Identification of Single-Atom Ni Site Active toward Electrochemical CO2 Conversion to CO

Title
Identification of Single-Atom Ni Site Active toward Electrochemical CO2 Conversion to CO
Authors
채근화오형석원다혜김해솔신동엽양우진정민욱정동혁김선희류지연이준성조성준서지원김형준최창혁
Keywords
CO2 reduction reaction (CO2RR); Single atom catalyst (SAC); Ni-N-C
Issue Date
2021-01
Publisher
Journal of the American Chemical Society
Citation
VOL 143-933
Abstract
Electrocatalytic conversion of CO2 into value-added products offers a new paradigm for a sustainable carbon economy. For active CO2 electrolysis, the single-atom Ni catalyst has been proposed as promising from experiments, but an idealized Ni?N4 site shows an unfavorable energetics from theory, leading to many debates on the chemical nature responsible for high activity. To resolve this conundrum, here we investigated CO2 electrolysis of Ni sites with well-defined coordination, tetraphenylporphyrin (N4?TPP) and 21-oxatetraphenylporphyrin (N3O?TPP). Advanced spectroscopic and computational studies revealed that the broken ligand-field symmetry is the key for active CO2 electrolysis, which subordinates an increase in the Ni redox potential yielding NiI. Along with their importance in activity, ligand-field symmetry and strength are directly related to the stability of the Ni center. This suggests the next quest for an activity?stability map in the domain of ligand-field strength, toward a rational ligand-field engineering of single-atom Ni catalysts for efficient CO2 electrolysis.
URI
http://pubs.kist.re.kr/handle/201004/72825
ISSN
0002-7863
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KIST Publication > Article
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