期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 22, 期 45, 页码 16047-16051出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201604197
关键词
electron mediator; electron-transport chain; hydrogen production; synthetic enzymatic pathway; water splitting
资金
- Department of Energy, Office of Energy Efficiency and Renewable Energy, Fuel Cell Technologies Office [DE-EE0006968]
- Virginia Agricultural Experiment Station
- Hatch Program of the National Institute of Food and Agriculture, U.S. Department of Agriculture
Hydrogen production by water splitting energized by biomass sugars is one of the most promising technologies for distributed green H-2 production. Direct H-2 generation from NADPH, catalysed by an NADPH-dependent, soluble [NiFe]-hydrogenase (SH1) is thermodynamically unfavourable, resulting in slow volumetric productivity. We designed the biomimetic electron transport chain from NADPH to H-2 by the introduction of an oxygen-insensitive electron mediator benzyl viologen (BV) and an enzyme (NADPH rubredoxin oxidoreductase, NROR), catalysing electron transport between NADPH and BV. The H-2 generation rates using this biomimetic chain increased by approximately five-fold compared to those catalysed only by SH1. The peak volumetric H-2 productivity via the in vitro enzymatic pathway comprised of hyperthermophilic glucose 6-phosphate dehydrogenase, 6-phosphogluconolactonase, and 6-phosphogluconate dehydrogenase, NROR, and SH1 was 310 mmol H-2/Lh(-1), the highest rate yet reported. The concept of biomimetic electron transport chains could be applied to both in vitro and in vivo H-2 production biosystems and artificial photo-synthesis.
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