期刊
ADVANCED FUNCTIONAL MATERIALS
卷 28, 期 24, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.201705232
关键词
artificial photosynthesis; biocatalysis; carbon nanotubes; graphitic carbon nitride; photoelectrochemical cells
类别
资金
- National Research Foundation (NRF) via the Creative Research Initiative Center, Republic of Korea [NRF-2015 R1A3A2066191]
- Netherlands Organisation for Scientific Research [724.014.003]
In green plants, solar-powered electrons are transferred through sophistically arranged photosystems and are subsequently channelled into the Calvin cycle to generate chemical energy. Inspired by the natural photosynthetic scheme, a photoelectrochemical cell (PEC) is constructed configured with protonated graphitic carbon nitride (p-g-C3N4) and carbon nanotube hybrid (CNT/p-g-C3N4) film cathode, and FeOOH-deposited bismuth vanadate (FeOOH/BiVO4) photoanode for the production of industrially useful chiral alkanes using an old yellow enzyme homologue from Thermus scotoductus (TsOYE). In the biocatalytic PEC platform, photoexcited electrons provided by the FeOOH/BiVO4 photoanode are transferred to the robust and self-standing CNT/p-g-C3N4 hybrid film that electrocatalytically reduces flavin mononucleotide (FMN) mediator. The p-g-C3N4 promotes a two-electron reduction of FMN coupled with an accelerated electron transfer by the conductive CNT network. The reduced FMN subsequently delivers the electrons to TsOYE for the highly enantioselective conversion of ketoisophorone to (R)-levodione. Under light illumination (>420 nm) and external bias, (R)-levodione is synthesized with the enantiomeric excess value of above 83%, not influenced by the scale of applied bias, simultaneously exhibiting stable and high current efficiency. The results suggest that the biocatalytic PEC made up of economical materials can selectively synthesize high-value organic chemicals using water as an electron donor.
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