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Accessing and Photo-Accelerating Low-Overpotential Pathways for CO2 Reduction: A Bis-Carbene Ruthenium Terpyridine Catalyst
dc.contributor.author | Assaf, Eric A. | |
dc.contributor.author | Gonell, Sergio | |
dc.contributor.author | Chen, Chun-Hsing | |
dc.contributor.author | Miller, Alexander | |
dc.date.accessioned | 2023-05-09T09:23:43Z | |
dc.date.available | 2023-05-09T09:23:43Z | |
dc.date.issued | 2022-10-21 | |
dc.identifier.citation | Assaf, E. A.; Gonell, S.; Chen, C. H.; Miller, A. J. Accessing and Photo-Accelerating Low-Overpotential Pathways for CO2 Reduction: A Bis-Carbene Ruthenium Terpyridine Catalyst. ACS Catal. 2022, 12, 20, 12596-12606. DOI: 10.1021/acscatal.2c03651 | ca_CA |
dc.identifier.issn | 2155-5435 | |
dc.identifier.uri | http://hdl.handle.net/10234/202437 | |
dc.description.abstract | A ruthenium catalyst bearing a bidentate bis(carbene) ligand is prepared and studied as a catalyst for CO2 electroreduction. The catalyst [Ru(tpy)(bis-mim)(MeCN)][PF6]2 (tpy) is 2,2′,:6′,2″-terpyridine; bis-mim is (methylenebis(N-methylimidazol-2-ylidene)) mediates reduction of CO2 into CO with a turnover frequency of 630 s–1 and Faradaic efficiency (FE) of 30% at an overpotential of 730 mV. The strongly donating bis(carbene) ligand also enables access to a pathway operating at a lower overpotential of ca. 310 mV. While low-overpotential catalysis is slow in the dark (TOF = 0.01 s–1), visible light illumination increases the rate 10-fold (TOF = 0.11 s–1). A full mechanistic picture is developed using kinetic analysis from cyclic voltammetry, spectroelectrochemistry, and computational methods, with the bis-mim ligand facilitating rapid CO2 activation at low overpotentials. Comparisons with other ruthenium catalysts yield insight into the ability to tune the rate of chemical steps (e.g., ligand dissociation and CO2 nucleophilic attack) and the overpotential by tailoring the primary coordination sphere while retaining the “redox-active” tpy ligand. | ca_CA |
dc.format.extent | 11 p. | ca_CA |
dc.format.mimetype | application/pdf | ca_CA |
dc.language.iso | eng | ca_CA |
dc.publisher | American Chemical Society | ca_CA |
dc.relation.isPartOf | Catalyst. ACS Catalysis, 2022, vol. 12, no 20 | ca_CA |
dc.rights | Copyright © American Chemical Society | ca_CA |
dc.rights.uri | http://rightsstatements.org/vocab/CNE/1.0/ | ca_CA |
dc.subject | CO2 reduction | ca_CA |
dc.subject | electroreduction | ca_CA |
dc.subject | ruthenium | ca_CA |
dc.subject | mechanistic studies | ca_CA |
dc.subject | carbene ligand | ca_CA |
dc.subject | photoelectrocatalysis | ca_CA |
dc.title | Accessing and Photo-Accelerating Low-Overpotential Pathways for CO2 Reduction: A Bis-Carbene Ruthenium Terpyridine Catalyst | ca_CA |
dc.type | info:eu-repo/semantics/article | ca_CA |
dc.identifier.doi | https://doi.org/10.1021/acscatal.2c03651 | |
dc.rights.accessRights | info:eu-repo/semantics/restrictedAccess | ca_CA |
dc.relation.publisherVersion | https://pubs.acs.org/doi/full/10.1021/acscatal.2c03651 | ca_CA |
dc.description.sponsorship | This work was primarily supported by the Center for Hybrid Approaches in Solar Fuels (CHASE), an Energy Innovation Hub funded by the US Department of Energy, Office of Science, Office of Basic Energy Sciences under award number DE-SC0021173 (electrochemical and photoelectrochemical measurements, computational calculations, and data analysis) and by the Alliance for Molecular PhotoElectrode Design for Solar Fuels (AMPED), an Energy Frontier Research Center (EFRC) funded by the US Department of Energy, Office of Science, Office of Basic Energy Science under award number DE-SC0001011 (synthesis and characterization of complexes). Henry M. Dodge assisted with crystallographic data collection. The authors acknowledge the University of North Carolina’s Department of Chemistry NMR Core Laboratory, with work supported by the National Science Foundation under Grant No. CHE-1828183. The University of North Carolina’s Mass Spectrometry Core Laboratory is acknowledged, with work supported by the National Science Foundation under Grant No. CHE-1726291. | |
dc.type.version | info:eu-repo/semantics/publishedVersion | ca_CA |
project.funder.name | United States Department of Energy (DOE) | ca_CA |
project.funder.name | National Science Foundation (NSF) | ca_CA |
oaire.awardNumber | DE-SC0021173 | ca_CA |
oaire.awardNumber | DE-SC0001011 | ca_CA |
oaire.awardNumber | CHE-1828183 | ca_CA |
oaire.awardNumber | CHE-1726291 | ca_CA |
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