was used to 1) explore the sensitivities of key output variables (e.g., OH exposure, O₃, HO₂/OH) to controlling factors (e.g., water vapor, external reactivity, UV irradiation), 2) develop simplified OH exposure estimation equations, 3) investigate under what conditions non-OH chemistry may be important, and 4) help guide design of future experiments to avoid conditions with undesired chemistry for a wide range of conditions applicable to the ambient, laboratory, and source studies. Uncertainties in the model were quantified and modeled OH exposure was compared to tracer decay measurements of OH exposure in the lab and field. Laboratory studies using OFRs were conducted to explore aerosol yields and composition from anthropogenic and biogenic VOC as well as crude oil evaporates. Various aspects of the modeling and laboratory results and tools were applied to interpretation of ambient and source measurements using OFR. Additionally, novel measurement methods were used to study gas/particle partitioning. The research conducted was highly successful and details of the key results are summarized in this report through narrative text, figures, and a complete list of publications acknowledging this grant.

Physico-Chemical Evolution of Organic Aerosol from Wildfire Emissions

Science.gov (United States)

Croteau, P.; Jathar, S.; Akherati, A.; Galang, A.; Tarun, S.; Onasch, T. B.; Lewane, L.; Herndon, S. C.; Roscioli, J. R.; Yacovitch, T. I.; Fortner, E.; Xu, W.; Daube, C.; Knighton, W. B.; Werden, B.; Wood, E.

2017-12-01

Wildfires are the largest combustion-related source of carbonaceous emissions to the atmosphere; these include direct emissions of black carbon (BC), primary organic aerosol (POA) and semi-volatile, intermediate-volatility, and volatile organic compounds (SVOCs, IVOCs, and VOCs). However, there are large uncertainties surrounding the evolution of these carbonaceous emissions as they are physically and chemically transformed in the atmosphere. To understand these transformations, we performed sixteen experiments using an environmental chamber to simulate day- and night-time chemistry of gas- and aerosol-phase emissions from 6 different fuels at the Fire Laboratory in Missoula, MT. Across the test matrix, the experiments simulated 2 to 8 hours of equivalent day-time aging (with the hydroxyl radical and ozone) or several hours of night-time aging (with the nitrate radical). Aging resulted in an average organic aerosol (OA) mass enhancement of 28% although the full range of OA mass enhancements varied between -10% and 254%. These enhancement findings were consistent with chamber and flow reactor experiments performed at the Fire Laboratory in 2010 and 2012 but, similar to previous studies, offered no evidence to link the OA mass enhancement to fuel type or oxidant exposure. Experiments simulating night-time aging resulted in an average OA mass enhancement of 10% and subsequent day-time aging resulted in a decrease in OA mass of 8%. While small, for the first time, these experiments highlighted the continuous nature of the OA evolution as the wildfire smoke cycled through night- and day-time processes. Ongoing work is focussed on (i) quantifying bulk compositional changes in OA, (ii) comparing the near-field aging simulated in this work with far-field aging simulated during the same campaign (via a mini chamber and flow tube) and (iii) integrating wildfire smoke aging datasets over the past decade to examine the relationship between OA mass enhancement ratios, modified

A study of the comparison between human and animal excretion data following inhalation exposure to plutonium 238 oxide aerosols

International Nuclear Information System (INIS)

Moss, W.D.; Martinez, G.; Gautier, M.A.

1985-01-01

Bioassay urine samples obtained since 1971 from eight Los Alamos employees, accidentally exposed by inhalation to high-fired plutonium-238 oxide aerosols, were studied and compared with excretion data obtained from Beagle dogs exposed to /sup 238/PuO/sub 2/ aerosols. The early period Pu human excretion data from the inhalation exposure were unexpected and were unlike previously studied occupational exposure urinary data obtained at Los Alamos. The initial urine samples collected on day one were below the detection limits of the analytical method (0.01 pCi). Within thirty days, however, detectible concentrations of Pu were measured in the urine for several of the exposed personnel. The amounts of Pu excreted continued to increase in each of the cases throughout the first year and the individual patterns of Pu excretion were similar. The human urinary excretion data was compared with similar excretion data obtained from an animal study conducted by the Inhalation Toxicology Research Institute (Me81). In the animal study, Beagle dogs received inhalation exposure to one of three sizes of monodisperse of polydisperse aerosol of /sup 238/PuO/sub 2/. Periodic sacrifice of pairs of dogs during the 4 years after the inhalation exposure provided data on the retention, translocation and mode of excretion of /sup 238/Pu. The comparison of human and animal /sup 238/Pu excretion data supported the observation that the excretion data were similar between the two species and that the animal excretion models can be applied to predict the human /sup 238/Pu excretion following inhalation exposure to high-fired oxides of /sup 238/Pu

Selective Oxidation Using Flame Aerosol Synthesized Iron and Vanadium-Doped Nano-TiO2

Directory of Open Access Journals (Sweden)

Zhong-Min Wang

2011-01-01

Full Text Available Selective photocatalytic oxidation of 1-phenyl ethanol to acetophenone using titanium dioxide (TiO2 raw and doped with Fe or V, prepared by flame aerosol deposition method, was investigated. The effects of metal doping on crystal phase and morphology of the synthesized nanostructured TiO2 were analyzed using XRD, TEM, Raman spectroscopy, and BET nitrogen adsorbed surface area measurement. The increase in the concentration of V and Fe reduced the crystalline structure and the anatase-to-rutile ratios of the synthesized TiO2. Synthesized TiO2 became fine amorphous powder as the Fe and V concentrations were increased to 3 and 5%, respectively. Doping V and Fe to TiO2 synthesized by the flame aerosol increased photocatalytic activity by 6 folds and 2.5 folds, respectively, compared to that of pure TiO2. It was found that an optimal doping concentration for Fe and V were 0.5% and 3%, respectively. The type and concentration of the metal dopants and the method used to add the dopant to the TiO2 are critical parameters for enhancing the activity of the resulting photocatalyst. The effects of solvents on the photocatalytic reaction were also investigated by using both water and acetonitrile as the reaction medium.

Chemical and physical transformations of organic aerosol from the photo-oxidation of open biomass burning emissions in an environmental chamber

Directory of Open Access Journals (Sweden)

C. J. Hennigan

2011-08-01

Full Text Available Smog chamber experiments were conducted to investigate the chemical and physical transformations of organic aerosol (OA during photo-oxidation of open biomass burning emissions. The experiments were carried out at the US Forest Service Fire Science Laboratory as part of the third Fire Lab at Missoula Experiment (FLAME III. We investigated emissions from 12 different fuels commonly burned in North American wildfires. The experiments feature atmospheric and plume aerosol and oxidant concentrations; aging times ranged from 3 to 4.5 h. OA production, expressed as a mass enhancement ratio (ratio of OA to primary OA (POA mass, was highly variable. OA mass enhancement ratios ranged from 2.9 in experiments where secondary OA (SOA production nearly tripled the POA concentration to 0.7 in experiments where photo-oxidation resulted in a 30 % loss of the OA mass. The campaign-average OA mass enhancement ratio was 1.7 ± 0.7 (mean ± 1σ; therefore, on average, there was substantial SOA production. In every experiment, the OA was chemically transformed. Even in experiments with net loss of OA mass, the OA became increasingly oxygenated and less volatile with aging, indicating that photo-oxidation transformed the POA emissions. Levoglucosan concentrations were also substantially reduced with photo-oxidation. The transformations of POA were extensive; using levoglucosan as a tracer for POA, unreacted POA only contributed 17 % of the campaign-average OA mass after 3.5 h of exposure to typical atmospheric hydroxyl radical (OH levels. Heterogeneous reactions with OH could account for less than half of this transformation, implying that the coupled gas-particle partitioning and reaction of semi-volatile vapors is an important and potentially dominant mechanism for POA processing. Overall, the results illustrate that biomass burning emissions are subject to extensive chemical processing in the atmosphere, and the timescale for these transformations is rapid.

Predicting Thermal Behavior of Secondary Organic Aerosols

Data.gov (United States)

U.S. Environmental Protection Agency — Volume concentrations of secondary organic aerosol (SOA) are measured in 139 steady-state, single precursor hydrocarbon oxidation experiments after passing through a...

Organic Aerosol Component (OACOMP) Value-Added Product

Energy Technology Data Exchange (ETDEWEB)

Fast, J [Pacific Northwest National Laboratory; Zhang, Q; tilp, A [Brookhaven National Laboratory; Shippert, T [Pacific Northwest National Laboratory; Parworth, C; Mei, F [Pacific Northwest National Laboratory

2013-08-23

Organic aerosol (OA, i.e., the organic fraction of particles) accounts for 10–90% of the fine aerosol mass globally and is a key determinant of aerosol radiative forcing. But atmospheric OA is poorly characterized and its life cycle insufficiently represented in models. As a result, current models are unable to simulate OA concentrations and properties accurately. This deficiency represents a large source of uncertainty in quantification of aerosol effects and prediction of future climate change. Evaluation and development of aerosol models require data products generated from field observations. Real-time, quantitative data acquired with aerosol mass spectrometers (AMS) (Canagaratna et al. 2007) are critical to this need. The AMS determines size-resolved concentrations of non-refractory (NR) species in submicrometer particles (PM1) with fast time resolution suitable for both ground-based and aircraft deployments. The high-resolution AMS (HR-AMS), which is equipped with a high mass resolution time-of-flight mass spectrometer, can be used to determine the elemental composition and oxidation degrees of OA (DeCarlo et al. 2006).

MATRIX-VBS (v1.0): Implementing an Evolving Organic Aerosol Volatility in an Aerosol Microphysics Model

Science.gov (United States)

Gao, Chloe Y.; Tsigaridis, Kostas; Bauer, Susanne E.

2017-01-01

The gas-particle partitioning and chemical aging of semi-volatile organic aerosol are presented in a newly developed box model scheme, where its effect on the growth, composition, and mixing state of particles is examined. The volatility-basis set (VBS) framework is implemented into the aerosol microphysical scheme MATRIX (Multiconfiguration Aerosol TRacker of mIXing state), which resolves mass and number aerosol concentrations and in multiple mixing-state classes. The new scheme, MATRIX-VBS, has the potential to significantly advance the representation of organic aerosols in Earth system models by improving upon the conventional representation as non-volatile particulate organic matter, often also with an assumed fixed size distribution. We present results from idealized cases representing Beijing, Mexico City, a Finnish forest, and a southeastern US forest, and investigate the evolution of mass concentrations and volatility distributions for organic species across the gas and particle phases, as well as assessing their mixing state among aerosol populations. Emitted semi-volatile primary organic aerosols evaporate almost completely in the intermediate-volatility range, while they remain in the particle phase in the low-volatility range. Their volatility distribution at any point in time depends on the applied emission factors, oxidation by OH radicals, and temperature. We also compare against parallel simulations with the original scheme, which represented only the particulate and non-volatile component of the organic aerosol, examining how differently the condensed-phase organic matter is distributed across the mixing states in the model. The results demonstrate the importance of representing organic aerosol as a semi-volatile aerosol, and explicitly calculating the partitioning of organic species between the gas and particulate phases.

Recent advances in understanding secondary organic aerosol: Implications for global climate forcing: Advances in Secondary Organic Aerosol

Energy Technology Data Exchange (ETDEWEB)

Shrivastava, Manish [Pacific Northwest National Laboratory, Richland Washington USA; Cappa, Christopher D. [Department of Civil and Environmental Engineering, University of California, Davis California USA; Fan, Jiwen [Pacific Northwest National Laboratory, Richland Washington USA; Goldstein, Allen H. [Department of Environmental Science, Policy and Management and Department of Civil and Environmental Engineering, University of California, Berkeley California USA; Guenther, Alex B. [Department of Earth System Science, University of California, Irvine California USA; Jimenez, Jose L. [Cooperative Institute for Research in Environmental Sciences and Department of Chemistry and Biochemistry, University of Colorado Boulder, Boulder Colorado USA; Kuang, Chongai [Brookhaven National Laboratory, Upton New York USA; Laskin, Alexander [Pacific Northwest National Laboratory, Richland Washington USA; Martin, Scot T. [School of Engineering and Applied Sciences and Department of Earth and Planetary Sciences, Harvard University, Cambridge Massachusetts USA; Ng, Nga Lee [School of Chemical and Biomolecular Engineering and School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta Georgia USA; Petaja, Tuukka [Department of Physics, University of Helsinki, Helsinki Finland; Pierce, Jeffrey R. [Department of Atmospheric Science, Colorado State University, Fort Collins Colorado USA; Rasch, Philip J. [Pacific Northwest National Laboratory, Richland Washington USA; Roldin, Pontus [Department of Physics, Lund University, Lund Sweden; Seinfeld, John H. [Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena California USA; Shilling, John [Pacific Northwest National Laboratory, Richland Washington USA; Smith, James N. [Department of Earth System Science, University of California, Irvine California USA; Thornton, Joel A. [Department of Atmospheric Sciences, University of Washington, Seattle Washington USA; Volkamer, Rainer [Cooperative Institute for Research in Environmental Sciences and Department of Chemistry and Biochemistry, University of Colorado Boulder, Boulder Colorado USA; Wang, Jian [Brookhaven National Laboratory, Upton New York USA; Worsnop, Douglas R. [Aerodyne Research, Inc., Billerica Massachusetts USA; Zaveri, Rahul A. [Pacific Northwest National Laboratory, Richland Washington USA; Zelenyuk, Alla [Pacific Northwest National Laboratory, Richland Washington USA; Zhang, Qi [Department of Environmental Toxicology, University of California, Davis California USA

2017-06-01

Anthropogenic emissions and land-use changes have modified atmospheric aerosol concentrations and size distributions over time. Understanding pre-industrial conditions and changes in organic aerosol due to anthropogenic activities is important because these features 1) influence estimates of aerosol radiative forcing and 2) can confound estimates of the historical response of climate to increases in greenhouse gases (e.g. the ‘climate sensitivity’). Secondary organic aerosol (SOA), formed in the atmosphere by oxidation of organic gases, represents a major fraction of global submicron-sized atmospheric organic aerosol. Over the past decade, significant advances in understanding SOA properties and formation mechanisms have occurred through a combination of laboratory and field measurements, yet current climate models typically do not comprehensively include all important SOA-relevant processes. Therefore, major gaps exist at present between current measurement-based knowledge on the one hand and model implementation of organic aerosols on the other. The critical review herein summarizes some of the important developments in understanding SOA formation that could potentially have large impacts on our understanding of aerosol radiative forcing and climate. We highlight the importance of some recently discovered processes and properties that influence the growth of SOA particles to sizes relevant for clouds and radiative forcing, including: formation of extremely low-volatility organics in the gas-phase; isoprene epoxydiols (IEPOX) multi-phase chemistry; particle-phase oligomerization; and physical properties such as viscosity. In addition, this review also highlights some of the important processes that involve interactions between natural biogenic emissions and anthropogenic emissions, such as the role of sulfate and oxides of nitrogen (NOx) on SOA formation from biogenic volatile organic compounds. Studies that relate the observed evolution of organic aerosol

Fractionation of Stable Isotopes in Atmospheric Aerosol Reactions

DEFF Research Database (Denmark)

Meusinger, Carl

-independent) fractionation processes of stable isotopes of C, N, O and S in order to investigate three different systems related to aerosols: 1. Post-depositional processes of nitrate in snow that obscure nitrate ice core records 2. Formation and aging of secondary organic aerosol generated by ozonolysis of X...... reactions and undergo complex chemical and physical changes during their lifetimes. In order to assess processes that form and alter aerosols, information provided by stable isotopes can be used to help constrain estimates on the strength of aerosol sources and sinks. This thesis studies (mass...... as required. The kndings provide important results for the studies' respective felds, including a description of the isotopic fractionation and quantum yield of nitrate photolysis in snow, equilibrium fractionation in secondary organic aerosol and fractionation constants of different oxidation pathways of SO2....

MATRIX-VBS Condensing Organic Aerosols in an Aerosol Microphysics Model

Science.gov (United States)

Gao, Chloe Y.; Tsigaridis, Konstas; Bauer, Susanne E.

2015-01-01

The condensation of organic aerosols is represented in a newly developed box-model scheme, where its effect on the growth and composition of particles are examined. We implemented the volatility-basis set (VBS) framework into the aerosol mixing state resolving microphysical scheme Multiconfiguration Aerosol TRacker of mIXing state (MATRIX). This new scheme is unique and advances the representation of organic aerosols in models in that, contrary to the traditional treatment of organic aerosols as non-volatile in most climate models and in the original version of MATRIX, this new scheme treats them as semi-volatile. Such treatment is important because low-volatility organics contribute significantly to the growth of particles. The new scheme includes several classes of semi-volatile organic compounds from the VBS framework that can partition among aerosol populations in MATRIX, thus representing the growth of particles via condensation of low volatility organic vapors. Results from test cases representing Mexico City and a Finish forrest condistions show good representation of the time evolutions of concentration for VBS species in the gas phase and in the condensed particulate phase. Emitted semi-volatile primary organic aerosols evaporate almost completely in the high volatile range, and they condense more efficiently in the low volatility range.

Defect-induced magnetism in undoped and Mn-doped wide band gapzinc oxide grown by aerosol spray pyrolysis

CSIR Research Space (South Africa)

Motaung, DE

2014-08-01

Full Text Available Surface Science Vol. 311, pp 14-26 Defect-induced magnetism in undoped and Mn-doped wide band gapzinc oxide grown by aerosol spray pyrolysis D.E. Motaunga,∗, I. Kortidise, D. Papadakie, S.S. Nkosib,∗∗, G.H. Mhlongoa,J. Wesley-Smitha, G.F. Malgasc, B....W. Mwakikungaa, E. Coetseed, H.C. Swartd,G. Kiriakidise,f, S.S. Raya aDST/CSIR Nanotechnology Innovation Centre, National Centre for Nano-Structured Materials, Council for Scientific and Industrial Research, P.O. Box 395,Pretoria 0001, South Africa b...

Atmospheric oxidation of 1,3-butadiene: characterization of gas and aerosol reaction products and implication for PM2.5

Science.gov (United States)

Jaoui, M.; Lewandowski, M.; Docherty, K.; Offenberg, J. H.; Kleindienst, T. E.

2014-06-01

-phase photooxidation products have also been examined. The contribution of SOA products from 13BD oxidation to ambient PM2.5 was investigated by analyzing a series of ambient PM2.5 samples collected in several locations around the United States. In addition to the occurrence of several organic compounds in field and laboratory samples, glyceric acid, d-threitol, erythritol, erythrose, and threonic acid were found to originate only from the oxidation of 13BD based on our previous experiments involving chamber oxidation of a series of hydrocarbons. Initial attempts have been made to quantify the concentrations of these compounds. The average concentrations of these compounds in ambient PM2.5 samples from the California Research at the Nexus of Air Quality and Climate Change (CalNex) study ranged from 0 to approximately 14.1 ng m-3. The occurrence of several other compounds in both laboratory and field samples suggests that SOA originating from 13BD oxidation could contribute to the ambient aerosol mainly in areas with high 13BD emission rates.

Origins and composition of fine atmospheric carbonaceous aerosol in the Sierra Nevada Mountains, California

Directory of Open Access Journals (Sweden)

D. R. Worton

2011-10-01

Full Text Available In this paper we report chemically resolved measurements of organic aerosol (OA and related tracers during the Biosphere Effects on Aerosols and Photochemistry Experiment (BEARPEX at the Blodgett Forest Research Station, California from 15 August–10 October 2007. OA contributed the majority of the mass to the fine atmospheric particles and was predominately oxygenated (OOA. The highest concentrations of OA were during sporadic wildfire influence when aged plumes were impacting the site. In situ measurements of particle phase molecular markers were dominated by secondary compounds and along with gas phase compounds could be categorized into six factors or sources: (1 aged biomass burning emissions and oxidized urban emissions, (2 oxidized urban emissions (3 oxidation products of monoterpene emissions, (4 monoterpene emissions, (5 anthropogenic emissions and (6 local methyl chavicol emissions and oxidation products. There were multiple biogenic components that contributed to OA at this site whose contributions varied diurnally, seasonally and in response to changing meteorological conditions, e.g. temperature and precipitation events. Concentrations of isoprene oxidation products were larger when temperatures were higher during the first half of the campaign (15 August–12 September due to more substantial emissions of isoprene and enhanced photochemistry. The oxidation of methyl chavicol, an oxygenated terpene emitted by ponderosa pine trees, contributed similarly to OA throughout the campaign. In contrast, the abundances of monoterpene oxidation products in the particle phase were greater during the cooler conditions in the latter half of the campaign (13 September–10 October, even though emissions of the precursors were lower, although the mechanism is not known. OA was correlated with the anthropogenic tracers 2-propyl nitrate and carbon monoxide (CO, consistent with previous observations, while being comprised of mostly non-fossil carbon

Aerosol characterization over the southeastern United States using high resolution aerosol mass spectrometry: spatial and seasonal variation of aerosol composition, sources, and organic nitrates

Science.gov (United States)

Xu, L.; Suresh, S.; Guo, H.; Weber, R. J.; Ng, N. L.

2015-04-01

We deployed a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and an Aerosol Chemical Speciation Monitor (ACSM) to characterize the chemical composition of submicron non-refractory particles (NR-PM1) in the southeastern US. Measurements were performed in both rural and urban sites in the greater Atlanta area, GA and Centreville, AL for approximately one year, as part of Southeastern Center of Air Pollution and Epidemiology study (SCAPE) and Southern Oxidant and Aerosol Study (SOAS). Organic aerosol (OA) accounts for more than half of NR1 mass concentration regardless of sampling sites and seasons. Positive matrix factorization (PMF) analysis of HR-ToF-AMS measurements identified various OA sources, depending on location and season. Hydrocarbon-like OA (HOA) and cooking OA (COA) have important but not dominant contributions to total OA in urban sites. Biomass burning OA (BBOA) concentration shows a distinct seasonal variation with a larger enhancement in winter than summer. We find a good correlation between BBOA and brown carbon, indicating biomass burning is an important source for brown carbon, although an additional, unidentified brown carbon source is likely present at the rural Yorkville site. Isoprene-derived OA (Isoprene-OA) is only deconvolved in warmer months and contributes 18-36% of total OA. The presence of Isoprene-OA factor in urban sites is more likely from local production in the presence of NOx than transport from rural sites. More-oxidized and less-oxidized oxygenated organic aerosol (MO-OOA and LO-OOA, respectively) are dominant fractions (47-79%) of OA in all sites. MO-OOA correlates well with ozone in summer, but not in winter, indicating MO-OOA sources may vary with seasons. LO-OOA, which reaches a daily maximum at night, correlates better with estimated nitrate functionality from organic nitrates than total nitrates. Based on the HR-ToF-AMS measurements, we estimate that the nitrate functionality from organic nitrates

Organic molecular composition of marine aerosols over the Arctic Ocean in summer: contributions of primary emission and secondary aerosol formation

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P. Q. Fu

2013-02-01

Full Text Available Organic molecular composition of marine aerosol samples collected during the MALINA cruise in the Arctic Ocean was investigated by gas chromatography/mass spectrometry. More than 110 individual organic compounds were determined in the samples and were grouped into different compound classes based on the functionality and sources. The concentrations of total quantified organics ranged from 7.3 to 185 ng m⁻³ (mean 47.6 ng m⁻³, accounting for 1.8–11.0% (4.8% of organic carbon in the marine aerosols. Primary saccharides were found to be dominant organic compound class, followed by secondary organic aerosol (SOA tracers formed from the oxidation of biogenic volatile organic compounds (VOCs such as isoprene, α-pinene and β-caryophyllene. Mannitol, the specific tracer for airborne fungal spores, was detected as the most abundant organic species in the samples with a concentration range of 0.052–53.3 ng m⁻³ (9.2 ng m⁻³, followed by glucose, arabitol, and the isoprene oxidation products of 2-methyltetrols. Biomass burning tracers such as levoglucosan are evident in all samples with trace levels. On the basis of the tracer-based method for the estimation of fungal-spore OC and biogenic secondary organic carbon (SOC, we estimate that an average of 10.7% (up to 26.2% of the OC in the marine aerosols was due to the contribution of fungal spores, followed by the contribution of isoprene SOC (mean 3.8% and α-pinene SOC (2.9%. In contrast, only 0.19% of the OC was due to the photooxidation of β-caryophyllene. This study indicates that primary organic aerosols from biogenic emissions, both from long-range transport of mid-latitude aerosols and from sea-to-air emission of marine organics, as well as secondary organic aerosols formed from the photooxidation of biogenic VOCs are important factors controlling the organic chemical composition of marine aerosols in the Arctic Ocean.

Variation in aerosol nucleation and growth in coal-fired power plant plumes due to background aerosol, meteorology and emissions: sensitivity analysis and parameterization.

Science.gov (United States)

Stevens, R. G.; Lonsdale, C. L.; Brock, C. A.; Reed, M. K.; Crawford, J. H.; Holloway, J. S.; Ryerson, T. B.; Huey, L. G.; Nowak, J. B.; Pierce, J. R.

2012-04-01

New-particle formation in the plumes of coal-fired power plants and other anthropogenic sulphur sources may be an important source of particles in the atmosphere. It remains unclear, however, how best to reproduce this formation in global and regional aerosol models with grid-box lengths that are 10s of kilometres and larger. The predictive power of these models is thus limited by the resultant uncertainties in aerosol size distributions. In this presentation, we focus on sub-grid sulphate aerosol processes within coal-fired power plant plumes: the sub-grid oxidation of SO2 with condensation of H2SO4 onto newly-formed and pre-existing particles. Based on the results of the System for Atmospheric Modelling (SAM), a Large-Eddy Simulation/Cloud-Resolving Model (LES/CRM) with online TwO Moment Aerosol Sectional (TOMAS) microphysics, we develop a computationally efficient, but physically based, parameterization that predicts the characteristics of aerosol formed within coal-fired power plant plumes based on parameters commonly available in global and regional-scale models. Given large-scale mean meteorological parameters, emissions from the power plant, mean background condensation sink, and the desired distance from the source, the parameterization will predict the fraction of the emitted SO2 that is oxidized to H2SO4, the fraction of that H2SO4 that forms new particles instead of condensing onto preexisting particles, the median diameter of the newly-formed particles, and the number of newly-formed particles per kilogram SO2 emitted. We perform a sensitivity analysis of these characteristics of the aerosol size distribution to the meteorological parameters, the condensation sink, and the emissions. In general, new-particle formation and growth is greatly reduced during polluted conditions due to the large preexisting aerosol surface area for H2SO4 condensation and particle coagulation. The new-particle formation and growth rates are also a strong function of the

Potential of secondary aerosol formation from Chinese gasoline engine exhaust.

Science.gov (United States)

Du, Zhuofei; Hu, Min; Peng, Jianfei; Guo, Song; Zheng, Rong; Zheng, Jing; Shang, Dongjie; Qin, Yanhong; Niu, He; Li, Mengren; Yang, Yudong; Lu, Sihua; Wu, Yusheng; Shao, Min; Shuai, Shijin

2018-04-01

Light-duty gasoline vehicles have drawn public attention in China due to their significant primary emissions of particulate matter and volatile organic compounds (VOCs). However, little information on secondary aerosol formation from exhaust for Chinese vehicles and fuel conditions is available. In this study, chamber experiments were conducted to quantify the potential of secondary aerosol formation from the exhaust of a port fuel injection gasoline engine. The engine and fuel used are common in the Chinese market, and the fuel satisfies the China V gasoline fuel standard. Substantial secondary aerosol formation was observed during a 4-5hr simulation, which was estimated to represent more than 10days of equivalent atmospheric photo-oxidation in Beijing. As a consequence, the extreme case secondary organic aerosol (SOA) production was 426±85mg/kg-fuel, with high levels of precursors and OH exposure. The low hygroscopicity of the aerosols formed inside the chamber suggests that SOA was the dominant chemical composition. Fourteen percent of SOA measured in the chamber experiments could be explained through the oxidation of speciated single-ring aromatics. Unspeciated precursors, such as intermediate-volatility organic compounds and semi-volatile organic compounds, might be significant for SOA formation from gasoline VOCs. We concluded that reductions of emissions of aerosol precursor gases from vehicles are essential to mediate pollution in China. Copyright © 2017. Published by Elsevier B.V.

