Design and Synthesis of Copper–Cobalt Catalysts for the Selective Conversion of Synthesis Gas to Ethanol and Higher Alcohols |
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| Authors: | Dr Gonzalo Prieto Steven Beijer Dr Miranda L Smith Dr Ming He Yuen Au Zi Wang Prof David A Bruce Prof Krijn P de Jong Prof James J Spivey Prof Petra E de Jongh |
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| Affiliation: | 1. Inorganic Chemistry and Catalysis, Debye Institute for Nanomaterials Science, Utrecht University, 3584 CG, Utrecht (The Netherlands);2. Cain Department of Chemical Engineering, Lousiana State University, Baton Rouge, LA 70803 (USA);3. Department of Chemical and Biomolecular Engineering, Clemson University, Clemson, SC 29634 (USA) |
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| Abstract: | Combining quantum‐mechanical simulations and synthesis tools allows the design of highly efficient CuCo/MoOx catalysts for the selective conversion of synthesis gas (CO+H2) 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 temperature‐resolved 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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| Keywords: | alloy nanoparticles CO hydrogenation heterogeneous catalysis high alcohols supported catalysts |
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