Sample records for tetraphenylborate catalyst development

  1. (Butoxymethylidenedimethylazanium tetraphenylborate acetonitrile monosolvate

    Directory of Open Access Journals (Sweden)

    Ioannis Tiritiris


    Full Text Available In the title solvated salt, C7H16NO+·C24H20B−·C2H3N, the C—N bond lengths in the cation are 1.2831 (19, 1.467 (2 and 1.465 (2 Å, indicating double- and single-bond character, respectively. The C—O bond length of 1.2950 (18 Å shows a double-bond character, pointing towards charge delocalization within the NCO plane of the iminium ion. The two C atoms of the n-butyl group are disordered over the two sites, with refined occupancy ratios of 0.890 (5:0.110 (5 and 0.888 (4:0.112 (4. In the crystal, C—H...π interactions occur between the methine H atom, H atoms of the –N(CH32 and –CH2 groups of the cation, and two of the phenyl rings of the tetraphenylborate anion. The latter interaction forms an aromatic pocket in which the cation is embedded. Thus, a two-dimensional pattern is created in the ac plane.

  2. Development of GREET Catalyst Module

    Energy Technology Data Exchange (ETDEWEB)

    Wang, Zhichao [Argonne National Lab. (ANL), Argonne, IL (United States); Benavides, Pahola T. [Argonne National Lab. (ANL), Argonne, IL (United States); Dunn, Jennifer B. [Argonne National Lab. (ANL), Argonne, IL (United States); Cronauer, Donald C. [Argonne National Lab. (ANL), Argonne, IL (United States)


    In this report, we develop energy and material flows for the production of five different catalysts (tar reforming, alcohol synthesis, Zeolite Socony Mobil-5 [ZSM-5], Mo/Co/ γ-Al2O3, and Pt/ γ-Al2O3) and two chemicals (olivine, dimethyl ether of polyethylene glycol [DEPG]). These compounds and catalysts are now included in the Greenhouse Gases, Regulated Emissions and Energy Use in Transportation (GREET™) catalyst module.

  3. Development of GREET Catalyst Module

    Energy Technology Data Exchange (ETDEWEB)

    Wang, Zhichao [Argonne National Lab. (ANL), Argonne, IL (United States). Energy Systems Division; Dunn, Jennifer B. [Argonne National Lab. (ANL), Argonne, IL (United States). Energy Systems Division; Cronauer, Donald C. [Argonne National Lab. (ANL), Argonne, IL (United States). Energy Systems Division


    Catalysts are critical inputs for many pathways that convert biomass into biofuels. Energy consumption and greenhouse gas (GHG) emissions during the production of catalysts and chemical inputs influence the life-cycle energy consumption, and GHG emissions of biofuels and need to be considered in biofuel life-cycle analysis (LCA). In this report, we develop energy and material flows for the production of three different catalysts (tar reforming, alcohol synthesis, Zeolite Socony Mobil-5 [ZSM-5]) and two chemicals (olivine, dimethyl ether of polyethylene glycol [DEPG]). These compounds and catalysts are now included in the Greenhouse Gases, Regulated Emissions and Energy Use in Transportation (GREET™) catalyst module. They were selected because they are consumed in existing U.S. Department of Energy (DOE) analyses of biofuel processes. For example, a thermochemical ethanol production pathway (indirect gasification and mixed alcohol synthesis) developed by the National Renewable Energy Laboratory (NREL) uses olivine, DEPG, and tar reforming and alcohol synthesis catalysts (Dutta et al., 2011). ZSM-5 can be used in biofuel production pathways such as catalytic upgrading of sugars into hydrocarbons (Biddy and Jones, 2013). Other uses for these compounds and catalysts are certainly possible. In this report, we document the data sources and methodology we used to develop material and energy flows for the catalysts and compounds in the GREET catalyst module. In Section 2 we focus on compounds used in the model Dutta et al. (2011) developed. In Section 3, we report material and energy flows associated with ZSM-5 production. Finally, in Section 4, we report results.


    Energy Technology Data Exchange (ETDEWEB)

    Adu-Wusu, K; Daniel McCabe, D; Bill Wilmarth, B


    A bench-scale feasibility study on the use of a Wet Air Oxidation (WAO) process to destroy a slurry laden with tetraphenylborate (TPB) compounds has been undertaken. WAO is an aqueous phase process in which soluble and/or insoluble waste constituents are oxidized using oxygen or oxygen in air at elevated temperatures and pressures ranging from 150 C and 1 MPa to 320 C and 22 MPa. The products of the reaction are CO{sub 2}, H{sub 2}O, and low molecular weight oxygenated organics (e.g. acetate, oxalate). Test results indicate WAO is a feasible process for destroying TPB, its primary daughter products [triphenylborane (3PB), diphenylborinic acid (2PB), and phenylboronic acid (1PB)], phenol, and most of the biphenyl byproduct. The required conditions are a temperature of 300 C, a reaction time of 3 hours, 1:1 feed slurry dilution with 2M NaOH solution, the addition of CuSO{sub 4}.5H{sub 2}O solution (500 mg/L Cu) as catalyst, and the addition of 2000 mL/L of antifoam. However, for the destruction of TPB, its daughter compounds (3PB, 2PB, and 1PB), and phenol without consideration for biphenyl destruction, less severe conditions (280 C and 1-hour reaction time with similar remaining above conditions) are adequate.

  5. Fuel cell development for transportation: Catalyst development

    Energy Technology Data Exchange (ETDEWEB)

    Doddapaneni, N. [Sandia National Lab., Albuquerque, NM (United States)


    Fuel cells are being considered as alternate power sources for transportation and stationary applications. With proton exchange membrane (PEM) fuel cells the fuel crossover to cathodes causes severe thermal management and cell voltage drop due to oxidation of fuel at the platinized cathodes. The main goal of this project was to design, synthesize, and evaluate stable and inexpensive transition metal macrocyclic catalysts for the reduction of oxygen and be electrochemically inert towards anode fuels such as hydrogen and methanol.

  6. Advanced Aqueous Phase Catalyst Development using Combinatorial Methods Project (United States)

    National Aeronautics and Space Administration — The use of combinatorial methods is proposed to rapidly screen catalyst formulations for the advanced development of aqueous phase oxidation catalysts with greater...

  7. Advanced Aqueous Phase Catalyst Development using Combinatorial Methods Project (United States)

    National Aeronautics and Space Administration — Combinatorial methods are proposed to develop advanced Aqueous Oxidation Catalysts (AOCs) with the capability to mineralize organic contaminants present in effluents...

  8. Demonstration of Small Tank Tetraphenylborate Precipitation Process Using Savannah River Site High Level Waste

    Energy Technology Data Exchange (ETDEWEB)

    Peters, T.B.


    This report details the experimental effort to demonstrate the continuous precipitation of cesium from Savannah River Site High Level Waste using sodium tetraphenylborate. In addition, the experiments examined the removal of strontium and various actinides through addition of monosodium titanate.


    Energy Technology Data Exchange (ETDEWEB)

    Davis, B.H.


    The goal of the proposed work described in this Final Report was the development of iron-based Fischer-Tropsch catalysts that combined high activity, selectivity and life with physical robustness for slurry phase reactors that will produce either low-alpha or high-alpha products. The work described here has optimized the catalyst composition and pretreatment operation for a low-alpha catalyst. In parallel, work has been conducted to design a high-alpha iron catalyst that is suitable for slurry phase synthesis. Studies have been conducted to define the chemical phases present at various stages of the pretreatment and synthesis stages and to define the course of these changes. The oxidation/reduction cycles that are anticipated to occur in large, commercial reactors have been studied at the laboratory scale. Catalyst performance has been determined for catalysts synthesized in this program for activity, selectivity and aging characteristics.

  10. Dates in the development of catalysts

    Energy Technology Data Exchange (ETDEWEB)



    A chronological listing is presented of the dates on which various I. G. Farbenindustrie catalysts were first used. In most cases the entries gave compositions and some hints at the methods of preparation of the catalysts as well as the code numbers for the catalysts. The listing started in December, 1924, and extended throught August, 1941. Some of the more important catalysts were the following: 5058, tungsten disulfide (WS/sub 2/), produced from the thio salt by dry decomposition (1930); 6434, a diluted mixture of hydrogen fluoride-treated ''Terrana'' and 10% WS/sub 2/ (1935); 6719, a prehydrogenation catalyst of 75 parts ferrous sulfide (FeS), 22 parts WS/sub 2/, and 3 parts nickel monosulfide (NiS) (1937); 7019, an aromatization catalyst of 100 parts primry coal, 15 parts chromic oxide (Cr/sub 2/O/sub 3/), and 5 parts vanadium sesquioxide (V/sub 2/O/sub 3/) (1938); 7360, a DHD catalyst of activated alumina (Al/sub 2/O/sub 3/) and 55 g/l molybdenum trioxide (MoO/sub 3/) (1939); 7846, a prehydrogenated catalyst, a sulfonated mixture of activated alumina, 100 g/l MoO/sub 3/, and 30 g/l nickel sesquioxide (Ni/sub 2/O/sub 3/) (1940); and 8376 W, a prehydrogenation catalyst, a sulfonated mixture of activated alumina, 250 g/l tungsten trioxide (WO/sub 3/), and 50 g/l Ni/sub 2/O/sub 3/ (1941). Other caalysts given included numbers 1724, 2365, 2473, 2500, 3510, 3884, 5053, 5676, 6525, and 6561. Compounds used other than those mentioned above included molybdenum disulfide (MoS/sub 2/), zinc sulfide (ZnS), zinc oxide (ZnO), and magnesium oxide (MgO).

  11. Technology development for iron Fischer-Tropsch catalysts

    Energy Technology Data Exchange (ETDEWEB)

    O`Brien, R.J.; Raje, A.; Keogh, R.A. [and others


    The objective of this research project is to develop the technology for the production of physically robust iron-based Fischer-Tropsch catalysts that have suitable activity, selectivity and stability to be used in the slurry phase synthesis reactor development. The catalysts that are developed shall be suitable for testing in the Advanced Fuels Development Facility at LaPorte, Texas, to produce either low-or high-alpha product distributions. Previous work by the offeror has produced a catalyst formulation that is 1.5 times as active as the {open_quotes}standard-catalyst{close_quotes} developed by German workers for slurry phase synthesis. In parallel, work will be conducted to design a high-alpha iron catalyst this is suitable for slurry phase synthesis. Studies will be conducted to define the chemical phases present at various stages of the pretreatment and synthesis stages and to define the course of these changes. The oxidation/reduction cycles that are anticipated to occur in large, commercial reactors will be studied at the laboratory scale. Catalyst performance will be determined for catalysts synthesized in this program for activity, selectivity and aging characteristics.

  12. Recent developments on ultrasound assisted catalyst-free organic synthesis. (United States)

    Banerjee, Bubun


    Mother Nature needs to be protected from ever increasing chemical pollutions associated with synthetic organic processes. The fundamental challenge for today's methodologists is to make their protocols more environmentally benign and sustainable by avoiding the extensive use of hazardous reagents and solvents, harsh reaction conditions, and toxic metal catalysts. However, the people of the twenty-first century are well aware about the side effects of those hazardous substances used and generated by the chemical processes. As a result, the last decade has seen a tremendous outburst in modifying chemical processes to make them 'sustainable' for the betterment of our environment. Catalysts play a crucial role in organic synthesis and thus they find huge applications and uses. Scientists' continuously trying to modify the catalysts to reduce their toxicity level, but the most benign way is to design an organic reaction without catalyst(s), if possible. It is worthy to mention that the involvement of ultrasound in organic synthesis is sometimes fulfilling this goal. In many occasions the applications of ultrasound can avoid the use of catalysts in organic reactions. Such beneficial features as a whole have motivated the organic chemists to apply ultrasonic irradiation in more heights and as a results, in recent past, there were immense applications of ultrasound in organic reactions for the synthesis of diverse organic scaffolds under catalyst-free condition. The present review summarizes the latest developments on ultrasound assisted catalyst-free organic synthesis reported so far. Copyright © 2016 Elsevier B.V. All rights reserved.

  13. Investigation and development of heavy oil upgrading catalysts. 3

    Energy Technology Data Exchange (ETDEWEB)

    Lee, D.K.; Lee, I.C.; Yoon, W.L.; Lee, H.T.; Chung, H.; Hwang, Y.J.; Park, S.H. [Korea Inst. of Energy Research, Taejon (Korea, Republic of)


    This study aimed at the domestic development of HDS catalysts which are most fundamental and wide-used in the petroleum refinery. In this year, some experimental works were conducted for developing the effective utilization technology of the novel dispersed-catalysts in the hydro-desulfurization of heavy oils, and improving the reaction performance of alumina-supported Mo-based hydro-treating catalysts conventionally used in most of refineries. First, it was experimentally proved that the dispersed catalysts of Co-Mo could be employed for the hydro-desulfurization of a heavy atmospheric residual oil excluding the catalyst deactivation. The utilization of a carbon-expanded reactor in combination with this dispersed catalyst system exhibited an enhanced reaction performance and provided an efficient way for the separation and recovery of the dispersed catalytic component from oils. Second, the tungsten-incorporated WCoMo/{gamma}-Al{sub 2}O{sub 3} catalyst revealed the improved catalytic performance in the various hydro-treating reactions and in the initial deactivation rates for the high pressure hydro-treatment of a heavy oil as compared with the commercial CoMo/{gamma}-Al{sub 2}O{sub 3} catalyst. This new experimental finding for the promoting role of the monomeric WO{sub 3} species in CoMo/{gamma}-Al{sub 2}O{sub 3} catalyst may be generally applicable to the Mo-based alumina-sulfide phase, higher catalytic activity, and more extended service life. (author). 101 refs., 33 figs., 18 tabs.

  14. Development of radioactive platinum group metal catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Chung, H.S.; Kim, Y.S.; Kim, Y.E. [and others


    The fission product nuclides generated during the irradiation of reactor fuel include many useful elements, among them platinum group metals such as ruthenium, rhodium and palladium which are of great industrial importance, occur rarely in nature and are highly valuable. In this research, the authors reviewed various PGM recovery methods. Recovery of palladium from seven-component simulated waste solutions was conducted by selective precipitation method. The recovery yield was more than 99.5% and the purity of the product was more than 99%. Wet-proof catalyst was prepared with the recovered palladium. The specific surface area of the catalyst support was more than 400m{sup 2}/g.The content of palladium impregnated on the support was 1 to 10 wt. %. Hydrogen isotope exchange efficiency of more than 93% to equilibrium with small amount of the catalyst was obtained. It was turned out possible to consider using such palladium or other very low active PGM materials in applications where its activity is unimportant as in nuclear industries. (author). 86 refs., 44 tabs., 88 figs.

  15. Developing physicians as catalysts for change. (United States)

    George, Aaron E; Frush, Karen; Michener, J Lloyd


    Failures in care coordination are a reflection of larger systemic shortcomings in communication and in physician engagement in shared team leadership. Traditional medical care and medical education neither focus on nor inspire responses to the challenges of coordinating care across episodes and sites. The authors suggest that the absence of attention to gaps in the continuum of care has led physicians to attempt to function as the glue that holds the health care system together. Further, medical students and residents have little opportunity to provide feedback on care processes and rarely receive the training and support they need to assess and suggest possible improvements.The authors argue that this absence of opportunity has driven cynicism, apathy, and burnout among physicians. They support a shift in culture and medical education such that students and residents are trained and inspired to act as catalysts who initiate and expedite positive changes. To become catalyst physicians, trainees require tools to partner with patients, staff, and faculty; training in implementing change; and the perception of this work as inherent to the role of the physician.The authors recommend that medical schools consider interprofessional training to be a necessary component of medical education and that future physicians be encouraged to grow in areas outside the "purely clinical" realm. They conclude that both physician catalysts and teamwork are essential for improving care coordination, reducing apathy and burnout, and supporting optimal patient outcomes.

  16. Technology development for iron Fischer-Tropsch catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Frame, R.R.


    Objectives are to develop active, stable iron Fischer-Tropsch catalysts for use in slurry-phase synthesis reactors and to develop a scaleup procedure for large-scale synthesis of such catalysts for process development and long-term testing in slurry bubble-column reactors. For a H[sub 2]-CO in molar ratio of 0.5 to 1.0, catalyst performance target is 88% CO+H[sub 2] conversion at a minimum space velocity of 2.4 NL/hr/gFe, with no more than 4% methane/ethane selectivity and 1% conversion loss per week. During this period, it was found that the performance of the slurry-phase iron and copper oxide-based catalyst depends on the amount of K. Five catalysts with differing K contents were studied. The catalysts with the lowest K were more active than the ones with higher K levels. The one with the middle K level was judged best.

  17. Water–gas shift catalyst development for energy efficient applications

    NARCIS (Netherlands)

    Hakeem, A.A.


    The water–gas shift (WGS) is a reversible, moderately exothermic reaction (1) and is used for the production of hydrogen from CO rich gas streams (synthesis gas). CO + H2O ? CO2 + H2 ?H°= –41 kJ mol?1 (1) This research has focused on the catalyst development of water–gas shift (WGS) reaction and

  18. Christian Church: A Catalyst for Economic Development in Nigeria ...

    African Journals Online (AJOL)

    Christian Church: A Catalyst for Economic Development in Nigeria. ... African Research Review ... The Nigerian economy had a truncated history from independence to present times and the economy has suffered series of economic instability because of a long period of unsustained growth in the per capital real income of ...


    Energy Technology Data Exchange (ETDEWEB)

    Andrew W. Wang


    The Alternative Fuels Field Test Unit (AFFTU) is a portable laboratory designed specifically to provide on-site evaluation of potential feedstocks for processes that produce alternative fuels from indigenous raw materials such as coal, natural gas or environmentally disadvantaged carbonaceous feedstocks. Since conversion of these raw materials into feed gas streams can produce a variety of bulk gas compositions, which furthermore can contain a myriad of trace components, it is necessary to evaluate each new feedstock on an individual basis. While it is possible to prepare blended gas mixtures to simulate the bulk composition of a known feedstock, it is neither possible nor cost-effective to simulate adequately the variety of trace chemicals present in that feedstock--some of which may not even be detected by routine analysis. Additionally, the transient composition of the gas during upsets or routine process changes may have an impact on the proposed process that is not foreseen in standard design. To address these concerns, the AFFTU was constructed with the following experimental capabilities: (1) A state-of-the-art gas chromatograph system to perform semi-continuous monitoring of both bulk composition and the concentration of key trace poisons down to one part per billion (ppb). (2) A 30-mL reactor system that can accept up to two feed streams from the customer, allowing a true life test with the actual gas projected for use in the proposed facility. (3) A manifold of four adsorbent beds, located upstream of the reactor, which permits the testing of adsorbents for the removal of contaminants from the feed stream. The effectiveness of these adsorbents may be evaluated either by analysis of the gas upstream and downstream of the bed (or at an intermediate point within the bed) or by observing the impact of the presence or absence of that bed on the actual stability of the catalyst activity. To achieve portability, the AFFTU was constructed in a commercial 48-foot

  20. FY 1997 report on the development of excellent catalysts for creation of new industries. New frontier catalyst 21; 1997 nendo chosa hokokusho (shinsangyo sosei no tame no excellence catalyst no kaihatsu). New frontier catalyst 21

    Energy Technology Data Exchange (ETDEWEB)



    Survey was made for establishment of an effective fast search technique of practical catalysts. Catalyst technology is an important basic technology for industrial fields such as energy and environment fields. In many cases, catalysts have been developed by trial and error consuming a long time and huge research cost. Study was made on efficient analysis and measurement techniques, and systematic production technique of advanced catalysts based on these techniques. This survey was effective in finding a guidance for improving catalysts used in the previous processes, and facilitating searches for fields previously slow in development of catalysts. Advanced catalysts possible to actively selectively produce target products under high pressure/temperature conditions are much in demand. Recently in-situ analysis technology for observing molecules and material surfaces under ultrahigh-pressure/temperature conditions has been studied. Observational study was made on catalytic behavior under catalytic reaction condition using partial oxidation, selective hydrogenation and isomerization as model reactions. 111 refs., 103 figs., 9 tabs.

  1. An Overview of Recent Development in Composite Catalysts from Porous Materials for Various Reactions and Processes

    Directory of Open Access Journals (Sweden)

    Zaiku Xie


    Full Text Available Catalysts are important to the chemical industry and environmental remediation due to their effective conversion of one chemical into another. Among them, composite catalysts have attracted continuous attention during the past decades. Nowadays, composite catalysts are being used more and more to meet the practical catalytic performance requirements in the chemical industry of high activity, high selectivity and good stability. In this paper, we reviewed our recent work on development of composite catalysts, mainly focusing on the composite catalysts obtained from porous materials such as zeolites, mesoporous materials, carbon nanotubes (CNT, etc. Six types of porous composite catalysts are discussed, including amorphous oxide modified zeolite composite catalysts, zeolite composites prepared by co-crystallization or overgrowth, hierarchical porous catalysts, host-guest porous composites, inorganic and organic mesoporous composite catalysts, and polymer/CNT composite catalysts.

  2. Preparation and Development of Advanced Battery Catalysts. (United States)


    Institute Advances Defense Metals & Ceramics Rue Georges Leclance Information Center BP 357-86009 Poitiers, France 505 King Avenue Columbus, OH 43201 1...Corporation Attn: D. E. Harney 1 Attn: Dr. J. N. Gleeson 1 Research & Development Center Amoco Research Center 625 East Street P. 0. Box 400 Fairport

  3. Isolation and stable nitrogen isotope analysis of ammonium ions in ammonium nitrate prills using sodium tetraphenylborate. (United States)

    Howa, John D; Lott, Michael J; Ehleringer, James R


    Because of the threat of bombings using improvised explosives containing ammonium nitrate (AN), law enforcement and intelligence communities have been interested in stable isotope techniques for tracking and discriminating AN sources. Separate analysis of the AN component ions ammonium and nitrate would add discriminatory power to these techniques. Ammonium ions in dissolved AN solution were isolated from samples by precipitation using sodium tetraphenylborate solution. We tested the isolation of ammonium from nitrates using solutions of ammonium and nitrate salts with different (15)N/(14)N isotope ratios. Ammonium tetraphenylborate and AN were separately analyzed for their (15)N/(14)N isotope ratios using EA-ConFlo-IRMS, and the (15)N/(14)N isotope ratios of the nitrate ions were calculated using mass balance. Ammonium and nitrate nitrogen isotope ratios were plotted as two separate variables. Isolation of ammonium precipitate from solutions containing dissolved nitrates did not influence the nitrogen isotope ratios of test ammonium salts. A survey set of 42 AN samples showed that the ammonium and nitrate (15)N/(14)N isotope ratios were not significantly correlated, and the paired mean differences were not statistically significant. Both ammonium and nitrate were depleted in (15)N relative to their theoretical atmospheric sources. Isolation of the ammonium ion from AN adds another dimension for the discrimination of forensic AN samples. This technique using sodium tetraphenylborate is robust and does not require specialized equipment. Our observations indicated that ammonium nitrogen and nitrate nitrogen have independent sources of isotopic variation. Copyright © 2014 John Wiley & Sons, Ltd.

  4. Development of a Catalyst/Sorbent for Methane Reforming

    Energy Technology Data Exchange (ETDEWEB)

    B.H. Shans; T.D. Wheelock; Justinus Satrio; Karl Albrecht; Tanya Harris Janine Keeley; Ben Silva; Aaron Shell; Molly Lohry; Zachary Beversdorf


    This project led to the further development of a combined catalyst and sorbent for improving the process technology required for converting CH{sub 4} and/or CO into H{sub 2} while simultaneously separating the CO{sub 2} byproduct all in a single step. The new material is in the form of core-in-shell pellets such that each pellet consists of a CaO core surrounded by an alumina-based shell capable of supporting a Ni catalyst. The Ni is capable of catalyzing the reactions of steam with CH{sub 4} or CO to produce H{sub 2} and CO{sub 2}, whereas the CaO is capable of absorbing the CO{sub 2} as it is produced. The absorption of CO{sub 2} eliminates the reaction inhibiting effects of CO{sub 2} and provides a means for recovering the CO{sub 2} in a useful form. The present work showed that the lifecycle performance of the sorbent can be improved either by incorporating a specific amount of MgO in the material or by calcining CaO derived from limestone at 1100 C for an extended period. It also showed how to prepare a strong shell material with a large surface area required for supporting an active Ni catalyst. The method combines graded particles of {alpha}-alumina with noncrystalline alumina having a large specific surface area together with a strength promoting additive followed by controlled calcination. Two different additives produced good results: 3 {micro}m limestone and lanthanum nitrate which were converted to their respective oxides upon calcination. The oxides partially reacted with the alumina to form aluminates which probably accounted for the strength enhancing properties of the additives. The use of lanthanum made it possible to calcine the shell material at a lower temperature, which was less detrimental to the surface area, but still capable of producing a strong shell. Core-in-shell pellets made with the improved shell materials and impregnated with a Ni catalyst were used for steam reforming CH{sub 4} at different temperatures and pressures. Under all

  5. Development and process evaluation of improved Fischer-Tropsch slurry catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Withers, H.P. (Air Products and Chemicals, Inc., Allentown, PA (United States)); Bukur, D.B.; Rosynek, M.P. (Texas A and M Univ., College Station, TX (United States))


    The objective of this contract is to develop a consistent technical data base on the use of iron-based catalysts in Fischer-Tropsch (FT) synthesis reactions. This data base will be developed to allow the unambiguous comparison of the performance of these catalysts with each other and with state-of-the-art iron catalyst comparisons. Particular attention will be devoted to generating reproducible kinetic and selectivity data and to developing reproducible improved catalyst compositions.

  6. Development and process evaluation of improved Fischer-Tropsch slurry catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Withers, H.P. (Air Products and Chemicals, Inc., Allentown, PA (United States)); Bukur, D.B.; Rosynek, M.P. (Texas A and M Univ., College Station, TX (United States))


    The objective of this contract is to develop a consistent technical data base on the use of iron-based catalysts in Fischer-Tropsch (FT) synthesis reactions. This data base will be developed to allow the unambiguous comparison of the performance of these catalysts with each other and with state-of-the-art iron catalyst compositions. Particular attention will be devoted to generating reproducible kinetic and selectivity data and to developing reproducible improved catalyst compositions.

  7. Entrepreneurship as a Catalyst for Rural Tourism Development

    Directory of Open Access Journals (Sweden)

    Md Sharif Norhafiza


    Full Text Available The tourism industry is seen as capable of being an agent of change in the landscape of economic, social and environment of a tourist destination. Tourism activity has also generated employment and entrepreneurship opportunities to the local community as well as using available resources as tourist attractions. The tourism sector has the potential to be a catalyst for the development of entrepreneurship and small business performance. Through the development of tourism, the rural community has the opportunity to offer services or sell products to the both local and foreign tourists. To fulfill this purpose, local community participation in entrepreneurship is very important in order to develope the economic potential and to determine the direction of a development in rural areas. In the context of entrepreneurship, local participation is important not only as an entrepreneur and labor in this sector as well as complementary sectors of the others, but they can serve to encourage the involvement of other residents to join together to develop this entrepreneurial. This article aims to discuss the extent of entrepreneurship as a catalyst to the development of tourism in rural areas. Through active participation among community members, rural entrepreneurship will hopefully move towards prosperity and success of rural development.

  8. Development of Sulfur and Carbon Tolerant Reforming Alloy Catalysts Aided Fundamental Atomistic Insights

    Energy Technology Data Exchange (ETDEWEB)

    Suljo Linic


    Current hydrocarbon reforming catalysts suffer from rapid carbon and sulfur poisoning. Even though there is a tremendous incentive to develop more efficient catalysts, these materials are currently formulated using inefficient trial and error experimental approaches. We have utilized a hybrid experimental/theoretical approach, combining quantum Density Functional Theory (DFT) calculations and various state-of-the-art experimental tools, to formulate carbon tolerant reforming catalysts. We have employed DFT calculations to develop molecular insights into the elementary chemical transformations that lead to carbon poisoning of Ni catalysts. Based on the obtained molecular insights, we have identified, using DFT quantum calculation, various Ni alloy catalysts as potential carbon tolerant reforming catalysts. The alloy catalysts were synthesized and tested in steam reforming and partial oxidation of methane, propane, and isooctane. We demonstrated that the alloy catalysts are much more carbon-tolerant than monometallic Ni catalysts under nearly stoichiometric steam-to-carbon ratios. Under these conditions, monometallic Ni is rapidly poisoned by sp2 carbon deposits. The research approach is distinguished by two characteristics: (a) knowledge-based, bottomup approach, compared to the traditional trial and error approach, allows for a more efficient and systematic discovery of improved catalysts. (b) the focus is on exploring alloy materials which have been largely unexplored as potential reforming catalysts.

  9. Development of vapor phase hydrogenation and of catalysts immune to poison (abstract)

    Energy Technology Data Exchange (ETDEWEB)


    The development of catalysts immune to poison and the development of vapor-phase hydrogenation were closely connected and they were considered together. Catalysts used at high thruputs and high partial pressures showed rapid deterioration of their activity caused by deposition and condensation of high-molecular-weight substances on the surface of the catalysts. This phenomenon made it necessary to divide hydrogenation into two phases: the liquid phase and the vapor phase. The first of the vapor-phase operating catalysts was catalyst 3510, which consisted of zinc--magnesium molybdate. Development of catalyst 5058, which consisted of pure tungsten disulfide and was produced by decomposing ammonium--sulfotungstate in H/sub 2/ atmosphere, largely terminated development of vapor-phase catalysts. Maximum activity had been obtained. Compared to 3510, two to three times as much gasoline was produced per hour with a fixed volume of catalyst, besides being able to work at a temperature about 100/sup 0/C lower, and gasification losses were considerably smaller. In order to use 5058 in mass production, the dry catalyst powder had to be compressed into cylindrical shapes 10 mm in diameter. The demands for higher antiknock gasolines in the processing of certain paraffinic raw material could not be met by 5058 because of its strong hydrogenation effect, and the dilute catalyst 6434, consisting of 90% Fullers earth treated with HF and 10% WS/sub 2/, was developed for this. 3 tables.

  10. Catalytic Upgrading of Ethanol to n-Butanol: Progress in Catalyst Development. (United States)

    Wu, Xianyuan; Fang, Geqian; Tong, Yuqin; Jiang, Dahao; Liang, Zhe; Leng, Wenhua; Liu, Liu; Tu, Pengxiang; Wang, Hongjing; Ni, Jun; Li, Xiaonian


    Because n-butanol as a fuel additive has more advantageous physicochemical properties than those of ethanol, ethanol valorization to n-butanol through homo- or heterogeneous catalysis has received much attention in recent decades in both scientific and industrial fields. Recent progress in catalyst development for upgrading ethanol to n-butanol, which involves homogeneous catalysts, such as iridium and ruthenium complexes, and heterogeneous catalysts, including metal oxides, hydroxyapatite (HAP), and, in particular, supported metal catalysts, is reviewed herein. The structure-activity relationships of catalysts and underlying reaction mechanisms are critically examined, and future research directions on the design and improvement of catalysts are also proposed. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  11. Development of micro-cogeneration system with porous catalyst microcombustor (United States)

    Takahashi, S.; Tanaka, M.; Ieda, N.; Ihara, T.


    A self-standing micro-cogeneration system was developed by coupling a microcombustor, thermoelectric (TE) modules, and an air supply device. The microcombustor has a porous monolithic Pt catalyst layer, and a combustion efficiency of 90% was achieved. A microblower is used to supply air to the combustor, and it is driven by electricity from the Bi-Te TE modules through a dc-dc converter. We investigated the optimal point where the output became maximal and the system was self-standing. At the optimal point, the input fuel enthalpy was 13.2 W, and 440 mW of electricity was generated from the TE modules. The microblower consumed 280 mW, and the net generated electricity was 160 mW. Therefore, the final thermal efficiency was 1.21%. The net thermal efficiency of the developed system was the same magnitude as that of TeeDee01 (COX Co. Ltd.), the world’s smallest model plane engine (0.163 cc), even though the magnitude of the output power was less than 1/20 in comparison.


    Energy Technology Data Exchange (ETDEWEB)

    Burtron H. Davis


    The impact of activation procedure on the phase composition of precipitated iron Fischer-Tropsch (FT) catalysts has been studied. Catalyst samples taken during activation and FT synthesis have been characterized by Moessbauer spectroscopy. Formation of iron carbide is necessary for high FT activity. Hydrogen activation of precipitated iron catalysts results in reduction to predominantly metallic iron and Fe{sub 3}O{sub 4}. Metallic iron is not stable under FT 3 4 conditions and is rapidly converted to {epsilon}{prime}-Fe{sub 2.2}C. Activation with carbon monoxide or syngas 2.2 with low hydrogen partial pressure reduces catalysts to {chi}-Fe{sub 5}C{sub 2} and a small amount of 5 2 superparamagnetic carbide. Exposure to FT conditions partially oxidizes iron carbide to Fe{sub 3}O{sub 4}; however, catalysts promoted with potassium or potassium and copper maintain a constant carbide content and activity after the initial oxidation. An unpromoted iron catalyst which was activated with carbon monoxide to produce 94% {chi}-Fe{sub 5}C{sub 2}, deactivated rapidly as the carbide was oxidized to Fe{sub 3}O{sub 4}. No difference in activity, stability or deactivation rate was found for {chi}-Fe{sub 5}C{sub 2} and {epsilon}{prime}-Fe{sub 2.2}C.

  13. Discovery, Development, and Commercialization of Gold Catalysts for Acetylene Hydrochlorination. (United States)

    Johnston, Peter; Carthey, Nicholas; Hutchings, Graham J


    Vinyl chloride monomer (VCM) is a major chemical intermediate for the manufacture of polyvinyl chloride (PVC), which is the third most important polymer in use today. Hydrochlorination of acetylene is a major route for the production of vinyl chloride, since production of the monomer is based in regions of the world where coal is abundant. Until now, mercuric chloride supported on carbon is used as the catalyst in the commercial process, and this exhibits severe problems associated with catalyst lifetime and mercury loss. It has been known for over 30 years that gold is a superior catalyst, but it is only now that it is being commercialized. In this Perspective we discuss the use and disadvantages of the mercury catalyst and the advent of the gold catalysts for this important reaction. The nature of the active site and the possible reaction mechanism are discussed. Recent advances in the design and preparation of active gold catalysts containing ultralow levels of gold are described. In the final part, a view to the future of this chemistry will be discussed as well as the possible avenues for the commercial potential of gold catalysis.

  14. Development of novel catalysts for the photocatalytic hydrogen formation

    Energy Technology Data Exchange (ETDEWEB)

    Pilz, Thomas David


    For future conversion of sunlight into chemical energy, intramolecular systems for artifical photosynthesis were developed in several stages. This comprised the fabrication of novel ligands and the resulting charge transfer chromophores (Ru(bpy)3-type) and/or catalytically active complexes (Pt, Pd). These were combined into heteronuclear diades consisting of covalently bonded functional subunits. In particular, the chromophores and catalysis centers were bridged so that their individual properties were retained while their individual functions were combined into a supramolecular photocatalyst. This makes it possible to reduce protons to hydrogen on these catalysts when exposed to light. As bridging units, oligodentate ligands were produced and used that can coordinate the active metal centers via bipyridines and N-heterocyclic carbenes (NHC). A number of such heterobimetal complexes, their initial compounds and appropriate reference compounds were produced, characterized, and compared. Apart from structural, photophysical and electrochemical analyses, also successful catalysis experiment were carried out with the manufactured photocatalysts for light-induced hydrogen production from water. Further representative control experiments and dynamic light scattering analyses were carried out in order to gain deeper understanding of the processes going on during catalysis. By comparing the properties of the fabricated catalysts with selected reference compounds, information was obtained on the structure-property relationships of the systems. (orig.) [German] Fuer die zukuenftige Umwandlung von Sonnenlicht in chemische Energie wurden schrittweise intramolekular arbeitende Systeme fuer eine artifizielle Photosynthese aufgebaut. Dabei wurde eine Anzahl von neuen Liganden und den resultierenden Charge-Transfer-Chromophoren (Ru(bpy)3-artig) bzw. katalyseaktiven Komplexen (Pt, Pd) hergestellt. Diese wurden zu heteronuklearen Diaden zusammengefuegt, welche aus kovalent

  15. Development of Non-Noble Metal Ni-Based Catalysts for Dehydrogenation of Methylcyclohexane

    KAUST Repository

    Al-ShaikhAli, Anaam H.


    Liquid organic chemical hydride is a promising candidate for hydrogen storage and transport. Methylcyclohexane (MCH) to toluene (TOL) cycle has been considered as one of the feasible hydrogen carrier systems, but selective dehydrogenation of MCH to TOL has only been achieved using the noble Pt-based catalysts. The aim of this study is to develop non-noble, cost-effective metal catalysts that can show excellent catalytic performance, mainly maintaining high TOL selectivity achievable by Pt based catalysts. Mono-metallic Ni based catalyst is a well-known dehydrogenation catalyst, but the major drawback with Ni is its hydrogenolysis activity to cleave C-C bonds, which leads to inferior selectivity towards dehydrogenation of MCH to TOL. This study elucidate addition of the second metal to Ni based catalyst to improve the TOL selectivity. Herein, ubiquitous bi-metallic nanoparticles catalysts were investigated including (Ni–M, M: Ag, Zn, Sn or In) based catalysts. Among the catalysts investigated, the high TOL selectivity (> 99%) at low conversions was achieved effectively using the supported NiZn catalyst under flow of excess H2. In this work, a combined study of experimental and computational approaches was conducted to determine the main role of Zn over Ni based catalyst in promoting the TOL selectivity. A kinetic study using mono- and bimetallic Ni based catalysts was conducted to elucidate reaction mechanism and site requirement for MCH dehydrogenation reaction. The impact of different reaction conditions (feed compositions, temperature, space velocity and stability) and catalyst properties were evaluated. This study elucidates a distinctive mechanism of MCH dehydrogenation to TOL reaction over the Ni-based catalysts. Distinctive from Pt catalyst, a nearly positive half order with respect to H2 pressure was obtained for mono- and bi-metallic Ni based catalysts. This kinetic data was consistent with rate determining step as (somewhat paradoxically) hydrogenation


    Energy Technology Data Exchange (ETDEWEB)

    Adeyinka A. Adeyiga


    Fischer-Tropsch (FT) synthesis to convert syngas (CO + H{sub 2}) derived from natural gas or coal to liquid fuels and wax is a well-established technology. For low H{sub 2} to CO ratio syngas produced from CO{sub 2} reforming of natural gas or from gasification of coal, the use of Fe catalysts is attractive because of their high water gas shift activity in addition to their high FT activity. Fe catalysts are also attractive due to their low cost and low methane selectivity. Because of the highly exothermic nature of the FT reaction, there has been a recent move away from fixed-bed reactors toward the development of slurry bubble column reactors (SBCRs) that employ 30 to 90 {micro}m catalyst particles suspended in a waxy liquid for efficient heat removal. However, the use of Fe FT catalysts in an SBCR has been problematic due to severe catalyst attrition resulting in fines that plug the filter employed to separate the catalyst from the waxy product. Fe catalysts can undergo attrition in SBCRs not only due to vigorous movement and collisions but also due to phase changes that occur during activation and reaction. The objectives of this research were to develop a better understanding of the parameters affecting attrition of Fe F-T catalysts suitable for use in SBCRs and to incorporate this understanding into the design of novel Fe catalysts having superior attrition resistance. The catalysts were prepared by co-precipitation, followed by binder addition and spray drying at 250 C in a 1 m diameter, 2 m tall spray dryer. The binder silica content was varied from 0 to 20 wt %. The results show that use of small amounts of precipitated SiO{sub 2} alone in spray-dried Fe catalysts can result in good attrition resistance. All catalysts investigated with SiO{sub 2} wt% {le} 12 produced fines less than 10 wt% during the jet cup attrition test, making them suitable for long-term use in a slurry bubble column reactor. Thus, concentration rather than type of SiO{sub 2

  17. Development of Sulfur and Carbon Tolerant Reforming Alloy Catalysts Aided by Fundamental Atomistics Insights

    Energy Technology Data Exchange (ETDEWEB)

    Suljo Linic


    Current hydrocarbon reforming catalysts suffer from rapid carbon and sulfur poisoning. Even though there is a tremendous incentive to develop more efficient catalysts, these materials are currently formulated using inefficient trial and error experimental approaches. We have utilized a novel hybrid experimental/theoretical approach, combining quantum Density Functional Theory (DFT) calculations and various state-of-the-art experimental tools, to formulate carbon tolerant reforming catalysts. We have employed DFT calculations to develop molecular insights into the elementary chemical transformations that lead to carbon poisoning of Ni catalysts. Based on the obtained molecular insights, we have identified, using DFT quantum calculation, Sn/Ni alloy as a potential carbon tolerant reforming catalyst. Sn/Ni alloy was synthesized and tested in steam reforming of methane, propane, and isooctane. We demonstrated that the alloy catalyst is carbon-tolerant under nearly stoichiometric steam-to-carbon ratios. Under these conditions, monometallic Ni is rapidly poisoned by sp2 carbon deposits. The research approach is distinguished by a few characteristics: (a) Knowledge-based, bottom-up approach, compared to the traditional trial and error approach, allows for a more efficient and systematic discovery of improved catalysts. (b) The focus is on exploring alloy materials which have been largely unexplored as potential reforming catalysts.

  18. Development and process evaluation of improved Fischer-Tropsch slurry catalysts. Quarterly technical progress report, 1 October-31 December 1987

    Energy Technology Data Exchange (ETDEWEB)

    Withers, H.P. [Air Products and Chemicals, Inc., Allentown, PA (United States); Bukur, D.B.; Rosynek, M.P. [Texas A and M Univ., College Station, TX (United States)


    The objective of this contract is to develop a consistent technical data base on the use of iron-based catalysts in Fischer-Tropsch (FT) synthesis reactions. This data base will be developed to allow the unambiguous comparison of the performance of these catalysts with each other and with state-of-the-art iron catalyst compositions. Particular attention will be devoted to generating reproducible kinetic and selectivity data and to developing reproducible improved catalyst compositions.

  19. The development of precipitated iron catalysts with improved stability; Final report, September 1987--September 1992

    Energy Technology Data Exchange (ETDEWEB)

    Abrevaya, H.


    Precipitated iron catalysts are expected to be used in next generation slurry reactors for large-scale production of transportation fuels from synthesis gas. These reactors are expected to operate at higher temperatures and lower H{sub 2}:CO ratios relative to the Sasol Arge reactor (Table 1A). The feasibility of using iron catalysts has been demonstrated under relatively mild Arge-type conditions but not under more severe slurry conditions. Possibly, an improvement in catalytic stability will be needed to make iron catalysts suitable for slurry operation. This program was aimed at identifying the chemical principles governing the deactivation of precipitated iron catalysts during Fischer-Tropsch synthesis and use of these chemical principles in the design of more stable catalysts. A new precipitated Fe catalyst was developed in this program for slurry reactor operation. The new Fe catalyst is predicted to perform slightly below the performance targets for slurry bubble column operation. Stability targets appear to be achievable. This catalyst did not noticeably deactivate during 1,740 hours on-stream. Compared to the selectivity target, an excess of 2% C{sub 1} + C{sub 2} was formed at 265{degrees}C. Based on the initial catalyst inventory in the autoclave, the catalyst seems to be short of the activity target by a factor of 1.8 at 265{degrees}C and 1.3 at 275{degrees}C. However, actual specific activities are likely to be closer to target because of catalyst inventory loss across the filter during the run and because catalytic activities were underestimated at low conversions.

  20. Scientist-teacher interactions: Catalysts for developing transformational classrooms (United States)

    McCarty, Robbie Von

    Professional development leading to standards-based teaching practices in U.S. schools is a remarkably subtle and lengthy process. Research indicates that there are many effective tools for teaching through inquiry available to teachers (Lawson, Abraham, & Renner, 1989), but also that teachers continue to present traditional positivistic views of science (Hashweh, 1985; Maor & Taylor, 1995; Zucker, Young, & Luczak, 1996) and appear to view constructivism as a "method" of teaching rather than a way of thinking about learning (Tobin, Tippins, & Gallard, 1984). Teachers are expected to create enriched environments where students can develop the thinking skills of scientists (Roth & Roychoudhury, 1993) but the majority of teachers have never experienced such environments; the involvement of scientists in science education is encouraged by the NRC, AAAS, and NSTA. Teachers and students are expected to act as coresearchers, where negotiation, debate, consensus, and reflection are key. It is believed that scientist and teachers interacting as co-researchers could assist teachers in developing attitudes of freedom in exploration: the essence of science and a mindset that constructivism is a referent, or tool for critical reflection (Tobin, Tippins & Gallard, 1994). This study seeks to identify aspects of scientist-teacher interactions in the field that could serve as catalysts for developing transformational classrooms. Multiple data sources were collected for this study: audiotapes and transcripts of laboratory interactions and informal interviews, written narratives from applications and funding documents, field notes, and personal communications. Data were simultaneously collected, analyzed and coded as a perpetual review of the literature was conducted as in the grounded theory methodology defined by Glaser (1967) and later by Strauss & Corbin (1990). Findings indicate all four teachers valued field experiences in personal ways, developed new understandings of

  1. Development of catalysts and ligands for enantioselective gold catalysis. (United States)

    Wang, Yi-Ming; Lackner, Aaron D; Toste, F Dean


    During the past decade, the use of Au(I) complexes for the catalytic activation of C-C π-bonds has been investigated intensely. Over this time period, the development of homogeneous gold catalysis has been extraordinarily rapid and has yielded a host of mild and selective methods for the formation of carbon-carbon and carbon-heteroatom bonds. The facile formation of new bonds facilitated by gold naturally led to efforts toward rendering these transformations enantioselective. In this Account, we survey the development of catalysts and ligands for enantioselective gold catalysis by our research group as well as related work by others. We also discuss some of our strategies to address the challenges of enantioselective gold(I) catalysis. Early on, our work with enantioselective gold-catalyzed transformations focused on bis(phosphinegold) complexes derived from axially chiral scaffolds. Although these complexes were highly successful in some reactions like cyclopropanation, the careful choice of the weakly coordinating ligand (or counterion) was necessary to obtain high levels of enantioselectivity for the case of allene hydroamination. These counterion effects led us to use the anion itself as a source of chirality, which was successful in the case of allene hydroalkoxylation. In general, these tactics enhance the steric influence around the reactive gold center beyond the two-coordinate ligand environment. The use of binuclear complexes allowed us to use the second gold center and its associated ligand (or counterion) to exert a further steric influence. In a similar vein, we employed a chiral anion (in place of or in addition to a chiral ligand) to move the chiral information closer to the reactive center. In order to expand the scope of reactions amenable to enantioselective gold catalysis to cycloadditions and other carbocyclization processes, we also developed a new class of mononuclear phosphite and phosphoramidite ligands to supplement the previously widely

  2. Metalloporphyrin catalysts for oxygen reduction developed using computer-aided molecular design

    Energy Technology Data Exchange (ETDEWEB)

    Ryba, G.N.; Hobbs, J.D.; Shelnutt, J.A. [and others


    The objective of this project is the development of a new class of metalloporphyrin materials used as catalsyts for use in fuel cell applications. The metalloporphyrins are excellent candidates for use as catalysts at both the anode and cathode. The catalysts reduce oxygen in 1 M potassium hydroxide, as well as in 2 M sulfuric acid. Covalent attachment to carbon supports is being investigated. The computer-aided molecular design is an iterative process, in which experimental results feed back into the design of future catalysts.

  3. Technology development for iron F-T catalysts. Final report

    Energy Technology Data Exchange (ETDEWEB)

    Frame, R.R.; Gala, H.B.


    The objectives of this work were twofold. The first objective was to design and construct a pilot plant for preparing precipitated iron oxide F-T precursors and demonstrate that the rate of production from this plant is equivalent to 100 lbs/day of dried metal oxide. Secondly, these precipitates were to be used to prepare catalysts capable of achieving 88% CO + H{sub 2} conversion with {le} 5 mole percent selectivity to methane + ethane.

  4. Discovery, development, and commercialization of gold catalysts for acetylene hydrochlorination


    Johnston, Peter; Carthey, Nicholas; Hutchings, Graham John


    Vinyl chloride monomer (VCM) is a major chemical intermediate for the manufacture of polyvinyl chloride (PVC), which is the third most important polymer in use today. Hydrochlorination of acetylene is a major route for the production of vinyl chloride, since production of the monomer is based in regions of the world where coal is abundant. Until now, mercuric chloride supported on carbon is used as the catalyst in the commercial process, and this exhibits severe problems associated with catal...

  5. 2-Dimethylamino-1-(2-ethoxy-2-oxoethyl-3-methyl-4,5-dihydroimidazolium tetraphenylborate

    Directory of Open Access Journals (Sweden)

    Ioannis Tiritiris


    Full Text Available In the crystal structure of the title salt, C10H20N3O2+·C24H20B−, the C—N bond lengths in the cation are 1.327 (3, 1.339 (3 and 1.342 (3 Å, indicating partial double-bond character. The central C atom is bonded to the three N atoms, indicating only a slight deviation from a trigonal–planar geometry. The positive charge is delocalized in the CN3 plane. The ethoxy group is disordered over two orientations, with an occupancy ratio of 0.60 (1:0.40 (1. C—H...π interactions are present between the guanidinium H atoms and the phenyl C atoms of the tetraphenylborate ions. The phenyl rings form aromatic pockets, in which the cations are embedded. This leads to the formation of a two-dimensional supramolecular pattern along the ac plane.

  6. Derivative spectrophotometric determination of trace lead in alloys and biological samples after separation and preconcentration with the ion pair of 2-(5-bromo-2-pyridylazo-5-diethylaminophenol and ammonium tetraphenylborate on microcrystalline naphthalene or by column method

    Directory of Open Access Journals (Sweden)

    Mohammad Ali Taher


    Full Text Available Lead is quantitatively retained on 2-(5-bromo-2-pyridylazo-5-diethylaminophenol-ammonium tetraphenylborate with microcrystalline naphthalene or by a column method in the pH range 4.0–6.0 from a large volume of aqueous solutions of various samples. After filtration, the solid mass consisting of the lead complex and naphthalene was dissolved with 5 mL of dimethylformamide and the metal was determined by third derivative spectrophotometry. Lead complex can alternatively be quantitatively adsorbed on ammonium tetraphenylborate-naphthalene adsorbent packed in a column and determined similarly. About 0.2 μg of lead can be concentrated in a column from 300 mL of aqueous sample, where its concentration is as low as 0.7 ng/mL. The interference of a large number of anions and cations has been studied and the optimized conditions developed have been utilized for the trace determination of lead in various samples.

  7. Development of Coke-tolerant Transition Metal Catalysts for Dry Reforming of Methane

    KAUST Repository

    Al-Sabban, Bedour E.


    Dry reforming of methane (DRM) is an attractive and promising process for the conversion of methane and carbon dioxide which are the most abundant carbon sources into valuable syngas. The produced syngas, which is a mixture of hydrogen and carbon monoxide, can be used as intermediates in the manufacture of numerous chemicals. To achieve high conversion, DRM reaction is operated at high temperatures (700-900 °C) that can cause major drawbacks of catalyst deactivation by carbon deposition, metal sintering or metal oxidation. Therefore, the primary goal is to develop a metal based catalyst for DRM that can completely suppress carbon formation by designing the catalyst composition. The strategy of this work was to synthesize Ni-based catalysts all of which prepared by homogeneous deposition precipitation method (HDP) to produce nanoparticles with narrow size distribution. In addition, control the reactivity of the metal by finely tuning the bimetallic composition and the reaction conditions in terms of reaction temperature and pressure. The highly endothermic dry reforming of methane proceeds via CH4 decomposition to leave surface carbon species, followed by removal of C with CO2-derived species to give CO. Tuning the reactivity of the active metal towards these reactions during DRM allows in principle the catalyst surface to remain active and clean without carbon deposition for a long-term. The initial attempt was to improve the resistance of Ni catalyst towards carbon deposition, therefore, a series of 5 wt.% bimetallic Ni9Pt1 were supported on various metal oxides (Al2O3, CeO2, and ZrO2). The addition of small amount of noble metal improved the stability of the catalyst compared to their monometallic Ni and Pt catalysts, but still high amount of carbon (> 0.1 wt.%) was formed after 24 h of the reaction. The obtained results showed that the catalytic performance, particle size and amount of deposited carbon depends on the nature of support. Among the tested

  8. Development of a catalyst for conversion of syngas-derived materials to isobutylene

    Energy Technology Data Exchange (ETDEWEB)

    Barger, P.T.; Spehlmann, B.C.; Gajda, G.J.


    The initial objective of this program was to develop a catalyst and process for the conversion of synthesis gas to isobutylene via the isosynthesis process. Preliminary work directed at identifying potential catalysts for this reaction did not have promising results. Therefore, the objectives of this program were revised to the development of a catalyst and process for the conversion of synthesis gas to isobutanol. Two approaches have been investigated in this area: the direct conversion of synthesis gas to higher alcohols and indirect conversion via methanol produced using conventional methanol synthesis technology. The isosynthesis reaction for the conversion of synthesis gas to branched hydrocarbons was pioneered by German workers during World War II The primary products of this reaction are either isobutane or isobutylene depending on the catalyst system used. Thoria-based catalysts were found to give the highest yields, but virtually all of the products were alkanes. More recently, there have been several reports of olefin production using ZrO{sub 2}-based. The preliminary work in this program focussed on the evaluation of ZrO{sub 2} and modified ZrO{sub 2} catalysts for the direct conversion of CO/H{sub 2} to isobutylene via the isosynthesis reaction. All of the catalysts and conditions evaluated in this work gave isobutylene yields of less than 4% which is far below that required for an economically viable process. A summary of the key results from this portion of the project is given in Section 3.6. In view of the poor performance of these catalysts and the lack any encouraging results from other research groups working in the isosynthesis area, this approach was abandoned in favor of approaches related to higher alcohols synthesis.

  9. Development of a supported tri-metallic catalyst and evaluation of the catalytic activity in biomass steam gasification. (United States)

    Li, Jianfen; Xiao, Bo; Yan, Rong; Xu, Xiaorong


    A supported tri-metallic catalyst (nano-Ni-La-Fe/gamma-Al(2)O(3)) was developed for tar reduction and enhanced hydrogen production in biomass steam gasification, with focuses on preventing coke deposition and sintering effects to lengthen the lifetime of developed catalysts. The catalyst was prepared by deposition-precipitation method and characterized by various analytical approaches. Following that, the activity of catalysts in biomass steam gasification was investigated in a bench-scale combined fixed bed reactor. With presence of the catalyst, the content of hydrogen in gas products was increased to over 10 vol.%, the tar removal efficiency reached 99% at 1073 K, and more importantly the coke deposition on the catalyst surfaces and sintering effects were avoided, leading to a long lifetime of catalysts.

  10. Development of New Diesel Oxidation and NH3 Slip Catalysts

    DEFF Research Database (Denmark)

    Hansen, Thomas Klint

    Diesel engines used in the transport sector and for other heavy machinery form pollutants during the combustion process. Emission of these pollutants into the atmosphere has harmful consequences on human health and the environment. In order to mitigate these harmful effects, regulations have been...... imposed by environmental protection agencies on the most significant pollutants, including CO, hydrocarbons, NOx, and particulate matter. To reduce emissions to the levels specified by the recent Euro VI regulations, it is necessary to apply catalytic exhaust gas aftertreat-ment systems. A modern diesel...... exhaust aftertreatment system commonly consists of a Pt-based diesel oxidation catalyst (DOC) to oxidize CO and unburnt hydrocarbons to CO2 and H2O, and oxidize NO to NO2. This is followed by the diesel particulate filter (DPF), which entraps particulate matter from the exhaust gas. A solution of urea...


    Energy Technology Data Exchange (ETDEWEB)

    Adu-Wusu, K


    Tank 48H return to service is critical to the processing of high level waste (HLW) at Savannah River Site (SRS). Liquid Waste Disposition (LWD) management has the goal of returning Tank 48H to routine service by January 2010 or as soon as practical. Tank 48H currently holds legacy material containing organic tetraphenylborate (TPB) compounds from the operation of the In-Tank Precipitation process. This material is not compatible with the waste treatment facilities at SRS and must be removed or undergo treatment to destroy the organic compounds before the tank can be returned to Tank Farm service. Tank 48H currently contains {approx}240,000 gallons of alkaline slurry with about 2 wt % potassium and cesium tetraphenylborate (KTPB and CsTPB). The main radioactive component in Tank 48H is {sup 137}Cs. The waste also contains {approx}0.15 wt % Monosodium Titanate (MST) which has adsorbed {sup 90}Sr, U, and Pu isotopes. A System Engineering Evaluation of technologies/ideas for the treatment of TPB identified Wet Air Oxidation (WAO) as a leading alternative technology to the baseline aggregation approach. Over 75 technologies/ideas were evaluated overall. Forty-one technologies/ideas passed the initial screening evaluation. The 41 technologies/ideas were then combined to 16 complete solutions for the disposition of TPB and evaluated in detail. Wet Air Oxidation (WAO) is an aqueous phase process in which soluble or suspended waste components are oxidized using molecular oxygen contained in air. The process operates at elevated temperatures and pressures ranging from 150 to 320 C and 7 to 210 atmospheres, respectively. The products of the reaction are CO{sub 2}, H{sub 2}O, and low molecular weight oxygenated organics (e.g. acetate, oxalate). The basic flow scheme for a typical WAO system is as follows. The waste solution or slurry is pumped through a high-pressure feed pump. An air stream containing sufficient oxygen to meet the oxygen requirements of the waste stream is

  12. Quality Service in the International Hotel Sector: A Catalyst for Strategic Human Resource Development? (United States)

    Maxwell, Gill; Watson, Sandra; Quail, Samantha


    This paper analyses the nature of, and relationship between, a quality service initiative and the concept of strategic human resource development. Hilton International is the case study used for this analysis. The principal finding is that the quality initiative is acting as a catalyst for a strategic approach to human resource development to…

  13. Development of Ultra-Low Platinum Alloy Cathode Catalysts for PEM Fuel Cells

    Energy Technology Data Exchange (ETDEWEB)

    Popov, Branko N. [Univ. of South Carolina, Columbia, SC (United States). Dept. of Chemical Engineering; Weidner, John [Univ. of South Carolina, Columbia, SC (United States)


    The goal of this project is to synthesize a low cost PEM fuel cell cathode catalyst and support with optimized average mass activity, stability of mass activity, initial high current density performance under H2/air (power density), and catalyst and support stability able to meet 2017 DOE targets for electrocatalysts for transportation applications. Pt*/ACCS-2 catalyst was synthesized according to a novel methodology developed at USC through: (i) surface modification, (ii) metal catalyzed pyrolysis and (iii) chemical leaching to remove excess meal used to dope the support. Pt* stands for suppressed platinum catalyst synthesized with Co doped platinum. The procedure results in increasing carbon graphitization, inclusion of cobalt in the bulk and formation of non-metallic active sites on the carbon surface. Catalytic activity of the support shows an onset potential of 0.86 V for the oxygen reduction reaction (ORR) with well-defined kinetic and mass transfer regions and 2.5% H2O2 production. Pt*/ACCS-2 catalyst durability under 0.6-1.0 V potential cycling and support stability under 1.0-1.5 V potential cycling was evaluated. The results indicated excellent catalyst and support performance under simulated start-up/shut down operating conditions (1.0 – 1.5 V, 5000 cycles) which satisfy DOE 2017 catalyst and support durability and activity. The 30% Pt*/ACCS-2 catalyst showed high initial mass activity of 0.34 A/mgPGM at 0.9 ViR-free and loss of mass activity of 45% after 30,000 cycles (0.6-1.0 V). The catalyst performance under H2-air fuel cell operating conditions showed only 24 mV (iR-free) loss at 0.8 A/cm2 with an ECSA loss of 42% after 30,000 cycles (0.6-1.0 V). The support stability under 1.0-1.5 V potential cycling showed mass activity loss of 50% and potential loss of 8 mV (iR-free) at 1.5 A/cm2. The ECSA loss was 22% after 5,000 cycles. Furthermore, the Pt*/ACCS-2 catalyst showed an

  14. Strategies for catalyst development: possibilities of the ``rational approach`` illustrated with partial oxidation reactions

    Energy Technology Data Exchange (ETDEWEB)

    Weiss, W.; Schedel-Niedrig, T.; Schloegl, R. [Fritz-Haber-Institut der Max-Planck-Gesellschaft, Berlin (Germany). Abt. Oberflaechenphysik


    The paper discusses two petrochemical selective oxidation reactions namely the practised formation of styrene (STY) and the desired oxidative functionalisation of propane. The present knowledge about the mode of operation of oxide catalysts is critically considered. The dehydrogenation of ethylbenzene (EB) should be described by an oxidehydration with water acting as oxidant. The potential role of the coke formed during catalytic reaction as co-catalyst will be discussed. Selective oxidation is connected with the participation of lattice oxygen mechanism which transforms unselective gas phase oxygen into selective oxygen. The atomistic description of this process is still quite unclear as well as the electron structural properties of the activated oxygen atom. The Role of solid state acidity as compared to the role of lattice oxygen is much less well investigated modern multiphase-multielement oxide (MMO) catalysts. The rationale is that the significant efforts made to improve current MMO systems by chemical modifications can be very much more fruitful when in a first step the mode of action of a catalyst is clarified on the basis of suitable experiments. Such time-consuming experiments at the beginning of a campaign for catalyst improvement pay back their investment in later stages of the project when strategies of chemical development can be derived on grounds of understanding. (orig.)

  15. Recent Development of Catalysts for Removal of Volatile Organic Compounds in Flue Gas by Combustion: A Review

    Directory of Open Access Journals (Sweden)

    Marco Tomatis


    Full Text Available Volatile organic compounds (VOCs emitted from anthropogenic sources pose direct and indirect hazards to both atmospheric environment and human health due to their contribution to the formation of photochemical smog and potential toxicity including carcinogenicity. Therefore, to abate VOCs emission, the catalytic oxidation process has been extensively studied in laboratories and widely applied in various industries. This report is mainly focused on the benzene, toluene, ethylbenzene, and xylene (BTEX with additional discussion about chlorinated VOCs. This review covers the recent developments in catalytic combustion of VOCs over noble metal catalysts, nonnoble metal catalysts, perovskite catalysts, spinel catalysts, and dual functional adsorbent-catalysts. In addition, the effects of supports, coke formation, and water effects have also been discussed. To develop efficient and cost-effective catalysts for VOCs removal, further research in catalytic oxidation might need to be carried out to strengthen the understanding of catalytic mechanisms involved.

  16. N,N,N′,N′-Tetramethyl-N′′-[2-(trimethylazaniumylethyl]guanidinium bis(tetraphenylborate acetone disolvate

    Directory of Open Access Journals (Sweden)

    Ioannis Tiritiris


    Full Text Available The asymmetric unit of the title solvated salt, C10H26N42+·2C24H20B−·2C3H6O, comprises one cation, two tetraphenylborate ions and two acetone solvent molecules. The N and methyl C atoms of the terminal trimethylammonium group are disordered over two sets of sites, with a refined occupancy ratio of 0.846 (3:0.154 (3. The C—N bond lengths in the central C3N unit of the guanidinium ion range between 1.3308 (16 and 1.3508 (16 Å, indicating a degree of double-bond character. The central C atom is bonded to the three N atoms in a nearly ideal trigonal–planar geometry and the positive charge is delocalized in the CN3 plane. The C—N bond lengths in the terminal trimethylammonium group have values close to that of a typical single bond, and the second positive charge is localized there. In the crystal, the guanidinium ion is connected by N—H...O and C—H...O hydrogen bonds with the acetone molecules. C—H...π interactions are present between the guanidinium H atoms and the phenyl rings of the tetraphenylborate ions, leading to the formation of a two-dimensional supramolecular pattern along the bc plane.