Secondary Aerosol Formation over the ESCOMPTE Area: Results from airborne Aerosol and Trace Gas Measurements

Science.gov (United States)

van Dingenen, R.; Martins-Dos Santos, S.; Putaud, J. P.; Allet, C.; Bretton, E.; Perros, P.

2003-04-01

From June 10th to July 14th 2001, the ESCOMPTE campaign took place in the Marseille-Berre area in Southern France. The goal of the campaign was to produce a high quality 3-D data base from emissions, transport and air composition measurements during urban photochemical pollution episodes at the meso-scale. The CAATER AEROPLUM project was embedded within this international field campaign. AEROPLUM aimed at mapping size distributions of aerosols and photo-oxidants in the mixed layer over the ESCOMPTE domain, using the ARAT Fokker 27 as measurement platform. Aircraft sub-micrometer aerosol measurements are validated during overpasses against ground-based measurements, carried out with similar instrumentation. We will present and discuss data during periods of seabreeze, transporting coastal industrial and urban pollution land-inwards. This leads to intense photochemical activity, evidenced by elevated O_3 concentrations and aerosol levels.

Updated aerosol module and its application to simulate secondary organic aerosols during IMPACT campaign May 2008

Directory of Open Access Journals (Sweden)

Y. P. Li

2013-07-01

Full Text Available The formation of Secondary organic aerosol (SOA was simulated with the Secondary ORGanic Aerosol Model (SORGAM by a classical gas-particle partitioning concept, using the two-product model approach, which is widely used in chemical transport models. In this study, we extensively updated SORGAM including three major modifications: firstly, we derived temperature dependence functions of the SOA yields for aromatics and biogenic VOCs (volatile organic compounds, based on recent chamber studies within a sophisticated mathematic optimization framework; secondly, we implemented the SOA formation pathways from photo oxidation (OH initiated of isoprene; thirdly, we implemented the SOA formation channel from NO3-initiated oxidation of reactive biogenic hydrocarbons (isoprene and monoterpenes. The temperature dependence functions of the SOA yields were validated against available chamber experiments, and the updated SORGAM with temperature dependence functions was evaluated with the chamber data. Good performance was found with the normalized mean error of less than 30%. Moreover, the whole updated SORGAM module was validated against ambient SOA observations represented by the summed oxygenated organic aerosol (OOA concentrations abstracted from aerosol mass spectrometer (AMS measurements at a rural site near Rotterdam, the Netherlands, performed during the IMPACT campaign in May 2008. In this case, we embedded both the original and the updated SORGAM module into the EURopean Air pollution and Dispersion-Inverse Model (EURAD-IM, which showed general good agreements with the observed meteorological parameters and several secondary products such as O3, sulfate and nitrate. With the updated SORGAM module, the EURAD-IM model also captured the observed SOA concentrations reasonably well especially those during nighttime. In contrast, the EURAD-IM model before update underestimated the observations by a factor of up to 5. The large improvements of the modeled

Characterisation of a uranium fire aerosol

International Nuclear Information System (INIS)

Leuscher, A.H.

1976-01-01

Uranium swarf, which can burn spontaneously in air, creates an aerosol which is chemically toxic and radiotoxic. The uptake of uranium oxide in the respiratory system is determined to a large extent by the characteristics of the aerosol. A study has been made of the methods by which aerosols can be characterised. The different measured and defined characteristics of particles are given. The normal and lognormal particle size distributions are discussed. Shape factors interrelating characteristics are explained. Experimental techniques for the characterisation of an aerosol are discussed, as well as the instruments that have been used in this study; namely the Andersen impactor, point-to-plane electrostatic precipitator and the Pollak counter. Uranium swarf was made to burn with a heated filament, and the resulting aerosol was measured. Optical and electron microscopy have been used for the determination of the projected area diameters, and the aerodynamic diameters have been determined with the impactor. The uranium fire aerosol can be represented by a bimodal, or monomodal, lognormal particle size distribution depending on the way in which the swarf burns. The determined activity median aerodynamic diameter of the two peaks were 0,49μm and 6,0μm respectively [af

Determination of the biogenic secondary organic aerosol fraction in the boreal forest by NMR spectroscopy

Directory of Open Access Journals (Sweden)

E. Finessi

2012-01-01

Full Text Available The study investigates the sources of fine organic aerosol (OA in the boreal forest, based on measurements including both filter sampling (PM₁ and online methods and carried out during a one-month campaign held in Hyytiälä, Finland, in spring 2007. Two aerosol mass spectrometers (Q-AMS, ToF-AMS were employed to measure on-line concentrations of major non-refractory aerosol species, while the water extracts of the filter samples were analyzed by nuclear magnetic resonance (NMR spectroscopy for organic functional group characterization of the polar organic fraction of the aerosol. AMS and NMR spectra were processed separately by non-negative factorization algorithms, in order to apportion the main components underlying the submicrometer organic aerosol composition and depict them in terms of both mass fragmentation patterns and functional group compositions.

The NMR results supported the AMS speciation of oxidized organic aerosol (OOA into two main fractions, which could be generally labelled as more and less oxidized organics. The more oxidized component was characterized by a mass spectrum dominated by the m/z 44 peak, and in parallel by a NMR spectrum showing aromatic and aliphatic backbones highly substituted with oxygenated functional groups (carbonyls/carboxyls and hydroxyls. Such component, contributing on average 50% of the OA mass throughout the observing period, was associated with pollution outbreaks from the Central Europe. The less oxidized component was enhanced in concomitance with air masses originating from the North-to-West sector, in agreement with previous investigations conducted at this site. NMR factor analysis was able to separate two distinct components under the less oxidized fraction of OA. One of these NMR-factors was associated with the formation of terrestrial biogenic secondary organic aerosol (BSOA, based on the comparison with spectral profiles obtained from laboratory experiments of

Characterization of biogenic secondary organic aerosols using statistical methods; Charakterisierung Biogener Sekundaerer Organischer Aerosole mit Statistischen Methoden

Energy Technology Data Exchange (ETDEWEB)

Spindler, Christian

2010-07-01

Atmospheric aerosols have important influence on the radiation balance of the Earth, on visibility and human health. Secondary organic aerosol is formed from gas-to-particle conversion of oxidized volatile organic compounds. A dominant fraction of the gases originates from plant emissions, making biogenic secondary organic aerosol (BSOA) an especially important constituent of the atmosphere. Knowing the chemical composition of BSOA particles is crucial for a thorough understanding of aerosol processes in the environment. In this work, the chemical composition of BSOA particles was measured with aerosol mass spectrometry and analyzed with statistical methods. The experimental part of the work comprises process studies of the formation and aging of biogenic aerosols in simulation chambers. Using a plant chamber, real tree emissions were used to produce particles in a way close to conditions in forest environments. In the outdoor chamber SAPHIR, OH-radicals were produced from the photooxidation of ozone under illumination with natural sunlight. Here, BSOA was produced from defined mixtures of mono- and sesquiterpenes that represent boreal forest emissions. A third kind of experiments was performed in the indoor chamber AIDA. Here, particles were produced from ozonolysis of single monoterpenes and aged by condensing OH-oxidation products. Two aerosol mass spectrometers (AMS) were used to measure the chemical composition of the particles. One of the instruments is equipped with a quadrupole mass spectrometer providing unit mass resolution. The second instrument contains a time-of-flight mass spectrometer and provides mass resolution sufficient to distinguish different fragments with the same nominal mass. Aerosol mass spectra obtained with these instruments are strongly fragmented due to electron impact ionization of the evaporated molecules. In addition, typical BSOA mass spectra are very similar to each other. In order to get a more detailed knowledge about the mass

Aerosol chemistry over a high altitude station at northeastern Himalayas, India.

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Abhijit Chatterjee

Full Text Available BACKGROUND: There is an urgent need for an improved understanding of the sources, distributions and properties of atmospheric aerosol in order to control the atmospheric pollution over northeastern Himalayas where rising anthropogenic interferences from rapid urbanization and development is becoming an increasing concern. METHODOLOGY/PRINCIPAL FINDINGS: An extensive aerosol sampling program was conducted in Darjeeling (altitude approximately 2200 meter above sea level (masl, latitude 27 degrees 01'N and longitude 88 degrees 15'E, a high altitude station in northeastern Himalayas, during January-December 2005. Samples were collected using a respirable dust sampler and a fine dust sampler simultaneously. Ion chromatograph was used to analyze the water soluble ionic species of aerosol. The average concentrations of fine and coarse mode aerosol were found to be 29.5+/-20.8 microg m(-3 and 19.6+/-11.1 microg m(-3 respectively. Fine mode aerosol dominated during dry seasons and coarse mode aerosol dominated during monsoon. Nitrate existed as NH(4NO(3 in fine mode aerosol during winter and as NaNO(3 in coarse mode aerosol during monsoon. Gas phase photochemical oxidation of SO(2 during premonsoon and aqueous phase oxidation during winter and postmonsoon were the major pathways for the formation of SO(4(2- in the atmosphere. Long range transport of dust aerosol from arid regions of western India was observed during premonsoon. The acidity of fine mode aerosol was higher in dry seasons compared to monsoon whereas the coarse mode acidity was higher in monsoon compared to dry seasons. Biomass burning, vehicular emissions and dust particles were the major types of aerosol from local and continental regions whereas sea salt particles were the major types of aerosol from marine source regions. CONCLUSIONS/SIGNIFICANCE: The year-long data presented in this paper provide substantial improvements to the heretofore poor knowledge regarding aerosol chemistry over

Aerosol chemistry over a high altitude station at northeastern Himalayas, India.

Science.gov (United States)

Chatterjee, Abhijit; Adak, Anandamay; Singh, Ajay K; Srivastava, Manoj K; Ghosh, Sanjay K; Tiwari, Suresh; Devara, Panuganti C S; Raha, Sibaji

2010-06-16

There is an urgent need for an improved understanding of the sources, distributions and properties of atmospheric aerosol in order to control the atmospheric pollution over northeastern Himalayas where rising anthropogenic interferences from rapid urbanization and development is becoming an increasing concern. An extensive aerosol sampling program was conducted in Darjeeling (altitude approximately 2200 meter above sea level (masl), latitude 27 degrees 01'N and longitude 88 degrees 15'E), a high altitude station in northeastern Himalayas, during January-December 2005. Samples were collected using a respirable dust sampler and a fine dust sampler simultaneously. Ion chromatograph was used to analyze the water soluble ionic species of aerosol. The average concentrations of fine and coarse mode aerosol were found to be 29.5+/-20.8 microg m(-3) and 19.6+/-11.1 microg m(-3) respectively. Fine mode aerosol dominated during dry seasons and coarse mode aerosol dominated during monsoon. Nitrate existed as NH(4)NO(3) in fine mode aerosol during winter and as NaNO(3) in coarse mode aerosol during monsoon. Gas phase photochemical oxidation of SO(2) during premonsoon and aqueous phase oxidation during winter and postmonsoon were the major pathways for the formation of SO(4)(2-) in the atmosphere. Long range transport of dust aerosol from arid regions of western India was observed during premonsoon. The acidity of fine mode aerosol was higher in dry seasons compared to monsoon whereas the coarse mode acidity was higher in monsoon compared to dry seasons. Biomass burning, vehicular emissions and dust particles were the major types of aerosol from local and continental regions whereas sea salt particles were the major types of aerosol from marine source regions. The year-long data presented in this paper provide substantial improvements to the heretofore poor knowledge regarding aerosol chemistry over northeastern Himalayas, and should be useful to policy makers in making control

Aerosol can puncture device operational test plan

International Nuclear Information System (INIS)

Leist, K.J.

1994-01-01

Puncturing of aerosol cans is performed in the Waste Receiving and Processing Facility Module 1 (WRAP 1) process as a requirement of the waste disposal acceptance criteria for both transuranic (TRU) waste and low-level waste (LLW). These cans have contained such things as paints, lubricating oils, paint removers, insecticides, and cleaning supplies which were used in radioactive facilities. Due to Westinghouse Hanford Company (WHC) Fire Protection concerns of the baseline system's fire/explosion proof characteristics, a study was undertaken to compare the baseline system's design to commercially available puncturing devices. While the study found no areas which might indicate a risk of fire or explosion, WHC Fire Protection determined that the puncturing system must have a demonstrated record of safe operation. This could be obtained either by testing the baseline design by an independent laboratory, or by substituting a commercially available device. As a result of these efforts, the commercially available Aerosolv can puncturing device was chosen to replace the baseline design. Two concerns were raised with the system. Premature blinding of the coalescing/carbon filter, due to its proximity to the puncture and draining operation; and overpressurization of the collection bottle due to its small volume and by blinding of the filter assembly. As a result of these concerns, testing was deemed necessary. The objective of this report is to outline test procedures for the Aerosolv

Aerosol characterization over the southeastern United States using high-resolution aerosol mass spectrometry: spatial and seasonal variation of aerosol composition and sources with a focus on organic nitrates

Science.gov (United States)

Xu, L.; Suresh, S.; Guo, H.; Weber, R. J.; Ng, N. L.

2015-07-01

We deployed a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and an Aerosol Chemical Speciation Monitor (ACSM) to characterize the chemical composition of submicron non-refractory particulate matter (NR-PM1) in the southeastern USA. Measurements were performed in both rural and urban sites in the greater Atlanta area, Georgia (GA), and Centreville, Alabama (AL), for approximately 1 year as part of Southeastern Center for Air Pollution and Epidemiology study (SCAPE) and Southern Oxidant and Aerosol Study (SOAS). Organic aerosol (OA) accounts for more than half of NR-PM1 mass concentration regardless of sampling sites and seasons. Positive matrix factorization (PMF) analysis of HR-ToF-AMS measurements identified various OA sources, depending on location and season. Hydrocarbon-like OA (HOA) and cooking OA (COA) have important, but not dominant, contributions to total OA in urban sites (i.e., 21-38 % of total OA depending on site and season). Biomass burning OA (BBOA) concentration shows a distinct seasonal variation with a larger enhancement in winter than summer. We find a good correlation between BBOA and brown carbon, indicating biomass burning is an important source for brown carbon, although an additional, unidentified brown carbon source is likely present at the rural Yorkville site. Isoprene-derived OA factor (isoprene-OA) is only deconvolved in warmer months and contributes 18-36 % of total OA. The presence of isoprene-OA factor in urban sites is more likely from local production in the presence of NOx than transport from rural sites. More-oxidized and less-oxidized oxygenated organic aerosol (MO-OOA and LO-OOA, respectively) are dominant fractions (47-79 %) of OA in all sites. MO-OOA correlates well with ozone in summer but not in winter, indicating MO-OOA sources may vary with seasons. LO-OOA, which reaches a daily maximum at night, correlates better with estimated nitrate functionality from organic nitrates than total nitrates. Based

Insights into Submicron Aerosol Composition and Sources from the WINTER Aircraft Campaign Over the Eastern US.

Science.gov (United States)

Schroder, J. C.; Campuzano Jost, P.; Day, D. A.; Fibiger, D. L.; McDuffie, E. E.; Blake, N. J.; Hills, A. J.; Hornbrook, R. S.; Apel, E. C.; Weinheimer, A. J.; Campos, T. L.; Brown, S. S.; Jimenez, J. L.

2015-12-01

The WINTER aircraft campaign was a recent field experiment to probe the sources and evolution of gas pollutants and aerosols in Northeast US urban and industrial plumes during the winter. A highly customized Aerodyne aerosol mass spectrometer (AMS) was flown on the NCAR C-130 to characterize submicron aerosol composition and evolution. Thirteen research flights were conducted covering a wide range of conditions, including rural, urban, and marine environments during day and night. Organic aerosol (OA) was a large component of the submicron aerosol in the boundary layer. The fraction of OA (fOA) was smaller (35-40%) than in recent US summer campaigns (~60-70%). Biomass burning was observed to be an important source of OA in the boundary layer, which is consistent with recent wintertime studies that show a substantial contribution of residential wood burning to the OA loadings. OA oxygenation (O/C ratio) shows a broad distribution with a substantial fraction of smaller O/C ratios when compared to previous summertime campaigns. Since measurements were rarely made very close to primary sources (i.e. directly above urban areas), this is consistent with oxidative chemistry being slower during winter. SOA formation and aging in the NYC plume was observed during several flights and compared with summertime results from LA (CalNex) and Mexico City (MILAGRO). Additionally, an oxidation flow reactor (OFR) capable of oxidizing ambient air up to several equivalent days of oxidation was deployed for the first time in an aircraft platform. The aerosol outflow of the OFR was sampled with the AMS to provide real-time snapshots of the potential for aerosol formation and aging. For example, a case study of a flight through the Ohio River valley showed evidence of oxidation of SO2 to sulfate. The measured sulfate enhancements were in good agreement with our OFR chemical model. OFR results for SOA will be discussed.

In situ secondary organic aerosol formation from ambient pine forest air using an oxidation flow reactor

Science.gov (United States)

Palm, Brett B.; Campuzano-Jost, Pedro; Ortega, Amber M.; Day, Douglas A.; Kaser, Lisa; Jud, Werner; Karl, Thomas; Hansel, Armin; Hunter, James F.; Cross, Eben S.; Kroll, Jesse H.; Peng, Zhe; Brune, William H.; Jimenez, Jose L.

2016-03-01

An oxidation flow reactor (OFR) is a vessel inside which the concentration of a chosen oxidant can be increased for the purpose of studying SOA formation and aging by that oxidant. During the BEACHON-RoMBAS (Bio-hydro-atmosphere interactions of Energy, Aerosols, Carbon, H2O, Organics & Nitrogen-Rocky Mountain Biogenic Aerosol Study) field campaign, ambient pine forest air was oxidized by OH radicals in an OFR to measure the amount of SOA that could be formed from the real mix of ambient SOA precursor gases, and how that amount changed with time as precursors changed. High OH concentrations and short residence times allowed for semicontinuous cycling through a large range of OH exposures ranging from hours to weeks of equivalent (eq.) atmospheric aging. A simple model is derived and used to account for the relative timescales of condensation of low-volatility organic compounds (LVOCs) onto particles; condensational loss to the walls; and further reaction to produce volatile, non-condensing fragmentation products. More SOA production was observed in the OFR at nighttime (average 3 µg m-3 when LVOC fate corrected) compared to daytime (average 0.9 µg m-3 when LVOC fate corrected), with maximum formation observed at 0.4-1.5 eq. days of photochemical aging. SOA formation followed a similar diurnal pattern to monoterpenes, sesquiterpenes, and toluene+p-cymene concentrations, including a substantial increase just after sunrise at 07:00 local time. Higher photochemical aging (> 10 eq. days) led to a decrease in new SOA formation and a loss of preexisting OA due to heterogeneous oxidation followed by fragmentation and volatilization. When comparing two different commonly used methods of OH production in OFRs (OFR185 and OFR254-70), similar amounts of SOA formation were observed. We recommend the OFR185 mode for future forest studies. Concurrent gas-phase measurements of air after OH oxidation illustrate the decay of primary VOCs, production of small oxidized organic

In situ secondary organic aerosol formation from ambient pine forest air using an oxidation flow reactor

Directory of Open Access Journals (Sweden)

B. B. Palm

2016-03-01

Full Text Available An oxidation flow reactor (OFR is a vessel inside which the concentration of a chosen oxidant can be increased for the purpose of studying SOA formation and aging by that oxidant. During the BEACHON-RoMBAS (Bio-hydro-atmosphere interactions of Energy, Aerosols, Carbon, H2O, Organics & Nitrogen–Rocky Mountain Biogenic Aerosol Study field campaign, ambient pine forest air was oxidized by OH radicals in an OFR to measure the amount of SOA that could be formed from the real mix of ambient SOA precursor gases, and how that amount changed with time as precursors changed. High OH concentrations and short residence times allowed for semicontinuous cycling through a large range of OH exposures ranging from hours to weeks of equivalent (eq. atmospheric aging. A simple model is derived and used to account for the relative timescales of condensation of low-volatility organic compounds (LVOCs onto particles; condensational loss to the walls; and further reaction to produce volatile, non-condensing fragmentation products. More SOA production was observed in the OFR at nighttime (average 3 µg m−3 when LVOC fate corrected compared to daytime (average 0.9 µg m−3 when LVOC fate corrected, with maximum formation observed at 0.4–1.5 eq. days of photochemical aging. SOA formation followed a similar diurnal pattern to monoterpenes, sesquiterpenes, and toluene+p-cymene concentrations, including a substantial increase just after sunrise at 07:00 local time. Higher photochemical aging (> 10 eq. days led to a decrease in new SOA formation and a loss of preexisting OA due to heterogeneous oxidation followed by fragmentation and volatilization. When comparing two different commonly used methods of OH production in OFRs (OFR185 and OFR254-70, similar amounts of SOA formation were observed. We recommend the OFR185 mode for future forest studies. Concurrent gas-phase measurements of air after OH oxidation illustrate the decay of primary VOCs, production

Hybrid plasma-catalytic reforming of ethanol aerosol

International Nuclear Information System (INIS)

Solomenko, O.V.; Nedybaliuk, O.A.; Chernyak, V.Ya.; Iukhymenko, V.V.; Veremii, Iu.P.; Iukhymenko, K.V.; Martysh, E.V.; Fedirchyk, I.I.; Demchina, V.P.; Levko, D.S.; Tsymbalyuk, O.M.; Liptuga, A.I.; Dragnev, S.V.

2015-01-01

Hybrid plasma-catalytic reforming of the ethanol aerosol with plasma activation of only the oxidant (air) was studied. Part of the oxidant (∼20%) was activated by means of rotational gliding arc with solid electrodes and injected into the reaction (pyrolytic) chamber as a plasma torch. This part of the oxidant interacted with a mixture of hydrocarbons and the rest of the oxidant (∼80%) in the reaction chamber. Temperature changes in the reaction chamber, the composition of the synthesis-gas and the products of synthesis-gas combustion were analyzed

Modeling organic aerosol concentrations and properties during winter 2014 in the northwestern Mediterranean region

OpenAIRE

Chrit, Mounir; Sartelet, Karine; Sciare, Jean; Majdi, Marwa; Nicolas, José; Petit, Jean-Eudes; Dulac, François

2018-01-01

Organic aerosols are measured at a remote site (Ersa) on Corsica Cape in the northwestern Mediterranean basin during the Chemistry-Aerosol Mediterranean Experiment (CharMEx) winter campaign of 2014, when high organic concentrations from anthropogenic origin are observed. This work aims at representing the observed organic aerosol concentrations and properties (oxidation state) using the air-quality model Polyphemus with a surrogate approach for secondary organic aerosol (SOA) formation. Becau...

Interpersonal Transport of Expiratory Aerosols among Three Manikins in a Full-Scale Test Room

DEFF Research Database (Denmark)

Liu, Li; Nielsen, Peter Vilhelm; Jensen, Rasmus Lund

2014-01-01

This study focuses on occupants’ exposure of aerosols exhaled by one susceptible in a full-scale test room. Three breathing thermal manikins are standing in the middle of room and both the process in the microenvironment and in the macroenvironment are considered. A diffusive ceiling has been...

Generation and characterization of biological aerosols for laser measurements

Energy Technology Data Exchange (ETDEWEB)

Cheng, Yung-Sung; Barr, E.B.

1995-12-01

Concerns for proliferation of biological weapons including bacteria, fungi, and viruses have prompted research and development on methods for the rapid detection of biological aerosols in the field. Real-time instruments that can distinguish biological aerosols from background dust would be especially useful. Sandia National Laboratories (SNL) is developing a laser-based, real-time instrument for rapid detection of biological aerosols, and ITRI is working with SNL scientists and engineers to evaluate this technology for a wide range of biological aerosols. This paper describes methods being used to generate the characterize the biological aerosols for these tests. In summary, a biosafe system has been developed for generating and characterizing biological aerosols and using those aerosols to test the SNL laser-based real-time instrument. Such tests are essential in studying methods for rapid detection of airborne biological materials.

Organic aerosol in the summertime southeastern United States: components and their link to volatility distribution, oxidation state and hygroscopicity

Directory of Open Access Journals (Sweden)

E. Kostenidou

2018-04-01

Full Text Available The volatility distribution of the organic aerosol (OA and its sources during the Southern Oxidant and Aerosol Study (SOAS; Centreville, Alabama was constrained using measurements from an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS and a thermodenuder (TD. Positive matrix factorization (PMF analysis was applied on both the ambient and thermodenuded high-resolution mass spectra, leading to four factors: more oxidized oxygenated OA (MO-OOA, less oxidized oxygenated OA (LO-OOA, an isoprene epoxydiol (IEPOX-related factor (isoprene-OA and biomass burning OA (BBOA. BBOA had the highest mass fraction remaining (MFR at 100 °C, followed by the isoprene-OA, and the LO-OOA. Surprisingly the MO-OOA evaporated the most in the TD. The estimated effective vaporization enthalpies assuming an evaporation coefficient equal to unity were 58 ± 13 kJ mol−1 for the LO-OOA, 89 ± 10 kJ mol−1 for the MO-OOA, 55 ± 11 kJ mol−1 for the BBOA, and 63 ± 15 kJ mol−1 for the isoprene-OA. The estimated volatility distribution of all factors covered a wide range including both semi-volatile and low-volatility components. BBOA had the lowest average volatility of all factors, even though it had the lowest O  :  C ratio among all factors. LO-OOA was the more volatile factor and its high MFR was due to its low enthalpy of vaporization according to the model. The isoprene-OA factor had intermediate volatility, quite higher than suggested by a few other studies. The analysis suggests that deducing the volatility of a factor only from its MFR could lead to erroneous conclusions. The oxygen content of the factors can be combined with their estimated volatility and hygroscopicity to provide a better view of their physical properties.

Meteorological support for aerosol radiometers: special aerosol sources

Energy Technology Data Exchange (ETDEWEB)

Belkina, S.K.; Zalmanzon, Yu.E.; Kuznetsov, Yu.V.; Fertman, D.E.

1988-07-01

A new method is described for transfer of the measure of unit volume activity of radioactive aerosols from the state special standard to the working instruments in the stage of regular operation. The differences from existing methods are examined. The principal distinction of the new method is the possibility of direct (rather than through the conversion factor) determination and subsequent testing of the fundamental meteorological characteristics of the instrument by means of special aerosol sources, which fosters a significant reduction in individual components of the indicated errors.

Effect of aerosolized acetylcholine on bronchial blood flow.

