Chelating N‐Heterocyclic Carbene Ligands Enable Tuning of Electrocatalytic CO<sub>2</sub> Reduction to Formate and Carbon Monoxide: Surface Organometallic Chemistry

  • Zhi Cao
    Department of Chemistry University of California Berkeley CA 94720 USA
  • Jeffrey S. Derrick
    Department of Chemistry University of California Berkeley CA 94720 USA
  • Jun Xu
    Department of Chemistry and Applied Biosciences ETH Zürich Vladimir Prelog Weg 1–5 8093 Zürich Switzerland
  • Rui Gao
    Institute of Coal Chemistry Chinese Academy of Sciences Taiyuan Shanxi 030001 China
  • Ming Gong
    Department of Chemistry University of California Berkeley CA 94720 USA
  • Eva M. Nichols
    Department of Chemistry University of California Berkeley CA 94720 USA
  • Peter T. Smith
    Department of Chemistry University of California Berkeley CA 94720 USA
  • Xingwu Liu
    Institute of Coal Chemistry Chinese Academy of Sciences Taiyuan Shanxi 030001 China
  • Xiaodong Wen
    Institute of Coal Chemistry Chinese Academy of Sciences Taiyuan Shanxi 030001 China
  • Christophe Copéret
    Department of Chemistry and Applied Biosciences ETH Zürich Vladimir Prelog Weg 1–5 8093 Zürich Switzerland
  • Christopher J. Chang
    Department of Chemistry University of California Berkeley CA 94720 USA

書誌事項

公開日
2018-03-23
権利情報
  • http://onlinelibrary.wiley.com/termsAndConditions#am
  • http://onlinelibrary.wiley.com/termsAndConditions#vor
DOI
  • 10.1002/anie.201800367
公開者
Wiley

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説明

<jats:title>Abstract</jats:title><jats:p>Reported here is the chelate effect as a design principle for tuning heterogeneous catalysts for electrochemical CO<jats:sub>2</jats:sub> reduction. Palladium functionalized with a chelating tris‐N‐heterocyclic carbene (NHC) ligand (Pd‐timtmb<jats:sup>Me</jats:sup>) exhibits a 32‐fold increase in activity for electrochemical reduction of CO<jats:sub>2</jats:sub> to C1 products with high Faradaic efficiency (FE<jats:sub>C1</jats:sub>=86 %) compared to the parent unfunctionalized Pd foil (FE=23 %), and with sustained activity relative to a monodentate NHC‐ligated Pd electrode (Pd‐mimtmb<jats:sup>Me</jats:sup>). The results highlight the contributions of the chelate effect for tailoring and maintaining reactivity at molecular‐materials interfaces enabled by surface organometallic chemistry.</jats:p>

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