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

Authors
Kim, HaesolShin, DongyupYang, WoojinWon, Da HyeOh, Hyung-SukChung, Min WookJeong, DonghyukKim, Sun HeeChae, Keun HwaRyu, Ji YeonLee, JunseongCho, Sung JuneSeo, JiwonKim, HyungjunChoi, Chang Hyuck
Issue Date
2021-01-20
Publisher
AMER CHEMICAL SOC
Citation
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, v.143, no.2, pp.925 - 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-N-4 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 (N-4-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 Ni-I. 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.
Keywords
CARBON-DIOXIDE; NICKEL-COMPLEXES; STRUCTURAL CHARACTERIZATION; ELECTROCATALYTIC REDUCTION; SELECTIVE CONVERSION; EFFICIENT CO2; ELECTROREDUCTION; ELECTRODES; CATALYSTS; GRAPHENE; CARBON-DIOXIDE; NICKEL-COMPLEXES; STRUCTURAL CHARACTERIZATION; ELECTROCATALYTIC REDUCTION; SELECTIVE CONVERSION; EFFICIENT CO2; ELECTROREDUCTION; ELECTRODES; CATALYSTS; GRAPHENE; CO2 reduction reaction (CO2RR); Single atom catalyst (SAC); Ni-N-C
ISSN
0002-7863
URI
https://pubs.kist.re.kr/handle/201004/117510
DOI
10.1021/jacs.0c11008
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KIST Article > 2021
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