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通过高效酶级联反应将二氧化碳光电还原为甲醇。

Photoelectrochemical Reduction of Carbon Dioxide to Methanol through a Highly Efficient Enzyme Cascade.

机构信息

Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology, 335 Science Road, Daejeon, 305-701, Republic of Korea.

Department of Chemical Engineering, Konkuk University, 120 Neungdong-ro, Seoul, 143-701, Republic of Korea.

出版信息

Angew Chem Int Ed Engl. 2017 Mar 27;56(14):3827-3832. doi: 10.1002/anie.201611379. Epub 2017 Jan 25.

DOI:10.1002/anie.201611379
PMID:28120367
Abstract

Natural photosynthesis is an effective route for the clean and sustainable conversion of CO into high-energy chemicals. Inspired by the natural process, a tandem photoelectrochemical (PEC) cell with an integrated enzyme-cascade (TPIEC) system was designed, which transfers photogenerated electrons to a multienzyme cascade for the biocatalyzed reduction of CO to methanol. A hematite photoanode and a bismuth ferrite photocathode were applied to fabricate the iron oxide based tandem PEC cell for visible-light-assisted regeneration of the nicotinamide cofactor (NADH). The cell utilized water as an electron donor and spontaneously regenerated NADH. To complete the TPIEC system, a superior three-dehydrogenase cascade system was employed in the cathodic part of the PEC cell. Under applied bias, the TPIEC system achieved a high methanol conversion output of 220 μm h , 1280 μmol g  h using readily available solar energy and water.

摘要

自然光化学反应是一种清洁、可持续将 CO 转化为高能化学物质的有效途径。受此启发,设计了一种具有集成酶级联(TPIEC)系统的串联光电化学(PEC)电池,该电池将光生电子转移到多酶级联系统中,用于生物催化还原 CO 为甲醇。采用氧化铁作为光阳极和铋铁氧体作为光阴极来制备基于氧化铁的串联 PEC 电池,以可见光辅助烟酰胺辅酶(NADH)的再生。该电池利用水作为电子供体,并自发地再生 NADH。为了完成 TPIEC 系统,在 PEC 电池的阴极部分采用了一种优越的三脱氢酶级联系统。在施加偏压的情况下,TPIEC 系统利用易得的太阳能和水实现了高达 220 μm h 、1280 μmol g h 的甲醇转化率输出。

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