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Activity and Selectivity Trends in Synthesis Gas Conversion to Higher Alcohols

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Abstract

Production of higher alcohols directly from synthesis gas is an attractive chemical process due to the high value of alcohols as fuel blends and the numerous possibilities for production of synthesis gas. Despite years of research the industrial viability of such a process is severely limited due to lack of suitable catalysts. In this work we contribute to an understanding why it has been difficult to find transition-metal higher alcohol catalysts, and point to possible strategies for discovering new active and selective catalysts. Our analysis is based on extensive density functional theory calculations to determine the energetics of ethanol formation on a series of metal (211) surfaces. The energetic information is used to construct a mean-field micro-kinetic model for the formation of ethanol via CHx–CO coupling. The kinetic model is used along with a descriptor-based analysis to gain insight into the fundamental factors determining activity and selectivity on transition-metal surfaces.

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Acknowledgments

Primary support by the U.S. Department of Energy (DOE), Office of Basic Energy Sciences to the SUNCAT Center for Interface Science and Catalysis is gratefully acknowledged (JKN, FS, FAP, ACL, AJM). In addition, AJM wishes to thank the Danish Ministry of Science, Technology and Innovation through the Catalysis for Sustainable Energy initiative, the Danish National Research Foundation and National Science Foundation through the Nordic Research Opportunity and Graduate Research Fellowship Program Grant No. DGE-1147470, and the Department of Defense (DoD) through the National Defense Science & Engineering Graduate Fellowship (NDSEG) Program.

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Authors and Affiliations

  1. Department of Chemical Engineering, Stanford University, Stanford, CA, 94305, USA

    Andrew J. Medford & Jens K. Nørskov

  2. SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA, 94025, USA

    Andrew J. Medford, Adam C. Lausche, Frank Abild-Pedersen, Jens K. Nørskov & Felix Studt

  3. Haldor Topsøe A/S, Nymøllevej 55, 2800, Kongens Lyngby, Denmark

    Burcin Temel & Niels C. Schjødt

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  1. Andrew J. Medford
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  2. Adam C. Lausche
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  7. Felix Studt
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Correspondence to Felix Studt.

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Medford, A.J., Lausche, A.C., Abild-Pedersen, F. et al. Activity and Selectivity Trends in Synthesis Gas Conversion to Higher Alcohols. Top Catal 57, 135–142 (2014). https://doi.org/10.1007/s11244-013-0169-0

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