Science.gov (United States)

Charan, N B; Carvalho, P; Johnson, S R; Thompson, W H; Lakshminarayan, S

1998-08-01

We studied the effects of aerosolized as well as intravenous infusion of acetylcholine on bronchial blood flow in six anesthetized sheep. Intravenous infusion of acetylcholine, at a dose of 2 microg/kg, increased bronchial blood flow from 45 +/- 15 (SE) to 74 +/- 30 ml/min, and vascular conductance increased by 76 +/- 22%. In contrast, aerosolized acetylcholine at doses of 2 and 20 microg/kg decreased bronchial vascular conductance by approximately 10%. At an aerosolized dose of 200 microg/kg, the bronchial vascular conductance increased by approximately 15%, and there was no further increase in conductance when the aerosolized dose was increased to 2,000 microg/kg. Pretreatment of animals with a nitric oxide synthase inhibitor, Nomega-nitro-L-arginine methyl ester hydrochloride, partially blocked the vasodilatory effects of intravenous acetylcholine and completely blocked the vasodilatory effects of high-dose aerosolized acetylcholine. These data suggest that aerosolized acetylcholine does not readily penetrate the vascular wall of bronchial circulatory system and, therefore, has minimal vasodilatory effects on the bronchial vasculature.

Characterization of aerosols from industrial fabrication of mixed-oxide nuclear reactor fuels

International Nuclear Information System (INIS)

Hoover, M.D.; Newton, G.J.

1997-01-01

Recycling plutonium into mixed-oxide (MOX) fuel for nuclear reactors is being given serious consideration as a safe and environmentally sound method of managing plutonium from weapons programs. Planning for the proper design and safe operation of the MOX fuel fabrication facilities can take advantage of studies done in the 1970s, when recycling of plutonium from nuclear fuel was under serious consideration. At that time, it was recognized that the recycle of plutonium and uranium in irradiated fuel could provide a significant energy source and that the use of 239 Pu in light water reactor fuel would reduce the requirements for enriched 235 U as a reactor fuel. It was also recognized that the fabrication of uranium and plutonium reactor fuels would not be risk-free. Despite engineered safety precautions such as the handling of uranium and plutonium in glove-box enclosures, accidental releases of radioactive aerosols from normal containment might occur. Workers might then be exposed to the released materials by inhalation

Global direct radiative forcing by process-parameterized aerosol optical properties

Science.gov (United States)

KirkevâG, Alf; Iversen, Trond

2002-10-01

A parameterization of aerosol optical parameters is developed and implemented in an extended version of the community climate model version 3.2 (CCM3) of the U.S. National Center for Atmospheric Research. Direct radiative forcing (DRF) by monthly averaged calculated concentrations of non-sea-salt sulfate and black carbon (BC) is estimated. Inputs are production-specific BC and sulfate from [2002] and background aerosol size distribution and composition. The scheme interpolates between tabulated values to obtain the aerosol single scattering albedo, asymmetry factor, extinction coefficient, and specific extinction coefficient. The tables are constructed by full calculations of optical properties for an array of aerosol input values, for which size-distributed aerosol properties are estimated from theory for condensation and Brownian coagulation, assumed distribution of cloud-droplet residuals from aqueous phase oxidation, and prescribed properties of the background aerosols. Humidity swelling is estimated from the Köhler equation, and Mie calculations finally yield spectrally resolved aerosol optical parameters for 13 solar bands. The scheme is shown to give excellent agreement with nonparameterized DRF calculations for a wide range of situations. Using IPCC emission scenarios for the years 2000 and 2100, calculations with an atmospheric global cliamte model (AFCM) yield a global net anthropogenic DRF of -0.11 and 0.11 W m-2, respectively, when 90% of BC from biomass burning is assumed anthropogenic. In the 2000 scenario, the individual DRF due to sulfate and BC has separately been estimated to -0.29 and 0.19 W m-2, respectively. Our estimates of DRF by BC per BC mass burden are lower than earlier published estimates. Some sensitivity tests are included to investigate to what extent uncertain assumptions may influence these results.

Experimental study of radioactive aerosols emission during the thermal degradation of organic materials in nuclear facilities

International Nuclear Information System (INIS)

Fernandez, Yvette

1993-01-01

Radioactive products may be released during a fire in nuclear fuel cycles facilities. These products must be confined to avoid a contamination spread in the environment. It is therefore necessary to be able to predict the amount and the physico-chemical forms of radioactive material that may be airborne. The aim of this study is to determine experimentally the release of contamination aerosols in a typical fire scenario involving plutonium oxide in a glove box. Firstly, this phenomenon has been studied in a small scale test chamber where samples of polymethylmethacrylate (Plexiglas) contaminated by cerium oxide (used as a substitute for plutonium oxide) were submitted to thermal degradation (pyrolysis and combustion). The release of radioactive material is determined by the quantity of contaminant emitted, the kinetics of the release and the particle size distribution of aerosols. Secondly, the development of an experimental procedure allowed to realize large scale fires in more realistic conditions. The experimental tools developed in the course of this study allow to consider application to other scenarios. (author) [fr

Electronic cigarette aerosols and copper nanoparticles induce mitochondrial stress and promote DNA fragmentation in lung fibroblasts

Energy Technology Data Exchange (ETDEWEB)

Lerner, Chad A.; Rutagarama, Pierrot; Ahmad, Tanveer; Sundar, Isaac K.; Elder, Alison; Rahman, Irfan, E-mail: irfan_rahman@urmc.rochester.edu

2016-09-02

Oxidants or nanoparticles have recently been identified as constituents of aerosols released from various styles of electronic cigarettes (E-cigs). Cells in the lung may be directly exposed to these constituents and harbor reactive properties capable of incurring acute cell injury. Our results show mitochondria are sensitive to both E-cig aerosols and aerosol containing copper nanoparticles when exposed to human lung fibroblasts (HFL-1) using an Air-Liquid Interface culture system, evident by elevated levels of mitochondrial ROS (mtROS). Increased mtROS after aerosol exposure is associated with reduced stability of OxPhos electron transport chain (ETC) complex IV subunit and nuclear DNA fragmentation. Increased levels of IL-8 and IL-6 in HFL-1 conditioned media were also observed. These findings reveal both mitochondrial, genotoxic, and inflammatory stresses are features of direct cell exposure to E-cig aerosols which are ensued by inflammatory duress, raising a concern on deleterious effect of vaping. - Graphical abstract: Oxidants and possibly reactive properties of metal particles in E-cig aerosols impart mitochondrial oxidative stress and DNA damage. These biological effects accompany inflammatory response which may raise concern regarding long term E-cig use. Mitochondria may be particularly sensitive to reactive properties of E-cig aerosols in addition to the potential for them to induce genotoxic stress by generating increased ROS. - Highlights: • Mitochondria are sensitive to both E-cig aerosols and metal nanoparticles. • Increased mtROS by E-cig aerosol is associated with disrupted mitochondrial energy. • E-cig causes nuclear DNA fragmentation. • E-cig aerosols induce pro-inflammatory response in human fibroblasts.

Electronic cigarette aerosols and copper nanoparticles induce mitochondrial stress and promote DNA fragmentation in lung fibroblasts

International Nuclear Information System (INIS)

Lerner, Chad A.; Rutagarama, Pierrot; Ahmad, Tanveer; Sundar, Isaac K.; Elder, Alison; Rahman, Irfan

2016-01-01

Oxidants or nanoparticles have recently been identified as constituents of aerosols released from various styles of electronic cigarettes (E-cigs). Cells in the lung may be directly exposed to these constituents and harbor reactive properties capable of incurring acute cell injury. Our results show mitochondria are sensitive to both E-cig aerosols and aerosol containing copper nanoparticles when exposed to human lung fibroblasts (HFL-1) using an Air-Liquid Interface culture system, evident by elevated levels of mitochondrial ROS (mtROS). Increased mtROS after aerosol exposure is associated with reduced stability of OxPhos electron transport chain (ETC) complex IV subunit and nuclear DNA fragmentation. Increased levels of IL-8 and IL-6 in HFL-1 conditioned media were also observed. These findings reveal both mitochondrial, genotoxic, and inflammatory stresses are features of direct cell exposure to E-cig aerosols which are ensued by inflammatory duress, raising a concern on deleterious effect of vaping. - Graphical abstract: Oxidants and possibly reactive properties of metal particles in E-cig aerosols impart mitochondrial oxidative stress and DNA damage. These biological effects accompany inflammatory response which may raise concern regarding long term E-cig use. Mitochondria may be particularly sensitive to reactive properties of E-cig aerosols in addition to the potential for them to induce genotoxic stress by generating increased ROS. - Highlights: • Mitochondria are sensitive to both E-cig aerosols and metal nanoparticles. • Increased mtROS by E-cig aerosol is associated with disrupted mitochondrial energy. • E-cig causes nuclear DNA fragmentation. • E-cig aerosols induce pro-inflammatory response in human fibroblasts.

Observations of gas- and aerosol-phase organic nitrates at BEACHON-RoMBAS 2011

Directory of Open Access Journals (Sweden)

J. L. Fry

2013-09-01

Full Text Available At the Rocky Mountain Biogenic Aerosol Study (BEACHON-RoMBAS field campaign in the Colorado front range, July–August 2011, measurements of gas- and aerosol-phase organic nitrates enabled a study of the role of NOx (NOx = NO + NO2 in oxidation of forest-emitted volatile organic compounds (VOCs and subsequent aerosol formation. Substantial formation of peroxy- and alkyl-nitrates is observed every morning, with an apparent 2.9% yield of alkyl nitrates from daytime RO2 + NO reactions. Aerosol-phase organic nitrates, however, peak in concentration during the night, with concentrations up to 140 ppt as measured by both optical spectroscopic and mass spectrometric instruments. The diurnal cycle in aerosol fraction of organic nitrates shows an equilibrium-like response to the diurnal temperature cycle, suggesting some reversible absorptive partitioning, but the full dynamic range cannot be reproduced by thermodynamic repartitioning alone. Nighttime aerosol organic nitrate is observed to be positively correlated with [NO2] × [O3] but not with [O3]. These observations support the role of nighttime NO3-initiated oxidation of monoterpenes as a significant source of nighttime aerosol. Nighttime production of organic nitrates is comparable in magnitude to daytime photochemical production at this site, which we postulate to be representative of the Colorado front range forests.

Synergistic reaction between SO2 and NO2 on mineral oxides: a potential formation pathway of sulfate aerosol.

Science.gov (United States)

Liu, Chang; Ma, Qingxin; Liu, Yongchun; Ma, Jinzhu; He, Hong

2012-02-07

Sulfate is one of the most important aerosols in the atmosphere. A new sulfate formation pathway via synergistic reactions between SO(2) and NO(2) on mineral oxides was proposed. The heterogeneous reactions of SO(2) and NO(2) on CaO, α-Fe(2)O(3), ZnO, MgO, α-Al(2)O(3), TiO(2), and SiO(2) were investigated by in situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (in situ DRIFTS) at ambient temperature. Formation of sulfate from adsorbed SO(2) was promoted by the coexisting NO(2), while surface N(2)O(4) was observed as the crucial oxidant for the oxidation of surface sulfite. This process was significantly promoted by the presence of O(2). The synergistic effect between SO(2) and NO(2) was not observed on other mineral particles (such as CaCO(3) and CaSO(4)) probably due to the lack of the surface reactive oxygen sites. The synergistic reaction between SO(2) and NO(2) on mineral oxides resulted in the formation of internal mixtures of sulfate, nitrate, and mineral oxides. The change of mixture state will affect the physicochemical properties of atmospheric particles and therefore further influence their environmental and climate effects.

Yields of aerosol precursor substances by the oxidation of DMS as a function of atmospheric conditions (temperature and NOx). Final report; Ausbeuten von Aerosolvorlaeufersubstanzen bei der DMS-Oxidation als Funktion von atmosphaerischen Bedingungen (Temperatur und NO{sub x}). Abschlussbericht

Energy Technology Data Exchange (ETDEWEB)

Barnes, I.; Albu, M.; Arsene, C.; Butkovskaya, N.I.; Patroescu, I.V.

2002-04-28

In-depth analyses have been made of the products and aerosol formation from the OH-radical initiated oxidation of dimethyl sulphide (CH3SCH3: DMS) as a function of temperature, O2 partial pressure and initial NO concentration in large photoreactors. The investigations have provided new insights into the oxidation mechanisms of both DMS and DMSO, e.g., it has been shown that interactions of the DMS-OH adduct with O2 form DMSO in the absence of NO and dimethyl sulphone (CH3SO2CH3: DMSO2) in its presence. The data support an SO2 yield of around 70% from OH + DMS in the remote marine atmosphere. Investigations on the OH-radical initiated oxidation of dimethyl sulphoxide (CH3SOCH3: DMSO) have shown for the first time that methane sulphinic acid (CH3S(O)OH: MSIA) is the major product. Within the experimental conditions employed in the experiments only a modest dependence of the aerosol yield on temperature and initial NO concentration was observed. The experiments support that sulphuric acid formed from OH + SO2 is the major component of the aerosol with only minor contributions from MSA and MSIA. The mechanistic information is being incorporated into a DMS atmospheric chemistry modeule for CTMs (http://www.dmi.dk/f+u/luft/eng/elcid/elcid.html) and also in a simplified form for a global climate model (http://ask.ii.uib.no/.climate/elcid/). (orig.)

Sodium aerosol recovering device

International Nuclear Information System (INIS)

Fujimori, Koji; Ueda, Mitsuo; Tanaka, Kazuhisa.

1997-01-01

A main body of a recovering device is disposed in a sodium cooled reactor or a sodium cooled test device. Air containing sodium aerosol is sucked into the main body of the recovering device by a recycling fan and introduced to a multi-staged metal mesh filter portion. The air about against each of the metal mesh filters, and the sodium aerosol in the air is collected. The air having a reduced sodium aerosol concentration circulates passing through a recycling fan and pipelines to form a circulation air streams. Sodium aerosol deposited on each of the metal mesh filters is scraped off periodically by a scraper driving device to prevent clogging of each of the metal filters. (I.N.)

Predicting Thermal Behavior of Secondary Organic Aerosols

Science.gov (United States)

Volume concentrations of steady-state secondary organic aerosol (SOA) were measured in 139 steadystate single precursor hydrocarbon oxidation experiments after passing through a temperature controlled inlet tube. Higher temperatures resulted in greater loss of particle volume, wi...

Investigation of molten corium-concrete interaction phenomena and aerosol release

International Nuclear Information System (INIS)

Spencer, B.W.; Thompson, D.H.; Armstrong, D.R.; Fink, J.K.; Gunther, W.H.; Kilsdonk, D.J.; Sehgal, B.R.

1987-01-01

The Electric Power Research Institute is sponsoring a program of laboratory investigations at Argonne National Laboratory to study the interaction between molten core materials and reactor concrete basemats during postulated severe reactor accidents, with particular emphasis on measurements of the magnitude and chemical species present in the aerosol releases. The approach in this program is to sustain internal heat generation in reactor-material corium using direct electrical heating and to develop test operating and diagnostics capabilities with a series of small- and intermediate-scale scoping tests followed by fully instrumented large-scale testing. Real reactor materials (UO 2 , ZrO 2 , oxides of stainless steel, plus metallics) are used, with small amounts of La 2 O 3 , BaO, and SrO added to simulate nonvolatile fission products. In intermediate-scale scoping tests completed to date, corium inventories of up to 29 kg have been heated with power inputs in excess of 1 kW/kg melt. The measured concrete ablation rates have ranged from 0.9 to 3.9 mm/minute. Aerosol samples have been examined using a scanning electron microscope and show submicron particles, 2-6 micrometer spheres, and agglomerates that range from a few micrometers to string 13 micrometers in length

Lightning-produced NOx in an explicit electrical scheme tested in a Stratosphere-Troposphere Experiment: Radiation, Aerosols, and Ozone case study

Science.gov (United States)

Barthe, Christelle; Pinty, Jean-Pierre; Mari, CéLine

2007-02-01

An explicit lightning-produced nitrogen oxide (LNOx) scheme has been implemented in a 3-D mesoscale model. The scheme is based on the simulation of the electrical state of the cloud and provides a prediction of the temporal and spatial distribution of the lightning flashes. The frequency and the 3-D morphology of the lightning flashes are captured realistically so fresh nitrogen oxide molecules can be added along the complex flash path as a function of the pressure, as suggested by results from laboratory experiments. The scheme is tested on the 10 July 1996 Stratosphere-Troposphere Experiment: Radiation, Aerosols, and Ozone (STERAO) storm. The model reproduces many features of the observed increase of electrical activity and LNOx flux density between the multicell and supercell stages. LNOx dominates the NOx budget in the upper part of the cells with instantaneous peak concentrations exceeding 4 ppbv, as observed. The computed flux of NOx across the anvil shows a mean value of 6 mol m-2 s-1 during the last 90 min of the simulation. This value is remarkably stable and compares favorably with the observations.

Aerosol Climate Time Series in ESA Aerosol_cci

Science.gov (United States)

Popp, Thomas; de Leeuw, Gerrit; Pinnock, Simon

2016-04-01

Within the ESA Climate Change Initiative (CCI) Aerosol_cci (2010 - 2017) conducts intensive work to improve algorithms for the retrieval of aerosol information from European sensors. Meanwhile, full mission time series of 2 GCOS-required aerosol parameters are completely validated and released: Aerosol Optical Depth (AOD) from dual view ATSR-2 / AATSR radiometers (3 algorithms, 1995 - 2012), and stratospheric extinction profiles from star occultation GOMOS spectrometer (2002 - 2012). Additionally, a 35-year multi-sensor time series of the qualitative Absorbing Aerosol Index (AAI) together with sensitivity information and an AAI model simulator is available. Complementary aerosol properties requested by GCOS are in a "round robin" phase, where various algorithms are inter-compared: fine mode AOD, mineral dust AOD (from the thermal IASI spectrometer, but also from ATSR instruments and the POLDER sensor), absorption information and aerosol layer height. As a quasi-reference for validation in few selected regions with sparse ground-based observations the multi-pixel GRASP algorithm for the POLDER instrument is used. Validation of first dataset versions (vs. AERONET, MAN) and inter-comparison to other satellite datasets (MODIS, MISR, SeaWIFS) proved the high quality of the available datasets comparable to other satellite retrievals and revealed needs for algorithm improvement (for example for higher AOD values) which were taken into account for a reprocessing. The datasets contain pixel level uncertainty estimates which were also validated and improved in the reprocessing. For the three ATSR algorithms the use of an ensemble method was tested. The paper will summarize and discuss the status of dataset reprocessing and validation. The focus will be on the ATSR, GOMOS and IASI datasets. Pixel level uncertainties validation will be summarized and discussed including unknown components and their potential usefulness and limitations. Opportunities for time series extension

Sources and atmospheric processing of organic aerosol in the Mediterranean: insights from aerosol mass spectrometer factor analysis

Directory of Open Access Journals (Sweden)

L. Hildebrandt

2011-12-01

Full Text Available Atmospheric particles were measured in the late winter (25 February–26 March 2009 at a remote coastal site on the island of Crete, Greece during the Finokalia Aerosol Measurement Experiment-2009. A quadrupole aerosol mass spectrometer (Q-AMS was employed to quantify the size-resolved chemical composition of non-refractory submicron aerosol, and a thermodenuder was used to analyze the organic aerosol (OA volatility. Complementary measurements included particle size distributions from a scanning mobility particle sizer, inorganic and organic particle composition from filter analysis, air ion concentrations, O₃, NO_x and NO_y concentrations, and meteorological measurements. Factor analysis was performed on the OA mass spectra, and the variability in OA composition could best be explained with three OA components. The oxygenated organic aerosol (OOA was similar in composition and volatility to the summertime OA previously measured at this site and may represent an effective endpoint in particle-phase oxidation of organics. The two other OA components, one associated with amines (Amine-OA and the other probably associated with the burning of olive branches (OB-OA, had very low volatility but were less oxygenated. Hydrocarbon-like organic aerosol (HOA was not detected. The absence of OB-OA and Amine-OA in the summer data may be due to lower emissions and/or photochemical conversion of these components to OOA.

Filtration of sodium-fire aerosols

International Nuclear Information System (INIS)

Alexas, A.; Jordan, S.; Lindner, W.

1979-01-01

Different filter devices have been developed and tested with respect to their use in the off-gas system of liquid-metal fast breeder reactors to prevent the escape of sodium-fire aerosols that might be formed in case of an accident. The testing results have shown that the use of a multilayer sand bed filter is still the best method to filter limited amounts of sodium-fire aerosols over a long operating time. Efficiencies on the order of 99.98 and 98.8% were reached for loading capacities of 500 and 1000 g/m 2 , respectively. Unlimited amounts of sodium-fire aerosols can be filtered by wet scrubbers with an efficiency of 70% per scrubber stage. Fiberglas filters connot be used for the filtration of sodium-fire aerosols over a long operating time because the filter material can be destroyed after several days of operating

Effect of aircraft exhaust sulfur emissions on near field plume aerosols

Energy Technology Data Exchange (ETDEWEB)

Brown, R.C.; Miake-Lye, R.C.; Anderson, M.R.; Kolb, C.E. [Aerodyne Research, Inc., Billerica, MA (United States). Center for Chemical and Environmental Physics

1997-12-31

Based on estimated exit plane sulfur speciation, a two dimensional, axisymmetric flow field model with coupled gas phase oxidation kinetics and aerosol nucleation and growth dynamics is used to evaluate the effect of fuel sulfur oxidation in the engine on the formation and growth of volatile H{sub 2}SO{sub 4}/H{sub 2}O aerosols in the near field plume. The conversion of fuel sulfur to sulfur trioxide and sulfuric acid in the engine is predicted to significantly increase the number density and surface area density of volatile H{sub 2}SO{sub 4}/H{sub 2}O aerosols and the chemical activation of exhaust soot particulates. This analysis indicates the need for experimental measurements of exhaust SO{sub x} emissions to fully assess the atmospheric impact of aircraft emissions. (author) 18 refs.; Submitted to Geophysical Research Letters

Effect of aircraft exhaust sulfur emissions on near field plume aerosols

Energy Technology Data Exchange (ETDEWEB)

Brown, R C; Miake-Lye, R C; Anderson, M R; Kolb, C E [Aerodyne Research, Inc., Billerica, MA (United States). Center for Chemical and Environmental Physics

1998-12-31

Based on estimated exit plane sulfur speciation, a two dimensional, axisymmetric flow field model with coupled gas phase oxidation kinetics and aerosol nucleation and growth dynamics is used to evaluate the effect of fuel sulfur oxidation in the engine on the formation and growth of volatile H{sub 2}SO{sub 4}/H{sub 2}O aerosols in the near field plume. The conversion of fuel sulfur to sulfur trioxide and sulfuric acid in the engine is predicted to significantly increase the number density and surface area density of volatile H{sub 2}SO{sub 4}/H{sub 2}O aerosols and the chemical activation of exhaust soot particulates. This analysis indicates the need for experimental measurements of exhaust SO{sub x} emissions to fully assess the atmospheric impact of aircraft emissions. (author) 18 refs.; Submitted to Geophysical Research Letters

21 CFR 862.3080 - Breath nitric oxide test system.

Science.gov (United States)

2010-04-01

... Systems § 862.3080 Breath nitric oxide test system. (a) Identification. A breath nitric oxide test system... 21 Food and Drugs 8 2010-04-01 2010-04-01 false Breath nitric oxide test system. 862.3080 Section... fractional nitric oxide concentration in expired breath aids in evaluating an asthma patient's response to...

Nucleation and growth of sulfate aerosol in coal-fired power plant plumes: sensitivity to background aerosol and meteorology

Science.gov (United States)

Stevens, R. G.; Pierce, J. R.; Brock, C. A.; Reed, M. K.; Crawford, J. H.; Holloway, J. S.; Ryerson, T. B.; Huey, L. G.; Nowak, J. B.

2012-01-01

New-particle formation in the plumes of coal-fired power plants and other anthropogenic sulfur sources may be an important source of particles in the atmosphere. It remains unclear, however, how best to reproduce this formation in global and regional aerosol models with grid-box lengths that are 10s of kilometers and larger. The predictive power of these models is thus limited by the resultant uncertainties in aerosol size distributions. In this paper, we focus on sub-grid sulfate aerosol processes within coal-fired power plant plumes: the sub-grid oxidation of SO2 with condensation of H2SO4 onto newly-formed and pre-existing particles. We have developed a modeling framework with aerosol microphysics in the System for Atmospheric Modelling (SAM), a Large-Eddy Simulation/Cloud-Resolving Model (LES/CRM). The model is evaluated against aircraft observations of new-particle formation in two different power-plant plumes and reproduces the major features of the observations. We show how the downwind plume aerosols can be greatly modified by both meteorological and background aerosol conditions. In general, new-particle formation and growth is greatly reduced during polluted conditions due to the large pre-existing aerosol surface area for H2SO4 condensation and particle coagulation. The new-particle formation and growth rates are also a strong function of the amount of sunlight and NOx since both control OH concentrations. The results of this study highlight the importance for improved sub-grid particle formation schemes in regional and global aerosol models.

Aerosol filtration

International Nuclear Information System (INIS)

Klein, M.; Goossens, W.R.A.; De Smet, M.; Trine, J.; Hertschap, M.

1984-01-01

This report summarizes the work on the development of fibre metallic prefilters to be placed upstream of HEPA filters for the exhaust gases of nuclear process plants. Investigations at ambient and high temperature were carried out. Measurements of the filtration performance of Bekipor porous webs and sintered mats were performed in the AFLT (aerosol filtration at low temperature) unit with a throughput of 15 m 3 /h. A parametric study on the influence of particle size, fibre diameter, number of layers and superficial velocity led to the optimum choice of the working parameters. Three selected filter types were then tested with polydisperse aerosols using a candle-type filter configuration or a flat-type filter configuration. The small-diameter candle type is not well suited for a spraying nozzles regeneration system so that only the flat-type filter was retained for high-temperature tests. A high-temperature test unit (AFHT) with a throughput of 8 to 10 m 3 /h at 400 0 C was used to test the three filter types with an aerosol generated by high-temperature calcination of a simulated nitric acid waste solution traced with 134 Cs. The regeneration of the filter by spray washing and the effect of the regeneration on the filter performance was studied for the three filter types. The porous mats have a higher dust loading capacity than the sintered web which means that their regeneration frequency can be kept lower

Phase identification of individual crystalline particles by combining EDX and EBSD: application to workplace aerosols.

Science.gov (United States)

Ervik, Torunn Kringlen; Benker, Nathalie; Weinbruch, Stephan; Skogstad, Asbjørn; Thomassen, Yngvar; Ellingsen, Dag G; Berlinger, Balázs

2018-04-01

This paper discusses the combined use of electron backscatter diffraction (EBSD) and energy dispersive X-ray microanalysis (EDX) to identify unknown phases in particulate matter from different workplace aerosols. Particles of α-silicon carbide (α-SiC), manganese oxide (MnO) and α-quartz (α-SiO 2 ) were used to test the method. Phase identification of spherical manganese oxide particles from ferromanganese production, with diameter less than 200 nm, was unambiguous, and phases of both MnO and Mn 3 O 4 were identified in the same agglomerate. The same phases were identified by selected area electron diffraction (SAED) in transmission electron microscopy (TEM). The method was also used to identify the phases of different SiC fibres, and both β-SiC and α-SiC fibres were found. Our results clearly demonstrate that EBSD combined with EDX can be successfully applied to the characterisation of workplace aerosols. Graphical abstract Secondary electron image of an agglomerate of manganese oxide particles collected at a ferromanganese smelter (a). EDX spectrum of the particle highlighted by an arrow (b). Indexed patterns after dynamic background subtraction from three particles shown with numbers in a (c).

