2018
DOI: 10.1002/cptc.201800012
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Visible‐Light‐Driven Reduction of CO2 to CO and Its Subsequent Valorization in Carbonylation Chemistry and 13C Isotope Labeling

Abstract: A convenient and safe approach in valorizing carbon monoxide (CO) produced from the photocatalytic reduction of carbon dioxide (CO 2 ) has been investigated. Visible light was used to drive an optimized photocatalytic reduction using a ruthenium trisbipyridine complex as a sensitizer and a rhenium bipyridyl carbonyl complex as a catalyst to perform an efficient reduction of CO 2 to CO, which was then simultaneously utilized in a palladium-catalyzed aminocarbonylation reaction at room temperature. This approach… Show more

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Cited by 23 publications
(28 citation statements)
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“…The activation of the Re catalyst by the Ru photosensitizer was previously investigated by our group in a bimolecular system with sodium ascorbate (Asc) as a reversible electron donor in Ar-saturated ACN/H 2 O solution. [40] We have utilized nanosecond transient absorption spectroscopy and upon detailed spectroscopic and kinetic analyses, we were able to distinguish the bipyridyl-based reductions on either the photoreduced Ru or Re. The reduced Ru species, noted formally as Ru I , has a characteristic transient absorption at 510 nm while the monoreduced Re species (formal Re 0 ) has similar transient absorption in this same region together with an additional absorption at 450 nm where the Ru I actually bleaches.…”
Section: Tracking the First Reductionmentioning
confidence: 99%
“…The activation of the Re catalyst by the Ru photosensitizer was previously investigated by our group in a bimolecular system with sodium ascorbate (Asc) as a reversible electron donor in Ar-saturated ACN/H 2 O solution. [40] We have utilized nanosecond transient absorption spectroscopy and upon detailed spectroscopic and kinetic analyses, we were able to distinguish the bipyridyl-based reductions on either the photoreduced Ru or Re. The reduced Ru species, noted formally as Ru I , has a characteristic transient absorption at 510 nm while the monoreduced Re species (formal Re 0 ) has similar transient absorption in this same region together with an additional absorption at 450 nm where the Ru I actually bleaches.…”
Section: Tracking the First Reductionmentioning
confidence: 99%
“…[5] A related approach was exploited for the synthesis of 13 C-labeled amides using 13 CO 2 as a carbon source, albeit by CO 2 photoreduction and not electroreduction. [6] In fact, these achievements were possible because the carbonylation steps proceed with subatmospheric partial pressures of CO and use noble-metal-based catalysts that are stable in the presence of air and moisture. In contrast, in most industrially relevant processes, CO, which is derived from fossil feedstocks (e. g., steam reforming of methane or autothermal reforming), has to be in the form of a pure stream or as a syngas and the catalytic reactions require high partial pressures of CO and are highly sensitive to air and moisture.…”
Section: Introductionmentioning
confidence: 99%
“…The first and unique illustration of such an integrated two‐reaction process (CO 2 electroconversion to CO and carbonylation) was provided in 2017 by Skrydstrup and co‐workers, who reported the preparation of pharmaceuticals through a palladium‐catalyzed carbonylative cross‐coupling reaction [5] . A related approach was exploited for the synthesis of 13 C‐labeled amides using 13 CO 2 as a carbon source, albeit by CO 2 photoreduction and not electroreduction [6] . In fact, these achievements were possible because the carbonylation steps proceed with sub‐atmospheric partial pressures of CO and use noble‐metal‐based catalysts that are stable in the presence of air and moisture.…”
Section: Introductionmentioning
confidence: 99%
“…Development of catalysts with high selectivity, efficiency, and stability for converting CO 2 is still very challenging. Molecular catalysts based on ruthenium transition metal complexes for electrochemical reduction of CO 2 have attracted considerable research attention due to their unique structural and electronic features, as well as, homogeneous complexes retaining the advantages of elucidating catalytic processes for optimizing the catalysts . A great many remarkable achievements have been reported by Meyer, Kubiak, Tanaka, Fujita, Miller, Huang, and others …”
Section: Introductionmentioning
confidence: 99%
“…Molecular catalysts based on ruthenium transition metal complexes for electrochemical reduction of CO 2 have attracted considerable research attention due to their unique structural and electronic features, as well as, homogeneous complexes retaining the advantages of elucidating catalytic processes for optimizing the catalysts. [9,10] A great many remarkable achievements have been reported by Meyer, [11][12][13] Kubiak, [10] Tanaka, [14][15][16][17][18][19] Fujita, [20][21][22] Miller, [1] Huang, [23] and others. [24][25][26][27] However, because of the exceptional thermodynamic stability of CO 2 and the multiple electrons required in the reaction process, many ruthenium catalysts have low efficiency and selectivity.…”
Section: Introductionmentioning
confidence: 99%