| Visible Light-Driven O2 Reduction by a Porphyrin-Laccase System. | |
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MedLine Citation:
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PMID: 23330664 Owner: NLM Status: Publisher |
Abstract/OtherAbstract:
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Several recent studies have shown that the combination of photosensitizers with metalloenzymes can support a light-driven multi-electron reduction of molecules such as CO2 or HCN. Here we show that the association of the Zn tetramethyl pyridinium porphyrin (ZnTMPyP4+) photosensitizer with the multi-copper oxidase laccase allows to link the oxidation of an organic molecule to the four electrons reduction of dioxygen into water. The enzyme is photoreduced within minutes with porphyrin/enzyme ratio as low as 1/40. With a 1/1 ratio, the dioxygen consumption rate is 2 µmol L-1 s-1. Flash photolysis experiments support the formation of the triplet excited state of ZnTMPyP4+ which reduces the enzyme to form a radical cation of the porphyrin with a kET ≈107 s-1 M-1. The long-lived triplet excited state of the ZnTMPyP4+ (τ0 0.72 ms) accounts for a substantial electron transfer quantum yield ϕET =0.26. Consequently, the enzyme-dependent photo-oxidation of the electron donor (EDTA) occurs with a turn-over of 8 min-1 for the one electron oxidation process, thereby supporting the suitability of such enzyme/sensitizer hybrid material for aerobic photo-driven transformations on substrates. This study is the first example of a phorphyrin-sensitized 4-electron reduction of an enzyme of the multicopper-oxidase family, leading to photoreduction of dioxygen into water. |
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Authors:
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Theodore Lazarides; Igor V Sazanovich; A Jalila Simaan; Maria Chrisanthi Kafentzi; Milan Delor; Yasmina Mekmouche; Bruno Faure; Marius Réglier; Julia A Weinstein; Athanassios Georgios Coutsolelos; Thierry Tron |
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Publication Detail:
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Type: JOURNAL ARTICLE Date: 2013-1-21 |
Journal Detail:
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Title: Journal of the American Chemical Society Volume: - ISSN: 1520-5126 ISO Abbreviation: J. Am. Chem. Soc. Publication Date: 2013 Jan |
Date Detail:
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Created Date: 2013-1-21 Completed Date: - Revised Date: - |
Medline Journal Info:
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Nlm Unique ID: 7503056 Medline TA: J Am Chem Soc Country: - |
Other Details:
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Languages: ENG Pagination: - Citation Subset: - |
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From MEDLINE®/PubMed®, a database of the U.S. National Library of Medicine
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