Chelating N‐Heterocyclic Carbene Ligands Enable Tuning of Electrocatalytic CO 2 Reduction to Formate and Carbon Monoxide: Surface Organometallic Chemistry
Abstract
Abstract Reported here is the chelate effect as a design principle for tuning heterogeneous catalysts for electrochemical CO 2 reduction. Palladium functionalized with a chelating tris‐N‐heterocyclic carbene (NHC) ligand (Pd‐timtmb Me ) exhibits a 32‐fold increase in activity for electrochemical reduction of CO 2 to C1 products with high Faradaic efficiency (FE C1 =86 %) compared to the parent unfunctionalized Pd foil (FE=23 %), and with sustained activity relative to a monodentate NHC‐ligated Pd electrode (Pd‐mimtmb Me ). The results highlight the contributions of the chelate effect for tailoring and maintaining reactivity at molecular‐materials interfaces enabled by surface organometallic chemistry.
- Authors:
-
- Department of Chemistry University of California Berkeley CA 94720 USA
- Department of Chemistry University of California Berkeley CA 94720 USA, Chemical Sciences Division Lawrence Berkeley National Laboratory Berkeley CA 94720 USA
- Department of Chemistry and Applied Biosciences ETH Zürich Vladimir Prelog Weg 1–5 8093 Zürich Switzerland
- Institute of Coal Chemistry Chinese Academy of Sciences Taiyuan Shanxi 030001 China, Synfuels China Beijing 100195 China
- Department of Chemistry University of California Berkeley CA 94720 USA, Department of Molecular and Cell Biology Howard Hughes Medical Institute University of California Berkeley CA 94720 USA, Chemical Sciences Division Lawrence Berkeley National Laboratory Berkeley CA 94720 USA
- Publication Date:
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1429155
- Grant/Contract Number:
- 101528-002
- Resource Type:
- Publisher's Accepted Manuscript
- Journal Name:
- Angewandte Chemie
- Additional Journal Information:
- Journal Name: Angewandte Chemie Journal Volume: 130 Journal Issue: 18; Journal ID: ISSN 0044-8249
- Publisher:
- Wiley Blackwell (John Wiley & Sons)
- Country of Publication:
- Germany
- Language:
- English
Citation Formats
Cao, Zhi, Derrick, Jeffrey S., Xu, Jun, Gao, Rui, Gong, Ming, Nichols, Eva M., Smith, Peter T., Liu, Xingwu, Wen, Xiaodong, Copéret, Christophe, and Chang, Christopher J. Chelating N‐Heterocyclic Carbene Ligands Enable Tuning of Electrocatalytic CO 2 Reduction to Formate and Carbon Monoxide: Surface Organometallic Chemistry. Germany: N. p., 2018.
Web. doi:10.1002/ange.201800367.
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. Chelating N‐Heterocyclic Carbene Ligands Enable Tuning of Electrocatalytic CO 2 Reduction to Formate and Carbon Monoxide: Surface Organometallic Chemistry. Germany. https://doi.org/10.1002/ange.201800367
Cao, Zhi, Derrick, Jeffrey S., Xu, Jun, Gao, Rui, Gong, Ming, Nichols, Eva M., Smith, Peter T., Liu, Xingwu, Wen, Xiaodong, Copéret, Christophe, and Chang, Christopher J. Fri .
"Chelating N‐Heterocyclic Carbene Ligands Enable Tuning of Electrocatalytic CO 2 Reduction to Formate and Carbon Monoxide: Surface Organometallic Chemistry". Germany. https://doi.org/10.1002/ange.201800367.
@article{osti_1429155,
title = {Chelating N‐Heterocyclic Carbene Ligands Enable Tuning of Electrocatalytic CO 2 Reduction to Formate and Carbon Monoxide: Surface Organometallic Chemistry},
author = {Cao, Zhi and Derrick, Jeffrey S. and Xu, Jun and Gao, Rui and Gong, Ming and Nichols, Eva M. and Smith, Peter T. and Liu, Xingwu and Wen, Xiaodong and Copéret, Christophe and Chang, Christopher J.},
abstractNote = {Abstract Reported here is the chelate effect as a design principle for tuning heterogeneous catalysts for electrochemical CO 2 reduction. Palladium functionalized with a chelating tris‐N‐heterocyclic carbene (NHC) ligand (Pd‐timtmb Me ) exhibits a 32‐fold increase in activity for electrochemical reduction of CO 2 to C1 products with high Faradaic efficiency (FE C1 =86 %) compared to the parent unfunctionalized Pd foil (FE=23 %), and with sustained activity relative to a monodentate NHC‐ligated Pd electrode (Pd‐mimtmb Me ). The results highlight the contributions of the chelate effect for tailoring and maintaining reactivity at molecular‐materials interfaces enabled by surface organometallic chemistry.},
doi = {10.1002/ange.201800367},
journal = {Angewandte Chemie},
number = 18,
volume = 130,
place = {Germany},
year = {Fri Mar 23 00:00:00 EDT 2018},
month = {Fri Mar 23 00:00:00 EDT 2018}
}
https://doi.org/10.1002/ange.201800367
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