Novel pathway of SO2 oxidation in the atmosphere: reactions with monoterpene ozonolysis intermediates and secondary organic aerosol

Science.gov (United States)

Ye, Jianhuai; Abbatt, Jonathan P. D.; Chan, Arthur W. H.

2018-04-01

Ozonolysis of monoterpenes is an important source of atmospheric biogenic secondary organic aerosol (BSOA). While enhanced BSOA formation has been associated with sulfate-rich conditions, the underlying mechanisms remain poorly understood. In this work, the interactions between SO2 and reactive intermediates from monoterpene ozonolysis were investigated under different humidity conditions (10 % vs. 50 %). Chamber experiments were conducted with ozonolysis of α-pinene or limonene in the presence of SO2. Limonene SOA formation was enhanced in the presence of SO2, while no significant changes in SOA yields were observed during α-pinene ozonolysis. Under dry conditions, SO2 primarily reacted with stabilized Criegee intermediates (sCIs) produced from ozonolysis, but at 50 % RH heterogeneous uptake of SO2 onto organic aerosol was found to be the dominant sink of SO2, likely owing to reactions between SO2 and organic peroxides. This SO2 loss mechanism to organic peroxides in SOA has not previously been identified in experimental chamber studies. Organosulfates were detected and identified using an electrospray ionization-ion mobility spectrometry-high-resolution time-of-flight mass spectrometer (ESI-IMS-TOF) when SO2 was present in the experiments. Our results demonstrate the synergistic effects between BSOA formation and SO2 oxidation through sCI chemistry and SO2 uptake onto organic aerosol and illustrate the importance of considering the chemistry of organic and sulfur-containing compounds holistically to properly account for their reactive sinks.

Secondary organic aerosol formation from biomass burning intermediates: phenol and methoxyphenols

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L. D. Yee

2013-08-01

Full Text Available The formation of secondary organic aerosol from oxidation of phenol, guaiacol (2-methoxyphenol, and syringol (2,6-dimethoxyphenol, major components of biomass burning, is described. Photooxidation experiments were conducted in the Caltech laboratory chambers under low-NOx (2O2 as the OH source. Secondary organic aerosol (SOA yields (ratio of mass of SOA formed to mass of primary organic reacted greater than 25% are observed. Aerosol growth is rapid and linear with the primary organic conversion, consistent with the formation of essentially non-volatile products. Gas- and aerosol-phase oxidation products from the guaiacol system provide insight into the chemical mechanisms responsible for SOA formation. Syringol SOA yields are lower than those of phenol and guaiacol, likely due to novel methoxy group chemistry that leads to early fragmentation in the gas-phase photooxidation. Atomic oxygen to carbon (O : C ratios calculated from high-resolution-time-of-flight Aerodyne Aerosol Mass Spectrometer (HR-ToF-AMS measurements of the SOA in all three systems are ~ 0.9, which represent among the highest such ratios achieved in laboratory chamber experiments and are similar to that of aged atmospheric organic aerosol. The global contribution of SOA from intermediate volatility and semivolatile organic compounds has been shown to be substantial (Pye and Seinfeld, 2010. An approach to representing SOA formation from biomass burning emissions in atmospheric models could involve one or more surrogate species for which aerosol formation under well-controlled conditions has been quantified. The present work provides data for such an approach.

Photochemical organonitrate formation in wet aerosols

Science.gov (United States)

Lim, Yong Bin; Kim, Hwajin; Kim, Jin Young; Turpin, Barbara J.

2016-10-01

Water is the most abundant component of atmospheric fine aerosol. However, despite rapid progress, multiphase chemistry involving wet aerosols is still poorly understood. In this work, we report results from smog chamber photooxidation of glyoxal- and OH-containing ammonium sulfate or sulfuric acid particles in the presence of NOx and O3 at high and low relative humidity. Particles were analyzed using ultra-performance liquid chromatography coupled to quadrupole time-of-flight mass spectrometry (UPLC-Q-TOF-MS). During the 3 h irradiation, OH oxidation products of glyoxal that are also produced in dilute aqueous solutions (e.g., oxalic acids and tartaric acids) were formed in both ammonium sulfate (AS) aerosols and sulfuric acid (SA) aerosols. However, the major products were organonitrogens (CHNO), organosulfates (CHOS), and organonitrogen sulfates (CHNOS). These were also the dominant products formed in the dark chamber, indicating non-radical formation. In the humid chamber (> 70 % relative humidity, RH), two main products for both AS and SA aerosols were organonitrates, which appeared at m / z- 147 and 226. They were formed in the aqueous phase via non-radical reactions of glyoxal and nitric acid, and their formation was enhanced by photochemistry because of the photochemical formation of nitric acid via reactions of peroxy radicals, NOx and OH during the irradiation.

Characterization of Halyomorpha halys (brown marmorated stink bug) biogenic volatile organic compound emissions and their role in secondary organic aerosol formation.

Science.gov (United States)

Solomon, Danielle; Dutcher, Dabrina; Raymond, Timothy

2013-11-01

The formation of aerosols is a key component in understanding cloud formation in the context of radiative forcings and global climate modeling. Biogenic volatile organic compounds (BVOCs) are a significant source of aerosols, yet there is still much to be learned about their structures, sources, and interactions. The aims of this project were to identify the BVOCs found in the defense chemicals of the brown marmorated stink bug Halymorpha halys and quantify them using gas chromatography-mass spectrometry (GC/MS) and test whether oxidation of these compounds by ozone-promoted aerosol and cloud seed formation. The bugs were tested under two conditions: agitation by asphyxiation and direct glandular exposure. Tridecane, 2(5H)-furanone 5-ethyl, and (E)-2-decenal were identified as the three most abundant compounds. H. halys were also tested in the agitated condition in a smog chamber. It was found that in the presence of 100-180 ppm ozone, secondary aerosols do form. A scanning mobility particle sizer (SMPS) and a cloud condensation nuclei counter (CCNC) were used to characterize the secondary aerosols that formed. This reaction resulted in 0.23 microg/ bug of particulate mass. It was also found that these secondary organic aerosol particles could act as cloud condensation nuclei. At a supersaturation of 1%, we found a kappa value of 0.09. Once regional populations of these stink bugs stablilize and the populations estimates can be made, the additional impacts of their contribution to regional air quality can be calculated.

Secondary organic aerosol importance in the future atmosphere

International Nuclear Information System (INIS)

Tsigaridis, K.; Kanakidou, M.

2007-01-01

In order to investigate the secondary organic aerosol (SOA) response to changes in biogenic volatile organic compounds (VOC) emissions in the future atmosphere and how important will SOA be relative to the major anthropogenic aerosol component (sulfate), the global three-dimensional chemistry/transport model TM3 has been used. Emission estimates of biogenic VOC (BVOC) and anthropogenic gases and particles from the literature for the year 2100 have been adopted. According to our present-day model simulations, isoprene oxidation produces 4.6 Tg SOA yr -1 , that is less than half of the 12.2 Tg SOA yr -1 formed by the oxidation of other BVOC. In the future, nitrate radicals and ozone become more important than nowadays, but remain minor oxidants for both isoprene and aromatics. SOA produced by isoprene is estimated to almost triple, whereas the production from other BVOC more than triples. The calculated future SOA burden change, from 0.8 Tg at present to 2.0 Tg in the future, is driven by changes in emissions, oxidant levels and pre-existing particles. The non-linearity in SOA formation and the involved chemical and physical feedbacks prohibit the quantitative attribution of the computed changes to the above-mentioned individual factors. In 2100, SOA burden is calculated to exceed that of sulfate, indicating that SOA might become more important than nowadays. These results critically depend on the biogenic emissions and thus are subject to the high uncertainty associated with these emissions estimated due to the insufficient knowledge on plant response to carbon dioxide changes. Nevertheless, they clearly indicate that the change in oxidants and primary aerosol caused by human activities can contribute as much as the change in BVOC emissions to the increase of the biogenic SOA production in the future atmosphere. (authors)

Improvement of the CULTEX® exposure technology by radial distribution of the test aerosol.

Science.gov (United States)

Aufderheide, Michaela; Heller, Wolf-Dieter; Krischenowski, Olaf; Möhle, Niklas; Hochrainer, Dieter

2017-07-05

The exposure of cellular based systems cultivated on microporous membranes at the air-liquid interface (ALI) has been accepted as an appropriate approach to simulate the exposure of cells of the respiratory tract to native airborne substances. The efficiency of such an exposure procedure with regard to stability and reproducibility depends on the optimal design at the interface between the cellular test system and the exposure technique. The actual exposure systems favor the dynamic guidance of the airborne substances to the surface of the cells in specially designed exposure devices. Two module types, based on a linear or radial feed of the test atmosphere to the test system, were used for these studies. In our technical history, the development started with the linear designed version, the CULTEX ® glass modules, fulfilling basic requirements for running ALI exposure studies (Mohr and Durst, 2005). The instability in the distribution of different atmospheres to the cells caused us to create a new exposure module, characterized by a stable and reproducible radial guidance of the aerosol to the cells. The outcome was the CULTEX ® RFS (Mohr et al., 2010). In this study, we describe the differences between the two systems with regard to particle distribution and deposition clarifying the advantages and disadvantages of a radial to a linear aerosol distribution concept. Copyright © 2017 Elsevier GmbH. All rights reserved.

Loading capacity of various filters for lithium fire generated aerosols

International Nuclear Information System (INIS)

Jeppson, D.W.; Barreca, J.R.

1980-01-01

The lithium aerosol loading capacity of a prefilter, HEPA filters and a sand and gravel bed filter was determined. The test aerosol was characterized and was generated by burning lithium in an unlimited air atmosphere. Correlation to sodium aerosol loading capacities were made to relate existing data to lithium aerosol loadings under varying conditions. This work is being conducted in support of the fusion reactor safety program. The lithium aerosol was generated by burning lithium pools, up to 45 kgs, in a 340 m 3 low humidity air atmosphere to supply aerosol to recirculating filter test loops. The aerosol was sampled to determine particle size, mass concentrations and chemical species. The dew point and gas concentrations were monitored throughout the tests. Loop inlet aerosol mass concentrations ranged up to 5 gr/m 3 . Chemical compounds analyzed to be present in the aerosol include Li 2 O, LiOH, and Li 2 CO 3 . HEPA filters with and without separators and a prefilter and HEPA filter in series were loaded with 7.8 to 11.1 kg/m 2 of aerosol at a flow rate of 1.31 m/sec and 5 kPa pressure drop. The HEPA filter loading capacity was determined to be greater at a lower flow rate. The loading capacity increased from 0.4 to 2.8 kg by decreasing the flow rate from 1.31 to 0.26 m/sec for a pressure drop of 0.11 kPa due to aerosol buildup. The prefilter tested in series with a HEPA did not increase the total loading capacity significantly for the same total pressure drop. Separators in the HEPA had only minor effect on loading capacity. The sand and gravel bed filter loaded to 0.50 kg/m 2 at an aerosol flow rate of 0.069 m/sec and final pressure drop of 6.2 kPa. These loading capacities and their dependence on test variables are similar to those reported for sodium aerosols except for the lithium aerosol HEPA loading capacity dependence upon flow rate

The DRAGON aerosol research facility to study aerosol behaviour for reactor safety applications

International Nuclear Information System (INIS)

Suckow, Detlef; Guentay, Salih

2008-01-01

During a severe accident in a nuclear power plant fission products are expected to be released in form of aerosol particles and droplets. To study the behaviour of safety relevant reactor components under aerosol loads and prototypical severe accident conditions the multi-purpose aerosol generation facility DRAGON is used since 1994 for several projects. DRAGON can generate aerosol particles by the evaporation-condensation technique using a plasma torch system, fluidized bed and atomization of particles suspended in a liquid. Soluble, hygroscopic aerosol (i.e. CsOH) and insoluble aerosol particles (i.e. SnO 2 , TiO 2 ) or mixtures of them can be used. DRAGON uses state-of-the-art thermal-hydraulic, data acquisition and aerosol measurement techniques and is mainly composed of a mixing chamber, the plasma torch system, a steam generator, nitrogen gas and compressed air delivery systems, several aerosol delivery piping, gas heaters and several auxiliary systems to provide vacuum, coolant and off-gas treatment. The facility can be operated at system pressure of 5 bars, temperatures of 300 deg. C, flow rates of non-condensable gas of 900 kg/h and steam of 270 kg/h, respectively. A test section under investigation is attached to DRAGON. The paper summarizes and demonstrates with the help of two project examples the capabilities of DRAGON for reactor safety studies. (authors)

The Optical Properties of Limonene Secondary Organic Aerosols: The Role of NO3, OH, and O3 in the Oxidation Processes

Science.gov (United States)

Peng, Chao; Wang, Weigang; Li, Kun; Li, Junling; Zhou, Li; Wang, Lingshu; Ge, Maofa

2018-03-01

Limonene, a typical proxy of monoterpenes emitted from biogenic sources, plays an important role in secondary organic aerosol (SOA) formation. However, the optical properties of SOA generated from limonene under various oxidation pathways remain poorly understood. In this study, we investigate the refractive index (RI) of limonene SOA produced from four oxidation conditions with cavity ring-down spectrometer (CRDS) and photoacoustic extinctiometer operated at 532 and 375 nm. Our results show that there is a significant difference in RI values of SOA produced from NO3 oxidation compared to other oxidation pathways. The mean values of RI of SOA produced from NO3 oxidation, NOx oxidation, OH oxidation with NOx-free, and O3 oxidation experiments are 1.578, 1.469, 1.495, and 1.494 at 532 nm; and 1.591, 1.527, 1.513, and 1.537 at 375 nm, respectively, while no detectable absorption is found in all oxidation conditions. We attribute the high RI values of SOA by NO3 oxidation to two factors: a large proportion of organic nitrates and high-molecular-weight dimers/oligomers in the SOA. Our study results indicate that the nighttime chemistry may significantly influence the optical properties of limonene oxidation products. The RI values of limonene SOA generated under various oxidation conditions at different wavelengths retrieved in our laboratory experiments could help improve the model predictions for evaluating the effect of biogenic SOA on the global radiative forcing as well as climate change.

Volatility measurement of atmospheric submicron aerosols in an urban atmosphere in southern China

Science.gov (United States)

Cao, Li-Ming; Huang, Xiao-Feng; Li, Yuan-Yuan; Hu, Min; He, Ling-Yan

2018-02-01

Aerosol pollution has been a very serious environmental problem in China for many years. The volatility of aerosols can affect the distribution of compounds in the gas and aerosol phases, the atmospheric fates of the corresponding components, and the measurement of the concentration of aerosols. Compared to the characterization of chemical composition, few studies have focused on the volatility of aerosols in China. In this study, a thermodenuder aerosol mass spectrometer (TD-AMS) system was deployed to study the volatility of non-refractory submicron particulate matter (PM1) species during winter in Shenzhen. To our knowledge, this paper is the first report of the volatilities of aerosol chemical components based on a TD-AMS system in China. The average PM1 mass concentration during the experiment was 42.7±20.1 µg m-3, with organic aerosol (OA) being the most abundant component (43.2 % of the total mass). The volatility of chemical species measured by the AMS varied, with nitrate showing the highest volatility, with a mass fraction remaining (MFR) of 0.57 at 50 °C. Organics showed semi-volatile characteristics (the MFR was 0.88 at 50 °C), and the volatility had a relatively linear correlation with the TD temperature (from the ambient temperature to 200 °C), with an evaporation rate of 0.45 % °C-1. Five subtypes of OA were resolved from total OA using positive matrix factorization (PMF) for data obtained under both ambient temperature and high temperatures through the TD, including a hydrocarbon-like OA (HOA, accounting for 13.5 %), a cooking OA (COA, 20.6 %), a biomass-burning OA (BBOA, 8.9 %), and two oxygenated OAs (OOAs): a less-oxidized OOA (LO-OOA, 39.1 %) and a more-oxidized OOA (MO-OOA, 17.9 %). Different OA factors presented different volatilities, and the volatility sequence of the OA factors at 50 °C was HOA (MFR of 0.56) > LO-OOA (0.70) > COA (0.85) ≈ BBOA (0.87) > MO-OOA (0.99), which was not completely consistent with the sequence of their O

Aerosols emitted in underground mine air by diesel engine fueled with biodiesel.

Science.gov (United States)

Bugarski, Aleksandar D; Cauda, Emanuele G; Janisko, Samuel J; Hummer, Jon A; Patts, Larry D

2010-02-01

Using biodiesel in place of petroleum diesel is considered by several underground metal and nonmetal mine operators to be a viable strategy for reducing the exposure of miners to diesel particulate matter. This study was conducted in an underground experimental mine to evaluate the effects of soy methyl ester biodiesel on the concentrations and size distributions of diesel aerosols and nitric oxides in mine air. The objective was to compare the effects of neat and blended biodiesel fuels with those of ultralow sulfur petroleum diesel. The evaluation was performed using a mechanically controlled, naturally aspirated diesel engine equipped with a muffler and a diesel oxidation catalyst. The effects of biodiesel fuels on size distributions and number and total aerosol mass concentrations were found to be strongly dependent on engine operating conditions. When fueled with biodiesel fuels, the engine contributed less to elemental carbon concentrations for all engine operating modes and exhaust configurations. The substantial increases in number concentrations and fraction of organic carbon (OC) in total carbon over the baseline were observed when the engine was fueled with biodiesel fuels and operated at light-load operating conditions. Size distributions for all test conditions were found to be single modal and strongly affected by engine operating conditions, fuel type, and exhaust configuration. The peak and total number concentrations as well as median diameter decreased with an increase in the fraction of biodiesel in the fuels, particularly for high-load operating conditions. The effects of the diesel oxidation catalyst, commonly deployed to counteract the potential increase in OC emissions due to use of biodiesel, were found to vary depending upon fuel formulation and engine operating conditions. The catalyst was relatively effective in reducing aerosol number and mass concentrations, particularly at light-load conditions, but also showed the potential for an

Effect of relative humidity on the composition of secondary organic aerosol from the oxidation of toluene

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M. L. Hinks

2018-02-01

Full Text Available The effect of relative humidity (RH on the chemical composition of secondary organic aerosol (SOA formed from low-NOx toluene oxidation in the absence of seed particles was investigated. SOA samples were prepared in an aerosol smog chamber at < 2 % RH and 75 % RH, collected on Teflon filters, and analyzed with nanospray desorption electrospray ionization high-resolution mass spectrometry (nano-DESI–HRMS. Measurements revealed a significant reduction in the fraction of oligomers present in the SOA generated at 75 % RH compared to SOA generated under dry conditions. In a separate set of experiments, the particle mass concentrations were measured with a scanning mobility particle sizer (SMPS at RHs ranging from < 2 to 90 %. It was found that the particle mass loading decreased by nearly an order of magnitude when RH increased from < 2 to 75–90 % for low-NOx toluene SOA. The volatility distributions of the SOA compounds, estimated from the distribution of molecular formulas using the molecular corridor approach, confirmed that low-NOx toluene SOA became more volatile on average under high-RH conditions. In contrast, the effect of RH on SOA mass loading was found to be much smaller for high-NOx toluene SOA. The observed increase in the oligomer fraction and particle mass loading under dry conditions were attributed to the enhancement of condensation reactions, which produce water and oligomers from smaller compounds in low-NOx toluene SOA. The reduction in the fraction of oligomeric compounds under humid conditions is predicted to partly counteract the previously observed enhancement in the toluene SOA yield driven by the aerosol liquid water chemistry in deliquesced inorganic seed particles.

Nucleation and growth of sulfate aerosol in coal-fired power plant plumes: sensitivity to background aerosol and meteorology

Directory of Open Access Journals (Sweden)

R. G. Stevens

2012-01-01

Full Text Available New-particle formation in the plumes of coal-fired power plants and other anthropogenic sulfur sources may be an important source of particles in the atmosphere. It remains unclear, however, how best to reproduce this formation in global and regional aerosol models with grid-box lengths that are 10s of kilometers and larger. The predictive power of these models is thus limited by the resultant uncertainties in aerosol size distributions. In this paper, we focus on sub-grid sulfate aerosol processes within coal-fired power plant plumes: the sub-grid oxidation of SO₂ with condensation of H₂SO₄ onto newly-formed and pre-existing particles. We have developed a modeling framework with aerosol microphysics in the System for Atmospheric Modelling (SAM, a Large-Eddy Simulation/Cloud-Resolving Model (LES/CRM. The model is evaluated against aircraft observations of new-particle formation in two different power-plant plumes and reproduces the major features of the observations. We show how the downwind plume aerosols can be greatly modified by both meteorological and background aerosol conditions. In general, new-particle formation and growth is greatly reduced during polluted conditions due to the large pre-existing aerosol surface area for H₂SO₄ condensation and particle coagulation. The new-particle formation and growth rates are also a strong function of the amount of sunlight and NO_x since both control OH concentrations. The results of this study highlight the importance for improved sub-grid particle formation schemes in regional and global aerosol models.

Aerosol typing - key information from aerosol studies

Science.gov (United States)

Mona, Lucia; Kahn, Ralph; Papagiannopoulos, Nikolaos; Holzer-Popp, Thomas; Pappalardo, Gelsomina

2016-04-01

Aerosol typing is a key source of aerosol information from ground-based and satellite-borne instruments. Depending on the specific measurement technique, aerosol typing can be used as input for retrievals or represents an output for other applications. Typically aerosol retrievals require some a priori or external aerosol type information. The accuracy of the derived aerosol products strongly depends on the reliability of these assumptions. Different sensors can make use of different aerosol type inputs. A critical review and harmonization of these procedures could significantly reduce related uncertainties. On the other hand, satellite measurements in recent years are providing valuable information about the global distribution of aerosol types, showing for example the main source regions and typical transport paths. Climatological studies of aerosol load at global and regional scales often rely on inferred aerosol type. There is still a high degree of inhomogeneity among satellite aerosol typing schemes, which makes the use different sensor datasets in a consistent way difficult. Knowledge of the 4d aerosol type distribution at these scales is essential for understanding the impact of different aerosol sources on climate, precipitation and air quality. All this information is needed for planning upcoming aerosol emissions policies. The exchange of expertise and the communication among satellite and ground-based measurement communities is fundamental for improving long-term dataset consistency, and for reducing aerosol type distribution uncertainties. Aerosol typing has been recognized as one of its high-priority activities of the AEROSAT (International Satellite Aerosol Science Network, http://aero-sat.org/) initiative. In the AEROSAT framework, a first critical review of aerosol typing procedures has been carried out. The review underlines the high heterogeneity in many aspects: approach, nomenclature, assumed number of components and parameters used for the

Primary and secondary aerosols in Beijing in winter: sources, variations and processes

Science.gov (United States)

Sun, Yele; Du, Wei; Fu, Pingqing; Wang, Qingqing; Li, Jie; Ge, Xinlei; Zhang, Qi; Zhu, Chunmao; Ren, Lujie; Xu, Weiqi; Zhao, Jian; Han, Tingting; Worsnop, Douglas R.; Wang, Zifa

2016-07-01

Winter has the worst air pollution of the year in the megacity of Beijing. Despite extensive winter studies in recent years, our knowledge of the sources, formation mechanisms and evolution of aerosol particles is not complete. Here we have a comprehensive characterization of the sources, variations and processes of submicron aerosols that were measured by an Aerodyne high-resolution aerosol mass spectrometer from 17 December 2013 to 17 January 2014 along with offline filter analysis by gas chromatography/mass spectrometry. Our results suggest that submicron aerosols composition was generally similar across the winter of different years and was mainly composed of organics (60 %), sulfate (15 %) and nitrate (11 %). Positive matrix factorization of high- and unit-mass resolution spectra identified four primary organic aerosol (POA) factors from traffic, cooking, biomass burning (BBOA) and coal combustion (CCOA) emissions as well as two secondary OA (SOA) factors. POA dominated OA, on average accounting for 56 %, with CCOA being the largest contributor (20 %). Both CCOA and BBOA showed distinct polycyclic aromatic hydrocarbons (PAHs) spectral signatures, indicating that PAHs in winter were mainly from coal combustion (66 %) and biomass burning emissions (18 %). BBOA was highly correlated with levoglucosan, a tracer compound for biomass burning (r2 = 0.93), and made a considerable contribution to OA in winter (9 %). An aqueous-phase-processed SOA (aq-OOA) that was strongly correlated with particle liquid water content, sulfate and S-containing ions (e.g. CH2SO2+) was identified. On average aq-OOA contributed 12 % to the total OA and played a dominant role in increasing oxidation degrees of OA at high RH levels (> 50 %). Our results illustrate that aqueous-phase processing can enhance SOA production and oxidation states of OA as well in winter. Further episode analyses highlighted the significant impacts of meteorological parameters on aerosol composition, size

Primary and secondary aerosols in Beijing in winter: sources, variations and processes

Directory of Open Access Journals (Sweden)

Y. Sun

2016-07-01

Full Text Available Winter has the worst air pollution of the year in the megacity of Beijing. Despite extensive winter studies in recent years, our knowledge of the sources, formation mechanisms and evolution of aerosol particles is not complete. Here we have a comprehensive characterization of the sources, variations and processes of submicron aerosols that were measured by an Aerodyne high-resolution aerosol mass spectrometer from 17 December 2013 to 17 January 2014 along with offline filter analysis by gas chromatography/mass spectrometry. Our results suggest that submicron aerosols composition was generally similar across the winter of different years and was mainly composed of organics (60 %, sulfate (15 % and nitrate (11 %. Positive matrix factorization of high- and unit-mass resolution spectra identified four primary organic aerosol (POA factors from traffic, cooking, biomass burning (BBOA and coal combustion (CCOA emissions as well as two secondary OA (SOA factors. POA dominated OA, on average accounting for 56 %, with CCOA being the largest contributor (20 %. Both CCOA and BBOA showed distinct polycyclic aromatic hydrocarbons (PAHs spectral signatures, indicating that PAHs in winter were mainly from coal combustion (66 % and biomass burning emissions (18 %. BBOA was highly correlated with levoglucosan, a tracer compound for biomass burning (r2 = 0.93, and made a considerable contribution to OA in winter (9 %. An aqueous-phase-processed SOA (aq-OOA that was strongly correlated with particle liquid water content, sulfate and S-containing ions (e.g. CH2SO2+ was identified. On average aq-OOA contributed 12 % to the total OA and played a dominant role in increasing oxidation degrees of OA at high RH levels (> 50 %. Our results illustrate that aqueous-phase processing can enhance SOA production and oxidation states of OA as well in winter. Further episode analyses highlighted the significant impacts of meteorological parameters on

Is there an aerosol signature of aqueous processing?

Science.gov (United States)

Ervens, B.; Sorooshian, A.

2017-12-01

The formation of aerosol mass in cloud water has been recognized as a substantial source of atmospheric aerosol mass. While sulfate formation can be relatively well constrained, the formation of secondary organic aerosol mass in the aqueous phase (aqSOA) is much more complex due to the multitude of precursors and variety in chemical processes. Aqueous phase processing adds aerosol mass to the droplet mode, which is formed due to mass addition to activated particles in clouds. In addition, it has been shown that aqSOA mass has specific characteristics in terms of oxidation state and hygroscopicity that might help to distinguish it from other SOA sources. Many models do not include detailed chemical mechanisms of sulfate and aqSOA formation and also lack details on the mass distribution of newly formed mass. Mass addition inside and outside clouds modifies different parts of an aerosol population and consequently affects predictions of properties and lifetime of particles. Using a combination of field data analysis and model studies for a variety of air masses, we will show which chemical and physical aerosol properties can be used, in order to identify an `aqueous phase signature' in processed aerosol populations. We will discuss differences in this signature in clean (e.g., background), moderately polluted (e.g., urban) and highly polluted (e.g., biomass burning) air masses and suggest air-mass-specific chemical and/or physical properties that will help to quantify the aqueous-phase derived aerosol mass.

