Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 59, Issue 37, Pages 15886-15890Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202006893
Keywords
eBiorefinery; photobiocatalysis; photoelectrochemistry; photosynthesis; redox biocatalysis
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Funding
- National Research Foundation via the Creative Research Initiative Center, Republic of Korea [NRF-2015R1A3A2066191]
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Inspired by natural photosynthesis, biocatalytic photoelectrochemical (PEC) platforms are gaining prominence for the conversion of solar energy into useful chemicals by combining redox biocatalysis and photoelectrocatalysis. Herein, we report a dual biocatalytic PEC platform consisting of a molybdenum (Mo)-doped BiVO4(Mo:BiVO4) photoanode and an inverse opal ITO (IO-ITO) cathode that gives rise to the coupling of peroxygenase and ene-reductase-mediated catalysis, respectively. In the PEC cell, the photoexcited electrons generated from the Mo:BiVO(4)are transferred to the IO-ITO and regenerate reduced flavin mononucleotides to drive ene-reductase-catalyzedtrans-hydrogenation of ketoisophrone to (R)-levodione. Meanwhile, the photoactivated Mo:BiVO(4)evolves H(2)O(2)in situ via a two-electron water-oxidation process with the aid of an applied bias, which simultaneously supplies peroxygenases to drive selective hydroxylation of ethylbenzene into enantiopure (R)-1-phenyl-1-hydroxyethane. Thus, the deliberate integration of PEC systems with redox biocatalytic reactions can simultaneously produce valuable chemicals on both electrodes using solar-powered electrons and water.
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