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Effect of Palladium Form on Tetraphenylborate Decomposition Rate

Description: Palladium catalyzes the decomposition of tetraphenylborate in alkaline solutions. Researchers postulate several decomposition mechanisms that differ in the form of the palladium catalyst. Potential forms include solid and soluble, different soluble species (such as aqueous or organic soluble), and different oxidation states (i.e., 0, II, and IV). Initial tests measured the reactivity and distribution of four Pd forms in tetraphenylborate slurries.
Date: April 28, 1998
Creator: Walker, D. D.
Partner: UNT Libraries Government Documents Department

Effects of Mineral Salts on Short-Term Incorporation of CarbonDioxide in Chlorella

Description: Although the functions of the essential major elements in plant metabolism have been studied for many years, little work has been done concerning the effect of these elements during short-term incorporation of radioactive carbon dioxide. This may be of some importance as it has been the general custom during photosynthesis studies in this laboratory to suspend algae in various dilute buffer solutions or in distilled water alone assuming that the salt remaining within the cells from the time of growth in nutrient solution are sufficient in quantity for the cells not to become deficient in one or more of the essential elements during the course of the experiment. There are some indications, however, that the addition of salts to algae suspended in distilled water may have a rapid, pronounced effect on some metabolic system within the plant. Thus, Clendenning, Brown and Eyster (1956) have reported that Nostoc muscorum, if rinsed and resuspended in distilled water, loses most of its photosynthetic capacity, which can, however, be completely restored by the addition of potassium ion in concentrations no greater than a few parts per million. Also, K. Baalorud (personal communication) found that the photosynthetic rate of a marine diatom, when suspended in synthetic magnesium-free water, can be greatly increased by the addition of magnesium salts. In view of these observations it appeared worthwhile to investigate the effects of the addition of the essential elements in those photosynthesis experiments in which the cells are kept in distilled water for varying periods of time.
Date: July 1, 1958
Creator: Holm-Hansen, O.; Nishida, K.; Moses, V. & Calvin, M.
Partner: UNT Libraries Government Documents Department


Description: The present study demonstrates that [Ru{sup II}(NH{sub 3})(q)(trpy)]{sup +} has an ability to oxidize alcohols catalytically under very mild conditions under electrolysis at +0.35 V in MeOH. The elucidation of the reaction mechanisms in the alcohol-oxidation is underway.
Date: November 30, 2007
Partner: UNT Libraries Government Documents Department

Influence of Carbon on the Electrical Properties of Crustal Rocks

Description: The report summarizes work to determine the nature and distribution of carbon on microcracks in crystalline rocks by time-of-flight secondary ion mass spectroscopy. It also summarizes the results of a workshop devoted to investigating how carbon in rocks influences electrical conductivity and whether carbon on fracture surfaces can account for the electrical conductivity structure of the crust.
Date: November 19, 2002
Creator: Mathez, E. A.
Partner: UNT Libraries Government Documents Department

Metal Carbonyl-Hydrosilane Reactions and Hydrosilation Catalysis

Description: Manganese carbonyl complexes serve as hydrosilation precatalysts for selectively transforming a carbonyl group into a siloxy methylene or a fully reduced methylene group. Substrates of interest include (1) aldehydes, ketones, carboxylic acids, silyl esters, and esters, and (2) their organometallic acyl counterparts. Three relevant catalytic reactions are shown. Two types of manganese precatalysts have been reported: (a) alkyl and acyl complexes (L)(C0){sub 4}MnR [L = CO, PPh{sub 3}; R = COCH{sub 3}, COPh, CH{sub 3}] and (b) halides (CO){sub 5}MnX and [(CO){sub 4}MnX]{sub 2} (X = Br, I). The former promote hydrosilation and deoxygenation catalysis; the latter promote dehydrogenative silation of alcohols and carboxylic acids as well as hydrosilation and deoxygenation of some metallocarboxylic acid derivatives. In every case studied, these Mn precatalysts are far more reactive or selective than traditional Rh(I) precatalysts.
Date: April 14, 2001
Creator: Cutler, A. R.
Partner: UNT Libraries Government Documents Department

Desulfurization of coal: Enhanced selectivity using phase transfer catalysts. Final technical report, September 1, 1995--August 31, 1996

Description: Due to environmental problems related to the combustion of high sulfur Illinois coal, there continues to be interest in the development of viable pre-combustion desulfurization processes. Recent studies by the authors have obtained very good sulfur removals but the reagents that are used are too expensive. Use of cheaper reagents leads to a loss of desired coal properties. This study investigated the application of phase transfer catalysts to the selective oxidation of sulfur in coal using air and oxygen as oxidants. The phase transfer catalyst was expected to function as a selectivity moderator by permitting the use of milder reaction conditions than otherwise necessary. This would enhance the sulfur selectivity and help retain the heating value of the coal. The use of certain coal combustion wastes for desulfurization, and the application of cerium (IV) catalyzed air oxidations for selective sulfur oxidation were also studied. If successful this project would have lead to the rapid development of a commercially viable desulfurization process. This would have significantly improved the marketability of Illinois coal. However, the phase transfer catalysts, the cerium and the scrubber sledge did not catalize the sulfur removal significantly.
Date: May 1, 1997
Creator: Palmer, S.R. & Hippo, E.J.
Partner: UNT Libraries Government Documents Department