Influence of corium oxidation on fission product release from molten pool

International Nuclear Information System (INIS)

Bechta, S.V.; Krushinov, E.V.; Vitol, S.A.

2009-01-01

Release of low-volatile fission products and core materials from molten oxidic corium was investigated in the EVAN project under the auspices of ISTC. The experiments carried out in cold crucible with induction heating and RASPLAV test facility are described. The results are discussed in terms of reactor application; in particular, pool configuration, melt oxidation kinetics, critical influence of melt surface temperature and oxidation index on the fission product release rate and aerosol particle composition. The relevance of measured high release of Sr from the molten pool for the reactor application is highlighted. Comparisons of the experimental data with those from the COLIMA CA-U3 test and the VERCORS tests, as well as with predictions from IVTANTHERMO and GEMINI/NUCLEA are set. (author)

Evolution of aerosol downwind of a major highway

Science.gov (United States)

Liggio, J.; Staebler, R. M.; Brook, J.; Li, S.; Vlasenko, A. L.; Sjostedt, S. J.; Gordon, M.; Makar, P.; Mihele, C.; Evans, G. J.; Jeong, C.; Wentzell, J. J.; Lu, G.; Lee, P.

2010-12-01

Primary aerosol from traffic emissions can have a considerable impact local and regional scale air quality. In order to assess the effect of these emissions and of future emissions scenarios, air quality models are required which utilize emissions representative of real world conditions. Often, the emissions processing systems which provide emissions input for the air quality models rely on laboratory testing of individual vehicles under non-ambient conditions. However, on the sub-grid scale particle evolution may lead to changes in the primary emitted size distribution and gas-particle partitioning that are not properly considered when the emissions are ‘instantly mixed’ within the grid volume. The affect of this modeling convention on model results is not well understood. In particular, changes in organic gas/particle partitioning may result in particle evaporation or condensation onto pre-existing aerosol. The result is a change in the particle distribution and/or an increase in the organic mass available for subsequent gas-phase oxidation. These effects may be missing from air-quality models, and a careful analysis of field data is necessary to quantify their impact. A study of the sub-grid evolution of aerosols (FEVER; Fast Evolution of Vehicle Emissions from Roadways) was conducted in the Toronto area in the summer of 2010. The study included mobile measurements of particle size distributions with a Fast mobility particle sizer (FMPS), aerosol composition with an Aerodyne aerosol mass spectrometer (AMS), black carbon (SP2, PA, LII), VOCs (PTR-MS) and other trace gases. The mobile laboratory was used to measure the concentration gradient of the emissions at perpendicular distances from the highway as well as the physical and chemical evolution of the aerosol. Stationary sites at perpendicular distances and upwind from the highway also monitored the particle size distribution. In addition, sonic anemometers mounted on the mobile lab provided measurements of

The effects of isoprene and NOx on secondary organic aerosols formed through reversible and irreversible uptake to aerosol water

Science.gov (United States)

El-Sayed, Marwa M. H.; Ortiz-Montalvo, Diana L.; Hennigan, Christopher J.

2018-01-01

Isoprene oxidation produces water-soluble organic gases capable of partitioning to aerosol liquid water. The formation of secondary organic aerosols through such aqueous pathways (aqSOA) can take place either reversibly or irreversibly; however, the split between these fractions in the atmosphere is highly uncertain. The aim of this study was to characterize the reversibility of aqSOA formed from isoprene at a location in the eastern United States under substantial influence from both anthropogenic and biogenic emissions. The reversible and irreversible uptake of water-soluble organic gases to aerosol water was characterized in Baltimore, Maryland, USA, using measurements of particulate water-soluble organic carbon (WSOCp) in alternating dry and ambient configurations. WSOCp evaporation with drying was observed systematically throughout the late spring and summer, indicating reversible aqSOA formation during these times. We show through time lag analyses that WSOCp concentrations, including the WSOCp that evaporates with drying, peak 6 to 11 h after isoprene concentrations, with maxima at a time lag of 9 h. The absolute reversible aqSOA concentrations, as well as the relative amount of reversible aqSOA, increased with decreasing NOx / isoprene ratios, suggesting that isoprene epoxydiol (IEPOX) or other low-NOx oxidation products may be responsible for these effects. The observed relationships with NOx and isoprene suggest that this process occurs widely in the atmosphere, and is likely more important in other locations characterized by higher isoprene and/or lower NOx levels. This work underscores the importance of accounting for both reversible and irreversible uptake of isoprene oxidation products to aqueous particles.

A critical role for autoxidation in the alpha-pinene + OH aerosol system

Science.gov (United States)

Oxidation of monoterpenes results in efficient formation of secondary organic aerosol (SOA) and is included as an SOA source in most chemical transport models. However, current model parameterizations lack a mechanistic dependence of monoterpene SOA on NOx and oxidant identity (e...

Influence of non-ideality on condensation to aerosol

Directory of Open Access Journals (Sweden)

S. Compernolle

2009-02-01

Full Text Available Secondary organic aerosol (SOA is a complex mixture of water and organic molecules. Its composition is determined by the presence of semi-volatile or non-volatile compounds, their saturation vapor pressure and activity coefficient. The activity coefficient is a non-ideality effect and is a complex function of SOA composition. In a previous publication, the detailed chemical mechanism (DCM for α-pinene oxidation and subsequent aerosol formation BOREAM was presented. In this work, we investigate with this DCM the impact of non-ideality by simulating smog chamber experiments for α-pinene degradation and aerosol formation and taking the activity coefficient into account of all molecules in the aerosol phase. Several versions of the UNIFAC method are tested for this purpose, and missing parameters for e.g. hydroperoxides and nitrates are inferred from fittings to activity coefficient data generated using the SPARC model. Alternative approaches to deal with these missing parameters are also tested, as well as an activity coefficient calculation method based on Hansen solubility parameters (HSP. It turns out that for most experiments, non-ideality has only a limited impact on the interaction between the organic molecules, and therefore on SOA yields and composition, when water uptake is ignored. The reason is that often, the activity coefficient is on average close to 1 and, specifically for high-VOC experiments, partitioning is not very sensitive on the activity coefficient because the equilibrium is shifted strongly towards condensation. Still, for ozonolysis experiments with low amounts of volatile organic carbon (low-VOC, the UNIFAC parameterization of Raatikainen et al. leads to significantly higher SOA yields (by up to a factor 1.6 compared to the ideal case and to other parameterizations. Water uptake is model dependent, in the order: ideal > UNIFAC-Raatikainen > UNIFAC-Peng > UNIFAC-Hansen ≈ UNIFAC-Magnussen ≈ UNIFAC-Ming. In the absence

Formation of secondary aerosols from gasoline vehicle exhaust when mixing with SO2

Directory of Open Access Journals (Sweden)

T. Liu

2016-01-01

Full Text Available Sulfur dioxide (SO2 can enhance the formation of secondary aerosols from biogenic volatile organic compounds (VOCs, but its influence on secondary aerosol formation from anthropogenic VOCs, particularly complex mixtures like vehicle exhaust, remains uncertain. Gasoline vehicle exhaust (GVE and SO2, a typical pollutant from coal burning, are directly co-introduced into a smog chamber, in this study, to investigate the formation of secondary organic aerosols (SOA and sulfate aerosols through photooxidation. New particle formation was enhanced, while substantial sulfate was formed through the oxidation of SO2 in the presence of high concentration of SO2. Homogenous oxidation by OH radicals contributed a negligible fraction to the conversion of SO2 to sulfate, and instead the oxidation by stabilized Criegee intermediates (sCIs, formed from alkenes in the exhaust reacting with ozone, dominated the conversion of SO2. After 5 h of photochemical aging, GVE's SOA production factor revealed an increase by 60–200 % in the presence of high concentration of SO2. The increase could principally be attributed to acid-catalyzed SOA formation as evidenced by the strong positive linear correlation (R2 = 0.97 between the SOA production factor and in situ particle acidity calculated by the AIM-II model. A high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS resolved OA's relatively lower oxygen-to-carbon (O : C (0.44 ± 0.02 and higher hydrogen-to-carbon (H : C (1.40 ± 0.03 molar ratios for the GVE / SO2 mixture, with a significantly lower estimated average carbon oxidation state (OSc of −0.51 ± 0.06 than −0.19 ± 0.08 for GVE alone. The relative higher mass loading of OA in the experiments with SO2 might be a significant explanation for the lower SOA oxidation degree.

Status of the LWR aerosol containment experiments (LACE) program

International Nuclear Information System (INIS)

Bloom, G.R.; Dickinson, D.R.; Hilliard, R.K.; McCormack, J.D.; Muhlestein, L.D.; Rahn, F.J.

1985-01-01

The LACE program, sponsored by an international consortium, is investigating inherent aerosol behavior for three postulated high consequence accident sequences; the containment bypass or V-sequence, failure to isolate containment, and delayed containment failure. Six large-scale tests are described which focus on these accident situations and which will be completed in the Containment Systems Test Facility at the Hanford Engineering Development Laboratory. The aerosol generation systems used to generate soluble and insoluble aerosols for the large-scale tests are described. The report then focuses on those tests which deal with the containment bypass accident sequence. Test results are presented and discussed for three containment bypass scoping tests

Scanning Transmission X-ray Microscopy: Applications in Atmospheric Aerosol Research

Energy Technology Data Exchange (ETDEWEB)

Moffet, Ryan C.; Tivanski, Alexei V.; Gilles, Mary K.

2011-01-20

Scanning transmission x-ray microscopy (STXM) combines x-ray microscopy and near edge x-ray absorption fine structure spectroscopy (NEXAFS). This combination provides spatially resolved bonding and oxidation state information. While there are reviews relevant to STXM/NEXAFS applications in other environmental fields (and magnetic materials) this chapter focuses on atmospheric aerosols. It provides an introduction to this technique in a manner approachable to non-experts. It begins with relevant background information on synchrotron radiation sources and a description of NEXAFS spectroscopy. The bulk of the chapter provides a survey of STXM/NEXAFS aerosol studies and is organized according to the type of aerosol investigated. The purpose is to illustrate the current range and recent growth of scientific investigations employing STXM-NEXAFS to probe atmospheric aerosol morphology, surface coatings, mixing states, and atmospheric processing.

Development of an aerosol decontamination factor evaluation method using an aerosol spectrometer

International Nuclear Information System (INIS)

Kanai, Taizo; Furuya, Masahiro; Arai, Takahiro; Nishi, Yoshihisa

2016-01-01

Highlights: • Aerosol DF of each diameter is evaluable by using optical scattering method. • Outlet aerosol concentration shows exponential decay by the submergence. • This decay constant depends on the aerosol diameter. • Aerosol DF at water scrubber is described by simple equation. - Abstract: During a severe nuclear power plant accident, the release of fission products into containment and an increase in containment pressure are assumed to be possible. When the containment is damaged by excess pressure or temperature, radioactive materials are released. Pressure suppression pools, containment spray systems and a filtered containment venting system (FCVS) reduce containment pressure and reduce the radioactive release into the environment. These devices remove radioactive materials via various mechanisms. Pressure suppression pools remove radioactive materials by pool scrubbing. Spray systems remove radioactive materials by droplet−aerosol interaction. FCVS, which is installed in the exhaust system, comprises multi-scrubbers (venturi-scrubber, pool scrubbing, static mixer, metal−fiber filter and molecular sieve). For the particulate radioactive materials, its size affects the removal performance and a number of studies have been performed on the removal effect of radioactive materials. This study has developed a new means of evaluating aerosol removal efficiency. The aerosol number density of each effective diameter (light scattering equivalent diameter) is measured using an optical method, while the decontamination factor (DF) of each effective diameter is evaluated by the inlet outlet number density ratio. While the applicable scope is limited to several conditions (geometry of test section: inner diameter 500 mm × height 8.0 m, nozzle shape and air-water ambient pressure conditions), this study has developed a numerical model which defines aerosol DF as a function of aerosol diameter (d) and submergences (x).

Development of an aerosol decontamination factor evaluation method using an aerosol spectrometer

Energy Technology Data Exchange (ETDEWEB)

Kanai, Taizo, E-mail: t-kanai@criepi.denken.or.jp; Furuya, Masahiro, E-mail: furuya@criepi.denken.or.jp; Arai, Takahiro, E-mail: t-arai@criepi.denken.or.jp; Nishi, Yoshihisa, E-mail: y-nishi@criepi.denken.or.jp

2016-07-15

Highlights: • Aerosol DF of each diameter is evaluable by using optical scattering method. • Outlet aerosol concentration shows exponential decay by the submergence. • This decay constant depends on the aerosol diameter. • Aerosol DF at water scrubber is described by simple equation. - Abstract: During a severe nuclear power plant accident, the release of fission products into containment and an increase in containment pressure are assumed to be possible. When the containment is damaged by excess pressure or temperature, radioactive materials are released. Pressure suppression pools, containment spray systems and a filtered containment venting system (FCVS) reduce containment pressure and reduce the radioactive release into the environment. These devices remove radioactive materials via various mechanisms. Pressure suppression pools remove radioactive materials by pool scrubbing. Spray systems remove radioactive materials by droplet−aerosol interaction. FCVS, which is installed in the exhaust system, comprises multi-scrubbers (venturi-scrubber, pool scrubbing, static mixer, metal−fiber filter and molecular sieve). For the particulate radioactive materials, its size affects the removal performance and a number of studies have been performed on the removal effect of radioactive materials. This study has developed a new means of evaluating aerosol removal efficiency. The aerosol number density of each effective diameter (light scattering equivalent diameter) is measured using an optical method, while the decontamination factor (DF) of each effective diameter is evaluated by the inlet outlet number density ratio. While the applicable scope is limited to several conditions (geometry of test section: inner diameter 500 mm × height 8.0 m, nozzle shape and air-water ambient pressure conditions), this study has developed a numerical model which defines aerosol DF as a function of aerosol diameter (d) and submergences (x).

Production of N2O5 and ClNO2 through Nocturnal Processing of Biomass-Burning Aerosol.

Science.gov (United States)

Ahern, Adam T; Goldberger, Lexie; Jahl, Lydia; Thornton, Joel; Sullivan, Ryan C

2018-01-16

Biomass burning is a source of both particulate chloride and nitrogen oxides, two important precursors for the formation of nitryl chloride (ClNO 2 ), a source of atmospheric oxidants that is poorly prescribed in atmospheric models. We investigated the ability of biomass burning to produce N 2 O 5 (g) and ClNO 2 (g) through nocturnal chemistry using authentic biomass-burning emissions in a smog chamber. There was a positive relationship between the amount of ClNO 2 formed and the total amount of particulate chloride emitted and with the chloride fraction of nonrefractory particle mass. In every fuel tested, dinitrogen pentoxide (N 2 O 5 ) formed quickly, following the addition of ozone to the smoke aerosol, and ClNO 2 (g) production promptly followed. At atmospherically relevant relative humidities, the particulate chloride in the biomass-burning aerosol was rapidly but incompletely displaced, likely by the nitric acid produced largely by the heterogeneous uptake of N 2 O 5 (g). Despite this chloride acid displacement, the biomass-burning aerosol still converted on the order of 10% of reacted N 2 O 5 (g) into ClNO 2 (g). These experiments directly confirm that biomass burning is a potentially significant source of atmospheric N 2 O 5 and ClNO 2 to the atmosphere.

Modeling SOA formation from the oxidation of intermediate volatility n-alkanes

Directory of Open Access Journals (Sweden)

J. Lee-Taylor

2012-08-01

Full Text Available The chemical mechanism leading to SOA formation and ageing is expected to be a multigenerational process, i.e. a successive formation of organic compounds with higher oxidation degree and lower vapor pressure. This process is here investigated with the explicit oxidation model GECKO-A (Generator of Explicit Chemistry and Kinetics of Organics in the Atmosphere. Gas phase oxidation schemes are generated for the C8–C24 series of n-alkanes. Simulations are conducted to explore the time evolution of organic compounds and the behavior of secondary organic aerosol (SOA formation for various preexisting organic aerosol concentration (COA. As expected, simulation results show that (i SOA yield increases with the carbon chain length of the parent hydrocarbon, (ii SOA yield decreases with decreasing COA, (iii SOA production rates increase with increasing COA and (iv the number of oxidation steps (i.e. generations needed to describe SOA formation and evolution grows when COA decreases. The simulated oxidative trajectories are examined in a two dimensional space defined by the mean carbon oxidation state and the volatility. Most SOA contributors are not oxidized enough to be categorized as highly oxygenated organic aerosols (OOA but reduced enough to be categorized as hydrocarbon like organic aerosols (HOA, suggesting that OOA may underestimate SOA. Results show that the model is unable to produce highly oxygenated aerosols (OOA with large yields. The limitations of the model are discussed.

Preparation and characterization of magnetizable aerosols.

Science.gov (United States)

Baumann, Romy; Glöckl, Gunnar; Nagel, Stefan; Weitschies, Werner

2012-04-11

Magnetizable aerosols can be used for inhalative magnetic drug targeting in order to enhance the drug concentration at a certain target site within the lung. The aim of the present study was to clarify how a typical ferrofluid can be atomized in a reproducible way. The influence of the atomization principle, the concentration of magnetic nanoparticles within the carrier liquid and the addition of commonly used pharmaceutical excipients on the aerosol droplet size were investigated. Iron oxide (magnetite) nanoparticles were synthesized by alkaline precipitation of mixtures of iron(II)- and iron(III)-chloride and coated with citric acid. The resulting ferrofluid was characterized by photon correlation spectroscopy and vibrating sample magnetometry. Two different nebulizers (Pari Boy and eFlow) with different atomization principles were used to generate ferrofluid aerosols. A range of substances that influence the surface tension, viscosity, density or vapor pressure of the ferrofluid were added to investigate their impact on the generated aerosol droplets. The particle size was determined by laser diffraction. A stable ferrofluid with a magnetic core diameter of 10.7 ± 0.45 nm and a hydrodynamic diameter of 124 nm was nebulized by Pari Boy and eFlow. The aerosol droplet size of Pari Boy was approximately 2.5 μm and remained unaffected by the addition of substances that changed the physical properties of the solvent. The droplet size of aerosols generated by eFlow was approximately 5 μm. It was significantly reduced by the addition of Cremophor RH 40, glycerol, polyvinyl pyrrolidone and ethanol. Copyright © 2012 Elsevier B.V. All rights reserved.

Contamination smoke: a simulation of heavy metal containing aerosols from fires in plutonium glove boxes: part II

International Nuclear Information System (INIS)

Buijs, K.; Chavane de Dalmassy, B.; Baumgaertner, E.

1992-01-01

The study of the dispersion of plutonium bearing aerosols during glove box fires on a laboratory scale has been, in part I of this work, focussed on fires of polymethylmethacrylate (PMMA - the major glove box construction material) whose surfaces were contaminated with cerium-europium oxide powder as a substitute for plutonium-uranium oxide. The present part II completes the study with comparative fire experiments involving contaminated samples of various glove box materials burning in or exposed to the flames of the standardized 0.6 MW fire source previously developed. Beyond spreading of the Ce-Eu-oxide powder as mentioned above, the other important surface contamination process is used, i.e. deposition and subsequent drying of droplets from acid cerium-europium solutions. It is shown that, among the tested materials, and with the exception of synthetic glove rubber, burning PMMA spreads the most radioactive contamination. On the other hand, this potential risk is much lower for fires involving materials contaminated from solution deposition than from powder or pellets. Attempts to measure the airborne contaminant particle sizes did not yield conclusive results. They suggest, however, that contamination from solutions leads to smaller heavy-metal containing aerosol particles than contamination with powder

Aqueous Oxidation of Green Leaf Volatiles as a Source of Secondary Organic Aerosol

Science.gov (United States)

Richards-Henderson, N. K.; Hansel, A.; Pham, A. T.; Vempati, H. S.; Valsaraj, K. T.; Anastasio, C.

2013-12-01

Vegetation emits volatile oxygenated hydrocarbons - the green leaf volatiles (GLVs) - which are formed from the biochemical conversion of linoleic and linolenic acids within plant cells. Stress or damage to vegetation can significantly elevate emission fluxes of these compounds, some of which are fairly water soluble. Aqueous-phase reactions of the GLVs with photochemically generated oxidants - such as hydroxyl radical (OH), singlet oxygen (1O2) and excited triplet states of organic compounds (3C*) _ might then form low-volatility products that can act as secondary organic aerosol (SOA). In order to determine if GLVs can be a significant source of secondary organic carbon in fogwater, studies of GLVs in laboratory solutions are needed to elucidate the oxidation kinetics and the corresponding SOA mass yields. In this study we are determining the second-order rate constants, and SOA mass yields, for five GLVs (cis-3-hexen-1-ol, cis-3-hexenylacetate, methyl salicylate, methyl jasmonate, and 2-methyl-3-butene-2-ol) reacting with OH,1O2 and 3C*. Experiments are performed at relevant fog water pHs, temperatures, and oxidant concentrations. Rate constants are determined using a relative rate approach in which the decay of GLVs and reference compounds are monitored as function of time by HPLC. The capacity of GLVs to form aqueous SOA was determined by following the formation of their decomposition products with HPLC-UV/DAD and HPLC-ESI/MS. SOA mass yields are measured gravimetrically from laboratory solutions containing atmospherically relevant concentrations of photooxidants and GLVs, and irradiated with simulated sunlight. We will use our results to assess the potential contribution of aqueous GLV reactions as a source of SOA in cloudy or foggy atmospheres.

Laboratory studies of stratospheric aerosol chemistry

Science.gov (United States)

Molina, Mario J.

1996-01-01

In this report we summarize the results of the two sets of projects funded by the NASA grant NAG2-632, namely investigations of various thermodynamic and nucleation properties of the aqueous acid system which makes up stratospheric aerosols, and measurements of reaction probabilities directly on ice aerosols with sizes corresponding to those of polar stratospheric cloud particles. The results of these investigations are of importance for the assessment of the potential stratospheric effects of future fleets of supersonic aircraft. In particular, the results permit to better estimate the effects of increased amounts of water vapor and nitric acid (which forms from nitrogen oxides) on polar stratospheric clouds and on the chemistry induced by these clouds.

Ambient Aerosol in Southeast Asia: High Resolution Aerosol Mass Spectrometer Measurements Over Oil Palm (Elaeis guineensis)

Science.gov (United States)

Phillips, G.; Dimarco, C.; Misztal, P.; Nemitz, E.; Farmer, D.; Kimmel, J.; Jimenez, J.

2008-12-01

The emission of organic compounds in the troposphere is important factor in the formation of secondary organic aerosol (SOA). A very large proportion of organic material emitted globally is estimated to arise from biogenic sources, with almost half coming from tropical and sub-tropical forests. Preliminary analyses of leave cuvette emission studies suggest that oil palm (Elaeis guineensis) is a significantly larger source of isoprene than tropical forest. Much larger sources of isoprene over oil palm allied with a larger anthropogenic component of local emissions contrast greatly with the remote tropical forest environment and therefore the character of SOA formed may differ significantly. These issues, allied with the high price of palm oil on international markets leading to increased use of land for oil palm production, could give rise to rapidly changing chemical and aerosol regimes in the tropics. It is therefore important to understand the current emissions and composition of organic aerosol over all important land-uses in the tropical environment. This in turn will lead to a greater understanding of the present, and to an improvement in predictive capacity for the future system. To help address these issues, a high resolution time of flight aerosol mass spectrometer (HR-ToF-AMS) was deployed in the Sabahmas (PPB OIL) oil palm plantation near Lahad Datu, in Eastern Sabah, as part of the field component of the Aerosol Coupling in the Earth System (ACES) project, part of the UK NERC APPRAISE program. This project was allied closely with measurements made of similar chemical species and aerosol components at a forest site in the Danum Valley as part of the UK Oxidant and Particle Photochemical Processes above a Southeast Asian tropical rainforest (OP3) project. Measurements of submicron non- refractory aerosol composition are presented along with some preliminary analysis of chemically resolved aerosol fluxes made with a new eddy covariance system, based on the

Remote detection and recognition of bio-aerosols by laser-induced fluorescense lidar: practical implementation and field tests

Science.gov (United States)

Boreysho, Anatoly; Savin, Andrey; Morozov, Alexey; Konyaev, Maxim; Konovalov, Konstantin

2007-06-01

Recognition of aerosol clouds material at some significant distance is now a key requirement for the wide range of applications. The elastic backscatter lidar have demonstrated high capabilities in aerosol remote detection, cloud real-time mapping at very long distances for low-concentration natural aerosols as well as artificial ones [1]. However, recognition ability is required to make them more relevant. Laser-induced fluorescence (LIF) looks very promising with respect to the recognition problem. New approach based on mobile lidar complex [2] equipped by spectrally-and range-resolved LIF-sensor is described as well as some results of field tests. The LIF-sensor consists of four-harmonics Nd:YAG laser equipped by an output expander to provide final beam divergence camera collimated with the lidar scanning direction. The LIF-lidar is mounted on a truck-based platform (20-feet container) as a part of multi-purpose mobile lidar complex and adjusted for field conditions.

The influence of chemistry on severe accident phenomena in integral tests

International Nuclear Information System (INIS)

Hobbins, R.R.; Osetek, D.J.; Hagrman, D.L.

1988-01-01

The influence of chemical processes on severe accident phenomena in integral tests is reviewed and recommendations for areas of additional work are made. The results reviewed include those from tests conducted in the in-pile facilities at ACRR, PBF, and TREAT and the TMI-2 accident. Progress has been made in understanding the influence of chemistry on important severe accident phenomena such as core melt progression, hydrogen generation, aerosol generation and transport, and fission product release and transport (including revaporization). An example is the chemistry of volatile fission products, especially iodine and tellurium. Areas where understanding is inadequate are also apparent, such as chemical interactions between fission product vapors and aerosols. Influential chemical processes reviewed include oxidation by steam and interactions among control, structural, fuel, fission product, and aerosol materials

Chemical composition, sources and secondary processes of aerosols in Baoji city of northwest China

Science.gov (United States)

Wang, Y. C.; Huang, R.-J.; Ni, H. Y.; Chen, Y.; Wang, Q. Y.; Li, G. H.; Tie, X. X.; Shen, Z. X.; Huang, Y.; Liu, S. X.; Dong, W. M.; Xue, P.; Fröhlich, R.; Canonaco, F.; Elser, M.; Daellenbach, K. R.; Bozzetti, C.; El Haddad, I.; Prévôt, A. S. H.; Canagaratna, M. R.; Worsnop, D. R.; Cao, J. J.

2017-06-01

Particulate air pollution is a severe environmental problem in China, affecting visibility, air quality, climate and human health. However, previous studies focus mainly on large cities such as Beijing, Shanghai, and Guangzhou. In this study, an Aerodyne Aerosol Chemical Speciation Monitor was deployed in Baoji, a middle size inland city in northwest China from 26 February to 27 March 2014. The non-refractory submicron aerosol (NR-PM1) was dominated by organics (55%), followed by sulfate (16%), nitrate (15%), ammonium (11%) and chloride (3%). A source apportionment of the organic aerosol (OA) was performed with the Sofi (Source Finder) interface of ME-2 (Multilinear Engine), and six main sources/factors were identified and classified as hydrocarbon-like OA (HOA), cooking OA (COA), biomass burning OA (BBOA), coal combustion OA (CCOA), less oxidized oxygenated OA (LO-OOA) and more oxidized oxygenated OA (MO-OOA), which contributed 20%, 14%, 13%, 9%, 23% and 21% of total OA, respectively. The contribution of secondary components shows increasing trends from clean days to polluted days, indicating the importance of secondary aerosol formation processes in driving particulate air pollution. The formation of LO-OOA and MO-OOA is mainly driven by photochemical reactions, but significantly influenced by aqueous-phase chemistry during periods of low atmospheric oxidative capacity.

