An Iron Pyridyl-Carbene Electrocatalyst for Low Overpotential CO2 Reduction to CO
comunitat-uji-handle:10234/9
comunitat-uji-handle2:10234/7053
comunitat-uji-handle3:10234/8639
comunitat-uji-handle4:
INVESTIGACIONMetadata
Title
An Iron Pyridyl-Carbene Electrocatalyst for Low Overpotential CO2 Reduction to CODate
2021-04-15Publisher
American Chemical SocietyISSN
2155-5435Bibliographic citation
Sergio Gonell, Julio Lloret-Fillol, and Alexander J. M. Miller. An Iron Pyridyl-Carbene Electrocatalyst for Low Overpotential CO2 Reduction to CO. ACS Catalysis 2021 11 (2), 615-626 DOI: 10.1021/acscatal.0c03798Type
info:eu-repo/semantics/articlePublisher version
https://pubs.acs.org/doi/10.1021/acscatal.0c03798Version
info:eu-repo/semantics/submittedVersionSubject
Abstract
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 ... [+]
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-methyl-benzimidazol-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. [-]
Is part of
ACS Catalysis, 2020, vol. 11, no 2Funder Name
Alliance for Molecular PhotoElectrode Design for Solar Fuels (AMPED) | U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences | National Science Foundation | European Commission | Ministerio de Ciencia, Innovación y Universidades | Horizon 2020
Project code
DE-SC0001011 | CHE-1726291 | ERC-CG-2014-648304 | CTQ2016-80038-R | 794119
Grant URL
Info:eu-repo/granAgreement/EC/H2020/794119
Rights
Copyright © American Chemical Society
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info:eu-repo/semantics/openAccess
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