An Iron Bis(carbene) Catalyst for Low Overpotential CO2 Electroreduction to CO: Mechanistic Insights from Kinetic Zone Diagrams, Spectroscopy, and Theory
Ver/ Abrir
Impacto
Scholar |
Otros documentos de la autoría: Gonell, Sergio; Assaf, Eric A.; Lloret Fillol, Julio; Miller, Alexander
Metadatos
Mostrar el registro completo del ítemcomunitat-uji-handle:10234/9
comunitat-uji-handle2:10234/160292
comunitat-uji-handle3:10234/160293
comunitat-uji-handle4:
INVESTIGACIONMetadatos
Título
An Iron Bis(carbene) Catalyst for Low Overpotential CO2 Electroreduction to CO: Mechanistic Insights from Kinetic Zone Diagrams, Spectroscopy, and TheoryFecha de publicación
2021-12-08Editor
American Chemical SocietyISSN
2155-5435Cita bibliográfica
Gonell, S.; Assaf, E. A.; Lloret-Fillol, J.; Miller, A. J. M. An Iron Bis(carbene) Catalyst for Low Overpotential CO2 Electroreduction to CO: Mechanistic Insights from Kinetic Zone Diagrams, Spectroscopy, and Theory. ACS Catal. 2021, 11 (24), 15212–15222. DOI: 10.1021/acscatal.1c04414Tipo de documento
info:eu-repo/semantics/articleVersión de la editorial
https://pubs.acs.org/doi/abs/10.1021/acscatal.1c04414Versión
info:eu-repo/semantics/submittedVersionPalabras clave / Materias
Resumen
A common challenge in molecular electrocatalysis is the relationship between maximum activity and the overpotential required to reach that rate, with faster catalysts incurring higher overpotentials. This work follows ... [+]
A common challenge in molecular electrocatalysis is the relationship between maximum activity and the overpotential required to reach that rate, with faster catalysts incurring higher overpotentials. This work follows a strategy based on independent tuning of ligands in the primary coordination sphere to discover a previously unreported iron catalyst for CO2 reduction with higher activity than similar complexes while maintaining the same overpotential. Iron complexes bearing a bis-N-heterocyclic carbene ligand (methylenebis(N-methylimidazol-2-ylidene), bis-mim) and a redox active 2,2′:6′,2″-terpyridine (tpy) ligand were synthesized and found to catalyze the selective reduction of CO2 to CO at low overpotential with water as the proton source. Mechanistic studies based on kinetic zone diagrams, spectroscopy, and computation enable comparisons with a previously studied pyridyl–carbene analogue. Changing the bidentate ligand donor ability accelerates catalysis at the same overpotential and changes the nature of the turnover-limiting step of the reaction. [-]
Publicado en
ACS Catalysis, 2021, vol. 11, no 24Entidad financiadora
United States Department of Energy (DOE) | National Science Foundation (NSF) | European Commission | Ministerio de Ciencia, Innovación y Universidades | EU for Horizon 2020 Marie Skłodowska-Curie Fellowship
Código del proyecto o subvención
DE-SC0001011 | CHE-1726291 | ERC-CoG-2015-64830 | MICIU/ICTI2017-2020/PID2019-110050RB-I00 | 794119
Derechos de acceso
Copyright © American Chemical Society
http://rightsstatements.org/vocab/CNE/1.0/
info:eu-repo/semantics/openAccess
http://rightsstatements.org/vocab/CNE/1.0/
info:eu-repo/semantics/openAccess
Aparece en las colecciones
- INAM_Articles [528]