UV photodissociation spectroscopy of oxidized undecylenic acid films.

Science.gov (United States)

Gomez, Anthony L; Park, Jiho; Walser, Maggie L; Lin, Ao; Nizkorodov, Sergey A

2006-03-16

Oxidation of thin multilayered films of undecylenic (10-undecenoic) acid by gaseous ozone was investigated using a combination of spectroscopic and mass spectrometric techniques. The UV absorption spectrum of the oxidized undecylenic acid film is significantly red-shifted compared to that of the initial film. Photolysis of the oxidized film in the tropospheric actinic region (lambda > 295 nm) readily produces formaldehyde and formic acid as gas-phase products. Photodissociation action spectra of the oxidized film suggest that organic peroxides are responsible for the observed photochemical activity. The presence of peroxides is confirmed by mass-spectrometric analysis of the oxidized sample and an iodometric test. Significant polymerization resulting from secondary reactions of Criegee radicals during ozonolysis of the film is observed. The data strongly imply the importance of photochemistry in aging of atmospheric organic aerosol particles.

Volcanic Plume Impact on the Atmosphere and Climate: O- and S-Isotope Insight into Sulfate Aerosol Formation

Directory of Open Access Journals (Sweden)

Erwan Martin

2018-05-01

Full Text Available The impact of volcanic eruptions on the climate has been studied over the last decades and the role played by sulfate aerosols appears to be major. S-bearing volcanic gases are oxidized in the atmosphere into sulfate aerosols that disturb the radiative balance on earth at regional to global scales. This paper discusses the use of the oxygen and sulfur multi-isotope systematics on volcanic sulfates to understand their formation and fate in more or less diluted volcanic plumes. The study of volcanic aerosols collected from air sampling and ash deposits at different distances from the volcanic systems (from volcanic vents to the Earth poles is discussed. It appears possible to distinguish between the different S-bearing oxidation pathways to generate volcanic sulfate aerosols whether the oxidation occurs in magmatic, tropospheric, or stratospheric conditions. This multi-isotopic approach represents an additional constraint on atmospheric and climatic models and it shows how sulfates from volcanic deposits could represent a large and under-exploited archive that, over time, have recorded atmospheric conditions on human to geological timescales.

Mechanisms of Formation of Secondary Organic Aerosols and Implications for Global Radiative Forcing

Energy Technology Data Exchange (ETDEWEB)

Seinfeld, John H. [California Inst. of Technology (CalTech), Pasadena, CA (United States)

2011-12-02

Organic material constitutes about 50% of global atmospheric aerosol mass, and the dominant source of organic aerosol is the oxidation of volatile hydrocarbons, to produce secondary organic aerosol (SOA). Understanding the formation of SOA is crucial to predicting present and future climate effects of atmospheric aerosols. The goal of this program is to significantly increase our understanding of secondary organic aerosol (SOA) formation in the atmosphere. Ambient measurements indicate that the amount of SOA in the atmosphere exceeds that predicted in current models based on existing laboratory chamber data. This would suggest that either the SOA yields measured in laboratory chambers are understated or that all major organic precursors have not been identified. In this research program we are systematically exploring these possibilities.

Aerosol indirect effect on tropospheric ozone via lightning

Science.gov (United States)

Yuan, T.; Remer, L. A.; Bian, H.; Ziemke, J. R.; Albrecht, R. I.; Pickering, K. E.; Oreopoulos, L.; Goodman, S. J.; Yu, H.; Allen, D. J.

2012-12-01

Tropospheric ozone (O3) is a pollutant and major greenhouse gas and its radiative forcing is still uncertain. The unresolved difference between modeled and observed natural background O3 concentrations is a key source of the uncertainty. Here we demonstrate remarkable sensitivity of lightning activity to aerosol loading with lightning activity increasing more than 30 times per unit of aerosol optical depth over our study area. We provide observational evidence that indicates the observed increase in lightning activity is caused by the influx of aerosols from a volcano. Satellite data analyses suggest O3 is increased as a result of aerosol-induced increase in lightning and lightning produced NOx. Model simulations with prescribed lightning change corroborate the satellite data analysis. This aerosol-O3 connection is achieved via aerosol increasing lightning and thus lightning produced nitrogen oxides. This aerosol-lightning-ozone link provides a potential physical mechanism that may account for a part of the model-observation difference in background O3 concentration. More importantly, O3 production increase from this link is concentrated in the upper troposphere, where O3 is most efficient as a greenhouse gas. Both of these implications suggest a stronger O3 historical radiative forcing. This introduces a new pathway, through which increasing in aerosols from pre-industrial time to present day enhances tropospheric O3 production. Aerosol forcing thus has a warming component via its effect on O3 production. Sensitivity simulations suggest that 4-8% increase of tropospheric ozone, mainly in the tropics, is expected if aerosol-lighting-ozone link is parameterized, depending on the background emission scenario. We note, however, substantial uncertainties remain on the exact magnitude of aerosol effect on tropospheric O3 via lightning. The challenges for obtaining a quantitative global estimate of this effect are also discussed. Our results have significant implications

Aerosol retrieval experiments in the ESA Aerosol_cci project

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T. Holzer-Popp

2013-08-01

Full Text Available Within the ESA Climate Change Initiative (CCI project Aerosol_cci (2010–2013, algorithms for the production of long-term total column aerosol optical depth (AOD datasets from European Earth Observation sensors are developed. Starting with eight existing pre-cursor algorithms three analysis steps are conducted to improve and qualify the algorithms: (1 a series of experiments applied to one month of global data to understand several major sensitivities to assumptions needed due to the ill-posed nature of the underlying inversion problem, (2 a round robin exercise of "best" versions of each of these algorithms (defined using the step 1 outcome applied to four months of global data to identify mature algorithms, and (3 a comprehensive validation exercise applied to one complete year of global data produced by the algorithms selected as mature based on the round robin exercise. The algorithms tested included four using AATSR, three using MERIS and one using PARASOL. This paper summarizes the first step. Three experiments were conducted to assess the potential impact of major assumptions in the various aerosol retrieval algorithms. In the first experiment a common set of four aerosol components was used to provide all algorithms with the same assumptions. The second experiment introduced an aerosol property climatology, derived from a combination of model and sun photometer observations, as a priori information in the retrievals on the occurrence of the common aerosol components. The third experiment assessed the impact of using a common nadir cloud mask for AATSR and MERIS algorithms in order to characterize the sensitivity to remaining cloud contamination in the retrievals against the baseline dataset versions. The impact of the algorithm changes was assessed for one month (September 2008 of data: qualitatively by inspection of monthly mean AOD maps and quantitatively by comparing daily gridded satellite data against daily averaged AERONET sun

Chemical characteristics of submicron particles at the central Tibetan Plateau: insights from aerosol mass spectrometry

Science.gov (United States)

Xu, Jianzhong; Zhang, Qi; Shi, Jinsen; Ge, Xinlei; Xie, Conghui; Wang, Junfeng; Kang, Shichang; Zhang, Ruixiong; Wang, Yuhang

2018-01-01

Recent studies have revealed a significant influx of anthropogenic aerosol from South Asia to the Himalayas and Tibetan Plateau (TP) during pre-monsoon period. In order to characterize the chemical composition, sources, and transport processes of aerosol in this area, we carried out a field study during June 2015 by deploying a suite of online instruments including an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-AMS) and a multi-angle absorption photometer (MAAP) at Nam Co station (90°57' E, 30°46' N; 4730 m a.s.l.) at the central of the TP. The measurements were made at a period when the transition from pre-monsoon to monsoon occurred. The average ambient mass concentration of submicron particulate matter (PM1) over the whole campaign was ˜ 2.0 µg m-3, with organics accounting for 68 %, followed by sulfate (15 %), black carbon (8 %), ammonium (7 %), and nitrate (2 %). Relatively higher aerosol mass concentration episodes were observed during the pre-monsoon period, whereas persistently low aerosol concentrations were observed during the monsoon period. However, the chemical composition of aerosol during the higher aerosol concentration episodes in the pre-monsoon season was on a case-by-case basis, depending on the prevailing meteorological conditions and air mass transport routes. Most of the chemical species exhibited significant diurnal variations with higher values occurring during afternoon and lower values during early morning, whereas nitrate peaked during early morning in association with higher relative humidity and lower air temperature. Organic aerosol (OA), with an oxygen-to-carbon ratio (O / C) of 0.94, was more oxidized during the pre-monsoon period than during monsoon (average O / C ratio of 0.72), and an average O / C was 0.88 over the entire campaign period, suggesting overall highly oxygenated aerosol in the central TP. Positive matrix factorization of the high-resolution mass spectra of OA identified two oxygenated

Photochemical aging of aerosol particles in different air masses arriving at Baengnyeong Island, Korea

Science.gov (United States)

Kang, Eunha; Lee, Meehye; Brune, William H.; Lee, Taehyoung; Park, Taehyun; Ahn, Joonyoung; Shang, Xiaona

2018-05-01

Atmospheric aerosol particles are a serious health risk, especially in regions like East Asia. We investigated the photochemical aging of ambient aerosols using a potential aerosol mass (PAM) reactor at Baengnyeong Island in the Yellow Sea during 4-12 August 2011. The size distributions and chemical compositions of aerosol particles were measured alternately every 6 min from the ambient air or through the highly oxidizing environment of a potential aerosol mass (PAM) reactor. Particle size and chemical composition were measured by using the combination of a scanning mobility particle sizer (SMPS) and a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). Inside the PAM reactor, O3 and OH levels were equivalent to 4.6 days of integrated OH exposure at typical atmospheric conditions. Two types of air masses were distinguished on the basis of the chemical composition and the degree of aging: air transported from China, which was more aged with a higher sulfate concentration and O : C ratio, and the air transported across the Korean Peninsula, which was less aged with more organics than sulfate and a lower O : C ratio. For both episodes, the particulate sulfate mass concentration increased in the 200-400 nm size range when sampled through the PAM reactor. A decrease in organics was responsible for the loss of mass concentration in 100-200 nm particles when sampled through the PAM reactor for the organics-dominated episode. This loss was especially evident for the m/z 43 component, which represents less oxidized organics. The m/z 44 component, which represents further oxidized organics, increased with a shift toward larger sizes for both episodes. It is not possible to quantify the maximum possible organic mass concentration for either episode because only one OH exposure of 4.6 days was used, but it is clear that SO2 was a primary precursor of secondary aerosol in northeast Asia, especially during long-range transport from China. In addition

Results of aerosol code comparisons with releases from ACE MCCI tests

International Nuclear Information System (INIS)

Fink, J.K.; Corradini, M.; Hidaka, A.; Hontanon, E.; Mignanelli, M.A.; Schroedl, E.; Strizhov, V.

1992-01-01

Results of aerosol release calculations by six groups from six countries are compared with the releases from ACE MCCI Test L6. The codes used for these calculations included: SOLGASMIX-PV, SOLGASMIX Reactor 1986, CORCON.UW, VANESA 1.01, and CORCON mod2.04/VANESA 1.01. Calculations were performed with the standard VANESA 1.01 code and with modifications to the VANESA code such as the inclusion of various zirconium-silica chemical reactions. Comparisons of results from these calculations were made with Test L6 release fractions for U, Zr, Si, the fission-product elements Te, Ba, Sr, Ce, La, Mo and control materials Ag, In, and Ru. Reasonable agreement was obtained between calculations and Test L6 results for the volatile elements Ag, In and Te. Calculated releases of the low volatility fission products ranged from within an order of magnitude to five orders of magnitude of Test L6 values. Releases were over and underestimated by calculations. Poorest agreements were obtained for Mo and Si

The Pasadena Aerosol Characterization Observatory (PACO: chemical and physical analysis of the Western Los Angeles basin aerosol

Directory of Open Access Journals (Sweden)

S. P. Hersey

2011-08-01

Full Text Available The Pasadena Aerosol Characterization Observatory (PACO represents the first major aerosol characterization experiment centered in the Western/Central Los Angeles Basin. The sampling site, located on the campus of the California Institute of Technology in Pasadena, was positioned to sample a continuous afternoon influx of transported urban aerosol with a photochemical age of 1–2 h and generally free from major local contributions. Sampling spanned 5 months during the summer of 2009, which were broken into 3 regimes on the basis of distinct meteorological conditions. Regime I was characterized by a series of low pressure systems, resulting in high humidity and rainy periods with clean conditions. Regime II typified early summer meteorology, with significant morning marine layers and warm, sunny afternoons. Regime III was characterized by hot, dry conditions with little marine layer influence. Regardless of regime, organic aerosol (OA is the most significant constituent of nonrefractory submicron Los Angeles aerosol (42, 43, and 55 % of total submicron mass in regimes I, II, and III, respectively. The overall oxidation state remains relatively constant on timescales of days to weeks (O:C = 0.44 ± 0.08, 0.55 ± 0.05, and 0.48 ± 0.08 during regimes I, II, and III, respectively, with no difference in O:C between morning and afternoon periods. Periods characterized by significant morning marine layer influence followed by photochemically favorable afternoons displayed significantly higher aerosol mass and O:C ratio, suggesting that aqueous processes may be important in the generation of secondary aerosol and oxidized organic aerosol (OOA in Los Angeles. Online analysis of water soluble organic carbon (WSOC indicates that water soluble organic mass (WSOM reaches maxima near 14:00–15:00 local time (LT, but the percentage of AMS organic mass contributed by WSOM remains relatively constant throughout the day. Sulfate and nitrate reside predominantly

Predicting the mineral composition of dust aerosols - Part 1: Representing key processes

Science.gov (United States)

Perlwitz, J. P.; Pérez García-Pando, C.; Miller, R. L.

2015-02-01

Soil dust aerosols created by wind erosion are typically assigned globally uniform physical and chemical properties within Earth system models, despite known regional variations in the mineral content of the parent soil. Mineral composition of the aerosol particles is important to their interaction with climate, including shortwave absorption and radiative forcing, nucleation of cloud droplets and ice crystals, coating by heterogeneous uptake of sulfates and nitrates, and atmospheric processing of iron into bioavailable forms that increase the productivity of marine phytoplankton. Here, aerosol mineral composition is derived by extending a method that provides the composition of a wet-sieved soil. The extension accounts for measurements showing significant differences between the mineral fractions of the wet-sieved soil and the resulting aerosol concentration. For example, some phyllosilicate aerosols are more prevalent at silt sizes, even though they are nearly absent in a soil whose aggregates are dispersed by wet sieving during analysis. We reconstruct the undispersed size distribution of the original soil that is subject to wind erosion. An empirical constraint upon the relative emission of clay and silt is applied that further differentiates the soil and aerosol mineral composition. In addition, a method is proposed for mixing minerals with small impurities composed of iron oxides. These mixtures are important for transporting iron far from the dust source, because pure iron oxides are more dense and vulnerable to gravitational removal than most minerals comprising dust aerosols. A limited comparison to measurements from North Africa shows that the extension brings the model into better agreement, consistent with a more extensive comparison to global observations as well as measurements of elemental composition downwind of the Sahara, as described in companion articles.

Modelling organic aerosol concentrations and properties during ChArMEx summer campaigns of 2012 and 2013 in the western Mediterranean region

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M. Chrit

2017-10-01

Full Text Available In the framework of the Chemistry-Aerosol Mediterranean Experiment, a measurement site was set up at a remote site (Ersa on Corsica Island in the northwestern Mediterranean Sea. Measurement campaigns performed during the summers of 2012 and 2013 showed high organic aerosol concentrations, mostly from biogenic origin. This work aims to represent the organic aerosol concentrations and properties (oxidation state and hydrophilicity using the air-quality model Polyphemus with a surrogate approach for secondary organic aerosol (SOA formation. Biogenic precursors are isoprene, monoterpenes and sesquiterpenes. In this work, the following model oxidation products of monoterpenes are added: (i a carboxylic acid (MBTCA to represent multi-generation oxidation products in the low-NOx regime, (ii organic nitrate chemistry and (iii extremely low-volatility organic compounds (ELVOCs formed by ozonolysis. The model shows good agreement of measurements of organic concentrations for both 2012 and 2013 summer campaigns. The modelled oxidation property and hydrophilic organic carbon properties of the organic aerosols also agree reasonably well with the measurements. The influence of the different chemical processes added to the model on the oxidation level of organics is studied. Measured and simulated water-soluble organic carbon (WSOC concentrations show that even at a remote site next to the sea, about 64 % of the organic carbon is soluble. The concentrations of WSOC vary with the origins of the air masses and the composition of organic aerosols. The marine organic emissions only contribute to a few percent of the organic mass in PM1, with maxima above the sea.

Modelling organic aerosol concentrations and properties during ChArMEx summer campaigns of 2012 and 2013 in the western Mediterranean region

Science.gov (United States)

Chrit, Mounir; Sartelet, Karine; Sciare, Jean; Pey, Jorge; Marchand, Nicolas; Couvidat, Florian; Sellegri, Karine; Beekmann, Matthias

2017-10-01

In the framework of the Chemistry-Aerosol Mediterranean Experiment, a measurement site was set up at a remote site (Ersa) on Corsica Island in the northwestern Mediterranean Sea. Measurement campaigns performed during the summers of 2012 and 2013 showed high organic aerosol concentrations, mostly from biogenic origin. This work aims to represent the organic aerosol concentrations and properties (oxidation state and hydrophilicity) using the air-quality model Polyphemus with a surrogate approach for secondary organic aerosol (SOA) formation. Biogenic precursors are isoprene, monoterpenes and sesquiterpenes. In this work, the following model oxidation products of monoterpenes are added: (i) a carboxylic acid (MBTCA) to represent multi-generation oxidation products in the low-NOx regime, (ii) organic nitrate chemistry and (iii) extremely low-volatility organic compounds (ELVOCs) formed by ozonolysis. The model shows good agreement of measurements of organic concentrations for both 2012 and 2013 summer campaigns. The modelled oxidation property and hydrophilic organic carbon properties of the organic aerosols also agree reasonably well with the measurements. The influence of the different chemical processes added to the model on the oxidation level of organics is studied. Measured and simulated water-soluble organic carbon (WSOC) concentrations show that even at a remote site next to the sea, about 64 % of the organic carbon is soluble. The concentrations of WSOC vary with the origins of the air masses and the composition of organic aerosols. The marine organic emissions only contribute to a few percent of the organic mass in PM1, with maxima above the sea.

Steam Oxidation Testing in the Severe Accident Test Station

Energy Technology Data Exchange (ETDEWEB)

Pint, Bruce A. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

2017-08-01

After the March 2011 accident at Fukushima Daiichi, Oak Ridge National Laboratory (ORNL) began conducting high temperature steam oxidation testing of candidate materials for accident tolerant fuel (ATF) cladding in August 2011 [1-11]. The ATF concept is to enhance safety margins in light water reactors (LWR) during severe accident scenarios by identifying materials with 100× slower steam oxidation rates compared to current Zr-based alloys. In 2012, the ORNL laboratory equipment was expanded and made available to the entire ATF community as the Severe Accident Test Station (SATS) [4,12]. Compared to the current UO2/Zr-based alloy fuel system, an ATF alternative would significantly reduce the rate of heat and hydrogen generation in the core during a coolant-limited severe accident [13-14]. The steam oxidation behavior of candidate materials is a key metric in the evaluation of ATF concepts and also an important input into models [15-17]. However, initial modeling work of FeCrAl cladding has used incomplete information on the physical properties of FeCrAl. Also, the steam oxidation data being collected at 1200°-1700°C is unique as no prior work has considered steam oxidation of alloys at such high temperatures. Also, because many accident scenarios include steadily increasing temperatures, the required data are not traditional isothermal exposures but exposures with varying “ramp” rates. In some cases, the steam oxidation behavior has been surprising and difficult to interpret. Thus, more fundamental information continues to be collected. In addition, more work continues to focus on commercially-manufactured tube material. This report summarizes recent work to characterize the behavior of candidate alloys exposed to high temperature steam, evaluate steam oxidation behavior in various ramp scenarios and continue to collect integral data on FeCrAl compared to conventional Zr-based cladding.

Continuous air monitor for alpha-emitting aerosol particles

International Nuclear Information System (INIS)

McFarland, A.R.; Ortiz, C.A.; Rodgers, J.C.; Nelson, D.C.

1991-01-01

A new alpha continuous air monitor (CAM) sampler is being developed for use in detecting the presence of alpha-emitting aerosol particles. The effort involves design, fabrication and evaluation of systems for the collection of aerosol and for the processing of data to speciate and quantify the alpha emitters of the interest. At the present time the authors have a prototype of the aerosol sampling system and they have performed wind tunnel tests to characterize the performance of the device for different particle sizes, wind speeds, flow rates and internal design parameters. The results presented herein deal with the aerosol sampling aspects of the new CAM sampler. Wind tunnel tests show that ≥ 50% of 10 μm aerodynamic equivalent diameter (AED) particles penetrate the flow system from the ambient air to the collection filter when the flow rate is 57 L/min (2 cfm) and the wind speed is 1 m/s. The coefficient of variation of deposits of 10 μm AED aerosol particles on the collection filter is 7%. An inlet fractionator for removing high mobility background aerosol particles has been designed and successfully tested. The results show that it is possible to strip 95% of freshly formed radon daughters and 33% of partially aged radon daughters from the aerosol sample. This approach offers the opportunity to improve the signal-to-noise ratio in the alpha energy spectrum region of interest thereby enhancing the performance of background compensation algorithms

Chemical composition, sources and evolution processes of aerosol at an urban site in Yangtze River Delta, China during wintertime

Science.gov (United States)

Zhang, Yunjiang; Tang, Lili; Yu, Hongxia; Wang, Zhuang; Sun, Yele; Qin, Wei; Chen, Wentai; Chen, Changhong; Ding, Aijun; Wu, Jing; Ge, Shun; Chen, Cheng; Zhou, Hong-cang

2015-12-01

To investigate the composition, sources and evolution processes of submicron aerosol during wintertime, a field experiment was conducted during December 1-31, 2013 in urban Nanjing, a megacity in Yangtze River Delta of China. Non-refractory submicron aerosol (NR-PM1) species were measured with an Aerodyne Aerosol Chemical Speciation Monitor. NR-PM1 is dominated by secondary inorganic aerosol (55%) and organic aerosol (OA, 42%) during haze periods. Six OA components were identified by positive matrix factorization of the OA mass spectra. The hydrocarbon-like OA and cooking-related OA represent the local traffic and cooking sources, respectively. A highly oxidized factor related to biomass burning OA accounted for 15% of the total OA mass during haze periods. Three types of oxygenated OA (OOA), i.e., a less-oxidized OOA (LO-OOA), a more-oxidized OOA (MO-OOA), and a low-volatility OOA (LV-OOA), were identified. LO-OOA is likely associated with fresh urban secondary OA. MO-OOA likely represents photochemical products showing a similar diurnal cycle to nitrate with a pronounced noon peak. LV-OOA appears to be a more oxidized factor with a pronounced noon peak. The OA composition is dominated by secondary species, especially during haze events. LO-OOA, MO-OOA and LV-OOA on average account for 11%, (18%), 24% (21%) and 23% (18%) of the total OA mass for the haze (clean) periods respectively. Analysis of meteorological influence suggested that regional transport from the northern and southeastern areas of the city is responsible for large secondary and low-volatility aerosol formation.

Substantial secondary organic aerosol formation in a coniferous forest: observations of both day- and nighttime chemistry

Directory of Open Access Journals (Sweden)

A. K. Y. Lee

2016-06-01

Full Text Available Substantial biogenic secondary organic aerosol (BSOA formation was investigated in a coniferous forest mountain region in Whistler, British Columbia. A largely biogenic aerosol growth episode was observed, providing a unique opportunity to investigate BSOA formation chemistry in a forested environment with limited influence from anthropogenic emissions. Positive matrix factorization of aerosol mass spectrometry (AMS measurement identified two types of BSOA (BSOA-1 and BSOA-2, which were primarily generated by gas-phase oxidation of monoterpenes and perhaps sesquiterpenes. The temporal variations of BSOA-1 and BSOA-2 can be explained by gas–particle partitioning in response to ambient temperature and the relative importance of different oxidation mechanisms between day and night. While BSOA-1 arises from gas-phase ozonolysis and nitrate radical chemistry at night, BSOA-2 is likely less volatile than BSOA-1 and consists of products formed via gas-phase oxidation by OH radical and ozone during the day. Organic nitrates produced through nitrate radical chemistry can account for 22–33 % of BSOA-1 mass at night. The mass spectra of BSOA-1 and BSOA-2 have higher values of the mass fraction of m/z 91 (f91 compared to the background organic aerosol. Using f91 to evaluate BSOA formation pathways in this unpolluted, forested region, heterogeneous oxidation of BSOA-1 is a minor production pathway of BSOA-2.

Radiation protection instrumentation. Monitoring equipment. Radioactive aerosols in the environment

International Nuclear Information System (INIS)

1996-01-01

This international standard applies to portable or installed equipment for continuous monitoring of radioactive aerosols in the environment in normal and emergency conditions. Monitoring involves continuous sampling and, where desirable, automatic start of sampling. The document applies particularly to the following assignments: (i) determination of the volume activity of radionuclides in the form of aerosols, either per time unit, along with its time changes, or in the integral form over a longer time period such as 24 h, and measurement of the volume sampled; (ii) triggering a warning alarm signal if the preset volume activity or time integral of the volume activity of aerosols has been exceeded. The document deals with radioactive aerosol monitor design, testing procedures, and documentation. Appended tables refer to the reference and normal testing conditions, tests in normal testing conditions, tests during changes of the affecting quantities, and tests of the air circuit. (P.A.)

Aerosol activation and cloud processing in the global aerosol-climate model ECHAM5-HAM

Directory of Open Access Journals (Sweden)

G. J. Roelofs

2006-01-01

Full Text Available A parameterization for cloud processing is presented that calculates activation of aerosol particles to cloud drops, cloud drop size, and pH-dependent aqueous phase sulfur chemistry. The parameterization is implemented in the global aerosol-climate model ECHAM5-HAM. The cloud processing parameterization uses updraft speed, temperature, and aerosol size and chemical parameters simulated by ECHAM5-HAM to estimate the maximum supersaturation at the cloud base, and subsequently the cloud drop number concentration (CDNC due to activation. In-cloud sulfate production occurs through oxidation of dissolved SO2 by ozone and hydrogen peroxide. The model simulates realistic distributions for annually averaged CDNC although it is underestimated especially in remote marine regions. On average, CDNC is dominated by cloud droplets growing on particles from the accumulation mode, with smaller contributions from the Aitken and coarse modes. The simulations indicate that in-cloud sulfate production is a potentially important source of accumulation mode sized cloud condensation nuclei, due to chemical growth of activated Aitken particles and to enhanced coalescence of processed particles. The strength of this source depends on the distribution of produced sulfate over the activated modes. This distribution is affected by uncertainties in many parameters that play a direct role in particle activation, such as the updraft velocity, the aerosol chemical composition and the organic solubility, and the simulated CDNC is found to be relatively sensitive to these uncertainties.