  17. Development of Vanadium Phosphaate Catalysts for Methanol Production by Selective Oxidation of Methane.

    Energy Technology Data Exchange (ETDEWEB)

    McCormick, R.L.


    This DOE sponsored study of methane partial oxidation was initiated at Amax Research and Development in Golden, CO in October of 1993. Shortly thereafter the management of Amax closed this R&D facility and the PI moved to the Colorado School of Mines. The project was begun again after contract transfer via a novation agreement. Experimental work began with testing of vandyl pyrophosphate (VPO), a well known alkane selective oxidation catalyst. It was found that VPO was not a selective catalyst for methane conversion yielding primarily CO. However, promotion of VPO with Fe, Cr, and other first row transition metals led to measurable yields for formaldehyde, as noted in the summary table. Catalyst characterization studies indicated that the role of promoters was to stabilize some of the vanadium in the V{sup 5+} oxidation state rather than the V{sup 4+} state formally expected for (VO){sub 2}P{sub 2}O{sub 7}.

  18. Visible-Light-Responsive Catalyst Development for Volatile Organic Carbon Remediation Project (United States)

    Zeitlin, Nancy; Hintze, Paul E.; Coutts, Janelle


    Photocatalysis is a process in which light energy is used to 'activate' oxidation/reduction reactions. Unmodified titanium dioxide (TiO2), a common photocatalyst, requires high-energy UV light for activation due to its large band gap (3.2 eV). Modification of TiO2 can reduce this band gap, leading to visible-light-responsive (VLR) photocatalysts. These catalysts can utilize solar and/or visible wavelength LED lamps as an activation source, replacing mercury-containing UV lamps, to create a "greener," more energy-efficient means for air and water revitalization. Recently, KSC developed several VLR catalysts that, on preliminary evaluation, possessed high catalytic activity within the visible spectrum; these samples out-performed existing commercial VLR catalysts.

  19. Request for Information from entities interested in commercializing Laboratory-developed homogeneous catalyst technology

    Energy Technology Data Exchange (ETDEWEB)

    Intrator, Miranda Huang [Los Alamos National Lab. (LANL), Los Alamos, NM (United States)


    Many industrial catalysts used for homogeneous hydrogenation and dehydrogenation of unsaturated substrates are derived from metal complexes that include (air-sensitive) ligands that are often expensive and difficult to synthesize. In particular, catalysts used for many hydrogenations are based on phosphorus containing ligands (in particular PNP pincer systems). These ligands are often difficult to make, are costly, are constrained to having two carbon atoms in the ligand backbone and are susceptible to oxidation at phosphorus, making their use somewhat complicated. Los Alamos researchers have recently developed a new and novel set of ligands that are based on a NNS (ENENES) skeleton (i.e. no phosphorus donors, just nitrogen and sulfur).

  20. Shopping malls as catalyst for sub-urban development in Ghana ...

    African Journals Online (AJOL)

    This study investigated the possibility of using the Shopping Mall concept as catalyst to both help develop the suburbia and decongest cities in Ghana. The West Hills Mall at Dunkonah, a suburb near Accra was selected for the study. A mixed research method including questionnaires, interviews, and observations was used ...

  1. Hydrocracking for oriented conversion of heavy oils. Recent trends for catalyst development

    Energy Technology Data Exchange (ETDEWEB)

    Bertoncini, F.; Bonduelle, A.; Simon, L.J. [IFP Energies nouvelles, Lyon Establishment, Solaize (France). Catalysis and separation Division; Raybaud, P.; Dulot, H. [IFP Energies nouvelles, Lyon Establishment, Solaize (France). Process Desing Modeling Division


    As a result of the global economic crisis since the end of 2008, HCK operators have been looking to increase the profitability of the unit by processing heavier feed streams, including sourer VGO. These feeds present the drawbacks of increased H{sub 2} consumption, lower products yields and quality, and reduction in cycle lengths. Along with optimised process parameters, catalysts manufacturers are also investigating novel formulations to deal with challenging feeds. This lecture briefly summarizes the market trends (fuel demand, refinery's product specification) and the driving forces for HCK catalyst development in order to face these new challenges. Finally, this lecture highlights the innovating trends for HCK catalyst's development. Overview of various ideas developed recently in our research laboratory about (i) rational approaches for the atomic scale design of active phases (morphology, preparation, inhibitor effects), (ii) new preparations of transition metal sulphides for maximising the hydrogenating function (precursors, activation,.), (iii) rational approaches of HCK acidic supports for maximizing the selectivity and (iv) better understanding of HCK reactions. These improvements will be discussed in term of improvement of activity and selectivity of HCK catalyst to cope with future market needs. (orig.)

  2. Facile and One Pot Synthesis of Gold Nanoparticles Using Tetraphenylborate and Polyvinylpyrrolidone for Selective Colorimetric Detection of Mercury Ions in Aqueous Medium

    Directory of Open Access Journals (Sweden)

    Sidhureddy Boopathi


    Full Text Available In this work, we reported for the first time, a facile and one step synthesis of gold nanoparticles from HAuCl4, employing tetraphenylborate as the reducing agent. The synthesis is not only facile but also yields “dumb-bell-shaped”particles. This shape appears to arise from a possible emulsion of the products of oxidation/decomposition of tetraphenylborate by HAuCl4, surrounding the particle. The size and shape of the AuNPs were characterized by Transmission electron microscopy (TEM and UV-visible Spectroscopy. Interestingly, the addition of polyvinylpyrrolidone (PVP during the synthesis was found to enhance the stability of the nanoparticle dispersion. The particles synthesized under these conditions assume “spherical” shape with the appearance of only transverse surface plasmon resonance band. The highlight of the observations is that the gold nanoparticles synthesized using tetraphenylborate as reducing agent and PVP as stabilizer are highly stable in alkaline medium, in contrast to the synthesis wherein borohydride is used as reducing agent. The AuNPs synthesized using tetraphenylborate and PVP show their mercury sensing behavior only in the alkaline medium. The color of the nanoparticle dispersion undergoes distinct color change from pink to blue with the addition of mercury ions. They also show dramatic selectivity to mercury ions in presence of other interfering ions, Pb2+, Zn2+ and Ca2+.

  3. Novel Catalyst Development for Synthetic Endothermic Fuels Project (United States)

    National Aeronautics and Space Administration — Physical Sciences Incorporated (PSI) and United Technologies Research Center (UTRC) propose to develop, characterize, and evaluate the performance of innovative...

  4. Security: A Catalyst for Sustainable Development | Solomon | African ...

    African Journals Online (AJOL)

    This paper explores intricate nexus between security, and the challenges of promoting sustainable development in a volatile environment. It conceptualises security, sustainable development, and volatile environment. The paper argues that the volatile environment in the country has led to security breaches and slowed ...

  5. Tax incentive as a catalyst for economic development in Nigeria ...

    African Journals Online (AJOL)

    An empirical study using a well structured questionnaire survey, the work assesses the relationship that exists between tax incentive and economic development in Nigeria. This study was undertaken primarily to evaluate the effectiveness of tax incentive in developing the Nigerian economy. One hundred and twenty ...

  6. The development of isomerization catalysts for production of high-octane products

    Energy Technology Data Exchange (ETDEWEB)

    Pedrosa, A.M. Garrido; Melo, D.M.A.; Araujo, A.S. [Universidade Federal do Rio Grande do Norte, Natal, RN (Brazil). Dept. de Quimica; Souza, M.J.B.; Silva, A.O.S. [Universidade Federal do Rio Grande do Norte, Natal, RN (Brazil). Dept. de Engenharia Quimica


    In current petroleum industry, paraffins larger than C5 are used for catalytic reform. The catalytic reform is one of the most important processes for petroleum refine in reason of all reactions they drive to production of high-octane products. Reformate has high-octane products, but they contain 60% aromatics. Isomerization of C5- C7 can improve the octane number. The octane number of n-heptane is zero and increases after isomerization. For tri branched C7, the octane number reaches 113, which is higher than that of benzene. So, isomerization of C5-C7 is suggested to be a reasonable way to replace or partly replace the catalytic reforming process. It can decrease aromatics content with enhancement of octane number. Liquid acid catalysts were widely used in chemical industry in past decades. However, they face strong environmental challenges. The heavy corrosion of the reactor system is one of the main problems. Thus, solid acid catalysts are investigated for the isomerization reactions. The aim of this work is to develop a catalysts for the production of reformate products. Isomerization is catalyzed by metal-acid bifunctional catalysts. The metal components aid in hydrogenation, while the support, such as, zirconium, clays or zeolites, is the acidic component. (author)

  7. Future Regulations – A Catalyst for Technology Development (United States)

    Summary of current mobile source regulations and EPA mobile source regulatory authority with an emphasis on how EPA regulations are a driver for the development and introduction of automotive technology.

  8. Cross-departmental collaboration in strategic sourcing as a catalyst for supplier development: The case of Eskom

    Directory of Open Access Journals (Sweden)

    Mzoxolo E. Mbiko


    Conclusion: For strategic sourcing to be a catalyst of supplier development, it is essential that an integrated strategic sourcing operating model incorporating the objectives of both CS and SD&L be developed.

  9. Christian Church: A Catalyst for Economic Development in Nigeria

    African Journals Online (AJOL)


    Abstract. The issue of economic development is of national concern. The. Nigerian economy had a truncated history from independence to present times and the economy has suffered series of economic instability because of a long period of unsustained growth in the per capital real income of the country, accompanied by ...

  10. Creating a Catalyst for the Development of Knowledge Work Competence

    NARCIS (Netherlands)

    Dr. Daan Andriessen; Linda Johnson


    With the rise of the knowledge-based economy, Higher Education Institutions not only have to produce (under)graduates that are skilled in their profession but who also are competent as knowledge workers. This study focused on the enabling competences of the knowledge worker. Our aim was to develop a

  11. Recent advances in the development of alkyne metathesis catalysts

    Directory of Open Access Journals (Sweden)

    Matthias Tamm


    Full Text Available The number of well-defined molybdenum and tungsten alkylidyne complexes that are able to catalyze alkyne metathesis reactions efficiently has been significantly expanded in recent years.The latest developments in this field featuring highly active imidazolin-2-iminato- and silanolate–alkylidyne complexes are outlined in this review.

  12. 2-Dimethylamino-1-(2-ethoxy-2-oxoethyl-3-methyl-3,4,5,6-tetrahydropyrimidin-1-ium tetraphenylborate

    Directory of Open Access Journals (Sweden)

    Ioannis Tiritiris


    Full Text Available Isolated guanidinium ions and tetraphenylborate ions are present in the crystal structure of the title compound, C11H22N3O2+·C24H20B−. In the guanidinium ion, the dihedral angle between the N/C/N and C/C/C planes being 49.9 (1°. The six-membered ring exhibits a half-chair conformation. The C—N bond lengths in the cation range between 1.3335 (16 and 1.3552 (16 Å, indicating charge delocalization on the CN3 plane. In the crystal, the cations are connected by C—H...O hydrogen bonds, generating a chain along the c axis.

  13. Preparation of ractopamine-tetraphenylborate complexed nanoparticles used as sensors to rapidly determine ractopamine residues in pork (United States)

    Zhang, Jing; Shao, Xintian; Yue, Jingli; Li, Donghui; Chen, Zhenhua


    In this work, we reported a simple, fast, and sensitive determination of ractopamine (RAC) residues in pork by using novel ractopamine-tetraphenylborate complexed nanoparticles (RT NPs) as sensors. The prepared RT NPs exhibited a fast response time of 10 s, a wide linear range from 0.1 to 1.0 × 10-7 mol/L, and a very low detection limit of 7.4 × 10-8 mol/L. The prepared sensor also presents a high selectivity for ractopamine under different pH conditions ranged from 2.85 to 7.18. These results reveal that the fabricated RT NPs can be used as efficient electrochemical sensors to determine ractopamine in animal productions.

  14. N,N,N′,N′,N′′-Pentamethyl-N′′-[2-(trimethylazaniumylethyl]guanidinium bis(tetraphenylborate acetone monosolvate

    Directory of Open Access Journals (Sweden)

    Ioannis Tiritiris


    Full Text Available The asymmetric unit of the title solvated salt, C11H28N42+·2C24H20B−·C3H6O, comprises two cations, four tetraphenylborate anions and two acetone molecules. One cation shows an orientational disorder at the CN3 moiety and two sets of N-atom positions were found related by a 60° rotation, with a refined occupancy ratio of 0.935 (1:0.065 (1. The respective nitrogen-bonded –CH2 and –CH3 groups are included in the disorder model. The C—N bond lengths in the central CN3 units of both guanidinium ions range between 1.3329 (17 and 1.364 (16 Å, indicating a degree of double-bond character. The central C atom is bonded to the three N atoms in a nearly ideal trigonal–planar geometry and one positive charge is delocalized in the CN3 plane. The C—N bond lengths in the terminal trimethylammonium groups have values close to a typical single bond, and the second positive charge is localized there. In the crystal, the guanidinium ions are connected by C—H...O hydrogen bonds with the acetone molecules. C—H...π interactions are present between the guanidinium and acetone hydrogen atoms and the phenyl rings of the tetraphenylborate ions, leading to the formation of a two-dimensional supramolecular pattern along the bc plane.

  15. Development and process evaluation of improved Fischer-Tropsch slurry catalysts. Sixth quarterly technical progress report, 1 January--31 March 1988

    Energy Technology Data Exchange (ETDEWEB)

    Withers, H.P. [Air Products and Chemicals, Inc., Allentown, PA (United States); Bukur, D.B.; Rosynek, M.P. [Texas A and M Univ., College Station, TX (United States)


    The objective of this contract is to develop a consistent technical data base on the use of iron-based catalysts in Fischer-Tropsch (FT) synthesis reactions. This data base will be developed to allow the unambiguous comparison of the performance of these catalysts with each other and with state-of-the-art iron catalyst comparisons. Particular attention will be devoted to generating reproducible kinetic and selectivity data and to developing reproducible improved catalyst compositions.

  16. Developing catalysts and catalytic processes with industrial relevance. (United States)

    Blaser, Hans-Ulrich


    The catalysis group of Solvias has its roots in the Central Research Laboratories of Ciba-Geigy. Since the early eighties its research has been focused on three areas of catalytic technology: heterogeneous hydrogenation, coupling catalysis, and enantioselective hydrogenation. Today, these are still the catalytic methods with the greatest industrial potential. In this overview a short description will be given how these methods have been developed further since the spin-off of Solvias in 1999. It will be discussed which strategies were successful and what the most important results have been in the first decade of Solvias.

  17. Developing Enzyme and Biomimetic Catalysts for Upgrading Heavy Crudes via Biological Hydrogenation and Hydrodesulfurization

    Energy Technology Data Exchange (ETDEWEB)

    Borole, A P


    The recovery and conversion of heavy oils is limited due to the high viscosity of these crudes and their high heteroatom content. Conventional technology relies on thermochemical hydrogenation and hydrodesulfurization to address these problems and is energy intensive due to the high operating temperature and pressure. This project was initiated to explore biological catalysts for adding hydrogen to the heavy oil molecules. Biological enzymes are efficient at hydrogen splitting at very mild conditions such as room temperature and pressure, however, they are very specific in terms of the substrates they hydrogenate. The goal of the project was to investigate how the specificity of these enzymes can be altered to develop catalysts for oil upgrading. Three approaches were used. First was to perform chemical modification of the enzyme surface to improve binding of other non-natural substrates. Second approach was to expose the deeply buried catalytic active site of the enzyme by removal of protein scaffolding to enable better interaction with other substrates. The third approach was based on molecular biology to develop genetically engineered systems for enabling targeted structural changes in the enzyme. The first approach was found to be limited in success due to the non-specificity of the chemical modification and inability to target the region near the active site or the site of substrate binding. The second approach produced a smaller catalyst capable of catalyzing hydrogen splitting, however, further experimentation is needed to address reproducibility and stability issues. The third approach which targeted cloning of hydrogenase in alternate hosts demonstrated progress, although further work is necessary to complete the cloning process. The complex nature of the hydrogenase enzyme structure-function relationship and role of various ligands in the protein require significant more research to better understand the enzyme and to enable success in strategies in

  18. Development of active, and stable water-gas-shift reaction catalysts for fuel cell applications

    NARCIS (Netherlands)

    Azzam, K.G.H.; Babich, Igor V.; Seshan, Kulathu Iyer; Lefferts, Leon


    Water-gas-shift (WGS) reaction CO + H2O = CO2 + H2, is a key step in the generation of H2 for fuel cells. Noble metal-based catalysts are promising single stage WGS catalysts because they less sensitive than LTS catalysts (Cu based) and more active than the HTS (Ni) catalysts. High activity in CO

  19. Carbon monoxide oxidation over three different states of copper: Development of a model metal oxide catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Jernigan, Glenn Geoffrey [California Univ., Berkeley, CA (United States). Dept. of Chemistry


    Carbon monoxide oxidation was performed over the three different oxidation states of copper -- metallic (Cu), copper (I) oxide (Cu2O), and copper (II) oxide (CuO) as a test case for developing a model metal oxide catalyst amenable to study by the methods of modern surface science and catalysis. Copper was deposited and oxidized on oxidized supports of aluminum, silicon, molybdenum, tantalum, stainless steel, and iron as well as on graphite. The catalytic activity was found to decrease with increasing oxidation state (Cu > Cu2O > CuO) and the activation energy increased with increasing oxidation state (Cu, 9 kcal/mol < Cu2O, 14 kcal/mol < CuO, 17 kcal/mol). Reaction mechanisms were determined for the different oxidation states. Lastly, NO reduction by CO was studied. A Cu and CuO catalyst were exposed to an equal mixture of CO and NO at 300--350 C to observe the production of N2 and CO2. At the end of each reaction, the catalyst was found to be Cu2O. There is a need to study the kinetics of this reaction over the different oxidation states of copper.

  20. Development of Pd-Cu/hematite catalyst for selective nitrate reduction. (United States)

    Jung, Sungyoon; Bae, Sungjun; Lee, Woojin


    A new hematite-supported Pd-Cu bimetallic catalyst (Pd-Cu/hematite) was developed in order to actively and selectively reduce nitrate (NO3(-)) to nitrogen gas (N2). Four different iron-bearing soil minerals (hematite (H), goethite (G), maghemite (M), and lepidocrocite (L)) were transformed to hematite by calcination and used for synthesis of different Pd-Cu/hematite-H, G, M, and L catalysts. Their characteristics were identified using X-ray diffraction (XRD), specific surface area (BET), temperature programed reduction (TPR), transmission electron microscopy with energy dispersive X-ray (TEM-EDX), H2 pulse chemisorption, zeta-potential, and X-ray photoelectron spectroscopy (XPS). Pd-Cu/hematite-H exhibited the highest NO3(-) removal (96.4%) after 90 min, while a lower removal (90.9, 51.1, and 30.5%) was observed in Pd-Cu/hematite-G, M, and L, respectively. The results of TEM-EDX, and TPR analysis revealed that Pd-Cu/hematite-H possessed the closest contact distance between the Cu and Pd sites on the hematite surface among the different Pd-Cu/hematite catalysts. The high removal can be also attributed to the highly active metallic sites on its positively charged surface. The XPS analysis demonstrated that the amount of hydrogen molecules can have a pivotal function on NO3(-) removal and a ratio of nitrogen to hydrogen molecule (N:H) on the Pd sites can critically determine N2 selectivity.

  1. Development of large aperture projection scatterometry for catalyst loading evaluation in proton exchange membrane fuel cells (United States)

    Stocker, Michael T.; Barnes, Bryan M.; Sohn, Martin; Stanfield, Eric; Silver, Richard M.


    Widespread commercialization of proton exchange membrane fuel cells remains curbed by various manufacturing and infrastructure challenges. One such technical barrier identified by the U. S. Department of Energy is the need for high-speed, in-line process control of platinum-based catalyst layers in the membrane electrode assembly of the fuel cell. Using multiple reflectivity-based optical methods, such as optical scatterometry and large aperture projection scatterometry, we demonstrate in-line-capable catalyst loading measurements of carbon-supported Pt nanoparticle and Pt-alloy nanostructured thin film catalyst coated membranes. Large aperture projection scatterometry is a new high-throughput approach developed at the National Institute of Standards and Technology specifically for fuel cell manufacturing metrology. Angle- and wavelength-resolved measurements of these fuel cell soft goods validate the ability of reflectivity-based measurements to produce industrially relevant sensitivities to changes in Pt and Pt-alloy loading. The successful application of these optical methods to fuel cell manufacturing metrology directly addresses the shortage of high-throughput process control approaches needed to facilitate performance improvements and manufacturing cost-reductions required to make fuel cells commercially viable.

  2. Development of Hydrotalcite Based Cobalt Catalyst by Hydrothermal and Co-precipitation Method for Fischer-Tropsch Synthesis

    Directory of Open Access Journals (Sweden)

    Muhammad Faizan Shareef


    Full Text Available This paper presents the effect of a synthesis method for cobalt catalyst supported on hydrotalcite material for Fischer-Tropsch synthesis. The hydrotalcite supported cobalt (HT-Co catalysts were synthesized by co-precipitation and hydrothermal method. The prepared catalysts were characterized by using various techniques like BET (Brunauer–Emmett–Teller, SEM (Scanning Electron Microscopy, TGA (Thermal Gravimetric Analysis, XRD (X-ray diffraction spectroscopy, and FTIR (Fourier Transform Infrared Spectroscopy. Fixed bed micro reactor was used to test the catalytic activity of prepared catalysts. The catalytic testing results demonstrated the performance of hydrotalcite based cobalt catalyst in Fischer-Tropsch synthesis with high selectivity for liquid products. The effect of synthesis method on the activity and selectivity of catalyst was also discussed. Copyright © 2017 BCREC Group. All rights reserved Received: 3rd November 2016; Revised: 26th February 2017; Accepted: 9th March 2017; Available online: 27th October 2017; Published regularly: December 2017 How to Cite: Sharif, M.S., Arslan, M., Iqbal, N., Ahmad, N., Noor, T. (2017. Development of Hydrotalcite Based Cobalt Catalyst by Hydrothermal and Co-precipitation Method for Fischer-Tropsch Synthesis. Bulletin of Chemical Reaction Engineering & Catalysis, 12(3: 357-363 (doi:10.9767/bcrec.12.3.762.357-363

  3. Catalyst Architecture

    DEFF Research Database (Denmark)

    Kiib, Hans; Marling, Gitte; Hansen, Peter Mandal


    How can architecture promote the enriching experiences of the tolerant, the democratic, and the learning city - a city worth living in, worth supporting and worth investing in? Catalyst Architecture comprises architectural projects, which, by virtue of their location, context and their combination...... of programs, have a role in mediating positive social and/or cultural development. In this sense, we talk about architecture as a catalyst for: sustainable adaptation of the city’s infrastructure appropriate renovation of dilapidated urban districts strengthening of social cohesiveness in the city development...

  4. Technology development for iron Fischer-Tropsch catalysts. Technical progress report No. 4, June 26, 1991--September 26, 1991

    Energy Technology Data Exchange (ETDEWEB)

    Frame, R.R.


    Objectives are to develop active, stable iron Fischer-Tropsch catalysts for use in slurry-phase synthesis reactors and to develop a scaleup procedure for large-scale synthesis of such catalysts for process development and long-term testing in slurry bubble-column reactors. For a H{sub 2}-CO in molar ratio of 0.5 to 1.0, catalyst performance target is 88% CO+H{sub 2} conversion at a minimum space velocity of 2.4 NL/hr/gFe, with no more than 4% methane/ethane selectivity and 1% conversion loss per week. During this period, it was found that the performance of the slurry-phase iron and copper oxide-based catalyst depends on the amount of K. Five catalysts with differing K contents were studied. The catalysts with the lowest K were more active than the ones with higher K levels. The one with the middle K level was judged best.

  5. N,N,N′,N′-Tetramethyl-N′′-[3-(trimethylazaniumylpropyl]guanidinium bis(tetraphenylborate acetone disolvate

    Directory of Open Access Journals (Sweden)

    Ioannis Tiritiris


    Full Text Available In the title solvated salt, C11H28N42+·2C24H20B−·2C3H6O, the C—N bond lengths in the central CN3 unit of the guanidinium ion are 1.3331 (16, 1.3407 (16 and 1.3454 (16 Å, indicating partial double-bond character in each. The central C atom is bonded to the three N atoms in a nearly ideal trigonal–planar geometry [N—C—N angles = 118.96 (11, 120.51 (12 and 120.53 (11°] and the positive charge is delocalized in the CN3 plane. The bonds between the N atoms and the terminal C-methyl groups of the guanidinium moiety all have values close to a typical single bond [1.4601 (16–1.4649 (16 Å]. In the crystal, the guanidinium ion is connected by N—H...O and C—H...O hydrogen bonds with the acetone molecules. C—H...π interactions are present between the guanidinium H atoms and the phenyl rings of both tetraphenylborate ions. The phenyl rings form aromatic pockets, in which the guanidinium ions are embedded.

  6. Development of vanadium-phosphate catalysts for methanol production by selective oxidation of methane

    Energy Technology Data Exchange (ETDEWEB)

    McCormick, R.L. [Colorado School of Mines, Golden, CO (United States)


    The United States has vast natural gas reserves which could contribute significantly to our energy security if economical technologies for conversion to liquid fuels and chemicals were developed. Many of these reserves are small scale or in remote locations and of little value unless they can be transported to consumers. Transportation is economically performed via pipeline, but this route is usually unavailable in remote locations. Another option is to convert the methane in the gas to liquid hydrocarbons, such as methanol, which can easily and economically be transported by truck. Therefore, the conversion of methane to liquid hydrocarbons has the potential to decrease our dependence upon oil imports by opening new markets for natural gas and increasing its use in the transportation and chemical sectors of the economy. In this project, we are attempting to develop, and explore new catalysts capable of direct oxidation of methane to methanol. The specific objectives of this work are discussed.

  7. Oxidation catalyst (United States)

    Ceyer, Sylvia T.; Lahr, David L.


    The present invention generally relates to catalyst systems and methods for oxidation of carbon monoxide. The invention involves catalyst compositions which may be advantageously altered by, for example, modification of the catalyst surface to enhance catalyst performance. Catalyst systems of the present invention may be capable of performing the oxidation of carbon monoxide at relatively lower temperatures (e.g., 200 K and below) and at relatively higher reaction rates than known catalysts. Additionally, catalyst systems disclosed herein may be substantially lower in cost than current commercial catalysts. Such catalyst systems may be useful in, for example, catalytic converters, fuel cells, sensors, and the like.

  8. Combinatorial Development of Water Splitting Catalysts Based on the Oxygen Evolving Complex of Photosystem II

    Energy Technology Data Exchange (ETDEWEB)

    Woodbury, Neal [Arizona State University


    The use of methods to create large arrays of potential catalysts for the reaction H2O ½ O2 + 2H+ on the anode of an electrolysis system were investigated. This reaction is half of the overall reaction involved in the splitting of water into hydrogen and oxygen gas. This method consisted of starting with an array of electrodes and developing patterned electrochemical approaches for creating a different, defined peptide at each position in the array. Methods were also developed for measuring the rate of reaction at each point in the array. In this way, the goal was to create and then tests many thousands of possible catalysts simultaneously. This type of approach should lead to an ability to optimize catalytic activity systematically, by iteratively designing and testing new libraries of catalysts. Optimization is important to decrease energy losses (over-potentials) associated with the water splitting reaction and thus for the generation of hydrogen. Most of the efforts in this grant period were focused on developing the chemistry and analytical methods required to create pattern peptide formation either using a photolithography approach or an electrochemical approach for dictating the positions of peptide bond formation. This involved testing a large number of different reactions and conditions. We have been able to find conditions that have allowed us to pattern peptide bond formation on both glass slides using photolithographic methods and on electrode arrays made by the company Combimatrix. Part of this effort involved generating novel approaches for performing mass spectroscopy directly from the patterned arrays. We have also been able to demonstrate the ability to measure current at each electrode due to electrolysis of water. This was performed with customized instrumentation created in collaboration with Combimatrix. In addition, several different molecular designs for peptides that bound metals (primarily Mn) were developed and synthesized and metal

  9. Enantioselective Decarboxylative Alkylation Reactions: Catalyst Development, Substrate Scope, and Mechanistic Studies

    KAUST Repository

    Behenna, Douglas C.


    α-Quaternary ketones are accessed through novel enantioselective alkylations of allyl and propargyl electrophiles by unstabilized prochiral enolate nucleophiles in the presence of palladium complexes with various phosphinooxazoline (PHOX) ligands. Excellent yields and high enantiomeric excesses are obtained from three classes of enolate precursor: enol carbonates, enol silanes, and racemic β-ketoesters. Each of these substrate classes functions with nearly identical efficiency in terms of yield and enantioselectivity. Catalyst discovery and development, the optimization of reaction conditions, the exploration of reaction scope, and applications in target-directed synthesis are reported. Experimental observations suggest that these alkylation reactions occur through an unusual inner-sphere mechanism involving binding of the prochiral enolate nucleophile directly to the palladium center.

  10. Development of an azanoradamantane-type nitroxyl radical catalyst for class-selective oxidation of alcohols. (United States)

    Doi, Ryusuke; Shibuya, Masatoshi; Murayama, Tsukasa; Yamamoto, Yoshihiko; Iwabuchi, Yoshiharu


    The development of 1,5-dimethyl-9-azanoradamantane N-oxyl (DMN-AZADO; 1,5-dimethyl-Nor-AZADO, 2) as an efficient catalyst for the selective oxidation of primary alcohols in the presence of secondary alcohols is described. The compact and rigid structure of the azanoradamantane nucleus confers potent catalytic ability to DMN-AZADO (2). A variety of hindered primary alcohols such as neopentyl primary alcohols were efficiently oxidized by DMN-AZADO (2) to the corresponding aldehydes, whereas secondary alcohols remained intact. DMN-AZADO (2) also has high catalytic efficiency for one-pot oxidation from primary alcohols to the corresponding carboxylic acids in the presence of secondary alcohols and for oxidative lactonization from diols.

  11. Downstream, catalyst companies ally with gas-to-liquids process developer

    Energy Technology Data Exchange (ETDEWEB)

    Rhodes, A.K.


    Texaco Natural Gas, Houston, and Syntroleum Corp., Tulsa, have struck two agreements regarding Syntroleum`s modified Fischer-Tropsch (F-T) process for producing fuels from natural gas. The first, a nonexclusive master license agreement, grants Texaco broad rights to use the process, according to Syntroleum. The companies also have agreed to work jointly to accelerate development of cost-savings improvements to Syntroleum`s synthetic fuels process. Product yields and qualities have been confirmed in large-scale pilot plant studies using the Criterion catalyst. Syntroleum`s 2 b/d pilot plant has been operating since 1990. The paper discusses gas-to-liquids processes, economics, the Syntroleum process modifications, and synthetic lubricants.

  12. Liquid phase methanol LaPorte process development unit: Modification operation, and support studies. Task 3.6/3.7: Alternative catalyst/life run

    Energy Technology Data Exchange (ETDEWEB)


    In April 1987, Air Products started the third and final contract with the US Department of Energy to develop the Liquid Phase Methanol (LPMEOH) process. One of the objectives was to identify alternative commercial catalyst(s) for the process. This objective was strategically important as we want to demonstrate that the LPMEOH process is flexible and not catalyst selection limited. Among three commercially available catalysts evaluated in the lab, the catalyst with a designation of F21/0E75-43 was the most promising candidate. The initial judging criteria included not only the intrinsic catalyst activity but also the ability to be used effectively in a slurry reactor. The catalyst was then advanced for a 40-day life test in a laboratory 300 cc autoclave. The life test result also revealed superior stability when compared with that of a standard catalyst. Consequently, the new catalyst was recommended for demonstration in the Process Development Unit (PDU) at LaPorte, Texas. This report details the methodology of testing and selecting the catalyst.

  13. Spectroscopic and structural elucidation of merocyanine dye 2,5-[1-metyl-4-[2-(4-hydroxyphenyl)ethenyl)]piridinium]-hexane tetraphenylborate. Aggregation processes (United States)

    Koleva, Bojidarka B.; Stoyanov, Stanimir; Kolev, Tsonko; Petkov, Ivan; Spiteller, Michael


    Structural and spectroscopic elucidation of merocyanine dye, 2,5-[1-metyl-4-[2-(4-hydroxyphenyl)ethenyl)]piridinium]-hexane tetraphenylborate, is performed in gas and condense phase by means of solution and solid-state conventional and linear-polarized IR-spectroscopy of oriented colloids in nematic liquid crystal suspension, UV-vis and fluorescence methods, HPLC MS/MS tandem and ESI mass spectrometry, 1H, 13C and 1H- 1H COSY NMR, TGV and DSC methods. Quantum chemical DFT calculations are performed for structural optimization and spectroscopic properties prediction.

  14. Design of heterogeneous catalysts

    DEFF Research Database (Denmark)

    Frey, Anne Mette

    was inspired by a computational screening, suggesting that alloys such as Ni-Fe, Co-Ni, and Co-Fe should show superior activity to the industrially used nickel catalyst. Especially the Ni-Fe system was considered to be interesting, since such alloy catalysts should be both more active and cheaper than the Ni....... Previously it has been shown that calcination of cobalt catalyst in a NO/He mixture resulted in improved catalytic activity compared to standard air calcined samples, since more homogenous cobalt particles with a narrow particle size distribution were formed. Unfortunately the C5+ selectivity decreased...... well, and the best catalyst prepared had a C5+ yield almost a factor of two higher than a standard air calcined Co catalyst. In the NH3-SCR reaction it is desirable to develop an active and stable catalyst for NOx removal in automotive applications, since the traditionally used vanadium-based catalyst...

  15. Coal catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Kroenig, W.


    Some considerations in the selection of a catalyst for the liquid phase of coal hydrogenation are discussed. Some of the previous history of such selections is mentioned. At one stage of the development, the principal catalyst had been iron sulfate (FeSO/sub 4/.7H/sub 2/O). Later, for reasons of cost and availability of large supplies, selections had turned to mixtures of iron sulfate and one or another of some iron oxide- and aluminum oxide-containing byproducts of aluminum manufacture, namely Bayermasse, Luxamsse, or Lautamasse. Much of the discussion centered on optimal proportions for such mixtures, particularly as related to pH values of resulting coal pastes. Upper Silesian coal was more alkaline than Ruhr coal, and Bayermasse, etc., were quite alkaline. Thus, since the iron sulfate served as a partial neutralizer for the coal as well as a catalyst, it seemed necessary to increase the proportions of iron sulfate in the catalyst mixture when processing coal of greater alkalinity. A further reason for a greater proportion of iron sulfate seemed to be that most of the catalytic activity of the iron came from the ferrous iron of iron sulfate rather than from the ferric iron of the other materials. Ferrous-ferric ratios also seemed to indicate that Luxmasse or Lautamasse might be better catalyst components than Bayermasse but their water content sometimes caused handling problems, so Bayermasse had been more widely used. Formation of deposits in the preheater was more likely due to the Bayermasse than to the iron sulfate; sodium sulfide could help to prevent them.

  16. Alkali promoted molybdenum (IV) sulfide based catalysts, development and characterization for alcohol synthesis from carbon monoxide and hydrogen (United States)

    Molina, Belinda Delilah

    For more than a century transition metal sulfides (TMS) have been the anchor of hydro-processing fuels and upgrading bitumen and coal in refineries worldwide. As oil supplies dwindle and environmental laws become more stringent, there is a greater need for cleaner alternative fuels and/or synthetic fuels. The depletion of oil reserves and a rapidly increasing energy demand worldwide, together with the interest to reduce dependence on foreign oil makes alcohol production for fuels and chemicals via the Fischer Tropsch synthesis (FTS) very attractive. The original Fischer-Tropsch (FT) reaction is the heart of all gas-to-liquid technologies; it creates higher alcohols and hydrocarbons from CO/H2 using a metal catalyst. This research focuses on the development of alkali promoted MoS2-based catalysts to investigate an optimal synthesis for their assistance in the production of long chain alcohols (via FTS) for their use as synthetic transportation liquid fuels. Properties of catalytic material are strongly affected by every step of the preparation together with the quality of the raw materials. The choice of a laboratory method for preparing a given catalyst depends on the physical and chemical characteristics desired in the final composition. Characterization methods of K0.3/Cs0.3-MoS2 and K0.3 /Cs0.3-Co0.5MoS2 catalysts have been carried out through Scanning Electron Microscopy (SEM), BET porosity and surface analysis, Transmission Electron Microscopy (TEM) and X-Ray Diffraction (XRD). Various characterization methods have been deployed to correlate FTS products versus crystal and morphological properties of these heterogeneous catalysts. A lab scale gas to liquid system has been developed to evaluate its efficiency in testing FT catalysts for their production of alcohols.

  17. Development of a Practical Hydrogen Storage System Based on Liquid Organic Hydrogen Carriers and a Homogeneous Catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Jensen, Craig [Hawaii Hydrogen Carriers, LLC, Honolulu, HI (United States); Brayton, Daniel [Hawaii Hydrogen Carriers, LLC, Honolulu, HI (United States); Jorgensen, Scott W. [General Motors, LLC, Warren, MI (United States). Research and Development Center. Chemical and Material Systems Lab.; Hou, Peter [General Motors, LLC, Warren, MI (United States). Research and Development Center. Chemical and Material Systems Lab.


    The objectives of this project were: 1) optimize a hydrogen storage media based on LOC/homogeneous pincer catalyst (carried out at Hawaii Hydrogen Carriers, LLC) and 2) develop space, mass and energy efficient tank and reactor system to house and release hydrogen from the media (carried out at General Motor Research Center).

  18. Preparation of Fe2O3-Clorprenaline/Tetraphenylborate Nanospheres and Their Application as Ion Selective Electrode for Determination of Clorprenaline in Pork (United States)

    Shao, Xintian; Zhang, Jing; Li, Donghui; Yue, Jingli; Chen, Zhenhua


    A novel modified ion selective electrode based on Fe2O3-clorprenaline/tetraphenylborate nanospheres (Fe2O3-CLPT NSs) as electroactive materials for the determination of clorprenaline hydrochloride (CLP) is described. The α-Fe2O3 nanoparticles (NPs) were prepared by hydrothermal synthesis, then self-assembled on CLP/tetraphenylborate (TPB) to form Fe2O3-CLPT NSs, which were used as a potentiometric electrode for analyte determination innovatively. The Fe2O3-CLPT NSs modified electrode exhibited a wider concentration range from 1.0 × 10-7 to 1.0 × 10-1 mol/L and a lower detection limit of 3.7 × 10-8 mol/L compared with unmodified electrodes. The selectivity of the modified electrode was evaluated by fixed interference method. The good performance of the modified electrode such as wide pH range (2.4-6.7), fast response time (15 s), and adequate lifetime (14 weeks) indicate the utility of the modified electrode for evaluation of CLP content in various real samples. Finally, the modified electrode was successfully employed to detect CLP in pork samples with satisfactory results. These results demonstrated the Fe2O3-CLPT NSs modified electrode to be a functional and convenient method to the field of potentiometry determination of CLP in real samples.

  19. Catalyst Alloys Processing (United States)

    Tan, Xincai


    Catalysts are one of the key materials used for diamond formation at high pressures. Several such catalyst products have been developed and applied in China and around the world. The catalyst alloy most widely used in China is Ni70Mn25Co5 developed at Changsha Research Institute of Mining and Metallurgy. In this article, detailed techniques for manufacturing such a typical catalyst alloy will be reviewed. The characteristics of the alloy will be described. Detailed processing of the alloy will be presented, including remelting and casting, hot rolling, annealing, surface treatment, cold rolling, blanking, finishing, packaging, and waste treatment. An example use of the catalyst alloy will also be given. Industrial experience shows that for the catalyst alloy products, a vacuum induction remelt furnace can be used for remelting, a metal mold can be used for casting, hot and cold rolling can be used for forming, and acid pickling can be used for metal surface cleaning.

  20. New catalyst developed at Argonne National Laboratory could help diesels meet NOx deadlines

    CERN Multimedia


    "A new catalyst could help auto makers meet the U.S. Environmental Protection Agency's deadline to eliminate 95 percent of nitrogen-oxide from diesel engine exhausts by 2007, while saving energy" (1 page).


    Directory of Open Access Journals (Sweden)

    O. S. Komarov


    Full Text Available The technology of processing of copper-bearing dead catalysts, which includes leaching and deposition of copper by means of electrolysis and also their application in composition of the mixture for alloy doping is offered.

  2. Brief Communication: CATALYST - a multi-regional stakeholder Think Tank for fostering capacity development in disaster risk reduction and climate change adaptation

    NARCIS (Netherlands)

    Terwisscha van Scheltinga, C.T.H.M.; Hare, M.P.; Bers, van C.; Keur, van der P.


    This brief communication presents the work and objectives of the CATALYST project on "Capacity Development for Hazard Risk Reduction and Adaptation" funded by the European Commission (October 2011–September 2013). CATALYST set up a multi-regional think tank covering four regions (Central America and

  3. Development of biomimetic catalytic oxidation methods and non-salt methods using transition metal-based acid and base ambiphilic catalysts (United States)

    MURAHASHI, Shun-Ichi


    This review focuses on the development of ruthenium and flavin catalysts for environmentally benign oxidation reactions based on mimicking the functions of cytochrome P-450 and flavoenzymes, and low valent transition-metal catalysts that replace conventional acids and bases. Several new concepts and new types of catalytic reactions based on these concepts are described. PMID:21558760

  4. Development of biomimetic catalytic oxidation methods and non-salt methods using transition metal-based acid and base ambiphilic catalysts. (United States)

    Murahashi, Shun-Ichi


    This review focuses on the development of ruthenium and flavin catalysts for environmentally benign oxidation reactions based on mimicking the functions of cytochrome P-450 and flavoenzymes, and low valent transition-metal catalysts that replace conventional acids and bases. Several new concepts and new types of catalytic reactions based on these concepts are described. (Communicated by Ryoji Noyori, M.J.A.).

  5. In-situ characterization of heterogeneous catalysts

    CERN Document Server

    Rodriguez, Jose A; Chupas, Peter J


    Helps researchers develop new catalysts for sustainable fuel and chemical production Reviewing the latest developments in the field, this book explores the in-situ characterization of heterogeneous catalysts, enabling readers to take full advantage of the sophisticated techniques used to study heterogeneous catalysts and reaction mechanisms. In using these techniques, readers can learn to improve the selectivity and the performance of catalysts and how to prepare catalysts as efficiently as possible, with minimum waste. In-situ Characterization of Heterogeneous Catalysts feat

  6. Visible-Light-Responsive Photocatalysis: Ag-Doped TiO2 Catalyst Development and Reactor Design Testing (United States)

    Coutts, Janelle L.; Hintze, Paul E.; Meier, Anne; Shah, Malay G.; Devor, Robert W.; Surma, Jan M.; Maloney, Phillip R.; Bauer, Brint M.; Mazyck, David W.


    In recent years, the alteration of titanium dioxide to become visible-light-responsive (VLR) has been a major focus in the field of photocatalysis. Currently, bare titanium dioxide requires ultraviolet light for activation due to its band gap energy of 3.2 eV. Hg-vapor fluorescent light sources are used in photocatalytic oxidation (PCO) reactors to provide adequate levels of ultraviolet light for catalyst activation; these mercury-containing lamps, however, hinder the use of this PCO technology in a spaceflight environment due to concerns over crew Hg exposure. VLR-TiO2 would allow for use of ambient visible solar radiation or highly efficient visible wavelength LEDs, both of which would make PCO approaches more efficient, flexible, economical, and safe. Over the past three years, Kennedy Space Center has developed a VLR Ag-doped TiO2 catalyst with a band gap of 2.72 eV and promising photocatalytic activity. Catalyst immobilization techniques, including incorporation of the catalyst into a sorbent material, were examined. Extensive modeling of a reactor test bed mimicking air duct work with throughput similar to that seen on the International Space Station was completed to determine optimal reactor design. A bench-scale reactor with the novel catalyst and high-efficiency blue LEDs was challenged with several common volatile organic compounds (VOCs) found in ISS cabin air to evaluate the system's ability to perform high-throughput trace contaminant removal. The ultimate goal for this testing was to determine if the unit would be useful in pre-heat exchanger operations to lessen condensed VOCs in recovered water thus lowering the burden of VOC removal for water purification systems.

  7. Catalysts and process developments for two-stage liquefaction. Final technical report, October 1, 1989--September 30, 1992

    Energy Technology Data Exchange (ETDEWEB)

    Cronauer, D.C.; Swanson, A.J.; Sajkowski, D.J.


    Research in this project centered upon developing and evaluating catalysts and process improvements for coal liquefaction in the two-stage, close-coupled catalytic process. The major results are summarized here and they are described in more detail under each Task. In tasks for coal pretreatment and beneficiation, it was shown for coal handling that drying of both lignite or subbituminous coals using warm air, vacuum oven or exposing to air for long time was detrimental to subsequent liquefaction. Both laboratory and bench-scale beneficiations indicated that in order to achieve increased liquefaction yield for Illinois No. 6 bituminous coal, size separation with in sink-float technique should be used. For subbituminous coal, the best beneficiation was aqueous SO{sub 2} treatment, which reduced mineral matter. In the case of lignite, the fines should be rejected prior to aqueous SO{sub 2} treatment and sink-float gravity separation. In liquefying coals with supported catalysts in both first and second stages, coal conversion was highest (93%) with Illinois No. 6 coal, which also had the highest total liquid yield of 80%, however, the product contained unacceptably high level of resid (30%). Both low rank coals gave lower conversion (85--87%) and liquid yields (57--59%), but lighter products (no resid). The analysis of spent first stage catalysts indicated significant sodium and calcium deposits causing severe deactivation. The second stage catalysts were in better condition showing high surface areas and low coke and metal deposits. The use of dispersed catalyst in the first stage would combat the severe deactivation.

  8. Current status, key challenges and its solutions in the design and development of graphene based ORR catalysts for the microbial fuel cell applications. (United States)

    Kannan, M V; Gnana Kumar, G


    Microbial fuel cells (MFC) are considered as the futuristic energy device that generates electricity from the catalytic degradation of biodegradable organic wastes using microbes, which exist in waste water. In MFCs, oxygen serves as a cathodic electron acceptor and oxygen reduction kinetics played a significant role in the determination of overall efficiency. A wide range of strategies have been developed for the preparation and substantial modification of oxygen reduction reaction (ORR) catalysts to improve the maximum volumetric power density of MFCs, in which the efforts on graphene based ORR catalysts are highly imperative. Although numerous research endeavors have been achieved in relation with the graphene based ORR catalysts applicable for MFCs, still their collective summary has not been developed, which hinders the acquirement of adequate knowledge on tuning the specific properties of said catalysts. The intension of this review is to outline the significant role of ORR catalysts, factors influencing the ORR activity, strategies behind the modifications of ORR catalysts and update the research efforts devoted on graphene based ORR catalysts. This review can be considered as a pertinent guide to understand the design and developmental strategies of competent graphene based ORR catalysts, which are not only applicable for MFCs but also for number of electrochemical applications. Copyright © 2015 Elsevier B.V. All rights reserved.

  9. Development and integration of a LabVIEW-based modular architecture for automated execution of electrochemical catalyst testing. (United States)

    Topalov, Angel A; Katsounaros, Ioannis; Meier, Josef C; Klemm, Sebastian O; Mayrhofer, Karl J J


    This paper describes a system for performing electrochemical catalyst testing where all hardware components are controlled simultaneously using a single LabVIEW-based software application. The software that we developed can be operated in both manual mode for exploratory investigations and automatic mode for routine measurements, by using predefined execution procedures. The latter enables the execution of high-throughput or combinatorial investigations, which decrease substantially the time and cost for catalyst testing. The software was constructed using a modular architecture which simplifies the modification or extension of the system, depending on future needs. The system was tested by performing stability tests of commercial fuel cell electrocatalysts, and the advantages of the developed system are discussed. © 2011 American Institute of Physics

  10. Polyoxometalate catalysts: toward the development of green H2O2-based epoxidation systems. (United States)

    Mizuno, Noritaka; Yamaguchi, Kazuya


    This paper describes the development of green, efficient H(2)O(2)-based epoxidation systems with three kinds of polyoxometalates: (i) a dinuclear peroxotungstate [W(2)O(3)(O(2))(4)(H(2)O)(2)](2-) (I), (ii) a divacant lacunary polyoxotungstate [gamma-SiW(10)O(34)(H(2)O)(2)]4 (II), (iii) and a divanadium-substituted polyoxotungstate [gamma-1,2-H(2)SiV(2)W(10)O(40)](4-) (III). The highly chemo-, regio-, and diastereoselective epoxidation of various allylic alcohols with only 1 equiv H(2)O(2) in water can be efficiently catalyzed by potassium salt of I (K-I). The catalyst K-I can be recycled with the retention of the catalytic performance. Protonation of a divacant lacunary polyoxotungstate [gamma-SiW(10)O(36)](8-) gives [gamma-SiW(10)O(34)(H(2)O)(2)](4-) (II) with two aquo ligands. The tetra-n-butylammonium salt of II (TBA-II) catalyzes epoxidation of common olefins including propylene with >or=99% selectivity to epoxide and >or=99% efficiency of H(2)O(2) utilization. The bis(mu-hydroxo)bridged dioxovanadium site in [gamma-1,2-H(2)SiV(2)W(10)O(40)](4-) (III) can also efficiently catalyze epoxidation of a variety of olefins with 1 equiv H(2)O(2). Notably, the system with III shows unique stereospecificity, diastereoselectivity, and regioselectivity for the epoxidation of cis/trans olefins, 3-substituted cyclohexenes, and nonconjugated dienes, respectively, which are quite different from those reported for epoxidation systems up to now. Furthermore, the heterogenization of the mentioned polyoxometalates can be achieved by using ionic liquid-modified SiO(2) as a support without loss of catalytic performance. (c) 2006 The Japan Chemical Journal Forum and Wiley Periodicals, Inc.

  11. Enhancement of Treatment Efficiency of Recalcitrant Wastewater Containing Textile Dyes Using a Newly Developed Iron Zeolite Socony Mobil-5 Heterogeneous Catalyst. (United States)

    Ahmad, Mushtaq; Asghar, Anam; Abdul Raman, Abdul Aziz; Wan Daud, Wan Mohd Ashri


    Fenton oxidation, an advanced oxidation process, is an efficient method for the treatment of recalcitrant wastewaters. Unfortunately, it utilizes H2O2 and iron-based homogeneous catalysts, which lead to the formation of high volumes of sludge and secondary pollutants. To overcome these problems, an alternate option is the usage of heterogeneous catalyst. In this study, a heterogeneous catalyst was developed to provide an alternative solution for homogeneous Fenton oxidation. Iron Zeolite Socony Mobile-5 (Fe-ZSM-5) was synthesized using a new two-step process. Next, the catalyst was characterized by scanning electron microscopy, energy-dispersive X-ray spectroscopy, fourier transform infrared spectroscopy, and Brunauer-Emmett-Teller analysis and tested against a model wastewater containing the azo dye Acid Blue 113. Results showed that the loading of iron particles reduced the surface area of the catalyst from 293.59 to 243.93 m2/g; meanwhile, the average particle size of the loaded material was 12.29 nm. Furthermore, efficiency of the developed catalyst was evaluated by performing heterogeneous Fenton oxidation. Taguchi method was coupled with principal component analysis in order to assess and optimize mineralization efficiency. Experimental results showed that under optimized conditions, over 99.7% degradation and 77% mineralization was obtained, with a 90% reduction in the consumption of the developed catalyst. Furthermore, the developed catalyst was stable and reusable, with less than 2% leaching observed under optimized conditions. Thus, the present study proved that newly developed catalyst has enhanced the oxidation process and reduced the chemicals consumption.

  12. Development of precipitated iron Fischer-Tropsch catalysts. Quarterly technical progress report, 1 April 1996--30 June 1996

    Energy Technology Data Exchange (ETDEWEB)

    Bukur, D.B.; Lang, X.; Ding, Y.; Chokkaram, S.


    The overall contract objectives are to: (1) demonstrate repeatability of performance and preparation procedure of two high activity, high alpha iron Fischer-Tropsch catalysts synthesized at Texas A&M University (TAMU) during the DOE Contract DE-AC22-89PC89868; (2) seek potential improvements in the catalyst performance through variations in process conditions, pretreatment procedures and/or modifications in catalyst synthesis; (3) investigate performance of catalysts in a small scale bubble column slurry reactor, and (4) investigate feasibility of producing catalysts on a large scale in collaboration with a catalyst manufacturer. The performance of an iron, and iron-copper-silica catalyst are described.

  13. (Naphthalene-2,3-diolato-κ2O,O′[tris(pyridin-2-ylmethylamine-κ4N]cobalt(III tetraphenylborate acetone monosolvate hemihydrate

    Directory of Open Access Journals (Sweden)

    Fan Yu


    Full Text Available In the title salt, [Co(C10H6O2(C18H18N4](C24H20B·C3H6O·0.5H2O, the CoIII ion in the complex cation is six-coordinated in a rigid octahedral N4O2 geometry. The asymmetric unit contains one complete [Co(C10H6O2(C18H18N4]+ unit, one tetraphenylborate counter-anion and one acetone and one water molecule that is located on an inversion centre. All the features of the CoIII ion are fully consistent with the formulation of the cation as a Co3+–catecholate complex. Variable-temperature magnetic measurements in the region 2–380 K show a obvious diamagnetism over the observed temperature range.

  14. Crystal structure of di-μ-aqua-μ-(pyrazine N,N′-dioxide-κ2O:O-bis(diaquasodium tetraphenylborate dihydrate pyrazine N,N′-dioxide monosolvate

    Directory of Open Access Journals (Sweden)

    Elaine P. Boron


    Full Text Available The search for novel lanthanide coordination networks using pyrazine N,N′-dioxide (pzdo, C4H4N2O2 as a structure-directing unit, led to the synthesis and the structure determination of the title compound, [Na2(C4H4N2O2(H2O6][B(C6H54]2·C4H4N2O2·2H2O. The crystal structure is comprised of discrete [{Na(H2O2}2(μ-H2O2(μ-pzdo]2+ cations and tetraphenylborate anions, as well as pzdo and H2O solvent molecules. The dinuclear cation is located about a twofold rotation axis, and the symmetry-related NaI atoms display a distorted square-pyramidal coordination sphere defined by two O atoms of terminal water ligands, two O atoms of bridging water ligands and one O atom of a bridging pzdo ligand. In the crystal, O—H...O hydrogen bonds link the dinuclear cation and solvent pzdo molecules (point-group symmetry -1 into rectangular grid-like layers parallel to the bc plane. Additional C—H...O, O—H...O, C—H...π and O—H...π interactions link the anion and solvent water molecules to the layers. The layers are further linked into a three-dimensional network through a combination of C—H...π and O—H...π hydrogen bonds involving the tetraphenylborate anion.

  15. Recent progress in the development of solid catalysts for biomass conversion into high value-added chemicals (United States)

    Hara, Michikazu; Nakajima, Kiyotaka; Kamata, Keigo


    In recent decades, the substitution of non-renewable fossil resources by renewable biomass as a sustainable feedstock has been extensively investigated for the manufacture of high value-added products such as biofuels, commodity chemicals, and new bio-based materials such as bioplastics. Numerous solid catalyst systems for the effective conversion of biomass feedstocks into value-added chemicals and fuels have been developed. Solid catalysts are classified into four main groups with respect to their structures and substrate activation properties: (a) micro- and mesoporous materials, (b) metal oxides, (c) supported metal catalysts, and (d) sulfonated polymers. This review article focuses on the activation of substrates and/or reagents on the basis of groups (a)-(d), and the corresponding reaction mechanisms. In addition, recent progress in chemocatalytic processes for the production of five industrially important products (5-hydroxymethylfurfural, lactic acid, glyceraldehyde, 1,3-dihydroxyacetone, and furan-2,5-dicarboxylic acid) as bio-based plastic monomers and their intermediates is comprehensively summarized.

  16. Development of refractory ceramic using waste of petrochemical catalysts; Desenvolvimento de ceramica refrataria utilizando residuos de catalisadores petroquimicos

    Energy Technology Data Exchange (ETDEWEB)

    Pedroso, M.A.; Mymrine, V. [Universidade Federal do Parana (UFPR), PR (Brazil)


    The manufacturing of catalytic catalysts by the company FCC SA. for the Brazilian petrochemical industry is 25,000 tons per annum, which after going through the cracking process cannot undergo regeneration any longer, being wasted with humidity near 70%. To increase the economical and environmental efficiency of the use of this rejected catalyst, without preliminary drying, a method of using it as main raw material in composition like kaolin was developed, as well as in ash and glass for the manufacturing of common (regular) and refractory ceramic. The mixture of these components were burnt at temperatures of 1100 deg C, 1200°C, 1250°C and 1300°C. The ceramics with 30% and 40% in weight of wasted catalyst, sintered in 1250 deg C or 1300 deg C have flexion of 10,8 - 12,9 MPa. After burning the mixtures, the chemical interaction of the initial components was determined by the methods of RXD, MEV and EDS, synthesizing new minerals like Diopside Ca(Mg,Al)(Si,Al){sub 2}O{sub 6}, Nepheline (K,Na)AlSiO{sub 4}, Lazurite Na{sub 8}[Al{sub 2}SiO{sub 4}]{sub 6}[SO{sub 4},S]{sub 2}, Magnetite Fe{sub 3}O{sub 4}, Albite Na Al Si{sub 3}O{sub 8} and high content of vitreous amorphous phase. (author)

  17. Design and stereoselective preparation of a new class of chiral olefin metathesis catalysts and application to enantioselective synthesis of quebrachamine: catalyst development inspired by natural product synthesis. (United States)

    Sattely, Elizabeth S; Meek, Simon J; Malcolmson, Steven J; Schrock, Richard R; Hoveyda, Amir H


    A total synthesis of the Aspidosperma alkaloid quebrachamine in racemic form is first described. A key catalytic ring-closing metathesis of an achiral triene is used to establish the all-carbon quaternary stereogenic center and the tetracyclic structure of the natural product; the catalytic transformation proceeds with reasonable efficiency through the use of existing achiral Ru or Mo catalysts. Ru- or Mo-based chiral olefin metathesis catalysts have proven to be inefficient and entirely nonselective in cases where the desired product is observed. In the present study, the synthesis route thus serves as a platform for the discovery of new olefin metathesis catalysts that allow for efficient completion of an enantioselective synthesis of quebrachamine. Accordingly, on the basis of mechanistic principles, stereogenic-at-Mo complexes bearing only monodentate ligands have been designed. The new catalysts provide significantly higher levels of activity than observed with the previously reported Ru- or Mo-based complexes. Enantiomerically enriched chiral alkylidenes are generated through diastereoselective reactions involving achiral Mo-based bispyrrolides and enantiomerically pure silyl-protected binaphthols. Such chiral catalysts initiate the key enantioselective ring-closing metathesis step in the total synthesis of quebrachamine efficiently (1 mol % loading, 22 degrees C, 1 h, >98% conversion, 84% yield) and with high selectivity (98:2 er, 96% ee).

  18. Latent olefin metathesis catalysts


    Monsaert, Stijn; Lozano Vila, Ana; Drozdzak, Renata; Van Der Voort, Pascal; Verpoort, Francis


    Olefin metathesis is a versatile synthetic tool for the redistribution of alkylidene fragments at carbon-carbon double bonds. This field, and more specifically the development of task-specific, latent catalysts, attracts emerging industrial and academic interest. This tutorial review aims to provide the reader with a concise overview of early breakthroughs and recent key developments in the endeavor to develop latent olefin metathesis catalysts, and to illustrate their use by prominent exampl...

  19. Development of the advanced nuclear materials -A study on the polymer catalyst process technology-

    Energy Technology Data Exchange (ETDEWEB)

    Kook, Il Hyun; Jung, Heung Suk; Lee, Han Soo; An, Doh Heui; Kang, Heui Suk; Baek, Seung Woo; Lee, Sung Hoh; Sung, Kee Woong; Kim, Kwang Lak; Kim, Jong Hoh; Koo, Je Hyoo; Park, Tae Keun; Kim, Sang Hwan; Yoo, Ryong; Song, Myung Jae; Son, Soon Hwan; Choi, Jung Kil; Lee, Jae Choon; Jung, Moon Kyoo [Korea Atomic Energy Research Institute, Taejon (Korea, Republic of)


    Heavy water is used as moderator and coolant in pressurized heavy water power plants. According to the governmental long-term plan for power supply, Korea is scheduled to construct new four pressurized heavy water power plants till the year 2006. Total heavy water make-up for these plants would be 22 Mg/a from the year 2006. Reformed hydrogen processes is considered best suited to Korea. Hydrophobic catalysts for this process were manufactured and the performance of hydrogen isotope exchange was investigated. The overall mass transfer coefficients varied between 0.004 and 2.295 m3 HD/m3 Bed.sec. and heavy water separation processes using the catalysts were optimized. 66 figs, 62 tabs, 19 refs. (Author).

  20. In Situ Generation of Molybdenum-Based Catalyst for Alkyne Metathesis: Further Developments and Mechanistic Insights

    Directory of Open Access Journals (Sweden)

    Geng Lopez Joaquin


    Full Text Available Molybdenum-based catalysts are among the best candidates to achieve alkyne metathesis. They can be either well-defined carbynes, previously synthesized before their use, but also prepared in situ upon using stable molybdenum carbonyl complexes, or high oxidation state molybdenum salts that need a previous alkylation, both type of precursors being “activated” by hydroxyl-containing compounds such as phenols and silanols. This paper is presenting studies made on these systems, directed towards the knowledge of the reaction paths leading to the active species, and in particular to define the essential role of hydroxyl-containing co-catalyst in the formation of the active species, still ill-defined. From an analysis of the byproducts formed during the reaction, as well as of the initial products, reaction paths to access catalytic carbyne species is suggested, where the ligand environment consists of phenoxy (or siloxy groups, typically required and identified to lead to alkyne metathesis in the case of well-defined catalysts.

  1. Development of an Innovative XRD-DRIFTS Prototype Allowing Operando Characterizations during Fischer-Tropsch Synthesis over Cobalt-Based Catalysts under Representative Conditions

    Directory of Open Access Journals (Sweden)

    Scalbert Julien


    Full Text Available An original system combining both X-Ray Diffraction and diffuse reflectance infrared Fourier transform spectroscopy was developed with the aim to characterize Fischer-Tropsch catalysts in relevant reaction conditions. The catalytic properties of a model PtCo/silica catalyst tested with this prototype have shown to be in the same range of those obtained in similar conditions with classical fixed-bed reactors. No bulk cobalt oxidation nor sintering were observed on operando XRD patterns. The formation of linear carbonyls and adsorbed hydrocarbons species at the surface of the catalyst was observed on operando DRIFT spectra. The surface of the catalyst was also suspected to be covered with carbon species inducing unfavorable changes in selectivity.

  2. Development of a demonstration reactor using thoria as a Fischer-Tropsch catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Colmenares, C.A.; McLean, W.


    We have demonstrated experimentally that thorium oxide may be used as a catalyst with CO + H/sub 2/ mixtures to produce either methanol or a mixture of hydrocarbons from C/sub 1/ to C/sub 5/ (saturated and unsaturated). The immunity of ThO/sub 2/ to poisoning by sulfur compounds makes its use very attractive for industrial applications. We are proposing to optimize the experimental conditions of the catalytic process using a one-inch reactor and to scope and define the experimental conditions for a pilot plant demonstration.

