期刊
ACS CATALYSIS
卷 5, 期 3, 页码 1717-1725出版社
AMER CHEMICAL SOC
DOI: 10.1021/cs501656x
关键词
CO2 hydrogenation; low temperature; methanol synthesis; cascade catalysis; heterogeneous catalysis; Mo2C-based catalysts; Cu-based catalysts; reaction pathways
资金
- National Science Foundation, under the CCI Center for Enabling New Technologies through Catalysis (CENTC) Phase II Renewal [CHE-1205189]
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [1205189] Funding Source: National Science Foundation
Research described in this paper targeted a cascade system for the hydrogenation of CO2 to methanol via formic acid and/or formate intermediates, a reaction sequence that has been accomplished previously using homogeneous catalysts. On the basis of results for the hydrogenation of CO2, formic acid, and ethyl formate over a series of Cu- and Mo2C-based catalysts, we selected a Cu chromite catalyst for CO2 hydrogenation to the formate and a Cu/Mo2C catalyst to convert the formate to methanol. These catalysts worked cooperatively in the presence of ethanol, yielding a methanol turnover frequency of 4.7 x 10(-4) s(-1) at 135 degrees C, 10 bar of CO2, and 30 bar of H-2 in 1,4-dioxane. The performance for this Cu chromite:Cu/Mo2C cascade system surpassed the additive production of the individual catalysts by similar to 60%. The results also allowed an investigation of the reaction pathways. The hydrogenation of CO2 to formic acid appeared to be the rate-limiting step for most of the catalysts. This is not surprising given the thermodynamics for this reaction. Finally, the hydrogenation of CO2 to dimethyl ether was also demonstrated using a system consisting of the Cu/Mo2C catalyst to produce methanol from CO2 and HZSM-5 to produce dimethyl ether from methanol. The systems described in this paper are, to our knowledge, the first demonstrating cascade CO2 hydrogenation via heterogeneous catalysts.
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