Behavior of aerosols in a steam-air environment

International Nuclear Information System (INIS)

Adams, R.E.; Tobias, M.L.; Longest, A.W.

1985-01-01

The behavior of aerosols assumed to be characteristic of those generated during light water reactor (LWR) accident sequences and released into containment is being studied in the Nuclear Safety Pilot Plant (NSPP) which is located at the Oak Ridge National Laboratory (ORNL). The program plan for the NSPP aerosol project provides for the study of the behavior, within containment, of simulated LWR accident aerosols emanating from fuel, reactor core structural materials, and from concrete-molten core materials interactions. The aerodynamic behavior of each of these aerosols was studied individually to establish its characteristics; current experiments involve mixtures of these aerosols to establish their interaction and collective behavior within containment. Tests have been conducted with U 3 O 8 aerosols, Fe 2 O 3 aerosols, and concrete aerosols in an environment of either dry air [relative humidity (RH) less than 20%] or steam-air [relative humidity (RH) approximately 100%] with aerosol mass concentration being the primary experimental variable

Comparison of computer codes related to the sodium oxide aerosol behavior in a containment building

International Nuclear Information System (INIS)

Fermandjian, J.

1984-09-01

In order to ensure that the problems of describing the physical behavior of sodium aerosols, during hypothetical fast reactor accidents, were adequately understood, a comparison of the computer codes (ABC/INTG, PNC, Japan; AEROSIM, UKAEA/SRD, United Kingdom; PARDISEKO IIIb, KfK, Germany; AEROSOLS/A2 and AEROSOLS/B1, CEA France) was undertaken in the frame of the CEC: exercise in which code users have run their own codes with a prearranged input

Sodium fire aerosol loading capacity of several sand and gravel filters

International Nuclear Information System (INIS)

Barreca, J.R.; McCormack, J.D.

1980-04-01

Improved specific loading capacity for sodium fire aerosols was the objective of a sand and gravel test series. The aerosol capacity and related differential pressure of eight aggregate filters is presented. A maximum specific aerosol capacity, for dry aerosol, of 2.4 kg (Na) m -2 was obtained. This filter was loaded to a final differential pressure of 2.6 kPa. The average superficial face velocity was 0.5 cm/s and the average efficiency was 99.8%. The test results indicate that filter capacity increases with aerosol moisture content and with decreasing superficial velocity

submitter Aqueous phase oxidation of sulphur dioxide by ozone in cloud droplets

CERN Document Server

Hoyle, C R; Järvinen, E; Saathoff, H; Dias, A; El Haddad, I; Gysel, M; Coburn, S C; Tröstl, J; Bernhammer, A -K; Bianchi, F; Breitenlechner, M; Corbin, J C; Craven, J; Donahue, N M; Duplissy, J; Ehrhart, S; Frege, C; Gordon, H; Höppel, N; Heinritzi, M; Kristensen, T B; Molteni, U; Nichman, L; Pinterich, T; Prévôt, A S H; Simon, M; Slowik, J G; Steiner, G; Tomé, A; Vogel, A L; Volkamer, R; Wagner, A C; Wagner, R; Wexler, A S; Williamson, C; Winkler, P M; Yan, C; Amorim, A; Dommen, J; Curtius, J; Gallagher, M W; Flagan, R C; Hansel, A; Kirkby, J; Kulmala, M; Möhler, O; Stratmann, F; Worsnop, D R; Baltensperger, U

2016-01-01

The growth of aerosol due to the aqueous phase oxidation of sulfur dioxide by ozone was measured in laboratory-generated clouds created in the Cosmics Leaving OUtdoor Droplets (CLOUD) chamber at the European Organization for Nuclear Research (CERN). Experiments were performed at 10 and −10 °C, on acidic (sulfuric acid) and on partially to fully neutralised (ammonium sulfate) seed aerosol. Clouds were generated by performing an adiabatic expansion – pressurising the chamber to 220 hPa above atmospheric pressure, and then rapidly releasing the excess pressure, resulting in a cooling, condensation of water on the aerosol and a cloud lifetime of approximately 6 min. A model was developed to compare the observed aerosol growth with that predicted using oxidation rate constants previously measured in bulk solutions. The model captured the measured aerosol growth very well for experiments performed at 10 and −10 °C, indicating that, in contrast to some previous studies, the oxidation rates of SO2 in ...

Importance of aerosol non-sphericity in estimating aerosol radiative forcing in Indo-Gangetic Basin.

Science.gov (United States)

Srivastava, Parul; Dey, Sagnik; Srivastava, Atul Kumar; Singh, Sachchidanand; Mishra, S K; Tiwari, Suresh

2017-12-01

Aerosols are usually presumed spherical in shape while estimating the direct radiative forcing (DRF) using observations or in the models. In the Indo-Gangetic Basin (IGB), a regional aerosol hotspot where dust is a major aerosol species and has been observed to be non-spherical in shape, it is important to test the validity of this assumption. We address this issue using measured chemical composition at megacity Delhi, a representative site of the western IGB. Based on the observation, we choose three non-spherical shapes - spheroid, cylinder and chebyshev, and compute their optical properties. Non-spherical dust enhances aerosol extinction coefficient (β ext ) and single scattering albedo (SSA) at visible wavelengths by >0.05km -1 and >0.04 respectively, while it decreases asymmetry parameter (g) by ~0.1. Accounting non-sphericity leads top-of-the-atmosphere (TOA) dust DRF to more cooling due to enhanced backscattering and increases surface dimming due to enhanced β ext . Outgoing shortwave flux at TOA increases by up to 3.3% for composite aerosols with non-spherical dust externally mixed with other spherical species. Our results show that while non-sphericity needs to be accounted for, choice of shape may not be important in estimating aerosol DRF in the IGB. Copyright © 2017 Elsevier B.V. All rights reserved.

Primary aerosol and secondary inorganic aerosol budget over the Mediterranean Basin during 2012 and 2013

Science.gov (United States)

Guth, Jonathan; Marécal, Virginie; Josse, Béatrice; Arteta, Joaquim; Hamer, Paul

2018-04-01

In the frame of the Chemistry-Aerosol Mediterranean Experiment (ChArMEx), we analyse the budget of primary aerosols and secondary inorganic aerosols over the Mediterranean Basin during the years 2012 and 2013. To do this, we use two year-long numerical simulations with the chemistry-transport model MOCAGE validated against satellite- and ground-based measurements. The budget is presented on an annual and a monthly basis on a domain covering 29 to 47° N latitude and 10° W to 38° E longitude. The years 2012 and 2013 show similar seasonal variations. The desert dust is the main contributor to the annual aerosol burden in the Mediterranean region with a peak in spring, and sea salt being the second most important contributor. The secondary inorganic aerosols, taken as a whole, contribute a similar level to sea salt. The results show that all of the considered aerosol types, except for sea salt aerosols, experience net export out of our Mediterranean Basin model domain, and thus this area should be considered as a source region for aerosols globally. Our study showed that 11 % of the desert dust, 22.8 to 39.5 % of the carbonaceous aerosols, 35 % of the sulfate and 9 % of the ammonium emitted or produced into the study domain are exported. The main sources of variability for aerosols between 2012 and 2013 are weather-related variations, acting on emissions processes, and the episodic import of aerosols from North American fires. In order to assess the importance of the anthropogenic emissions of the marine and the coastal areas which are central for the economy of the Mediterranean Basin, we made a sensitivity test simulation. This simulation is similar to the reference simulation but with the removal of the international shipping emissions and the anthropogenic emissions over a 50 km wide band inland along the coast. We showed that around 30 % of the emissions of carbonaceous aerosols and 35 to 60 % of the exported carbonaceous aerosols originates from the marine and

Anthropogenic influence on the distribution of tropospheric sulphate aerosol

Energy Technology Data Exchange (ETDEWEB)

Langner, J; Rodhe, H; Crutzen, P J; Zimmermann, P [Swedish Meteorological and Hydrological Institute, Norrkoeping (Sweden)

1992-10-22

Human activities have increased global emissions of sulphur gases by about a factor of three during the past century, leading to increased sulphate aerosol concentrations, mainly in the Northern Hemisphere. Sulphate aerosols can affect the climate directly, by increasing the backscattering of solar radiation in cloud-free air, and indirectly, by providing additional cloud condensation nuclei. Here a global transport-chemistry model is used to estimate the changes in the distribution of tropospheric sulphate aerosol and deposition of non-seasalt sulphur that have occurred since pre-industrial times. The increase in sulphate aerosol concentration is small over the Southern Hemisphere oceans, but reaches a factor of 100 over northern Europe in winter. Calculations indicate, however, that at most 6% of the anthropogenic sulphur emissions is available for the formation of new aerosol particles. This is because about one-half of the sulphur dioxide is deposited on the Earth's surface, and most of the remainder is oxidized in cloud droplets so that the sulphate becomes associated with pre-existing particles. Even so, the rate of formation of new sulphate particles may have doubled since pre-industrial times. 18 refs., 3 figs.

Non-ammonium reduced nitrogen species in atmospheric aerosol particles

Energy Technology Data Exchange (ETDEWEB)

Dod, R.L.; Gundel, L.A.; Benner, W.H.; Novakov, T.

1983-08-01

The traditional belief that ambient aerosol particles contain nitrogen predominantly in the form of inorganic ionic species such as NH/sub 4//sup +/ and NO/sub 3//sup -/ was challenged about 10 years ago by results from x-ray photoelectron spectroscopic analysis (ESCA) of California aerosol particles. A significant fraction (approx. 50%) of the reduced nitrogen was observed to have an oxidation state more reduced than ammonium, characteristic of organic nitrogen species. We have used a recently developed thermal evolved gas analysis method (NO/sub x/) in conjunction with ESCA to confirm the existence of these species in aerosol particles collected in both the United States and Europe. The agreement of EGA and ESCA analyses indicates that these species are found not only on the surface but also throughout the particles. 9 references, 6 figures.

Atmospheric and aerosol chemistry

International Nuclear Information System (INIS)

McNeill, V. Faye; Ariya, Parisa A.; McGill Univ. Montreal, QC

2014-01-01

This series presents critical reviews of the present position and future trends in modern chemical research. Short and concise reports on chemistry, each written by the world renowned experts. Still valid and useful after 5 or 10 years. More information as well as the electronic version of the whole content available at: springerlink.com. Christian George, Barbara D'Anna, Hartmut Herrmann, Christian Weller, Veronica Vaida, D. J. Donaldson, Thorsten Bartels-Rausch, Markus Ammann Emerging Areas in Atmospheric Photochemistry. Lisa Whalley, Daniel Stone, Dwayne Heard New Insights into the Tropospheric Oxidation of Isoprene: Combining Field Measurements, Laboratory Studies, Chemical Modelling and Quantum Theory. Neil M. Donahue, Allen L. Robinson, Erica R. Trump, Ilona Riipinen, Jesse H. Kroll Volatility and Aging of Atmospheric Organic Aerosol. P. A. Ariya, G. Kos, R. Mortazavi, E. D. Hudson, V. Kanthasamy, N. Eltouny, J. Sun, C. Wilde Bio-Organic Materials in the Atmosphere and Snow: Measurement and Characterization V. Faye McNeill, Neha Sareen, Allison N. Schwier Surface-Active Organics in Atmospheric Aerosols.

Small molecules as tracers in atmospheric secondary organic aerosol

Science.gov (United States)

Yu, Ge

Secondary organic aerosol (SOA), formed from in-air oxidation of volatile organic compounds, greatly affects human health and climate. Although substantial research has been devoted to SOA formation and evolution, the modeled and lab-generated SOA are still low in mass and degree of oxidation compared to ambient measurements. In order to compensate for these discrepancies, the aqueous processing pathway has been brought to attention. The atmospheric waters serve as aqueous reaction media for dissolved organics to undergo further oxidation, oligomerization, or other functionalization reactions, which decreases the vapor pressure while increasing the oxidation state of carbon atoms. Field evidence for aqueous processing requires the identification of tracer products such as organosulfates. We synthesized the standards for two organosulfates, glycolic acid sulfate and lactic acid sulfate, in order to measure their aerosol-state concentration from five distinct locations via filter samples. The water-extracted filter samples were analyzed by LC-MS. Lactic acid sulfate and glycolic acid sulfate were detected in urban locations in the United States, Mexico City, and Pakistan with varied concentrations, indicating their potential as tracers. We studied the aqueous processing reaction between glyoxal and nitrogen-containing species such as ammonium and amines exclusively by NMR spectrometry. The reaction products formic acid and several imidazoles along with the quantified kinetics were reported. The brown carbon generated from these reactions were quantified optically by UV-Vis spectroscopy. The organic-phase reaction between oxygen molecule and alkenes photosensitized by alpha-dicarbonyls were studied in the same manner. We observed the fast kinetics transferring alkenes to epoxides under simulated sunlight. Statistical estimations indicate a very effective conversion of aerosol-phase alkenes to epoxides, potentially forming organosulfates in a deliquescence event and

Volatility measurement of atmospheric submicron aerosols in an urban atmosphere in southern China

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L.-M. Cao

2018-02-01

Full Text Available Aerosol pollution has been a very serious environmental problem in China for many years. The volatility of aerosols can affect the distribution of compounds in the gas and aerosol phases, the atmospheric fates of the corresponding components, and the measurement of the concentration of aerosols. Compared to the characterization of chemical composition, few studies have focused on the volatility of aerosols in China. In this study, a thermodenuder aerosol mass spectrometer (TD-AMS system was deployed to study the volatility of non-refractory submicron particulate matter (PM1 species during winter in Shenzhen. To our knowledge, this paper is the first report of the volatilities of aerosol chemical components based on a TD-AMS system in China. The average PM1 mass concentration during the experiment was 42.7±20.1 µg m−3, with organic aerosol (OA being the most abundant component (43.2 % of the total mass. The volatility of chemical species measured by the AMS varied, with nitrate showing the highest volatility, with a mass fraction remaining (MFR of 0.57 at 50 °C. Organics showed semi-volatile characteristics (the MFR was 0.88 at 50 °C, and the volatility had a relatively linear correlation with the TD temperature (from the ambient temperature to 200 °C, with an evaporation rate of 0.45 % °C−1. Five subtypes of OA were resolved from total OA using positive matrix factorization (PMF for data obtained under both ambient temperature and high temperatures through the TD, including a hydrocarbon-like OA (HOA, accounting for 13.5 %, a cooking OA (COA, 20.6 %, a biomass-burning OA (BBOA, 8.9 %, and two oxygenated OAs (OOAs: a less-oxidized OOA (LO-OOA, 39.1 % and a more-oxidized OOA (MO-OOA, 17.9 %. Different OA factors presented different volatilities, and the volatility sequence of the OA factors at 50 °C was HOA (MFR of 0.56  >  LO-OOA (0.70  >  COA (0.85  ≈  BBOA (0.87�

Real-time measurements of secondary organic aerosol formation and aging from ambient air in an oxidation flow reactor in the Los Angeles area

Science.gov (United States)

Ortega, Amber M.; Hayes, Patrick L.; Peng, Zhe; Palm, Brett B.; Hu, Weiwei; Day, Douglas A.; Li, Rui; Cubison, Michael J.; Brune, William H.; Graus, Martin; Warneke, Carsten; Gilman, Jessica B.; Kuster, William C.; de Gouw, Joost; Gutiérrez-Montes, Cándido; Jimenez, Jose L.

2016-06-01

Field studies in polluted areas over the last decade have observed large formation of secondary organic aerosol (SOA) that is often poorly captured by models. The study of SOA formation using ambient data is often confounded by the effects of advection, vertical mixing, emissions, and variable degrees of photochemical aging. An oxidation flow reactor (OFR) was deployed to study SOA formation in real-time during the California Research at the Nexus of Air Quality and Climate Change (CalNex) campaign in Pasadena, CA, in 2010. A high-resolution aerosol mass spectrometer (AMS) and a scanning mobility particle sizer (SMPS) alternated sampling ambient and reactor-aged air. The reactor produced OH concentrations up to 4 orders of magnitude higher than in ambient air. OH radical concentration was continuously stepped, achieving equivalent atmospheric aging of 0.8 days-6.4 weeks in 3 min of processing every 2 h. Enhancement of organic aerosol (OA) from aging showed a maximum net SOA production between 0.8-6 days of aging with net OA mass loss beyond 2 weeks. Reactor SOA mass peaked at night, in the absence of ambient photochemistry and correlated with trimethylbenzene concentrations. Reactor SOA formation was inversely correlated with ambient SOA and Ox, which along with the short-lived volatile organic compound correlation, indicates the importance of very reactive (τOH ˜ 0.3 day) SOA precursors (most likely semivolatile and intermediate volatility species, S/IVOCs) in the Greater Los Angeles Area. Evolution of the elemental composition in the reactor was similar to trends observed in the atmosphere (O : C vs. H : C slope ˜ -0.65). Oxidation state of carbon (OSc) in reactor SOA increased steeply with age and remained elevated (OSC ˜ 2) at the highest photochemical ages probed. The ratio of OA in the reactor output to excess CO (ΔCO, ambient CO above regional background) vs. photochemical age is similar to previous studies at low to moderate ages and also extends to

Real-time measurements of secondary organic aerosol formation and aging from ambient air in an oxidation flow reactor in the Los Angeles area

Directory of Open Access Journals (Sweden)

A. M. Ortega

2016-06-01

Full Text Available Field studies in polluted areas over the last decade have observed large formation of secondary organic aerosol (SOA that is often poorly captured by models. The study of SOA formation using ambient data is often confounded by the effects of advection, vertical mixing, emissions, and variable degrees of photochemical aging. An oxidation flow reactor (OFR was deployed to study SOA formation in real-time during the California Research at the Nexus of Air Quality and Climate Change (CalNex campaign in Pasadena, CA, in 2010. A high-resolution aerosol mass spectrometer (AMS and a scanning mobility particle sizer (SMPS alternated sampling ambient and reactor-aged air. The reactor produced OH concentrations up to 4 orders of magnitude higher than in ambient air. OH radical concentration was continuously stepped, achieving equivalent atmospheric aging of 0.8 days–6.4 weeks in 3 min of processing every 2 h. Enhancement of organic aerosol (OA from aging showed a maximum net SOA production between 0.8–6 days of aging with net OA mass loss beyond 2 weeks. Reactor SOA mass peaked at night, in the absence of ambient photochemistry and correlated with trimethylbenzene concentrations. Reactor SOA formation was inversely correlated with ambient SOA and Ox, which along with the short-lived volatile organic compound correlation, indicates the importance of very reactive (τOH  ∼  0.3 day SOA precursors (most likely semivolatile and intermediate volatility species, S/IVOCs in the Greater Los Angeles Area. Evolution of the elemental composition in the reactor was similar to trends observed in the atmosphere (O : C vs. H : C slope  ∼  −0.65. Oxidation state of carbon (OSc in reactor SOA increased steeply with age and remained elevated (OSC  ∼  2 at the highest photochemical ages probed. The ratio of OA in the reactor output to excess CO (ΔCO, ambient CO above regional background vs. photochemical age is similar to

The economics (or lack thereof) of aerosol geoengineering

Science.gov (United States)

Goes, M.; Keller, K.; Tuana, N.

2009-04-01

Anthropogenic greenhouse gas emissions are changing the Earth's climate and impose substantial risks for current and future generations. What are scientifically sound, economically viable, and ethically defendable strategies to manage these climate risks? Ratified international agreements call for a reduction of greenhouse gas emissions to avoid dangerous anthropogenic interference with the climate system. Recent proposals, however, call for the deployment of a different approach: to geoengineer climate by injecting aerosol precursors into the stratosphere. Published economic studies typically suggest that substituting aerosol geoengineering for abatement of carbon dioxide emissions results in large net monetary benefits. However, these studies neglect the risks of aerosol geoengineering due to (i) the potential for future geoengineering failures and (ii) the negative impacts associated with the aerosol forcing. Here we use a simple integrated assessment model of climate change to analyze potential economic impacts of aerosol geoengineering strategies over a wide range of uncertain parameters such as climate sensitivity, the economic damages due to climate change, and the economic damages due to aerosol geoengineering forcing. The simplicity of the model provides the advantages of parsimony and transparency, but it also imposes severe caveats on the interpretation of the results. For example, the analysis is based on a globally aggregated model and is hence silent on the question of intragenerational distribution of costs and benefits. In addition, the analysis neglects the effects of endogenous learning about the climate system. We show that the risks associated with a future geoengineering failure and negative impacts of aerosol forcings can cause geoenginering strategies to fail an economic cost-benefit test. One key to this finding is that a geoengineering failure would lead to dramatic and abrupt climatic changes. The monetary damages due to this failure can

Comparison of Aerosol Delivery by Face Mask and Tracheostomy Collar.

Science.gov (United States)

Bugis, Alaa A; Sheard, Meryl M; Fink, James B; Harwood, Robert J; Ari, Arzu

2015-09-01

The purpose of this study was to compare the performance of a tracheostomy collar, Wright mask, and aerosol mask attached to a jet nebulizer in facilitating aerosolized medication delivery to the lungs. We also compared albuterol delivery with open versus closed fenestration and determined the effect of inspiratory-expiratory ratio (I:E) on aerosol delivery. Albuterol (2.5 mg/3 mL) was administered to an in vitro model consisting of an adult teaching mannequin extrathoracic and upper airway with stoma intubated with an 8-mm fenestrated tracheostomy tube. The cuff was deflated. A collecting filter at the level of the bronchi was connected to a breathing simulator at a tidal volume of 400 mL, breathing frequency of 20 breaths/min, and I:E of 2:1 and 1:2. A jet nebulizer was operated with O2 at 8 L/min. Each interface was tested in triplicate. The flow was discontinued at the end of nebulization. For each test, the nebulizer was attached to a tracheostomy collar with the fenestration open or closed, a Wright mask, or an aerosol mask. Drug was analyzed by spectrophotometry (276 nm). A paired t test and analysis of variance were performed (P mask (4.1 ± 0.6%) and aerosol mask (3.5 ± 0.04%) were both less than with the tracheostomy collar under either condition (P mask (7.2 ± 0.6%), and aerosol mask (6.1 ± 0.5%). In an adult tracheostomy model, the tracheostomy collar delivered more aerosol to the bronchi than the Wright or aerosol mask. An I:E of 2:1 caused greater aerosol deposition compared with an I:E of 1:2. During aerosol administration via a tracheostomy collar, closing the fenestration improved aerosol delivery. Copyright © 2015 by Daedalus Enterprises.

Organic aerosols

International Nuclear Information System (INIS)

Penner, J.E.

1994-01-01

Organic aerosols scatter solar radiation. They may also either enhance or decrease concentrations of cloud condensation nuclei. This paper summarizes observed concentrations of aerosols in remote continental and marine locations and provides estimates for the sources of organic aerosol matter. The anthropogenic sources of organic aerosols may be as large as the anthropogenic sources of sulfate aerosols, implying a similar magnitude of direct forcing of climate. The source estimates are highly uncertain and subject to revision in the future. A slow secondary source of organic aerosols of unknown origin may contribute to the observed oceanic concentrations. The role of organic aerosols acting as cloud condensation nuclei (CCN) is described and it is concluded that they may either enhance or decrease the ability of anthropogenic sulfate aerosols to act as CCN

X-ray fluorimetry in tests of the aerosol substances. [In the atmosphere]. Rentgenowska analiza fluorescencyjna w badaniach skladu pierwiastkowego aerozoli w atmosferze

Energy Technology Data Exchange (ETDEWEB)

Walentek, A.; Cudny, W.; Marzec, J.; Pawlowski, Z.; Zaremba, K. (Politechnika Warszawska, Warsaw (Poland). Inst. Radioelektroniki)

1992-01-01

Test results of aerosol samples from atmospheric air collected from membrane drains were presented. The ANFLU-2 analyzer constructed at the Warsaw Technical University were used for testing. (author). 3 figs, 1 tab.

Aqueous-phase mechanism for secondary organic aerosol formation from isoprene: application to the southeast United States and co-benefit of SO2 emission controls

Directory of Open Access Journals (Sweden)

E. A. Marais

2016-02-01

Full Text Available Isoprene emitted by vegetation is an important precursor of secondary organic aerosol (SOA, but the mechanism and yields are uncertain. Aerosol is prevailingly aqueous under the humid conditions typical of isoprene-emitting regions. Here we develop an aqueous-phase mechanism for isoprene SOA formation coupled to a detailed gas-phase isoprene oxidation scheme. The mechanism is based on aerosol reactive uptake coefficients (γ for water-soluble isoprene oxidation products, including sensitivity to aerosol acidity and nucleophile concentrations. We apply this mechanism to simulation of aircraft (SEAC4RS and ground-based (SOAS observations over the southeast US in summer 2013 using the GEOS-Chem chemical transport model. Emissions of nitrogen oxides (NOx  ≡  NO + NO2 over the southeast US are such that the peroxy radicals produced from isoprene oxidation (ISOPO2 react significantly with both NO (high-NOx pathway and HO2 (low-NOx pathway, leading to different suites of isoprene SOA precursors. We find a mean SOA mass yield of 3.3 % from isoprene oxidation, consistent with the observed relationship of total fine organic aerosol (OA and formaldehyde (a product of isoprene oxidation. Isoprene SOA production is mainly contributed by two immediate gas-phase precursors, isoprene epoxydiols (IEPOX, 58 % of isoprene SOA from the low-NOx pathway and glyoxal (28 % from both low- and high-NOx pathways. This speciation is consistent with observations of IEPOX SOA from SOAS and SEAC4RS. Observations show a strong relationship between IEPOX SOA and sulfate aerosol that we explain as due to the effect of sulfate on aerosol acidity and volume. Isoprene SOA concentrations increase as NOx emissions decrease (favoring the low-NOx pathway for isoprene oxidation, but decrease more strongly as SO2 emissions decrease (due to the effect of sulfate on aerosol acidity and volume. The US Environmental Protection Agency (EPA projects 2013–2025 decreases in

Chemical characteristics of submicron particles at the central Tibetan Plateau: insights from aerosol mass spectrometry

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J. Xu

2018-01-01

Full Text Available Recent studies have revealed a significant influx of anthropogenic aerosol from South Asia to the Himalayas and Tibetan Plateau (TP during pre-monsoon period. In order to characterize the chemical composition, sources, and transport processes of aerosol in this area, we carried out a field study during June 2015 by deploying a suite of online instruments including an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-AMS and a multi-angle absorption photometer (MAAP at Nam Co station (90°57′ E, 30°46′ N; 4730 m a.s.l. at the central of the TP. The measurements were made at a period when the transition from pre-monsoon to monsoon occurred. The average ambient mass concentration of submicron particulate matter (PM1 over the whole campaign was  ∼  2.0 µg m−3, with organics accounting for 68 %, followed by sulfate (15 %, black carbon (8 %, ammonium (7 %, and nitrate (2 %. Relatively higher aerosol mass concentration episodes were observed during the pre-monsoon period, whereas persistently low aerosol concentrations were observed during the monsoon period. However, the chemical composition of aerosol during the higher aerosol concentration episodes in the pre-monsoon season was on a case-by-case basis, depending on the prevailing meteorological conditions and air mass transport routes. Most of the chemical species exhibited significant diurnal variations with higher values occurring during afternoon and lower values during early morning, whereas nitrate peaked during early morning in association with higher relative humidity and lower air temperature. Organic aerosol (OA, with an oxygen-to-carbon ratio (O ∕ C of 0.94, was more oxidized during the pre-monsoon period than during monsoon (average O ∕ C ratio of 0.72, and an average O ∕ C was 0.88 over the entire campaign period, suggesting overall highly oxygenated aerosol in the central TP. Positive matrix factorization of the

Laboratory Experiments and Instrument Intercomparison Studies of Carbonaceous Aerosol Particles

Energy Technology Data Exchange (ETDEWEB)

Davidovits, Paul [Boston College, Chestnut Hill, MA (United States)

2015-10-20

Aerosols containing black carbon (and some specific types of organic particulate matter) directly absorb incoming light, heating the atmosphere. In addition, all aerosol particles backscatter solar light, leading to a net-cooling effect. Indirect effects involve hydrophilic aerosols, which serve as cloud condensation nuclei (CCN) that affect cloud cover and cloud stability, impacting both atmospheric radiation balance and precipitation patterns. At night, all clouds produce local warming, but overall clouds exert a net-cooling effect on the Earth. The effect of aerosol radiative forcing on climate may be as large as that of the greenhouse gases, but predominantly opposite in sign and much more uncertain. The uncertainties in the representation of aerosol interactions in climate models makes it problematic to use model projections to guide energy policy. The objective of our program is to reduce the uncertainties in the aerosol radiative forcing in the two areas highlighted in the ASR Science and Program Plan. That is, (1) addressing the direct effect by correlating particle chemistry and morphology with particle optical properties (i.e. absorption, scattering, extinction), and (2) addressing the indirect effect by correlating particle hygroscopicity and CCN activity with particle size, chemistry, and morphology. In this connection we are systematically studying particle formation, oxidation, and the effects of particle coating. The work is specifically focused on carbonaceous particles where the uncertainties in the climate relevant properties are the highest. The ongoing work consists of laboratory experiments and related instrument inter-comparison studies both coordinated with field and modeling studies, with the aim of providing reliable data to represent aerosol processes in climate models. The work is performed in the aerosol laboratory at Boston College. At the center of our laboratory setup are two main sources for the production of aerosol particles: (a

Evidence for a significant proportion of Secondary Organic Aerosol from isoprene above a maritime tropical forest

Directory of Open Access Journals (Sweden)

N. H. Robinson

2011-02-01

Full Text Available Isoprene is the most abundant non-methane biogenic volatile organic compound (BVOC, but the processes governing secondary organic aerosol (SOA formation from isoprene oxidation are only beginning to become understood and selective quantification of the atmospheric particulate burden remains difficult. Organic aerosol above a tropical rainforest located in Danum Valley, Borneo, Malaysia, a high isoprene emission region, was studied during Summer 2008 using Aerosol Mass Spectrometry and offline detailed characterisation using comprehensive two dimensional gas chromatography. Observations indicate that a substantial fraction (up to 15% by mass of atmospheric sub-micron organic aerosol was observed as methylfuran (MF after thermal desorption. This observation was associated with the simultaneous measurements of established gas-phase isoprene oxidation products methylvinylketone (MVK and methacrolein (MACR. Observations of MF were also made during experimental chamber oxidation of isoprene. Positive matrix factorisation of the AMS organic mass spectral time series produced a robust factor which accounts for an average of 23% (0.18 μg m⁻³, reaching as much as 53% (0.50 μg m⁻³ of the total oraganic loading, identified by (and highly correlated with a strong MF signal. Assuming that this factor is generally representative of isoprene SOA, isoprene derived aerosol plays a significant role in the region. Comparisons with measurements from other studies suggest this type of isoprene SOA plays a role in other isoprene dominated environments, albeit with varying significance.