  3. Cross-departmental collaboration in strategic sourcing as a catalyst for supplier development: The case of Eskom

    Directory of Open Access Journals (Sweden)

    Mzoxolo E. Mbiko


    Full Text Available Objective: The objective was to analyse the integration of and collaboration between strategic sourcing and supplier development at Eskom, South Africa’s primary electricity supplier, and to determine how strategic sourcing can be a catalyst for supplier development.Problem investigated: To address fragmented and inefficient procurement, Eskom instituted two departments, Commodity Sourcing (CS, to drive strategic sourcing, and Supplier Development and Localisation (SD&L, to drive supplier development. The problem is that collaboration between CS and SD&L has not materialised and thus their mandates have not been entirely achieved.Research design: A case study research design was employed, drawing from multiple sources of data to triangulate findings. Managers from two departments, CS and SD&L, were separately surveyed, while face-to-face interviews were conducted with executive management.Results: The findings revealed a lack of planning, implementation and monitoring of supplier development in the strategic sourcing process of CS. Although the procurement spend in CS is used to drive supplier development objectives, from the perspective of SD&L, in practice this does not fully materialise.Originality and/or value of the research: The study is unique as it focuses on cross-departmental collaboration within the organisation, rather than collaboration across the supply chain with external partners. From insights into the dysfunctional relationship between the departments, solutions for increased collaboration and effective supplier development could be suggested.Conclusion: For strategic sourcing to be a catalyst of supplier development, it is essential that an integrated strategic sourcing operating model incorporating the objectives of both CS and SD&L be developed.

  4. Catalyst development and systems analysis of methanol partial oxidation for the fuel processor - fuel cell integration

    Energy Technology Data Exchange (ETDEWEB)

    Newson, E.; Mizsey, P.; Hottinger, P.; Truong, T.B.; Roth, F. von; Schucan, Th.H. [Paul Scherrer Inst. (PSI), Villigen (Switzerland)


    Methanol partial oxidation (pox) to produce hydrogen for mobile fuel cell applications has proved initially more successful than hydrocarbon pox. Recent results of catalyst screening and kinetic studies with methanol show that hydrogen production rates have reached 7000 litres/hour/(litre reactor volume) for the dry pox route and 12,000 litres/hour/(litre reactor volume) for wet pox. These rates are equivalent to 21 and 35 kW{sub th}/(litre reactor volume) respectively. The reaction engineering problems remain to be solved for dry pox due to the significant exotherm of the reaction (hot spots of 100-200{sup o}C), but wet pox is essentially isothermal in operation. Analyses of the integrated fuel processor - fuel cell systems show that two routes are available to satisfy the sensitivity of the fuel cell catalysts to carbon monoxide, i.e. a preferential oxidation reactor or a membrane separator. Targets for individual system components are evaluated for the base and best case systems for both routes to reach the combined 40% efficiency required for the integrated fuel processor - fuel cell system. (author) 2 figs., 1 tab., 3 refs.

  5. Developing an approach for first-principles catalyst design: application to carbon-capture catalysis. (United States)

    Kulik, Heather J; Wong, Sergio E; Baker, Sarah E; Valdez, Carlos A; Satcher, Joe H; Aines, Roger D; Lightstone, Felice C


    An approach to catalyst design is presented in which local potential energy surface models are first built to elucidate design principles and then used to identify larger scaffold motifs that match the target geometries. Carbon sequestration via hydration is used as the model reaction, and three- and four-coordinate sp(2) or sp(3) nitrogen-ligand motifs are considered for Zn(II) metals. The comparison of binding, activation and product release energies over a large range of interaction distances and angles suggests that four-coordinate short Zn(II)-Nsp(3) bond distances favor a rapid turnover for CO2 hydration. This design strategy is then confirmed by computationally characterizing the reactivity of a known mimic over a range of metal-nitrogen bond lengths. A search of existing catalysts in a chemical database reveals structures that match the target geometry from model calculations, and subsequent calculations have identified these structures as potentially effective for CO2 hydration and sequestration.

  6. Development of Cobalt Hydroxide as a Bifunctional Catalyst for Oxygen Electrocatalysis in Alkaline Solution. (United States)

    Zhan, Yi; Du, Guojun; Yang, Shiliu; Xu, Chaohe; Lu, Meihua; Liu, Zhaolin; Lee, Jim Yang


    Co(OH)2 in the form of hexagonal nanoplates synthesized by a simple hydrothermal reaction has shown even greater activity than cobalt oxides (CoO and Co3O4) in oxygen reduction and oxygen evolution reactions (ORR and OER) under alkaline conditions. The bifunctionality for oxygen electrocatalysis as shown by the OER-ORR potential difference (ΔE) could be reduced to as low as 0.87 V, comparable to the state-of-the-art non-noble bifunctional catalysts, when the Co(OH)2 nanoplates were compounded with nitrogen-doped reduced graphene oxide (N-rGO). The good performance was attributed to the nanosizing of Co(OH)2 and the synergistic interaction between Co(OH)2 and N-rGO. A zinc-air cell assembled with a Co(OH)2-air electrode also showed a performance comparable to that of the state-of-the-art zinc-air cells. The combination of bifunctional activity and operational stability establishes Co(OH)2 as an effective low-cost alternative to the platinum group metal catalysts.

  7. High-Activity Dealloyed Catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Kongkanand, Anusorn [General Motors LLC, Pontiac, MI (United States)


    Reduction of costly Pt usage in proton exchange membrane fuel cell electrodes is one of the major challenges towards development and commercialization of fuel cell vehicles. Although few have met the initial-kinetic activity requirements in a realistic fuel cell device, no catalyst material has ever met the demanding fuel cell durability targets set by DOE. In this project, a team of 4 universities and 2 companies came together to investigate a concept that appeared promising in preliminary non-fuel cell tests then to further develop the catalyst to a mature level ready for vehicle implementation. The team consists of academia with technical leadership in their respective areas, a catalyst supplier, and a fuel cell system integrator.The tightly collaborative project enabled development of a highly active and durable catalyst with performance that significantly exceeds that of previous catalysts and meets the DOE targets for the first time (Figure 1A). The catalyst was then further evaluated in full-active-area stack in a realistic vehicle operating condition (Figure 1B). This is the first public demonstration that one can realize the performance benefit and Pt cost reduction over a conventional pure Pt catalyst in a long-term realistic PEMFC system. Furthermore, systematic analyses of a range of catalysts with different performance after fuel cell testing allowed for correlation between catalyst microstructure and its electrocatalytic activity and durability. This will in turn aid future catalyst development.

  8. Development of a reaction cell for in-situ/operando studies of surface of a catalyst under a reaction condition and during catalysis

    Energy Technology Data Exchange (ETDEWEB)

    Nguyen, Luan; Tao, Franklin, E-mail: [Department of Chemistry and Biochemistry, University of Notre Dame, Notre Dame, Indiana 46556 (United States); Department of Chemical and Petroleum Engineering, University of Kansas, Lawrence, Kansas 66045 (United States)


    Tracking surface chemistry of a catalyst during catalysis is significant for fundamental understanding of catalytic performance of the catalyst since it allows for establishing an intrinsic correlation between surface chemistry of a catalyst at its working status and its corresponding catalytic performance. Ambient pressure X-ray photoelectron spectroscopy can be used for in-situ studies of surfaces of different materials or devices in a gas. To simulate the gaseous environment of a catalyst in a fixed-bed a flowing gaseous environment of reactants around the catalyst is necessary. Here, we report the development of a new flowing reaction cell for simulating in-situ study of a catalyst surface under a reaction condition in gas of one reactant or during catalysis in a mixture of reactants of a catalytic reaction. The homemade reaction cell is installed in a high vacuum (HV) or ultrahigh vacuum (UHV) environment of a chamber. The flowing gas in the reaction cell is separated from the HV or UHV environment through well sealings at three interfaces between the reaction cell and X-ray window, sample door and aperture of front cone of an energy analyzer. Catalyst in the cell is heated through infrared laser beam introduced through a fiber optics interfaced with the reaction cell through a homemade feedthrough. The highly localized heating on the sample holder and Au-passivated internal surface of the reaction cell effectively minimizes any unwanted reactions potentially catalyzed by the reaction cell. The incorporated laser heating allows a fast heating and a high thermal stability of the sample at a high temperature. With this cell, a catalyst at 800 °C in a flowing gas can be tracked readily.


    Energy Technology Data Exchange (ETDEWEB)

    Adu-Wusu, K; Paul Burket, P


    Wet Air Oxidation (WAO) is one of the two technologies being considered for the destruction of Tetraphenylborate (TPB) in Tank 48H. Batch bench-scale autoclave testing with radioactive (actual) Tank 48H waste is among the tests required in the WAO Technology Maturation Plan. The goal of the autoclave testing is to validate that the simulant being used for extensive WAO vendor testing adequately represents the Tank 48H waste. The test objective was to demonstrate comparable test results when running simulated waste and real waste under similar test conditions. Specifically: (1) Confirm the TPB destruction efficiency and rate (same reaction times) obtained from comparable simulant tests, (2) Determine the destruction efficiency of other organics including biphenyl, (3) Identify and quantify the reaction byproducts, and (4) Determine off-gas composition. Batch bench-scale stirred autoclave tests were conducted with simulated and actual Tank 48H wastes at SRNL. Experimental conditions were chosen based on continuous-flow pilot-scale simulant testing performed at Siemens Water Technologies Corporation (SWT) in Rothschild, Wisconsin. The following items were demonstrated as a result of this testing. (1) Tetraphenylborate was destroyed to below detection limits during the 1-hour reaction time at 280 C. Destruction efficiency of TPB was > 99.997%. (2) Other organics (TPB associated compounds), except biphenyl, were destroyed to below their respective detection limits. Biphenyl was partially destroyed in the process, mainly due to its propensity to reside in the vapor phase during the WAO reaction. Biphenyl is expected to be removed in the gas phase during the actual process, which is a continuous-flow system. (3) Reaction byproducts, remnants of MST, and the PUREX sludge, were characterized in this work. Radioactive species, such as Pu, Sr-90 and Cs-137 were quantified in the filtrate and slurry samples. Notably, Cs-137, boron and potassium were shown as soluble as a

  10. Development of Optimal Catalyst Designs and Operating Strategies for Lean NOx Reduction in Coupled LNT-SCR Systems

    Energy Technology Data Exchange (ETDEWEB)

    Harold, Michael [Univ. of Houston, TX (United States); Crocker, Mark [Univ. of Kentucky, Lexington, KY (United States); Balakotaiah, Vemuri [Univ. of Houston, TX (United States); Luss, Dan [Univ. of Houston, TX (United States); Choi, Jae-Soon [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Dearth, Mark [Ford Motor Company, Dearborn, MI (United States); McCabe, Bob [Ford Motor Company, Dearborn, MI (United States); Theis, Joe [Ford Motor Company, Dearborn, MI (United States)


    alternative reductants such as propylene, representing the hydrocarbon component of diesel exhaust. First-principle models of the LNT and SCR converters, which utilized the mechanistic-based kinetics and realistic treatments of the flow and transport processes, in combination with bench-scale reactor experiments helped to identify the best designs for combining the NSR and SCR catalysts over a range of operating conditions encountered in practice. This included catalysts having multiple zones and layers and additives with the focus on determining the minimal precious metal component needed to meet emission abatement targets over a wide range of operating conditions. The findings from this study provide diesel vehicle and catalyst companies valuable information to develop more cost effective diesel emissions catalysts which helps to expand the use of more fuel efficient diesel power. The fundamental modeling and experimental tools and findings from this project can be applied to catalyst technologies used in the energy and chemical industries. Finally, the project also led to training of several doctoral students who were placed in research jobs in industry and academia.

  11. Reflection as learning about the self in context: mentoring as catalyst for reflective development in pre-service teachers

    Directory of Open Access Journals (Sweden)

    Liezel Frick


    Full Text Available Establishing a close alignment between teacher education programmes and the realities of the actual classroom remains a challenge in preparing pre-service teachers at higher education institutions. The literature indicates that reflection is a core quality of effective teachers. We investigate how the development of reflective practice through mentoring programmes can facilitate the inevitable transitions that students have to make to the professional sector. Through a narrative analysis, we report on the insights of a selected group of Postgraduate Certificate in Education (PGCE students participating in the initial development phase of a mentoring system during their practice teaching in schools guiding them to reflect critically on their learning and practice. The data suggest that mentoring can act as a catalyst to enhance reflection. The development of reflection as praxis can assist in bridging the gap between theory and practice.

  12. Development of a method for the preparation of ruthenium indenylidene-ether olefin metathesis catalysts. (United States)

    Jimenez, Leonel R; Tolentino, Daniel R; Gallon, Benjamin J; Schrodi, Yann


    The reactions between several derivatives of 1-(3,5-dimethoxyphenyl)-prop-2-yn-1-ol and different ruthenium starting materials [i.e., RuCl₂(PPh₃)₃ and RuCl₂(p-cymene)(L), where L is tricyclohexylphosphine di-t-butylmethylphosphine, dicyclohexylphenylphosphine, triisobutylphosphine, triisopropylphosphine, or tri-n-propylphosphine] are described. Several of these reactions allow for the easy, in-situ and atom-economic preparation of olefin metathesis catalysts. Organic precursor 1-(3,5-dimethoxyphenyl)-1-phenyl-prop-2-yn-1-ol led to the formation of active ruthenium indenylidene-ether complexes, while 1-(3,5-dimethoxyphenyl)-prop-2-yn-1-ol and 1-(3,5-dimethoxyphenyl)-1-methyl-prop-2-yn-1-ol did not. It was also found that a bulky and strong σ-donor phosphine ligand was required to impart good catalytic activity to the new ruthenium complexes.

  13. Development of Hydrotalcite Based Cobalt Catalyst by Hydrothermal and Co-precipitation Method for Fischer-Tropsch Synthesis


    Muhammad Faizan Shareef; Muhammad Arslan; Naseem Iqbal; Nisar Ahmad; Tayyaba Noor


    This paper presents the effect of a synthesis method for cobalt catalyst supported on hydrotalcite material for Fischer-Tropsch synthesis. The hydrotalcite supported cobalt (HT-Co) catalysts were synthesized by co-precipitation and hydrothermal method. The prepared catalysts were characterized by using various techniques like BET (Brunauer–Emmett–Teller), SEM (Scanning Electron Microscopy), TGA (Thermal Gravimetric Analysis), XRD (X-ray diffraction spectroscopy), and FTIR (Fourier Transform I...

  14. Catalyst mixtures (United States)

    Masel, Richard I.; Rosen, Brian A.


    Catalysts that include at least one catalytically active element and one helper catalyst can be used to increase the rate or lower the overpotential of chemical reactions. The helper catalyst can simultaneously act as a director molecule, suppressing undesired reactions and thus increasing selectivity toward the desired reaction. These catalysts can be useful for a variety of chemical reactions including, in particular, the electrochemical conversion of CO.sub.2 or formic acid. The catalysts can also suppress H.sub.2 evolution, permitting electrochemical cell operation at potentials below RHE. Chemical processes and devices using the catalysts are also disclosed, including processes to produce CO, OH.sup.-, HCO.sup.-, H.sub.2CO, (HCO.sub.2).sup.-, H.sub.2CO.sub.2, CH.sub.3OH, CH.sub.4, C.sub.2H.sub.4, CH.sub.3CH.sub.2OH, CH.sub.3COO.sup.-, CH.sub.3COOH, C.sub.2H.sub.6, O.sub.2, H.sub.2, (COOH).sub.2, or (COO.sup.-).sub.2, and a specific device, namely, a CO.sub.2 sensor.

  15. Development of a Method for the Preparation of Ruthenium Indenylidene-Ether Olefin Metathesis Catalysts

    Directory of Open Access Journals (Sweden)

    Yann Schrodi


    Full Text Available The reactions between several derivatives of 1-(3,5-dimethoxyphenyl-prop-2-yn-1-ol and different ruthenium starting materials [i.e., RuCl2(PPh33 and RuCl2(p-cymene(L, where L is tricyclohexylphosphine di-t-butylmethylphosphine, dicyclohexylphenylphosphine, triisobutylphosphine, triisopropylphosphine, or tri-n-propylphosphine] are described. Several of these reactions allow for the easy, in-situ and atom-economic preparation of olefin metathesis catalysts. Organic precursor 1-(3,5-dimethoxyphenyl-1-phenyl-prop-2-yn-1-ol led to the formation of active ruthenium indenylidene-ether complexes, while 1-(3,5-dimethoxyphenyl-prop-2-yn-1-ol and 1-(3,5-dimethoxyphenyl-1-methyl-prop-2-yn-1-ol did not. It was also found that a bulky and strong σ-donor phosphine ligand was required to impart good catalytic activity to the new ruthenium complexes.

  16. Challenges in polyoxometalate-mediated aerobic oxidation catalysis: catalyst development meets reactor design. (United States)

    Lechner, Manuel; Güttel, Robert; Streb, Carsten


    Selective catalytic oxidation is one of the most widely used chemical processes. Ideally, highly active and selective catalysts are used in combination with molecular oxygen as oxidant, leading to clean, environmentally friendly process conditions. For homogeneous oxidation catalysis, molecular metal oxide anions, so-called polyoxometalates (POMs) are ideal prototypes which combine high reactivity and stability with chemical tunability on the molecular level. Typically, POM-mediated aerobic oxidations are biphasic, using gaseous O2 and liquid reaction mixtures. Therefore, the overall efficiency of the reaction is not only dependent on the chemical components, but requires chemical engineering insight to design reactors with optimized productivity. This Perspective shows that POM-mediated aerobic liquid-phase oxidations are ideal reactions to be carried out in microstructured flow reactors as they enable facile mass and energy transfer, provide large gas-liquid interfaces and can be easily upscaled. Recent advances in POM-mediated aerobic catalytic oxidations are therefore summarized with a focus on technological importance and mechanistic insight. The principles of reactor design are discussed from a chemical engineering point of view with a focus on homogeneous oxidation catalysis using O2 in microfluidic systems. Further, current limitations to catalytic activity are identified and future directions based on combined chemistry and chemical engineering approaches are discussed to show that this approach could lead to sustainable production methods in industrial chemistry based on alternative energy sources and chemical feedstocks.

  17. Concentration of ions Co(II), Ni(II) at the Tokem-250 carboxylic cation exchange for catalysts development (United States)

    Zharkova, Valentina; Bobkova, Ludmila; Brichkov, Anton; Kozik, Vladimir


    Sorption and catalytic properties of the cation exchanger are investigated. It was found that the Tokem-250 has a wide operating range of pH. The value of the effective ionization constant of the functional groups of the cation exchanger (pKa) is 6.59. The Tokem-250 cation exchanger exhibits selectivity to Ni2+ ions to Co2+ (D˜103). This is probably due to the stability of ion-exchange complexes detected by the method of diffuse reflectance electron spectroscopy (ESDD). According to these data, for Co2+ ions, in contrast to Ni2+, tetragonal distortion of octahedral coordination is characteristic, which has a positive effect on the stability of complexes with Co2+. To obtain spherical catalysts on the basis of Tokem-250, cobalt-containing samples of cation exchanger were used. The developed spherical materials have catalytic activity in the reactions of deep and partial oxidation of n-heptane.

  18. Base-Catalyzed Depolymerization of Lignin with Heterogeneous Catalysts: Cooperative Research and Development Final Report, CRADA Number CRD-13-513

    Energy Technology Data Exchange (ETDEWEB)

    Beckham, Gregg T. [National Renewable Energy Lab. (NREL), Golden, CO (United States)


    We will synthesize and screen solid catalysts for the depolymerization of lignin to monomeric and oligomeric oxygenated species, which could be fractionated and integrated into refinery intermediate streams for selective upgrading, or catalytically upgraded to fuels and chemicals. This work will primarily focus on the synthesis and application of layered double hydroxides (LDHs) as recyclable, heterogeneous catalysts for depolymerization of lignin model compounds and softwood lignin. LDHs have been shown in our group to offer good supports and catalysts to promote base-catalyzed depolymerization of lignin model compounds and in preliminary experiments for the depolymerization of lignin from an Organosolv process. We will also include additional catalyst supports such as silica, alumina, and carbon as identified in ongoing and past efforts at NREL. This work will consist of two tasks. Overall, this work will be synergistic with ongoing efforts at NREL, funded by the DOE Biomass Program, on the development of catalysts for lignin depolymerization in the context of biochemical and thermochemical conversion of corn stover and other biomass feedstocks to advanced fuels and chemicals.

  19. Non-PGM cell catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Colon-Mercado, H. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Elvington, M. [Savannah River Consulting, Aiken, SC (United States); Ganesan, P. [Savannah River Consulting, Aiken, SC (United States)


    A unique approach has been developed to probe the non-PGM catalyst active site for the Oxygen Reduction Reaction (ORR) for PEMFCs. Iron based functionalities have been engineered into a variety of catalysts to evaluate their impact on activity for the ORR. A series of high surface area catalysts were synthesized and the impact of the chemical structure on the electrochemical and electrocatalytic properties was investigated. Elemental and surface analyses of the prepared catalysts reveal the incorporation of iron in a targeted and controlled manner. A high surface area framework catalyst was prepared that shows exceptional activity, comparable to state-of-the-art materials. The results of this research project provided critical seed data for the newly awarded ElectroCat project, which focuses on rationally designed framework catalysts for the oxygen reduction reaction.

  20. Development of bioinspired Mn4O4-cubane water oxidation catalysts: lessons from photosynthesis. (United States)

    Dismukes, G Charles; Brimblecombe, Robin; Felton, Greg A N; Pryadun, Ruslan S; Sheats, John E; Spiccia, Leone; Swiegers, Gerhard F


    Hydrogen is the most promising fuel of the future owing to its carbon-free, high-energy content and potential to be efficiently converted into either electrical or thermal energy. The greatest technical barrier to accessing this renewable resource remains the inability to create inexpensive catalysts for the solar-driven oxidation of water. To date, the most efficient system that uses solar energy to oxidize water is the photosystem II water-oxidizing complex (PSII-WOC), which is found within naturally occurring photosynthetic organisms. The catalytic core of this enzyme is a CaMn(4)O(x) cluster, which is present in all known species of oxygenic phototrophs and has been conserved since the emergence of this type of photosynthesis about 2.5 billion years ago. The key features that facilitate the catalytic success of the PSII-WOC offer important lessons for the design of abiological water oxidation catalysts. In this Account, we examine the chemical principles that may govern the PSII-WOC by comparing the water oxidation capabilities of structurally related synthetic manganese-oxo complexes, particularly those with a cubical Mn(4)O(4) core ("cubanes"). We summarize this research, from the self-assembly of the first such clusters, through the elucidation of their mechanism of photoinduced rearrangement to release O(2), to recent advances highlighting their capability to catalyze sustained light-activated electrolysis of water. The [Mn(4)O(4)](6+) cubane core assembles spontaneously in solution from monomeric precursors or from [Mn(2)O(2)](3+) core complexes in the presence of metrically appropriate bidentate chelates, for example, diarylphosphinates (ligands of Ph(2)PO(2)(-) and 4-phenyl-substituted derivatives), which bridge pairs of Mn atoms on each cube face (Mn(4)O(4)L(6)). The [Mn(4)O(4)](6+) core is enlarged relative to the [Mn(2)O(2)](3+) core, resulting in considerably weaker Mn-O bonds. Cubanes are ferocious oxidizing agents, stronger than analogous complexes

  1. Highly dispersed metal catalyst (United States)

    Xiao, Xin; West, William L.; Rhodes, William D.


    A supported catalyst having an atomic level single atom structure is provided such that substantially all the catalyst is available for catalytic function. A process of forming a single atom catalyst unto a porous catalyst support is also provided.

  2. Bimetal catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Ng, K. Y. Simon; Salley, Steve O.; Wang, Huali


    A catalyst comprises a carbide or nitride of a metal and a promoter element. The metal is selected from the group consisting of Mo, W, Co, Fe, Rh or Mn, and the promoter element is selected from the group consisting of Ni, Co, Al, Si, S or P, provided that the metal and the promoter element are different. The catalyst also comprises a mesoporous support having a surface area of at least about 170 m.sup.2 g.sup.-1, wherein the carbide or nitride of the metal and the promoter element is supported by the mesoporous support, and is in a non-sulfided form and in an amorphous form.

  3. High-Throughput Screening as a Supplemental Tool for the Development of Advanced Emission Control Catalysts: Methodological Approaches and Data Processing

    Directory of Open Access Journals (Sweden)

    Andreas Sundermann


    Full Text Available A high-throughput (HT screening platform developed at hte with the application focus on automotive catalysis is described. hte HT units are configured for performing steady-state testing, as well as dynamic tests with fast feed switches, such as lean/rich excursions for the evaluation of NOx storage capacity and efficiency of lean NOx traps (LNT, ammonia storage capacity for selective catalytic reduction (SCR, evaluation of oxygen storage capacity (OSC, as well as lambda sweep tests for screening of three-way catalysts (TWC. Even though catalysts are screened on a rather small scale (~100 mg powder, experience showed that dosing rather complex gas mixtures in concentrations close to that found in real exhaust for the given application is mandatory to generate relevant data. The objective of this work is to give additional insight into HT technology. In the industrial research laboratory, HT screening has matured to become a reliable approach for rapid screening of both reaction parameter spaces, as well as material properties relevant for exhaust gas catalyst development. Due to the speed of optimized screening involving 48 parallel reactors, automated handling of primary data is an imported requirement. Software for data reduction, like estimation of light-off temperature, needs to be robust and handle results for diverse sample libraries in an unattended fashion. In combination with the statistical design of experiment and multivariate data analysis, HT testing has become a valuable enhancement to automotive catalyst development.

  4. Highly Stable and Active Catalyst for Sabatier Reactions (United States)

    Hu, Jianli; Brooks, Kriston P.


    Highly active Ru/TiO2 catalysts for Sabatier reaction have been developed. The catalysts have shown to be stable under repeated shutting down/startup conditions. When the Ru/TiO2 catalyst is coated on the engineered substrate Fe-CrAlY felt, activity enhancement is more than doubled when compared with an identically prepared engineered catalyst made from commercial Degussa catalyst. Also, bimetallic Ru-Rh/TiO2 catalysts show high activity at high throughput.

  5. Part I: pathogenetic role of peroxynitrite in the development of diabetes and diabetic vascular complications: studies with FP15, a novel potent peroxynitrite decomposition catalyst. (United States)

    Szabó, Csaba; Mabley, Jon G; Moeller, Suzanne M; Shimanovich, Roman; Pacher, Pál; Virag, László; Soriano, Francisco G; Van Duzer, John H; Williams, William; Salzman, Andrew L; Groves, John T


    Peroxynitrite is a cytotoxic oxidant formed from nitric oxide (NO) and superoxide. Tyrosine nitration, a footprint of peroxynitrite, has been demonstrated in the pancreatic islets as well as in the cardiovascular system of diabetic subjects. Delineation of the pathogenetic role of peroxynitrite in disease conditions requires the use of potent, in vivo active peroxynitrite decomposition catalysts. The aim of the current work was to produce a potent peroxynitrite decomposition catalyst and to test its effects in rodent models of diabetes and its complications. FP15 was synthesized and analyzed using standard chemical methods. Diabetes was triggered by the administration of streptozotocin. Tyrosine nitration was measured immunohistochemically. Cardiovascular and vascular measurements were conducted according to standard physiologic methods. FP15, a potent porphyrinic peroxynitrite decomposition catalyst, potently inhibited tyrosine nitration and peroxynitrite-induced cytotoxicity in vitro and in vivo. FP15 treatment (3-10 mg/kg/d) dose dependently and reduced the incidence and severity of diabetes mellitus in rats subjected to multiple low doses of streptozotocin, as well as in nonobese mice developing spontaneous autoimmune diabetes. Furthermore, treatment with FP15 protected against the development of vascular dysfunction (loss of endothelium-dependent relaxations) and the cardiac dysfunction (loss of myocardial contractility) in diabetic mice. FP15 treatment reduced tyrosine nitration in the diabetic pancreatic islets. The current results demonstrate the importance of endogenous peroxynitrite generation in the pathogenesis of autoimmune diabetes and diabetic cardiovascular complications. Peroxynitrite decomposition catalysts may be of therapeutic utility in diabetes and other pathophysiologic conditions.

  6. Development of Integrated TiO2 on Carburized Si Nanowires as a Catalyst/Support Structure for Alkaline Fuel Cells (United States)

    Lemke, Adam J.

    Due to a combination of environmental and economic motivations, there is a strong impetus to transition away from fossil fuels towards renewable sources of energy. Critical to achieving this goal will be technologies that allow for the storage and transmission of energy derived from renewable sources. Hydrogen fuel cells may play a significant role in making this a reality, allowing for the use of hydrogen as a non-carbon based fuel, in particular for vehicle applications. Hydrogen fuel cells directly convert chemical energy into electrical energy, with only water vapor and heat as waste products. There are challenges facing fuel cell technology that inhibit its wider implementation. One of the most significant of these is the cost of the platinum that is typically used in fuel cells to catalyze the oxygen reduction reaction (ORR), which is the bottleneck reaction in hydrogen fuel cells. The rarity and expense of platinum significantly add to the cost of fuel cells, thus reducing their economic viability. Therefore there is much interest in developing catalysts from alternative materials with a lower cost. A second, and related issue facing fuel cells is the degradation over time of the support structure that puts the catalyst into electrical connection with the external load. The carbon structure that currently serves as the standard catalyst support degrades over time under the harsh operating conditions of the cell, leading to catalyst agglomeration and reducing the lifetime of the cell. It is therefore desirable to develop support structures that will be more stable, while still providing electrical conductivity. The following presents original research pertaining to the development of catalyst/support materials making use of non-noble metal oxides synthesized by means of wet chemical methods. Metal oxides such as manganese oxide and titanium oxide are capable of serving as support materials and (in the case of alkaline fuel cells) even as catalysts. Wet

  7. Novel metalloporphyrin catalysts for the oxidation of hydrocarbons

    Energy Technology Data Exchange (ETDEWEB)

    Showalter, M.C.; Nenoff, T.M.; Shelnutt, J.A.


    Work was done for developing biomimetic oxidation catalysts. Two classes of metalloporphyrin catalysts were studied. The first class of catalysts studied were a novel series of highly substituted metalloporphyrins, the fluorinated iron dodecaphenylporphyrins. These homogeneous metalloporphyrin catalysts were screened for activity as catalysts in the oxidation of hydrocarbons by dioxygen. Results are discussed with respect to catalyst structural features. The second type of catalysts studied were heterogeneous catalysts consisting of metalloporphyrins applied to inorganic supports. Preliminary catalytic testing results with these materials are presented.

  8. Development and Comparison of the Substrate Scope of Pd-Catalysts for the Aerobic Oxidation of Alcohols (United States)

    Schultz, Mitchell J.; Hamilton, Steven S.; Jensen, David R.; Sigman, Matthew S.


    Three catalysts for aerobic oxidation of alcohols are discussed and the effectiveness of each is evaluated for allylic, benzylic, aliphatic, and functionalized alcohols. Additionally, chiral nonracemic substrates as well as chemoselective and diastereoselective oxidations are investigated. In this study, the most convenient system for the Pd-catalyzed aerobic oxidation of alcohols is Pd(OAc)2 in combination with triethylamine. This system functions effectively for the majority of alcohols tested and uses mild conditions (3 to 5 mol % of catalyst, room temperature). Pd(IiPr)(OAc)2(H2O) (1) also successfully oxidizes the majority of alcohols evaluated. This system has the advantage of significantly lowering catalyst loadings but requires higher temperatures (0.1 to 1 mol % of catalyst, 60 °C). A new catalyst is also disclosed, Pd(IiPr)(OPiv)2 (2). This catalyst operates under very mild conditions (1 mol %, room temperature, and air as the O2 source) but with a more limited substrate scope. PMID:15844968

  9. Salesperson, Catalyst, Manager, Leader. (United States)

    Worth, Michael J.; Asp, James W., II


    This article examines four roles of the college or university development officer: salesperson (when direct solicitation is seen as the officer's primary role); catalyst (or sales manager, adviser, expert, facilitator); manager (stressing the importance of the overall office functioning); and leader (who exerts a leadership role in the…

  10. Follow the Yellow Brick Road: Websites as Catalysts for National Development

    Directory of Open Access Journals (Sweden)

    Pearson Broome


    Full Text Available Small-island developing states (SIDS enhance their competitiveness by advertising development initiatives that promote and encourage direct foreign inward investment opportunities in major markets. Failure to make use of information communication technologies (ICTs can undermine national development initiatives with transformative potential. Based on this logic, some Caribbean governments have followed international best practices of businesses and have moved towards the creation of websites and the establishment of portals or gateway sites on the World Wide Web to announce their presence.  One of the practical implications of such initiatives is based on the assumption that once websites are built, persons will come. Although for many, the development of a website appears to be an innocuous endeavour this mistaken perception in most cases has led to several sites being designed and commissioned as technical projects mostly employing techno-centric approaches. These policies often ignore the accompanying important socio-technical institutional considerations, such as the importance of timely and accurate information to potential business clients or prospective developers, language capabilities, and a range of standards, guidelines, rules and legislative changes. The central thesis of this conceptual paper is that if member states of the region properly conceptualise and design websites and portals they can be used to achieve strategic national and international development objectives of egovernance in its broadest meaning. The arguments are intended to stimulate thought among policy makers and the private sector alike in the Caribbean with a view to bringing about change that will promote sustainable development.

  11. The Mediterranean solar plan, a development catalyst; Le plan solaire mediterraneen, un catalyseur de developpement

    Energy Technology Data Exchange (ETDEWEB)

    Lorec, Ph. [Energie du Climat, 92 - La Defense (France); Laffitte, M. [Inspection Generale des Finances, 75 - Paris (France)


    In the framework of the 'Union for the Mediterranean area', the Mediterranean Solar Plan aims at answering the energy needs of populations but the global and regional challenges of the decades to come as well. Using mature technologies, for which an acceleration of the industrial development and a cost reduction are requested, it proposes a new sustainable development policy and a durable, profitable and shared economic model. (J.S.)

  12. Development of membrane electrode assembly for high temperature proton exchange membrane fuel cell by catalyst coating membrane method (United States)

    Liang, Huagen; Su, Huaneng; Pollet, Bruno G.; Pasupathi, Sivakumar


    Membrane electrode assembly (MEA), which contains cathode and anode catalytic layer, gas diffusion layers (GDL) and electrolyte membrane, is the key unit of a PEMFC. An attempt to develop MEA for ABPBI membrane based high temperature (HT) PEMFC is conducted in this work by catalyst coating membrane (CCM) method. The structure and performance of the MEA are examined by scanning electron microscopy (SEM), electrochemical impedance spectroscopy (EIS) and I-V curve. Effects of the CCM preparation method, Pt loading and binder type are investigated for the optimization of the single cell performance. Under 160 °C and atmospheric pressure, the peak power density of the MEA, with Pt loading of 0.5 mg cm-2 and 0.3 mg cm-2 for the cathode and the anode, can reach 277 mW cm-2, while a current density of 620 A cm-2 is delivered at the working voltage of 0.4 V. The MEA prepared by CCM method shows good stability operating in a short term durability test: the cell voltage maintained at ∼0.45 V without obvious drop when operated at a constant current density of 300 mA cm-2 and 160 °C under ambient pressure for 140 h.


    Directory of Open Access Journals (Sweden)

    Felix Kayode OLAKULEHIN


    Full Text Available Educational provision in developing sub-Saharan Africa states has been severely hindered by the hydra-headed problems of access, cost and quality. Amidst these challenges is the pledge of regional and national education policymakers and development planners to ensure that there is maximum access equitable and qualitative education for all (EFA in Africa. There is also a burning need for improved literacy levels and functional education, in order to overcome the development deficits that are currently facing the region. The pledge of education for all resonates the agreement which representatives of several nations of the world signed at the Jomtien summit on Education for All and the subsequent evaluation meetings. Following this pledge, several developing, sub-Sahara African nations have evolved initiatives for instituting sustainable Open Flexible Learning (ODL systems in order to meet up with the seemingly intractable EFA objectives. This paper examined the potential impact of these OFL initiatives on the achievement of the EFA objectives which is seen as the basis of development planning, administration and implementation in Africa. It identified the various challenges confronting effective implementation of ODL on the continent, amidst the need to expand access to educational opportunities. An attempt was made to situate the OFL system at the centre of the strategies for achieving these EFA objectives in the region and finally, a proposal for sustainable policy initiatives for implementing OFL systems for the attainment of education for all in Africa is made.

  14. Chemical Insights into the Design and Development of Face-Centered Cubic Ruthenium Catalysts for Fischer-Tropsch Synthesis. (United States)

    Li, Wei-Zhen; Liu, Jin-Xun; Gu, Jun; Zhou, Wu; Yao, Si-Yu; Si, Rui; Guo, Yu; Su, Hai-Yan; Yan, Chun-Hua; Li, Wei-Xue; Zhang, Ya-Wen; Ma, Ding


    Ruthenium is a promising low-temperature catalyst for Fischer-Tropsch synthesis (FTS). However, its scarcity and modest specific activity limit its widespread industrialization. We demonstrate here a strategy for tuning the crystal phase of catalysts to expose denser and active sites for a higher mass-specific activity. Density functional theory calculations show that upon CO dissociation there are a number of open facets with modest barrier available on the face-centered cubic (fcc) Ru but only a few step edges with a lower barrier on conventional hexagonal-closest packed (hcp) Ru. Guided by theoretical calculations, water-dispersible fcc Ru catalysts containing abundant open facets were synthesized and showed an unprecedented mass-specific activity in the aqueous-phase FTS, 37.8 molCO·molRu-1·h-1 at 433 K. The mass-specific activity of the fcc Ru catalysts with an average size of 6.8 nm is about three times larger than the previous best hcp catalyst with a smaller size of 1.9 nm and a higher specific surface area. The origin of the higher mass-specific activity of the fcc Ru catalysts is identified experimentally from the 2 orders of magnitude higher density of the active sites, despite its slightly higher apparent barrier. Experimental results are in excellent agreement with prediction of theory. The great influence of the crystal phases on site distribution and their intrinsic activities revealed here provides a rationale design of catalysts for higher mass-specific activity without decrease of the particle size.

  15. Recent Development in Hydrogen Evolution Reaction Catalysts and Their Practical Implementation

    DEFF Research Database (Denmark)

    Vesborg, Peter Christian Kjærgaard; Seger, Brian; Chorkendorff, Ib


    conditions offering nearly platinum like catalytic performance. The developments have been particularly fast in the last 5 years, and the present Perspective highlights key developments and discusses them, along with hydrogen evolution in general, in the context of the global energy problem.......The past 10 years have seen great advances in the field of electrochemical hydrogen evolution. In particular, several new nonprecious metal electrocatalysts, for example, the MoS2 or the Ni2P family of materials, have emerged as contenders for electrochemical hydrogen evolution under harsh acidic...

  16. Catalysts of Women's Talent Development in STEM: A Systematic Review (United States)

    Mullet, Dianna R.; Rinn, Anne N.; Kettler, Todd


    Numbers of women in the physical sciences, mathematics, and engineering are growing, yet women are still far outnumbered by men at upper levels of those fields. The purpose of the study is to review the literature on academic women who develop exceptional talent in science, technology, engineering, and mathematics (STEM). Data sources included 18…

  17. Re-positioning Nigeria's radio broadcast as a catalyst for development

    African Journals Online (AJOL)

    In conclusion, the paper, focuses on the Development Media Theory and Social Responsibility Theory arguing that this trend must be consciously viewed as a real challenge by the Nigeria radio broadcast that needs not waste time to counter the negative trend being perpetuated over the years but however to reposition her ...


    Energy Technology Data Exchange (ETDEWEB)

    Panagiotis G. Smirniotis; Robert G. Jenkins


    The work performed during this project focused on the identification of materials capable of providing high activity and selectivity for the selective catalytic reduction of nitric oxide with ammonia. The material surface characteristics were correlated with the catalytic behavior of our catalysts to increase our understanding and to help improve the DeNO{sub x} efficiency. The catalysts employed in this study include mixed oxide composite powders (TiO{sub 2}-Cr{sub 2}O{sub 3}, TiO{sub 2}-ZrO{sub 2}, TiO{sub 2}-WO{sub 3}, TiO{sub 2}-SiO{sub 2}, and TiO{sub 2}-Al{sub 2}O{sub 3}) loaded with varying amounts of V{sub 2}O{sub 5}, along with 5 different commercial sources of TiO{sub 2}. V{sub 2}O{sub 5} was added to the commercial sources of TiO{sub 2} to achieve monolayer coverage. Since the valence state of vanadium in the precursor solution during the impregnation step significantly impacted catalytic performance, catalysts were synthesized from both V{sup +4} and V{sup +5} solutions explain this phenomenon. Specifically, the synthesis of catalysts from V{sup 5+} precursor solutions yields lower-performance catalysts compared to the case of V{sup 4+} under identical conditions. Aging the vanadium precursor solution, which is associated with the reduction of V{sup 5+} to V{sup 4+} (VO{sub 2}{sup +} {yields} VO{sup 2+}), prior to impregnation results in catalysts with excellent catalytic behavior under identical activation and operating conditions. This work also added vanadia to TiO{sub 2}-based supports with low crystallinity. These supports, which have traditionally performed poorly, are now able to function as effective SCR catalysts. Increasing the acidity of the support by incorporating oxides such as WO{sub 3} and Al{sub 2}O{sub 3} significantly improves the SCR activity and nitrogen selectivity. It was also found that the supports should be synthesized with the simultaneous precipitation of the corresponding precursors. The mixed oxide catalysts possess

  19. Civil society: the catalyst for ensuring health in the age of sustainable development. (United States)

    Smith, Julia; Buse, Kent; Gordon, Case


    Sustainable Development Goal Three is rightly ambitious, but achieving it will require doing global health differently. Among other things, progressive civil society organisations will need to be recognised and supported as vital partners in achieving the necessary transformations. We argue, using illustrative examples, that a robust civil society can fulfill eight essential global health functions. These include producing compelling moral arguments for action, building coalitions beyond the health sector, introducing novel policy alternatives, enhancing the legitimacy of global health initiatives and institutions, strengthening systems for health, enhancing accountability systems, mitigating the commercial determinants of health and ensuring rights-based approaches. Given that civil society activism has catalyzed tremendous progress in global health, there is a need to invest in and support it as a global public good to ensure that the 2030 Agenda for Sustainable Development can be realised.

  20. Development of Pd and Pd-Co catalysts supported on multi-walled carbon nanotubes for formic acid oxidation

    Energy Technology Data Exchange (ETDEWEB)

    Morales-Acosta, D.; Godinez, Luis A.; Rodriguez, H.G.; Arriaga, L.G. [Centro de Investigacion y Desarrollo Tecnologico en Electroquimica, Parque Tecnologico Queretaro, Sanfandila, Pedro Escobedo, C.P. 76703 Queretaro (Mexico); Ledesma-Garcia, J. [Division de Investigacion y Posgrado, Facultad de Ingenieria, Universidad Autonoma de Queretaro, Cerro de las Campanas S/N, C.P. 76010, Queretaro, Qro. (Mexico); Alvarez-Contreras, L. [Centro de Investigacion en Materiales Avanzados S. C., Complejo Industrial Chihuahua, C.P. 31109, Chihuahua, Chih. (Mexico)


    Pd-Co and Pd catalysts were prepared by the impregnation synthesis method at low temperature on multi-walled carbon nanotubes (MWCNTs). The nanotubes were synthesized by spray pyrolysis technique. Both catalysts were obtained with high homogeneous distribution and particle size around 4 nm. The morphology, composition and electrocatalytic properties were investigated by transmission electron microscopy, scanning electron microscopy-energy dispersive X-ray analysis, X-ray diffraction and electrochemical measurements, respectively. The electrocatalytic activity of Pd and PdCo/MWCNTs catalysts was investigated in terms of formic acid electrooxidation at low concentration in H{sub 2}SO{sub 4} aqueous solution. The results obtained from voltamperometric studies showed that the current density achieved with the PdCo/MWCNTs catalyst is 3 times higher than that reached with the Pd/MWCNTs catalyst. The onset potential for formic acid electrooxidation on PdCo/MWCNTs electrocatalyst showed a negative shift ca. 50 mV compared with Pd/MWCNTs. (author)

  1. Development of a complete kinetic model for the Fischer-Tropsch synthesis over Co/Al{sub 2}O{sub 3} catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Visconti, C.G.; Tronconi, E.; Lietti, L.; Forzatti, P. [Politecnico di Milano (Italy). Dipt. di Chimica, Materiali e Ingegneria Chimica ' ' G.Natta' ' ; Zennaro, R. [EniTecnologie, San Donato Milanese (Italy). Catalysis and Process Technology Research Centre


    A global kinetic model of the FTS over a Co/Al{sub 2}O{sub 3} state-of-the-art catalyst is developed in a fixed bed micro-reactor under conditions relevant to industrial operation (temperature, 210- 235 C; pressure, 8-25 bar; H{sub 2}/CO feed molar ratio, 1.8-2.7; gas hourly space velocity, 2000- 7000 cm{sup 3}(STP)/h/g{sub catalyst}). On the basis of proposed reaction mechanisms, developed according to the carbide theory and the alkyl mechanism, the kinetic expressions for n-paraffins and {alpha}-olefins formation are derived. Both the calculated CO conversion and the hydrocarbons distribution (up to N=49) in FTS reaction are satisfactorily predicted. (orig.)

  2. Effective Communication as Catalyst of Developmental Local Government and Rural Development amid Threats of Overpopulation

    Directory of Open Access Journals (Sweden)

    Naledzani Rasila


    Full Text Available South Africa’s population has risen from 40.5 million in 1996  to 44.8 million in 2001 and to 51.77 in 2011. Africans are in majority making 79.2% of the whole population. About 22.3% of blacks have received no schooling with the unemployment rate of the blacks at 28.1%. Most of these unemployed and uneducated blacks are found in rural areas. This compelled government to introduce Developmental Local government. Developmental Local government refers to the layer of public service that has the capacity to deliver and account to the people in a responsive, accountable, and efficient manner. It is also described as a sphere that encourages community participation in matters of governance and developmental initiatives. However, Developmental Local government is hindered by continuous growth of population which is likely to lead to overpopulation. Overpopulation is characterised by lack of basic resources such as water and  food. Developmental Local government on the other hand is expected to deliver on these needs. Lack of fulfilment of goals of Developmental Local government is attributed to lack of effective communication between local government and community members. Although population growth is not attributed only to high birth rate, governments around the continent have introduced measures to encourage healthy reproductive life. However, this needs community members that are self-motivated to be active participants in government initiatives. This is not achievable as there is an indication of lack of effective communication. This paper’s main focus is the provision of effective communication model at local sphere which will see community members working together with government on matters of their own development including initiatives  to preserve limited resources amid the challenges of overpopulation. This paper is based on the qualitative study on effectiveness of communication in Mutale local municipality on the enhancement of

  3. Semisynthetic and Biomolecular Hydrogen Evolution Catalysts. (United States)

    Kandemir, Banu; Chakraborty, Saikat; Guo, Yixing; Bren, Kara L


    There has been great interest in the development of stable, inexpensive, efficient catalysts capable of reducing aqueous protons to hydrogen (H2), an alternative to fossil fuels. While synthetic H2 evolution catalysts have been in development for decades, recently there has been great progress in engineering biomolecular catalysts and assemblies of synthetic catalysts and biomolecules. In this Forum Article, progress in engineering proteins to catalyze H2 evolution from water is discussed. The artificial enzymes described include assemblies of synthetic catalysts and photosynthetic proteins, proteins with cofactors replaced with synthetic catalysts, and derivatives of electron-transfer proteins. In addition, a new catalyst consisting of a thermophilic cobalt-substituted cytochrome c is reported. As an electrocatalyst, the cobalt cytochrome shows nearly quantitative Faradaic efficiency and excellent longevity with a turnover number of >270000.

  4. Exploring Catalyst Behaviours


    Austin, Annie; Cox, Jayne; Barnett, Julia; Thomas, Christine


    The ‘Exploring catalyst behaviours’ project continues Defra’s programme of research designed to develop a deeper understanding of pro-environmental behaviour. The research, conducted by Brook Lyndhurst, Dr Julie Barnett of the University of Surrey and Dr Christine Thomas of the Open University, feeds into the body of evidence that is guiding Defra and other stakeholders in developing policy, communications and other interventions to galvanise public action on the environment.The aim of the pr...

  5. Development and characterisation of novel heterogeneous palm oil mill boiler ash-based catalysts for biodiesel production. (United States)

    Ho, Wilson Wei Sheng; Ng, Hoon Kiat; Gan, Suyin


    Novel heterogeneous catalysts from calcium oxide (CaO)/calcined calcium carbonate (CaCO(3)) loaded onto different palm oil mill boiler ashes were synthesised and used in the transesterification of crude palm oil (CPO) with methanol to yield biodiesel. Catalyst preparation parameters including the type of ash support, the weight percentage of CaO and calcined CaCO(3) loadings, as well as the calcination temperature of CaCO(3) were optimised. The catalyst prepared by loading of 15 wt% calcined CaCO(3) at a fixed temperature of 800°C on fly ash exhibited a maximum oil conversion of 94.48%. Thermogravimetric analysis (TGA) revealed that the CaCO(3) was transformed into CaO at 770°C and interacted well with the ash support, whereas rich CaO, Al(2)O(3) and SiO(2) were identified in the composition using X-ray diffraction (XRD). The fine morphology size (<5 μm) and high surface area (1.719 m(2)/g) of the fly ash-based catalyst rendered it the highest catalytic activity. Copyright © 2012 Elsevier Ltd. All rights reserved.

  6. Coupling Noble Metals and Carbon Supports in the Development of Combustion Catalysts for the Abatement of BTX Compounds in Air Streams

    Directory of Open Access Journals (Sweden)

    Sergio Morales-Torres


    Full Text Available The catalytic combustion of volatile organic compounds (VOCs is one of the most important techniques to remove these pollutants from the air stream, but it should be carried out at the lowest possible temperature, saving energy and avoiding the simultaneous formation of nitrogen oxides (NOx. Under these experimental conditions, the chemisorption of water generated from VOCs combustion may inhibit hydrophilic catalysts. Nowadays, a wide variety of carbon materials is available to be used in catalysis. The behavior of these hydrophobic materials in the development of highly active and selective combustion catalysts is analyzed in this manuscript. The support characteristics (porosity, hydrophobicity, structure, surface chemistry, etc. and the active phase nature (noble metals: Pt, Pd and dispersion were analyzed by several techniques and the results correlated with the dual adsorptive and/or catalytic performance of the corresponding catalysts. The coupling of highly active phases and carbon materials (activated carbons, honeycomb coated monoliths, carbon aerogels, etc. with tuneable physicochemical properties leads to the complete abatement of benzene, toluene and xylenes (BTX from dilute air streams, being selectively oxidized to CO2 at low temperatures.

  7. Operando chemistry of catalyst surfaces during catalysis. (United States)

    Dou, Jian; Sun, Zaicheng; Opalade, Adedamola A; Wang, Nan; Fu, Wensheng; Tao, Franklin Feng


    Chemistry of a catalyst surface during catalysis is crucial for a fundamental understanding of mechanism of a catalytic reaction performed on the catalyst in the gas or liquid phase. Due to the pressure- or molecular density-dependent entropy contribution of gas or liquid phase of the reactants and the potential formation of a catalyst surface during catalysis different from that observed in an ex situ condition, the characterization of the surface of a catalyst under reaction conditions and during catalysis can be significant and even necessary for understanding the catalytic mechanism at a molecular level. Electron-based analytical techniques are challenging for studying catalyst nanoparticles in the gas or liquid phase although they are necessary techniques to employ. Instrumentation and further development of these electron-based techniques have now made in situ/operando studies of catalysts possible. New insights into the chemistry and structure of catalyst nanoparticles have been uncovered over the last decades. Herein, the origin of the differences between ex situ and in situ/operando studies of catalysts, and the technical challenges faced as well as the corresponding instrumentation and innovations utilized for characterizing catalysts under reaction conditions and during catalysis, are discussed. The restructuring of catalyst surfaces driven by the pressure of reactant(s) around a catalyst, restructuring in reactant(s) driven by reaction temperature and restructuring during catalysis are also reviewed herein. The remaining challenges and possible solutions are briefly discussed.

  8. Control in the Rate-Determining Step Provides a Promising Strategy To Develop New Catalysts for CO2 Hydrogenation: A Local Pair Natural Orbital Coupled Cluster Theory Study. (United States)

    Mondal, Bhaskar; Neese, Frank; Ye, Shengfa


    The development of efficient catalysts with base metals for CO2 hydrogenation has always been a major thrust of interest. A series of experimental and theoretical work has revealed that the catalytic cycle typically involves two key steps, namely, base-promoted heterolytic H2 splitting and hydride transfer to CO2, either of which can be the rate-determining step (RDS) of the entire reaction. To explore the determining factor for the nature of RDS, we present herein a comparative mechanistic investigation on CO2 hydrogenation mediated by [M(H)(η(2)-H2)(PP3(Ph))](n+) (M = Fe(II), Ru(II), and Co(III); PP3(Ph) = tris(2-(diphenylphosphino)phenyl)phosphine) type complexes. In order to construct reliable free energy profiles, we used highly correlated wave function based ab initio methods of the coupled cluster type alongside the standard density functional theory. Our calculations demonstrate that the hydricity of the metal-hydride intermediate generated by H2 splitting dictates the nature of the RDS for the Fe(II) and Co(III) systems, while the RDS for the Ru(II) catalyst appears to be ambiguous. CO2 hydrogenation catalyzed by the Fe(II) complex that possesses moderate hydricity traverses an H2-splitting RDS, whereas the RDS for the high-hydricity Co(III) species is found to be the hydride transfer. Thus, our findings suggest that hydricity can be used as a practical guide in future catalyst design. Enhancing the electron-accepting ability of low-hydricity catalysts is likely to improve their catalytic performance, while increasing the electron-donating ability of high-hydricity complexes may speed up CO2 conversion. Moreover, we also established the active roles of base NEt3 in directing the heterolytic H2 splitting and assisting product release through the formation of an acid-base complex.

  9. Development of stable pollution free TiO2/Au nanoparticle immobilized green photo catalyst for degradation of methyl orange. (United States)

    Murugan, Eagambaram; Rangasamy, Rajmohan


    Two types of heterogeneous nanoparticle immobilized photocatalysts viz., PSP4VP-TiO2 and PSP4VP-TiO2-Au were synthesized by immobilization of TiO2 and TiO2-Au nanoparticles individually onto the insoluble cross-linked poly(styrene)-co-poly(4-vinylpyridine) as a common matrix. These two different green photocatalysts were characterized by FT-IR, SEM, HRTEM and EDS analyses and proves that the respective nanoparticles were found to immobilize onto the matrix. The photocatalytic efficiency of these catalysts was examined using degradation of methyl orange as a model reaction and found they are excellent in UV and sunlight. The stability and recycle/reusability of the catalysts were also observed to be good.

  10. Development of high-performance cathode catalyst of polypyrrole modified carbon supported CoOOH for direct borohydride fuel cell (United States)

    He, Yan; Zhu, Cai; Chen, Kaijian; Wang, Juan; Qin, Haiying; Liu, Jiabin; Yan, Shuai; Yang, Ke; Li, Aiguo


    Polypyrrole modified carbon supported CoOOH electrocatalyst (CoOOH-PPy-C) is prepared by impregnation-chemical method, and the catalytic properties for the oxygen reduction reaction (ORR) in alkaline media are investigated. The X-ray diffraction and transmission electron microscopy results confirm the presence of the expected CoOOH. The electrochemical tests show that the CoOOH-PPy-C catalyst exhibits good electrocatalytic activity towards ORR. The direct borohydride fuel cell using CoOOH-PPy-C as the cathode catalyst demonstrates a good stability performance. There is only 4% decrease of the cell voltage after 80-h operation. The ORR occurs an average 4-electron transfer pathway on the CoOOH-PPy-C catalyst. The good catalytic activity towards ORR benefits from the Cosbnd N bond, which is identified by X-ray photoelectron spectroscopy test. X-ray absorption fine structure experiments further show that two nearest O atoms are substituted by two N atoms bonding to Co ion at a distance of 1.64 Å. The CoOOH-PPy-C exhibits better electrochemical properties than the Co(OH)2 counterpart even though the valence state of Co ion is +3 in CoOOH-PPy-C. Those results indicate that the bonding of Co ion with N atoms should be a key issue regardless the valence of Co ion.

  11. Molecular catalysts structure and functional design

    CERN Document Server

    Gade, Lutz H


    Highlighting the key aspects and latest advances in the rapidly developing field of molecular catalysis, this book covers new strategies to investigate reaction mechanisms, the enhancement of the catalysts' selectivity and efficiency, as well as the rational design of well-defined molecular catalysts. The interdisciplinary author team with an excellent reputation within the community discusses experimental and theoretical studies, along with examples of improved catalysts, and their application in organic synthesis, biocatalysis, and supported organometallic catalysis. As a result, readers wil

  12. Organic synthesis with olefin metathesis catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Grubbs, R.H. [California Institute of Technology, Pasadena, CA (United States)


    Over the past nine years, early transition metal catalysts for the ring opening metathesis polymerization of cyclic olefins have been developed. These catalysts are simple organometallic complexes containing metal carbon multiple bonds that in most cases polymerize olefins by a living process. These catalysts have been used to prepare a family of near monodispersed and structurally homogeneous polymers. A series of group VII ROMP catalysts that allow a wide range of functionality to be incorporated into the polymer side chains have been prepared. The most important member of this family of complexes are the bisphosphinedihalo-ruthenium carbene complexes. These polymerization catalysts can also be used in the synthesis of fine chemicals by ring closing (RCM) and vinyl coupling reactions. The availability of the group VII catalysts allow metathesis to be carried out on highly functionalized substrates such as polypeptides and in unusual environments such as in aqueous emulsions.

  13. Interaction between Nafion ionomer and noble metal catalyst for PEMFCs

    DEFF Research Database (Denmark)

    Andersen, Shuang Ma

    The implement of polymer impregnation in electrode structure (catalyst layer) decreasing the noble metal catalyst loading by a factor of ten , , is one of the essential mile stones in the evolution of Proton Exchange Membrane Fuel Cells’ development among the application of catalyst support...... and electrode deposition etc. In fuel cell reactions, both electrons and protons are involved. Impregnation of Nafion ionomer in catalyst layer effectively increases the proton-electron contact, enlarge the reaction zone, extend the reaction from the surface to the entire electrode. Therefore, the entire...... catalyst layer conducts both electrons and protons so that catalyst utilization in the layer is improved dramatically. The catalyst layer will in turn generate and sustain a higher current density. One of the generally adapted methods to impregnate Nafion into the catalyst layer is to mix the catalysts...

  14. Foundation Flash Catalyst

    CERN Document Server

    Goralski, Greg


    This book offers an introduction to Flash Catalyst for designers with intermediate to advanced skills. It discusses where Catalyst sits within the production process and how it communicates with other programs. It covers all of the features of the Flash Catalyst workspace, teaching you how to create designs from scratch, how to build application designs and add functionality, and how to master the Catalyst/Flex workflow. * Introduces Flash Catalyst * Focuses on production process * Covers the interrelation between Flash Catalyst and Photoshop/Illustrator/Flex/Flash What you'll learn Starting f

  15. Catalyst and electrode research for phosphoric acid fuel cells (United States)

    Antoine, A. C.; King, R. B.


    An account is given of the development status of phosphoric acid fuel cells' high performance catalyst and electrode materials. Binary alloys have been identified which outperform the baseline platinum catalyst; it has also become apparent that pressurized operation is required to reach the desired efficiencies, calling in turn for the use of graphitized carbon blacks in the role of catalyst supports. Efforts to improve cell performance and reduce catalyst costs have led to the investigation of a class of organometallic cathode catalysts represented by the tetraazaannulenes, and a mixed catalyst which is a mixture of carbons catalyzed with an organometallic and a noble metal.

  16. Designing the "search pathway" in the development of a new class of highly efficient stereoselective hydrosilylation catalysts. (United States)

    César, Vincent; Bellemin-Laponnaz, Stéphane; Wadepohl, Hubert; Gade, Lutz H


    The direct coupling of oxazolines and N-heterocyclic carbenes leads to chelating C,N ancillary ligands for asymmetric catalysis that combine both an "anchor" unit and a stereodirecting element. Reacting various N-substituted imidazoles with 2-bromo-4(S)-tert-butyl- and 2-bromo-4(S)-isopropyloxazoline gave the imidazolium precursors of the stereodirecting ancillary ligands. A library of ten different ligand precursors was obtained by using this simple procedure (65-97 % yield). These protioligands were metalated in a subsequent step by reaction with [{Rh(mu-OtBu)(nbd)}2] (nbd=norbornadiene), generated in situ from KOtBu and [{RhCl(nbd)}2] giving the corresponding N-heterocyclic carbene complexes [RhBr(nbd)(oxazolinyl-carbene)] 4 a-j in good yields. X-ray diffraction studies of two of the rhodium complexes, 4 d and 4 j, established a distorted square-pyramidal coordination geometry with the bromo ligand occupying the apical position. The rhodium-carbene bond length was found to be 2.070(4) A (4 d) and 2.012(3) A (4 j). Complexes 4 a-j were treated with AgBF4 in dichloromethane, giving the active cationic square-planar catalysts for the hydrosilylation of ketones. As a reference reaction for the catalyst optimisation, the hydrosilylation of acetophenone with diphenylsilane was studied and the system optimised with respect to the counterion (BF(4) (-)), solvent (THF) and the silane reducing agent (diphenylsilane). The reaction product (1-phenylethanol) was obtained with the highest enantiomeric excess (ee) by carrying out the reaction at -60 degrees C, whilst the enantioselectivity drops upon going both to lower and higher temperatures. The observation that the temperature dependence of the ee values goes through a maximum indicated a change in the rate-determining step as the temperature is varied. The determination of the initial reaction rate in the hydrosilylation of acetophenone upon varying the catalyst (4 d) and substrate concentrations at -55 degrees C

  17. Development of acidity on sol-gel prepared TiO{sub 2}-SiO{sub 2} catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Calvino, J.J.; Cauqui, M.A.; Gatica, J.M.; Perez, J.A.; Rodriguez-Izquierdo, J.M. [Univ. de Cadiz, Puerto Real (Spain)


    Three different TiO{sub 2}-SiO{sub 2} gels (Xerogel, Carbogel and Aerogel) are more active acid catalysts than other reference samples used here. As deduced from FTIR, XRD and XANES studies, the structural properties of these gels are quite different to each other, thus revealing the strong influence of the drying treatment. It is found that the degree of Si-O-Ti linking and the surface acidity follows the same trend (X > C > A). The authors conclude that supercritical drying at 600 K and 190 bars can induce Ti leaching followed by redeposition in the narrower pores of the gel. These effects modify both the textural and surface chemical properties of the resulting material.

