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Direct Detection of Key Intermediates during the Product Release in Rhenium Bipyridine-Catalyzed CO2 Reduction Reaction
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.ORCID iD: 0000-0003-4759-0362
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.ORCID iD: 0000-0001-5732-1524
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.ORCID iD: 0000-0003-2246-1863
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.ORCID iD: 0000-0002-9933-9084
2024 (English)In: ACS Catalysis, E-ISSN 2155-5435, Vol. 14, no 21, p. 16324-16334Article in journal (Refereed) Published
Abstract [en]

Rhenium bipyridine tricarbonyl complexes, fac-[Re(bpy)(CO)(3)X](n+), are highly effective in selectively converting CO2 to CO under electrochemical and photochemical conditions. Despite numerous mechanistic studies aimed at understanding its CO2 reduction reaction (CO2RR) pathway, the intermediates further into the catalytic cycle have escaped detection, and the steps leading to product release remained elusive. In this study, employing stopped-flow mixing coupled with time-resolved infrared spectroscopy, we observed, for the first time, the reduced Re-tetracarbonyl species, [Re(bpy)(CO)(4)](0), with a half-life of approximately 55 ms in acetonitrile solvent. This intermediate is proposed to be common in both electrochemical and photochemical CO2RR. Furthermore, we directly observed the release of the product (CO) from this intermediate. Additionally, we detected the accumulation of [Re(bpy)(CO)(3)(CH3CN)](+) as a byproduct following product release, a significant side reaction under conditions with a limited supply of reducing equivalents mirroring photochemical conditions. The process could be unambiguously attributed to an electron transfer-catalyzed ligand substitution reaction involving [Re(bpy)(CO)(4)](0) by simultaneous real-time detection of all involved species. We believe that this side reaction significantly impacts the CO2RR efficiency of this class of catalysts under photochemical conditions or during electrocatalysis at mild overpotentials.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2024. Vol. 14, no 21, p. 16324-16334
Keywords [en]
CO2 reduction reaction, molecular catalysts, time-resolved FTIR, stopped-flowmixing, reactiveintermediates, CO release step, kinetic studies
National Category
Organic Chemistry
Identifiers
URN: urn:nbn:se:uu:diva-546566DOI: 10.1021/acscatal.4c06044ISI: 001340250900001Scopus ID: 2-s2.0-85207255152OAI: oai:DiVA.org:uu-546566DiVA, id: diva2:1926570
Funder
Knut and Alice Wallenberg FoundationAvailable from: 2025-01-13 Created: 2025-01-13 Last updated: 2025-01-13Bibliographically approved

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Chattopadhyay, SamirCheah, Mun HonLomoth, ReinerHammarström, Leif

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