Platinum Catalyzed Decomposition of Activated Carbon: 1. Initial Studies

Description: Carbon is an important support for heterogeneous catalysts, such as platinum supported on activated carbon (AC). An important property of these catalysts is that they decompose upon heating in air. Consequently, Pt/AC catalysts can be used in applications requiring rapid decomposition of a material, leaving little residue. This report describes the catalytic effects of platinum on carbon decomposition in an attempt to maximize decomposition rates. Catalysts were prepared by impregnating the AC with two different Pt precursors, Pt(NH{sub 3}){sub 4}(NO{sub 3}){sub 2} and H{sub 2}PtCl{sub 6}. Some catalysts were treated in flowing N{sub 2} or H{sub 2} at elevated temperatures to decompose the Pt precursor. The catalysts were analyzed for weight loss in air at temperatures ranging from 375 to 450 C, using thermogravimetric analysis (TGA). The following results were obtained: (1) Pt/AC decomposes much faster than pure carbon; (2) treatment of the as-prepared 1% Pt/AC samples in N{sub 2} or H{sub 2} enhances decomposition; (3) autocatalytic behavior is observed for 1% Pt/AC samples at temperatures {ge} 425 C; (4) oxygen is needed for decomposition to occur. Overall, the Pt/AC catalyst with the highest activity was impregnated with H{sub 2}PtCl{sub 6} dissolved in acetone, and then treated in H{sub 2}. However, further research and development should produce a more active Pt/AC material.
Date: December 1, 2001
Partner: UNT Libraries Government Documents Department

Evaluation of fine-particle size catalysts using bituminous and subbituminous coals

Description: The objectives of Sandia`s fine-particle size catalyst testing project are to evaluate and compare the activities of fine-particle size catalysts being developed in DOE/PETC`s Advanced Research Coal Liquefaction Program by using Sandia`s standard coal liquefaction test procedures. The first test procedure uses bituminous coal (DECS-17 Blind Canyon coal), phenanthrene as the reaction solvent, and a factorial experimental design that is used to evaluate catalysts over ranges of temperature, time, and catalyst loading. The best catalyst evaluated to date is West Virginia University`s iron catalyst that was impregnated onto the coal. Current work is aimed at developing a standard test procedure using subbituminous Wyodak coal. Ibis test is being developed using Pacific Northwest Laboratories` 6-line ferrihydrite catalyst and coal samples impregnated with either molybdenum or iron at Argonne National Laboratories. Results of testing catalysts with bituminous coal will be summarized and the development of the subbituminous coal test procedure will be presented.
Date: June 1, 1996
Creator: Stohl, F.V.; Diegert, K.V. & Goodnow, D.C.
Partner: UNT Libraries Government Documents Department

Task 4.7 - diesel fuel desulfurization. Semi-annual report, July 1, 1995--December 31, 1995

Description: Reductions in the maximum permissible sulfur content of diesel fuel to less than 0.05 wt% will require deep desulfurization to meet these standards. In some refineries, a new hydrogenation catalyst may be required for diesel fuel production. The work very briefly described in this document is on the use of hydrotalcite-supported molybdenum sulfide in the catalysis of ethanol. The catalyst reaction was highly selective for 1-butanol, providing a very clean reaction. Since the catalysis contains the MoS{sub 2} needed for the dehydrogenation and hydrogenation steps, the reaction can be performed at lower temperatures and higher selectivity. The catalyst was very stable and not destroyed by the water produced in the reaction.
Date: December 31, 1998
Creator: Olson, E.S.
Partner: UNT Libraries Government Documents Department

Technology development for iron fisher-tropsch catalysis

Description: The goal of the proposed work is 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 catalyst that is developed will be suitable for testing at the Advanced Fuels Development Facility at LaPorte, Texas or similar sized plant. Previous work by the offeror has produced a catalyst formulation that is 1.5 times as active as the standard-catalyst developed by German workers for slurry phase synthesis, The proposed work will optimize the catalyst composition and pretreatment operation for this low-alpha catalyst. In parallel, work will be conducted to design a high-alpha iron catalyst that 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 studies at the laboratory scale. Catalyst performance will be determined for catalysts synthesized in this program for activity, selectivity, and aging characteristics.
Date: July 15, 1997
Creator: Davis, B.H.
Partner: UNT Libraries Government Documents Department