  18. Developments in the use of rare earth metal complexes as efficient catalysts for ring-opening polymerization of cyclic esters used in biomedical applications (United States)

    Cota, Iuliana


    Biodegradable polymers represent a class of particularly useful materials for many biomedical and pharmaceutical applications. Among these types of polyesters, poly(ɛ-caprolactone) and polylactides are considered very promising for controlled drug delivery devices. These polymers are mainly produced by ring-opening polymerization of their respective cyclic esters, since this method allows a strict control of the molecular parameters (molecular weight and distribution) of the obtained polymers. The most widely used catalysts for ring-opening polymerization of cyclic esters are tin- and aluminium-based organometallic complexes; however since the contamination of the aliphatic polyesters by potentially toxic metallic residues is particularly of concern for biomedical applications, the possibility of replacing organometallic initiators by novel less toxic or more efficient organometallic complexes has been intensively studied. Thus, in the recent years, the use of highly reactive rare earth initiators/catalysts leading to lower polymer contamination has been developed. The use of rare earth complexes is considered a valuable strategy to decrease the polyester contamination by metallic residues and represents an attractive alternative to traditional organometallic complexes.

  19. Supported metal catalysts for alcohol/sugar alcohol steam reforming. (United States)

    Davidson, Stephen D; Zhang, He; Sun, Junming; Wang, Yong


    Despite extensive studies on hydrogen production via steam reforming of alcohols and sugar alcohols, catalysts typically suffer a variety of issues from poor hydrogen selectivity to rapid deactivation. Here, we summarize recent advances in fundamental understanding of functionality and structure of catalysts for alcohol/sugar alcohol steam reforming, and provide perspectives on further development required to design highly efficient steam reforming catalysts.

  20. Calcined eggshell (CES): An efficient natural catalyst for ...

    Indian Academy of Sciences (India)

    juice as a natural acid catalyst.27. In continuation with our research program concern- ing the development of natural catalysts, we are report- ing here CES as an efficient natural base catalyst for. Knoevenagel condensation of aromatic aldehydes and active methylene compounds (scheme 1). To optimize the reaction ...

  1. Nanostructured Basic Catalysts: Opportunities for Renewable Fuels

    Energy Technology Data Exchange (ETDEWEB)

    Conner, William C; Huber, George; Auerbach, Scott


    This research studied and developed novel basic catalysts for production of renewable chemicals and fuels from biomass. We focused on the development of unique porous structural-base catalysts zeolites. These catalysts were compared to conventional solid base materials for aldol condensation, that were being commercialized for production of fuels from biomass and would be pivotal in future biomass conversion to fuels and chemicals. Specifically, we had studied the aldolpyrolysis over zeolites and the trans-esterification of vegetable oil with methanol over mixed oxide catalysts. Our research has indicated that the base strength of framework nitrogen in nitrogen substituted zeolites (NH-zeolites) is nearly twice as strong as in standard zeolites. Nitrogen substituted catalysts have been synthesized from several zeolites (including FAU, MFI, BEA, and LTL) using NH3 treatment.

  2. Preparation of Heterogeneous CaO Catalysts for Biodiesel Production (United States)

    Widayat, W.; Darmawan, T.; Hadiyanto, H.; Rosyid, R. Ar


    The objective of this research was to develop heterogeneous catalysts from three CaO sources for biodiesel synthesis. The CaO catalyst were prepared from limestone, calcium hydroxide and calciun carbonate with thermal processing in a muffle furnace at 900°C.. The results showed that CaO catalyst from limestone has better characteristic than catalyst from Calcium Hydroxide and Calcium Carbonate. From morphology testing, the CaO catalyst derived from limestone formed a crystal, while The X-ray difraction analysis showed that the amount of CaO contained in limestone was the highest among the others. The yield of biodiesel obtained from the experiment was 89.98% for the catalyst from limestone; 85.15% for the catalyst Ca (OH)2; and 78.71% for CaCO3 catalyst.

  3. New Claus catalyst tests accurately reflect process conditions

    Energy Technology Data Exchange (ETDEWEB)

    Maglio, A.; Schubert, P.F.


    Methods for testing Claus catalysts are developed that more accurately represent the actual operating conditions in commercial sulfur recovery units. For measuring catalyst activity, an aging method has been developed that results in more meaningful activity data after the catalyst has been aged, because all catalysts undergo rapid initial deactivation in commercial units. An activity test method has been developed where catalysts can be compared at less than equilibrium conversion. A test has also been developed to characterize abrasion loss of Claus catalysts, in contrast to the traditional method of determining physical properties by measuring crush strengths. Test results from a wide range of materials correlated well with actual pneumatic conveyance attrition. Substantial differences in Claus catalyst properties were observed as a result of using these tests.

  4. Photocatalytic hydrogen production on SOLECTRO {sup registered} titanium dioxide layers. Development and characterization of an efficient catalyst; Photokatalytische Wasserstoffgewinnung an SOLECTRO {sup registered} -Titandioxidschichten. Entwicklung und Charakterisierung eines geeigneten Katalysators

    Energy Technology Data Exchange (ETDEWEB)

    Saborowski, Sarah


    A catalyst for photocatalytic hydrogen production from methanol and water was developed on the basis of SOLECTRO {sup registered} titanium dioxide layers. A test facility was constructed in which several modified catalysts could be tested for this reaction. Detailed characterization of the electronic and optical characteristics of these catalysts made it possible to gain deeper insight into the processes involved in the reaction. (orig.) [German] Auf Basis der SOLECTRO {sup registered} -TiO{sub 2} -Schichten wurde ein Katalysator fuer die photokatalytische Wasserstoffdarstellung aus Methanol und Wasser entwickelt. Der Aufbau einer geeigneten Versuchsanlage ermoeglichte es, verschieden modifizierte Katalysatoren fuer diese Reaktion zu testen. Durch die ausfuehrliche Charakterisierung insbesondere der elektronischen und optischen Eigenschaften dieser Katalysatoren konnten vertiefende Erkenntnisse zu den waehrend der Reaktion ablaufenden Prozessen gewonnen werden. (orig.)

  5. Process development for the separation and recovery of Mo and Co from chloride leach liquors of petroleum refining catalyst by solvent extraction

    Energy Technology Data Exchange (ETDEWEB)

    Banda, Raju [Department of Advanced Material Science and Engineering, Mokpo National University, Chonnam 534-729 (Korea, Republic of); Sohn, Seong Ho [Korea Institute of Industrial Technology, Incheon Technology Service Centre, 7-47, Songdo-dong, Incheon 406-840 (Korea, Republic of); Lee, Man Seung, E-mail: [Department of Advanced Material Science and Engineering, Mokpo National University, Chonnam 534-729 (Korea, Republic of)


    Highlights: Black-Right-Pointing-Pointer Separation of Mo and Co from HCl solution was investigated by solvent extraction. Black-Right-Pointing-Pointer The solution was synthetic leaching solution of spent HDS catalysts. Black-Right-Pointing-Pointer Extraction with TOPO led to complete separation of Mo. Black-Right-Pointing-Pointer Alamine 308 can separate Co from the Mo free raffinate. Black-Right-Pointing-Pointer Recovery percentage of both metals was higher than 99%. - Abstract: The separation and recovery of Mo and Co from the synthetic chloride leach liquors of petroleum refining catalyst has been investigated by employing TOPO and Alamine 308 as extractants. The synthetic leach liquor contained Mo 394 mg/L, Al 1782 mg/L, Co 119 mg/L in 3 M HCl. The separation of Mo from Co and Al was achieved with 0.05 M TOPO in Escaid 110 and complete stripping of Mo was attained with combination of 0.1 M NH{sub 4}OH and 0.05 M (NH{sub 4}){sub 2}CO{sub 3}. After separation of molybdenum, cobalt can be selectively extracted by Alamine 308 from Mo free raffinate after adjusting the concentration of chloride ion to 5 M by adding AlCl{sub 3}. The back-extraction of cobalt was obtained easily from loaded Alamine 308 with acidified water (pH = 1.0). McCabe-Thiele diagrams were constructed from the extraction and stripping experiments of each element (Mo and Co). From the batch simulation of the counter-current extraction and stripping experiments, it was confirmed that Mo and Co recovery of 99.4% and 99.1% respectively was obtained from the synthetic leach liquor of the chloride solutions. Finally a hydrometallurgical process flow sheet was developed.

  6. Environmentally benign catalysts for clean organic reactions

    CERN Document Server

    Patel, Anjali


    Heterogeneous catalysis attracts researchers and industry because it satisfies most of green chemistry's requirements. Emphasizing the development of third generation catalysts, this book surveys trends and opportunities in academic and industrial research.

  7. Alloy catalyst material

    DEFF Research Database (Denmark)


    The present invention relates to a novel alloy catalyst material for use in the synthesis of hydrogen peroxide from oxygen and hydrogen, or from oxygen and water. The present invention also relates to a cathode and an electrochemical cell comprising the novel catalyst material, and the process use...... of the novel catalyst material for synthesising hydrogen peroxide from oxygen and hydrogen, or from oxygen and water....

  8. Hydroxide catalysts for lignin depolymerization

    Energy Technology Data Exchange (ETDEWEB)

    Beckham, Gregg T.; Biddy, Mary J.; Chmely, Stephen C.; Sturgeon, Matthew


    Solid base catalysts and their use for the base-catalyzed depolymerization (BCD) of lignin to compounds such as aromatics are presented herein. Exemplary catalysts include layered double hydroxides (LDHs) as recyclable, heterogeneous catalysts for BCD of lignin.

  9. Hydroxide catalysts for lignin depolymerization (United States)

    Beckham, Gregg T; Biddy, Mary J.; Kruger, Jacob S.; Chmely, Stephen C.; Sturgeon, Matthew


    Solid base catalysts and their use for the base-catalyzed depolymerization (BCD) of lignin to compounds such as aromatics are presented herein. Exemplary catalysts include layered double hydroxides (LDHs) as recyclable, heterogeneous catalysts for BCD of lignin.

  10. Ceramic catalyst materials

    Energy Technology Data Exchange (ETDEWEB)

    Sault, A.G.; Gardner, T.J. [Sandia National Laboratories, Albuquerque, NM (United States); Hanprasopwattanna, A.; Reardon, J.; Datye, A.K. [Univ. of New Mexico, Albuquerque, NM (United States)


    Hydrous titanium oxide (HTO) ion-exchange materials show great potential as ceramic catalyst supports due to an inherently high ion-exchange capacity which allows facile loading of catalytically active transition metal ions, and an ability to be cast as thin films on virtually any substrate. By coating titania and HTO materials onto inexpensive, high surface area substrates such as silica and alumina, the economics of using these materials is greatly improved, particularly for the HTO materials, which are substantially more expensive in the bulk form than other oxide supports. In addition, the development of thin film forms of these materials allows the catalytic and mechanical properties of the final catalyst formulation to be separately engineered. In order to fully realize the potential of thin film forms of titania and HTO, improved methods for the deposition and characterization of titania and HTO films on high surface area substrates are being developed. By varying deposition procedures, titania film thickness and substrate coverage can be varied from the submonolayer range to multilayer thicknesses on both silica and alumina. HTO films can also be formed, but the quality and reproducibility of these films is not nearly as good as for pure titania films. The films are characterized using a combination of isopropanol dehydration rate measurements, point of zero charge (PZC) measurements, BET surface area, transmission electron microscopy (TEM), and elemental analysis. In order to assess the effects of changes in film morphology on catalytic activity, the films are being loaded with MoO{sub 3} using either incipient wetness impregnation or ion-exchange of heptamolybdate anions followed by calcining. The MoO{sub 3} is then sulfided to form MOS{sub 2}, and tested for catalytic activity using pyrene hydrogenation and dibenzothiophene (DBT) desulfurization, model reactions that simulate reactions occurring during coal liquefaction.

  11. Reducible oxide based catalysts (United States)

    Thompson, Levi T.; Kim, Chang Hwan; Bej, Shyamal K.


    A catalyst is disclosed herein. The catalyst includes a reducible oxide support and at least one noble metal fixed on the reducible oxide support. The noble metal(s) is loaded on the support at a substantially constant temperature and pH.

  12. Fischer-Tropsch Catalysts (United States)

    White, James H. (Inventor); Taylor, Jesse W. (Inventor)


    Catalyst compositions and methods for F-T synthesis which exhibit high CO conversion with minor levels (preferably less than 35% and more preferably less than 5%) or no measurable carbon dioxide generation. F-T active catalysts are prepared by reduction of certain oxygen deficient mixed metal oxides.

  13. Catalyst for Ammonia Oxidation

    DEFF Research Database (Denmark)


    The present invention relates to a bimetallic catalyst for ammonia oxidation, a method for producing a bimetallic catalyst for ammonia oxidation and a method for tuning the catalytic activity of a transition metal. By depositing an overlayer of less catalytic active metal onto a more catalytic...

  14. Nanostructured catalyst supports (United States)

    Zhu, Yimin; Goldman, Jay L.; Qian, Baixin; Stefan, Ionel C.


    The present invention relates to SiC nanostructures, including SiC nanopowder, SiC nanowires, and composites of SiC nanopowder and nanowires, which can be used as catalyst supports in membrane electrode assemblies and in fuel cells. The present invention also relates to composite catalyst supports comprising nanopowder and one or more inorganic nanowires for a membrane electrode assembly.

  15. Catalyst Deactivation 2001

    Energy Technology Data Exchange (ETDEWEB)

    Spivey, J.J. (ed.); Roberts, G.W. (ed.) [Department of Chemical Engineering, 2401 Stinson Avenue, Riddick Engineering Labs, NC State University, Box 7905, Raleigh, NC 27695 (United States); Davis, B.H. (ed.) [University of Kentucky, Centre for Applied Energy Research, 2540 Research Park Drive, Lexington, KY 40511-8433 (United States)


    Selected Papers: Maxted Award Lecture. Whisker carbon revisited (J.R. Rostrup-Nielsen, J Sehested). Carbon Deposition. Various forms of the carbonaceous deposit on the model cobalt catalyst studied in hydrogenation of ethylene (J. Lojewska). Hydrodechlorination of 1,2-dichloropropane over Pt-Cu/C catalysts: coke formation determined by a novel technique-TEOM (Weidung. Zhu et al.). Characterization of structure and combustion behavior of the coke formed on a hydroisomerization catalyst (Jin-an Wang et al.). The effects of pore structure on catalyst deactivation by coke formation (L.D.T. Camara et al.). Coke deactivation of acid sites on ZSM-5 zeolite (G.V. Echevsky et al.). Characterization of the Working Catalyst. Deactivation of a zirconia supported chromia aromatization catalyst investigated by in-situ H-D tracer experiments (H. Ehwald et al.). Deactivation/Regeneration in Environmental Processes. Study of the sintering of a DeNOx commercial catalyst (I. Nova et al.). Deactivation of chromium oxide catalyst for the removal of perchloroethylene (PCE) (Sung Dae Yim et al.). Deactivation/Regeneration in Industrial Processes. Deactivation of Pd-based combustion catalysts supported on modified alumina (P.O. Thevenin et al.). Selective acid-base poisoning on bifunctional alkylation reaction (A. Borgna et al.). Processes occurring during deactivation/regeneration of a vanadia/alumina catalyst under propane dehydrogenation conditions (S David Jackson et al.). Regeneration of supported palladium catalyst for selective hydrogenation of acetylene (L.O. Almanza, O.I. Martinez). Quinone mediated stabilization of a palladium catalyst for the synthesis of hydrogen peroxide from carbon monoxide, water and oxygen (D. Bianchi et al.). Metals on a novel USY zeolite after hydrothermal aging (Huiping Tian et al.). General Papers. Partial oxidation of toluene to benzaldehyde over vanadium antimonate catalysts doped with titanium: The influence (S. Larrondo et al.). Deactivation and

  16. Highly Durable Catalysts for Ignition of Advanced Monopropellants Project (United States)

    National Aeronautics and Space Administration — This proposed SBIR Phase I addresses the development of catalysts and technology for the ignition of advanced monopropellants consisting of mixtures of...

  17. Design of porous nanostructured solid catalysts

    DEFF Research Database (Denmark)

    Abildstrøm, Jacob Oskar

    This thesis aims at developing and characterize novel porous nanostructered materials for heterogeneous catalysis. The catalysts are prepared with the goals of increased activity and stability in mind. This will result in lessened waste of precious elements, starting materials, and energy, for a ...... of reactants. The catalyst is extensively characterize with respect to both the platinum nanoparticles and the carbon shell. Lastly the catalyst is employed in the electrooxidations of methanol, ethanol, and formic acid.......This thesis aims at developing and characterize novel porous nanostructered materials for heterogeneous catalysis. The catalysts are prepared with the goals of increased activity and stability in mind. This will result in lessened waste of precious elements, starting materials, and energy...... conventional counterpart in terms of crystallinity and acidity. Samples of conventional and mesoporous zeolites were tested in a model catalytic reaction. Here, the mesoporous zeolite exhibited much higher conversion, which is contributed to the enhanced diffusion. Chapter 5 explains the fundamentals of fuel...

  18. Study on MEA preparation with CoTETA/C catalysts as ORR catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Gan, T.; Zhang, H.J.; Jiang, Q.Z.; Ma, Z.F. [Shanghai Jiao Tong Univ., Shanghai (China). Dept. of Chemical Engineering


    Although carbon platinum is the most common cathode catalyst for proton exchange membrane fuel cells (PEMFCs) and zinc-air fuel cells, platinum is rare and costly. As such, there is a need to substitute platinum with a new and inexpensive catalyst for the oxygen reduction reaction (ORR). This paper presented a study in which a new non-platinum ORR catalysts was developed, notably the CoTETA/C. Although it demonstrated good performance, it had lower current density. Because of the conductivity and surface wetting properties of CoTETA/C, there was a poor contact between the catalyst layer and membrane of the membrane electrode assembly (MEA) prepared by the traditional method, which resulted in higher contact resistance and lower current density. The study showed that the performance of a single cell can be improved by adjusting the ratio of Nafion and catalyst in ink and adding a specified amount of additives to the ink. 1 ref.

  19. Catalysts, methods of making catalysts, and methods of use

    KAUST Repository

    Renard, Laetitia


    Embodiments of the present disclosure provide for catalysts, methods of making catalysts, methods of using catalysts, and the like. In an embodiment, the method of making the catalysts can be performed in a single step with a metal nanoparticle precursor and a metal oxide precursor, where a separate stabilizing agent is not needed.

  20. Privatization and economic liberalization: The role of the entrepreneur as a catalyst for economic development in transition economies

    NARCIS (Netherlands)

    Dibrell, Clay; Englis-Danskin, Paula; Kedia, Ben L.; Lakatos, Gergo M.


    Many nations with transition economies are attempting to develop their national competitiveness through such processes as privatisation of state owned enterprises (SOEs) and/or the use of economic liberalisation (e.g. lessening of tariffs, industry regulations, etc.) to spur economic growth and

  1. Consonance and Dissonance in a Study Abroad Program as a Catalyst for Professional Development of Pre-Service Teachers (United States)

    Brindley, Roger; Quinn, Suzanne; Morton, Mary Lou


    This research examines the experiences of elementary and early childhood pre-service teachers from the U.S. engaged in a month long study abroad internship program in England. Using data from participants written journals, we use a hermeneutic approach to interrogate their evolving sense of professional development and their understanding of…

  2. Catalyst in Basic Oleochemicals

    Directory of Open Access Journals (Sweden)

    Eva Suyenty


    Full Text Available Currently Indonesia is the world largest palm oil producer with production volume reaching 16 million tones per annum. The high crude oil and ethylene prices in the last 3 – 4 years contribute to the healthy demand growth for basic oleochemicals: fatty acids and fatty alcohols. Oleochemicals are starting to replace crude oil derived products in various applications. As widely practiced in petrochemical industry, catalyst plays a very important role in the production of basic oleochemicals. Catalytic reactions are abound in the production of oleochemicals: Nickel based catalysts are used in the hydrogenation of unsaturated fatty acids; sodium methylate catalyst in the transesterification of triglycerides; sulfonic based polystyrene resin catalyst in esterification of fatty acids; and copper chromite/copper zinc catalyst in the high pressure hydrogenation of methyl esters or fatty acids to produce fatty alcohols. To maintain long catalyst life, it is crucial to ensure the absence of catalyst poisons and inhibitors in the feed. The preparation methods of nickel and copper chromite catalysts are as follows: precipitation, filtration, drying, and calcinations. Sodium methylate is derived from direct reaction of sodium metal and methanol under inert gas. The sulfonic based polystyrene resin is derived from sulfonation of polystyrene crosslinked with di-vinyl-benzene. © 2007 BCREC UNDIP. All rights reserved.[Presented at Symposium and Congress of MKICS 2007, 18-19 April 2007, Semarang, Indonesia][How to Cite: E. Suyenty, H. Sentosa, M. Agustine, S. Anwar, A. Lie, E. Sutanto. (2007. Catalyst in Basic Oleochemicals. Bulletin of Chemical Reaction Engineering and Catalysis, 2 (2-3: 22-31.  doi:10.9767/bcrec.2.2-3.6.22-31][How to Link/DOI: || or local:


    DEFF Research Database (Denmark)


    The present invention concerns the selective removal of nitrogen oxides (NOx) from gasses. In particular, the invention concerns a process, a catalyst and the use of a catalyst for the selective removal of nitrogen oxides in the presence of ammonia from gases containing a significant amount...... of alkali metal and/or alkali-earth compounds which process comprises using a catalyst combined of (i) a formed porous superacidic support, said superacidic support having an Hammett acidity stronger than Ho=-12, and (ii) a metal oxide catalytic component deposited on said superacidic support selected from...

  4. Mechanistic studies aimed at the development of single site metal alkoxide catalysts for the production of polyoxygenates from renewable resources.

    Energy Technology Data Exchange (ETDEWEB)

    Chisholm, Malcolm H. [The Ohio State Univ., Columbus, OH (United States)


    The work proposed herein follows on directly from the existing 3 year grant and the request for funding is for 12 months to allow completion of this work and graduation of current students supported by DOE. The three primary projects are as follows. 1.) A comparative study of the reactivity of LMg(OR) (solvent), where L= a β-diiminate or pyrromethene ligand, in the ring-opening of cyclic esters. 2.) The homopolymerization of expoxides, particularly propylene oxide and styrene oxide, and their copolymerizations with carbon dioxide or organic anhydrides to yield polycarbonates or polyesters, respectively. 3.) The development of well-defined bismuth (III) complexes for ring-opening polymerizations that are tolerant of both air and water. In each of these topics special emphasis is placed on developing a detailed mechanistic understanding of the ring-opening event and how this is modified by the employment of specific metal and ligand combinations. This document also provides a report on findings of the past grant period that are not yet in the public domain/published and shows how the proposed work will bring the original project to conclusion.

  5. Epoxidation catalyst and process (United States)

    Linic, Suljo; Christopher, Phillip


    Disclosed herein is a catalytic method of converting alkenes to epoxides. This method generally includes reacting alkenes with oxygen in the presence of a specific silver catalyst under conditions suitable to produce a yield of the epoxides. The specific silver catalyst is a silver nanocrystal having a plurality of surface planes, a substantial portion of which is defined by Miller indices of (100). The reaction is performed by charging a suitable reactor with this silver catalyst and then feeding the reactants to the reactor under conditions to carry out the reaction. The reaction may be performed in batch, or as a continuous process that employs a recycle of any unreacted alkenes. The specific silver catalyst has unexpectedly high selectivity for epoxide products. Consequently, this general method (and its various embodiments) will result in extraordinarily high epoxide yields heretofore unattainable.

  6. Catalyst for microelectromechanical systems microreactors (United States)

    Morse, Jeffrey D [Martinez, CA; Sopchak, David A [Livermore, CA; Upadhye, Ravindra S [Pleasanton, CA; Reynolds, John G [San Ramon, CA; Satcher, Joseph H [Patterson, CA; Gash, Alex E [Brentwood, CA


    A microreactor comprising a silicon wafer, a multiplicity of microchannels in the silicon wafer, and a catalyst coating the microchannels. In one embodiment the catalyst coating the microchannels comprises a nanostructured material. In another embodiment the catalyst coating the microchannels comprises an aerogel. In another embodiment the catalyst coating the microchannels comprises a solgel. In another embodiment the catalyst coating the microchannels comprises carbon nanotubes.

  7. Synergistic effect of UV pretreated Fe-ZSM-5 catalysts for heterogeneous catalytic complete oxidation of VOC: A technology development for sustainable use. (United States)

    Aziz, Abdul; Kim, Kwang Soo


    In this work, the performance of benzene, toluene, ethylbenzene, and xylene (BTEX) removal and degradation from gas, air streams on UV pretreated Fe-ZSM-5 in a batch reactor at room temperature were studied. The Fe-ZSM-5 zeolite catalyst was prepared by hydrothermal reaction method. The influence of UV pre-irradiation time on the removal of BTEX were assessed by varying the time, ranging from 15min to 60smin. Then, sustainability of the activation of the catalyst resulted by UV pretreatment was studied by the four-cycle experiment with one time UV irradiation and after each cycle irradiation followed by BTEX removal after every cycle respectively. The results of BTEX removal depicted that 30min of UV pretreatment was sufficient for complete organics removal. The UV pretreatment effect on the catalytic oxidation and the stability of the catalyst were studied by modern instrumental techniques. The novelty of the process was the sustainable reuse of catalyst with persistent VOC removal, which works on the -adsorption-oxidation-regeneration-adsorption- cycle, which was confirmed by the characterization studies of the catalyst after four runs. The results revealed that the change in the structure, stability, morphology, and removal efficiency of the catalyst during the experiments was negligible. The VOC degradation mechanism studies showed that the oxidation occurs due to the formation of free radicals as well as hydroxyl ions, so named it heterogeneous photo-Fenton oxidation. The residual materials analysis showed the complete mineralization of VOC except small amount of acetone as oxidation product. Lastly, the kinetics of the VOC removal was studied. Copyright © 2017 Elsevier B.V. All rights reserved.

  8. Heterogeneous chromium catalysts



    The present invention relates to a heterogeneous chromium catalyst system for the polymerisation of ethylene and/or alpha olefins prepared by the steps of: (a) providing a silica-containing support, (b) treating the silica-containing support with a chromium compound to form a chromium-based silica-containing support, (c) activating the chromium-based silica-containing support, (d) chemically reducing the activated chromium-based silica-containing support to produce a precursor catalyst, (e) r...

  9. Catalyst system comprising a first catalyst system tethered to a supported catalyst (United States)

    Angelici, Robert J.; Gao, Hanrong


    The present invention provides new catalyst formats which comprise a supported catalyst tethered to a second and different catalyst by a suitable tethering ligand. A preferred system comprises a heterogeneous supported metal catalyst tethered to a homogeneous catalyst. This combination of homogeneous and heterogeneous catalysts has a sufficient lifetime and unusually high catalytic activity in arene hydrogenations, and potentially many other reactions as well, including, but not limited to hydroformylation, hydrosilation, olefin oxidation, isomerization, hydrocyanation, olefin metathesis, olefin polymerization, carbonylation, enantioselective catalysis and photoduplication. These catalysts are easily separated from the products, and can be reused repeatedly, making these systems very economical.

  10. Development of new heterogeneous catalysts for the decomposition of methanol into hydrogen and carbon monoxide applying high throughput methods; Entwicklung neuer heterogener Katalysatoren zur Spaltung von Methanol in Wasserstoff und Kohlenmonoxid mittels Hochdurchsatz-Methoden

    Energy Technology Data Exchange (ETDEWEB)

    Weiss, Torsten


    The topic of this thesis has been the development of new heterogeneous catalysts for the decomposition of methanol into hydrogen and carbon monoxide. As an important constraint here, the content of noble metals of the catalysts should be as low as possible. High-throughput-methods were applied in some of the syntheses and experiments to accelerate the development, as, for example, the use of liquid based sol-gel syntheses and the examination of catalyst libraries by spatial resolution gas chromatography. This screening technique allowed to test up to 207 different substances during one single experiment. Then, different combinatorial strategies were applied. First, these methods led to a highly active and stable catalyst in the ternary system of Cu-Ni-Zn, which showed high conversion and selectivity comparable to an industrial reference catalyst. Its activity during an 18 hour long term run was constant in contrast to the reference. Second, an additional approach starting from a broader variety of elements led to a Ce- Ru- and to a Cr-Ru-catalyst. Both of them were highly active in short term experiments, but lost their outstanding performances during long term runs. (orig.) [German] Die vorliegende Arbeit befasste sich mit der Entwicklung neuer heterogener Katalysatoren fuer die Spaltung von Methanol zu Wasserstoff und Kohlenmonoxid, die einen moeglichst geringen Gehalt an Edelmetallen aufweisen sollten. Um diesen Prozess zu beschleunigen, wurden in einem Teil der Synthesen und Experimente Hochdurchsatzmethoden verwendet. Neben der Roboter gestuetzten Sol-Gel-Synthese umfasste dies die Untersuchung von Katalysatorbibliotheken mittels ortsaufgeloester Gaschromatographie, die es ermoeglichte, in einem Experiment bis zu 207 verschiedene Substanzen auf ihre katalytische Aktivitaet zu testen. Unter Anwendung verschiedener kombinatorischer Strategien wurde zunaechst ein sehr aktiver und stabiler Katalysator im ternaeren Cu-Ni-Zn-System entdeckt. Neben Umsaetzen und

  11. Catalyst and Fuel Interactions to Optimize Endothermic Cooling (United States)


    AFRL-AFOSR-VA-TR-2016-0315 Catalyst and Fuel Interactions to Optimize Endothermic Cooling Scott Anderson UNIVERSITY OF UTAH SALT LAKE CITY 201...Technical Report 3. DATES COVERED (From - To) 30-09-2012 to 31-05-2016 4. TITLE AND SUBTITLE Catalyst and Fuel Interactions to Optimize Endothermic...developing improved catalysts to enhance and control endothermic fuel reactions, to enhance cooling capacity for aircraft. In addition there was

  12. Chelated ruthenium catalysts for Z-selective olefin metathesis. (United States)

    Endo, Koji; Grubbs, Robert H


    We report the development of ruthenium-based metathesis catalysts with chelating N-heterocyclic carbene (NHC) ligands that catalyze highly Z-selective olefin metathesis. A very simple and convenient procedure for the synthesis of such catalysts has been developed. Intramolecular C-H bond activation of the NHC ligand, promoted by anion ligand substitution, forms the appropriate chelate for stereocontrolled olefin metathesis.

  13. The innovation catalysts. (United States)

    Martin, Roger L


    A few years ago the software development company Intuit realized that it needed a new approach to galvanizing customers. The company's Net Promoter Score was faltering, and customer recommendations of new products were especially disappointing. Intuit decided to hold a two-day, off-site meeting for the company's top 300 managers with a focus on the role of design in innovation. One of the days was dedicated to a program called Design for Delight. The centerpiece of the day was a PowerPoint presentation by Intuit founder Scott Cook, who realized midway through that he was no Steve Jobs: The managers listened dutifully, but there was little energy in the room. By contrast, a subsequent exercise in which the participants worked through a design challenge by creating prototypes, getting feedback, iterating, and refining, had them mesmerized. The eventual result was the creation of a team of nine design-thinking coaches--"innovation catalysts"--from across Intuit who were made available to help any work group create prototypes, run experiments, and learn from customers. The process includes a "painstorm" (to determine the customer's greatest pain point), a "soljam" (to generate and then winnow possible solutions), and a "code-jam" (to write code "good enough" to take to customers within two weeks). Design for Delight has enabled employees throughout Intuit to move from satisfying customers to delighting them.

  14. A further step toward H2 in automobile : development of an efficient bi-functional catalyst for single stage water gas shift

    NARCIS (Netherlands)

    Azzam, K.G.H.


    The suitability of polymer electrolyte fuel (PEM) cells for stationary and vehicular applications initiated research in all areas of fuel processor (i.e. reformer, water-gas-shift, preferential oxidation of CO (PROX)) catalysts for hydrogen generation. Water gas shift (WGS) reaction is an essential

  15. Development of a high-performance nanostructured V(sub2)O(sub5)/SnO(sub2)catalyst for efficient benzene hydroxylation

    CSIR Research Space (South Africa)

    Makgwane, PR


    Full Text Available Nanostructured vanadium-tin oxide (V(sub2)O(sub5)/SnO(sub2)) catalysts with V(sub2)O(sub5) loading in a range of 5–20 wt% have been synthesized. The V(sub2)O(sub5)/SnO(sub2) nanostructures exhibited effective catalytic performance...


    Energy Technology Data Exchange (ETDEWEB)

    Hoard, J; Schmieg, S; Brooks, D; Peden, C; Barlow, S; Tonkyn, R


    A three-stage plasma-catalyst system was developed and tested on an engine dynamometer. Previous laboratory testing suggested high NOx efficiency could be obtained. With hexene reductant added to the exhaust, over 90% NOx reduction was observed. However, with diesel or Fischer-Tropsch reductant the catalyst efficiency rapidly dropped off. Heating the catalyst in air removed brown deposit from the surface and restored conversion efficiency. Following the engine tests, the used catalysts were evaluated. BET surface area decreased, and TPD revealed significant storage. This storage appears to be partly unburned diesel fuel that can be removed by heating to around 250-300 C, and partly hydrocarbons bonded to the surface that remain in place until 450-500 C. Laboratory testing with propene reductant demonstrated that the catalyst regains efficiency slowly even when operating temperature does not exceed 300 C. This suggests that control strategies may be able to regenerate the catalyst by occasional moderate heating.

  17. Core-shell nanostructured catalysts. (United States)

    Zhang, Qiao; Lee, Ilkeun; Joo, Ji Bong; Zaera, Francisco; Yin, Yadong


    Novel nanotechnologies have allowed great improvements in the syn-thesis of catalysts with well-controlled size, shape, and surface properties. Transition metal nanostructures with specific sizes and shapes, for instance, have shown great promise as catalysts with high selectivities and relative ease of recycling. Researchers have already demonstrated new selective catalysis with solution-dispersed or supported-metal nanocatalysts, in some cases applied to new types of reactions. Several challenges remain, however, particularly in improving the structural stability of the catalytic active phase. Core-shell nanostructures are nanoparticles encapsulated and protected by an outer shell that isolates the nanoparticles and prevents their migration and coalescence during the catalytic reactions. The synthesis and characterization of effective core-shell catalysts has been at the center of our research efforts and is the focus of this Account. Efficient core-shell catalysts require porous shells that allow free access of chemical species from the outside to the surface of nanocatalysts. For this purpose, we have developed a surface-protected etching process to prepare mesoporous silica and titania shells with controllable porosity. In certain cases, we can tune catalytic reaction rates by adjusting the porosity of the outer shell. We also designed and successfully applied a silica-protected calcination method to prepare crystalline shells with high surface area, using anatase titania as a model system. We achieved a high degree of control over the crystallinity and porosity of the anatase shells, allowing for the systematic optimization of their photocatalytic activity. Core-shell nanostructures also provide a great opportunity for controlling the interaction among the different components in ways that might boost structural stability or catalytic activity. For example, we fabricated a SiO₂/Au/N-doped TiO₂ core-shell photocatalyst with a sandwich structure that showed

  18. Heterogeneities of the Nanostructure of Platinum/Zeolite Y Catalysts Revealed by Electron Tomography

    NARCIS (Netherlands)

    Zecevic, J.|info:eu-repo/dai/nl/341386715; van der Eerden, A.M.J.|info:eu-repo/dai/nl/304840483; Friedrich, H.|info:eu-repo/dai/nl/304837350; de Jongh, P.E.|info:eu-repo/dai/nl/186125372; de Jong, K.P.|info:eu-repo/dai/nl/06885580X


    To develop structure–performance relationships for important catalysts, a detailed characterization of their morphology is essential. Using electron tomography, we determined in three dimensions the structure of Pt/zeolite Y bifunctional catalysts. Optimum experimental conditions enabled for the

  19. Selective Oxidations using Nanostructured Heterogeneous Catalysts

    DEFF Research Database (Denmark)

    Mielby, Jerrik Jørgen

    and because they produce H2O as the only by-product. Chapter 1 gives a short introduction to basic concepts in heterogeneous catalysis and green chemistry. Furthermore, the chapter gives an overview of the most important strategies to synthesise functional nanostructured materials and highlights how detailed......The aim of this thesis is to investigate and develop new efficient methods to oxidise alcohols and amines using heterogeneous catalysts and either O2 or H2O2 as oxidants. From an economic and environmental point of view, these oxidants are ideal, because they are cheap and readily available...... understanding of size, shape and structure can help in the development of new and more efficient heterogeneous catalysts. The chapter is not intended to give a complete survey, but rather to introduce some of the recent developments in the synthesis of nanostructured heterogeneous catalysts. Finally...

  20. New catalysts for exhaust gas cleaning

    Energy Technology Data Exchange (ETDEWEB)

    Haerkoenen, M. [Kemira Metalkat Oy, Oulu (Finland)


    Major challenge for future catalyst systems was to develop thermally more stable washcoats for close coupled operating conditions and for engines operating under high speed and load conditions. To design these future emission systems extensive research and development was undertaken to develop methods to disperse and stabilize the key catalytic materials for operation at much higher temperatures. Second priority was to design catalysts that are more effective under low temperature exhaust conditions and have improved oxygen storage properties in the washcoats. Incorporating new materials and modified preparation technology a new generation of metallic catalyst formulations emerged, those being trimetallic K6 (Pt:Pd:Rh and bimetallic K7) (Pd+Pd:Rh). The target was to combine the best property of Pt:Rh (good NO{sub x} reduction) with that of the good HC oxidation activity of Pd and to ensure that precious metal/support interactions were positively maintained. Both K6 and K7 concepts contain special catalyst structures with optimized washcoat performance which can be brick converter configuration. Improvement in light-off, thermal stability and transient performance with these new catalyst formulations have clearly been shown in both laboratory and vehicle testing. (author) (20 refs.)

  1. Mesoporous molecular sieve catalysts

    DEFF Research Database (Denmark)

    Højholt, Karen Thrane

    This thesis deals with a very specific class of molecular sieves known as zeolites. Zeolites are a class of crystalline aluminosilicates characterised by pores or cavities of molecular dimensions as part of their crystal structure. In this work zeolites were modified for the use and understanding...... of different catalytic applications. Primarily the zeolites were modified regarding the porosity and the introduction of metals to the framework. The obtained materials were used as solid acid catalysts, as an inert matrix for stabilising metal nanoparticles and as an anchoring material for molecular metal...... be used as solid acid catalysts but can also be used as a size-selective matrix. It was shown that it is possible to encapsulate 1-2 nm sized gold nanoparticles by silicalite-1 or ZSM-5 zeolite crystals thereby forming a sintering-stable and substrate size-selective oxidation catalyst. After carrying out...

  2. Dynamics of Catalyst Nanoparticles

    DEFF Research Database (Denmark)

    Hansen, Thomas Willum; Cavalca, Filippo; Wagner, Jakob Birkedal

    under gas exposure, dynamic phenomena such as sintering and growth can be observed with sub-Ångstrøm resolution. Metal nanoparticles contain the active sites in heterogeneous catalysts, which are important for many industrial applications including the production of clean fuels, chemicals...... and pharmaceuticals, and the cleanup of exhaust from automobiles and stationary power plants. Sintering, or thermal deactivation, is an important mechanism for the loss of catalyst activity. In order to initiate a systematic study of the dynamics and sintering of nanoparticles, various catalytic systems have been...... that particle sintering is not solely governed by the mechanisms previously proposed. These results are divided into the different phases of the catalyst lifetime....

  3. Catalyst, method of making, and reactions using the catalyst (United States)

    Tonkovich, Anna Lee Y [Pasco, WA; Wang, Yong [Richland, WA; Gao, Yufei [Kennewick, WA


    The present invention includes a catalyst having a layered structure with, (1) a porous support, (2) a buffer layer, (3) an interfacial layer, and optionally (4) a catalyst layer. The invention also provides a process in which a reactant is converted to a product by passing through a reaction chamber containing the catalyst.

  4. Olefin metathesis catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Kukes, S.G.; Banks, R.L.


    A process is described for preparing a disproportionation catalyst comprising admixing a catalytically effective amount of a calcined and activated catalyst consisting essentially of at least one metal oxide selected from molybdenum oxide and tungsten oxide and a support containing a major proportion of silica or alumina with a promoting amount of a methylating agent selected from the group consisting of dimethyl sulfate, dimethylsulfoxide, trimethyloxonium tetrafluorborate, methyl iodide, and methyl bromide, and subjecting same to inert atmospheric conditions for the methylating agent to promote the activity of the calcined molybdenum and tungsten oxides for the disproportionation of olefins.

  5. Fuel cell catalyst degradation

    DEFF Research Database (Denmark)

    Arenz, Matthias; Zana, Alessandro


    Fuel cells are an important piece in our quest for a sustainable energy supply. Although there are several different types of fuel cells, the by far most popular is the proton exchange membrane fuel cell (PEMFC). Among its many favorable properties are a short start up time and a high power density...... increasing focus. Activity of the catalyst is important, but stability is essential. In the presented perspective paper, we review recent efforts to investigate fuel cell catalysts ex-situ in electrochemical half-cell measurements. Due to the amount of different studies, this review has no intention to give...


    Energy Technology Data Exchange (ETDEWEB)

    Dr. Dragomir B. Bukur; Dr. Ketil Hanssen; Alec Klinghoffer; Dr. Lech Nowicki; Patricia O' Dowd; Dr. Hien Pham; Jian Xu


    This report describes research conducted to support the DOE program in novel slurry phase catalysts for converting coal-derived synthesis gas to diesel fuels. The primary objective of this research program is to develop attrition resistant catalysts that exhibit high activities for conversion of coal-derived syngas.

  7. Supported organometallic catalysts for hydrogenation and Olefin Polymerization (United States)

    Marks, Tobin J.; Ahn, Hongsang


    Novel heterogeneous catalysts for the which hydrogenation of olefins and arenes with high conversion rates under ambient conditions and the polymerization of olefins have been developed. The catalysts are synthesized from Ziegler-type precatalysts by supporting them on sulfate-modified zirconia.

  8. Nanoscale intimacy in bifunctional catalysts for selective conversion of hydrocarbons

    NARCIS (Netherlands)

    Zecevic, Jovana|info:eu-repo/dai/nl/341386715; Vanbutsele, Gina; de Jong, Krijn P.|info:eu-repo/dai/nl/06885580X; Martens, Johan A.


    The ability to control nanoscale features precisely is increasingly being exploited to develop and improve monofunctional catalysts(1-4). Striking effects might also be expected in the case of bifunctional catalysts, which are important in the hydrocracking of fossil and renewable hydrocarbon

  9. Biomimetic Water-Oxidation Catalysts: Manganese Oxides. (United States)

    Kurz, Philipp


    The catalytic oxidation of water to molecular oxygen is a key process for the production of solar fuels. Inspired by the biological manganese-based active site for this reaction in the enzyme Photosystem II, researchers have made impressive progress in the last decades regarding the development of synthetic manganese catalysts for water oxidation. For this, it has been especially fruitful to explore the many different types of known manganese oxides MnOx. This chapter first offers an overview of the structural, thermodynamic, and mechanistic aspects of water-oxidation catalysis by MnOx. The different test systems used for catalytic studies are then presented together with general reactivity trends. As a result, it has been possible to identify layered, mixed Mn (III/IV)-oxides as an especially promising class of bio-inspired catalysts and an attempt is made to give structure-based reasons for the good performances of these materials. In the outlook, the challenges of catalyst screenings (and hence the identification of a "best MnOx catalyst") are discussed. There is a great variety of reaction conditions which might be relevant for the application of manganese oxide catalysts in technological solar fuel-producing devices, and thus catalyst improvements are currently still addressing a very large parameter space. Nonetheless, detailed knowledge about the biological catalyst and a solid experimental basis concerning the syntheses and water-oxidation reactivities of MnOx materials have been established in the last decade and thus this research field is well positioned to make important contributions to solar fuel research in the future.

  10. Walkable new urban LEED_Neighborhood-Development (LEED-ND community design and children's physical activity: selection, environmental, or catalyst effects?

    Directory of Open Access Journals (Sweden)

    Stevens, Robert B


    Full Text Available Abstract Background Interest is growing in physical activity-friendly community designs, but few tests exist of communities explicitly designed to be walkable. We test whether students living in a new urbanist community that is also a pilot LEED_ND (Leadership in Energy and Environmental Design-Neighborhood Development community have greater accelerometer-measured moderate-to-vigorous physical activity (MVPA across particular time periods compared to students from other communities. We test various time/place periods to see if the data best conform to one of three explanations for MVPA. Environmental effects suggest that MVPA occurs when individuals are exposed to activity-friendly settings; selection effects suggest that walkable community residents prefer MVPA, which leads to both their choice of a walkable community and their high levels of MVPA; catalyst effects occur when walking to school creates more MVPA, beyond the school commute, on schooldays but not weekends. Methods Fifth graders (n = 187 were sampled from two schools representing three communities: (1 a walkable community, Daybreak, designed with new urbanist and LEED-ND pilot design standards; (2 a mixed community (where students lived in a less walkable community but attended the walkable school so that part of the route to school was walkable, and (3 a less walkable community. Selection threats were addressed through controlling for parental preferences for their child to walk to school as well as comparing in-school MVPA for the walkable and mixed groups. Results Minutes of MVPA were tested with 3 × 2 (Community by Gender analyses of covariance (ANCOVAs. Community walkability related to more MVPA during the half hour before and after school and, among boys only, more MVPA after school. Boys were more active than girls, except during the half hour after school. Students from the mixed and walkable communities--who attended the same school--had similar in-school MVPA levels, and

  11. Precious metal compounds and recovery. Fischer-Tropsch catalysts and catalysts for hydroformylation and oxo processes

    Energy Technology Data Exchange (ETDEWEB)

    Schapp, J.; Arndt, M. [W.C. Heraeus GmbH, Hanau (Germany); Meyer, H. [Heraeus Metal Processing Inc., Santa Fe Springs, CA (United States)


    Solid-phase Fischer-Tropsch catalysts, which are used in the emerging field of interest known as ''Gas-to-Liquid'' (GTL), consist to a high percentage of cobalt. In addition, they contain on a value basis, a considerable amount of platinum group metals or rhenium as promoters. Therefore, there is an imperative need for economically feasible recycling processes triggered not only by the value of the metals in spent Fischer-Tropsch catalysts, but also by the potentially limited availability of promoters like rhenium. Heraeus, as a precious metal expert, is supporting this important technology with its profound know-how in developing tailor-made hydrometallurgical recycling processes for all kinds of catalyst systems. Besides giving an overview of state-of-the-art recovery processes, this paper will clarify the economic and environmental aspects involved. Hydroformylation and oxo processes are technologies which consume a major percentage of homogeneous catalysts worldwide. The focus lies on organometallic compounds with rhodium as the catalytic center. With significant rises of the rhodium price, many companies are being pushed to look more closely at the involved recycling terms. Accordingly, Heraeus is proud to offer its HeraCYCLE {sup registered} recovery process recently developed for homogeneous catalysts in particular. Furthermore, Heraeus manufactures the required quantities of fresh homogeneous catalysts ensuring highest quality standards. Key economic, technical, and environmental aspects of the precious metal loops will be covered by this paper. (orig.)

  12. Development of Fe-Ni/YSZ-GDC electro-catalysts for application as SOFC anodes. XRD and TPR characterization, and evaluation in ethanol steam reforming reaction

    Energy Technology Data Exchange (ETDEWEB)

    Paz Fiuza, Raigenis da; Silva, Marcos Aurelio da; Boaventura, Jaime Soares [UFBA, Salvador, Bahia (Brazil). Energy and Materials Science Group


    Electro-catalysts based on Fe-Ni alloys were prepared using physical mixture and modified Pechini methods; they were supported on a composite of Yttria Stabilized Zirconia (YSZ) and Gadolinia Doped Ceria (GDC). The composites had compositions of 35% metal load and 65% support (70% wt. YSZ and 30% wt. GDC mixture) (cermets). The samples were characterized by Temperature-Programmed Reduction (TPR) and X-Ray Diffraction (XRD) and evaluated in ethanol steam reforming at 650 C for six hours and in the temperature range 300 - 900 C. The XRD results showed that the bimetallic sample calcined at 800 C formed a mixed oxide (NiFe{sub 2}O{sub 4}) in spinel structure; after reducing the sample in hydrogen, Ni-Fe alloys were formed. The presence of Ni decreased the final reduction temperature of the NiFe{sub 2}O{sub 4} species. The addition of Fe to Ni anchored to YSZ-GDC increased the hydrogen production and inhibits the carbon deposition. The bimetallic 30Fe5Ni samples reached an ethanol conversion of about 95%, and a hydrogen yield up to 48% at 750 C. In general, the ethanol conversion and hydrogen production were independent of the metal content in the electro-catalyst. However, the substitution of Ni for Fe significantly reduced the carbon deposition on the electro-catalyst: 74, 31 and 9 wt. % in the 35Ni, 20Fe15Ni, and 30Fe5Ni samples, respectively. (orig.)

  13. Deactivation-resistant catalyst for selective catalyst reduction of NOx

    DEFF Research Database (Denmark)


    The present invention relates to a catalyst for selective catalytic reduction of NOx in alkali metal containing flue gas using ammonia as reductant, the catalyst comprising a surface with catalytically active sites, wherein the surface is at least partly coated with a coating comprising at least...... one metal oxide. In another aspect the present invention relates to the use of said catalyst and to a method of producing said catalyst. In addition, the present invention relates to a method of treating an catalyst for conferring thereon an improved resistance to alkali poisoning....

  14. CATALYSTS NHI Thermochemical Systems FY 2009 Year-End Report

    Energy Technology Data Exchange (ETDEWEB)

    Daniel M. Ginosar


    Fiscal Year 2009 work in the Catalysts project focused on advanced catalysts for the decomposition of sulfuric acid, a reaction common to both the Sulfur-Iodine (S-I) cycle and the Hybrid Sulfur cycle. Prior years’ effort in this project has found that although platinum supported on titanium oxide will be an acceptable catalyst for sulfuric acid decomposition in the integrated laboratory scale (ILS) project, the material has short comings, including significant cost and high deactivation rates due to sintering and platinum evaporation. For pilot and larger scale systems, the catalyst stability needs to be improved significantly. In Fiscal Year 2008 it was found that at atmospheric pressure, deactivation rates of a 1 wt% platinum catalyst could be reduced by 300% by adding either 0.3 wt% iridium (Ir) or 0.3 wt% ruthenium (Ru) to the catalyst. In Fiscal Year 2009, work focused on examining the platinum group metal catalysts activity and stability at elevated pressures. In addition, simple and complex metal oxides are known to catalyze the sulfuric acid decomposition reaction. These metal oxides could offer activities comparable to platinum but at significantly reduced cost. Thus a second focus for Fiscal Year 2009 was to explore metal oxide catalysts for the sulfuric acid decomposition reaction. In Fiscal Year 2007 several commercial activated carbons had been identified for the HI decomposition reaction; a reaction specific to the S-I cycle. Those materials should be acceptable for the pilot scale project. The activated carbon catalysts have some disadvantages including low activity at the lower range of reactor operating temperature (350 to 400°C) and a propensity to generate carbon monoxide in the presence of water that could contaminate the hydrogen product, but due to limited funding, this area had low priority in Fiscal Year 2009. Fiscal Year 2009 catalyst work included five tasks: development, and testing of stabilized platinum based H2SO4 catalysts

  15. Heterogeneous chromium catalysts

    NARCIS (Netherlands)


    The present invention relates to a heterogeneous chromium catalyst system for the polymerisation of ethylene and/or alpha olefins prepared by the steps of: (a) providing a silica-containing support, (b) treating the silica-containing support with a chromium compound to form a chromium-based

  16. Olefin metathesis and catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Kukes, S. G.; Banks, R. L.


    Olefins are converted into other olefins having different numbers of carbon atoms by contact with a catalyst comprising an inorganic refractory oxide support containing at least one of tungsten oxide and molybdenum oxide and a promoting amount of at least one methylating agent under conditions suitable for the methylating agent compounds to promote the activity of tungsten and molybdenum oxides for the disproportionation reaction.

  17. Sabatier Catalyst Poisoning Investigation (United States)

    Nallette, Tim; Perry, Jay; Abney, Morgan; Knox, Jim; Goldblatt, Loel


    The Carbon Dioxide Reduction Assembly (CRA) on the International Space Station (ISS) has been operational since 2010. The CRA uses a Sabatier reactor to produce water and methane by reaction of the metabolic CO2 scrubbed from the cabin air and the hydrogen byproduct from the water electrolysis system used for metabolic oxygen generation. Incorporating the CRA into the overall air revitalization system has facilitated life support system loop closure on the ISS reducing resupply logistics and thereby enhancing longer term missions. The CRA utilizes CO2 which has been adsorbed in a 5A molecular sieve within the Carbon Dioxide Removal Assembly, CDRA. There is a potential of compounds with molecular dimensions similar to, or less than CO2 to also be adsorbed. In this fashion trace contaminants may be concentrated within the CDRA and subsequently desorbed with the CO2 to the CRA. Currently, there is no provision to remove contaminants prior to entering the Sabatier catalyst bed. The risk associated with this is potential catalyst degradation due to trace organic contaminants in the CRA carbon dioxide feed acting as catalyst poisons. To better understand this risk, United Technologies Aerospace System (UTAS) has teamed with MSFC to investigate the impact of various trace contaminants on the CRA catalyst performance at relative ISS cabin air concentrations and at about 200/400 times of ISS concentrations, representative of the potential concentrating effect of the CDRA molecular sieve. This paper summarizes our initial assessment results.

  18. Hydrogen evolution reaction catalyst (United States)

    Subbaraman, Ram; Stamenkovic, Vojislav; Markovic, Nenad; Tripkovic, Dusan


    Systems and methods for a hydrogen evolution reaction catalyst are provided. Electrode material includes a plurality of clusters. The electrode exhibits bifunctionality with respect to the hydrogen evolution reaction. The electrode with clusters exhibits improved performance with respect to the intrinsic material of the electrode absent the clusters.

  19. Synthesis of supported catalysts

    NARCIS (Netherlands)

    Jong, Krijn P. de


    Research reports on the synthesis of supported catalysts during the review period (1997-1998) have shown the use of carbon nanotubes and new hetropolyanions as examples of novel supports and of novel precursors of active components, respectively. Studies of absorption and precipitation chemistry

  20. Synthesis of the catalyst

    Indian Academy of Sciences (India)


    50 585; Duan Y C, Ma Y C, Zhang E, Shi X J, Wang M M, Ye X W and Liu H M 2013 Design and synthesis of novel 1,2,3-triazole-dithiocarbamate hybrids as ... M, Minato T, Bao M and Yamamoto Y 2011 Nanoporous Copper Metal Catalyst in Click Chemistry: Nanoporosity-Dependent Activity without Supports and Bases; ...

  1. Catalysts for Environmental Remediation

    DEFF Research Database (Denmark)

    Abrams, B. L.; Vesborg, Peter Christian Kjærgaard


    The properties of catalysts used in environmental remediation are described here through specific examples in heterogeneous catalysis and photocatalysis. In the area of heterogeneous catalysis, selective catalytic reduction (SCR) of NOx was used as an example reaction with vanadia and tungsta...

  2. Characterization of Deactivated Bio-oil Hydrotreating Catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Wang, Huamin; Wang, Yong


    Deactivation of bio-oil hydrotreating catalysts remains a significant challenge because of the poor quality of pyrolysis bio-oil input for hydrotreating and understanding their deactivation mode is critical to developing improved catalysts and processes. In this research, we developed an understanding of the deactivation of two-step bio-oil hydrotreating catalysts (sulfided Ru/C and sulfided CoMo/C) through detailed characterization of the catalysts using various complimentary analytical techniques. Severe fouling of both catalysts by carbonaceous species was the major form of deactivation, which is consistent with the significant loss of surface area and pore volume of both deactivated catalysts and the significant increase of the bulk density. Further analysis of the carbonaceous species by thermogravimetric analysis and x-ray photoelectron spectroscopy indicated that the carbonaceous species was formed by condensation reaction of active species such as sugars and sugar derivatives (aldehydes and ketones) in bio-oil feedstock during bio-oil hydrotreating under the conditions and catalysts used. Microscopy results did not show metal sintering of the Ru/C catalyst. However, X-ray diffraction indicated a probable transformation of the highly-active CoMoS phase in the sulfided CoMo/C catalyst to Co8S9 and MoS2 phase with low activity. Loss of the active site by transport of inorganic elements from the bio-oil and the reactor construction material onto the catalyst surface also might be a cause of deactivation as indicated by elemental analysis of spent catalysts.

  3. Bifunctional catalysts for the direct production of liquid fuels from syngas

    NARCIS (Netherlands)

    Sartipi, S.


    Design and development of catalyst formulations that maximize the direct production of liquid fuels by combining Fischer-Tropsch synthesis (FTS), hydrocarbon cracking, and isomerization into one single catalyst particle (bifunctional FTS catalyst) have been investigated in this thesis. To achieve

  4. Design, synthesis, and characterization of novel fine-particle, unsupported catalysts for coal liquefaction

    Energy Technology Data Exchange (ETDEWEB)

    Klein, M.T.


    The purpose of this work is to investigate the kinetics-assisted design, synthesis and characterization of fme-pardcle, unsupported catalysts for coal liquefaction. The goal is to develop a fundamental understanding of coal catalysis and catalysts that will, in turn, allow for the specification of a novel optimal catalyst for coal liquefaction.

  5. Mechanochemical Immobilisation of Metathesis Catalysts in a Metal–Organic Framework

    NARCIS (Netherlands)

    Spekreijse, Jurjen; Öhrström, Lars; Sanders, Johan P.M.; Bitter, Harry; Scott, Elinor L.


    A simple, one-step mechanochemical procedure for immobilisation of homogeneous metathesis catalysts in metal–organic frameworks was developed. Grinding MIL-101-NH2(Al) with a Hoveyda–Grubbs second-generation catalyst resulted in a heterogeneous catalyst that is active for metathesis

  6. Recent Advancements in Stereoselective Olefin Metathesis Using Ruthenium Catalysts

    Directory of Open Access Journals (Sweden)

    T. Patrick Montgomery


    Full Text Available Olefin metathesis is a prevailing method for the construction of organic molecules. Recent advancements in olefin metathesis have focused on stereoselective transformations. Ruthenium olefin metathesis catalysts have had a particularly pronounced impact in the area of stereoselective olefin metathesis. The development of three categories of Z-selective olefin metathesis catalysts has made Z-olefins easily accessible to both laboratory and industrial chemists. Further design enhancements to asymmetric olefin metathesis catalysts have streamlined the construction of complex molecules. The understanding gained in these areas has extended to the employment of ruthenium catalysts to stereoretentive olefin metathesis, the first example of a kinetically E-selective process. These advancements, as well as synthetic applications of the newly developed catalysts, are discussed.

  7. Catalyst support structure, catalyst including the structure, reactor including a catalyst, and methods of forming same (United States)

    Van Norman, Staci A.; Aston, Victoria J.; Weimer, Alan W.


    Structures, catalysts, and reactors suitable for use for a variety of applications, including gas-to-liquid and coal-to-liquid processes and methods of forming the structures, catalysts, and reactors are disclosed. The catalyst material can be deposited onto an inner wall of a microtubular reactor and/or onto porous tungsten support structures using atomic layer deposition techniques.

  8. Catalysts for biobased fuels. New catalyst formulations for vehicles fuelled by biobased motor fuels

    Energy Technology Data Exchange (ETDEWEB)

    Pettersson, L.J.; Wahlberg, A.M.; Jaeraas, S.G. [Royal Inst. of Tech., Stockholm (Sweden). Dept. of Chemical Technology


    The long-term objective for the project is to develop tailor-made exhaust gas catalysts for heavy-duty vehicles fuelled by biobased motor fuels operating in urban traffic. In this report an experimental study of catalytic oxidation of ethanol in a laboratory flow reactor is presented. The miniature catalyst samples consisted of monolithic cordierite substrates onto which various combinations of washcoat material and active material were applied. Oxides of Cu and Cu-Mn, as well as different combinations of precious metals were evaluated as active material supported on various washcoat materials. The experimental conditions were chosen in order to simulate the exhaust from a diesel engine fuelled by neat ethanol. Catalyst characterization included measurements of BET surface area and pore size distribution as well as temperature programmed reduction (TPR) analysis. When comparing the TPR profiles with the light-off curves from the ethanol oxidation experiments, we have found an indication of a correlation between activity and reducibility of the catalyst. There also seems to be a correlation between TPR profile and pore size distribution for titania-supported catalysts. When combining two precious metals as active material, a positive synergistic effect has been observed. The light-off temperature (T{sub 50}) is considerably lower for some of these combinations than for the corresponding monometallic catalysts. The base metal oxide catalysts tested were more selective for oxidation of ethanol to carbon dioxide and water than the precious metal catalysts. The results also indicate that the oxidation of nitric oxide to the more hazardous nitrogen dioxide can be suppressed by using a suitable combination of active material and washcoat material 45 refs, 97 figs, 4 tabs

  9. Catalysis by nonmetals rules for catalyst selection

    CERN Document Server

    Krylov, Oleg V


    Catalysis by Non-metals: Rules of Catalyst Selection presents the development of scientific principles for the collection of catalysts. It discusses the investigation of the mechanism of chemosorption and catalysis. It addresses a series of properties of solid with catalytic activity. Some of the topics covered in the book are the properties of a solid and catalytic activity in oxidation-reduction reactions; the difference of electronegativities and the effective charges of atoms; the role of d-electrons in the catalytic properties of a solid; the color of solids; and proton-acid and proton-ba

  10. Silver Cluster Catalysts for Green Organic Synthesis


    Shimizu, Ken-ichi; Satsuma, Atsushi


    Development of platinum-group-metal (PGM)-free  catalysts for green chemical synthesis is an important topic in synthetic catalysis, because PGM will soon be in short supply in the near future. Our group has paid attention to the catalytic functions of Ag clusters. Here, we summarize our recent work on size- and support-specific catalysis of Ag clusters for green organic synthesis. Ag clusters supported on Al2O3 act as effective heterogeneous catalysts for (1) oxidant-free dehydrogenation of ...

  11. New catalysts for clean environment

    Energy Technology Data Exchange (ETDEWEB)

    Maijanen, A.; Hase, A. [eds.] [VTT Chemical Technology, Espoo (Finland)


    VTT launched a Research Programme on Chemical Reaction Mechanisms (CREAM) in 1993. The three-year programme (1993-1995) has focused on reaction mechanisms relevant to process industries and aimed at developing novel catalysts and biocatalysts for forest, food, and specialty chemicals industries as well as for energy production. The preliminary results of this programme have already been presented in the first symposium organized in Espoo in September 1994. To conclude the programme the second symposium is organized in Otaniemi, Espoo on January 29 - 30, 1996. Papers by 19 speakers and 17 poster presentations of the 1996 Symposium are included in this book. The Symposium consists of four sessions: Biotechnology for Natural Fibers Processing, New Biocatalysts, Catalysts for Clean Energy, and New Opportunities for Chemical Industry. The CREAM programme has tried to foresee solutions for the problems challenged by the public concern on environmental aspects, especially dealing with industrial processes and novel use of raw materials and energy. The programme has followed the basic routes that can lead to natural and simple solutions to develop processes in the fields of forest, food fine chemicals, and energy industry. This symposium presents the results of the programme to learn and further discuss together with the international experts that have been invited as keynote speakers. (author)

  12. Development of an Efficient Methanol Production Process for Direct CO2 Hydrogenation over a Cu/ZnO/Al2O3 Catalyst

    Directory of Open Access Journals (Sweden)

    Fereshteh Samimi


    Full Text Available Carbon capture and utilization as a raw material for methanol production are options for addressing energy problems and global warming. However, the commercial methanol synthesis catalyst offers a poor efficiency in CO2 feedstock because of a low conversion of CO2 and its deactivation resulting from high water production during the process. To overcome these barriers, an efficient process consisting of three stage heat exchanger reactors was proposed for CO2 hydrogenation. The catalyst volume in the conventional methanol reactor (CR is divided into three sections to load reactors. The product stream of each reactor is conveyed to a flash drum to remove methanol and water from the unreacted gases (H2, CO and CO2. Then, the gaseous stream enters the top of the next reactor as the inlet feed. This novel configuration increases CO2 conversion almost twice compared to one stage reactor. Also to reduce water production, a water permselective membrane was assisted in each reactor to remove water from the reaction side. The proposed process was compared with one stage reactor and CR from coal and natural gas. Methanol is produced 288, 305, 586 and 569 ton/day in CR, one-stage, three-stage and three-stage membrane reactors (MR, respectively. Although methanol production rate in three-stage MR is a bit lower than three stage reactors, the produced water, as the cause of catalyst poisoning, is notably reduced in this configuration. Results show that the proposed process is a strongly feasible way to produce methanol that can competitive with a traditional synthesis process.

