Chelating N-Heterocyclic Carbene Ligands Enable Tuning of Electrocatalytic CO2 Reduction to Formate and Carbon Monoxide: Surface Organometallic Chemistry.
- 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 Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir Prelog Weg 1-5, 8093, Zürich, Switzerland.
- Gao R Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan, Shanxi, 030001, China.
- Gong M Department of Chemistry, University of California, Berkeley, CA, 94720, USA.
- Nichols EM Department of Chemistry, University of California, Berkeley, CA, 94720, USA.
- Smith PT Department of Chemistry, University of California, Berkeley, CA, 94720, USA.
- Liu X Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan, Shanxi, 030001, China.
- Wen X Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan, Shanxi, 030001, China.
- Copéret C Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir Prelog Weg 1-5, 8093, Zürich, Switzerland.
- Chang CJ Department of Chemistry, University of California, Berkeley, CA, 94720, USA.
- 2018-03-03
Published in:
- Angewandte Chemie (International ed. in English). - 2018
English
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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- English
- Open access status
- hybrid
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- DOI 10.1002/anie.201800367
- PMID 29498168
- Persistent URL
- https://sonar.ch/global/documents/64820
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