BVOC-aerosol-climate interactions in the global aerosol-climate model ECHAM5.5-HAM2

Directory of Open Access Journals (Sweden)

R. Makkonen

2012-11-01

Full Text Available The biosphere emits volatile organic compounds (BVOCs which, after oxidation in the atmosphere, can partition on the existing aerosol population or even form new particles. The large quantities emitted provide means for a large potential impact on both aerosol direct and indirect effects. Biogenic responses to atmospheric temperature change can establish feedbacks even in rather short timescales. However, due to the complexity of organic aerosol partitioning, even the sign of these feedbacks is of large uncertainty. We use the global aerosol-climate model ECHAM5.5-HAM2 to explore the effect of BVOC emissions on new particle formation, clouds and climate. Two BVOC emission models, MEGAN2 and LPJ-GUESS, are used. MEGAN2 shows a 25% increase while LPJ-GUESS shows a slight decrease in global BVOC emission between years 2000 and 2100. The change of shortwave cloud forcing from year 1750 to 2000 ranges from −1.4 to −1.8 W m⁻² with 5 different nucleation mechanisms. We show that the change in shortwave cloud forcing from the year 2000 to 2100 ranges from 1.0 to 1.5 W m⁻². Although increasing future BVOC emissions provide 3–5% additional CCN, the effect on the cloud albedo change is modest. Due to simulated decreases in future cloud cover, the increased CCN concentrations from BVOCs can not provide significant additional cooling in the future.

Sensitivity of aerosol loading and properties to cloudiness

Science.gov (United States)

Iversen, T.; Seland, O.; Kirkevag, A.; Kristjansson, J. E.

2005-12-01

Clouds influence aerosols in various ways. Sulfate is swiftly produced in liquid phase provided there is both sulfur dioxide and oxidants available. Nucleation and Aitken mode aerosol particles efficiently grow in size by collision and coagulation with cloud droplets. When precipitation is formed, aerosol and precursor gases may be quickly removed bay rainout. The dynamics associated with clouds in some cases may swiftly mix aerosols deeply into the troposphere. In some cases Aitken-mode particles may be formed in cloud droplets by splitting agglomerates of particulate matter such as black carbon In this presentation we will discuss how global cloudiness may influence the burden, residence time, and spatial distribution of sulfate, black carbon and particulate organic matter. A similar physico-chemical scheme for there compounds has been implemented in three generations of the NCAR community climate model (CCM3, CAM2 and CAM3). The scheme is documented in the literature and is a part of the Aerocom-intercomparison. There are many differences between these models. With respect to aerosols, a major difference is that CAM3 has a considerably higher global cloud volume and more then twice the amount of cloud water than CAM2 and CCM3. Atmospheric simulations have been made with prescribed ocean temperatures. It is slightly surprising to discover that certain aspects of the aerosols are not particularly sensitive to these differences in cloud availability. This sensitivity will be compared to sensitivities with respect to processing in deep convective clouds.

The uptake of HO2 radicals to organic aerosols

Science.gov (United States)

Matthews, Pascale; Krapf, Manuel; Dommen, Josef; George, Ingrid; Whalley, Lisa; Ingham, Trevor; Baeza-Romero, Maria Teresa; Ammann, Markus; Heard, Dwayne

2014-05-01

HOx (OH + HO2) radicals are responsible for the majority of the oxidation in the troposphere and control the concentrations of many trace species in the atmosphere. There have been many field studies where the measured HO2 concentrations have been smaller than the concentration predicted by model calculations [1,2]. The difference has often been attributed to HO2 uptake by aerosols. Organics are a major component of aerosols accounting for 10 - 70 % of their mass [3]. However, there have been very few laboratory studies measuring HO2 uptake onto organic aerosols [4]. Uptake coefficients (γ) were measured for a range of aerosols using a Fluorescence Assay By Gas Expansion (FAGE) detector combined with an aerosol flow tube. HO2 was injected into the flow tube using a moveable injector which allowed first order HO2 decays to be measured along the flow tube both with and without aerosols. Laboratory generated aerosols were made using an atomiser or by homogeneous nucleation. Secondary organic aerosols (SOA) were made using the Paul Scherrer Institute smog chamber and also by means of a Potential Aerosol Mass (PAM) chamber. The total aerosol surface area was then measured using a Scanning Mobility Particle Sizer (SMPS). Experiments were carried out on aerosols containing glutaric acid, glyoxal, malonic acid, stearic acid, oleic acid and squalene. The HO2 uptake coefficients for these species were measured in the range of γ contained elevated levels of transition metal ions. For humic acid the uptake coefficient was highly dependent on humidity and this may be explained by the liquid water content of the aerosols. Measurements were also performed on copper doped aerosols containing different organics. An uptake coefficient of 0.23 ± 0.07 was measured for copper doped ammonium sulphate, however, this was reduced to 0.008 ± 0.009 when EDTA was added in a 1:1 ratio with copper and 0.003 ± 0.004 when oxalic acid was added in a 10:1 ratio with copper. SOA aerosols were

A novel hybrid tobacco product that delivers a tobacco flavour note with vapour aerosol (Part 2): In vitro biological assessment and comparison with different tobacco-heating products.

Science.gov (United States)

Breheny, Damien; Adamson, Jason; Azzopardi, David; Baxter, Andrew; Bishop, Emma; Carr, Tony; Crooks, Ian; Hewitt, Katherine; Jaunky, Tomasz; Larard, Sophie; Lowe, Frazer; Oke, Oluwatobiloba; Taylor, Mark; Santopietro, Simone; Thorne, David; Zainuddin, Benjamin; Gaça, Marianna; Liu, Chuan; Murphy, James; Proctor, Christopher

2017-08-01

This study assessed the toxicological and biological responses of aerosols from a novel hybrid tobacco product. Toxicological responses from the hybrid tobacco product were compared to those from a commercially available Tobacco Heating Product (c-THP), a prototype THP (p-THP) and a 3R4F reference cigarette, using in vitro test methods which were outlined as part of a framework to substantiate the risk reduction potential of novel tobacco and nicotine products. Exposure matrices used included total particulate matter (TPM), whole aerosol (WA), and aqueous aerosol extracts (AqE) obtained after machine-puffing the test products under the Health Canada Intense smoking regime. Levels of carbonyls and nicotine in these matrices were measured to understand the aerosol dosimetry of the products. The hybrid tobacco product tested negative across the in vitro assays including mutagenicity, genotoxicity, cytotoxicity, tumour promotion, oxidative stress and endothelial dysfunction. All the THPs tested demonstrated significantly reduced responses in these in vitro assays when compared to 3R4F. The findings suggest these products have the potential for reduced health risks. Further pre-clinical and clinical assessments are required to substantiate the risk reduction of these novel products at individual and population levels. Copyright © 2017 The Authors. Published by Elsevier Ltd.. All rights reserved.

LMFBR aerosol release and transport program. Quarterly progress report, July-September 1981

International Nuclear Information System (INIS)

Kress, T.S.; Tobias, M.L.

1982-01-01

This report summarizes progress for the Aerosol Release and Transport Program sponsored by the Office of Nuclear Regulatory Research, Division of Accident Evaluation of the Nuclear Regulatory Commission for the period July-September 1981. Topics discussed include (1) preparations for under-sodium tests at the Fast Aerosol Simulant Test Facility, (2) progress in interpretation of Oak Ridge National Laboratory-Sandia Laboratory normalization test results, (3) U 3 O 8 in steam (light-water reactor accident) aerosol experiments conducted in the Nuclear Safety Power Plant, (4) experiments on B 2 O 3 and SiO 2 aerosols at the Containment Research Installation-II Facility, (5) fuel-melting tests in small-scale experimental facilities for the core-melt aerosol program, (6) analytical comparison of simple adiabatic nonlinear and linear analytical models of bubble oscillation phenomena with experimental data

Sources and Characterization of Submicron Aerosols in a Rural Forest During the PROPHET-AMOS 2016 Campaign

Science.gov (United States)

Bui, A. T.; Wallace, H. W., IV; Alvarez, S. L.; Erickson, M.; Alwe, H. D.; May, N.; Cook, R.; Connor, M.; Slade, J. H., Jr.; Shi, Q.; Kavassalis, S.; Tyndall, G. S.; Shepson, P. B.; Pratt, K.; Ault, A. P.; Millet, D. B.; Murphy, J. G.; Usenko, S.; Sheesley, R. J.; Flynn, J. H., III; Griffin, R. J.; Wang, W.

2017-12-01

Forests are a rich source of biogenic volatile organic compounds (BVOCs). Oxidation of BVOCs can result in the formation of secondary organic aerosol (SOA) and in the presence of NOx (NO+NO2) produce organic nitrate-containing particles. However, the distribution of both BVOCs and oxidants can be dramatically altered by the physical barriers provided by a forest canopy. Global models currently neglect the effect of these canopies on SOA formation in forested regions. In this work, we characterize non-refractory submicron aerosol (NR-PM1) using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) during the 2016 Program on Oxidants: Photochemistry, Emissions, and Transport-Atmospheric Measurements of Oxidants in Summer (PROPHET-AMOS) campaign. This site is located in a rural forest in northern Michigan and features a tower that allowed for both above and below canopy measurements. Our results indicate that organic aerosols (OA) account for a substantial portion of the NR-PM1 measured at this site. Organic nitrate aerosol can contribute up to 18% of the total OA and an average of 75% of the total measured nitrate aerosol. Episodes of above- and below-canopy NR-PM1 concentration differences indicate that above-canopy OA concentrations can be up to 40% greater than below-canopy, which represents an increase of up to 1.5 µg/m3. Organic fragment ions such as CxHy, CxHyOz, and CxHyO1 contribute to enhanced above-canopy OA concentrations. Positive matrix factorization analysis of the high-resolution OA mass spectra identified three SOA factors: low volatility oxygenated OA (LVOOA), isoprene-derived OOA (ISOOA), and oxygenated organic aerosol. Analysis of air mass backward trajectories and correlations with external data indicate that LVOOA correlates well with sulfate and aged, urban-influenced air masses, whereas ISOOA correlates well with isoprene SOA tracers and air masses originating from semi-remote areas. Our results indicate that the OA at this

Photodegradation of secondary organic aerosol generated from limonene oxidation by ozone studied with chemical ionization mass spectrometry

Directory of Open Access Journals (Sweden)

X. Pan

2009-06-01

Full Text Available Photodegradation of secondary organic aerosol (SOA prepared by ozone-initiated oxidation of D-limonene is studied with an action spectroscopy approach, which relies on detection of volatile photoproducts with chemical ionization mass-spectrometry as a function of the UV irradiation wavelength. Efficient photodegradation is observed for a broad range of ozone (0.1–300 ppm and D-limonene (0.02–3 ppm concentrations used in the preparation of SOA. The observed photoproducts are dominated by oxygenated C1-C3 compounds such as methanol, formic acid, acetaldehyde, acetic acid, and acetone. The irradiation wavelength dependence of the combined yield of the photoproducts closely tracks the absorption spectrum of the SOA material suggesting that photodegradation is not limited to the UV wavelengths. Kinetic simulations suggest that RO₂+HO₂/RO₂ reactions represent the dominant route to photochemically active carbonyl and peroxide species in the limonene SOA prepared in these experiments. Similar photodegradation processes are likely to occur in realistic SOA produced by OH- or O₃-initiated oxidation of biogenic volatile organic compounds in clean air.

Multi-sensor cloud and aerosol retrieval simulator and remote sensing from model parameters - Part 2: Aerosols

Science.gov (United States)

Wind, Galina; da Silva, Arlindo M.; Norris, Peter M.; Platnick, Steven; Mattoo, Shana; Levy, Robert C.

2016-07-01

The Multi-sensor Cloud Retrieval Simulator (MCRS) produces a "simulated radiance" product from any high-resolution general circulation model with interactive aerosol as if a specific sensor such as the Moderate Resolution Imaging Spectroradiometer (MODIS) were viewing a combination of the atmospheric column and land-ocean surface at a specific location. Previously the MCRS code only included contributions from atmosphere and clouds in its radiance calculations and did not incorporate properties of aerosols. In this paper we added a new aerosol properties module to the MCRS code that allows users to insert a mixture of up to 15 different aerosol species in any of 36 vertical layers.This new MCRS code is now known as MCARS (Multi-sensor Cloud and Aerosol Retrieval Simulator). Inclusion of an aerosol module into MCARS not only allows for extensive, tightly controlled testing of various aspects of satellite operational cloud and aerosol properties retrieval algorithms, but also provides a platform for comparing cloud and aerosol models against satellite measurements. This kind of two-way platform can improve the efficacy of model parameterizations of measured satellite radiances, allowing the assessment of model skill consistently with the retrieval algorithm. The MCARS code provides dynamic controls for appearance of cloud and aerosol layers. Thereby detailed quantitative studies of the impacts of various atmospheric components can be controlled.In this paper we illustrate the operation of MCARS by deriving simulated radiances from various data field output by the Goddard Earth Observing System version 5 (GEOS-5) model. The model aerosol fields are prepared for translation to simulated radiance using the same model subgrid variability parameterizations as are used for cloud and atmospheric properties profiles, namely the ICA technique. After MCARS computes modeled sensor radiances equivalent to their observed counterparts, these radiances are presented as input to

Multi-Sensor Cloud and Aerosol Retrieval Simulator and Remote Sensing from Model Parameters . Part 2; Aerosols

Science.gov (United States)

Wind, Galina; Da Silva, Arlindo M.; Norris, Peter M.; Platnick, Steven; Mattoo, Shana; Levy, Robert C.

2016-01-01

The Multi-sensor Cloud Retrieval Simulator (MCRS) produces a simulated radiance product from any high-resolution general circulation model with interactive aerosol as if a specific sensor such as the Moderate Resolution Imaging Spectroradiometer (MODIS) were viewing a combination of the atmospheric column and land ocean surface at a specific location. Previously the MCRS code only included contributions from atmosphere and clouds in its radiance calculations and did not incorporate properties of aerosols. In this paper we added a new aerosol properties module to the MCRS code that allows users to insert a mixture of up to 15 different aerosol species in any of 36 vertical layers. This new MCRS code is now known as MCARS (Multi-sensor Cloud and Aerosol Retrieval Simulator). Inclusion of an aerosol module into MCARS not only allows for extensive, tightly controlled testing of various aspects of satellite operational cloud and aerosol properties retrieval algorithms, but also provides a platform for comparing cloud and aerosol models against satellite measurements. This kind of two-way platform can improve the efficacy of model parameterizations of measured satellite radiances, allowing the assessment of model skill consistently with the retrieval algorithm. The MCARS code provides dynamic controls for appearance of cloud and aerosol layers. Thereby detailed quantitative studies of the impacts of various atmospheric components can be controlled. In this paper we illustrate the operation of MCARS by deriving simulated radiances from various data field output by the Goddard Earth Observing System version 5 (GEOS-5) model. The model aerosol fields are prepared for translation to simulated radiance using the same model sub grid variability parameterizations as are used for cloud and atmospheric properties profiles, namely the ICA technique. After MCARS computes modeled sensor radiances equivalent to their observed counterparts, these radiances are presented as input to

Mixed phase Pt-Ru catalyst for direct methanol fuel cell anode by flame aerosol synthesis

DEFF Research Database (Denmark)

Chakraborty, Debasish; Bischoff, H.; Chorkendorff, Ib

2005-01-01

A spray-flame aerosol catalyzation technique was studied for producing Pt-Ru anode electrodes for the direct methanol fuel cell. Catalysts were produced as aerosol nanoparticles in a spray-flame reactor and deposited directly as a thin layer on the gas diffusion layer. The as-prepared catalyst wa......Ru1/Vulcan carbon. The kinetics of methanol oxidation on the mixed phase catalyst was also explored by electrochemical impedance spectroscopy. (c) 2005 The Electrochemical Society.......A spray-flame aerosol catalyzation technique was studied for producing Pt-Ru anode electrodes for the direct methanol fuel cell. Catalysts were produced as aerosol nanoparticles in a spray-flame reactor and deposited directly as a thin layer on the gas diffusion layer. The as-prepared catalyst...... was found to be a mixture of nanocrystalline, mostly unalloyed Pt and an amorphous phase mostly of Ru and to a lesser extent of Pt oxides on top of the crystalline phase. The flame-produced Pt1Ru1 demonstrated similar onset potential but similar to 60% higher activity compared to commercially available Pt1...

Whole-body nanoparticle aerosol inhalation exposures.

Science.gov (United States)

Yi, Jinghai; Chen, Bean T; Schwegler-Berry, Diane; Frazer, Dave; Castranova, Vince; McBride, Carroll; Knuckles, Travis L; Stapleton, Phoebe A; Minarchick, Valerie C; Nurkiewicz, Timothy R

2013-05-07

Inhalation is the most likely exposure route for individuals working with aerosolizable engineered nano-materials (ENM). To properly perform nanoparticle inhalation toxicology studies, the aerosols in a chamber housing the experimental animals must have: 1) a steady concentration maintained at a desired level for the entire exposure period; 2) a homogenous composition free of contaminants; and 3) a stable size distribution with a geometric mean diameter generation of aerosols containing nanoparticles is quite challenging because nanoparticles easily agglomerate. This is largely due to very strong inter-particle forces and the formation of large fractal structures in tens or hundreds of microns in size (6), which are difficult to be broken up. Several common aerosol generators, including nebulizers, fluidized beds, Venturi aspirators and the Wright dust feed, were tested; however, none were able to produce nanoparticle aerosols which satisfy all criteria (5). A whole-body nanoparticle aerosol inhalation exposure system was fabricated, validated and utilized for nano-TiO2 inhalation toxicology studies. Critical components: 1) novel nano-TiO2 aerosol generator; 2) 0.5 m(3) whole-body inhalation exposure chamber; and 3) monitor and control system. Nano-TiO2 aerosols generated from bulk dry nano-TiO2 powders (primary diameter of 21 nm, bulk density of 3.8 g/cm(3)) were delivered into the exposure chamber at a flow rate of 90 LPM (10.8 air changes/hr). Particle size distribution and mass concentration profiles were measured continuously with a scanning mobility particle sizer (SMPS), and an electric low pressure impactor (ELPI). The aerosol mass concentration (C) was verified gravimetrically (mg/m(3)). The mass (M) of the collected particles was determined as M = (Mpost-Mpre), where Mpre and Mpost are masses of the filter before and after sampling (mg). The mass concentration was calculated as C = M/(Q*t), where Q is sampling flowrate (m(3)/min), and t is the sampling

78 FR 6400 - Results of FAA Nitrous Oxide BLEVE Characterization Testing

Science.gov (United States)

2013-01-30

... DEPARTMENT OF TRANSPORTATION Federal Aviation Administration Results of FAA Nitrous Oxide BLEVE Characterization Testing AGENCY: Federal Aviation Administration (FAA), DOT. ACTION: Notice of public... FAA sponsored testing of nitrous oxide (N 2 O) characteristics. Nitrous oxide is an important oxidizer...

PIXE application to the study of atmospheric aerosol

International Nuclear Information System (INIS)

Zhu Guanghua

1998-11-01

In order to confirm the measurement accuracy of PIXE (Particle Induced X-ray Emission), cross-check test were carried out between three laboratories. Thirty single element samples and one plural elements sample were used in the test. The agreements between three laboratories were evaluated to be better than 10% for the most of tested samples. The reproducibility test showed very good agreement and the dispersion in three times repeated PIXE measurements was within 6% on average. Using an automatic time sequence step sampler in Beijing collected atmospheric aerosol samples. Element concentrations were analyzed by PIXE technique. Then the data were analyzed by the absolute principal factor analysis (APFA) to evaluate the principal components and the percent variance explained by them. As a result, it shows that the PIXE analysis combed with statistical method can effectively resolve the aerosol components in urban area and distinguish between local and remote area aerosol components. The atmospheric aerosol samples were collected at four representative sites with an 8-stage cascade impactor sampler and analyzed for their elemental mass concentrations by PIXE analytic method. Based on some indicator elements, the characteristics of size distributions of particles from different sources were obtained

Unspeciated organic emissions from combustion sources and their influence on the secondary organic aerosol budget in the United States

Science.gov (United States)

Secondary organic aerosol (SOA) formed from the atmospheric oxidation of nonmethane organic gases (NMOG) is a major contributor to atmospheric aerosol mass. Emissions and smog chamber experiments were performed to investigate SOA formation from gasoline vehicles, diesel vehicles,...

Using the OMI aerosol index and absorption aerosol optical depth to evaluate the NASA MERRA Aerosol Reanalysis

Science.gov (United States)

Buchard, V.; da Silva, A. M.; Colarco, P. R.; Darmenov, A.; Randles, C. A.; Govindaraju, R.; Torres, O.; Campbell, J.; Spurr, R.

2015-05-01

A radiative transfer interface has been developed to simulate the UV aerosol index (AI) from the NASA Goddard Earth Observing System version 5 (GEOS-5) aerosol assimilated fields. The purpose of this work is to use the AI and aerosol absorption optical depth (AAOD) derived from the Ozone Monitoring Instrument (OMI) measurements as independent validation for the Modern Era Retrospective analysis for Research and Applications Aerosol Reanalysis (MERRAero). MERRAero is based on a version of the GEOS-5 model that is radiatively coupled to the Goddard Chemistry, Aerosol, Radiation, and Transport (GOCART) aerosol module and includes assimilation of aerosol optical depth (AOD) from the Moderate Resolution Imaging Spectroradiometer (MODIS) sensor. Since AI is dependent on aerosol concentration, optical properties and altitude of the aerosol layer, we make use of complementary observations to fully diagnose the model, including AOD from the Multi-angle Imaging SpectroRadiometer (MISR), aerosol retrievals from the AErosol RObotic NETwork (AERONET) and attenuated backscatter coefficients from the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) mission to ascertain potential misplacement of plume height by the model. By sampling dust, biomass burning and pollution events in 2007 we have compared model-produced AI and AAOD with the corresponding OMI products, identifying regions where the model representation of absorbing aerosols was deficient. As a result of this study over the Saharan dust region, we have obtained a new set of dust aerosol optical properties that retains consistency with the MODIS AOD data that were assimilated, while resulting in better agreement with aerosol absorption measurements from OMI. The analysis conducted over the southern African and South American biomass burning regions indicates that revising the spectrally dependent aerosol absorption properties in the near-UV region improves the modeled-observed AI comparisons

Landscape fires dominate terrestrial natural aerosol - climate feedbacks

Science.gov (United States)

Scott, C.; Arnold, S.; Monks, S. A.; Asmi, A.; Paasonen, P.; Spracklen, D. V.

2017-12-01

The terrestrial biosphere is an important source of natural aerosol including landscape fire emissions and secondary organic aerosol (SOA) formed from biogenic volatile organic compounds (BVOCs). Atmospheric aerosol alters the Earth's climate by absorbing and scattering radiation (direct radiative effect; DRE) and by perturbing the properties of clouds (aerosol indirect effect; AIE). Natural aerosol sources are strongly controlled by, and can influence, climate; giving rise to potential natural aerosol-climate feedbacks. Earth System Models (ESMs) include a description of some of these natural aerosol-climate feedbacks, predicting substantial changes in natural aerosol over the coming century with associated radiative perturbations. Despite this, the sensitivity of natural aerosols simulated by ESMs to changes in climate or emissions has not been robustly tested against observations. Here we combine long-term observations of aerosol number and a global aerosol microphysics model to assess terrestrial natural aerosol-climate feedbacks. We find a strong positive relationship between the summertime anomaly in observed concentration of particles greater than 100 nm diameter and the anomaly in local air temperature. This relationship is reproduced by the model and driven by variability in dynamics and meteorology, as well as natural sources of aerosol. We use an offline radiative transfer model to determine radiative effects due to changes in two natural aerosol sources: landscape fire and biogenic SOA. We find that interannual variability in the simulated global natural aerosol radiative effect (RE) is negatively related to the global temperature anomaly. The magnitude of global aerosol-climate feedback (sum of DRE and AIE) is estimated to be -0.15 Wm-2 K-1 for landscape fire aerosol and -0.06 Wm-2 K-1 for biogenic SOA. These feedbacks are comparable in magnitude, but opposite in sign to the snow albedo feedback, highlighting the need for natural aerosol feedbacks to