  13. Monolith catalysts for closed-cycle carbon dioxide lasers (United States)

    Herz, Richard K.


    The general subject area of the project involved the development of solid catalysts that have high activity at low temperature for the oxidation of gases such as CO. The original application considered was CO oxidation in closed-cycle CO2 lasers. The scope of the project was subsequently extended to include oxidation of gases in addition to CO and applications such as air purification and exhaust gas emission control. The primary objective of the final phase grant was to develop design criteria for the formulation of new low-temperature oxidation catalysts utilizing Monte Carlo simulations of reaction over NASA-developed catalysts.

  14. Combination of plasma with a honeycomb-structured catalyst for automobile exhaust treatment. (United States)

    Kang, Woo Seok; Lee, Dae Hoon; Lee, Jae-Ok; Hur, Min; Song, Young-Hoon


    To activate a catalyst efficiently at low temperature by plasma for environmental control, we developed a hybrid reactor that combines plasma with a honeycomb-structured catalyst in a practical manner. The reactor developed generated stable cold plasma at atmospheric pressure because of the dielectric and conductive nature of the honeycomb catalyst by consuming low amounts of power. In this reactor, the applied voltage and temperature determined the balance between the oxidation and adsorption by the plasma and catalyst. The synergistic reaction of the plasma and catalyst was more effective at low temperatures, resulting in a reduction in a lowered light-off temperature.

  15. Graphitic Carbon Nitride Supported Catalysts for Polymer Electrolyte Fuel Cells (United States)


    Graphitic carbon nitrides are investigated for developing highly durable Pt electrocatalyst supports for polymer electrolyte fuel cells (PEFCs). Three different graphitic carbon nitride materials were synthesized with the aim to address the effect of crystallinity, porosity, and composition on the catalyst support properties: polymeric carbon nitride (gCNM), poly(triazine) imide carbon nitride (PTI/Li+Cl–), and boron-doped graphitic carbon nitride (B-gCNM). Following accelerated corrosion testing, all graphitic carbon nitride materials are found to be more electrochemically stable compared to conventional carbon black (Vulcan XC-72R) with B-gCNM support showing the best stability. For the supported catalysts, Pt/PTI-Li+Cl– catalyst exhibits better durability with only 19% electrochemical surface area (ECSA) loss versus 36% for Pt/Vulcan after 2000 scans. Superior methanol oxidation activity is observed for all graphitic carbon nitride supported Pt catalysts on the basis of the catalyst ECSA. PMID:24748912

  16. Comparison of the activities of fine-particle size catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Stohl, F.V.; Diegert, K.V.; Goodnow, D.C.


    The objectives of Sandia`s fine-particle size catalyst testing project are to evaluate and compare the activities of the fine-particle size catalysts being developed in DOE/PETCs Advanced Research Coal Liquefaction Program by using standard coal liquefaction test procedures. The standard procedures use Blind Canyon coal, phenanthrene as the reaction solvent, and a factorial experimental design with temperatures from 350{degrees}C to 400{degrees}C, reaction times from 20 to 60 minutes, and catalyst loadings up to 1 wt%. Catalytic activity is measured in terms of tetrahydrofuran conversion, heptane conversion, the amount of 9,10-dihydrophenanthrene in the product, and the gas yield. Several catalysts have been evaluated including a commercially available pyrite, a sulfated iron oxide from the University of Pittsburgh, and several preparations of 6-line ferrihydrites from Pacific Northwest Laboratories. Results have demonstrated that significant differences in activity can be detected among these catalysts.

  17. Homogeneous and heterogenized iridium water oxidation catalysts (United States)

    Macchioni, Alceo


    The development of an efficient catalyst for the oxidative splitting of water into molecular oxygen, protons and electrons is of key importance for producing solar fuels through artificial photosynthesis. We are facing the problem by means of a rational approach aimed at understanding how catalytic performance may be optimized by the knowledge of the reaction mechanism of water oxidation and the fate of the catalytic site under the inevitably harsh oxidative conditions. For the purposes of our study we selected iridium water oxidation catalysts, exhibiting remarkable performance (TOF > 5 s-1 and TON > 20000). In particular, we recently focused our attention on [Cp*Ir(N,O)X] (N,O = 2-pyridincarboxylate; X = Cl or NO3) and [IrCl(Hedta)]Na water oxidation catalysts. The former exhibited a remarkable TOF whereas the latter showed a very high TON. Furthermore, [IrCl(Hedta)]Na was heterogenized onto TiO2 taking advantage of the presence of a dandling -COOH functionality. The heterogenized catalyst maintained approximately the same catalytic activity of the homogeneous analogous with the advantage that could be reused many times. Mechanistic studies were performed in order to shed some light on the rate-determining step and the transformation of catalysts when exposed to "oxidative stress". It was found that the last oxidative step, preceding oxygen liberation, is the rate-determining step when a small excess of sacrificial oxidant is used. In addition, several intermediates of the oxidative transformation of the catalyst were intercepted and characterized by NMR, X-Ray diffractometry and ESI-MS.

  18. IN SITU Device for Real-Time Catalyst Deactivation Measurements

    Energy Technology Data Exchange (ETDEWEB)

    Fossil Energy Research


    SCR catalyst management has become an important operations and maintenance activity for coal-fired utility boilers in the United States. To facilitate this activity, a method to determine Catalyst Activity in situ is being developed. This report describes the methodology and presents the results of a two ozone season demonstration conducted at Alabama Power Company's Gorgas Unit 10 during the 2005 and 2006 ozone seasons. The results showed that the in situ measurements are in good agreement with the laboratory measurements and the technique has some advantages over the traditional laboratory method of determining Catalyst Activity and Reactor Potential. SCR Performance is determined by the overall Reactor Potential (the product of the Catalyst Activity and the available surface area per unit of flue gas). The in situ approach provides a direct measurement of Reactor Potential under actual operating conditions, whereas laboratory measurements of Catalyst Activity need to be coupled with estimates of catalyst pluggage and flue gas flowrate in order to assess Reactor Potential. The project also showed that the in situ activity results can easily be integrated into catalyst management software to aid in making informed catalyst decisions.

  19. Polyaromatic polymers as binders in PEMFC catalyst layers

    Energy Technology Data Exchange (ETDEWEB)

    Peron, J.M.; Edwards, D.; Le Marquand, P.; Shi, Z.; Holdcroft, S. [National Research Council of Canada, Vancouver, BC (Canada). Inst. for Fuel Cell Innovation


    The catalyst layers in proton exchange membrane (PEM) fuel cells are typically composed of platinum as the catalyst and carbon as the electron conductor. The binder that ensures the ionic pathway between catalyst particles and the electrolyte membrane is a perfluorinated polymer that brings the electrolyte, gaseous reactants, electrocatalyst and current collector into close contact within a confined spatial region known as the triple-phase-boundary. New non-fluorinated polymers have been developed in an effort to lower the cost and improve the stability of fuel cells. Although polyaromatic polymers have been extensively presented in the literature for membrane preparation, these new materials have been mainly characterized in presence of Nafion as a binder in the catalyst layer. This paper discussed the incorporation of polyaromatic polymers, such as sulfonated-PEEK (sPEEK), and its properties as a binder. sPEEK-based catalyst ink solutions, using different sPEEK/Pt ratios and preparation methods, have been deposited on membranes to form catalyst-coated-membranes (CCM). Initial catalyst ink were characterized using dynamic light scattering to determine agglomerate size. Catalyst layers were examined using SEM and TEM and their porosity was determined by Hg porosimetry. Various electrochemical techniques were used for in-situ characterization of prepared sPEEK CCMs.

  20. Development of Hierarchical Polymer@Pd Nanowire‐Network: Synthesis and Application as Highly Active Recyclable Catalyst and Printable Conductive Ink (United States)

    Mir, Sajjad Husain


    Abstract A facile one‐pot approach for preparing hierarchical nanowire‐networks of hollow polymer@Pd nanospheres is reported. First, polymer@Pd hollow nanospheres were produced through metal‐complexation‐induced phase separation with functionalized graft copolymers and subsequent self‐assembly of PdNPs. The nanospheres hierarchically assembled into the nanowire‐network upon drying. The Pd nanowire‐network served as an active catalyst for Mizoroki–Heck and Suzuki–Miyaura coupling reactions. As low as 500 μmol % Pd was sufficient for quantitative reactions, and the origin of the high activity is ascribed to the highly active sites originating from high‐index facets, kinks, and coalesced structures. The catalyst can be recycled via simple filtration and washing, maintaining its high activity owing to the micrometer‐sized hierarchical structure of the nanomaterial. The polymer@Pd nanosphere also served as a printable conductive ink for a translucent grid pattern with excellent horizontal conductivity (7.5×105 S m−1). PMID:27551657

  1. Development of Hierarchical Polymer@Pd Nanowire-Network: Synthesis and Application as Highly Active Recyclable Catalyst and Printable Conductive Ink. (United States)

    Mir, Sajjad Husain; Ochiai, Bungo


    A facile one-pot approach for preparing hierarchical nanowire-networks of hollow polymer@Pd nanospheres is reported. First, polymer@Pd hollow nanospheres were produced through metal-complexation-induced phase separation with functionalized graft copolymers and subsequent self-assembly of PdNPs. The nanospheres hierarchically assembled into the nanowire-network upon drying. The Pd nanowire-network served as an active catalyst for Mizoroki-Heck and Suzuki-Miyaura coupling reactions. As low as 500 μmol % Pd was sufficient for quantitative reactions, and the origin of the high activity is ascribed to the highly active sites originating from high-index facets, kinks, and coalesced structures. The catalyst can be recycled via simple filtration and washing, maintaining its high activity owing to the micrometer-sized hierarchical structure of the nanomaterial. The polymer@Pd nanosphere also served as a printable conductive ink for a translucent grid pattern with excellent horizontal conductivity (7.5×10(5) S m(-1)).

  2. Olefin metathesis and catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Kukes, S. G.; Banks, R. L.


    Olefins are converted into other olefins having different numbers of carbon atoms by contact with a catalyst comprising an inorganic refractory material containing at least one of tungsten oxide and molybdenum oxide and a promoting amount of at least one treating agent selected from chlorinated silicon compounds, thionyl chloride, and sulfuryl chloride under conditions suitable for the treating agent to promote the activity of tungsten and molybdenum oxides for the disporoportionation reaction.

  3. Steam reforming catalyst (United States)

    Kramarz, Kurt W.; Bloom, Ira D.; Kumar, Romesh; Ahmed, Shabbir; Wilkenhoener, Rolf; Krumpelt, Michael


    A method of forming a hydrogen rich gas from a source of hydrocarbon fuel. A vapor of the hydrocarbon fuel and steam is brought in contact with a two-part catalyst having a dehydrogenation powder portion and an oxide-ion conducting powder portion at a temperature not less than about for a time sufficient to generate the hydrogen rich. The H.sub.2 content of the hydrogen gas is greater than about 70 percent by volume. The dehydrogenation portion of the catalyst includes a group VIII metal, and the oxide-ion conducting portion is selected from a ceramic oxide from the group crystallizing in the fluorite or perovskite structure and mixtures thereof. The oxide-ion conducting portion of the catalyst is a ceramic powder of one or more of ZrO.sub.2, CeO.sub.2, Bi.sub.2 O.sub.3, (BiVO).sub.4, and LaGaO.sub.3.

  4. Ziegler-Natta Catalysts

    Directory of Open Access Journals (Sweden)

    G. Pircheraghi


    Full Text Available The effects of temperature, time and the strategy of prepolymerization were studied on the morphology of polypropylene particles. propylene polymerization was carried out in slurry phase using 4th generation of Ziegler-Natta Catalyst, cyclohexylmethyl dimethoxysilane as external electron donor, and triethyl aluminum as co-catalyst. Prepolymerizations were carried out based on two strategies: isothermal and non-isothermal conditions. Particle imaging using SEM, bulk density, and particle size distribution was used to analyse the particle morphology. It was found that the variation of initial condition together with the change in the mechanism of particle fracture has a dominant effect on particle morphology. Each combination between the temperature and reaction time causes to have a special effect on the product particle morphology. It has become clear that in isothermal prepolymerization, spherical particles with identical properties were produced. In low temperature experiments particles with porous surface were observed. At increasing temperature, however, the pores disappeared. Non-isothermal prepolymerization produced different morphological types. In all experiments coreshell structures were observed that seemed to be related to the structure of catalysts.

  5. Graphene-supported platinum catalysts for fuel cells

    DEFF Research Database (Denmark)

    Seselj, Nedjeljko; Engelbrekt, Christian; Zhang, Jingdong


    Increasing concerns with non-renewable energy sources drive research and development of sustainable energy technology. Fuel cells have become a central part in solving challenges associated with energy conversion. This review summarizes recent development of catalysts used for fuel cells over...... the past 15 years. It is focused on polymer electrolyte membrane fuel cells as an environmentally benign and feasible energy source. Graphene is used as a promising support material for Pt catalysts. It ensures high catalyst loading, good electrocatalysis and stability. Attention has been drawn...

  6. The generation of efficient supported (Heterogeneous) olefin metathesis catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Grubbs, Robert H


    Over the past decade, a new family of homogeneous metathesis catalysts has been developed that will tolerate most organic functionalities as well as water and air. These homogeneous catalysts are finding numerous applications in the pharmaceutical industry as well as in the production of functional polymers. In addition the catalysts are being used to convert seed oils into products that can substitute for those that are now made from petroleum products. Seed oils are unsaturated, contain double bonds, and are a ready source of linear hydrocarbon fragments that are specifically functionalized. To increase the number of applications in the area of biomaterial conversion to petrol chemicals, the activity and efficiency of the catalysts need to be as high as possible. The higher the efficiency of the catalysts, the lower the cost of the conversion and a larger number of practical applications become available. Active supported catalysts were prepared and tested in the conversion of seed oils and other important starting materials. The outcome of the work was successful and the technology has been transferred to a commercial operation to develop viable applications of the discovered systems. A biorefinery that converts seed oils is under construction in Indonesia. The catalysts developed in this study will be considered for the next generation of operations.

  7. Dispersed catalysts for co-processing and coal liquefaction

    Energy Technology Data Exchange (ETDEWEB)

    Bockrath, B.; Parfitt, D.; Miller, R. [Pittsburgh Energy Technology Center, PA (United States)


    The basic goal is to improve dispersed catalysts employed in the production of clean fuels from low value hydrocarbons. The immediate objective is to determine how the properties of the catalysts may be altered to match the demands placed on them by the properties of the feedstock, the qualities of the desired end products, and the economic constraints put upon the process. Several interrelated areas of the application of dispersed catalysts to co-processing and coal conversion are under investigation. The first involves control of the selectivity of MoS{sub 2} catalysts for HDN, HDS, and hydrogenation of aromatics. A second area of research is the development and use of methods to evaluate dispersed catalysts by means of activity and selectivity tests. A micro-flow reactor has been developed for determining intrinsic reactivities using model compounds, and will be used to compare catalysts prepared in different ways. Micro-autoclaves will also be used to develop data in batch experiments at higher partial pressures of hydrogen. The third area under investigation concerns hydrogen spillover reactions between MoS{sub 2} catalysts and carbonaceous supports. Preliminary results obtained by monitoring H{sub 2}/D{sub 2} exchange reactions with a pulse-flow microreactor indicate the presence of spillover between MoS{sub 2} and a graphitic carbon. A more complete study will be made at a later stage of the project. Accomplishments and conclusions are discussed.

  8. Understanding the Performance of Automotive Catalysts via Spatial Resolution of Reactions inside Honeycomb Monoliths

    Energy Technology Data Exchange (ETDEWEB)

    Partridge Jr, William P. [ORNL; Choi, Jae-Soon [ORNL


    By directly resolving spatial and temporal species distributions within operating honeycomb monolith catalysts, spatially resolved capillary inlet mass spectrometry (SpaciMS) provides a uniquely enabling perspective for advancing automotive catalysis. Specifically, the ability to follow the spatiotemporal evolution of reactions throughout the catalyst is a significant advantage over inlet-and-effluent-limited analysis. Intracatalyst resolution elucidates numerous catalyst details including the network and sequence of reactions, clarifying reaction pathways; the relative rates of different reactions and impacts of operating conditions and catalyst state; and reaction dynamics and intermediate species that exist only within the catalyst. These details provide a better understanding of how the catalyst functions and have basic and practical benefits; e.g., catalyst system design; strategies for on-road catalyst state assessment, control, and on-board diagnostics; and creating robust and accurate predictive catalyst models. Moreover, such spatiotemporally distributed data provide for critical model assessment, and identification of improvement opportunities that might not be apparent from effluent assessment; i.e., while an incorrectly formulated model may provide correct effluent predictions, one that can accurately predict the spatiotemporal evolution of reactions along the catalyst channels will be more robust, accurate, and reliable. In such ways, intracatalyst diagnostics comprehensively enable improved design and development tools, and faster and lower-cost development of more efficient and durable automotive catalyst systems. Beyond these direct contributions, SpaciMS has spawned and been applied to enable other analytical techniques for resolving transient distributed intracatalyst performance. This chapter focuses on SpaciMS applications and associated catalyst insights and improvements, with specific sections related to lean NOx traps, selective catalytic

  9. Microchannel Reactors for ISRU Applications Using Nanofabricated Catalysts Project (United States)

    National Aeronautics and Space Administration — Makel Engineering, Inc. (MEI) and USRA propose to develop microchannel reactors for In-Situ Resources Utilization (ISRU) using nanofabricated catalysts. The proposed...

  10. Preparation of odour removal catalysts with self-regeneration capability

    National Research Council Canada - National Science Library

    Zhao, Yongxiang; Zhao, Lili; Huang, Yu; Chen, Haoyi; Xiao, Tiancun


    .... Here, for the first time, we have developed an activated carbon-alumina composite-supported ZnCu bimetallic metal oxide catalyst, which not only has very high capacity to absorb the strong smell...

  11. Functionalized magnetic nanoparticles: A novel heterogeneous catalyst support (United States)

    Functionalized magnetic nanoparticles have emerged as viable alternatives to conventional materials, as robust, high-surface-area heterogeneous catalyst supports. Post-synthetic surface modification protocol for magnetic nanoparticles has been developed that imparts desirable che...

  12. Visible Light Responsive Catalyst for Air Water Purification Project (United States)

    Wheeler, Raymond M.


    Investigate and develop viable approaches to render the normally UV-activated TIO2 catalyst visible light responsive (VLR) and achieve high and sustaining catalytic activity under the visible region of the solar spectrum.

  13. Biomass Conversion over Heteropoly Acid Catalysts

    KAUST Repository

    Zhang, Jizhe


    Biomass is a natural resource that is both abundant and sustainable. Its efficient utilization has long been the focus of research and development efforts with the aim to substitute it for fossil-based feedstock. In addition to the production of biofuels (e.g., ethanol) from biomass, which has been to some degree successful, its conversion to high value-added chemicals is equally important. Among various biomass conversion pathways, catalytic conversion is usually preferred, as it provides a cost-effective and eco-benign route to the desired products with high selectivities. The research of this thesis is focused on the conversion of biomass to various chemicals of commercial interest by selective catalytic oxidation. Molecular oxygen is chosen as the oxidant considering its low cost and environment friendly features in comparison with commonly used hydrogen peroxide. However, the activation of molecular oxygen usually requires high reaction temperatures, leading to over oxidation and thus lower selectivities. Therefore, it is highly desirable to develop effective catalysts for such conversion systems. We use kegging-type heteropoly acids (HPAs) as a platform for catalysts design because of their high catalytic activities and ease of medication. Using HPA catalysts allows the conversion taking place at relatively low temperature, which is beneficial to saving production cost as well as to improving the reaction selectivity. The strong acidity of HPA promotes the hydrolysis of biomass of giant molecules (e.g. cellulose), which is the first as well as the most difficult step in the conversion process. Under certain circumstances, a HPA combines the merits of homogeneous and heterogeneous catalysts, acting as an efficient homogeneous catalyst during the reaction while being easily separated as a heterogeneous catalyst after the reaction. We have successfully applied HPAs in several biomass conversion systems. Specially, we prepared a HPA-based bi-functional catalyst

  14. Nano Catalysts for Diesel Engine Emission Remediation

    Energy Technology Data Exchange (ETDEWEB)

    Narula, Chaitanya Kumar [ORNL; Yang, Xiaofan [ORNL; Debusk, Melanie Moses [ORNL; Mullins, David R [ORNL; Mahurin, Shannon Mark [ORNL; Wu, Zili [ORNL


    The objective of this project was to develop durable zeolite nanocatalysts with broader operating temperature windows to treat diesel engine emissions to enable diesel engine based equipment and vehicles to meet future regulatory requirements. A second objective was to improve hydrothermal durability of zeolite catalysts to at least 675 C. The results presented in this report show that we have successfully achieved both objectives. Since it is accepted that the first step in NO{sub x} conversion under SCR (selective catalytic reduction) conditions involves NO oxidation to NO{sub 2}, we reasoned that catalyst modification that can enhance NO oxidation at low-temperatures should facilitate NO{sub x} reduction at low temperatures. Considering that Cu-ZSM-5 is a more efficient catalyst than Fe-ZSM-5 at low-temperature, we chose to modify Cu-ZSM-5. It is important to point out that the poor low-temperature efficiency of Fe-ZSM-5 has been shown to be due to selective absorption of NH{sub 3} at low-temperatures rather than poor NO oxidation activity. In view of this, we also reasoned that an increased electron density on copper in Cu-ZSM-5 would inhibit any bonding with NH{sub 3} at low-temperatures. In addition to modified Cu-ZSM-5, we synthesized a series of new heterobimetallic zeolites, by incorporating a secondary metal cation M (Sc{sup 3+}, Fe{sup 3+}, In{sup 3+}, and La{sup 3+}) in Cu exchanged ZSM-5, zeolite-beta, and SSZ-13 zeolites under carefully controlled experimental conditions. Characterization by diffuse-reflectance ultra-violet-visible spectroscopy (UV-Vis), X-ray powder diffraction (XRD), extended X-ray absorption fine structure spectroscopy (EXAFS) and electron paramagnetic resonance spectroscopy (EPR) does not permit conclusive structural determination but supports the proposal that M{sup 3+} has been incorporated in the vicinity of Cu(II). The protocols for degreening catalysts, testing under various operating conditions, and accelerated aging

  15. Catalyst systems and uses thereof (United States)

    Ozkan, Umit S [Worthington, OH; Holmgreen, Erik M [Columbus, OH; Yung, Matthew M [Columbus, OH


    A method of carbon monoxide (CO) removal comprises providing an oxidation catalyst comprising cobalt supported on an inorganic oxide. The method further comprises feeding a gaseous stream comprising CO, and oxygen (O.sub.2) to the catalyst system, and removing CO from the gaseous stream by oxidizing the CO to carbon dioxide (CO.sub.2) in the presence of the oxidation catalyst at a temperature between about 20 to about C.

  16. Oxygen-reducing catalyst layer (United States)

    O'Brien, Dennis P [Maplewood, MN; Schmoeckel, Alison K [Stillwater, MN; Vernstrom, George D [Cottage Grove, MN; Atanasoski, Radoslav [Edina, MN; Wood, Thomas E [Stillwater, MN; Yang, Ruizhi [Halifax, CA; Easton, E Bradley [Halifax, CA; Dahn, Jeffrey R [Hubley, CA; O'Neill, David G [Lake Elmo, MN


    An oxygen-reducing catalyst layer, and a method of making the oxygen-reducing catalyst layer, where the oxygen-reducing catalyst layer includes a catalytic material film disposed on a substrate with the use of physical vapor deposition and thermal treatment. The catalytic material film includes a transition metal that is substantially free of platinum. At least one of the physical vapor deposition and the thermal treatment is performed in a processing environment comprising a nitrogen-containing gas.

  17. Supported Molten Metal Catalysis. A New Class of Catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Ravindra Datta; Ajeet Singh; Manuela Serban; Istvan Halasz


    We describe a new class of heterogeneous catalysts called supported molten metal catalysis (SMMC), in which molten metal catalysts are dispersed as nanodroplets on the surface of porous supports, allowing much larger active surface area than is possible in conventional contacting techniques for catalytic metals that are molten under reaction conditions, thus greatly enhancing their activity and potential utility. Specific examples of different types of reactions are provided to demonstrate the broad applicability of the technique in designing active, selective, and stable new catalysts. It is shown that dispersing the molten metal on a support in the suggested manner can enhance the rate of a reaction by three to four orders of magnitude as a result of the concomitant increase in the active surface area. New reaction examples include {gamma}-Al{sub 2}O{sub 3} supported molten Te (melting point 450 C) and Ga (MP 30 C) catalysts for bifunctional methylcyclohexane dehydrogenation. These catalysts provide activity similar to conventional Pt-based catalysts for this with better resistance to coking. In addition, results are described for a controlled pore glass supported molten In (MP 157 C) catalyst for the selective catalytic reduction of NO with ethanol in the presence of water, demonstrating activities superior to conventional catalysts for this reaction. A discussion is also provided on the characterization of the active surface area and dispersion of these novel supported catalysts. It is clear based on the results described that the development of new active and selective supported molten metal catalysts for practical applications is entirely plausible.

  18. Method of Heating a Foam-Based Catalyst Bed (United States)

    Fortini, Arthur J.; Williams, Brian E.; McNeal, Shawn R.


    A method of heating a foam-based catalyst bed has been developed using silicon carbide as the catalyst support due to its readily accessible, high surface area that is oxidation-resistant and is electrically conductive. The foam support may be resistively heated by passing an electric current through it. This allows the catalyst bed to be heated directly, requiring less power to reach the desired temperature more quickly. Designed for heterogeneous catalysis, the method can be used by the petrochemical, chemical processing, and power-generating industries, as well as automotive catalytic converters. Catalyst beds must be heated to a light-off temperature before they catalyze the desired reactions. This typically is done by heating the assembly that contains the catalyst bed, which results in much of the power being wasted and/or lost to the surrounding environment. The catalyst bed is heated indirectly, thus requiring excessive power. With the electrically heated catalyst bed, virtually all of the power is used to heat the support, and only a small fraction is lost to the surroundings. Although the light-off temperature of most catalysts is only a few hundred degrees Celsius, the electrically heated foam is able to achieve temperatures of 1,200 C. Lower temperatures are achievable by supplying less electrical power to the foam. Furthermore, because of the foam s open-cell structure, the catalyst can be applied either directly to the foam ligaments or in the form of a catalyst- containing washcoat. This innovation would be very useful for heterogeneous catalysis where elevated temperatures are needed to drive the reaction.

  19. Host cell and expression engineering for development of an E. coli ketoreductase catalyst: Enhancement of formate dehydrogenase activity for regeneration of NADH

    Directory of Open Access Journals (Sweden)

    Mädje Katharina


    Full Text Available Abstract Background Enzymatic NADH or NADPH-dependent reduction is a widely applied approach for the synthesis of optically active organic compounds. The overall biocatalytic conversion usually involves in situ regeneration of the expensive NAD(PH. Oxidation of formate to carbon dioxide, catalyzed by formate dehydrogenase (EC; FDH, presents an almost ideal process solution for coenzyme regeneration that has been well established for NADH. Because isolated FDH is relatively unstable under a range of process conditions, whole cells often constitute the preferred form of the biocatalyst, combining the advantage of enzyme protection in the cellular environment with ease of enzyme production. However, the most prominent FDH used in biotransformations, the enzyme from the yeast Candida boidinii, is usually expressed in limiting amounts of activity in the prime host for whole cell biocatalysis, Escherichia coli. We therefore performed expression engineering with the aim of enhancing FDH activity in an E. coli ketoreductase catalyst. The benefit resulting from improved NADH regeneration capacity is demonstrated in two transformations of technological relevance: xylose conversion into xylitol, and synthesis of (S-1-(2-chlorophenylethanol from o-chloroacetophenone. Results As compared to individual expression of C. boidinii FDH in E. coli BL21 (DE3 that gave an intracellular enzyme activity of 400 units/gCDW, co-expression of the FDH with the ketoreductase (Candida tenuis xylose reductase; XR resulted in a substantial decline in FDH activity. The remaining FDH activity of only 85 U/gCDW was strongly limiting the overall catalytic activity of the whole cell system. Combined effects from increase in FDH gene copy number, supply of rare tRNAs in a Rosetta strain of E. coli, dampened expression of the ketoreductase, and induction at low temperature (18°C brought up the FDH activity threefold to a level of 250 U/gCDW while reducing the XR activity by

  20. Mixed Alcohol Synthesis Catalyst Screening

    Energy Technology Data Exchange (ETDEWEB)

    Gerber, Mark A.; White, James F.; Stevens, Don J.


    National Renewable Energy Laboratory (NREL) and Pacific Northwest National Laboratory (PNNL) are conducting research to investigate the feasibility of producing mixed alcohols from biomass-derived synthesis gas (syngas). PNNL is tasked with obtaining commercially available or preparing promising mixed-alcohol catalysts and screening them in a laboratory-scale reactor system. Commercially available catalysts and the most promising experimental catalysts are provided to NREL for testing using a slipstream from a pilot-scale biomass gasifier. From the standpoint of producing C2+ alcohols as the major product, it appears that the rhodium catalyst is the best choice in terms of both selectivity and space-time yield (STY). However, unless the rhodium catalyst can be improved to provide minimally acceptable STYs for commercial operation, mixed alcohol synthesis will involve significant production of other liquid coproducts. The modified Fischer-Tropsch catalyst shows the most promise for providing both an acceptable selectivity to C2+ alcohols and total liquid STY. However, further optimization of the Fischer-Tropsch catalysts to improve selectivity to higher alcohols is highly desired. Selection of a preferred catalyst will likely entail a decision on the preferred coproduct slate. No other catalysts tested appear amenable to the significant improvements needed for acceptable STYs.

  1. Chelated Ruthenium Catalysts for Z-Selective Olefin Metathesis


    Endo, Koji; Grubbs, Robert H


    We report the development of ruthenium-based metathesis catalysts with chelating N-heterocyclic carbene (NHC) ligands which catalyze highly Z-selective olefin metathesis. A very simple and convenient synthetic procedure of such a catalyst has been developed. An intramolecular C-H bond activation of the NHC ligand, which is promoted by anion ligand substitution, forms the appropriate chelate for stereo- controlled olefin metathesis.


    NARCIS (Netherlands)

    Sie, S.T.


    Abstract of WO 9521691 (A1) Described is a reactor (1) at least partially filled with catalyst granules (11), which is intended for catalytically reacting at least one gas and at least one liquid with each other. According to the invention the catalyst granules (11) are collected in agglomerates

  3. Optimization of catalyst layer composition for PEMFC using graphene-based oxygen reduction reaction catalysts (United States)

    Park, Jong Cheol; Park, Sung Hyeon; Chung, Min Wook; Choi, Chang Hyuck; Kho, Back Kyun; Woo, Seong Ihl


    The focus in recent years is on developing high performance non-precious metal catalysts (NPMCs) to reduce the catalyst cost in fuel cells. However, little attention has been paid to improve the utilization of NPMCs. Thus, this study focuses on the optimization of electrode component, particularly the Nafion content. With the synthesized graphene based oxygen reduction reaction (ORR) catalyst, the catalyst inks were prepared at various Nafion contents with suitable amounts of catalysts sprayed on the gas diffusion media. Twenty different single cells were assembled and measured for polarization, resistance and electrochemical impedance. Electrodes of 66.7 and 50.0% Nafion contents showed the highest performance for hydrogen/oxygen and hydrogen/air operation, respectively. These results were explained using the electrochemical impedance spectra, where the highest performance electrode resulted with the lowest charge transfer resistance. Moreover, negligible change in performance was observed during the 80 h of stability test. The optimization compositions of NPMC-based MEAs were very different to Pt-based MEAs, indicating the importance of optimization studies for the practical use of NPMCs.

  4. Novel Reforming Catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Pfefferle, Lisa D; Haller, Gary L


    Aqueous phase reforming is useful for processing oxygenated hydrocarbons to hydrogen and other more useful products. Current processing is hampered by the fact that oxide based catalysts are not stable under high temperature hydrothermal conditions. Silica in the form of structured MCM-41 is thermally a more stable support for Co and Ni than conventional high surface area amorphous silica but hydrothermal stability is not demonstrated. Carbon nanotube supports, in contrast, are highly stable under hydrothermal reaction conditions. In this project we show that carbon nanotubes are stable high activity/selectivity supports for the conversion of ethylene glycol to hydrogen.

  5. A Catalyst for Change

    DEFF Research Database (Denmark)

    Lønsmann, Dorte


    into in a process that hinges on new members functioning as tools for management to bring about the desired change. The article shows that while the newcomer is used as a catalyst for increased use of English and for the creation of a 'global mindset,' she is at the same time socialized into the existing Danish...... for changing language practices toward more English, with the ultimate aim of creating a 'global mindset' in the organization. Language socialization in a transient multilingual setting is shown to focus on and assign positive value to new linguistic norms that experienced members are socialized...

  6. Building Indenylidene-Ruthenium Catalysts for Metathesis Transformations (United States)

    Clavier, Hervé; Nolan, Steven P.

    Ruthenium-mediated olefin metathesis has emerged as an indispensable tool in organic synthesis for the formation carbon-carbon double bonds, attested by the large number of applications for natural product synthesis. Among the numerous catalysts developed to mediate olefin metathesis transformations, ruthenium-indenylidene complexes are robust and powerful pre-catalysts. The discovery of this catalyst category was slightly muddled due to a first mis-assignment of the compound structure. This report provides an overview of the synthetic routes for the construction of the indenylidene pattern in ruthenium complexes. The parameters relating to the indenylidene moiety construction will be discussed as well as the mechanism of this formation

  7. A bioinspired iron catalyst for nitrate and perchlorate reduction. (United States)

    Ford, Courtney L; Park, Yun Ji; Matson, Ellen M; Gordon, Zachary; Fout, Alison R


    Nitrate and perchlorate have considerable use in technology, synthetic materials, and agriculture; as a result, they have become pervasive water pollutants. Industrial strategies to chemically reduce these oxyanions often require the use of harsh conditions, but microorganisms can efficiently reduce them enzymatically. We developed an iron catalyst inspired by the active sites of nitrate reductase and (per)chlorate reductase enzymes. The catalyst features a secondary coordination sphere that aids in oxyanion deoxygenation. Upon reduction of the oxyanions, an iron(III)-oxo is formed, which in the presence of protons and electrons regenerates the catalyst and releases water. Copyright © 2016, American Association for the Advancement of Science.

  8. Development plus kinetic and mechanistic studies of a prototype supported-nanoparticle heterogeneous catalyst formation system in contact with solution: Ir(1,5-COD)Cl/gamma-Al2O3 and its reduction by H2 to Ir(0)n/gamma-Al2O3. (United States)

    Mondloch, Joseph E; Wang, Qi; Frenkel, Anatoly I; Finke, Richard G


    An important question and hence goal in catalysis is how best to transfer the synthetic and mechanistic insights gained from the modern revolution in nanoparticle synthesis, characterization, and catalysis to prepare the next generation of improved, supported-nanoparticle heterogeneous catalysts. It is precisely this question and to-date somewhat elusive goal which are addressed by the present work. More specifically, the global hypothesis investigated herein is that the use of speciation-controlled, well-characterized, solid oxide supported-organometallic precatalysts in contact with solution will lead to the next generation of better composition, size- and shape-controlled, as well as highly active and reproducible, supported-nanoparticle heterogeneous catalysts-ones that can also be understood kinetically and mechanistically. Developed herein are eight criteria defining a prototype system for supported-nanoparticle heterogeneous catalyst formation in contact with solution. The initial prototype system explored is the precatalyst, Ir(1,5-COD)Cl/gamma-Al(2)O(3) (characterized via ICP, CO adsorption, IR, and XAFS spectroscopies), and the well-defined product, Ir(0)(n)/gamma-Al(2)O(3) (characterized by reaction stoichiometry, TEM, and XAFS). The Ir(0)(n)/gamma-Al(2)O(3) system proved to be a highly active and long-lived catalyst in the simple test reaction of cyclohexene hydrogenation and in comparison to two literature Ir(0)(n)/Al(2)O(3) heterogeneous catalysts examined under identical conditions. High activity (2.2-4.8-fold higher than that of the literature Ir(0)(n)/Al(2)O(3) catalysts tested under the same conditions) and good lifetime (> or = 220,000 total turnovers of cyclohexene hydrogenation) are observed, in part by design since only acetone solvent, cyclohexene, and H(2) are possible ligands in the resultant "weakly ligated/labile-ligand" supported nanoclusters. Significantly, the Ir(1,5-COD)Cl/gamma-Al(2)O(3) + H(2) --> Ir(0)(n)/gamma-Al(2)O(3

  9. Shock activation of catalysts (United States)

    Graham, R. A.; Morosin, B.; Richards, P. M.; Stohl, F. V.; Granoff, B.


    Scientists in the Soviet Union have demonstrated that high pressure shock-wave loading can cause significant improvement in the performance of catalysts. This increased catalytic activity is apparently the result of the shock-induced defects, especially vacancies, which act to facilitate atomic migration. We have carried out shock activation experiments on a coal-derived pyrite which has been previously used as a catalyst in coal liquefaction studies. The pyrite powder was packed to a density of about 2.0 Mg/m3 in a copper capsule and explosively loaded to a pressure of about 15 GPa in the copper. The starting and shock-activated samples were analyzed by x-ray diffraction and magnetization measurements. The diffraction patterns of the shock-activated samples were dominated by broadened pyrite lines indicative of a significant increase in crystal defects. The diffraction patterns also showed the presence of pyrrhotite (Fe1-xS) in quantities of a few percent. An iron carbide found in the shocked material was apparently formed from carbon originating from either the calcite or organic impurities in the starting material. Magnetic properties of the sample were found to be substantially changed by the shock loading. The study has demonstrated that shock loading can significantly alter the crystalline order of pyrite and produce measurable quantities of pyrrhotite. The effects of shock-activated pyrite on the liquefaction of coal are being assessed by means by tubing reactor experiments.

  10. Hydrogenation of citral into its derivatives using heterogeneous catalyst (United States)

    Sudiyarmanto, Hidayati, Luthfiana Nurul; Kristiani, Anis; Aulia, Fauzan


    Citral as known as a monoterpene can be found in plants and citrus fruits. The hydrogenation of citral into its derivatives become interesting area for scientist. This compound and its derivatives can be used for many application in pharmaceuticals and food areas. The development of heterogeneous catalysts become an important aspect in catalytic hydrogenation citral process. Nickel supported catalysts are well known as hydrogenation catalyst. These heterogeneous catalysts were tested their catalytic activity in hydrogenation of citral. The effect of various operation conditions, in term of feed concentration, catalyst loading, temperature, and reaction time were also studied. The liquid products produced were analyzed by using Gas Chromatography-Mass Spectroscopy (GC-MS). The result of catalytic activity tests showed nickel skeletal catalyst exhibits best catalytic activity in hydrogenation of citral. The optimum of operation condition was achieved in citral concentration 0.1 M with nickel skeletal catalyst loading of 10% (w/w) at 80 °C and 20 bar for 2 hours produced the highest conversion as of 64.20% and the dominant product resulted was citronellal as of 56.48%.

  11. Design criteria for stable Pt/C fuel cell catalysts

    Directory of Open Access Journals (Sweden)

    Josef C. Meier


    Full Text Available Platinum and Pt alloy nanoparticles supported on carbon are the state of the art electrocatalysts in proton exchange membrane fuel cells. To develop a better understanding on how material design can influence the degradation processes on the nanoscale, three specific Pt/C catalysts with different structural characteristics were investigated in depth: a conventional Pt/Vulcan catalyst with a particle size of 3–4 nm and two Pt@HGS catalysts with different particle size, 1–2 nm and 3–4 nm. Specifically, Pt@HGS corresponds to platinum nanoparticles incorporated and confined within the pore structure of the nanostructured carbon support, i.e., hollow graphitic spheres (HGS. All three materials are characterized by the same platinum loading, so that the differences in their performance can be correlated to the structural characteristics of each material. The comparison of the activity and stability behavior of the three catalysts, as obtained from thin film rotating disk electrode measurements and identical location electron microscopy, is also extended to commercial materials and used as a basis for a discussion of general fuel cell catalyst design principles. Namely, the effects of particle size, inter-particle distance, certain support characteristics and thermal treatment on the catalyst performance and in particular the catalyst stability are evaluated. Based on our results, a set of design criteria for more stable and active Pt/C and Pt-alloy/C materials is suggested.

  12. Heterogeneous electro-Fenton catalyst for 1-butylpyridinium chloride degradation. (United States)

    Meijide, Jessica; Pazos, Marta; Sanromán, Maria Ángeles


    The application of the electro-Fenton process for organic compound mineralisation has been widely reported over the past years. However, operational problems related to the use of soluble iron salt as a homogeneous catalyst involve the development of novel catalysts that are able to operate in a wide pH range. For this purpose, polyvinyl alcohol-alginate beads, containing goethite as iron, were synthesised and evaluated as heterogeneous electro-Fenton catalyst for 1-butylpyridinium chloride mineralisation. The influence of catalyst dosage and pH solution on ionic liquid degradation was analysed, achieving almost total oxidation after 60 min under optimal conditions (2 g/L catalyst concentration and pH 3). The results showed good catalyst stability and reusability, although its effectiveness decreases slightly after three successive cycles. Furthermore, a plausible mineralisation pathway was proposed based on the oxidation byproducts determined by chromatographic techniques. Finally, the Microtox® test revealed notable detoxification after treatment which demonstrates high catalyst ability for pyridinium-based ionic liquid degradation by the electro-Fenton process.


    Energy Technology Data Exchange (ETDEWEB)

    K. Jothimurugesan; James G. Goodwin, Jr.; Santosh K. Gangwal


    Fischer-Tropsch (FT) synthesis to convert syngas (CO + H{sub 2}) derived from natural gas or coal to liquid fuels and wax is a well-established technology. For low H{sub 2} to CO ratio syngas produced from CO{sub 2} reforming of natural gas or from gasification of coal, the use of Fe catalysts is attractive because of their high water gas shift activity in addition to their high FT activity. Fe catalysts are also attractive due to their low cost and low methane selectivity. Because of the highly exothermic nature of the FT reaction, there has been a recent move away from fixed-bed reactors toward the development of slurry bubble column reactors (SBCRs) that employ 30 to 90 {micro}m catalyst particles suspended in a waxy liquid for efficient heat removal. However, the use of FeFT catalysts in an SBCR has been problematic due to severe catalyst attrition resulting in fines that plug the filter employed to separate the catalyst from the waxy product. Fe catalysts can undergo attrition in SBCRs not only due to vigorous movement and collisions but also due to phase changes that occur during activation and reaction.

  14. Promoted Iron Nanocrystals Obtained via Ligand Exchange as Active and Selective Catalysts for Synthesis Gas Conversion (United States)


    Colloidal synthesis routes have been recently used to fabricate heterogeneous catalysts with more controllable and homogeneous properties. Herein a method was developed to modify the surface composition of colloidal nanocrystal catalysts and to purposely introduce specific atoms via ligands and change the catalyst reactivity. Organic ligands adsorbed on the surface of iron oxide catalysts were exchanged with inorganic species such as Na2S, not only to provide an active surface but also to introduce controlled amounts of Na and S acting as promoters for the catalytic process. The catalyst composition was optimized for the Fischer–Tropsch direct conversion of synthesis gas into lower olefins. At industrially relevant conditions, these nanocrystal-based catalysts with controlled composition were more active, selective, and stable than catalysts with similar composition but synthesized using conventional methods, possibly due to their homogeneity of properties and synergic interaction of iron and promoters. PMID:28824820

  15. Application, Deactivation, and Regeneration of Heterogeneous Catalysts in Bio-Oil Upgrading

    Directory of Open Access Journals (Sweden)

    Shouyun Cheng


    Full Text Available The massive consumption of fossil fuels and associated environmental issues are leading to an increased interest in alternative resources such as biofuels. The renewable biofuels can be upgraded from bio-oils that are derived from biomass pyrolysis. Catalytic cracking and hydrodeoxygenation (HDO are two of the most promising bio-oil upgrading processes for biofuel production. Heterogeneous catalysts are essential for upgrading bio-oil into hydrocarbon biofuel. Although advances have been achieved, the deactivation and regeneration of catalysts still remains a challenge. This review focuses on the current progress and challenges of heterogeneous catalyst application, deactivation, and regeneration. The technologies of catalysts deactivation, reduction, and regeneration for improving catalyst activity and stability are discussed. Some suggestions for future research including catalyst mechanism, catalyst development, process integration, and biomass modification for the production of hydrocarbon biofuels are provided.

  16. Catalysts for Efficient Production of Carbon Nanotubes (United States)

    Sun, Ted X.; Dong, Yi


    Several metal alloys have shown promise as improved catalysts for catalytic thermal decomposition of hydrocarbon gases to produce carbon nanotubes (CNTs). Heretofore almost every experiment on the production of carbon nanotubes by this method has involved the use of iron, nickel, or cobalt as the catalyst. However, the catalytic-conversion efficiencies of these metals have been observed to be limited. The identification of better catalysts is part of a continuing program to develop means of mass production of high-quality carbon nanotubes at costs lower than those achieved thus far (as much as $100/g for purified multi-wall CNTs or $1,000/g for single-wall CNTs in year 2002). The main effort thus far in this program has been the design and implementation of a process tailored specifically for high-throughput screening of alloys for catalyzing the growth of CNTs. The process includes an integral combination of (1) formulation of libraries of catalysts, (2) synthesis of CNTs from decomposition of ethylene on powders of the alloys in a pyrolytic chemical-vapor-decomposition reactor, and (3) scanning- electron-microscope screening of the CNTs thus synthesized to evaluate the catalytic efficiencies of the alloys. Information gained in this process is put into a database and analyzed to identify promising alloy compositions, which are to be subjected to further evaluation in a subsequent round of testing. Some of these alloys have been found to catalyze the formation of carbon nano tubes from ethylene at temperatures as low as 350 to 400 C. In contrast, the temperatures typically required for prior catalysts range from 550 to 750 C.

  17. Researching the Possibility of Creating Highly Effective Catalysts for the Thermochemical Heat Regeneration and Hydrocarbon Reforming

    National Research Council Canada - National Science Library

    Kuranov, Alexander L


    ...) develop the plasma spraying technique for applying the catalysts to the substrate material; (3) manufacture samples for testing; and (4) conduct tests to evaluate mechanical and catalytic properties.

  18. Mapping Reactive Flow Patterns in Monolithic Nanoporous Catalysts

    CERN Document Server

    Falcucci, Giacomo; Montessori, Andrea; Melchionna, Simone; Prestininzi, Pietro; Barroo, Cedric; Bell, David C; Biener, Monika M; Biener, Juergen; Zugic, Branko; Kaxiras, Efthimios


    The development of high-efficiency porous catalyst membranes critically depends on our understanding of where the majority of the chemical conversions occur within the porous structure. This requires mapping of chemical reactions and mass transport inside the complex nano-scale architecture of porous catalyst membranes which is a multiscale problem in both the temporal and spatial domain. To address this problem, we developed a multi-scale mass transport computational framework based on the Lattice Boltzmann Method (LBM) that allows us to account for catalytic reactions at the gas-solid interface by introducing a new boundary condition. In good agreement with experiments, the simulations reveal that most catalytic reactions occur near the gas-flow facing side of the catalyst membrane if chemical reactions are fast compared to mass transport within the porous catalyst membrane.

  19. Six-flow operations for catalyst development in Fischer-Tropsch synthesis: bridging the gap between high-throughput experimentation and extensive product evaluation. (United States)

    Sartipi, Sina; Jansma, Harrie; Bosma, Duco; Boshuizen, Bart; Makkee, Michiel; Gascon, Jorge; Kapteijn, Freek


    Design and operation of a "six-flow fixed-bed microreactor" setup for Fischer-Tropsch synthesis (FTS) is described. The unit consists of feed and mixing, flow division, reaction, separation, and analysis sections. The reactor system is made of five heating blocks with individual temperature controllers, assuring an identical isothermal zone of at least 10 cm along six fixed-bed microreactor inserts (4 mm inner diameter). Such a lab-scale setup allows running six experiments in parallel, under equal feed composition, reaction temperature, and conditions of separation and analysis equipment. It permits separate collection of wax and liquid samples (from each flow line), allowing operation with high productivities of C5+ hydrocarbons. The latter is crucial for a complete understanding of FTS product compositions and will represent an advantage over high-throughput setups with more than ten flows where such instrumental considerations lead to elevated equipment volume, cost, and operation complexity. The identical performance (of the six flows) under similar reaction conditions was assured by testing a same catalyst batch, loaded in all microreactors.

  20. Highly Dispersed Alloy Catalyst for Durability

    Energy Technology Data Exchange (ETDEWEB)

    Murthi, Vivek S.; Izzo, Elise; Bi, Wu; Guerrero, Sandra; Protsailo, Lesia


    Achieving DOE's stated 5000-hr durability goal for light-duty vehicles by 2015 will require MEAs with characteristics that are beyond the current state of the art. Significant effort was placed on developing advanced durable cathode catalysts to arrive at the best possible electrode for high performance and durability, as well as developing manufacturing processes that yield significant cost benefit. Accordingly, the overall goal of this project was to develop and construct advanced MEAs that will improve performance and durability while reducing the cost of PEMFC stacks. The project, led by UTC Power, focused on developing new catalysts/supports and integrating them with existing materials (membranes and gas diffusion layers (GDLs)) using state-of-the-art fabrication methods capable of meeting the durability requirements essential for automotive applications. Specifically, the project work aimed to lower platinum group metals (PGM) loading while increasing performance and durability. Appropriate catalysts and MEA configuration were down-selected that protects the membrane, and the layers were tailored to optimize the movements of reactants and product water through the cell to maximize performance while maintaining durability.

  1. Recent Advancements in Stereoselective Olefin Metathesis Using Ruthenium Catalysts


    T. Patrick Montgomery; Johns, Adam M.; Grubbs, Robert H


    Olefin metathesis is a prevailing method for the construction of organic molecules. Recent advancements in olefin metathesis have focused on stereoselective transformations. Ruthenium olefin metathesis catalysts have had a particularly pronounced impact in the area of stereoselective olefin metathesis. The development of three categories of Z-selective olefin metathesis catalysts has made Z-olefins easily accessible to both laboratory and industrial chemists. Further design enhancements to as...

  2. Novel Attrition-Resistant Fischer Tropsch Catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Weast, Logan, E.; Staats, William, R.


    There is a strong national interest in the Fischer-Tropsch synthesis process because it offers the possibility of making liquid hydrocarbon fuels from reformed natural gas or coal and biomass gasification products. This project explored a new approach that had been developed to produce active, attrition-resistant Fischer-Tropsch catalysts that are based on glass-ceramic materials and technology. This novel approach represented a promising solution to the problem of reducing or eliminating catalyst attrition and maximizing catalytic activity, thus reducing costs. The technical objective of the Phase I work was to demonstrate that glass-ceramic based catalytic materials for Fischer-Tropsch synthesis have resistance to catalytic deactivation and reduction of particle size superior to traditional supported Fischer-Tropsch catalyst materials. Additionally, these novel glass-ceramic-based materials were expected to exhibit catalytic activity similar to the traditional materials. If successfully developed, the attrition-resistant Fischer-Tropsch catalyst materials would be expected to result in significant technical, economic, and social benefits for both producers and public consumers of Fischer-Tropsch products such as liquid fuels from coal or biomass gasification. This program demonstrated the anticipated high attrition resistance of the glass-ceramic materials. However, the observed catalytic activity of the materials was not sufficient to justify further development at this time. Additional testing documented that a lack of pore volume in the glass-ceramic materials limited the amount of surface area available for catalysis and consequently limited catalytic activity. However, previous work on glass-ceramic catalysts to promote other reactions demonstrated that commercial levels of activity can be achieved, at least for those reactions. Therefore, we recommend that glass-ceramic materials be considered again as potential Fischer-Tropsch catalysts if it can be

  3. Development of the Ni/Al{sub 2}O{sub 3}/ZrO{sub 2} catalyst to steam reforming of the natural gas process; Desenvolvimento do catalisador Ni/Al2O3/ZrO2 para o processo de reforma do gas natural

    Energy Technology Data Exchange (ETDEWEB)

    Neiva, Laedna Souto; Ramalho, Melanea A.F.; Costa, Ana Cristina Figueiredo de Melo; Gama, Lucianna [Universidade Federal de Campina Grande (UFCG), PB (Brazil); Andrade, Heloysa M.C. [Universidade Federal da Bahia (UFBA), Salvador, BA (Brazil); Kiminami, Ruth Herta G.A. [Universidade Federal de Sao Carlos (UFSCAR), SP (Brazil)


    The aim of this work is to develop catalyst of the type Ni/{alpha}-Al{sub 2}O{sub 3} modified with 0.005 mol of ZrO{sub 2} and structural, morphologic and catalytic characterizations, aiming employ in the reforming process of the natural gas. The catalytic supports were obtained by synthesis method for combustion reaction according to the concepts of the propellants chemistry. The active species of the catalyst (nickel) was deposited over the support by humid impregnation method. The catalytic supports were characterized by XRD, morphologic analysis by SEM and TEM, textural analysis by BET method before and after of the impregnation with nickel and were done catalytic tests in laboratory. The catalytic supports shows structure without any secondary phase with crystallinity elevated degree and crystal size varying between 5.7 and 7.0 nm. The catalytic test shows that these catalysts promoted a conversion percentile considerable of the natural gas in syngas. (author)

  4. Sustainable Utility of Magnetically Recyclable Nano-Catalysts in Water: Applications in Organic Synthesis

    Directory of Open Access Journals (Sweden)

    Manoj B. Gawande


    Full Text Available Magnetically recyclable nano-catalysts and their use in aqueous media is a perfect combination for the development of greener sustainable methodologies in organic synthesis. It is well established that magnetically separable nano-catalysts avoid waste of catalysts or reagents and it is possible to recover >95% of catalysts, which is again recyclable for subsequent use. Water is the ideal medium to perform the chemical reactions with magnetically recyclable nano-catalysts, as this combination adds tremendous value to the overall benign reaction process development. In this review, we highlight recent developments inthe use of water and magnetically recyclable nano-catalysts (W-MRNs for a variety of organic reactions namely hydrogenation, condensation, oxidation, and Suzuki–Miyaura cross-coupling reactions, among others.

  5. Catalytic Converter Developed By Washcoat Of γ-Alumina On Nickel Oxide (Nio Catalyst In FeCrAl Substrate For Exhaust Emission Control : A Review

    Directory of Open Access Journals (Sweden)

    Leman A.M.


    Full Text Available Automobile exhaust emission control is one of the trending issues in automobile research field. The existing catalytic converter using the noble metals of platinum (Pt, palladium (Pd and rhodium (Rd recently were in limited supply and higher in cost. There is a need for the automotive industry to produce ultra-low emitting vehicles at a reasonable cost. The objective of this study is to investigate the effectiveness of methods of fabrication of modified catalytic converter by approaching FeCrAl as a substrate which treated using ultrasonic bath technique to improve the exhaust emission control. The modified catalytic converter preparation will involve the ultrasonic bath process of FeCrAl foil which has fabricated as metallic monolith coated by γ-Al2O3 powder. Nickel as catalyst material will be prepared using electroplating process. The oxidation test will be conducted using a tube and automatic furnace in temperature of 1100°C for 100 hours. Mitsubishi 4G93 1800cc Petrol E.F.I with a multi -gas analyzer equipped with a hydraulic dynamometer will be used for emission measurements of HC, CO, and NOx in varying speed and load for both conditions with and without catalytic converter. The result will expect the γ-Al2O3 as the washcoat material that fully embedded to FeCrAl substrate with the combination of ultrasonic and electroplating technique will effectively convert the CO, NOx and HC to CO2, NO2 and H2O which means that catalytic converter is effective to improve exhaust emission control of diesel engine. The FeCrAl substrate as a metallic catalytic converter which coated by γ-Al2O3 using ultrasonic and nickelelectroplating technique may improve the exhaust emission control.

  6. Fuel cell applications for novel metalloporphyrin catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Ryba, G.; Shelnutt, J.; Doddapaneni, N.; Zavadil, K.


    This project utilized Computer-Aided Molecular Design (CAMD) to develop a new class of metalloporphyrin materials for use as catalysts for two fuel cell reactions. The first reaction is the reduction of oxygen at the fuel cell cathode, and this reaction was the main focus of the research. The second reaction we attempted to catalyze was the oxidation of methanol at the anode. Two classes of novel metalloporphyrins were developed. The first class comprised the dodecaphenylporphyrins whose steric bulk forces them into a non-planar geometry having a pocket where oxygen or methanol is more tightly bound to the porphyrin than it is in the case of planar porphyrins. Significant improvements in the catalytic reduction of oxygen by the dodecaphenyl porphyrins were measured in electrochemical cells. The dodecaphenylporphyrins were further modified by fluorinating the peripheral phenyl groups to varying degrees. The fluorination strongly affected their redox potential, but no effect on their catalytic activity towards oxygen was observed. The second class of porphyrin catalysts was a series of hydrogen-bonding porphyrins whose interaction with oxygen is enhanced. Enhancements in the interaction of oxygen with the porphyrins having hydrogen bonding groups were observed spectroscopically. Computer modeling was performed using Molecular Simulations new CERIUS2 Version 1.6 and a research version of POLYGRAF from Bill Goddard`s research group at the California Institute of Technology. We reoptimized the force field because of an error that was in POLYGRAF and corrected a problem in treatment of the metal in early versions of the program. This improved force field was reported in a J. Am. Chem. Soc. manuscript. Experimental measurements made on the newly developed catalysts included the electrochemical testing in a fuel cell configuration and spectroscopic measurements (UV-Vis, Raman and XPS) to characterize the catalysts.

  7. Catalytic Membranes Embedding Selective Catalysts: Preparation and Applications (United States)

    Drioli, Enrico; Fontananova, Enrica

    The embedding of a catalyst in membranes is today recognized as a promising strategy to develop highly efficient and eco-friendly heterogeneous catalytic chemical processes. When a catalyst is heterogenized within or on the surface of a membrane, the membrane composition (characteristics of the membrane material: hydrophobic or hydrophilic, presence of chemical groups with specific functionality, etc.) and the membrane structure (dense or porous, symmetric or asymmetric), can positively influence the catalyst performance, not only by the selective sorption and diffusion of reagents and/or products, but also influencing the catalyst activity by electronic and conformational effect. These effects are similar to those occurring in biological membranes. In this chapter, after a preliminary presentation of the basic principles of membrane reactors and polymer membranes, the preparation, characterization and applications of polymeric catalytic membranes, will be discussed.

  8. Chalcogen catalysts for polymer electrolyte fuel cell (United States)

    Alonso-Vante, Nicolas [Buxerolles, FR; Zelenay, Piotr [Los Alamos, NM; Choi, Jong-Ho [Los Alamos, NM; Wieckowski, Andrzej [Champaign, IL; Cao, Dianxue [Urbana, IL


    A methanol-tolerant cathode catalyst and a membrane electrode assembly for fuel cells that includes such a cathode catalyst. The cathode catalyst includes a support having at least one transition metal in elemental form and a chalcogen disposed on the support. Methods of making the cathode catalyst and membrane electrode assembly are also described.

  9. Increasing the lifetime of fuel cell catalysts

    NARCIS (Netherlands)

    Latsuzbaia, R.


    In this thesis, I discuss a novel idea of fuel cell catalyst regeneration to increase lifetime of the PEM fuel cell electrode/catalyst operation and, therefore, reduce the catalyst costs. As many of the catalyst degradation mechanisms are difficult to avoid, the regeneration is alternative option to

  10. Impeded solid state reactions and transformations in ceramic catalysts supports and catalysts

    Directory of Open Access Journals (Sweden)

    Ernő E. Kiss


    Full Text Available Impeded chemical reactions and impeded polymorphous transformation in materials are discussed, as desired effects, for stabilization of ceramic catalyst supports and ceramic based catalysts. This paper gives a short overview about the possibilities of slowing down the aging processes in ceramic catalyst supports and catalysts. Special attention is given to alumina and titania based catalysts.

  11. Highly active carbon supported Pd cathode catalysts for direct formic acid fuel cells (United States)

    Mikolajczuk-Zychora, A.; Borodzinski, A.; Kedzierzawski, P.; Mierzwa, B.; Mazurkiewicz-Pawlicka, M.; Stobinski, L.; Ciecierska, E.; Zimoch, A.; Opałło, M.


    One of the drawbacks of low-temperature fuel cells is high price of platinum-based catalysts used for the electroreduction of oxygen at the cathode of the fuel cell. The aim of this work is to develop the palladium catalyst that will replace commonly used platinum cathode catalysts. A series of palladium catalysts for oxygen reduction reaction (ORR) were prepared and tested on the cathode of Direct Formic Acid Fuel Cell (DFAFC). Palladium nanoparticles were deposited on the carbon black (Vulcan) and on multiwall carbon nanotubes (MWCNTs) surface by reduction of palladium(II) acetate dissolved in ethanol. Hydrazine was used as a reducing agent. The effect of functionalization of the carbon supports on the catalysts physicochemical properties and the ORR catalytic activity on the cathode of DFAFC was studied. The supports were functionalized by treatment in nitric acid for 4 h at 80 °C. The structure of the prepared catalysts has been characterized by thermogravimetric analysis (TGA), X-ray diffraction (XRD), transmission electron microscope (TEM) and cyclic voltammetry (CV). Hydrophilicity of the catalytic layers was determined by measuring contact angles of water droplets. The performance of the prepared catalysts has been compared with that of the commercial 20 wt.% Pt/C (Premetek) catalyst. The maximum power density obtained for the best palladium catalyst, deposited on the surface of functionalized carbon black, is the same as that for the commercial Pt/C (Premetek). Palladium is cheaper than platinum, therefore the developed cathode catalyst is promising for future applications.

  12. Catalyst Deactivation: Control Relevance of Model Assumptions

    Directory of Open Access Journals (Sweden)

    Bernt Lie


    Full Text Available Two principles for describing catalyst deactivation are discussed, one based on the deactivation mechanism, the other based on the activity and catalyst age distribution. When the model is based upon activity decay, it is common to use a mean activity developed from the steady-state residence time distribution. We compare control-relevant properties of such an approach with those of a model based upon the deactivation mechanism. Using a continuous stirred tank reactor as an example, we show that the mechanistic approach and the population balance approach lead to identical models. However, common additional assumptions used for activity-based models lead to model properties that may deviate considerably from the correct one.

  13. Spheroidal catalyst for oxidation of sulfur dioxide

    Energy Technology Data Exchange (ETDEWEB)

    Mukhlenov, I.P.; Safonov, I.S.; Khripunov, N.F.


