Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 58, Issue 44, Pages 15834-15840Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201909069
Keywords
carbene ligands; CO2 reduction; electrocatalysis; metal nanoparticles; polymeric ligands
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Funding
- ACS Petroleum Research Fund
- University of Connecticut
- Jiangsu Specially Appointed Professor plan
- Natural Science Foundation of Jiangsu Province [BK20180723]
- Priority Academic Program Development of Jiangsu Higher Education Institutions
- National and Local Joint Engineering Research Center of Biomedical Functional Materials
- Green Emulsions Micelles and Surfactants (GEMS) Center, UCONN
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The stability of metal nanocatalysts for electrocatalytic CO2 reduction is of key importance for practical application. We report the use of two polymeric N-heterocyclic carbenes (NHC) (polydentate and monodentate) to stabilize metal nanocatalysts (Au and Pd) for efficient CO2 electroreduction. Compared with other conventional ligands including thiols and amines, metal-carbene bonds that are stable under reductive potentials prevent the nanoclustering of nanoparticles. Au nanocatalysts modified by polymeric NHC ligands show an activity retention of 86 % after CO2 reduction at -0.9 V for 11 h, while it is less than 10 % for unmodified Au. We demonstrate that the hydrophobicity of polymer ligands and the enriched surface electron density of metal NPs through sigma-donation of NHCs substantially improve the selectivity for CO2 reduction over proton.
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