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Chelating N-Heterocyclic Carbene Ligands Enable Tuning of Electrocatalytic CO2 Reduction to Formate and Carbon Monoxide: Surface Organometallic Chemistry.
Cao, Zhi; Derrick, Jeffrey S; Xu, Jun; Gao, Rui; Gong, Ming; Nichols, Eva M; Smith, Peter T; Liu, Xingwu; Wen, Xiaodong; Copéret, Christophe; Chang, Christopher J.
Afiliação
  • Cao Z; Department of Chemistry, University of California, Berkeley, CA, 94720, USA.
  • Derrick JS; Department of Chemistry, University of California, Berkeley, CA, 94720, USA.
  • Xu J; Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720, USA.
  • Gao R; Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir Prelog Weg 1-5, 8093, Zürich, Switzerland.
  • Gong M; Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan, Shanxi, 030001, China.
  • Nichols EM; Synfuels China, Beijing, 100195, China.
  • Smith PT; Department of Chemistry, University of California, Berkeley, CA, 94720, USA.
  • Liu X; Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720, USA.
  • Wen X; Department of Chemistry, University of California, Berkeley, CA, 94720, USA.
  • Copéret C; Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720, USA.
  • Chang CJ; Department of Chemistry, University of California, Berkeley, CA, 94720, USA.
Angew Chem Int Ed Engl ; 57(18): 4981-4985, 2018 04 23.
Article em En | MEDLINE | ID: mdl-29498168
ABSTRACT
Reported here is the chelate effect as a design principle for tuning heterogeneous catalysts for electrochemical CO2 reduction. Palladium functionalized with a chelating tris-N-heterocyclic carbene (NHC) ligand (Pd-timtmbMe ) exhibits a 32-fold increase in activity for electrochemical reduction of CO2 to C1 products with high Faradaic efficiency (FEC1 =86 %) compared to the parent unfunctionalized Pd foil (FE=23 %), and with sustained activity relative to a monodentate NHC-ligated Pd electrode (Pd-mimtmbMe ). The results highlight the contributions of the chelate effect for tailoring and maintaining reactivity at molecular-materials interfaces enabled by surface organometallic chemistry.
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Texto completo: 1 Base de dados: MEDLINE Idioma: En Revista: Angew Chem Int Ed Engl Ano de publicação: 2018 Tipo de documento: Article País de afiliação: Estados Unidos

Texto completo: 1 Base de dados: MEDLINE Idioma: En Revista: Angew Chem Int Ed Engl Ano de publicação: 2018 Tipo de documento: Article País de afiliação: Estados Unidos