    Fluidized beds have proven useful in a number of oxidation processes, including the oxidation of sulfur dioxide. However, oxidation of SO/sub 2/ to SO/sub 3/ under fluidized bed conditions is a fairly difficult task which involves solving a number of problems of various character. A fluidized bed catalyst (KS catalyst) was developed using the recipes proposed by F.F. Zamyatina and N.S. Gol'derbiter. The support, which permitted the problem of wear resistance to be solved, was spherical aluminosilicate to which a sufficient amount of active component could be applied and whose structure could be easily modified in the synthesis process, thereby creating a specific range of pore sizes providing high activity.

  14. Accelerated deployment of nanostructured hydrotreating catalysts. Final CRADA Report.

    Energy Technology Data Exchange (ETDEWEB)

    Libera, J.A.; Snyder, S.W.; Mane, A.; Elam, J.W.; Cronauer, D.C.; Muntean, J.A.; Wu, T.; Miller, J.T. (Chemical Sciences and Engineering Division); ( ES)


    Nanomanufacturing offers an opportunity to create domestic jobs and facilitate economic growth. In response to this need, U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy issued a Research Call to develop nanomanufacturing capabilities at the National Laboratories. High performance catalysts represent a unique opportunity to deploy nanomanufacturing technologies. Re-refining of used lube oil offers an opportunity to create manufacturing jobs and decrease dependence on imported petroleum. Improved catalysts are required to produce a better quality product, decrease environmental impact, extend catalyst life, and improve overall economics of lube oil re-refining. Argonne National Laboratory (Argonne) in cooperation with Universal Lubricants, Inc. (ULI) and Chemical Engineering Partners (CEP) have carried out a Cooperative Research and Development Agreement (CRADA) to prepare nanostructured hydrotreating catalysts using atomic layer deposition (ALD) to exhibit superior performance for the re-refining of used lube oil. We investigated the upgrading of recycled lube oil by hydrogenation using commercial, synthetically-modified commercial catalysts, and synthesized catalysts. A down-flow (trickle bed) catalytic unit was used for the hydrogenation experiments. In addition to carrying out elemental analyses of the various feed and product fractions, characterization was undertaken using H{sup 1} and C{sup 13} NMR. Initially commercial were evaluated. Second these commercial catalysts were promoted with precious metals using atomic layer deposition (ALD). Performance improvements were observed that declined with catalyst aging. An alternate approach was undertaken to deeply upgrade ULI product oils. Using a synthesized catalyst, much lower hydrogenation temperatures were required than commercial catalysts. Other performance improvements were also observed. The resulting lube oil fractions were of high purity even at low reaction severity. The

  15. Biomass processing over gold catalysts

    CERN Document Server

    Simakova, Olga A; Murzin, Dmitry Yu


    The book describes the valorization of biomass-derived compounds over gold catalysts. Since biomass is a rich renewable feedstock for diverse platform molecules, including those currently derived from petroleum, the interest in various transformation routes has become intense. Catalytic conversion of biomass is one of the main approaches to improving the economic viability of biorefineries.  In addition, Gold catalysts were found to have outstanding activity and selectivity in many key reactions. This book collects information about transformations of the most promising and important compounds derived from cellulose, hemicelluloses, and woody biomass extractives. Since gold catalysts possess high stability under oxidative conditions, selective oxidation reactions were discussed more thoroughly than other critical reactions such as partial hydrogenation, acetalization, and isomerization. The influence of reaction conditions, the role of the catalyst, and the advantages and disadvantages of using gold are pre...

  16. Light Absorbers and Catalysts for Solar to Fuel Conversion (United States)

    Kornienko, Nikolay I.

    Increasing fossil fuel consumption and the resulting consequences to the environment has propelled research into means of utilizing alternative, clean energy sources. Solar power is among the most promising of renewable energy sources but must be converted into an energy dense medium such as chemical bonds to render it useful for transport and energy storage. Photoelectrochemistry (PEC), the splitting of water into oxygen and hydrogen fuel or reducing CO 2 to hydrocarbon fuels via sunlight is a promising approach towards this goal. Photoelectrochemical systems are comprised of several components, including light absorbers and catalysts. These parts must all synergistically function in a working device. Therefore, the continual development of each component is crucial for the overall goal. For PEC systems to be practical for large scale use, the must be efficient, stable, and composed of cost effective components. To this end, my work focused on the development of light absorbing and catalyst components of PEC solar to fuel converting systems. In the direction of light absorbers, I focused of utilizing Indium Phosphide (InP) nanowires (NWs) as photocathodes. I first developed synthetic techniques for InP NW solution phase and vapor phase growth. Next, I developed light absorbing photocathodes from my InP NWs towards PEC water splitting cells. I studied cobalt sulfide (CoSx) as an earth abundant catalyst for the reductive hydrogen evolution half reaction. Using in situ spectroscopic techniques, I elucidated the active structure of this catalyst and offered clues to its high activity. In addition to hydrogen evolution catalysts, I established a new generation of earth abundant catalysts for CO2 reduction to CO fuel/chemical feedstock. I first worked with molecularly tunable homogeneous catalysts that exhibited high selectivity for CO2 reduction in non-aqueous media. Next, in order to retain molecular tunability while achieving stability and efficiency in aqueous

  17. Highly active carbon supported Pd cathode catalysts for direct formic acid fuel cells

    Energy Technology Data Exchange (ETDEWEB)

    Mikolajczuk-Zychora, A., E-mail: [Institute of Physical Chemistry, Polish Academy of Sciences, Kasprzaka 44/52, 01-224 Warsaw (Poland); Borodzinski, A.; Kedzierzawski, P.; Mierzwa, B. [Institute of Physical Chemistry, Polish Academy of Sciences, Kasprzaka 44/52, 01-224 Warsaw (Poland); Mazurkiewicz-Pawlicka, M. [Faculty of Materials Science and Engineering, Warsaw University of Technology, Wołoska 141, 02-507 Warsaw (Poland); Faculty of Chemical and Process Engineering, Warsaw University of Technology, Warynskiego 1, Warsaw (Poland); Stobinski, L. [Institute of Physical Chemistry, Polish Academy of Sciences, Kasprzaka 44/52, 01-224 Warsaw (Poland); Faculty of Chemical and Process Engineering, Warsaw University of Technology, Warynskiego 1, Warsaw (Poland); Ciecierska, E. [Faculty of Materials Science and Engineering, Warsaw University of Technology, Wołoska 141, 02-507 Warsaw (Poland); Zimoch, A.; Opałło, M. [Institute of Physical Chemistry, Polish Academy of Sciences, Kasprzaka 44/52, 01-224 Warsaw (Poland)


    Highlights: • Palladium catalyst used on the cathode DFAFC is comparable to commercial platinum catalyst. • The treatment of carbon supports in nitric acid(V) increases the electrochemically available metal surface area and the catalytic activity in oxygen reduction reaction of catalysts. - Abstract: One of the drawbacks of low-temperature fuel cells is high price of platinum-based catalysts used for the electroreduction of oxygen at the cathode of the fuel cell. The aim of this work is to develop the palladium catalyst that will replace commonly used platinum cathode catalysts. A series of palladium catalysts for oxygen reduction reaction (ORR) were prepared and tested on the cathode of Direct Formic Acid Fuel Cell (DFAFC). Palladium nanoparticles were deposited on the carbon black (Vulcan) and on multiwall carbon nanotubes (MWCNTs) surface by reduction of palladium(II) acetate dissolved in ethanol. Hydrazine was used as a reducing agent. The effect of functionalization of the carbon supports on the catalysts physicochemical properties and the ORR catalytic activity on the cathode of DFAFC was studied. The supports were functionalized by treatment in nitric acid for 4 h at 80 °C. The structure of the prepared catalysts has been characterized by thermogravimetric analysis (TGA), X-ray diffraction (XRD), transmission electron microscope (TEM) and cyclic voltammetry (CV). Hydrophilicity of the catalytic layers was determined by measuring contact angles of water droplets. The performance of the prepared catalysts has been compared with that of the commercial 20 wt.% Pt/C (Premetek) catalyst. The maximum power density obtained for the best palladium catalyst, deposited on the surface of functionalized carbon black, is the same as that for the commercial Pt/C (Premetek). Palladium is cheaper than platinum, therefore the developed cathode catalyst is promising for future applications.

  18. Single-Site Palladium(II) Catalyst for Oxidative Heck Reaction: Catalytic Performance and Kinetic Investigations

    Energy Technology Data Exchange (ETDEWEB)

    Duan, Hui; Li, Mengyang; Zhang, Guanghui; Gallagher, James R.; Huang, Zhiliang; Sun, Yu; Luo, Zhong; Chen, Hongzhong; Miller, Jeffrey T.; Zou, Ruqiang; Lei, Aiwen; Zhao, Yanli


    ABSTRACT: The development of organometallic single-site catalysts (SSCs) has inspired the designs of new heterogeneous catalysts with high efficiency. Nevertheless, the application of SSCs in certain modern organic reactions, such as C-C bond formation reactions, has still been less investigated. In this study, a single-site Pd(II) catalyst was developed, where 2,2'-bipyridine-grafted periodic mesoporous organosilica (PMO) was employed as the support of a Pd(II) complex. The overall performance of the single-site Pd(II) catalyst in the oxidative Heck reaction was then investigated. The investigation results show that the catalyst displays over 99% selectivity for the product formation with high reaction yield. Kinetic profiles further confirm its high catalytic efficiency, showing that the rate constant is nearly 40 times higher than that for the free Pd(II) salt. X-ray absorption spectroscopy reveals that the catalyst has remarkable lifetime and recyclability.

  19. Waste catalysts for waste polymer. (United States)

    Salmiaton, A; Garforth, A


    Catalytic cracking of high-density polyethylene (HDPE) over fluid catalytic cracking (FCC) catalysts (1:6 ratio) was carried out using a laboratory fluidized bed reactor operating at 450 degrees C. Two fresh and two steam deactivated commercial FCC catalysts with different levels of rare earth oxide (REO) were compared as well as two used FCC catalysts (E-Cats) with different levels of metal poisoning. Also, inert microspheres (MS3) were used as a fluidizing agent to compare with thermal cracking process at BP pilot plant at Grangemouth, Scotland, which used sand as its fluidizing agent. The results of HDPE degradation in terms of yield of volatile hydrocarbon product are fresh FCC catalysts>steamed FCC catalysts approximately used FCC catalysts. The thermal cracking process using MS3 showed that at 450 degrees C, the product distribution gave 46 wt% wax, 14% hydrocarbon gases, 8% gasoline, 0.1% coke and 32% nonvolatile product. In general, the product yields from HDPE cracking showed that the level of metal contamination (nickel and vanadium) did not affect the product stream generated from polymer cracking. This study gives promising results as an alternative technique for the cracking and recycling of polymer waste.

  20. Vapor phase hydrogenation of furfural over nickel mixed metal oxide catalysts derived from layered double hydroxides

    Energy Technology Data Exchange (ETDEWEB)

    Sulmonetti, Taylor P.; Pang, Simon H.; Claure, Micaela Taborga; Lee, Sungsik; Cullen, David A.; Agrawal, Pradeep K.; Jones, Christopher W.


    The hydrogenation of furfural is investigated over various reduced nickel mixed metal oxides derived from layered double hydroxides (LDHs) containing Ni-Mg-Al and Ni-Co-Al. Upon reduction, relatively large Ni(0) domains develop in the Ni-Mg-Al catalysts, whereas in the Ni-Co-Al catalysts smaller metal particles of Ni(0) and Co(0), potentially as alloys, are formed, as evidenced by XAS, XPS, STEM and EELS. All the reduced Ni catalysts display similar selectivities towards major hydrogenation products (furfuryl alcohol and tetrahydrofurfuryl alcohol), though the side products varied with the catalyst composition. The 1.1Ni-0.8Co-Al catalyst showed the greatest activity per titrated site when compared to the other catalysts, with promising activity compared to related catalysts in the literature. The use of base metal catalysts for hydrogenation of furanic compounds may be a promising alternative to the well-studied precious metal catalysts for making biomass-derived chemicals if catalyst selectivity can be improved in future work by alloying or tuning metal-oxide support interactions.

  1. Optimum Platinum Loading In Pt/SnO2 CO-Oxidizing Catalysts (United States)

    Schryer, David R.; Upchurch, Billy T.; Davis, Patricia P.; Brown, Kenneth G.; Schryer, Jacqueline


    Platinum on tin oxide (Pt/SnO2) good catalyst for oxidation of carbon monoxide at or near room temperature. Catalytic activity peaks at about 17 weight percent Pt. Catalysts with platinum loadings as high as 46 percent fabricated by technique developed at Langley Research Center. Work conducted to determine optimum platinum loading for this type of catalyst. Major application is removal of unwanted CO and O2 in CO2 lasers.

  2. Organometallic catalysts for primary phosphoric acid fuel cells (United States)

    Walsh, Fraser


    A continuing effort by the U.S. Department of Energy to improve the competitiveness of the phosphoric acid fuel cell by improving cell performance and/or reducing cell cost is discussed. Cathode improvement, both in performance and cost, available through the use of a class of organometallic cathode catalysts, the tetraazaannulenes (TAAs), was investigated. A new mixed catalyst was identified which provides improved cathode performance without the need for the use of a noble metal. This mixed catalyst was tested under load for 1000 hr. in full cell at 160 to 200 C in phosphoric acid H3PO4, and was shown to provide stable performance. The mixed catalyst contains an organometallic to catalyze electroreduction of oxygen to hydrogen peroxide and a metal to catalyze further electroreduction of the hydrogen peroxide to water. Cathodes containing an exemplar mixed catalyst (e.g., Co bisphenyl TAA/Mn) operate at approximately 650 mV vs DHE in 160 C, 85% H3PO4 with oxygen as reactant. In developing this mixed catalyst, a broad spectrum of TAAs were prepared, tested in half-cell and in a rotating ring-disk electrode system. TAAs found to facilitate the production of hydrogen peroxide in electroreduction were shown to be preferred TAAs for use in the mixed catalyst. Manganese (Mn) was identified as a preferred metal because it is capable of catalyzing hydrogen peroxide electroreduction, is lower in cost and is of less strategic importance than platinum, the cathode catalyst normally used in the fuel cell.

  3. Solid Catalysts and theirs Application in Biodiesel Production

    Directory of Open Access Journals (Sweden)

    Ramli Mat


    Full Text Available The reduction of oil resources and increasing petroleum price has led to the search for alternative fuel from renewable resources such as biodiesel. Currently biodiesel is produced from vegetable oil using liquid catalysts. Replacement of liquid catalysts with solid catalysts would greatly solve the problems associated with expensive separation methods and corrosion problems, yielding to a cleaner product and greatly decreasing the cost of biodiesel production. In this paper, the development of solid catalysts and its catalytic activity are reviewed. Solid catalysts are able to perform trans-esterification and esterification reactions simultaneously and able to convert low quality oils with high amount of Free Fatty Acids. The parameters that effect the production of biodiesel are discussed in this paper. Copyright © 2012 by BCREC UNDIP. All rights reservedReceived: 6th April 2012, Revised: 24th October 2012, Accepted: 24th October 2012[How to Cite: R. Mat, R.A. Samsudin, M. Mohamed, A. Johari, (2012. Solid Catalysts and Their Application in Biodiesel Production. Bulletin of Chemical Reaction Engineering & Catalysis, 7(2: 142-149. doi:10.9767/bcrec.7.2.3047.142-149] [How to Link / DOI: ] | View in 

  4. Low Temperature Catalyst for NH3 Removal (United States)

    Monje, Oscar; Melendez, Orlando


    Air revitalization technologies maintain a safe atmosphere inside spacecraft by the removal of C02, ammonia (NH3), and trace contaminants. NH3 onboard the International Space Station (ISS) is produced by crew metabolism, payloads, or during an accidental release of thermal control refrigerant. Currently, the ISS relies on removing NH3 via humidity condensate and the crew wears hooded respirators during emergencies. A different approach to cabin NH3 removal is to use selective catalytic oxidation (SCO), which builds on thermal catalytic oxidation concepts that could be incorporated into the existing TCCS process equipment architecture on ISS. A low temperature platinum-based catalyst (LTP-Catalyst) developed at KSC was used for converting NH3 to H20 and N2 gas by SCO. The challenge of implementing SCO is to reduce formation of undesirable byproducts like NOx (N20 and NO). Gas mixture analysis was conducted using FTIR spectrometry in the Regenerable VOC Control System (RVCS) Testbed. The RVCS was modified by adding a 66 L semi-sealed chamber, and a custom NH3 generator. The effect of temperature on NH3 removal using the LTP-Catalyst was examined. A suitable temperature was found where NH3 removal did not produce toxic NO, (NO, N02) and N20 formation was reduced.

  5. Catalyst preactivation using EURECAT TOTSUCAT CFP technology

    Energy Technology Data Exchange (ETDEWEB)

    Brahma, N.; Alexander, R.; Robinson, J. [Eurecat US Inc., Houston, TX (United States)


    This presentation described EURECAT's newly developed and patented technology that allows the start up of a hydrotreating process without the introduction of sulphur containing chemicals. This ex-situ process known as TOTSUCAT ensures complete activation and sulphiding of the catalyst prior to loading in the reactor. The benefits of TOTSUCAT include the elimination of sour water formation; the prevention of potential exotherms; minimal hydrogen sulphide (H{sub 2}) pressure; and no need for additional hydrogen. TOTSUCAT can be used in cases where the unit has temperature limitations that prevent a complete activation of the catalyst. The TOTSUCAT cracked feed protection (CFP) is an enhanced treatment that combines the advantages of preactivation with the ability to start up a unit with cracked stocks. It eliminates the need to delay the introduction of cracked feeds for 3 to 5 days after start-up, as is typical in commercial hydroprocessing units. The acidity of the catalyst is reduced in the CFP treatment, making it suitable for early introduction of cracked stocks. As such, the technology has potential use in the field of residual hydrocracking. The technology has been successfully applied in several commercial refineries in North America. tabs., figs.

  6. Intermediate Ethanol Blends Catalyst Durability Program

    Energy Technology Data Exchange (ETDEWEB)

    West, Brian H; Sluder, Scott; Knoll, Keith; Orban, John; Feng, Jingyu


    In the summer of 2007, the U.S. Department of Energy (DOE) initiated a test program to evaluate the potential impacts of intermediate ethanol blends (also known as mid-level blends) on legacy vehicles and other engines. The purpose of the test program was to develop information important to assessing the viability of using intermediate blends as a contributor to meeting national goals for the use of renewable fuels. Through a wide range of experimental activities, DOE is evaluating the effects of E15 and E20 - gasoline blended with 15% and 20% ethanol - on tailpipe and evaporative emissions, catalyst and engine durability, vehicle driveability, engine operability, and vehicle and engine materials. This report provides the results of the catalyst durability study, a substantial part of the overall test program. Results from additional projects will be reported separately. The principal purpose of the catalyst durability study was to investigate the effects of adding up to 20% ethanol to gasoline on the durability of catalysts and other aspects of the emissions control systems of vehicles. Section 1 provides further information about the purpose and context of the study. Section 2 describes the experimental approach for the test program, including vehicle selection, aging and emissions test cycle, fuel selection, and data handling and analysis. Section 3 summarizes the effects of the ethanol blends on emissions and fuel economy of the test vehicles. Section 4 summarizes notable unscheduled maintenance and testing issues experienced during the program. The appendixes provide additional detail about the statistical models used in the analysis, detailed statistical analyses, and detailed vehicle specifications.

  7. Study and development of membrane electrode assemblies for Proton Exchange Membrane Fuel Cell (PEMFC) with palladium based catalysts; Estudo e desenvolvimento de conjuntos membrana-eletrodos (MEA) para celula a combustivel de eletrolito polimerico condutor de protons (PEMFC) com eletrocatalisadores a base de paladio

    Energy Technology Data Exchange (ETDEWEB)

    Bonifacio, Rafael Nogueira


    PEMFC systems are capable of generating electricity with high efficiency and low or no emissions, but durability and cost issues prevent its large commercialization. In this work MEA with palladium based catalysts were developed, Pd/C, Pt/C and alloys PdPt/C catalysts with different ratios between metals and carbon were synthesized and characterized. A study of the ratio between catalyst and Nafion Ionomer for formation of high performance triple-phase reaction was carried out, a mathematical model to implement this adjustment to catalysts with different relations between metal and support taking into account the volumetric aspects of the catalyst layer was developed and then a study of the catalyst layer thickness was performed. X-ray diffraction, Transmission and Scanning Electron Microscopy, X-ray Energy Dispersive, Gas Pycnometry, Mercury Intrusion Porosimetry, Gas adsorption according to the BET and BJH equations, and Thermo Gravimetric Analysis techniques were used for characterization and particle size, specific surface areas and lattice parameters determinations were also carried out. All catalysts were used on MEAs preparation and evaluated in 5 cm{sup 2} single cell from 25 to 100 °C at 1 atm and the best composition was also evaluated at 3 atm. In the study of metals for reactions, to reduce the platinum applied to the electrodes without performance losses, Pd/C and PdPt/C 1:1 were selected for anodes and cathodes, respectively. The developed MEA structure used 0,25{sup -2}, showing power densities up to 550{sup -2} and power of 2.2 kW{sub net} per gram of platinum. The estimated costs showed that there was a reduction of up to 64.5 %, compared to the MEA structures previously known. Depending on the temperature and operating pressure, values from US$ 1,475.30 to prepare MEAs for each installed kilowatt were obtained. Taking into account recent studies, it was concluded that the cost of the developed MEA is compatible with PEMFC stationary

  8. Hydrogenation of coal in the presence of stationary wide-pore alumo-cobalt-molybdenum catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Dembovskaya, E.A.; Karmanova, E.L.; Yulin, M.K.; Zaidman, N.M.; Milova, L.P.


    Results are presented from investigations of hydrogenation of Irsha-Borodinsk brown coal on stationary wide-pore alumo-cobalt-molybdenum catalysts. A significant part of the surface area of the catalysts used was made up of pores with radii exceeding 1000 Angstrom. Without the catalysts only 58% of the coal organic mass was converted; with the catalysts 67-84%. The method of hydrogenation was developed by the Institute of Fossil Fuels. The experimental catalysts were prepared by the Institute of Catalysis. Hydrogenation was carried out in a drum autoclave at 420-430 C. The activity of the catalysts was attributed to their porous structure, i.e. a specific ratio between small, medium and large pores, and to the concentration of active components, especially molybdenum oxide. 8 references.

  9. Supported Catalysts Useful in Ring-Closing Metathesis, Cross Metathesis, and Ring-Opening Metathesis Polymerization

    Directory of Open Access Journals (Sweden)

    Jakkrit Suriboot


    Full Text Available Ruthenium and molybdenum catalysts are widely used in synthesis of both small molecules and macromolecules. While major developments have led to new increasingly active catalysts that have high functional group compatibility and stereoselectivity, catalyst/product separation, catalyst recycling, and/or catalyst residue/product separation remain an issue in some applications of these catalysts. This review highlights some of the history of efforts to address these problems, first discussing the problem in the context of reactions like ring-closing metathesis and cross metathesis catalysis used in the synthesis of low molecular weight compounds. It then discusses in more detail progress in dealing with these issues in ring opening metathesis polymerization chemistry. Such approaches depend on a biphasic solid/liquid or liquid separation and can use either always biphasic or sometimes biphasic systems and approaches to this problem using insoluble inorganic supports, insoluble crosslinked polymeric organic supports, soluble polymeric supports, ionic liquids and fluorous phases are discussed.

  10. Development of a catalysts technology to disclosure ultra low emission concepts for vehicles with combustion engines. Final report; Entwicklung einer Katalysatortechnologie zur Darstellung von Niedrigstemissionskonzepten an Kraftfahrzeugen mit Verbrennungsmotor. Abschlussbericht

    Energy Technology Data Exchange (ETDEWEB)

    Reizig, M.; Hirth, P.; Bergmann, A.; Hodgson, J.; Althoefer, K.; Konieczny, R.


    The goal of the research was the development of concepts that support ultra low emission concepts for vehicles with combustion engines. This has been done in the 4 subprojects 'Increase of mass transfer', 'Catalyst isolation', 'Reduction of thermal mass' and 'Homogenization of flow distribution'. In the fifth subproject 'catalyst design' the gained experiences should be used to realize the achieved results for practical applications. Phases of the project: Literature investigation - theoretical consideration and interpretation - investigations on favoured variants - durability tests - study of parameters of manufacturing process - emission tests. The gained experiences were slipped in several products that can be realized in serial production. To be mentioned: (a) The TS-Designs and the LS-Design (see subproject A), (b) the HD-Design (see subproject B, C, E), (c) and the mixing device (see subproject D). Additional know-how was gained in subproject D that was used to work out the PM-Design in a separate developement project. These substrates can be used to reduce soot emissions in vehicles with diesel engines. (orig.) [German] Ziel des Forschungsprojektes war es, in den 4 Teilprojekten 'Verbesserung des Massentransportes', 'Katalysatorisolation', 'Reduzierung der thermischen Masse' und 'Interner Stroemungsausgleich' Konzepte zu entwickeln, die Niedrigstemissionen an Kraftfahrzeugen mit Verbrennungsmotoren unterstuetzen. Im 5. Teilprojekt 'Katalysatordesign' sollten die gewonnenen Erfahrungen ganz oder teilweise genutzt weden, um die erzielten Ergebnisse praktisch umzusetzen. Projektphasen: Literaturrecherche - Theoretische Betrachtung/Auslegung - Untersuchungen an favorisierten Varianten - Dauerhaltbarkeitsuntersuchungen - Studie Fertigungsparameter - Emissionsmessungen. Die im Rahmen des Forschungsprojektes gewonnenen Erkenntnisse konnten in verschiedene Produkte

  11. Effect of catalyst pretreatment on the olefin metathesis catalyzed by alumina-supported (9%) rhenium oxide

    Energy Technology Data Exchange (ETDEWEB)

    Hsu, J.C.


    A kinetic model was developed to express the time-on-stream profile of the activity during catalyst break-in and deactivation. The catalyst surface is in geometric and energetic heterogeneity. Partial catalyst reduction is a prerequisite step for olefin metathesis. The metathesis activity may be affected by the coordination number and the type of ligands associated with the sites on the catalyst. The deactivation is proposed due to deposition of residues on the active sites, and to sintering, etc. A dispersion pretreatment increased activity. Oxygen is an activator. The hydrogen reduction at 500/sup 0/C causes partial but permanent loss of activity.

  12. Graphitic Layer Encapsulated Iron Based Non‐precious Catalysts for the Oxygen Reduction Reaction

    DEFF Research Database (Denmark)

    Zhong, Lijie

    evidences are found from the catalyst synthesized from nitrogen free precursors. This catalyst, consisting of only carbon encapsulated iron-based nanoparticles, shows some, though low, ORR activity, which is enhanced by the post heat treatment in an ammonia atmosphere, indicating the contribution...... are made to develop non-precious metal catalysts (NPMCs) as a replacement to the Pt/C electrocatalysts. In this thesis, a new type of NPMCs is synthesized by means of a dry autoclave with volatile ferrocene and cyanamide as precursors. The catalysts are morphologically featured by porous microspheres...

  13. A Review on Bimetallic Nickel-Based Catalysts for CO2 Reforming of Methane. (United States)

    Bian, Zhoufeng; Das, Sonali; Wai, Ming Hui; Hongmanorom, Plaifa; Kawi, Sibudjing


    In recent years, CO2 reforming of methane (dry reforming of methane, DRM) has become an attractive research area because it converts two major greenhouse gasses into syngas (CO and H2 ), which can be directly used as fuel or feedstock for the chemical industry. Ni-based catalysts have been extensively used for DRM because of its low cost and good activity. A major concern with Ni-based catalysts in DRM is severe carbon deposition leading to catalyst deactivation, and a lot of effort has been put into the design and synthesis of stable Ni catalysts with high carbon resistance. One effective and practical strategy is to introduce a second metal to obtain bimetallic Ni-based catalysts. The synergistic effect between Ni and the second metal has been shown to increase the carbon resistance of the catalyst significantly. In this review, a detailed discussion on the development of bimetallic Ni-based catalysts for DRM including nickel alloyed with noble metals (Pt, Ru, Ir etc.) and transition metals (Co, Fe, Cu) is presented. Special emphasis has been provided on the underlying principles that lead to synergistic effects and enhance catalyst performance. Finally, an outlook is presented for the future development of Ni-based bimetallic catalysts. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  14. Light-off temperature determination of oxidation catalyst using FTIR technique

    Energy Technology Data Exchange (ETDEWEB)

    Hsu, C.C. (Army Chemical Research, Development and Engineering Center, Aberdeen Proving Ground, MD (USA))


    There are various techniques to evaluate the performance of oxidation catalysts. Measurements of surface composition, surface structure, surface area, porosity, acidity, and dispersion of active metals of oxidation catalysts, etc., can be related to the catalyst performance. Other methods such as the decoloration of the indigo carmine solution to correlate the catalytic activity with the flash point and the recorder-equipped calorimeter technique to determine the ignition time, maximum temperature and maximum combustion temperature were used. For an oxidation catalyst, however, one direct measurement of its performance is to determine its light-off temperature, the temperature at which significant oxidation reactions occur. In generation, it is true that the lower the light-off temperature, the more effective will be the catalyst performance. Indeed, this correlation was used in the past to select the optimum reduction temperature and the duration of reduction for the preparation of the best Ni-containing catalyst. The authors have developed an in-situ FTIR technique for simultaneously determining the light-off temperatures and identifying catalytic oxidation products of oxidation catalysts. Using this newly developed technique, three three-way automatic catalysts were evaluated. The details of the subject technique and the results of catalyst performance evaluation are described in this paper.

  15. Formic acid oxidation at platinum-bismuth catalysts

    Directory of Open Access Journals (Sweden)

    Popović Ksenija Đ.


    Full Text Available The field of heterogeneous catalysis, specifically catalysis on bimetallic surfaces, has seen many advances over the past few decades. Bimetallic catalysts, which often show electronic and chemical properties that are distinct from those of their parent metals, offer the opportunity to obtain new catalysts with enhanced selectivity, activity, and stability. The oxidation of formic acid is of permanent interest as a model reaction for the mechanistic understanding of the electrooxidation of small organic molecules and because of its technical relevance for fuel cell applications. Platinum is one of the most commonly used catalysts for this reaction, despite the fact that it shows a few significant disadvantages: high cost and extreme susceptibility to poisoning by CO. To solve this problem, several approaches have been used, but generally, they all consist in the modification of platinum with a second element. Especially, bismuth has received significant attention as Pt modifier. According to the results presented in this survey dealing with the effects influencing the formic acid oxidation it was found that two types of Pt-Bi bimetallic catalysts (bulk and low loading deposits on GC showed superior catalytic activity in terms of the lower onset potential and oxidation current density, as well as exceptional stability compared to Pt. The findings in this report are important for the understanding of mechanism of formic acid electrooxidation on a bulk alloy and decorated surface, for the development of advanced anode catalysts for direct formic acid fuel cells, as well as for the synthesis of novel low-loading bimetallic catalysts. The use of bimetallic compounds as the anode catalysts is an effective solution to overcoming the problems of the formic acid oxidation current stability for long term applications. In the future, the tolerance of both CO poisoning and electrochemical leaching should be considered as the key factors in the development

  16. Rhodium diesel-reforming catalysts for fuel cell applications

    Energy Technology Data Exchange (ETDEWEB)

    Karatzas, Xanthias


    Heavy-duty diesel truck engines are routinely idled at standstill to provide cab heating or air conditioning, and in addition to supply electricity to comfort units such as radio and TV. Idling is an inefficient and unfavorable process resulting in increased fuel consumption, increased emissions, shortened engine life, impaired driver rest and health, and elevated noise. Hydrogen-fueled, polymer-electrolyte fuel-cell auxiliary power unit (PEFC-APU) as a silent external power supply, working independently of the main engine, is proposed as viable solution for better fuel economy and abatement of idling emissions. In a diesel PEFC-APU, the hydrogen storage problem is circumvented as hydrogen can be generated onboard from diesel by using a catalytic reformer. In order to make catalytic diesel PEFC-APU systems viable for commercialization research is still needed. Two key areas are the development of reforming catalyst and reformer design, which both are the scope of this thesis. For diesel-reforming catalysts, low loadings of Rh and RhPt alloys have proven to exhibit excellent reforming and hydrogen selectivity properties. For the development of a stable reforming catalyst, more studies have to be conducted in order to find suitable promoters and support materials to optimize and sustain the long-term performance of the Rh catalyst. The next step will be full-scale tests carried out at realistic operating conditions in order to fully comprehend the overall reforming process and to validate promising Rh catalysts. This thesis can be divided into two parts; the first part addresses the development of catalysts in the form of wash coated cordierite monoliths for autothermal reforming (ATR) of diesel. A variety of catalyst compositions were developed containing Rh or RhPt as active metals, CeO{sub 2}, La{sub 2}O{sub 3}, MgO, Y{sub 2}O{sub 3} as promoters and Al{sub 2}O{sub 3}, CeO{sub 2}-ZrO{sub 2}, SiO{sub 2} and TiO{sub 2} as support materials. The catalysts were tested

  17. Regeneration of Hydrotreating and FCC Catalysts

    Energy Technology Data Exchange (ETDEWEB)

    CM Wai; JG Frye; JL Fulton; LE Bowman; LJ Silva; MA Gerber


    Hydrotreating, hydrocracking, and fluid catalytic cracking (FCC) catalysts are important components of petroleum refining processes. Hydrotreating and hydrocracking catalysts are used to improve the yield of high-quality light oil fractions from heavier crude oil and petroleum feedstocks containing high levels of impurities. FCC catalysts improve the yield of higher octane gasoline from crude oil. Residuum hydrotreating and cracking catalysts are susceptible to irreversible deactivation caused by adsorption of sulfur and by metals impurities, such as vanadium and nickel. The gradual buildup of these impurities in a hydrotreating catalyst eventually plugs the pores and deactivates it. Nickel and vanadium adversely affect the behavior of cracking catalysts, reducing product yield and quality. Replacing deactivated catalysts represents a significant cost in petroleum refining. Equally important are the costs and potential liabilities associated with treating and disposing spent catalysts. For example, recent US Environmental Protection Agency rulings have listed spent hydrotreating and hydrorefining catalysts as hazardous wastes. FCC catalysts, though more easily disposed of as road-base or as filler in asphalt and cement, are still an economic concern mainly because of the large volumes of spent catalysts generated. New processes are being considered to increase the useful life of catalysts or for meeting more stringent disposal requirements for spent catalysts containing metals. This report discusses a collaborative effort between Pacific Northwest National Laboratory (PNNL) and Phillips Petroleum, Inc., to identify promising chemical processes for removing metals adhered to spent hydrodesulfurization (HDS, a type of hydrotreating catalyst) and FCC catalysts. This study, conducted by PNNL, was funded by the US Department of Energy's Bartlesville Project Office. Fresh and spent catalysts were provided by Phillips Petroleum. The FCC catalyst was a rare

  18. Catalyst containing oxygen transport membrane

    Energy Technology Data Exchange (ETDEWEB)

    Lane, Jonathan A.; Wilson, Jamie R.; Christie, Gervase Maxwell; Petigny, Nathalie; Sarantopoulos, Christos


    A composite oxygen transport membrane having a dense layer, a porous support layer and an intermediate porous layer located between the dense layer and the porous support layer. Both the dense layer and the intermediate porous layer are formed from an ionic conductive material to conduct oxygen ions and an electrically conductive material to conduct electrons. The porous support layer has a high permeability, high porosity, and a microstructure exhibiting substantially uniform pore size distribution as a result of using PMMA pore forming materials or a bi-modal particle size distribution of the porous support layer materials. Catalyst particles selected to promote oxidation of a combustible substance are located in the intermediate porous layer and in the porous support adjacent to the intermediate porous layer. The catalyst particles can be formed by wicking a solution of catalyst precursors through the porous support toward the intermediate porous layer.

  19. Catalyst containing oxygen transport membrane (United States)

    Christie, Gervase Maxwell; Wilson, Jamie Robyn; van Hassel, Bart Antonie


    A composite oxygen transport membrane having a dense layer, a porous support layer and an intermediate porous layer located between the dense layer and the porous support layer. Both the dense layer and the intermediate porous layer are formed from an ionic conductive material to conduct oxygen ions and an electrically conductive material to conduct electrons. The porous support layer has a high permeability, high porosity, and a high average pore diameter and the intermediate porous layer has a lower permeability and lower pore diameter than the porous support layer. Catalyst particles selected to promote oxidation of a combustible substance are located in the intermediate porous layer and in the porous support adjacent to the intermediate porous layer. The catalyst particles can be formed by wicking a solution of catalyst precursors through the porous support toward the intermediate porous layer.

  20. Heterogenization of alkene epoxidation catalysts

    Directory of Open Access Journals (Sweden)

    Buffon Regina


    Full Text Available This account describes our efforts to heterogenize epoxidation catalysts. Anchored and sol-gel entrapped molybdenum were shown to be very selective, but had a strongly reduced activity. On the other hand, molybdenum silicates were very active and stable as long as no diols were present in the reaction mixture. Heterogenized rhenium catalysts were less active but allowed the use of anhydrous hydrogen peroxide as oxidant. However, the high cost and difficult regeneration prevents the industrial use of these catalysts. During these investigations, we found that alumina alone is active in the epoxidation with anhydrous hydrogen peroxide, giving good conversions to epoxides with high selectivity. More research is needed in order to clarify the nature of the hydroxyl groups responsible for its catalytic activity and thus to produce an appropriate material which would allow the obtention of epoxides with high selectivity under industrial conditions.

  1. Rural Colleges as Catalysts for Community Change: The RCCI Experience. (United States)

    Rubin, Sarah


    The Rural Community College Initiative challenges colleges in economically distressed regions to become catalysts for economic and community development and improved access to education. Led by college-community teams, the 24 sites have experimented with strategic approaches that include leadership development, entrepreneurship education, small…

  2. Engineering New Catalysts for In-Process Elimination of Tars

    Energy Technology Data Exchange (ETDEWEB)

    Felix, Larry G. [Gas Technology Inst., Des Plaines, IL (United States)


    The key objective of this project was to develop a new and more efficient methodology for engineering and economically producing optimized robust catalysts for the reduction or elimination of tars in biomass gasification. Whereas current catalyst technology typically disposes thin layers of catalytically-active material onto rigid supports via wet chemistry-based methods, this project investigated novel thermal methods for directly incorporating catalytically active materials onto robust supports as well as novel approaches for incorporating catalytically active materials on and/or within an otherwise inert refractory support material which is then subsequently formed and processed to create a catalytically-active material on all exposed surfaces. Specifically, the focus of this engineered catalyst development was on materials which were derived from, or otherwise related to, olivine-like minerals, due to the inherent attrition resistance and moderate catalytic properties exhibited by natural olivine when used in a fluidized bed biomass gasifier. Task 1 of this project successfully demonstrated the direct thermal impregnation of catalytically-active materials onto an olivine substrate, with the production of a Ni-olivine catalyst. Nickel and nickel oxide were thermally impregnated onto an olivine substrate and when reduced were shown to demonstrate improved catalytic activity over the baseline olivine material and equal the tar-decomposing performance of Ni-olivine catalysts prepared by conventional wet impregnation. Task 2 involved coordination with our subcontracted project partners to further develop and characterize catalyst formulations and to optimize activity and production methods. Within this task, several significant new materials were developed. NexTech Materials developed a sintered ceramic nickel-magnesium-silicate catalyst that demonstrated superb catalytic activity and high resistance to deactivation by H2S. Alfred University developed both supported

  3. Bifunctional Nanostructured Base Catalysts: Opportunities for BioFuels

    Energy Technology Data Exchange (ETDEWEB)

    Connor, William


    ABSTRACT This research studied and develop novel basic catalysts for production of renewable chemicals and fuels from biomass. We will focus on the development of unique porous structural-base catalysts formed by two techniques: from (mixed) metal-oxide bases and by nitrogen substitution for oxygen in zeolites. These catalysts will be compared to conventional solid base materials for aldol condensation, catalytic fast pyrolysis, and transesterification reactions. These reactions are important in processes that are currently being commercialized for production of fuels from biomass and will be pivotal in future biomass conversion to fuels and chemicals. Specifically, we have studied the aldol-condensation of acetone with furfural over oxides and zeolites, the conversion of sugars by rapid pyrolysis over zeolites and the trans-esterification of vegetable oil with methanol over mixed oxide catalysts. Our previous research has indicated that the base strength of framework nitrogen in nitrogen-substituted zeolites (NH-zeolites) is nearly twice as strong as in standard zeolites. Nitrogen substituted catalysts have been synthesized from several zeolites (including FAU, MFI, BEA, and LTL) using NH3 treatment.

  4. Noble metal catalysts in the production of biofuels

    Energy Technology Data Exchange (ETDEWEB)

    Gutierrez, A.


    The energy demand is increasing in the world together with the need to ensure energy security and the desire to decrease greenhouse gas emissions. While several renewable alternatives are available for the production of electricity, e.g. solar energy, wind power, and hydrogen, biomass is the only renewable source that can meet the demand for carbon-based liquid fuels and chemicals. The technology applied in the conversion of biomass depends on the type and complexity of the biomass, and the desired fuel. Hydrogen and hydrogen-rich mixtures (synthesis gas) are promising energy sources as they are more efficient and cleaner than existing fuels, especially when they are used in fuel cells. Hydrotreatment is a catalytic process that can be used in the conversion of biomass or biomass-derived liquids into fuels. In autothermal reforming (ATR), catalysts are used in the production of hydrogen-rich mixtures from conventional fuels or bio-fuels. The different nature of biomass and biomass-derived liquids and mineral oil makes the use of catalysts developed for the petroleum industry challenging. This requires the improvement of available catalysts and the development of new ones. To overcome the limitations of conventional hydrotreatment and ATR catalysts, zirconia-supported mono- and bimetallic rhodium, palladium, and platinum catalysts were developed and tested in the upgrading of model compounds for wood-based pyrolysis oil and in the production of hydrogen, using model compounds for gasoline and diesel. Catalysts were also tested in the ATR of ethanol. For comparative purposes commercial catalysts were tested and the results obtained with model compounds were compared with those obtained with real feedstocks (hydrotreatmet tests with wood-based pyrolysis oil and ATR tests with NExBTL renewable diesel). Noble metal catalysts were active and selective in the hydrotreatment of guaiacol used as the model compound for the lignin fraction of wood-based pyrolysis oil and wood

  5. Rhenium Nanochemistry for Catalyst Preparation

    Directory of Open Access Journals (Sweden)

    Vadim G. Kessler


    Full Text Available The review presents synthetic approaches to modern rhenium-based catalysts. Creation of an active center is considered as a process of obtaining a nanoparticle or a molecule, immobilized within a matrix of the substrate. Selective chemical routes to preparation of particles of rhenium alloys, rhenium oxides and the molecules of alkyltrioxorhenium, and their insertion into porous structure of zeolites, ordered mesoporous MCM matrices, anodic mesoporous alumina, and porous transition metal oxides are considered. Structure-property relationships are traced for these catalysts in relation to such processes as alkylation and isomerization, olefin metathesis, selective oxidation of olefins, methanol to formaldehyde conversion, etc.

  6. Bismuth catalysts in aqueous media. (United States)

    Kobayashi, Shū; Ueno, Masaharu; Kitanosono, Taku


    Several bismuth-catalyzed synthetic reactions, which proceed well in aqueous media, are discussed. Due to increasing demand of water as a solvent in organic synthesis, catalysts that can be used in aqueous media are becoming more and more important. Although bismuth Lewis acids are not very stable in water, it has been revealed that they can be stabilized by basic ligands. Chiral amine and related basic ligands combined with bismuth Lewis acids are particularly useful in asymmetric catalysis in aqueous media. On the other hand, bismuth hydroxide is stable and works as an efficient catalyst for carbon-carbon bond-forming reactions in water.

  7. Quick Guide to Flash Catalyst

    CERN Document Server

    Elmansy, Rafiq


    How do you transform user interface designs created in Photoshop or Illustrator into interactive web pages? It's easier than you think. This guide shows you how to use Adobe Flash Catalyst to create interactive UIs and website wireframes for Rich Internet Applications-without writing a single line of code. Ideal for web designers, this book introduces Flash Catalyst basics with detailed step-by-step instructions and screenshots that illustrate every part of the process. You'll learn hands-on how to turn your static design or artwork into working user interfaces that can be implemented in Fla

  8. Novel Fischer-Tropsch catalysts. [DOE patent (United States)

    Vollhardt, K.P.C.; Perkins, P.

    Novel compounds are described which are used as improved Fischer-Tropsch catalysts particularly for the conversion of CO + H/sub 2/ to gaseous and liquid hydrocarbons at milder conditions than with prior catalysts.

  9. Automotive Catalyst State Diagnosis Using Microwaves

    National Research Council Canada - National Science Library

    Moos, Ralf; Fischerauer, Gerhard


    .... The soot or ash loading of Diesel particulate filters, the oxygen loading degree in three-way catalysts, the amount of stored ammonia in SCR catalysts, or the NOx loading degree in NOx storage...

  10. Catalyst for Decomposition of Nitrogen Oxides (United States)

    Schryer, David R. (Inventor); Jordan, Jeffrey D. (Inventor); Akyurtlu, Ates (Inventor); Akyurtlu, Jale (Inventor)


    This invention relates generally to a platinized tin oxide-based catalyst. It relates particularly to an improved platinized tin oxide-based catalyst able to decompose nitric oxide to nitrogen and oxygen without the necessity of a reducing gas.

  11. Quantification of a Heterogeneous Ruthenium Catalyst on Carbon-black using ADF Imaging (United States)

    Varambhia, A. M.; Jones, L.; Nellist, P. D.; Lozano-Perez, S.; Ozkaya, D.


    Using recent developments in ADF quantification techniques, we utilise a rapid atom counting procedure to document the evolution of a heterogeneous ruthenium catalyst on carbon black. Selected areas of the ruthenium catalyst were imaged for approximately 15 minutes. The imaged areas show that the Ru wets the support forming a thin amorphous layer that transforms to a crystalline layer under beam irradiation.

  12. Magnetic silica supported palladium catalyst: synthesis of allyl aryl ethers in water (United States)

    A simple and benign procedure for the synthesis of aryl allyl ethers has been developed using phenols, allyl acetates and magnetically recyclable silica supported palladium catalyst in water; performance of reaction in air and easy separation of the catalyst using an external mag...

  13. New CO tolerant electro-catalysts exceeding Pt-Ru for the anode of fuel cells. (United States)

    Yano, Hiroshi; Ono, Chisato; Shiroishi, Hidenobu; Okada, Tatsuhiro


    Novel types of CO tolerant electro-catalysts from Pt and organic metal complexes that are far superior to Pt-Ru and practically usable as anode catalysts in reformate gas fuel cells with 100 ppm CO tolerance have been developed.

  14. Confined-interface-directed synthesis of Palladium single-atom catalysts on graphene/amorphous carbon

    DEFF Research Database (Denmark)

    Xi, Jiangbo; Sun, Hongyu; Zhang, Zheye


    The maximized atomic efficiency of supported catalysts is highly desired in heterogeneous catalysis. Therefore, the design and development of active, stable, and atomic metal-based catalysts remains a formidable challenge. To tackle these problems, it is necessary to investigate the interaction b...

  15. Supporting Statewide Implementation of the Learning School Initiative. Catalyst Schools Research Study Report (United States)

    Hammer, Patricia Cahape


    This is the first in a series of reports based on a research study, Developing Effective Professional Learning Communities in Catalyst Schools, conducted between February 2015 and June 2016. "Catalyst schools" were elementary- and secondary-level schools selected to participate in a pilot project intended to explore how best to support…

  16. Poly (Ethylene Glycol)-Bound Sulphonic Acid as a Novel Catalyst for ...

    African Journals Online (AJOL)


    cient, reusable, economic and eco-friendly catalyst has led to development of polymer-bound catalyst. They are used in solu- tion phase, solid phase synthesis, microwave-assisted synthesis because these methods offer benefits such as enhanced reaction rate, greater selectivity, ease at experimental work-up and com-.

  17. Catalyst-controlled site-selective asymmetric epoxidation of nerylamine and geranylamine derivatives. (United States)

    Nobuta, Tomoya; Kawabata, Takeo


    Novel catalysts for site- and enantioselective epoxidation of nerylamine and geranylamine derivatives have been developed. Although mCPBA oxidation took place selectively at the more electron-rich double bond to give the 6,7-epoxides, these catalysts provide the 2,3-epoxides in moderate to high enantioselectivity via the oxidation of the relatively electron-deficient double bond.

  18. Cooperative catalysis designing efficient catalysts for synthesis

    CERN Document Server

    Peters, René


    Written by experts in the field, this is a much-needed overview of the rapidly emerging field of cooperative catalysis. The authors focus on the design and development of novel high-performance catalysts for applications in organic synthesis (particularly asymmetric synthesis), covering a broad range of topics, from the latest progress in Lewis acid / Br?nsted base catalysis to e.g. metal-assisted organocatalysis, cooperative metal/enzyme catalysis, and cooperative catalysis in polymerization reactions and on solid surfaces. The chapters are classified according to the type of cooperating acti

  19. Catalyst for Change: An Action Research Study Using Job-Embedded Professional Development to Integrate Technology in a Rural School District (United States)

    Jenkins, William A., Jr.


    This action research study was designed to determine how job-embedded professional development changes teachers' perceptions about integrating technology into their classrooms. The study was based on an action research and matrix/logical analysis design. The researcher facilitated an action research intervention utilizing job-embedded professional…

  20. Selective methane oxidation over promoted oxide catalysts. Topical report, September 8, 1992--September 7, 1996

    Energy Technology Data Exchange (ETDEWEB)

    Klier, K.; Herman, R.G.


    The objective of this research was to selectively oxidize methane to C{sub 2} hydrocarbons and to oxygenates, in particular formaldehyde and methanol, in high space time yields using air at the oxidant under milder reaction conditions that heretofore employed over industrially practical oxide catalysts. The research carried out under this US DOE-METC contract was divided into the following three tasks: Task 1, maximizing selective methane oxidation to C{sub 2}{sup +} products over promoted SrO/La{sub 2}O{sub 3} catalysts; Task 2, selective methane oxidation to oxygenates; and Task 3, catalyst characterization and optimization. Principal accomplishments include the following: the 1 wt% SO{sub 4}{sup 2{minus}}/SrO/La{sub 2}O{sub 3} promoted catalyst developed here produced over 2 kg of C{sub 2} hydrocarbons/kg catalyst/hr at 550 C; V{sub 2}O{sub 5}/SiO{sub 2} catalysts have been prepared that produce up to 1.5 kg formaldehyde/kg catalyst/hr at 630 C with low CO{sub 2} selectivities; and a novel dual bed catalyst system has been designed and utilized to produce over 100 g methanol/kg catalyst/hr at 600 C with the presence of steam in the reactant mixture.

  1. Life Support Catalyst Regeneration Using Ionic Liquids and In Situ Resources (United States)

    Abney, Morgan B.; Karr, Laurel J.; Paley, Mark S.; Donovan, David N.; Kramer, Teersa J.


    Oxygen recovery from metabolic carbon dioxide is an enabling capability for long-duration manned space flight. Complete recovery of oxygen (100%) involves the production of solid carbon. Catalytic approaches for this purpose, such as Bosch technology, have been limited in trade analyses due in part to the mass penalty for high catalyst resupply caused by carbon fouling of the iron or nickel catalyst. In an effort to mitigate this challenge, several technology approaches have been proposed. These approaches have included methods to prolong the life of the catalysts by increasing the total carbon mass loading per mass catalyst, methods for simplified catalyst introduction and removal to limit the resupply container mass, methods of using in situ resources, and methods to regenerate catalyst material. Research and development into these methods is ongoing, but only use of in situ resources and/or complete regeneration of catalyst material has the potential to entirely eliminate the need for resupply. The use of ionic liquids provides an opportunity to combine these methods in a technology approach designed to eliminate the need for resupply of oxygen recovery catalyst. Here we describe the results of an initial feasibility study using ionic liquids and in situ resources for life support catalyst regeneration, we discuss the key challenges with the approach, and we propose future efforts to advance the technology.

  2. Palladium was supported on superparamagnetic nanoparticles: A magnetically recoverable catalyst for Heck reaction

    Energy Technology Data Exchange (ETDEWEB)

    Zhang, Fengwei; Niu, Jianrui; Wang, Haibo; Yang, Honglei; Jin, Jun; Liu, Na; Zhang, Yubin [College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000 (China); Li, Rong, E-mail: [College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000 (China); Ma, Jiantai, E-mail: [College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000 (China)


    Highlights: Black-Right-Pointing-Pointer Palladium-based heterogeneous catalyst was prepared facilely via the co-precipitation method. Black-Right-Pointing-Pointer The particles are nearly spherical in shape with an average size of 20 {+-} 1.0 nm. Black-Right-Pointing-Pointer The developed magnetic catalyst showed high activity for Heck reaction. Black-Right-Pointing-Pointer The catalyst was easily recovered from the reaction mixture with external magnetic field. Black-Right-Pointing-Pointer The catalytic efficiency for Heck reaction remains unaltered even after 6 repeated cycles. -- Abstract: A novel and high-performance palladium-based catalyst for Heck reaction was prepared easily by the co-precipitation method. The catalyst was characterized by transmission electron microscopy (TEM), X-ray powder diffraction (XRD), vibrating sample magnetometry (VSM), X-ray photoelectron spectroscopy (XPS) and atomic absorption spectrophotometry (AAS). The catalyst afforded a fast conversion of the 4-bromonitrobenzene to 4-nitrostilbene at a catalyst loading of 5 mol%, and the efficiency of the catalyst remains unaltered even after 6 repeated cycles. The excellent catalytic performance of the Pd/Fe{sub 3}O{sub 4} catalyst might be attributed to the enhanced synergistic effect between Pd nanoparticles and magnetite.

  3. Synthesis of CaO-CeO2 catalysts by soft template method for biodiesel production (United States)

    Zheng, Y. C.; Yu, X. H.; Yang, J.


    Biodiesel has recently gained extensive attention. Catalysts play an important role in producing biodiesel by transesterification reaction. In this study, CaO-CeO2 catalysts are developed as the solid base catalyst. Using PDMS-PEO as a structure-directing agent, the prepared CaO-CeO2 catalysts have a three-dimensional interconnected porous structure, which benefits the transesterification reaction. While the added Ce slightly decreases the catalytic activity, the stability of the catalyst shows remarkable improvement. Considering the catalytic activity and stability, the best catalyst is determined to be catalyst 0.15-1073 (Ce/Ca molar ratio of 0.15 and calcination temperature of 1073 K). Under optimum reaction conditions, the biodiesel yield reaches to 97.5% and metal leaching is 117.7 ppm. For catalyst 0.15-1073 regenerated after four reaction cycles, the biodiesel yield is 94.1%. The results reveal that the CaO-CeO2 catalyst has good potential for application in large-scale biodiesel production in the future.

  4. Rare behaviour of a catalyst pellet catalyst dynamics

    NARCIS (Netherlands)

    Westerterp, K.R.; Loonen, R.A.; Martens, A.


    Temperature overshoots and undershoots were found for a Pd on alumina catalyst pellet in its course towards a new steady state after a change in concentration of one of the reactants ethylene or hydrogen. When cooling the pellet, after heat-up by reaction, with pure hydrogen a sudden temperature

  5. Paraffin Alkylation Using Zeolite Catalysts in a slurry reactor: Chemical Engineering Principles to Extend Catalyst Lifetime

    NARCIS (Netherlands)

    Jong, K.P. de; Mesters, C.M.A.M.; Peferoen, D.G.R.; Brugge, P.T.M. van; Groot, C. de


    The alkylation of isobutane with 2-butene is carried out using a zeolitic catalyst in a well stirred slurry reactor. Whereas application of fixed bed technology using a solid acid alkylation catalyst has in the led to catalysts lifetimes in the range of minutes, in this work we report catalyst

  6. High Coke-Resistance Pt/Mg1-xNixO Catalyst for Dry Reforming of Methane. (United States)

    Al-Doghachi, Faris A J; Islam, Aminul; Zainal, Zulkarnain; Saiman, Mohd Izham; Embong, Zaidi; Taufiq-Yap, Yun Hin


    A highly active and stable nano structured Pt/Mg1-xNixO catalysts was developed by a simple co-precipitation method. The obtained Pt/Mg1-xNixO catalyst exhibited cubic structure nanocatalyst with a size of 50-80 nm and realized CH4 and CO2 conversions as high as 98% at 900°C with excellent stability in the dry reforming of methane. The characterization of catalyst was performed using various kinds of analytical techniques including XRD, BET, XRF, TPR-H2, TGA, TEM, FESEM, FT-IR, and XPS analyses. Characterization of spent catalyst further confirms that Pt/Mg1-xNixO catalyst has high coke-resistance for dry reforming. Thus, the catalyst demonstrated in this study, offers a promising catalyst for resolving the dilemma between dispersion and reducibility of supported metal, as well as activity and stability during high temperature reactions.

  7. High Coke-Resistance Pt/Mg1-xNixO Catalyst for Dry Reforming of Methane.

    Directory of Open Access Journals (Sweden)

    Faris A J Al-Doghachi

    Full Text Available A highly active and stable nano structured Pt/Mg1-xNixO catalysts was developed by a simple co-precipitation method. The obtained Pt/Mg1-xNixO catalyst exhibited cubic structure nanocatalyst with a size of 50-80 nm and realized CH4 and CO2 conversions as high as 98% at 900°C with excellent stability in the dry reforming of methane. The characterization of catalyst was performed using various kinds of analytical techniques including XRD, BET, XRF, TPR-H2, TGA, TEM, FESEM, FT-IR, and XPS analyses. Characterization of spent catalyst further confirms that Pt/Mg1-xNixO catalyst has high coke-resistance for dry reforming. Thus, the catalyst demonstrated in this study, offers a promising catalyst for resolving the dilemma between dispersion and reducibility of supported metal, as well as activity and stability during high temperature reactions.

  8. High Coke-Resistance Pt/Mg1-xNixO Catalyst for Dry Reforming of Methane (United States)

    Al-Doghachi, Faris A. J.; Islam, Aminul; Zainal, Zulkarnain; Saiman, Mohd Izham; Embong, Zaidi; Taufiq-Yap, Yun Hin


    A highly active and stable nano structured Pt/Mg1-xNixO catalysts was developed by a simple co-precipitation method. The obtained Pt/Mg1-xNixO catalyst exhibited cubic structure nanocatalyst with a size of 50–80 nm and realized CH4 and CO2 conversions as high as 98% at 900°C with excellent stability in the dry reforming of methane. The characterization of catalyst was performed using various kinds of analytical techniques including XRD, BET, XRF, TPR-H2, TGA, TEM, FESEM, FT-IR, and XPS analyses. Characterization of spent catalyst further confirms that Pt/Mg1-xNixO catalyst has high coke-resistance for dry reforming. Thus, the catalyst demonstrated in this study, offers a promising catalyst for resolving the dilemma between dispersion and reducibility of supported metal, as well as activity and stability during high temperature reactions. PMID:26745623

  9. Pt/SnO2-based CO-oxidation catalysts for long-life closed-cycle CO2 lasers (United States)

    Schryer, David R.; Upchurch, Billy T.; Hess, Robert V.; Wood, George M.; Sidney, Barry D.; Miller, Irvin M.; Brown, Kenneth G.; Vannorman, John D.; Schryer, Jacqueline; Brown, David R.


    Noble-metal/tin-oxide based catalysts such as Pt/SnO2 have been shown to be good catalysts for the efficient oxidation of CO at or near room temperature. These catalysts require a reductive pretreatment and traces of hydrogen or water to exhibit their full activity. Addition of Palladium enhances the activity of these catalysts with about 15 to 20 percent Pt, 4 percent Pd, and the balance SnO2 being an optimum composition. Unfortunately, these catalysts presently exhibit significant decay due in part to CO2 retention, probably as a bicarbonate. Research on minimizing the decay in activity of these catalysts is currently in progress. A proposed mechanism of CO oxidation on Pt/SnO2-based catalysts has been developed and is discussed.

  10. Attrition resistant catalysts and sorbents based on heavy metal poisoned FCC catalysts (United States)

    Gangwal, Santosh; Jothimurugesan, Kandaswamy


    A heavy metal poisoned, spent FCC catalyst is treated by chemically impregnating the poisoned catalyst with a new catalytic metal or metal salt to provide an attrition resistant catalyst or sorbent for a different catalytic or absorption processes, such as catalysts for Fischer-Tropsh Synthesis, and sorbents for removal of sulfur gasses from fuel gases and flue-gases. The heavy metal contaminated FCC catalyst is directly used as a support for preparing catalysts having new catalytic properties and sorbents having new sorbent properties, without removing or "passivating" the heavy metals on the spent FCC catalyst as an intermediate step.

  11. The Universal Basic Education (UBE) Programme and Women Entrepreneurship in Science and Technology: a Catalyst for Enhancing Female Participation in National Development


    J.B. Bilesanmi-Awoderu; O.O. Kalesanwo


    This paper discussed how UBE programme could be used to promote women entrepreneurship in science and technology with the resultant effect of enhance female scientists’ participation in National development in Nigeria. Relevant literature on – UBE programme, Entrepreneurship, women entrepreneurship and women scientists were thoroughly reviewed. Militating factors against women scientists’ entrepreneurship in Nigeria were established. Based on these factors, suggestions for encouraging and pro...

  12. Efficient epoxidation of propene using molecular catalysts

    DEFF Research Database (Denmark)

    Markovits, Iulius I. E.; Anthofer, Michael H.; Kolding, Helene


    The epoxidation of propene is performed in homogeneous phase using various molecular catalysts and H2O2 or tert-butyl hydroperoxide as oxidants. A comparison between some molybdenum catalysts and methyltrioxorhenium (MTO) shows that the well known Re catalyst is the best among the examined...

  13. Low platinum catalyst and method of preparation

    Energy Technology Data Exchange (ETDEWEB)

    Liu, Di-Jia; Chong, Lina


    A low platinum catalyst and method for making same. The catalyst comprises platinum-transition metal bimetallic alloy microcrystallites over a transition metal-nitrogen-carbon composite. A method of making a catalyst comprises preparation of transition metal organic frameworks, infusion of platinum, thermal treatment, and reduction to form the microcrystallites and composite.

  14. Novel non-platinum metal catalyst material

    DEFF Research Database (Denmark)


    The present invention relates to a novel non-platinum metal catalyst material for use in low temperature fuel cells and electrolysers and to fuel cells and electrolysers comprising the novel non-platinum metal catalyst material. The present invention also relates to a novel method for synthesizing...... the novel non-platinum metal catalyst material....

  15. Catalysts and methods of using the same (United States)

    Slowing, Igor Ivan; Kandel, Kapil


    The present invention provides a catalyst including a mesoporous silica nanoparticle and a catalytic material comprising iron. In various embodiments, the present invention provides methods of using and making the catalyst. In some examples, the catalyst can be used to hydrotreat fatty acids or to selectively remove fatty acids from feedstocks.

