CO<sub>2</sub>‐to‐Methanol Hydrogenation on Zirconia‐Supported Copper Nanoparticles: Reaction Intermediates and the Role of the Metal–Support Interface

DOI Web Site Web Site 被引用文献2件
  • Kim Larmier
    Department of Chemistry and Applied Biosciences ETH Zürich Vladimir-Prelog Weg 1–5 8093 Zürich Switzerland
  • Wei‐Chih Liao
    Department of Chemistry and Applied Biosciences ETH Zürich Vladimir-Prelog Weg 1–5 8093 Zürich Switzerland
  • Shohei Tada
    Department of Chemistry and Applied Biosciences ETH Zürich Vladimir-Prelog Weg 1–5 8093 Zürich Switzerland
  • Erwin Lam
    Department of Chemistry and Applied Biosciences ETH Zürich Vladimir-Prelog Weg 1–5 8093 Zürich Switzerland
  • René Verel
    Department of Chemistry and Applied Biosciences ETH Zürich Vladimir-Prelog Weg 1–5 8093 Zürich Switzerland
  • Atul Bansode
    Institute of Chemical Research of Catalonia (ICIQ) The Barcelona Institute of Science and Technology Av. Països Catalans 16 43007 Tarragona Spain
  • Atsushi Urakawa
    Institute of Chemical Research of Catalonia (ICIQ) The Barcelona Institute of Science and Technology Av. Països Catalans 16 43007 Tarragona Spain
  • Aleix Comas‐Vives
    Department of Chemistry and Applied Biosciences ETH Zürich Vladimir-Prelog Weg 1–5 8093 Zürich Switzerland
  • Christophe Copéret
    Department of Chemistry and Applied Biosciences ETH Zürich Vladimir-Prelog Weg 1–5 8093 Zürich Switzerland

書誌事項

公開日
2017-02-14
権利情報
  • http://onlinelibrary.wiley.com/termsAndConditions#vor
DOI
  • 10.1002/ange.201610166
公開者
Wiley

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説明

<jats:title>Abstract</jats:title><jats:p>Methanol synthesis by CO<jats:sub>2</jats:sub> hydrogenation is a key process in a methanol‐based economy. This reaction is catalyzed by supported copper nanoparticles and displays strong support or promoter effects. Zirconia is known to enhance both the methanol production rate and the selectivity. Nevertheless, the origin of this observation and the reaction mechanisms associated with the conversion of CO<jats:sub>2</jats:sub> to methanol still remain unknown. A mechanistic study of the hydrogenation of CO<jats:sub>2</jats:sub> on Cu/ZrO<jats:sub>2</jats:sub> is presented. Using kinetics, in situ IR and NMR spectroscopies, and isotopic labeling strategies, surface intermediates evolved during CO<jats:sub>2</jats:sub> hydrogenation were observed at different pressures. Combined with DFT calculations, it is shown that a formate species is the reaction intermediate and that the zirconia/copper interface is crucial for the conversion of this intermediate to methanol.</jats:p>

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