期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 53, 期 25, 页码 6397-6401出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201402680
关键词
alloy nanoparticles; CO hydrogenation; heterogeneous catalysis; high alcohols; supported catalysts
资金
- Center for Atomic-Level Catalyst Design, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001058]
Combining quantum-mechanical simulations and synthesis tools allows the design of highly efficient CuCo/MoOx catalysts for the selective conversion of synthesis gas (CO + H-2) into ethanol and higher alcohols, which are of eminent interest for the production of platform chemicals from non-petroleum feedstocks. Density functional theory calculations coupled to microkinetic models identify mixed Cu-Co alloy sites, at Co-enriched surfaces, as ideal for the selective production of long-chain alcohols. Accordingly, a versatile synthesis route is developed based on metal nanoparticle exsolution from a molybdate precursor compound whose crystalline structure isomorphically accommodates Cu2+ and Co2+ cations in a wide range of compositions. As revealed by energy-dispersive X-ray nanospectroscopy and temperaturere-solved X-ray diffraction, superior mixing of Cu and Co species promotes formation of CuCo alloy nanocrystals after activation, leading to two orders of magnitude higher yield to high alcohols than a benchmark CuCoCr catalyst. Substantiating simulations, the yield to high alcohols is maximized in parallel to the CuCo alloy contribution, for Co-rich surface compositions, for which Cu phase segregation is prevented.
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