Cofactor‐Free Light‐Driven Whole‐Cell Cytochrome P450 Catalysis |
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Authors: | Jong Hyun Park Dr. Sahng Ha Lee Gun Su Cha Da Som Choi Dong Heon Nam Jae Hyung Lee Prof. Dr. Jung‐Kul Lee Prof. Dr. Chul‐Ho Yun Prof. Dr. Ki Jun Jeong Prof. Dr. Chan Beum Park |
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Affiliation: | 1. Department of Chemical and Biomolecular Engineering, Korea Advanced Institute of Science and Technology, 335 Science Road, Daejeon 305‐701 (Republic of Korea);2. Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology, 335 Science Road, Daejeon 305‐701 (Republic of Korea);3. School of Biological Sciences and Technology, Chonnam National University, Gwangju 500‐757 (Republic of Korea);4. Department of Chemical Engineering, Konkuk University, Seoul 143‐701 (Republic of Korea) |
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Abstract: | Cytochromes P450 can catalyze various regioselective and stereospecific oxidation reactions of non‐functionalized hydrocarbons. Here, we have designed a novel light‐driven platform for cofactor‐free, whole‐cell P450 photo‐biocatalysis using eosin Y (EY) as a photosensitizer. EY can easily enter into the cytoplasm of Escherichia coli and bind specifically to the heme domain of P450. The catalytic turnover of P450 was mediated through the direct transfer of photoinduced electrons from the photosensitized EY to the P450 heme domain under visible light illumination. The photoactivation of the P450 catalytic cycle in the absence of cofactors and redox partners is successfully conducted using many bacterial P450s (variants of P450 BM3) and human P450s (CYPs 1A1, 1A2, 1B1, 2A6, 2E1, and 3A4) for the bioconversion of different substrates, including marketed drugs (simvastatin, lovastatin, and omeprazole) and a steroid (17β‐estradiol), to demonstrate the general applicability of the light‐driven, cofactor‐free system. |
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Keywords: | cofactors cytochromes P450 enzymatic catalysis photocatalysis photoinduced electron transfer |
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