  16. Catalyst Deactivation Simulation Through Carbon Deposition in Carbon Dioxide Reforming over Ni/CaO-Al2O3 Catalyst

    Directory of Open Access Journals (Sweden)

    Istadi Istadi


    Full Text Available Major problem in CO2 reforming of methane (CORM process is coke formation which is a carbonaceous residue that can physically cover active sites of a catalyst surface and leads to catalyst deactivation. A key to develop a more coke-resistant catalyst lies in a better understanding of the methane reforming mechanism at a molecular level. Therefore, this paper is aimed to simulate a micro-kinetic approach in order to calculate coking rate in CORM reaction. Rates of encapsulating and filamentous carbon formation are also included. The simulation results show that the studied catalyst has a high activity, and the rate of carbon formation is relatively low. This micro-kinetic modeling approach can be used as a tool to better understand the catalyst deactivation phenomena in reaction via carbon deposition. Copyright © 2011 BCREC UNDIP. All rights reserved.(Received: 10th May 2011; Revised: 16th August 2011; Accepted: 27th August 2011[How to Cite: I. Istadi, D.D. Anggoro, N.A.S. Amin, and D.H.W. Ling. (2011. Catalyst Deactivation Simulation Through Carbon Deposition in Carbon Dioxide Reforming over Ni/CaO-Al2O3 Catalyst. Bulletin of Chemical Reaction Engineering & Catalysis, 6 (2: 129-136. doi:10.9767/bcrec.6.2.1213.129-136][How to Link / DOI: || or local: ] | View in  |  

  17. Fundamental investigations of catalyst nanoparticles

    DEFF Research Database (Denmark)

    Elkjær, Christian Fink

    of better catalysts. It was found that sintering proceeded via Ostwald ripening, i. e. the migration of atomic species between particles, with a net flow from small to larger particles resulting in an overall growth in particle size. The presence of CO increased the rate of sintering significantly...

  18. Organic Synthesis using Clay Catalysts

    Indian Academy of Sciences (India)

    Home; Journals; Resonance – Journal of Science Education; Volume 7; Issue 1. Organic Synthesis using Clay Catalysts - Clays for 'Green Chemistry'. Gopalpur Nagendrappa. General Article Volume 7 Issue 1 January 2002 pp 64-77. Fulltext. Click here to view fulltext PDF. Permanent link:

  19. Catalyst. Issue 2, Fall 2008 (United States)

    Hawkins, B. Denise, Ed.


    Catalyst, a quarterly newsletter from the Institute's Communications Office, contains news, information, and features about the programs and services of the National Institute for Literacy. Contents of this issue include: (1) Shanahan on the National Early Literacy Panel Report: What's in Store; (2) Director's Message; (3) Representative Fattah to…

  20. Perovskite catalysts for oxidative coupling (United States)

    Campbell, Kenneth D.


    Perovskites of the structure A.sub.2 B.sub.2 C.sub.3 O.sub.10 are useful as catalysts for the oxidative coupling of lower alkane to heavier hydrocarbons. A is alkali metal; B is lanthanide or lanthanum, cerium, neodymium, samarium, praseodymium, gadolinium or dysprosium; and C is titanium.

  1. Development of Asymmetric Hydrogenation Catalysts via High Throughput Experimentation Développement de catalyseurs d’hydrogénation asymétrique par criblage haut débit

    Directory of Open Access Journals (Sweden)

    de Vries J. G.


    Full Text Available The dynamics of drugs discovery imposes severe time constraints on the development chemist in charge of implementing the large scale production of a new Active Pharmaceutical Ingredient (API. This results in the use of well-established and robust transformations at the expense of the cost-efficiency and the sustainability of the process. In order to cope with the short development time and allow the implementation of new more efficient production technologies such as asymmetric hydrogenation, we have turned towards the use of high throughput experimentation for the discovery of new catalysts. The protocol for the preparation of a library of chiral ligands and its application to real-life pharmaceutical molecules is described in this article. La découverte de nouvelles molécules pharmaceutiques a sa propre dynamique qui impose des contraintes temporelles très strictes au chimiste en charge de développer la production du principe actif à large échelle. En conséquence, ce dernier va se tourner vers l’utilisation de technologies éprouvées et robustes quitte à rendre le procédé plus coûteux ou plus polluant. Afin de pouvoir faire face à des temps de développement très courts et d’introduire en production des technologies modernes et non polluantes comme l’hydrogénation asymétrique, nous avons développé une plateforme de criblage haut débit pour la découverte de nouveaux catalyseurs. Dans cet article, nous décrivons une des facettes de cette plateforme qui est la synthèse de librairies de ligands chiraux et leur application au cas réel d’une molécule pharmaceutique.

  2. Supported Catalysts for CO2 Methanation: A Review

    Directory of Open Access Journals (Sweden)

    Patrizia Frontera


    Full Text Available CO2 methanation is a well-known reaction that is of interest as a capture and storage (CCS process and as a renewable energy storage system based on a power-to-gas conversion process by substitute or synthetic natural gas (SNG production. Integrating water electrolysis and CO2 methanation is a highly effective way to store energy produced by renewables sources. The conversion of electricity into methane takes place via two steps: hydrogen is produced by electrolysis and converted to methane by CO2 methanation. The effectiveness and efficiency of power-to-gas plants strongly depend on the CO2 methanation process. For this reason, research on CO2 methanation has intensified over the last 10 years. The rise of active, selective, and stable catalysts is the core of the CO2 methanation process. Novel, heterogeneous catalysts have been tested and tuned such that the CO2 methanation process increases their productivity. The present work aims to give a critical overview of CO2 methanation catalyst production and research carried out in the last 50 years. The fundamentals of reaction mechanism, catalyst deactivation, and catalyst promoters, as well as a discussion of current and future developments in CO2 methanation, are also included.

  3. Hydrogen Production by Steam Reforming of Liquefied Natural Gas (LNG) Over Nickel-Phosphorus-Alumina Xerogel Catalyst Prepared by a Carbon-Templating Epoxide-Driven Sol-Gel Method. (United States)

    Bang, Yongju; Park, Seungwon; Han, Seung Ju; Yoo, Jaekyeong; Choi, Jung Ho; Kang, Tae Hun; Lee, Jinwon; Song, In Kyu


    A nickel-phosphorus-alumina xerogel catalyst was prepared by a carbon-templating epoxide-driven sol-gel method (denoted as CNPA catalyst), and it was applied to the hydrogen production by steam reforming of liquefied natural gas (LNG). For comparison, a nickel-phosphorus-alumina xerogel catalyst was also prepared by a similar method in the absence of carbon template (denoted as NPA catalyst). The effect of carbon template addition on the physicochemical properties and catalytic activities of the catalysts in the steam reforming of LNG was investigated. Both CNPA and NPA catalysts showed excellent textural properties with well-developed mesoporous structure. However, CNPA catalyst retained a more reducible nickel aluminate phase than NPA catalyst. XRD analysis of the reduced CNPA and NPA catalysts revealed that nickel sintering on the CNPA catalyst was suppressed compared to that on the NPA catalyst. From H2-TPD and CH4-TPD measurements of the reduced CNPA and NPA catalysts, it was also revealed that CNPA catalyst with large amount of hydrogen uptake and strong hydrogen-binding sites showed larger amount of methane adsorption than NPA catalyst. In the hydrogen production by steam reforming of LNG, CNPA catalyst with large methane adsorption capacity showed a better catalytic activity than NPA catalyst.

  4. Design, synthesis, and characterization of novel fine-particle, unsupported catalysts for coal liquefaction. Technical progress report, October 25, 1990--October 24, 1991: Draft

    Energy Technology Data Exchange (ETDEWEB)

    Klein, M.T.


    The purpose of this work is to investigate the kinetics-assisted design, synthesis and characterization of fme-pardcle, unsupported catalysts for coal liquefaction. The goal is to develop a fundamental understanding of coal catalysis and catalysts that will, in turn, allow for the specification of a novel optimal catalyst for coal liquefaction.

  5. Industrial production of catalyst 5058

    Energy Technology Data Exchange (ETDEWEB)

    von Fuener, W.


    Catalyst 5058 was tungsten sulfide, WS/sub 2/. It was produced from tungstic acid, WO/sub 3/.H/sub 2/O, which was itself produced from concentrated tungsten ores. The formation of tungstic acid from the ore proceeded in two or three cycles of dissolving the substance in a base (sodium hydroxide, ammonia, lime), decomposing the result with acid, and the filtering, washing, and drying the resulting impure tungstic acid. The final tungstic acid had only about 0.2% impurities. The formation of tungsten sulfide from the tungstic acid proceeded in several steps. First, the tungstic acid was reacted with ammonium hydroxide to give ammonium tungstate, (NH/sub 4/)/sub 2/WO/sub 4/, which was then saturated with hydrogen sulfide to give ammonium sulfotungstate, (NH/sub 4/)/sub 2/WS/sub 4/, which precipitated out of solution at reduced temperature as monoclinic crystals in an orange-red powder. The saturation itself had to be done at about 70/sup 0/C to prevent formation (and later coprecipitation) of an interfering oxysulfate compound, (NH/sub 4/)/sub 2/WO/sub 2/S/sub 2/. The ammonium sulfotungstate precipitate was filtered out under suction and dried in hydrogen in a steam-heated vessel. The ammonium sulfotungstate was then decomposed in a stream of hydrogen in a furnace, at high temperature, to give tungsten sulfide in a monoclinic crystalline structure, which was different from the usual hexagonal crystal structure of tungsten sulfide. The resulting porous structure of the crystal lattice contributed to the activity of the catalyst. Finally, the catalyst was powdered into a fine powder and then compressed into cylindrical tablets as the form in which the catalyst was introduced into the hydrogenation ovens for use. Regeneration of the catalyst was necessary after 1 or 2 years of use.

  6. Alternative alkali resistant deNOx catalysts

    DEFF Research Database (Denmark)

    Putluru, Siva Sankar Reddy; Kristensen, Steffen Buus; Due-Hansen, Johannes


    potassium doping (250 and 280 µmol of K/g, respectively). The increased poisoning resistance was due to high substrate acidity (sulphated, heteropoly acid promoted and zeolite supports), substituting the active species of the catalyst (other than vanadium species, i.e. Cu, Fe) and new catalyst synthesis...... by onepot sol–gel method. All catalysts were characterized by BET, XRPD and NH3-TPD. Initial SCR activities of 8 out of 9 catalysts showed higher NO conversion at least at one temperature in the temperature range 300–500 ◦C compared to the conventional V2O5-WO3/TiO2 catalyst. After potassium poisoning (100...

  7. Mechanism for the Sabatier reaction over a nickel catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Naumov, V.A.; Krylov, O.V.


    A mechanism for the Sabatier reaction over a nickel catalyst has been developed for the whole range of hydrogen/carbon dioxide molar ratios, based on the previously derived kinetic equation. The mechanism consists of five reversible elementary reactions, each occurring on a uniform catalyst surface, with no rate-limiting step and involves the formation from gas-phase CO/sub 2/ and adsorbed H/sub 2/ of a surface C(OH)/sub 2/ radical which is consecutively hydrogenated by gas-phase H/sub 2/ to CHOH and CH/sub 2/ surface species and gas-phase methane.

  8. Estimation of Kinetic Parameters in an Automotive SCR Catalyst Model

    DEFF Research Database (Denmark)

    Åberg, Andreas; Widd, Anders; Abildskov, Jens


    A challenge during the development of models for simulation of the automotive Selective Catalytic Reduction catalyst is the parameter estimation of the kinetic parameters, which can be time consuming and problematic. The parameter estimation is often carried out on small-scale reactor tests......, or powder samples of the catalyst, which leads to problems when upscaling is done to the full-scale application. This contribution presents a methodology to sequentially estimate the kinetic parameters in 2 steps using steady-state limited small-scale reactor data, with the goal that the parameters should...

  9. Chemical interactions in multimetal/zeolite catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Sachtler, W.M.H.


    For Pt/NaY catalysts our analysis of the mechanism of metal particle formation has enabled us to produce at will samples which contain either the majority of the Pt particles in supercages, without filling these cages completely, or the Pt particles bulge into neighboring cages. The catalytic selectivity is distinctly different for these preparations, in the former case molecules can enter a supercage which is partially filled by the Pt cluster, in the second case adsorption takes place through the cage window. Applying the same principles of catalyst preparation of bimetallic catalysts enables us to produce PtCu particles in supercages of NaY, which contain, initially a Pt core, surrounded by a Cu mantle. Earlier we have found that Ni ions migrate into hexagonal prisms during calcination of Ni/NaY; this process can be partially suppressed by first filling these prisms with Mn or Cr ions. In more recent work we found that addition of Pt strongly lowers the temperature of Ni reduction. Part of the Ni ions is reduced by hydrogen while still inside the smaller cages. This reduction process is, however, reversible; at elevated temperature and in an inert atmosphere protons re-oxidize the Ni atoms and dihydrogen gas is developed. In this way it seems possible to count the Ni atoms in small cages. The calcination stage in the preparation of zeolite supported metals has been studied in considerable detail for Pd/NaY. The Pd is introduced as a tetrammin complex; during calcination the ammine ligands are successively oxidized. Once three ammine ligands are destroyed, the Pd ions which carry only one ligand, surprisingly jump from the supercages to the sodalite cage.

  10. Automotive Catalyst State Diagnosis Using Microwaves

    Directory of Open Access Journals (Sweden)

    Moos Ralf


    Full Text Available The state of catalysts plays a key role in automotive exhaust gas aftertreatment. The soot or ash loading of Diesel particulate filters, the oxygen loading degree in three-way catalysts, the amount of stored ammonia in SCR catalysts, or the NOx loading degree in NOx storage catalysts are important parameters that are today determined indirectly and in a model-based manner with gas sensors installed upstream and/or downstream of the catalysts. This contribution gives an overview on a novel approach to determine the catalyst state directly by a microwave-based technique. The method exploits the fact that the catalyst housing acts as a microwave cavity resonator. As “sensing” elements, one or two simple antennas are mounted inside the catalyst canning. The electrical properties of the catalyst device (ceramic honeycomb plus coating and storage material can be measured. Preferably, the resonance characteristics, e.g., the resonance frequencies, of selected cavity modes are observed. The information on the catalyst interior obtained in such a contactless manner is very well correlated with the catalyst state as will be demonstrated for different exhaust gas aftertreatment systems.

  11. Iron Fischer-Tropsch Catalysts Prepared by Solvent-Deficient Precipitation (SDP: Effects of Washing, Promoter Addition Step, and Drying Temperature

    Directory of Open Access Journals (Sweden)

    Kyle M. Brunner


    Full Text Available A novel, solvent-deficient precipitation (SDP method for catalyst preparation in general and for preparation of iron FT catalysts in particular is reported. Eight catalysts using a 23 factorial design of experiments to identify the key preparation variables were prepared. The catalysts were characterized by electron microprobe, N2 adsorption, TEM, XRD, and ICP. Results show that the morphology of the catalysts, i.e., surface area, pore volume, pore size distribution, crystallite sizes, and promoter distribution are significantly influenced by (1 whether or not the precursor catalyst is washed, (2 the promoter addition step, and (3 the drying condition (temperature. Consequently, the activity, selectivity, and stability of the catalysts determined from fixed-bed testing are also affected by these three variables. Unwashed catalysts prepared by a one-step method and dried at 100 °C produced the most active catalysts for FT synthesis. The catalysts of this study prepared by SDP compared favorably in activity, productivity, and stability with Fe FT catalysts reported in the literature. It is believed that this facile SDP approach has promise for development of future FT catalysts, and also offers a potential alternate route for the preparation of other catalysts for various other applications.


    Energy Technology Data Exchange (ETDEWEB)

    Michael T. Klein


    There are several aspects of the Direct Coal Liquefaction process which are not fully understood and which if better understood might lead to improved yields and conversions. Among these questions are the roles of the catalyst and the solvent. While the solvent is known to act by transfer of hydrogen atoms to the free radicals formed by thermal breakdown of the coal in an uncatalyzed system, in the presence of a solid catalyst as is now currently practiced, the yields and conversions are higher than in an uncatalyzed system. The role of the catalyst in this case is not completely understood. DOE has funded many projects to produce ultrafine and more active catalysts in the expectation that better contact between catalyst and coal might result. This approach has met with limited success probably because mass transfer between two solids in a fluid medium i.e. the catalyst and the coal, is very poor. It is to develop an understanding of the role of the catalyst and solvent in Direct Liquefaction that this project was initiated. Specifically it was of interest to know whether direct contact between the coal and the catalyst was important. By separating the solid catalyst in a stainless steel basket permeable to the solvent but not the coal in the liquefaction reactor, it was shown that the catalyst still maintains a catalytic effect on the liquefaction process. There is apparently transfer of hydrogen atoms from the catalyst through the basket wall to the coal via the solvent. Strong hydrogen donor solvents appear to be more effective in this respect than weak hydrogen donors. It therefore appears that intimate contact between catalyst and coal is not a requirement, and that the role of the catalyst may be to restore the hydrogen donor strength to the solvent as the reaction proceeds. A range of solvents of varying hydrogen donor strength was investigated. Because of the extensive use of thermogravimetric analysis in this laboratory in was noted that the peak

  13. Autothermal reforming catalyst having perovskite structure (United States)

    Krumpel, Michael [Naperville, IL; Liu, Di-Jia [Naperville, IL


    The invention addressed two critical issues in fuel processing for fuel cell application, i.e. catalyst cost and operating stability. The existing state-of-the-art fuel reforming catalyst uses Rh and platinum supported over refractory oxide which add significant cost to the fuel cell system. Supported metals agglomerate under elevated temperature during reforming and decrease the catalyst activity. The catalyst is a perovskite oxide or a Ruddlesden-Popper type oxide containing rare-earth elements, catalytically active firs row transition metal elements, and stabilizing elements, such that the catalyst is a single phase in high temperature oxidizing conditions and maintains a primarily perovskite or Ruddlesden-Popper structure under high temperature reducing conditions. The catalyst can also contain alkaline earth dopants, which enhance the catalytic activity of the catalyst, but do not compromise the stability of the perovskite structure.

  14. Nanoscale intimacy in bifunctional catalysts for selective conversion of hydrocarbons (United States)

    Zecevic, Jovana; Vanbutsele, Gina; de Jong, Krijn P.; Martens, Johan A.


    The ability to control nanoscale features precisely is increasingly being exploited to develop and improve monofunctional catalysts. Striking effects might also be expected in the case of bifunctional catalysts, which are important in the hydrocracking of fossil and renewable hydrocarbon sources to provide high-quality diesel fuel. Such bifunctional hydrocracking catalysts contain metal sites and acid sites, and for more than 50 years the so-called intimacy criterion has dictated the maximum distance between the two types of site, beyond which catalytic activity decreases. A lack of synthesis and material-characterization methods with nanometre precision has long prevented in-depth exploration of the intimacy criterion, which has often been interpreted simply as ‘the closer the better’ for positioning metal and acid sites. Here we show for a bifunctional catalyst—comprising an intimate mixture of zeolite Y and alumina binder, and with platinum metal controllably deposited on either the zeolite or the binder—that closest proximity between metal and zeolite acid sites can be detrimental. Specifically, the selectivity when cracking large hydrocarbon feedstock molecules for high-quality diesel production is optimized with the catalyst that contains platinum on the binder, that is, with a nanoscale rather than closest intimacy of the metal and acid sites. Thus, cracking of the large and complex hydrocarbon molecules that are typically derived from alternative sources, such as gas-to-liquid technology, vegetable oil or algal oil, should benefit especially from bifunctional catalysts that avoid locating platinum on the zeolite (the traditionally assumed optimal location). More generally, we anticipate that the ability demonstrated here to spatially organize different active sites at the nanoscale will benefit the further development and optimization of the emerging generation of multifunctional catalysts.

  15. Catalyst for Carbon Monoxide Oxidation (United States)

    Davis, Patricia; Brown, Kenneth; VanNorman, John; Brown, David; Upchurch, Billy; Schryer, David; Miller, Irvin


    In many applications, it is highly desirable to operate a CO2 laser in a sealed condition, for in an open system the laser requires a continuous flow of laser gas to remove the dissociation products that occur in the discharge zone of the laser, in order to maintain a stable power output. This adds to the operating cost of the laser, and in airborne or space applications, it also adds to the weight penalty of the laser. In a sealed CO2 laser, a small amount of CO2 gas is decomposed in the electrical discharge zone into corresponding quantities of CO and O2. As the laser continues to operate, the concentration of CO2 decreases, while the concentrations of CO and O2 correspondingly increase. The increasing concentration of O2 reduces laser power, because O2 scavenges electrons in the electrical discharge, thereby causing arcing in the electric discharge and a loss of the energetic electrons required to boost CO2 molecules to lasing energy levels. As a result, laser power decreases rapidly. The primary object of this invention is to provide a catalyst that, by composition of matter alone, contains chemisorbed water within and upon its structure. Such bound moisture renders the catalyst highly active and very long-lived, such that only a small quantity of it needs to be used with a CO2 laser under ambient operating conditions. This object is achieved by a catalyst that consists essentially of about 1 to 40 percent by weight of one or more platinum group metals (Pt, Pd, Rh, Ir, Ru, Os, Pt being preferred); about 1 to 90 percent by weight of one or more oxides of reducible metals having multiple valence states (such as Sn, Ti, Mn, Cu, and Ce, with SnO2 being preferred); and about 1 to 90 percent by weight of a compound that can bind water to its structure (such as silica gel, calcium chloride, magnesium sulfate, hydrated alumina, and magnesium perchlorate, with silica gel being preferred). Especially beneficial results are obtained when platinum is present in the

  16. SunShot Catalyst Prize Competition Fact Sheet

    Energy Technology Data Exchange (ETDEWEB)

    Solar Energy Technologies Office


    This fact sheet is an overview of the Catalyst Energy Innovation Prize, an open innovation program launched in 2014 by the U.S. Department of Energy SunShot Initiative. This program aims to catalyze the rapid creation and development of products and solutions that address near-term challenges in the U.S. solar energy marketplace.

  17. Early intervention as a catalyst for effective early childhood ...

    African Journals Online (AJOL)

    Early childhood intervention is an essential contributor and catalyst for the development of a culture of positive attitudes towards children with disabilities in a country like Ghana. ... This would provide mutual benefits for children with disabilities, parents and families, educators and professionals and the society at large.

  18. Renewable feedstocks: the problem of catalyst deactivation and its mitigation

    NARCIS (Netherlands)

    Lange, Jean Paul


    Much research has been carried out in the last decade to convert bio-based feedstock into fuels and chemicals. Most of the research focuses on developing active and selective catalysts, with much less attention devoted to their long-term stability. This Review considers the main challenges in

  19. An efficient ultrasound promoted catalyst-free protocol for the ...

    Indian Academy of Sciences (India)

    A convenient, catalyst-free protocol for the quantitative synthesis of fused chromeno[4,3-b]quinolin-6-ones has been developed by simple one-pot reaction of substituted anilines with 4-chloro-3-formylcoumarin using ultrasound irradiation. The protocol offers the advantages of mild reaction conditions, short reaction times ...

  20. Development of the first well-defined tungsten oxo alkyl derivatives supported on silica by SOMC: towards a model of WO3/SiO2 olefin metathesis catalyst

    KAUST Repository

    Mazoyer, Etienne


    A well-defined, silica-supported tungsten oxo alkyl species prepared by the surface organometallic chemistry approach displays high and sustained activity in propene metathesis. Remarkably, its catalytic performances outpace those of the parent imido derivative, underlining the importance of the oxo ligand in the design of robust catalysts. © 2010 The Royal Society of Chemistry.

  1. Tanks Focus Area Alternative Salt Processing Research and Development Program Plan

    Energy Technology Data Exchange (ETDEWEB)

    Harmon, Harry D.


    In March 2000, DOE-Headquarters (HQ) requested the Tanks Focus Area (TFA) to assume management responsibility for the Salt Processing Project technology development program at Savannah River Site. The TFA was requested to conduct several activities, including review and revision of the technology development roadmaps, development of down-selection criteria, and preparation of a comprehensive Research and Development (R&D) Program Plan for three candidate cesium removal technologies, as well as the Alpha and strontium removal processes that must also be carried out. The three cesium removal candidate technologies are Crystalline Silicotitanate (CST) Non-Elutable Ion Exchange, Caustic Side Solvent Extraction (CSSX), and Small Tank Tetraphenylborate Precipitation (STTP). This plan describes the technology development needs for each process that must be satisfied in order to reach a down-selection decision, as well as continuing technology development required to support conceptual design activities.

  2. Tanks Focus Area Alternative Salt Processing Research and Development Program Plan

    Energy Technology Data Exchange (ETDEWEB)

    Harmon, Harry D.


    In March 2000, DOE-Headquarters (HQ) requested the Tanks Focus Area (TFA)to assume management responsibility for the Salt Processing Project technology development program at Savannah River Site. The TFA was requested to conduct several activities, including review and revision of the technology development roadmaps, development of down-selection criteria, and preparation of a comprehensive Research and Development (R&D) Program Plan for three candidate cesium removal technologies, as well as the Alpha and strontium removal processes that must also be carried out. The three cesium removal candidate technologies are Crystalline Silicotitanate (CST) Non-Elutable Ion Exchange, Caustic Side Solvent Extraction (CSSX), and Small Tank Tetraphenylborate Precipitation (STTP). This plan describes the technology development needs for each process that must be satisfied in order to reach a down-selection decision, as well as continuing technology development required to support conceptual design activities.

  3. Advanced technologies in biodiesel new advances in designed and optimized catalysts

    CERN Document Server

    Islam, Aminul


    The inadequacy of fossil fuel is the main driving force of the future sustainable energy around the world. Since heterogeneous catalysis is used in chemical industry for biodiesel production, achieving optimal catalytic performance is a significant issue for chemical engineers and chemists. Enormous attention has been placed in recent years on the selection of heterogeneous catalyst in biodiesel industry, where the catalyst could be facilitated highly selective toward desired products, easily handled, separated from the reaction medium, and subsequently reused. This book stresses an overview on the contributions of tailored solid acid and base catalysts to catalytic biodiesel synthesis, and the in uences of heterogeneous catalyst properties on biodiesel yield in order to develop a better understanding of catalyst design for the green production process as well as practical applications in the biodiesel industry.

  4. Preparation Of KF-Modified Kaolinite As Green And Reusable Catalyst For Microwave Assisted Biodiesel Conversion (United States)

    Fatimah, I.; Andiena, R. Z.; Yudha, S. P.


    Preparation of KF-modified kaolinite catalyst for microwave-assisted biodiesel conversion has been investigated. Kaolinite modification was conducted by solid-solid reaction between naturally occurring kaolinite mineral and KF salt followed by heating at 200oC for 2h. Prepared catalyst was characterized by using XRD, BET surface area analyzer, and SEM-EDX analysis and for catalytic activity tests, biodiesel conversion of jatropha oil was simulated. The comparison between microwave utilization and conventional method of biodiesel conversion were studied, moreover study on the catalyst reusability was performed. The results show that prepared catalyst gives the better physicochemical character of kaolinite as heterogeneous catalysts application as shown by the higher conversion and also reusability. Furthermore, the use of microwave irradiation exhibits the more time effectiveness. In general, the greener biodiesel conversion using presented methods is promising technique to be developed.

  5. Potassium hydroxide catalyst supported on palm shell activated carbon for transesterification of palm oil

    Energy Technology Data Exchange (ETDEWEB)

    Baroutian, Saeid; Aroua, Mohamed Kheireddine; Raman, Abdul Aziz Abdul; Sulaiman, Nik Meriam Nik [Department of Chemical Engineering, Faculty of Engineering, University of Malaya, 50603 Kuala Lumpur (Malaysia)


    In this study, potassium hydroxide catalyst supported on palm shell activated carbon was developed for transesterification of palm oil. The Central Composite Design (CCD) of the Response Surface Methodology (RSM) was employed to investigate the effects of reaction temperature, catalyst loading and methanol to oil molar ratio on the production of biodiesel using activated carbon supported catalyst. The highest yield was obtained at 64.1 C reaction temperature, 30.3 wt.% catalyst loading and 24:1 methanol to oil molar ratio. The physical and chemical properties of the produced biodiesel met the standard specifications. This study proves that activated carbon supported potassium hydroxide is an effective catalyst for transesterification of palm oil. (author)

  6. Metal catalysts for steam reforming of tar derived from the gasification of lignocellulosic biomass. (United States)

    Li, Dalin; Tamura, Masazumi; Nakagawa, Yoshinao; Tomishige, Keiichi


    Biomass gasification is one of the most important technologies for the conversion of biomass to electricity, fuels, and chemicals. The main obstacle preventing the commercial application of this technology is the presence of tar in the product gas. Catalytic reforming of tar appears a promising approach to remove tar and supported metal catalysts are among the most effective catalysts. Nevertheless, improvement of catalytic performances including activity, stability, resistance to coke deposition and aggregation of metal particles, as well as catalyst regenerability is greatly needed. This review focuses on the design and catalysis of supported metal catalysts for the removal of tar in the gasification of biomass. The recent development of metal catalysts including Rh, Ni, Co, and their alloys for steam reforming of biomass tar and tar model compounds is introduced. The role of metal species, support materials, promoters, and their interfaces is described. Copyright © 2014 Elsevier Ltd. All rights reserved.

  7. Model of Infiltration of Spent Automotive Catalysts by Molten Metal in Process of Platinum Metals Recovery

    Directory of Open Access Journals (Sweden)

    Agnieszka Fornalczyk


    Full Text Available This paper presents the model for the washing-out process of precious metals from spent catalysts by the use of molten lead in which the metal flow is caused by the rotating electromagnetic field and the Lorentz force. The model includes the coupling of the electromagnetic field with the hydrodynamic field, the flow of metal through anisotropic and porous structure of the catalyst, and the movement of the phase boundary (air-metal during infiltration of the catalyst carrier by the molten metal. The developed model enabled analysis of the impact of spacing between the catalysts and the supply current on the degree of catalyst infiltration by the molten metal. The results of calculations carried out on the basis of the model were verified experimentally.

  8. Supported fischer-tropsch catalyst and method of making the catalyst (United States)

    Dyer, Paul N.; Pierantozzi, Ronald; Withers, Howard P.


    A Fischer-Tropsch catalyst and a method of making the catalyst for a Fischer-Tropsch process utilizing the catalyst by which synthesis gas, particularly carbon-monoxide rich synthesis gas, is selectively converted to higher hydrocarbons of relatively narrow carbon number range is disclosed. In general, the selective and notably stable catalyst, consist of an inert carrier first treated with a Group IV B metal compound (such as zirconium or titanium), preferably an alkoxide compound, and subsequently treated with an organic compound of a Fischer-Tropsch metal catalyst, such as cobalt, iron or ruthenium carbonyl. Reactions with air and water and calcination are specifically avoided in the catalyst preparation procedure.

  9. Catalysts, Protection Layers, and Semiconductors

    DEFF Research Database (Denmark)

    Chorkendorff, Ib


    acid or alkaline conditions. Since most relevant semiconductors are very prone to corrosion the advantage of using buried junctions and using protection layers offering shall be discussed [2-4]. Next we shall discuss the availability of various catalysts for being coupled to these protections layers...... and how their stability may be evaluated [5, 6]. Examples of half-cell reaction using protection layers for both cathode and anode will be discussed though some of recent examples under both alkaline and acidic conditions. Si is a very good low band gap semiconductor and by using TiO2 as a protection...... layer we can stabilize it for both H2 and O2 evolution [7, 8, 9, 10]. Notably NiOx promoted by iron is a material that is transparent, providing protection, and is a good catalyst for O2 evolution. We have also recently started searching for large band gap semicondutors like III-V based or pervoskite...

  10. Zeolites as catalysts in oil refining. (United States)

    Primo, Ana; Garcia, Hermenegildo


    Oil is nowadays the main energy source and this prevalent position most probably will continue in the next decades. This situation is largely due to the degree of maturity that has been achieved in oil refining and petrochemistry as a consequence of the large effort in research and innovation. The remarkable efficiency of oil refining is largely based on the use of zeolites as catalysts. The use of zeolites as catalysts in refining and petrochemistry has been considered as one of the major accomplishments in the chemistry of the XXth century. In this tutorial review, the introductory part describes the main features of zeolites in connection with their use as solid acids. The main body of the review describes important refining processes in which zeolites are used including light naphtha isomerization, olefin alkylation, reforming, cracking and hydrocracking. The final section contains our view on future developments in the field such as the increase in the quality of the transportation fuels and the coprocessing of increasing percentage of biofuels together with oil streams. This review is intended to provide the rudiments of zeolite science applied to refining catalysis.

  11. Novel bimetallic dispersed catalysts for temperature-programmed coal liquefaction. Final report

    Energy Technology Data Exchange (ETDEWEB)

    Chunshan Song; Schobert, H.H.; Parfitt, D.P. [and others


    Development of new catalysts is a promising approach to more efficient coal liquefaction. It has been recognized that dispersed catalysts are superior to supported catalysts for primary liquefaction of coals, because the control of initial coal dissolution or depolymerization requires intimate contact between the catalyst and coal. This research is a fundamental and exploratory study on catalytic coal liquefaction, with the emphasis on exploring novel bimetallic dispersed catalysts for coal liquefaction and the effectiveness of temperature-programmed liquefaction using dispersed catalysts. The primary objective of this research was to explore novel bimetallic dispersed catalysts from organometallic molecular precursors, that could be used in low concentrations but exhibit relatively high activity for efficient hydroliquefaction of coals under temperature-programmed conditions. We have synthesized and tested various catalyst precursors in liquefaction of subbituminous and bituminous coals and in model compound studies to examine how do the composition and structure of the catalytic precursors affect their effectiveness for coal liquefaction under different reaction conditions, and how do these factors affect their catalytic functions for hydrogenation of polyaromatic hydrocarbons, for cleavage of C-C bonds in polycyclic systems such as 4-(1-naphthylmethyl)bibenzyl, for hydrogenolysis of C-O bond such as that in dinaphthylether, for hydrodeoxygenation of phenolic compounds and other oxygen-containing compounds such as xanthene, and for hydrodesulfurization of polycyclic sulfur compounds such as dibenzothiophene. The novel bimetallic and monometallic precursors synthesized and tested in this project include various Mo- and Fe-based compounds.

  12. Copper-containing zeolite catalysts (United States)

    Price, Geoffrey L.; Kanazirev, Vladislav


    A catalyst useful in the conversion of nitrogen oxides or in the synthesis of nitriles or imines from amines, formed by preparing an intimate mechanical mixture of a copper (II)-containing species, such as CuO or CuCl.sub.2, or elemental copper, with a zeolite having a pore mouth comprising 10 oxygen atoms, such as ZSM-5, converting the elemental copper or copper (II) to copper (I), and driving the copper (I) into the zeolite.

  13. Catalyst for Expanding Human Spaceflight (United States)

    Lueders, Kathryn L.


    History supplies us with many models of how and how not to commercialize an industry. This presentation draws parallels between industries with government roots, like the railroad, air transport, communications and the internet, and NASAs Commercial Crew Program. In these examples, government served as a catalyst for what became a booming industry. The building block approach the Commercial Crew Program is taking is very simple -- establish a need, laying the groundwork, enabling industry and legal framework.

  14. Attrition Resistant Iron-Based Catalysts For F-T SBCRs

    Energy Technology Data Exchange (ETDEWEB)

    Adeyinka A. Adeyiga


    The Fischer-Tropsch (F-T) reaction provides a way of converting coal-derived synthesis gas (CO+ H{sub 2}) to liquid fuels. Since the reaction is highly exothermic, one of the major problems in control of the reaction is heat removal. Recent work has shown that the use of slurry bubble column reactors (SBCRs) can largely solve this problem. The use of iron-(FE) based catalysts is attractive not only due to their low cost and ready availability, but also due to their high water-gas shift activity which makes it possible to use these catalysts with low H{sub 2}/CO ratios. However, a serious problem with the use of Fe catalysts in a SBCR is their tendency to undergo attrition. This can cause fouling/plugging of downstream filters and equipment; makes the separation of catalyst from the oil/wax product very difficult, if not impossible; and results in a steady loss of catalyst from the reactor. Under a previous Department of Energy (DOE)/University Research Grant (UCR) grant, Hampton University reported, for the first time, the development of demonstrably attrition-resistant Fe F-T synthesis catalysts having good activity, selectivity, and attrition resistance. These catalysts were prepared by spray drying Fe catalysts with potassium (K), copper (Cu), and silica (SiO{sub 2}) as promoters. SiO{sub 2} was also used as a binder for spray drying. These catalysts were tested for activity and selectivity in a laboratory-scale fixed-bed reactor. Fundamental understanding of attrition is being addressed by incorporating suitable binders into the catalyst recipe. This has resulted in the preparation of a spray dried HPR-43 catalyst having average particle size (aps) of 70 {micro}m with high attrition resistance. This HPR-43 attrition resistant, active and selective catalyst gave 95% CO conversion through 125 hours of testing in a fixed-bed at 270 C, 1.48 MPa, H{sub 2}/CO=0.67 and 2.0 NL/g-cat/h with C{sub 5+} selectivity of >78% and methane selectivity of less than 5% at an

  15. Enhancement in electro-oxidation of methanol over PtRu black catalyst through strong interaction with iron oxide nanocluster. (United States)

    Jeon, Min Ku; Lee, Ki Rak; Woo, Seong Ihl


    One of the major issues in direct methanol fuel cell research is to develop a new catalyst for methanol electro-oxidation reaction (MOR) with high activity and low cost. In this study, a new, simple, and economic way was introduced to improve the catalytic activity of commercial PtRu black catalyst for the MOR. A nanocomposite electrode was fabricated by mixing the PtRu catalyst with Fe(2)O(3) nanoclusters. When 10 wt % of the PtRu catalyst was replaced by the Fe(2)O(3) nanoclusters, mass activity (A/g(Pt)) increased by 80% compared to that of the pure PtRu catalyst. Specific activity of the mixed catalyst was 100% higher than that of the pure PtRu catalyst. The nanocomposite catalysts were also applied to single cells. Although the amount of the PtRu catalyst was reduced by 10 wt %, 10% higher potential was observed in the nanocomposite catalysts at a current density of 100 mA/cm(2).

  16. Nitrogen-doped Carbon Derived from ZIF-8 as a High-performance Metal-free Catalyst for Acetylene Hydrochlorination


    Songlin Chao; Fang Zou; Fanfan Wan; Xiaobin Dong; Yanlin Wang; Yuxuan Wang; Qingxin Guan; Guichang Wang; Wei Li


    Acetylene hydrochlorination is a major industrial technology for manufacturing vinyl chloride monomer in regions with abundant coal resources; however, it is plagued by the use of mercury(II) chloride catalyst. The development of a nonmercury catalyst has been extensively explored. Herein, we report a N-doped carbon catalyst derived from ZIF-8 with both high activity and quite good stability. The acetylene conversion reached 92% and decreased slightly during a 200?h test at 220??C and atmosph...

  17. Platinum Group Metal-free Catalysts for Hydrogen Evolution Reaction in Microbial Electrolysis Cells. (United States)

    Yuan, Heyang; He, Zhen


    Hydrogen gas is a green energy carrier with great environmental benefits. Microbial electrolysis cells (MECs) can convert low-grade organic matter to hydrogen gas with low energy consumption and have gained a growing interest in the past decade. Cathode catalysts for the hydrogen evolution reaction (HER) present a major challenge for the development and future applications of MECs. An ideal cathode catalyst should be catalytically active, simple to synthesize, durable in a complex environment, and cost-effective. A variety of noble-metal free catalysts have been developed and investigated for HER in MECs, including Nickel and its alloys, MoS 2 , carbon-based catalysts and biocatalysts. MECs in turn can serve as a research platform to study the durability of the HER catalysts. This personal account has reviewed, analyzed, and discussed those catalysts with an emphasis on synthesis and modification, system performance and potential for practical applications. It is expected to provide insights into the development of HER catalysts towards MEC applications. © 2017 The Chemical Society of Japan & Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  18. Controlling the catalyst during carbon nanotube growth. (United States)

    Robertson, J; Hofmann, S; Cantoro, M; Parvez, A; Ducati, C; Zhong, G; Sharma, R; Mattevi, C


    We have recently been able to grow single-walled carbon nanotubes by purely thermal chemical vapour deposition (CVD) at temperatures as low as 400 degrees C. This has been achieved by separating the catalyst pre-treatment step from the growth step. In the pre-treatment step, a thin film catalyst is re-arranged into a series of nano-droplets, which are then the active catalysts. Both steps have been studied by in-situ environmental transmission electron microscopy and X-ray photoemission spectroscopy. We have also studied the catalyst yield, the weight of nanotubes grown per weight of transition metal catalyst. Using very thin layers of Fe on Al2O3 support in a remote plasma-assisted CVD, we have achieved yields of order 100,000. This may be due to control of catalyst poisoning by ensuring an etching path.

  19. Organoiridium Complexes: Anticancer Agents and Catalysts (United States)


    Conspectus Iridium is a relatively rare precious heavy metal, only slightly less dense than osmium. Researchers have long recognized the catalytic properties of square-planar IrI complexes, such as Crabtree’s hydrogenation catalyst, an organometallic complex with cyclooctadiene, phosphane, and pyridine ligands. More recently, chemists have developed half-sandwich pseudo-octahedral pentamethylcyclopentadienyl IrIII complexes containing diamine ligands that efficiently catalyze transfer hydrogenation reactions of ketones and aldehydes in water using H2 or formate as the hydrogen source. Although sometimes assumed to be chemically inert, the reactivity of low-spin 5d6 IrIII centers is highly dependent on the set of ligands. Cp* complexes with strong σ-donor C∧C-chelating ligands can even stabilize IrIV and catalyze the oxidation of water. In comparison with well developed Ir catalysts, Ir-based pharmaceuticals are still in their infancy. In this Account, we review recent developments in organoiridium complexes as both catalysts and anticancer agents. Initial studies of anticancer activity with organoiridium complexes focused on square-planar IrI complexes because of their structural and electronic similarity to PtII anticancer complexes such as cisplatin. Recently, researchers have studied half-sandwich IrIII anticancer complexes. These complexes with the formula [(Cpx)Ir(L∧L′)Z]0/n+ (with Cp* or extended Cp* and L∧L′ = chelated C∧N or N∧N ligands) have a much greater potency (nanomolar) toward a range of cancer cells (especially leukemia, colon cancer, breast cancer, prostate cancer, and melanoma) than cisplatin. Their mechanism of action may involve both an attack on DNA and a perturbation of the redox status of cells. Some of these complexes can form IrIII-hydride complexes using coenzyme NAD(P)H as a source of hydride to catalyze the generation of H2 or the reduction of quinones to semiquinones. Intriguingly, relatively unreactive organoiridium

  20. Preparation of Supported Metal Catalysts by Atomic and Molecular Layer Deposition for Improved Catalytic Performance (United States)

    Gould, Troy D.

    Creating catalysts with enhanced selectivity and activity requires precise control over particle shape, composition, and size. Here we report the use of atomic layer deposition (ALD) to synthesize supported Ni, Pt, and Ni-Pt catalysts in the size regime (nanoparticles by depositing Ni on Al2O3 with two half-reactions of Ni(Cp)2 and H2. By changing the number of ALD cycles, Ni weight loadings were varied from 4.7 wt% to 16.7 wt% and the average particle sizes ranged from 2.5 to 3.3 nm, which increased the selectivity for C 3H6 hydrogenolysis by an order of magnitude over a much larger Ni/Al2O3 catalyst. Pt particles were deposited by varying the number of ALD cycles and the reaction chemistry (H2 or O 2) to control the particle size from approximately 1 to 2 nm, which allowed lower-coordinated surface atoms to populate the particle surface. These Pt ALD catalysts demonstrated some of the highest oxidative dehydrogenation of propane selectivities (37%) of a Pt catalyst synthesized by a scalable technique. Dry reforming of methane (DRM) is a reaction of interest due to the recent increased recovery of natural gas, but this reaction is hindered from industrial implementation because the Ni catalysts are plagued by deactivation from sintering and coking. This work utilized Ni ALD and NiPt ALD catalysts for the DRM reaction. These catalysts did not form destructive carbon whiskers and had enhanced reaction rates due to increased bimetallic interaction. To further limit sintering, the Ni and NiPt ALD catalysts were coated with a porous alumina matrix by molecular layer deposition (MLD). The catalysts were evaluated for DRM at 973 K, and the MLD-coated Ni catalysts outperformed the uncoated Ni catalysts in either activity (with 5 MLD cycles) or stability (with 10 MLD cycles). In summary, this thesis developed a new Ni nanoparticle ALD chemistry, explored possibilities for changing Pt ALD particle size, brought the two techniques together to create enhanced bimetallic

  1. Lanthanoid-free perovskite oxide catalyst for dehydrogenation of ethylbenzene working with redox mechanism (United States)

    Watanabe, Ryo; Ikushima, Maiko; Mukawa, Kei; Sumomozawa, Fumitaka; Ogo, Shuhei; Sekine, Yasushi


    For the development of highly active and robust catalysts for dehydrogenation of ethylbenzene (EBDH) to produce styrene; an important monomer for polystyrene production, perovskite-type oxides were applied to the reaction. Controlling the mobility of lattice oxygen by changing the structure of Ba1 − xSrxFeyMn1 − yO3 − δ (0 ≤ x ≤ 1, 0.2 ≤ y ≤ 0.8), perovskite catalyst showed higher activity and stability on EBDH. The optimized Ba/Sr and Fe/Mn molar ratios were 0.4/0.6 and 0.6/0.4, respectively. Comparison of the dehydrogenation activity of Ba0.4Sr0.6Fe0.6Mn0.4O3 − δ catalyst with that of an industrial potassium promoted iron (Fe–K) catalyst revealed that the Ba0.4Sr0.6Fe0.6Mn0.4O3 − δ catalyst showed higher initial activity than the industrial Fe–K oxide catalyst. Additionally, the Ba0.4Sr0.6Fe0.6Mn0.4O3 − δ catalyst showed high activity and stability under severe conditions, even at temperatures as low as 783 K, or at the low steam/EB ratio of 2, while, the Fe–K catalyst showed low activity in such conditions. Comparing reduction profiles of the Ba0.4Sr0.6Fe0.6Mn0.4O3 − δ and the Fe–K catalysts in a H2O/H2 atmosphere, reduction was suppressed by the presence of H2O over the Ba0.4Sr0.6Fe0.6Mn0.4O3 − δ catalyst while the Fe–K catalyst was reduced. In other words, Ba0.4Sr0.6Fe0.6Mn0.4O3 − δ catalyst had higher potential for activating the steam than the Fe–K catalyst. The lattice oxygen in perovskite-structure was consumed by H2, subsequently the consumed lattice oxygen was regenerated by H2O. So the catalytic performance of Ba0.4Sr0.6Fe0.6Mn0.4O3 − δ was superior to that of Fe–K catalyst thanks to the high redox property of the Ba0.4Sr0.6Fe0.6Mn0.4O3 − δ perovskite oxide. PMID:24790949

  2. Oxidation catalysts on alkaline earth supports (United States)

    Mohajeri, Nahid


    An oxidation catalyst includes a support including particles of an alkaline earth salt, and first particles including a palladium compound on the support. The oxidation catalyst can also include precious metal group (PMG) metal particles in addition to the first particles intermixed together on the support. A gas permeable polymer that provides a continuous phase can completely encapsulate the particles and the support. The oxidation catalyst may be used as a gas sensor, where the first particles are chemochromic particles.

  3. Thermally Stable, Latent Olefin Metathesis Catalysts


    Thomas, Renee M.; Fedorov, Alexey; Keitz, Benjamin K.; Grubbs, Robert H.


    Highly thermally stable N-aryl,N-alkyl N-heterocyclic carbene (NHC) ruthenium catalysts were designed and synthesized for latent olefin metathesis. These catalysts showed excellent latent behavior toward metathesis reactions, whereby the complexes were inactive at ambient temperature and initiated at elevated temperatures, a challenging property to achieve with second generation catalysts. A sterically hindered N-tert-butyl substituent on the NHC ligand of the ruthenium complex was found to i...

  4. Helical Oligourea Foldamers as Powerful Hydrogen Bonding Catalysts for Enantioselective C-C Bond-Forming Reactions. (United States)

    Bécart, Diane; Diemer, Vincent; Salaün, Arnaud; Oiarbide, Mikel; Nelli, Yella Reddy; Kauffmann, Brice; Fischer, Lucile; Palomo, Claudio; Guichard, Gilles


    Substantial progress has been made toward the development of metal-free catalysts of enantioselective transformations, yet the discovery of organic catalysts effective at low catalyst loadings remains a major challenge. Here we report a novel synergistic catalyst combination system consisting of a peptide-inspired chiral helical (thio)urea oligomer and a simple tertiary amine that is able to promote the Michael reaction between enolizable carbonyl compounds and nitroolefins with excellent enantioselectivities at exceptionally low (1/10 000) chiral catalyst/substrate molar ratios. In addition to high selectivity, which correlates strongly with helix folding, the system we report here is also highly amenable to optimization, as each of its components can be fine-tuned separately to increase reaction rates and/or selectivities. The predictability of the foldamer secondary structure coupled to the high level of control over the primary sequence results in a system with significant potential for future catalyst design.

  5. Catalyst technology roadmap report

    Energy Technology Data Exchange (ETDEWEB)

    Jackson, N.B.


    This report outlines the future technology needs of the Chemical Industry in the area of catalysis and is a continuation of the process that produced the report Technology Vision 2020: The U.S. Chemical Industry and the Council for Chemical Research`s (CCR) Chemical Synthesis Team follow-up work in chemical synthesis. Vision 2020 developed a 25-year vision for the chemical industry and outlined the challenges to be addressed in order to achieve this vision. This report, which outlines the catalysis technology roadmap, is based on the output of the CCR`s Chemical Synthesis Team, plus a workshop held March -20-21, 1997, which included about 50 participants, with catalysis experts from industry, academia, and government. It is clear that all participants view catalysis as a fundamental driver to the 0274 economic and environmental viability of the chemical industry. Advances in catalytic science and technology are among the most crucial challenges to achieving the goals of the chemical industry advanced in Vision 2020.

  6. Nitrogen oxides storage catalysts containing cobalt (United States)

    Lauterbach, Jochen; Snively, Christopher M.; Vijay, Rohit; Hendershot, Reed; Feist, Ben


    Nitrogen oxides (NO.sub.x) storage catalysts comprising cobalt and barium with a lean NO.sub.x storage ratio of 1.3 or greater. The NO.sub.x storage catalysts can be used to reduce NO.sub.x emissions from diesel or gas combustion engines by contacting the catalysts with the exhaust gas from the engines. The NO.sub.x storage catalysts can be one of the active components of a catalytic converter, which is used to treat exhaust gas from such engines.

  7. Biomimetic catalysts responsive to specific chemical signals

    Energy Technology Data Exchange (ETDEWEB)

    Zhao, Yan [Iowa State Univ., Ames, IA (United States)


    amphiphilic principles used in the foldamer catalysts were extended to a few other systems, particularly to interfacially cross-linked reverse micelles and micelles. These features enabled unusual catalytic features such as basic/nucleophilic catalysis under acidic conditions. We were able to create highly active metal nanoclusters catalysts whose local environment could be tuned by the organic framework. We were even able to create a “catalytic nanomachine” that grabs the substrate to the encapsulated Au clusters, which efficiently convert the substrate to the product that is rapidly ejected due to its different binding properties. Our research has important impacts on fundamental and applied energy-related sciences. On the fundamental level, it tests important biocatalytic principles on relatively simple synthetic systems and is expected to afford deeper understanding of biological catalysis. On the practical level, the research is anticipated to lead to “smart” catalysts and open up exiting applications in chemical analysis, reaction control, and materials synthesis. Part 2. Electrochemical Reduction of CO₂ The primary objective of our research involving the electrochemical reduction of carbon dioxide is to apply a multidisciplinary approach toward developing a greater understanding of the problem of efficiently converting CO₂ to hydrocarbons through electrochemical routes. Our goal is to provide a better understanding of the principles that underlie the electrocatalytic reduction of CO₂ at electrode surfaces and the molecular pathways that lead to desired compounds. This understanding is essential for the design and development of new catalytic materials for the selective production of renewable feedstocks. The electrochemical reduction of CO₂ involves the formation of various reaction products and adsorbed intermediates whose distribution depends upon the nature of the electrode material and the electrochemical conditions, including applied potential

  8. Imaging Catalysts at Work: A Hierarchical Approach from the Macro- to the Meso- and Nano-scale

    DEFF Research Database (Denmark)

    Grunwaldt, Jan-Dierk; Wagner, Jakob Birkedal; Dunin-Borkowski, Rafal E.


    /heat/mass transport gradients in shaped catalysts and catalyst grains and c)meso- and nano-scale information about particles and clusters, whose physical and electronic properties are linked directly to the micro-kinetic behaviour of the catalysts. Techniques such as X-ray diffraction (XRD), infrared (IR), Raman, X......This review highlights the importance of developing multi-scale characterisation techniques for analysing operating catalysts in their working environment. We emphasise that a hierarchy of insitu techniques that provides macro-, meso- and nano-scale information is required to elucidate and optimise...

  9. Impacto dos catalisadores automotivos no controle da qualidade do ar Impact of automotive catalysts in the control of air quality

    Directory of Open Access Journals (Sweden)

    Maria do Carmo Rangel


    Full Text Available Advanced industrialized nations have experienced severe pollution problems over the past forty years, caused mainly by carbon monoxide, hydrocarbons and nitrogen oxide emissions from automobiles. Catalyst technology has played a major part in minimizing these emissions as required by even more restrictive laws. The catalyst has been optimized over the years to meet the requirements of high activity and long life. The oxidation of hydrocarbon and carbon monoxide are in advanced development stage while that of NOx catalysts is far less advanced. In the future, catalyst technology is expected to contribute to overcome the challenges to get a cleaner air.

  10. Pilot Testing of Mercury Oxidation Catalysts for Upstream of Wet FGD Systems

    Energy Technology Data Exchange (ETDEWEB)

    Richard Rhudy


    This final report presents and discusses results from a mercury control process development project entitled ''Pilot Testing of Mercury Oxidation Catalysts for Upstream of Wet FGD Systems''. The objective of this project was to demonstrate at pilot scale a mercury control technology that uses solid honeycomb catalysts to promote the oxidation of elemental mercury in the flue gas from coal combustion. Oxidized mercury is removed in downstream wet flue gas desulfurization (FGD) absorbers and leaves with the FGD byproducts. The goal of the project was to achieve 90% oxidation of elemental mercury in the flue gas and 90% overall mercury capture with the downstream wet FGD system. The project was co-funded by EPRI and the U.S. Department of Energy's National Energy Technology Laboratory (DOE NETL) under Cooperative Agreement DE-FC26-01NT41185. Great River Energy (GRE) and City Public Service (now CPS Energy) of San Antonio were also project co-funders and provided host sites. URS Group, Inc. was the prime contractor. Longer-term pilot-scale tests were conducted at two sites to provide catalyst life data. GRE provided the first site, at their Coal Creek Station (CCS), which fires North Dakota lignite, and CPS Energy provided the second site, at their Spruce Plant, which fires Powder River Basin (PRB) coal. Mercury oxidation catalyst testing began at CCS in October 2002 and continued through the end of June 2004, representing nearly 21 months of catalyst operation. An important finding was that, even though the mercury oxidation catalyst pilot unit was installed downstream of a high-efficiency ESP, fly ash buildup began to plug flue gas flow through the horizontal catalyst cells. Sonic horns were installed in each catalyst compartment and appeared to limit fly ash buildup. A palladium-based catalyst showed initial elemental mercury oxidation percentages of 95% across the catalyst, declining to 67% after 21 months in service. A carbon

  11. Monolitni katalizatori i reaktori: osnovne značajke, priprava i primjena (Monolith catalysts and reactors: preparation and applications

    Directory of Open Access Journals (Sweden)

    Tomašić, V.


    Full Text Available Monolithic (honeycomb catalysts are continuous unitary structures containing many narrow, parallel and usually straight channels (or passages. Catalytically active components are dispersed uniformly over the whole porous ceramic monolith structure (so-called incorporated monolithic catalysts or are in a layer of porous material that is deposited on the walls of channels in the monolith's structure (washcoated monolithic catalysts. The material of the main monolithic construction is not limited to ceramics but includes metals, as well. Monolithic catalysts are commonly used in gas phase catalytic processes, such as treatment of automotive exhaust gases, selective catalytic reduction of nitrogen oxides, catalytic removal of volatile organic compounds from industrial processes, etc. Monoliths continue to be the preferred support for environmental applications due to their high geometric surface area, different design options, low pressure drop, high temperature durability, mechanical strength, ease of orientation in a reactor and effectiveness as a support for a catalytic washcoat. As known, monolithic catalysts belong to the class of the structured catalysts and/or reactors (in some cases the distinction between "catalyst" and "reactor" has vanished. Structured catalysts can greatly intensify chemical processes, resulting in smaller, safer, cleaner and more energy efficient technologies. Monolith reactors can be considered as multifunctional reactors, in which chemical conversion is advantageously integrated with another unit operation, such as separation, heat exchange, a secondary reaction, etc. Finally, structured catalysts and/or reactors appear to be one of the most significant and promising developments in the field of heterogeneous catalysis and chemical engineering of the recent years. This paper gives a description of the background and perspectives for application and development of monolithic materials. Different methods and techniques

  12. Co-Production of Electricity and Hydrogen Using a Novel Iron-based Catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Hilaly, Ahmad; Georgas, Adam; Leboreiro, Jose; Arora, Salil; Head, Megann; Trembly, Jason; Turk, Brian; Gupta, Raghubir


    The primary objective of this project was to develop a hydrogen production technology for gasification applications based on a circulating fluid-bed reactor and an attrition resistant iron catalyst. The work towards achieving this objective consisted of three key activities: Development of an iron-based catalyst suitable for a circulating fluid-bed reactor; Design, construction, and operation of a bench-scale circulating fluid-bed reactor system for hydrogen production; Techno-economic analysis of the steam-iron and the pressure swing adsorption hydrogen production processes. This report describes the work completed in each of these activities during this project. The catalyst development and testing program prepared and iron-based catalysts using different support and promoters to identify catalysts that had sufficient activity for cyclic reduction with syngas and steam oxidation and attrition resistance to enable use in a circulating fluid-bed reactor system. The best performing catalyst from this catalyst development program was produced by a commercial catalyst toll manufacturer to support the bench-scale testing activities. The reactor testing systems used during material development evaluated catalysts in a single fluid-bed reactor by cycling between reduction with syngas and oxidation with steam. The prototype SIP reactor system (PSRS) consisted of two circulating fluid-bed reactors with the iron catalyst being transferred between the two reactors. This design enabled demonstration of the technical feasibility of the combination of the circulating fluid-bed reactor system and the iron-based catalyst for commercial hydrogen production. The specific activities associated with this bench-scale circulating fluid-bed reactor systems that were completed in this project included design, construction, commissioning, and operation. The experimental portion of this project focused on technical demonstration of the performance of an iron-based catalyst and a

  13. Alternative deNO{sub x} catalysts and technologies

    Energy Technology Data Exchange (ETDEWEB)

    Due-Hansen, J.


    Two approaches are undertaken in the present work to reduce the emission of NO{sub x}: by means of catalytic removal, and by NO absorption in ionic liquids. The commercial catalyst used for the selective catalytic reduction (SCR) of nitrogen oxides exhibits high activity and selectivity towards N{sub 2}. However, the vanadia-titania-based catalyst used is very sensitive to deactivation by alkali-species (primarily potassium), which are typically present in high amounts in the flue gas when biomass is combusted. By co-firing with large amounts of CO{sub 2}-neutral straw or wood (to meet stringent CO{sub 2} emission legislation), the lifetime of the traditional SCR catalyst is thus significantly reduced due to the presence of deactivating species originating from the fuel. To develop a catalyst less susceptible to the poisons present in the flue gas, a number of catalysts have been synthesized and tested in the present work, all based on commercially available supports. A highly acidic support consisting of sulfated zirconia was chosen based on preliminary studies. A number of different active species distributed on the support were investigated, such as iron, copper and vanadium oxides. However, based on the catalysts performance in the SCR reaction and their resistances towards potassium, the most promising candidate of the formulations studied was the vanadia-loaded catalyst, i.e. V{sub 2}O{sub 5}-SO{sub 4}2-ZrO{sub 2}. This work, together with an introduction to the catalytic removal of NO{sub x}, are described in chapter 3. The remainder of the first part is concerned with the catalytic NO{sub x} removal (chapter 4) and it addresses the upscaling of the best catalyst candidate. The catalyst was mixed with the natural binding clay (sepiolite) to upscale the selected catalyst to the monolithic level, suitable for installation in gas stream with high flows, e.g. a flue gas duct of a power plant. A series of catalyst pellets with increasing levels of sepiolite were

  14. Machine-learning models for combinatorial catalyst discovery (United States)

    Landrum, Gregory A.; Penzotti, Julie E.; Putta, Santosh


    A variety of machine learning algorithms, including hierarchical clustering, decision trees, k-nearest neighbours, support vector machines and bagging, were applied to construct models to predict the molecular weight of the polymers produced by a set of 96 homogeneous catalysts. The goal of the study was to develop models that could be used to screen large virtual libraries of catalysts in order to suggest candidates for further synthesis and screening. The descriptors used to represent the catalysts did not require detailed information about the catalysts themselves; they could be calculated using only the topology of the ligands. Using an initial set of five descriptors, model accuracies of about 70% were observed from each learning algorithm. A larger descriptor set (with ten descriptors) allowed bag classifiers that were 80% accurate to be built. All models were carefully evaluated to detect overfitting (memorization of the training data) and one example of the effects of overfitting is provided. Because the descriptors used in this study can be calculated very rapidly and the models themselves are very efficient, these bag classifiers are well suited to screening very large virtual libraries.

  15. Ceria-based solid catalysts for organic chemistry. (United States)

    Vivier, Laurence; Duprez, Daniel


    Ceria has been the subject of thorough investigations, mainly because of its use as an active component of catalytic converters for the treatment of exhaust gases. However, ceria-based catalysts have also been developed for different applications in organic chemistry. The redox and acid-base properties of ceria, either alone or in the presence of transition metals, are important parameters that allow to activate complex organic molecules and to selectively orient their transformation. Pure ceria is used in several organic reactions, such as the dehydration of alcohols, the alkylation of aromatic compounds, ketone formation, and aldolization, and in redox reactions. Ceria-supported metal catalysts allow the hydrogenation of many unsaturated compounds. They can also be used for coupling or ring-opening reactions. Cerium atoms can be added as dopants to catalytic system or impregnated onto zeolites and mesoporous catalyst materials to improve their performances. This Review demonstrates that the exceptional surface (and sometimes bulk) properties of ceria make cerium-based catalysts very effective for a broad range of organic reactions.

  16. High-throughput technology for novel SO2 oxidation catalysts

    Directory of Open Access Journals (Sweden)

    Jonas Loskyll, Klaus Stoewe and Wilhelm F Maier


    Full Text Available We review the state of the art and explain the need for better SO2 oxidation catalysts for the production of sulfuric acid. A high-throughput technology has been developed for the study of potential catalysts in the oxidation of SO2 to SO3. High-throughput methods are reviewed and the problems encountered with their adaptation to the corrosive conditions of SO2 oxidation are described. We show that while emissivity-corrected infrared thermography (ecIRT can be used for primary screening, it is prone to errors because of the large variations in the emissivity of the catalyst surface. UV-visible (UV-Vis spectrometry was selected instead as a reliable analysis method of monitoring the SO2 conversion. Installing plain sugar absorbents at reactor outlets proved valuable for the detection and quantitative removal of SO3 from the product gas before the UV-Vis analysis. We also overview some elements used for prescreening and those remaining after the screening of the first catalyst generations.