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

Description: 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}.
Date: October 1, 1997
Creator: McCormick, R.L.
Partner: UNT Libraries Government Documents Department

Aerial oxidation of tetraethyl silicate and effect on ammonia catalyzed hydrolysis

Description: Colloidal suspensions of Si0{sub 2} in ethanol prepared by the ammonia catalyzed hydrolysis of tetraethyl silicate (TEOS) in ethanol have been routinely used for over 10 years to prepare antireflective (AR) coatings on the fused silica transmissive optical components of high power fusion lasers. Very high purity coatings are required to avoid laser damage and these are obtained when the TEOS is fractionally distilled under N{sub 2} prior to use. Recently we found that products from aerial oxidation of distilled TEOS, had a significant effect on the particle size of our coating suspensions to the detriment of the optical performance. We require particle sizes less than 20 nm to avoid light loss due to scatter and contaminated TEOS gave suspensions with much higher particle sizes. Oxidation products were identified by GC mass spectroscopy and included acetaldehyde, acetic acid, silicon acetates and reaction products of these compounds with ethanol. Acetic acid and silicon acetates were found to be the major cause of large particle formation. These could be removed by careful redistillation preferably in the presence of a small quantity of magnesium ethoxide. Storage in sealed containers over N{sub 2} avoided further problems.
Date: June 25, 1997
Creator: Thomas, I. M.
Partner: UNT Libraries Government Documents Department

Nano-scale materials

Description: This is the final report of a three-year, Laboratory Directed Research and Development (LDRD) project at the Los Alamos National Laboratory (LANL). Highly selective, alumina-supported molybdenum carbonitrides were prepared by solution impregnation using the metal amide Mo{sub 2}(N(CH{sub 3}){sub 2}){sub 6} as a molecular precursor. On the basis of relative weight percents, these materials demonstrate a 5- to 8-fold increase in catalytic activity over similar materials prepared by traditional solid-state approaches. The catalytic activities of these materials are very dependent upon the type of alumina support used. Impregnation of Mo{sub m}C{sub x}N{sub y} into preformed alumina pellets resulted in a material that specifically isomerized n-heptane into equal amounts of 2- and 3-methylhexanes, as well as iso-butane. No evidence of aromatic products was observed at operating temperatures below 420{degrees}C. The product selectivity of the isomers was 56% at a n-heptane conversion efficiency of 57%. Impregnating Mo{sub m}C{sub x}N{sub y} into an alumina powder resulted in an extremely selective aromatized and dehydrogenated material. The products from this material consist only of aromatics and n-heptenes with less than 2% isomerization or cracking products.
Date: December 31, 1998
Creator: Barrera, J.; Smith, D.C. & Devlin, D.J.
Partner: UNT Libraries Government Documents Department

Atom transfer and rearrangement reactions catalyzed by methyltrioxorhenium, MTO

Description: Methyltrioxorhenium (MTO) catalyzes the desulfurization of thiiranes by triphenylphosphine. Enormous enhancement in rate is observed when the catalyst is pretreated with hydrogen sulfide prior to the reaction. Using 2-mercaptomethylthiophenol as a ligand, the author synthesized several model complexes to study the mechanism of this reaction. With suitable model systems, they were able to show that the active catalyst is a Re(V) species. The reactions are highly stereospecific and very tolerant to functional groups. As part of the studies, he synthesized and crystallographically characterized the first examples of neutral terminal and bridging Re(V)sulfidocomplexes. Some of these complexes undergo fast oxygen atom transfer reactions with organic and inorganic oxidants. Studies on these model complexes led them to the discovery that MTO catalyzes the selective oxidation of thiols to disulfides. This report contains the Introduction; ``Chapter 6: Isomerization of Propargylic Alcohols to Enones and Enals Catalyzed by Methylrhenium Trioxide``; and Conclusions.
Date: May 10, 1999
Creator: Jacob, J.
Partner: UNT Libraries Government Documents Department

Method of Dehalogenation using Diamonds

Description: A method for preparing olefins and halogenated olefins is provided comprising contacting halogenated compounds with diamonds for a sufficient time and at a sufficient temperature to convert the halogenated compounds to olefins and halogenated olefins via elimination reactions.
Date: February 26, 1999
Creator: Farcasiu, Malvina; Kaufman, Phillip B.; Ladner, Edward P. & Anderson, Richard R.
Partner: UNT Libraries Government Documents Department

Cu(II) - Catalyzed Hydrazine Reduction of Ferrous Nitrate

Description: This report discusses the results of a study of catalyzed hydrazine reduction of ferrous nitrate. It is apparent that there is a substantial reaction between hydrazine and nitrate ion (or nitric acid) to produce HN3 during both the reduction of Fe(III) and during storage at room temperature.
Date: October 15, 2001
Creator: Karraker, D.G.
Partner: UNT Libraries Government Documents Department