期刊
ACS CATALYSIS
卷 11, 期 2, 页码 615-626出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.0c03798
关键词
CO2 reduction; electrocatalysis; iron; mechanistic studies; hemilability; carbene ligand
资金
- Alliance for Molecular PhotoElectrode Design for Solar Fuels (AMPED), an Energy Frontier Research Center (EFRC) - U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001011]
- National Science Foundation [CHE-1726291]
- European Commission [ERC-CG-2014-648304]
- Spanish Ministry of Science [CTQ2016-80038-R]
- EU [794119]
- Marie Curie Actions (MSCA) [794119] Funding Source: Marie Curie Actions (MSCA)
The newly synthesized nonheme iron electrocatalyst shows high selectivity and efficiency in converting CO2 to CO at low overpotentials, promising a wide range of applications. By studying the nature of catalytic intermediates and optimizing continuous CO2 flow conditions, the performance of the catalyst can be improved and the product yield increased.
Electrocatalysts for CO2 reduction based on first-row transition metal ions have attracted attention as abundant and affordable candidates for energy conversion applications. Yet very few molecular iron electrocatalysts exhibit high selectivity for CO. Iron complexes supported by a redox-active 2,2':6',2 ''-terpyridine (tpy) ligand and a strong trans effect pyridyl-N-heterocyclic carbene ligand (1-methylbenzimidazol-2-ylidene-3-(2-pyridine)) were synthesized and found to catalyze the selective electroreduction of CO2 to CO at very low overpotentials. Mechanistic studies using electrochemical and computational methods provided insights into the nature of catalytic intermediates that guided the development of continuous CO2 flow conditions that improved the performance, producing CO with >95% Faradaic efficiency at an overpotential of only 150 mV. The studies reveal general design principles for nonheme iron electrocatalysts, including the importance of lability and geometric isomerization, that can serve to guide future developments in the design of affordable and efficient catalysts for CO2 electroreduction.
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