Development of Vanadium-phosphate Catalysts for Methanol Production by Selective Oxidation of Methane. Quarterly Technical Progress Report 9, April-June, 1995 PDF Download
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This document is the ninth quarterly technical progress report under Contract No. DE-AC22-92PC92110 {open_quotes}Development of Vanadium-Phosphate Catalysts for Methanol Production by Selective Oxidation of Methane{close_quotes}. Activities were focused on fine tuning of the microreactor system by elimination of transport effects and improvements in the analytical system. Process variable studies were conducted on vanadyl pyrophosphate and screening studies were conducted on several modified catalyst. One additional catalyst was prepared and characterization studies continued. These results are reported.
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This document is the third quarterly technical progress report under Contract No. AC22-92PC92110, ''Development of Vanadium-Phosphate Catalysts for Methanol Production by Selective Oxidation of Methane.'' During this quarter, we have continued to develop methods for catalyst activation by investigating activation in wet gas environments. This procedure leads to the formation of highly crystalline (VO)2P2O--, while activation under identical conditions, but with no moisture, leads to a poorly crystalline sample. Published data indicate that the highly crystalline form is representative of commercial butane oxidation catalysts. The main focus of our work during this quarter has been in the area of catalyst testing in the microreactor system. In order to confirm that our microreactor system was providing reliable data, we tested a V2O5/SiO2 catalyst at atmospheric pressure and temperatures from 500 to 600°C using 90 to 95 percent CH4/O2. Several studies of methane oxidation using this catalyst have been published with reasonably good agreement between different research groups. We were not able to reproduce the literature data using steel reactors. However, when the steel reactor was lined with quartz and the postcatalyst reactor volume was minimized by packing with quartz chips, we obtained results which agree closely with those previously published. Using the same quartz reactor and test conditions, we also tested a highly crystalline (wet activated) VPO catalyst.
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This document is the thirteenth quarterly technical progress report under Contract No. DE-AC22-92PC92110 {open_quotes}Development of Vanadium-Phosphate Catalysts for Methanol Production by Selective Oxidation of Methane{close_quotes} and covers the period April-June 1996. The basic premise of this project is that vanadyl pyrophosphate (VPO), a catalyst used commercially in the selective oxidation of butane to maleic anhydride, can be developed as a catalyst for selective methane oxidation. Data supporting this idea include published reports indicating moderate to high selectivity in oxidation of ethane, propane, and pentane, as well as butane. Methane oxidation is a much more difficult reaction to catalyze than that of other alkanes and it is expected that considerable modification of vanadyl pyrophosphate will be required for this application. It is well known that VPO can be modified extensively with a large number of different promoters and in particular that promoters can enhance selectivity and lower the temperature required for butane conversion.
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This document is the tenth quarterly technical progress report under Contract No. DE-AC22-92PC92110 {open_quotes}Development of Vanadium-Phosphate Catalysts for Methanol Production by Selective Oxidation of Methane{close_quotes}. Activities focused on testing of additional modified and promoted catalysts and characterization of these materials. Attempts at improving the sensitivity of our GC based analytical systems were also made with some success. Methanol oxidation studies were initiated. These results are reported. Specific accomplishments include: (1) Methane oxidation testing of a suite of catalysts promoted with most of the first row transition metals was completed. Several of these materials produced low, difficult to quantify yields of formaldehyde. (2) Characterization of these materials by XRD and FTIR was performed with the goal of correlating activity and selectivity with catalyst properties. (3) We began to characterize catalysts prepared via modified synthesis methods designed to enhance acidity using TGA measurements of acetonitrile chemisorption and methanol dehydration to dimethyl ether as a test reaction. (4) A catalyst prepared in the presence of naphthalene methanol as a structural disrupter was tested for activity in methane oxidation. It was found that this material produced low yields of formaldehyde which were difficult to quantify. (5) Preparation of catalysts with no Bronsted acid sites. This was accomplished by replacement of exchangeable protons with potassium, and (6) Methanol oxidation studies were initiated to provide an indication of catalyst activity for decomposition of this desired product and as a method of characterizing the catalyst surface.
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During the second quarter, we initiated Task 2 (Process and Catalyst Variable Study). This task involves an investigation of methods for vanadium phosphate (VPO) catalyst synthesis and activation as well as detailed testing of the catalysts produced for activity and selectivity in methane selective oxidation. As we initiated work on Task 2, three problem areas were identified: Preparation of catalysts with P:V ratio greater than 1. Activation of the precursor to produce the B-phase described in the patent literature. Achieving high (>95 percent) carbon balances in the bench-scale test unit. Each of these problems has been addressed and overcome during this quarter. Several catalysts with P:V ratios ranging from 0.95 to 1.1 have been prepared. Activation procedures are continuing to be investigated. We have found several procedures which yield catalysts having the desired X-ray diffraction pattern. The reactor system was modified and analytical procedures improved so that in a 7-day run using V2O5 as the catalyst, carbon balances ranged from 95 to 105 percent.
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Pages : 94
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Martin Huber, son of Henry Huber and Maria Wenger, married Annie Wenger (b. 1799). They had four children. After Martin's death, Annie married John Gayman. They had five children. They lived in Pennsylvania. Includes Bricker, Thrush and related families.