  17. Hierarchical hybrid peroxidase catalysts for remediation of phenol wastewater

    KAUST Repository

    Duan, Xiaonan


    We report a new family of hierarchical hybrid catalysts comprised of horseradish peroxidase (HRP)-magnetic nanoparticles for advanced oxidation processes and demonstrate their utility in the removal of phenol from water. The immobilized HRP catalyzes the oxidation of phenols in the presence of H2O2, producing free radicals. The phenoxy radicals react with each other in a non-enzymatic process to form polymers, which can be removed by precipitation with salts or condensation. The hybrid peroxidase catalysts exhibit three times higher activity than free HRP and are able to remove three times more phenol from water compared to free HRP under similar conditions. In addition, the hybrid catalysts reduce substrate inhibition and limit inactivation from reaction products, which are common problems with free or conventionally immobilized enzymes. Reusability is improved when the HRP-magnetic nanoparticle hybrids are supported on micron-scale magnetic particles, and can be retained with a specially designed magnetically driven reactor. The performance of the hybrid catalysts makes them attractive for several industrial and environmental applications and their development might pave the way for practical applications by eliminating most of the limitations that have prevented the use of free or conventionally immobilized enzymes. © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  18. Monodisperse Platinum and Rhodium Nanoparticles as Model Heterogeneous Catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Grass, Michael Edward [Univ. of California, Berkeley, CA (United States)


    Model heterogeneous catalysts have been synthesized and studied to better understand how the surface structure of noble metal nanoparticles affects catalytic performance. In this project, monodisperse rhodium and platinum nanoparticles of controlled size and shape have been synthesized by solution phase polyol reduction, stabilized by polyvinylpyrrolidone (PVP). Model catalysts have been developed using these nanoparticles by two methods: synthesis of mesoporous silica (SBA-15) in the presence of nanoparticles (nanoparticle encapsulation, NE) to form a composite of metal nanoparticles supported on SBA-15 and by deposition of the particles onto a silicon wafer using Langmuir-Blodgett (LB) monolayer deposition. The particle shapes were analyzed by transmission electron microscopy (TEM) and high resolution TEM (HRTEM) and the sizes were determined by TEM, X-ray diffraction (XRD), and in the case of NE samples, room temperature H2 and CO adsorption isotherms. Catalytic studies were carried out in homebuilt gas-phase reactors. For the nanoparticles supported on SBA-15, the catalysts are in powder form and were studied using the homebuilt systems as plug-flow reactors. In the case of nanoparticles deposited on silicon wafers, the same systems were operated as batch reactors. This dissertation has focused on the synthesis, characterization, and reaction studies of model noble metal heterogeneous catalysts. Careful control of particle size and shape has been accomplished though solution phase synthesis of Pt and Rh nanoparticles in order to elucidate further structure-reactivity relationships in noble metal catalysis.


    Directory of Open Access Journals (Sweden)

    Danute Vaiciukyniene


    Full Text Available Zeolites are commonly used in the fluid catalytic cracking process. Zeolite polluted with oil products and became waste after some time used. The quantity of this waste inevitably rises by expanding rapidly oil industry. The composition of these catalysts depends on the manufacturer and on the process that is going to be used. The main factors retarding hydration process of cement systems and modifying them strength are organic compounds impurities in the waste FCC catalyst. The present paper shows the results of using purified waste FCC catalyst (pFCC from Lithuania oil refinery, as Portland cement replacement material. For this purpose, the purification of waste FCC catalyst (FCC samples was treated with hydrogen peroxide. Hydrogen peroxide (H2O2 is one of the most powerful oxidizers known. By acting of waste with H2O2 it can eliminate the aforementioned waste deficiency, and the obtained product becomes one of the most promising ingredients, in new advanced building materials. Hardened cement paste samples with FCC or pFCC were formed. It was observed that the pFCC blended cements developed higher strength, after 28 days, compared to the samples with FCC or reference samples. Typical content of Portland cement substituting does not exceed 30 % of mass of Portland cement in samples. Reducing the consumption of Portland cement with utilizing waste materials is preferred for reasons of environmental protection.

  20. Attrition resistant fluidizable reforming catalyst (United States)

    Parent, Yves O [Golden, CO; Magrini, Kim [Golden, CO; Landin, Steven M [Conifer, CO; Ritland, Marcus A [Palm Beach Shores, FL


    A method of preparing a steam reforming catalyst characterized by improved resistance to attrition loss when used for cracking, reforming, water gas shift and gasification reactions on feedstock in a fluidized bed reactor, comprising: fabricating the ceramic support particle, coating a ceramic support by adding an aqueous solution of a precursor salt of a metal selected from the group consisting of Ni, Pt, Pd, Ru, Rh, Cr, Co, Mn, Mg, K, La and Fe and mixtures thereof to the ceramic support and calcining the coated ceramic in air to convert the metal salts to metal oxides.

  1. New Trends in Gold Catalysts

    Directory of Open Access Journals (Sweden)

    Leonarda F. Liotta


    Full Text Available Gold is an element that has fascinated mankind for millennia. The catalytic properties of gold have been a source of debate, due to its complete chemical inertness when in a bulk form, while it can oxidize CO at temperatures as low as ~200 K when in a nanocrystalline state, as discovered by Haruta in the late 1980s [1]. Since then, extensive activity in both applied and fundamental research on gold has been initiated. The importance of the catalysis by gold represents one of the fasted growing fields in science and is proven by the promising applications in several fields, such as green chemistry and environmental catalysis, in the synthesis of single-walled carbon nanotubes, as modifiers of Ni catalysts for methane steam and dry reforming reactions and in biological and electrochemistry applications. The range of reactions catalyzed by gold, as well as the suitability of different supports and the influence of the preparation conditions have been widely explored and optimized in applied research [2]. Gold catalysts appeared to be very different from the other noble metal-based catalysts, due to their marked dependence on the preparation method, which is crucial for the genesis of the catalytic activity. Several methods, including deposition-precipitation, chemical vapor deposition and cation adsorption, have been applied for the preparation of gold catalysts over reducible oxides, like TiO2. Among these methods, deposition-precipitation has been the most frequently employed method for Au loading, and it involves the use of tetrachloroauric (III acid as a precursor. On the other hand, the number of articles dealing with Au-loaded acidic supports is smaller than that on basic supports, possibly because the deposition of [AuCl4]− or [AuOHxCl4−x]− species on acidic supports is difficult, due to their very low point of zero charge. Despite this challenge, several groups have reported the use of acidic zeolites as supports for gold. Zeolites

  2. Hydrogen generation from decomposition of hydrous hydrazine over Ni-Ir/CeO2 catalyst


    Dai, Hongbin; Zhong, Yujie; Wang, Ping


    The synthesis of highly active and selective catalysts is the central issue in the development of hydrous hydrazine (N2H4·H2O) as a viable hydrogen carrier. Herein, we report the synthesis of bimetallic Ni-Ir nanocatalyts supported on CeO2 using a one-pot coprecipitation method. A combination of XRD, HRTEM and XPS analyses indicate that the Ni-Ir/CeO2 catalyst is composed of tiny Ni-Ir alloy nanoparticles with an average size of around 4 nm and crystalline CeO2 matrix. The Ni-Ir/CeO2 catalyst...

  3. Tunable synthetic approaches for the optimization of nanostructured fuel cell catalysts: An overview

    Directory of Open Access Journals (Sweden)

    Bönnemann H.


    Full Text Available Highly active nanostructured pluri-metal catalysts for fuel cell applications can be obtained by designing synthetic protocol where the particle size, metal composition and morphology can be readily tailored. Tunable synthesis relates to combining the various synthetic methodologies available for generating nanostructured metal catalysts with desired catalytic properties. Herein, we discuss some of these synthetic methodologies which were developed to combine the advantages of each pathway in generating efficient fuel cell catalysts and to learn how the composition and morphology of the metals be fine tuned.

  4. Advanced FCC catalyst matrix technology for reduced coke and slurry yields

    Energy Technology Data Exchange (ETDEWEB)

    Maglio, A.; Keweshan, C.F.; Madon, R.J. (Engelhard Corp., Iselin, NJ (United States)); McLean, J.B. (Engelhard Corp., Houston, TX (United States))


    Engelhard's new Reduxion line of FCC catalysts have been developed to offer 10 to 20% lower coke versus current catalysts, while maintaining high bottoms upgrading selectivity. Aspects of Engelhard's PyroChem zeolite technology featured in the Precision Catalyst line have been combined with a controlled matrix acidity distribution which maintains sites selective for bottoms cracking while reducing the strong sites which lead to coke and gas formation. Results from pilot unit testing are presented and projections for commercial operations are provided.

  5. Sixtieth Anniversary of Ziegler-Natta Catalysts and Stereospecific Polymerization

    Directory of Open Access Journals (Sweden)

    Janović Z.


    Full Text Available This review article highlights the history of the discoveries of organometallic catalysts and stereospecific polymerization of α-olefins, dienes and a number of vinyl monomers by Karl Ziegler and Giulio Natta sixty years ago, their developments and recent progress. As one of the most important achievements in the field of catalysis, macromolecular science and polymer materials, their inventors were awarded the Nobel Prize in Chemistry in 1963 “for their discoveries in the field of chemistry and technology of high polymers”. These discoveries have stimulated an intensive, both basic and applied research all over the world, up to the present times, leading to great development of the polymer industry. The important biographical data and scientific advancements of K. Ziegler and G. Natta are presented as well. Karl Ziegler, a German scientist, Director of Max Planck Institute for Coal Research in Mülheim, besides many scientific achievements, in 1953 discovered a new process for the polymerization of ethylene into linear polyethylene under mild conditions by using titanium chloride and alkyl aluminium catalytic system that was superior to all existing polymerization. Giulio Natta, an Italian scientist, Director of the Department of Industrial Chemistry at Polytechnic, University of Milan, besides many achievements in petrochemical processes, in 1954 obtained for the first time isotactic polypropylene and Montecatini Co. started its production already in 1958. He conducted pioneering studies on the chain microstructure of synthetic organic polymers and postulated the mechanisms of stereospecific polymerizations. Since the discovery of the Zeigler-Natta catalyst, stereospecific polymerization and processes, significant developments have occurred. The breakthrough in polymerization processes such as fluid bed, liquid phase loop reactor and reactor granule technology led to significant development and growth of polyolefin production. In the 1980s

  6. Synthesis of copper chromite catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Kawamoto, A.M.; Claudio Rezende, L. [Space Aeronautical Institute/Aerospace Center, Chemistry Div., Sao Jose dos Campos, SP (Brazil); Claudio Pardini, L. [Space Aeronautical Institute/Aerospace Center, Materials Div., Sao Jose dos Campos, SP (Brazil)


    The present work has the objective to investigate the catalytic behaviour of copper chromite (CuCr{sub 2}O{sub 4}) in the burning rate of poly-butadiene hydroxyl terminated (HTPB) which is an ammonium perchlorate propellant for solid fueled rockets. Copper chromite catalysts were prepared by ceramic and coprecipitation methods and characterized by X-ray diffraction, scanning electron microscopy (SEM), elemental, differential calorimetric (DSC), thermogravimetric and granulometric analysis, mass spectroscopy and infrared spectroscopy (IR). Elemental and IR analysis have shown similarities among the samples for both synthetic methods. However, DSC, SEM and X-ray analysis of the samples synthesized by coprecipitation method presented different physical properties. For those samples, DSC could identify a tetragonal {yields} cubic phase transition, SEM showed particles with defined crystalline shapes and X-ray analysis contains the main assignments which identify the formation of CuCr{sub 2}O{sub 4}. HTPB propellants containing CuCr{sub 2}O{sub 4} samples were manufactured, then burning rate and mechanical properties have been measured. The results were compared with HTPB propellants containing iron (III) oxide as catalyst. The highest burning rate values were obtained with samples which present a more defined crystalline shape, i.e., the ones synthesized by the coprecipitation method. (authors)

  7. Olefin polymerization over supported chromium oxide catalysts

    NARCIS (Netherlands)

    Weckhuysen, B.M.; Schoonheydt, R.A.


    Cr/SiO2 or Phillips-type catalysts are nowadays responsible for a large fraction of all polyethylene (HDPE and LLDPE) worldwide produced. In this review, several key-properties of Cr/SiO2 catalysts will be discussed in relation to their polymerization characteristics. It will be shown how the

  8. Solid acid catalysts: Stain and shine (United States)

    Chen, Peng


    Catalyst particles for fluid catalytic cracking are vital for the oil-refinery industry, but their activity is hard to diagnose because of their inter- and intra-particle structural inhomogeneity. With fluorescence confocal microscopy and selective staining, one can now pinpoint the catalytic activity within single catalyst particles from an industrial reactor.

  9. Chemical engineering design of CO oxidation catalysts (United States)

    Herz, Richard K.


    How a chemical reaction engineer would approach the challenge of designing a CO oxidation catalyst for pulsed CO2 lasers is described. CO oxidation catalysts have a long history of application, of course, so it is instructive to first consider the special requirements of the laser application and then to compare them to the characteristics of existing processes which utilize CO oxidation catalysts. All CO2 laser applications require a CO oxidation catalyst with the following characteristics: (1) active at stoichiometric ratios of O2 and CO, (2) no inhibition by CO2 or other components of the laser environment, (3) releases no particulates during vibration or thermal cycling, and (4) long lifetime with a stable activity. In all applications, low consumption of power is desirable, a characteristic especially critical in aerospace applications and, thus, catalyst activity at low temperatures is highly desirable. High power lasers with high pulse repetition rates inherently require circulation of the gas mixture and this forced circulation is available for moving gas past the catalyst. Low repetition rate lasers, however, do not inherently require gas circulation, so a catalyst that did not require such circulation would be favorable from the standpoint of minimum power consumption. Lasers designed for atmospheric penetration of their infrared radiation utilize CO2 formed from rare isotopes of oxygen and this application has the additional constraint that normal abundance oxygen isotopes in the catalyst must not exchange with rare isotopes in the gas mixture.

  10. Membrane catalyst layer for fuel cells (United States)

    Wilson, Mahlon S.


    A gas reaction fuel cell incorporates a thin catalyst layer between a solid polymer electrolyte (SPE) membrane and a porous electrode backing. The catalyst layer is preferably less than about 10 .mu.m in thickness with a carbon supported platinum catalyst loading less than about 0.35 mgPt/cm.sup.2. The film is formed as an ink that is spread and cured on a film release blank. The cured film is then transferred to the SPE membrane and hot pressed into the surface to form a catalyst layer having a controlled thickness and catalyst distribution. Alternatively, the catalyst layer is formed by applying a Na.sup.+ form of a perfluorosulfonate ionomer directly to the membrane, drying the film at a high temperature, and then converting the film back to the protonated form of the ionomer. The layer has adequate gas permeability so that cell performance is not affected and has a density and particle distribution effective to optimize proton access to the catalyst and electronic continuity for electron flow from the half-cell reaction occurring at the catalyst.

  11. The strange case of the "oscillating" catalysts

    NARCIS (Netherlands)

    Busico, [No Value; Cipullo, R; Kretschmer, W; Talarico, G; Vacatello, M; Castelli, VV


    The field of stereoselective propene polymerization has been dramatically innovated by the discovery of homogeneous metallocene-based catalysts with well-defined and tunable molecular structure. Of all, "oscillating" metallocenes are probably the most ingenious and challenging example of catalyst

  12. Catalyst and method for production of methylamines (United States)

    Klier, Kamil; Herman, Richard G.; Vedage, Gamini A.


    This invention relates to an improved catalyst and method for the selective production of methylamines. More particularly, it is concerned with the preparation of stable highly active catalysts for producing methylamines by a catalytic reaction of ammonia or substituted amines and binary synthesis gas (CO+H.sub.2).

  13. Chemical engineering design of CO oxidation catalysts (United States)

    Herz, Richard K.


    How a chemical reaction engineer would approach the challenge of designing a CO oxidation catalyst for pulsed CO2 lasers is described. CO oxidation catalysts have a long history of application, of course, so it is instructive to first consider the special requirements of the laser application and then to compare them to the characteristics of existing processes which utilize CO oxidation catalysts. All CO2 laser applications require a CO oxidation catalyst with the following characteristics: (1) active at stoichiometric ratios of O2 and CO, (2) no inhibition by CO2 or other components of the laser environment, (3) releases no particulates during vibration or thermal cycling, and (4) long lifetime with a stable activity. In all applications, low consumption of power is desirable, a characteristic especially critical in aerospace applications and, thus, catalyst activity at low temperatures is highly desirable. High power lasers with high pulse repetition rates inherently require circulation of the gas mixture and this forced circulation is available for moving gas past the catalyst. Low repetition rate lasers, however, do not inherently require gas circulation, so a catalyst that did not require such circulation would be favorable from the standpoint of minimum power consumption. Lasers designed for atmospheric penetration of their infrared radiation utilize CO2 formed from rare isotopes of oxygen and this application has the additional constraint that normal abundance oxygen isotopes in the catalyst must not exchange with rare isotopes in the gas mixture.

  14. European workshop on spent catalysts. Book of abstracts

    Energy Technology Data Exchange (ETDEWEB)



    In 1999 and 2002 two well attended workshops on recycling, regeneration, reuse and disposal of spent catalysts took place in Frankfurt. This series has been continued in Berlin. The workshop was organized in collaboration with DGMK, the German Society for Petroleum and Coal Science and Technology. Contributions were in the following areas of catalyst deactivation: recycling of spent catalysts in chemical and petrochemical industry, recycling of precious metal catalysts and heterogenous base metal catalysts, legal aspects of transboundary movements, catalyst regeneration, quality control, slurry catalysts, commercial reactivation of hydrotreating catalysts. (uke)

  15. A heterogeneous catalyst, SiO2-ZnBr2: An efficient neat access for α ...

    Indian Academy of Sciences (India)

    high yield of the product. Recent synthetic specifics of our group on the new methodologies using Lewis acid catalysts26 have encouraged us to focus initially develop a new method, before going on to evaluation of medicinal chemistry, for achieving high yield of the α- aminophosphonates. In search for an effective catalyst.

  16. Nano-Engineered Catalysts for Direct Methanol Fuel Cells (United States)

    Myung, Nosang; Narayanan, Sekharipuram; Wiberg, Dean


    Nano-engineered catalysts, and a method of fabricating them, have been developed in a continuing effort to improve the performances of direct methanol fuel cells as candidate power sources to supplant primary and secondary batteries in a variety of portable electronic products. In order to realize the potential for high energy densities (as much as 1.5 W h/g) of direct methanol fuel cells, it will be necessary to optimize the chemical compositions and geometric configurations of catalyst layers and electrode structures. High performance can be achieved when catalyst particles and electrode structures have the necessary small feature sizes (typically of the order of nanometers), large surface areas, optimal metal compositions, high porosity, and hydrophobicity. The present method involves electrodeposition of one or more catalytic metal(s) or a catalytic-metal/polytetrafluoroethylene nanocomposite on an alumina nanotemplate. The alumina nanotemplate is then dissolved, leaving the desired metal or metal/polytetrafluoroethylene-composite catalyst layer. Unlike some prior methods of making fine metal catalysts, this method does not involve processing at elevated temperature; all processing can be done at room temperature. In addition, this method involves fewer steps and is more amenable to scaling up for mass production. Alumina nanotemplates are porous alumina membranes that have been fabricated, variously, by anodizing either pure aluminum or aluminum that has been deposited on silicon by electronbeam evaporation. The diameters of the pores (7 to 300 nm), areal densities of pores (as much as 7 x 10(exp 10)sq cm), and lengths of pores (up to about 100 nm) can be tailored by selection of fabrication conditions. In a given case, the catalytic metal, catalytic metal alloy, or catalytic metal/ polytetrafluoroethylene composite is electrodeposited in the pores of the alumina nanotemplate. The dimensions of the pores, together with the electrodeposition conditions

  17. Heteropoly acid encapsulated into zeolite imidazolate framework (ZIF-67) cage as an efficient heterogeneous catalyst for Friedel–Crafts acylation

    Energy Technology Data Exchange (ETDEWEB)

    Ammar, Muhammad; Jiang, Sai; Ji, Shengfu, E-mail:


    A new strategy has been developed for the encapsulation of the phosphotungstic heteropoly acid (H{sub 3}PW{sub 12}O{sub 40} denoted as PTA) into zeolite imidazolate framework (ZIF-67) cage and the PTA@ZIF-67(ec) catalysts with different PTA content were prepared. The structure of the catalysts was characterized by XRD, BET, SEM, FT-IR, ICP-AES and TG. The catalytic activity and recovery properties of the catalysts for the Friedel-Crafts acylation of anisole with benzoyl chloride were evaluated. The results showed that 14.6–31.7 wt% PTA were encapsulated in the ZIF-67 cage. The PTA@ZIF-67(ec) catalysts had good catalytic activity for Friedel-Crafts acylation. The conversion of anisole can reach ~100% and the selectivity of the production can reach ~94% over 26.5 wt% PTA@ZIF-67(ec) catalyst under the reaction condition of 120 °C and 6 h. After reaction, the catalyst can be easily separated from the reaction mixture by the centrifugation. The recovered catalyst can be reused five times and the selectivity can be kept over 90%. - Graphical abstract: The PTA@ZIF-67 catalysts with different PTA content were prepared by encapsulating the PTA into ZIF-67 cage and the as-synthesized catalysts exhibited good catalytic activity for the Friedel–Craft acylation of anisole with benzoyl chloride.

  18. Review on Copper and Palladium Based Catalysts for Methanol Steam Reforming to Produce Hydrogen

    Directory of Open Access Journals (Sweden)

    Xinhai Xu


    Full Text Available Methanol steam reforming is a promising technology for producing hydrogen for onboard fuel cell applications. The methanol conversion rate and the contents of hydrogen, carbon monoxide and carbon dioxide in the reformate, significantly depend on the reforming catalyst. Copper-based catalysts and palladium-based catalysts can effectively convert methanol into hydrogen and carbon dioxide. Copper and palladium-based catalysts with different formulations and compositions have been thoroughly investigated in the literature. This work summarized the development of the two groups of catalysts for methanol steam reforming. Interactions between the activity components and the supports as well as the effects of different promoters were discussed. Compositional and morphological characteristics, along with the methanol steam reforming performances of different Cu/ZnO and Pd/ZnO catalysts promoted by Al2O3, CeO2, ZrO2 or other metal oxides, were reviewed and compared. Moreover, the reaction mechanism of methanol steam reforming over the copper based and palladium based catalysts were discussed.

  19. Highly coke-resistant ni nanoparticle catalysts with minimal sintering in dry reforming of methane. (United States)

    Han, Joung Woo; Kim, Chanyeon; Park, Jun Seong; Lee, Hyunjoo


    Nickel catalysts are typically used for hydrogen production by reforming reactions. Reforming methane with carbon dioxide, called dry reforming of methane (DRM), is a good way to produce hydrogen or syngas (a mixture of hydrogen and carbon monoxide) from two notable greenhouse gases. However, Ni catalysts used for DRM suffer from severe coke deposition. It has been known that small Ni nanoparticles are advantageous to reduce coke formation, but the high reaction temperature of DRM (800 °C) inevitably induces aggregation of the nanoparticles, leading to severe coke formation and degraded activity. Here, we develop highly coke-resistant Ni catalysts by immobilizing premade Ni nanoparticles of 5.2 nm in size onto functionalized silica supports, and then coating the Ni/SiO2 catalyst with silica overlayers. The silica overlayers enable the transfer of reactants and products while preventing aggregation of the Ni nanoparticles. The silica-coated Ni catalysts operate stably for 170 h without any degradation in activity. No carbon deposition was observed by temperature programmed oxidation (TPO), transmission electron microscopy (TEM), X-ray diffraction (XRD), and Raman spectroscopy. The Ni catalysts without silica coating show severe sintering after DRM reaction, and the formation of filamentous carbon was observed. The coke-resistant Ni catalyst is potentially useful in various hydrocarbon transformations. Copyright © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  20. Novel Fischer-Tropsch slurry catalysts and process concepts for selective transportation fuel production: Final report

    Energy Technology Data Exchange (ETDEWEB)

    Withers, H.P. Jr.; Eliezer, K.F.; Mitchell, J.W.


    The preparation, characterization and performance of cobalt and ruthenium carbonyl cluster-based catalysts for use in slurry-phase Fischer-Tropsch (FT) technology was investigated. The use of metal carbonyls as active metal precursor allows for the possible control of metal particle size on the support surface and thus offers the potential for better control of activity and selectivity of the FT reaction. Accomplishments included reproducible catalyst preparation, improvements in activity by use of a silica support, understanding diffeences between nitrate and carbonyl precursors, a nd good activity maintenance in the slurry reactor. A CO/sub 2/(CO)/sub 8/Zr(OPr)/sub 4/SiO/sub 2/ catalyst (3.5% CO, 6.6% Zr) was developed as the most active system in the slurry reactor and also gave the best liquid fuel selectivity. Silica support provided the highest catalyst activities. This catalyst was successfully tested in an extended slurry-phase run that achieved 6 months on stream with a 10% loss in activity. Ru catalysts showed the highest activity in the fixed-bed reactor but deactivated rapidly in the slurry reactor. In the analysis of the kinetic data, catalyst deactivation was assumed to proceed linearly between baseline experients at fixed temperture. Causes of the deactivation are not fully understood. 27 refs., 37 figs., 20 tabs.

  1. Degree of rate control approach to computational catalyst screening

    Energy Technology Data Exchange (ETDEWEB)

    Wolcott, Christopher A.; Medford, Andrew J.; Studt, Felix; Campbell, Charles T.


    A new method for computational catalyst screening that is based on the concept of the degree of rate control (DRC) is introduced. It starts by developing a full mechanism and microkinetic model at the conditions of interest for a reference catalyst (ideally, the best known material) and then determines the degrees of rate control of the species in the mechanism (i.e., all adsorbed intermediates and transition states). It then uses the energies of the few species with the highest DRCs for this reference catalyst as descriptors to estimate the rates on related materials and predict which are most active. The predictions of this method regarding the relative rates of twelve late transition metals for methane steam reforming, using the Rh(2 1 1) surface as the reference catalyst, are compared to the most commonly-used approach for computation catalyst screening, the Nørskov–Bligaard (NB) method which uses linear scaling relationships to estimate the energies of all adsorbed intermediates and transition states. It is slightly more accurate than the NB approach when the metals are similar to the reference metal (<0.5 eV different on a plot where the axes are the bond energies to C and O adatoms), but worse when too different from the reference. It is computationally faster than the NB method when screening a moderate number of materials (<100), thus adding a valuable complement to the NB approach. It can be implemented without a microkinetic model if the degrees of rate control are already known approximately, e.g., from experiments.

  2. Theoretical investigations of olefin metathesis catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Cundari, T.R.; Gordon, M.S. [North Dakota State Univ., Fargo, ND (United States)


    An ab initio analysis of the electronic structure of high-valent, transition-metal alkylidenes as models for olefin metathesis catalysts is presented. The catalyst models studied fall into three categories: {open_quotes}new{close_quotes} metathesis catalyst models-tetrahedral M(OH){sup 2}(XH)(CH{sub 2}) complexes; {open_quotes}old{close_quotes} metathesis catalyst models-tetrahedral MCl{sub 2}(Y)(CH{sub 2}) complexes and alkylidene-substituted Mo metathesis catalysts, Mo(OH){sub 2}(NH)(=C(H)Z). The effect on the bonding caused by modification of either the metal, ligands, or alkylidene substitutents is considered. 21 refs., 2 figs., 5 tabs.

  3. Process intensification of biodiesel production by using microwave and ionic liquids as catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Handayani, Prima Astuti [Department of Chemical Engineering, Diponegoro University (Indonesia); Chemical Engineering Program, Faculty of Engineering, Semarang State University (Indonesia); Abdullah; Hadiyanto, Dan, E-mail: [Department of Chemical Engineering, Diponegoro University (Indonesia)


    The energy crisis pushes the development and intensification of biodiesel production process. Biodiesel is produced by transesterification of vegetable oils or animal fats and conventionally produced by using acid/base catalyst. However, the conventional method requires longer processing time and obtains lower yield of biodiesel. The microwave has been intensively used to accelerate production process and ionic liquids has been introduced as source of catalyst. This paper discusses the overview of the development of biodiesel production through innovation using microwave irradiation and ionic liquids catalyst to increase the yield of biodiesel. The potential microwave to reduce the processing time will be discussed and compared with other energy power, while the ionic liquids as a new generation of catalysts in the chemical industry will be also discussed for its use. The ionic liquids has potential to enhance the economic and environmental aspects because it has a low corrosion effect, can be recycled, and low waste form.

  4. Process intensification of biodiesel production by using microwave and ionic liquids as catalyst (United States)

    Handayani, Prima Astuti; Abdullah, dan Hadiyanto


    The energy crisis pushes the development and intensification of biodiesel production process. Biodiesel is produced by transesterification of vegetable oils or animal fats and conventionally produced by using acid/base catalyst. However, the conventional method requires longer processing time and obtains lower yield of biodiesel. The microwave has been intensively used to accelerate production process and ionic liquids has been introduced as source of catalyst. This paper discusses the overview of the development of biodiesel production through innovation using microwave irradiation and ionic liquids catalyst to increase the yield of biodiesel. The potential microwave to reduce the processing time will be discussed and compared with other energy power, while the ionic liquids as a new generation of catalysts in the chemical industry will be also discussed for its use. The ionic liquids has potential to enhance the economic and environmental aspects because it has a low corrosion effect, can be recycled, and low waste form.

  5. A Study of Iron-Nitrogen-Carbon Fuel Cell Catalysts: Chemistry - Nanostructure - Performance (United States)

    Workman, Michael J., Jr.

    Fuel cells have the potential to be a pollution-free, low-cost, and energy efficient alternative to the internal combustion engine for transportation and small-scale stationary power applications. The current state of fuel cell technology has already achieved two of these three lofty goals. The remaining barrier to wide-scale deployment is the high cost, which is primarily caused by dependence on large amounts of platinum to catalyze the energy conversion reactions. To overcome this barrier and facilitate the integration of fuel cells into mainstream applications, research into a new class of catalyst materials that do not require platinum is needed. There has been a significant amount of research effort directed toward the development of platinum-group metal free (PGM-free) catalysts, yet there is a lack of consensus on both the engineering parameters necessary to improve the technology and the fundamental science that would facilitate rational design. I have engaged in research on PGM-free catalysts based on inexpensive and abundant reagents, specifically: nicarbazin and iron. Catalysts made from these precursors have previously proven to be among the best PGM-free catalysts, but their continued advancement suffered from the same lack of understanding that besets all catalysts in this class. The work I have performed address both engineering concerns and fundamental underlying principles. I present results demonstrating correlations between physical structure, chemical speciation, and synthesis parameters, as well as addressing active site chemistry and likely locations. My research presented herein introduces new morphology analysis techniques and elucidates several key structure-to-property characteristics of catalysts derived from iron and nicarbazin. I discuss the development and application of a new length-scale specific surface analysis technique that allows for analysis of well-defined size ranges from a few nm to several microns. The existing technique of

  6. Activity and Stability of Nanoscale Oxygen Reduction Catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Shao-Horn, Yang


    Design of highly active and stable nanoscale catalysts for electro-oxidation of small organic molecules is of great importance to the development of efficient fuel cells. The amount and instability of Pt-based catalysts in the cathode limits the cost, efficiency and lifetime of proton exchange membrane fuel cells. We developed a microscopic understanding of the factors governing activity and stability in Pt and PtM alloys. Experimental efforts were focused on probing the size and shape dependence of ORR activity of Pt-based nanoparticles supported on carbon nanotubes. A microscopic understanding of the activity was achieved by correlating voltammetry and rotating ring disk electrodes to surface atomic and electronic structures, which were elucidated predominantly by high-resolution transmission electron microscopy (HRTEM), Scanning transmission electron microscopy energy dispersive X-ray Spectroscopy (STEM-EDS) and synchrotron X-ray absorption spectroscopy (XAS).

  7. Activity Descriptors for CO2 Electroreduction to Methane on Transition-Metal Catalysts

    DEFF Research Database (Denmark)

    Peterson, Andrew; Nørskov, Jens K.


    The electrochemical reduction of CO2 into hydrocarbons and alcohols would allow renewable energy sources to be converted into fuels and chemicals. However, no electrode catalysts have been developed that can perform this transformation with a low overpotential at reasonable current densities. In ...... electrocatalyst. The protonation of adsorbed CO is singled out as the most important step dictating the overpotential. New strategies are presented for the discovery of catalysts that can operate with a reduced overpotential....

  8. Visible Light Responsive Catalysts Using Quantum Dot-Modified Ti02 for Air and Water Purification (United States)

    Coutts, Janelle L.; Levine, Lanfang H.; Richards, Jeffrey T.; Hintze, paul; Clausen, Christian


    The method of photocatalysis utilizing titanium dioxide, TiO2, as the catalyst has been widely studied for trace contaminant control for both air and water applications because of its low energy consumption and use of a regenerable catalyst. Titanium dioxide requires ultraviolet light for activation due to its band gap energy of 3.2 eV. Traditionally, Hg-vapor fluorescent light sources are used in PCO reactors and are a setback for the technology for space application due to the possibility of Hg contamination. The development of a visible light responsive (VLR) TiO2-based catalyst could lead to the use of solar energy in the visible region (approx.45% of the solar spectrum lies in the visible region; > 400 nm) or highly efficient LEDs (with wavelengths > 400 nm) to make PCO approaches more efficient, economical, and safe. Though VLR catalyst development has been an active area of research for the past two decades, there are few commercially available VLR catalysts; those that are available still have poor activity in the visible region compared to that in the UV region. Thus, this study was aimed at the further development of VLR catalysts by a new method - coupling of quantum dots (QD) of a narrow band gap semiconductor (e.g., CdS, CdSe, PbS, ZnSe, etc.) to the TiO2 by two preparation methods: 1) photodeposition and 2) mechanical alloying using a high-speed ball mill. A library of catalysts was developed and screened for gas and aqueous phase applications, using ethanol and 4-chlorophenol as the target contaminants, respectively. Both target compounds are well studied in photocatalytic systems serve as model contaminants for this research. Synthesized catalysts were compared in terms of preparation method, type of quantum dots, and dosage of quantum dots.

  9. Hydrocarbon reforming catalysts and new reactor designs for compact hydrogen generators

    Energy Technology Data Exchange (ETDEWEB)

    Schaefer, A.; Schwab, E.; Urtel, H. [BASF SE, Ludwigshafen (Germany); Farrauto, R. [BASF Catalysts LLC, Iselin, NJ (United States)


    the reforming of oxygen containing feedstocks like (bio-)ethanol or methanol, new catalyst formulations are needed which have been successfully developed and field tested. (orig.)

  10. Transitioning Rationally Designed Catalytic Materials to Real 'Working' Catalysts Produced at Commercial Scale: Nanoparticle Materials

    Energy Technology Data Exchange (ETDEWEB)

    Schaidle, Joshua A.; Habas, Susan E.; Baddour, Frederick G.; Farberow, Carrie A.; Ruddy, Daniel A.; Hensley, Jesse E.; Brutchey, Richard L.; Malmstadt, Noah; Robota, Heinz


    Catalyst design, from idea to commercialization, requires multi-disciplinary scientific and engineering research and development over 10-20 year time periods. Historically, the identification of new or improved catalyst materials has largely been an empirical trial-and-error process. However, advances in computational capabilities (new tools and increased processing power) coupled with new synthetic techniques have started to yield rationally-designed catalysts with controlled nano-structures and tailored properties. This technological advancement represents an opportunity to accelerate the catalyst development timeline and to deliver new materials that outperform existing industrial catalysts or enable new applications, once a number of unique challenges associated with the scale-up of nano-structured materials are overcome.

  11. Catalyst for producing lower alcohols (United States)

    Rathke, Jerome W.; Klingler, Robert J.; Heiberger, John J.


    A process and system for the production of the lower alcohols such as methanol, ethanol and propanol involves the reaction of carbon monoxide and water in the presence of a lead salt and an alkali metal formate catalyst combination. The lead salt is present as solid particles such as lead titanate, lead molybdate, lead vanadate, lead zirconate, lead tantalate and lead silicates coated or in slurry within molten alkali metal formate. The reactants, carbon monoxide and steam are provided in gas form at relatively low pressures below 100 atmospheres and at temperatures of C. The resulted lower alcohols can be separated into boiling point fractions and recovered from the excess reactants by distillation.


    Energy Technology Data Exchange (ETDEWEB)

    Constance Senior


    The objectives of this program were to measure the oxidation of mercury in flue gas across SCR catalyst in a coal-fired power plant burning low rank fuels using a slipstream reactor containing multiple commercial catalysts in parallel and to develop a greater understanding of mercury oxidation across SCR catalysts in the form of a simple model. The Electric Power Research Institute (EPRI) and Argillon GmbH provided co-funding for this program. REI used a multicatalyst slipstream reactor to determine oxidation of mercury across five commercial SCR catalysts at a power plant that burned a blend of 87% subbituminous coal and 13% bituminous coal. The chlorine content of the blend was 100 to 240 {micro}g/g on a dry basis. Mercury measurements were carried out when the catalysts were relatively new, corresponding to about 300 hours of operation and again after 2,200 hours of operation. NO{sub x}, O{sub 2} and gaseous mercury speciation at the inlet and at the outlet of each catalyst chamber were measured. In general, the catalysts all appeared capable of achieving about 90% NO{sub x} reduction at a space velocity of 3,000 hr{sup -1} when new, which is typical of full-scale installations; after 2,200 hours exposure to flue gas, some of the catalysts appeared to lose NO{sub x} activity. For the fresh commercial catalysts, oxidation of mercury was in the range of 25% to 65% at typical full-scale space velocities. A blank monolith showed no oxidation of mercury under any conditions. All catalysts showed higher mercury oxidation without ammonia, consistent with full-scale measurements. After exposure to flue gas for 2,200 hours, some of the catalysts showed reduced levels of mercury oxidation relative to the initial levels of oxidation. A model of Hg oxidation across SCRs was formulated based on full-scale data. The model took into account the effects of temperature, space velocity, catalyst type and HCl concentration in the flue gas.

  13. Novel Fischer-Tropsch slurry catalysts and process concepts for selective transportation fuel production: Quarterly technical progress report for the period 1 April-30 June 1986

    Energy Technology Data Exchange (ETDEWEB)

    Carroll, W.E.; Eliezer, K.F.; Mitchell, J.W.; Withers, H.P. Jr.


    In the seventh, and final quarter, work continued on the three major tasks: Task 2 - Development of Improved Supported Catalyst Compositions, Task 3 - Slurry Reactor Kinetic Studies, and Task 4 - Fuel Product Characterization. To examine the importance of surface area effects on the activity enhancement of the Co/Zr/silica catalyst, a Co/Zr/silica catalyst having the same surface area as the Co/Zr/alumina catalyst was tested in the fixed bed reactor. Silica provided an inherently more active catalyst than alumina but some of the enhancement that was initially observed was due to the increased surface area. The effect of increasing metal loadings on the performance of the Co/Zr/silica catalyst was examined with tests of 11% and 14.4$ Co catalysts in the fixed bed reactor. The 11% Co catalyst gave the highest syngas conversion (52%) at 220/sup 0/C of any catalyst tested at this temperature during this contract. Selectivity to liquid fuel product declined with increasing Co loading with an overall flattening of the hydrocarbon distribution. Slurry screening tests were performed on two catalysts. One was a cobalt on silica catalyst without any added promoter atoms such as Zr or Ti. The other screening test was a Zr promoted cobalt on silica catalyst with a high loading of Co. The extended slurry test which was begun in December 1985 was completed in June. During this quarter, a series of experiments was run to try to determine reaction kinetics. The spent catalyst from the extended slurry test of the Co/Zr/SiO/sub 2/ catalyst was found to contain 43.2% carbon and 2.4% hydrogen. This indicated a significant amount of coke formation. A second sample of liquid organic product was collected from the extended slurry test for testing as a diesel fuel. This sample met all the requirements for the highest quality diesel fuel except for viscosity and cloud point. 6 refs., 57 figs., 98 tabs.

  14. Oxidation Catalysts for Elemental Mercury in Flue Gases—A Review

    Directory of Open Access Journals (Sweden)

    Liliana Lazar


    Full Text Available The removal of mercury from flue gases in scrubbers is greatly facilitated if the mercury is present as water-soluble oxidized species. Therefore, increased mercury oxidation upstream of scrubber devices will improve overall mercury removal. For this purpose heterogeneous catalysts have recently attracted a great deal of interest. Selective catalytic reduction (SCR, noble metal and transition metal oxide based catalysts have been investigated at both the laboratory and plant scale with this objective. A review article published in 2006 covers the progress in the elemental mercury (Hgel catalytic oxidation area. This paper brings the review in this area up to date. To this end, 110 papers including several reports and patents are reviewed. For each type of catalyst the possible mechanisms as well as the effect of flue gas components on activity and stability are examined. Advantages and main problems are analyzed. The possible future directions of catalyst development in this environmental research area are outlined.

  15. Comparison of particle size of cracking catalyst determined by laser light scattering and dry sieve methods

    Energy Technology Data Exchange (ETDEWEB)

    Dishman, K.L.; Doolin, P.K.; Hoffman, J.F. (Ashland Petroleum Co., Ashland, KY (United States))


    A method of interconversion of dry sieve and laser light scattering particle size values has been developed for cracking catalysts. Values obtained by light scattering techniques were consistently larger than those obtained by dry sieve analysis. The differences were primarily due to lack of sphericity of the particles. The particle size distribution determined by light scattering techniques was based on an average particle diameter. Conversely, the sieve measured the smallest diameter of the particle which can pass through the opening. Microscopic examination of commercial cracking catalysts confirmed their nonuniformity. The sphericity of the catalyst particles decreased as particle size increased. Therefore, the divergence between the laser light scattering and dry sieving value became greater as the catalyst particle size increased.

  16. Modeling Deactivation of Catalysts for Selective Catalytic Reduction of NOx by KCl Aerosols

    DEFF Research Database (Denmark)

    Olsen, Brian Kjærgaard; Castellino, Francesco; Jensen, Anker Degn


    A detailed model for the deactivation of a V2O5–WO3/TiO2-based SCR monolith catalyst by potassium poisoning has been developed and validated. The model accounts for deposition of KCl aerosol particles present in the flue gas on the external catalyst surface, the reaction of the deposited particles...... deactivation rate of a 3 wt % V2O5-7 wt % WO3/TiO2 monolith catalyst, exposed to a KCl aerosol at 350 °C for about 1000 h, as well as the resulting potassium-to-vanadium molar ratios in the catalyst wall. Simulations show that the particle deposition rate, as well as the deactivation rate, decreases...

  17. ɛ-Iron carbide as a low-temperature Fischer-Tropsch synthesis catalyst (United States)

    Xu, Ke; Sun, Bo; Lin, Jun; Wen, Wen; Pei, Yan; Yan, Shirun; Qiao, Minghua; Zhang, Xiaoxin; Zong, Baoning


    ɛ-Iron carbide has been predicted to be promising for low-temperature Fischer-Tropsch synthesis (LTFTS) targeting liquid fuel production. However, directional carbidation of metallic iron to ɛ-iron carbide is challenging due to kinetic hindrance. Here we show how rapidly quenched skeletal iron featuring nanocrystalline dimensions, low coordination number and an expanded lattice may solve this problem. We find that the carbidation of rapidly quenched skeletal iron occurs readily in situ during LTFTS at 423-473 K, giving an ɛ-iron carbide-dominant catalyst that exhibits superior activity to literature iron and cobalt catalysts, and comparable to more expensive noble ruthenium catalyst, coupled with high selectivity to liquid fuels and robustness without the aid of electronic or structural promoters. This finding may permit the development of an advanced energy-efficient and clean fuel-oriented FTS process on the basis of a cost-effective iron catalyst.

  18. ε-Iron carbide as a low-temperature Fischer-Tropsch synthesis catalyst. (United States)

    Xu, Ke; Sun, Bo; Lin, Jun; Wen, Wen; Pei, Yan; Yan, Shirun; Qiao, Minghua; Zhang, Xiaoxin; Zong, Baoning


    ε-Iron carbide has been predicted to be promising for low-temperature Fischer-Tropsch synthesis (LTFTS) targeting liquid fuel production. However, directional carbidation of metallic iron to ε-iron carbide is challenging due to kinetic hindrance. Here we show how rapidly quenched skeletal iron featuring nanocrystalline dimensions, low coordination number and an expanded lattice may solve this problem. We find that the carbidation of rapidly quenched skeletal iron occurs readily in situ during LTFTS at 423-473 K, giving an ε-iron carbide-dominant catalyst that exhibits superior activity to literature iron and cobalt catalysts, and comparable to more expensive noble ruthenium catalyst, coupled with high selectivity to liquid fuels and robustness without the aid of electronic or structural promoters. This finding may permit the development of an advanced energy-efficient and clean fuel-oriented FTS process on the basis of a cost-effective iron catalyst.

  19. The renaissance of iron-based Fischer-Tropsch synthesis: on the multifaceted catalyst deactivation behaviour. (United States)

    de Smit, Emiel; Weckhuysen, Bert M


    Iron-based Fischer-Tropsch catalysts, which are applied in the conversion of CO and H2 into longer hydrocarbon chains, are historically amongst the most intensively studied systems in heterogeneous catalysis. Despite this, fundamental understanding of the complex and dynamic chemistry of the iron-carbon-oxygen system and its implications for the rapid deactivation of the iron-based catalysts is still a developing field. Fischer-Tropsch catalysis is characterized by its multidisciplinary nature and therefore deals with a wide variety of fundamental chemical and physical problems. This critical review will summarize the current state of knowledge of the underlying mechanisms for the activation and eventual deactivation of iron-based Fischer-Tropsch catalysts and suggest systematic approaches for relating chemical identity to performance in next generation iron-based catalyst systems (210 references).

  20. Discovery of a Ni-Ga catalyst for carbon dioxide reduction to methanol

    DEFF Research Database (Denmark)

    Studt, Felix; Sharafutdinov, Irek; Abild-Pedersen, Frank


    The use of methanol as a fuel and chemical feedstock could become very important in the development of a more sustainable society if methanol could be efficiently obtained from the direct reduction of CO 2 using solar-generated hydrogen. If hydrogen production is to be decentralized, small-scale CO...... 2 reduction devices are required that operate at low pressures. Here, we report the discovery of a Ni-Ga catalyst that reduces CO 2 to methanol at ambient pressure. The catalyst was identified through a descriptor-based analysis of the process and the use of computational methods to identify Ni......-Ga intermetallic compounds as stable candidates with good activity. We synthesized and tested a series of catalysts and found that Ni 5 Ga 3 is particularly active and selective. Comparison with conventional Cu/ZnO/Al 2 O 3 catalysts revealed the same or better methanol synthesis activity, as well as considerably...

  1. Chemoselective single-site Earth-abundant metal catalysts at metal-organic framework nodes (United States)

    Manna, Kuntal; Ji, Pengfei; Lin, Zekai; Greene, Francis X.; Urban, Ania; Thacker, Nathan C.; Lin, Wenbin


    Earth-abundant metal catalysts are critically needed for sustainable chemical synthesis. Here we report a simple, cheap and effective strategy of producing novel earth-abundant metal catalysts at metal-organic framework (MOF) nodes for broad-scope organic transformations. The straightforward metalation of MOF secondary building units (SBUs) with cobalt and iron salts affords highly active and reusable single-site solid catalysts for a range of organic reactions, including chemoselective borylation, silylation and amination of benzylic C-H bonds, as well as hydrogenation and hydroboration of alkenes and ketones. Our structural, spectroscopic and kinetic studies suggest that chemoselective organic transformations occur on site-isolated, electron-deficient and coordinatively unsaturated metal centres at the SBUs via σ-bond metathesis pathways and as a result of the steric environment around the catalytic site. MOFs thus provide a novel platform for the development of highly active and affordable base metal catalysts for the sustainable synthesis of fine chemicals.

  2. Confinement dependence of electro-catalysts for hydrogen evolution from water splitting

    Directory of Open Access Journals (Sweden)

    Mikaela Lindgren


    Full Text Available Density functional theory is utilized to articulate a particular generic deconstruction of the electrode/electro-catalyst assembly for the cathode process during water splitting. A computational model was designed to determine how alloying elements control the fraction of H2 released during zirconium oxidation by water relative to the amount of hydrogen picked up by the corroding alloy. This model is utilized to determine the efficiencies of transition metals decorated with hydroxide interfaces in facilitating the electro-catalytic hydrogen evolution reaction. A computational strategy is developed to select an electro-catalyst for hydrogen evolution (HE, where the choice of a transition metal catalyst is guided by the confining environment. The latter may be recast into a nominal pressure experienced by the evolving H2 molecule. We arrived at a novel perspective on the uniqueness of oxide supported atomic Pt as a HE catalyst under ambient conditions.

  3. Decomposition kinetics of ammonia in gaseous stream by a nanoscale copper-cerium bimetallic catalyst. (United States)

    Hung, Chang-Mao


    This study performance is to examine the kinetics over nanoscale copper-cerium bimetallic catalyst under selective catalytic oxidation (SCO) of ammonia to N(2) in a tubular fixed-bed reactor (TFBR) at temperatures from 150 to 400 degrees C in the presence of oxygen. The nanoscale copper-cerium bimetallic catalyst was prepared by co-precipitation with Cu(NO(3))(2) and Ce(NO(3))(3) at molar ratio of 6:4. Experimental results showed that the catalyst with transmission electron microscopy (TEM) revealed that copper and cerium are well dispersed and catalyst in the form of nanometer-sized particles. Moreover, the kinetic behavior of NH(3) oxidation with catalysis can be accounted by using the rate expression of the Langmuir-Hinshelwood type kinetic model. Kinetic parameters are also developed on the basis of the differential reactor data. Also, experimental results are compared with those of the model predicted.

  4. Catalyst dispersion and activity under conditions of temperature-staged liquefaction

    Energy Technology Data Exchange (ETDEWEB)

    Davis, A.; Schobert, H.H.; Mitchell, G.D.; Artok, L.


    The general objectives of this research are (1) to investigate the use of highly dispersed catalysts for the pretreatment of coal by mild hydrogenation, (2) to identify the active forms of the catalysts under reaction conditions and (3) to clarify the mechanisms of catalysis. The ultimate objective is to ascertain if mild catalytic hydrogenation resulting in very limited or no coal solubilization is an advantageous pretreatment for the transformation of coal into transportable fuels. The experimental program will focus upon the development of effective methods of impregnating coal with catalysts, evaluating the conditions under which the catalysts are most active and establishing the relative impact of improved impregnation on conversion and product distributions obtained from coal hydrogenation.

  5. K (Na)-promoted Ni, Al layered double hydroxide catalysts for the steam reforming of methanol (United States)

    Qi, Caixia; Amphlett, John C.; Peppley, Brant A.

    Production of hydrogen by methanol steam reforming has been studied over a series of Ni/Al layered double hydroxide catalysts prepared by the co-precipitation method, with the aim to develop a stable catalyst that can be used in a membrane-joint performer at temperatures greater than 300 °C. H 2, CO and CO 2 are generally the major products together with trace amounts of CH 4. The presence of potassium and/or sodium cations was found to improve the activity of methanol conversion. The selectivity for CO 2 rather than CO was better with K ions than Na ions, especially at higher temperatures (e.g. 390-400 °C). Methanol steam reforming over a K-promoted Ni/Al layered double hydroxide catalyst resulted in better activity and similar stability compared to a commercial Cu catalyst.

  6. Carbon nanocages: A new support material for Pt catalyst with remarkably high durability (United States)

    Wang, Xiao Xia; Tan, Zhe Hua; Zeng, Min; Wang, Jian Nong


    Low durability is the major challenge hindering the large-scale implementation of proton exchange membrane fuel cell (PEMFC) technology, and corrosion of carbon support materials of current catalysts is the main cause. Here, we describe the finding of remarkably high durability with the use of a novel support material. This material is based on hollow carbon nanocages developed with a high degree of graphitization and concurrent nitrogen doping for oxidation resistance enhancement, uniform deposition of fine Pt particles, and strong Pt-support interaction. Accelerated degradation testing shows that such designed catalyst possesses a superior electrochemical activity and long-term stability for both hydrogen oxidation and oxygen reduction relative to industry benchmarks of current catalysts. Further testing under conditions of practical fuel cell operation reveals almost no degradation over long-term cycling. Such a catalyst of high activity, particularly, high durability, opens the door for the next-generation PEMFC for “real world” application. PMID:24658614

  7. Highly Selective Deoxydehydration of Tartaric Acid over Supported and Unsupported Rhenium Catalysts with Modified Acidities. (United States)

    Li, Xiukai; Zhang, Yugen


    The deoxydehydration (DODH) of sugar acids to industrially important carboxylic acids is a very attractive topic. Oxorhenium complexes are the most-often employed DODH catalysts. Because of the acidity of the rhenium catalysts, the DODH products of sugar acids were usually in the form of mixture of free carboxylic acids and esters. Herein, we demonstrate strategies for the selective DODH of sugar acids to free carboxylic acids by tuning the Lewis acidity or the Brønsted acidity of the rhenium-based catalysts. Starting from tartaric acid, up to 97 % yield of free maleic acid was achieved. Based on our strategies, functional polymer immobilized heterogeneous rhenium catalysts were also developed for the selective DODH conversion of sugar acids. © 2016 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  8. Synthesis of carbon tubule nanocoils using Fe-In-Sn-O fine particles as catalysts. (United States)

    Okazaki, Nobuharu; Hosokawa, Shoji; Goto, Toshiki; Nakayama, Yoshikazu


    We have developed Fe-In-Sn-O fine particle or powder catalysts for synthesizing carbon nanocoils by catalytic thermal chemical vapor deposition. The coprecipitation technique was used to produce the powder catalysts. By optimizing the composition ratios of Fe, In (between 10 and 33% of Fe), and Sn (less than 3.3% of Fe), carbon nanocoils could be grown in high yield. From the study of optimizing the compositions of In and Sn and the study of crystal structures of the catalysts using X-ray diffraction measurements, it was also found that Sn in the catalysts was required to grow carbon nanocoils and that In plays roles in increasing the yield of carbon nanocoils and controlling the coil diameters. This study will lead to the mass production of carbon nanocoils and therefore widen their applications.

  9. A Novel FCC Catalyst Based on a Porous Composite Material Synthesized via an In Situ Technique

    Directory of Open Access Journals (Sweden)

    Shu-Qin Zheng


    Full Text Available To overcome diffusion limitations and improve transport in microporous zeolite, the materials with a wide-pore structure have been developed. In this paper, composite microspheres with hierarchical porous structure were synthesized by an in situ technique using sepiolite, kaolin and pseudoboehmite as raw material. A novel fluid catalytic cracking (FCC catalyst for maximizing light oil yield was prepared based on the composite materials. The catalyst was characterized by XRD, FT-IR, SEM, nitrogen adsorption-desorption techniques and tested in a bench FCC unit. The results indicated that the catalyst had more meso- and macropores and more acid sites than the reference catalyst, and thus can increase light oil yield by 1.31 %, while exhibiting better gasoline and coke selectivity.

  10. Chitosan as a Natural Polymer for Heterogeneous Catalysts Support: A Short Review on Its Applications

    Directory of Open Access Journals (Sweden)

    Mengshan Lee


    Full Text Available Chitosan, a bio-based polymer which has similar characteristics to those of cellulose, exhibits cationic behavior in acidic solutions and strong affinity for metals ions. Thus, it has received increased attention for the preparation of heterogeneous catalysts. Recent studies demonstrated that chitosan-based catalysts had high sorption capacities, chelating activities, stability and versatility, which could be potentially applied as green reactants in various scientific and engineering applications. This study intends to review the recent development of chitosan-based catalysts, particularly in the aspects of the main mechanisms for preparing the materials and their applications in environmental green chemistry. Studies on the preparation of catalyst nanoparticles/nanospheres supported on chitosan were also reviewed.

  11. Numerical assessment of dependence of polymer electrolyte membrane fuel cell performance on cathode catalyst layer parameters

    Energy Technology Data Exchange (ETDEWEB)

    Obut, Salih [TUBITAK Marmara Research Center, Energy Institute, TR-41470, Kocaeli (Turkey); Alper, Erdogan [Chemical Engineering Department, Hacettepe University, TR-06800, Ankara (Turkey)


    In this work, a three-dimensional, non-isothermal and two-phase computational fluid dynamics model of a proton exchange membrane (PEM) fuel cell with straight flow field channel is developed and validated. The model is used to predict the performance of the PEM fuel cell with changing parameters of the cathode catalyst layer which was usually assumed to be composed of spherical agglomerates. The effect of cathode catalyst layer parameters such as catalyst layer thickness, ionomer film thickness, agglomerate size and porosity, on the current density and power output of the PEM fuel cell is investigated. The numerical results reveal that competitive influence of resistances to transport of species, electron and proton within the cathode catalyst layer determines the performance of the PEM fuel cell in terms of area specific power density (W cm{sup -2}) and mass specific power density (kW g{sub Pt}{sup -1}). (author)

  12. Effects of Catalyst Variation on Biodiesel Yield


    A. O. Adeodu


    The type, purity and amount of catalyst used affect the conversion efficiency of the transesterification process of converting oil to biodiesel. In this study, the effect of alkali and acid catalysts variation was examined on biodiesel yield. Sodium hydroxide at different concentration of 0.6-1.6% to unused oil was used as a catalyst for transesesterifying unused oil to biodiesel. The optimum biodiesel yield was achieved using 1.4 wt. % of NaOH to oil weight, which produced an 88.0% yield of ...

  13. Tribenzylbis(triphenylarsine oxide-κOtin(IV tetraphenylborate

    Directory of Open Access Journals (Sweden)

    Thy Chun Keng


    Full Text Available The crystal structure of the title salt, [Sn(C7H73(C18H15AsO2][B(C6H54], consists of discrete cations and anions; the tin atom of the cation is five-coordinated in a distorted trans-C3SnO2 trigonal-bipyramidal geometry [summation of C–Sn–C angles 360.0 (3° and O–Sn–O angle 173.1 (1°]. The structure contains voids of 113 (19 Å3, but no solvent molecule could reasonably be located there.

  14. Sodium tetraphenylborate solution stability: A long term study

    Energy Technology Data Exchange (ETDEWEB)

    Barnes, M.J.


    Sodium tetraphenylborata (NaTPB) is a specialty chemical required for the In Tank Precipitation Process (ITP). It precipitates cesium, aiding in the decontamination of high level radioactive waste solutions. Long term stability of aqueous alkaline solutions of NATPB has been investigated. The focus of the investigation is on the relative stabilities of NATPB solutions exposed to varying temperatures and copper concentrations over an extended period of time. Additionally, vendor-supplied samples, incubated at 40{degree}C, were stored for more than a year without decomposing. Collected data demonstrates that in the absence of elevated copper concentrations, NATPB solutions will remain stable for periods of 1 to 2 years (at a minimum) at maximum expected operating conditions (<40{degree}C). Additionally, biuret, (H{sub 2}NCO){sub 2}NH, was tested as an additive to prevent copper-induced decomposition without success.

  15. Sodium tetraphenylborate solution stability: A long term study

    Energy Technology Data Exchange (ETDEWEB)

    Barnes, M.J.


    Sodium tetraphenylborata (NaTPB) is a specialty chemical required for the In Tank Precipitation Process (ITP). It precipitates cesium, aiding in the decontamination of high level radioactive waste solutions. Long term stability of aqueous alkaline solutions of NATPB has been investigated. The focus of the investigation is on the relative stabilities of NATPB solutions exposed to varying temperatures and copper concentrations over an extended period of time. Additionally, vendor-supplied samples, incubated at 40[degree]C, were stored for more than a year without decomposing. Collected data demonstrates that in the absence of elevated copper concentrations, NATPB solutions will remain stable for periods of 1 to 2 years (at a minimum) at maximum expected operating conditions (<40[degree]C). Additionally, biuret, (H[sub 2]NCO)[sub 2]NH, was tested as an additive to prevent copper-induced decomposition without success.

  16. 40 CFR 90.427 - Catalyst thermal stress resistance evaluation. (United States)


    ... 40 Protection of Environment 20 2010-07-01 2010-07-01 false Catalyst thermal stress resistance... Gaseous Exhaust Test Procedures § 90.427 Catalyst thermal stress resistance evaluation. (a) The purpose of... catalyst conversion efficiency for Phase 1 engines. The thermal stress is imposed on the test catalyst by...

  17. Investigation of activity and selectivity of redox catalysts in oxidative ...

    African Journals Online (AJOL)

    In this study, oxidative coupling of methane on Redox catalysts in fluidized bed reactor was investigated. For this purpose, the catalyst Mn-Na2WO4/SiO2 was selected as a Redox catalyst. In order to investigate this catalyst, transient state experiments were designed and performed. Then, the different reaction conditions on ...

  18. Bio-oil hydrodeoxygenation catalysts produced using strong electrostatic adsorption (United States)

    We synthesized hydrothermally stable metal catalysts with controlled particle size and distribution, with the goal of determining which catalyst(s) can selectively catalyze the production of aromatics from bio-oil (from pyrolysis of biomass). Both precious and base transition metal catalysts (Ru, Pt...

  19. Supported catalyst systems and method of making biodiesel products using such catalysts (United States)

    Kim, Manhoe; Yan, Shuli; Salley, Steven O.; Ng, K. Y. Simon


    A heterogeneous catalyst system, a method of preparing the catalyst system and a method of forming a biodiesel product via transesterification reactions using the catalyst system is disclosed. The catalyst system according to one aspect of the present disclosure represents a class of supported mixed metal oxides that include at least calcium oxide and another metal oxide deposited on a lanthanum oxide or cerium oxide support. Preferably, the catalysts include CaO--CeO.sub.2ZLa.sub.2O.sub.3 or CaO--La.sub.2O.sub.3/CeO.sub.2. Optionally, the catalyst may further include additional metal oxides, such as CaO--La.sub.2O.sub.3--GdOxZLa.sub.2O.sub.3.

  20. Biodiesel synthesis via transesterification of lipid Chlorophyta cultivated in walne rich carbon medium using KOH/Zeolite catalyst (United States)

    Dianursanti, Hayati, Siti Zahrotul; Putri, Dwini Normayulisa


    Microalgae from the Chlorophyta division such as Nannochloropsis oculata and Chlorella vulgaris are highly potential to be developed as biodiesel feedstocks because they have a high oil content up to 58%. Biodiesel is produced by transesterification of triglycerides and alcohols with the aid of homogeneous catalysts such as KOH. However, the use of KOH catalysts produces soaps in the biodiesel synthesis. Heterogeneous catalysts are known to solve this problem. One of them is natural zeolite. Zeolite can be used as a catalyst and as a support catalyst. Loading KOH on the zeolite surface is expected to increase alkalinity in KOH/Zeolite catalysts so as to increase the activity of KOH/Zeolite catalyst in transesterification of triglyceride with methanol. In this experimental lipid of microalgae will be used for produced biodiesel via transesterification reaction with methanol and KOH/Zeolite as a catalyst heterogeneous at 60 °C for 3h and utilized catalyst modificated KOH/Zeolite with variation 0.5 M, 1 M and 1.5 M KOH. The modified zeolite was then analyzed by XRF, XRD and BET. The result showed that the yield of biodiesel from lipid N.oculata was 81,09% by 0.5KOH/Zeolite catalyst, 86,53% by 1KOH/Zeolite catalyst, 1,5KOH/Zeolite and 88,13% by 1.5KOH/Zeolit, while the biodiesel produced from lipid C.vulgaris was 59.29% by 0.5KOH/Zeolite, 82.27% by 1KOH/Zeolite and 83.72% by 1.5KOH/Zeolite.