Identification of Single-Atom Ni Site Active toward Electrochemical CO2 Conversion to CO
- Identification of Single-Atom Ni Site Active toward Electrochemical CO2 Conversion to CO
- 채근화; 오형석; 원다혜; 김해솔; 신동엽; 양우진; 정민욱; 정동혁; 김선희; 류지연; 이준성; 조성준; 서지원; 김형준; 최창혁
- CO2 reduction reaction (CO2RR); Single atom catalyst (SAC); Ni-N-C
- Issue Date
- Journal of the American Chemical Society
- VOL 143-933
- 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.
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