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• W2264483710 endingPage "1600" @default.
• W2264483710 startingPage "1591" @default.
• W2264483710 abstract "This paper describes the use of cadmium sulfide quantum dots (CdS QDs) as visible-light photocatalysts for the reduction of nitrobenzene to aniline through six sequential photoinduced, proton-coupled electron transfers. At pH 3.6-4.3, the internal quantum yield of photons-to-reducing electrons is 37.1% over 54 h of illumination, with no apparent decrease in catalyst activity. Monitoring of the QD exciton by transient absorption reveals that, for each step in the catalytic cycle, the sacrificial reductant, 3-mercaptopropionic acid, scavenges the excitonic hole in ∼5 ps to form QD(•-); electron transfer to nitrobenzene or the intermediates nitrosobenzene and phenylhydroxylamine then occurs on the nanosecond time scale. The rate constants for the single-electron transfer reactions are correlated with the driving forces for the corresponding proton-coupled electron transfers. This result suggests, but does not prove, that electron transfer, not proton transfer, is rate-limiting for these reactions. Nuclear magnetic resonance analysis of the QD-molecule systems shows that the photoproduct aniline, left unprotonated, serves as a poison for the QD catalyst by adsorbing to its surface. Performing the reaction at an acidic pH not only encourages aniline to desorb but also increases the probability of protonated intermediates; the latter effect probably ensures that recruitment of protons is not rate-limiting." @default.
• W2264483710 created "2016-06-24" @default.
• W2264483710 creator A5056693902 @default.
• W2264483710 creator A5058144700 @default.
• W2264483710 creator A5080135553 @default.
• W2264483710 date "2016-01-29" @default.
• W2264483710 modified "2023-10-01" @default.
• W2264483710 title "Photocatalytic Conversion of Nitrobenzene to Aniline through Sequential Proton-Coupled One-Electron Transfers from a Cadmium Sulfide Quantum Dot" @default.
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• W2264483710 doi "https://doi.org/10.1021/jacs.5b11353" @default.
• W2264483710 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/26784531" @default.
• W2264483710 hasPublicationYear "2016" @default.
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