Exceptionally High Rates of Biological Hydrogen Production by Biomimetic In Vitro Synthetic Enzymatic Pathways
Abstract
Hydrogen production by water splitting energized by biomass sugars is one of the most promising technologies for distributed green H2 production. Direct H2 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 H2 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 H2 generation rates using this biomimetic chain increased by approximately five-fold compared to those catalysed only by SH1. The peak volumetric H2 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 H2/L h-1, the highest rate yet reported. The concept of biomimetic electron transport chains could be applied to both in vitro and in vivo H2 production biosystems and artificial photosynthesis.
- Authors:
-
- Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
- Univ. of Georgia, Athens, GA (United States)
- Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States); Chinese Academy of Sciences (CAS), Tianjin (China)
- Publication Date:
- Research Org.:
- Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE)
- OSTI Identifier:
- 1533133
- Grant/Contract Number:
- EE0006968
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry - A European Journal
- Additional Journal Information:
- Journal Volume: 22; Journal Issue: 45; Journal ID: ISSN 0947-6539
- Publisher:
- ChemPubSoc Europe
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; chemistry; electron mediator; electron-transport chain; hydrogen production; synthetic enzymatic pathway; water splitting
Citation Formats
Kim, Eui-Jin, Wu, Chang-Hao, Adams, Michael W. W., and Zhang, Y. -H. Percival. Exceptionally High Rates of Biological Hydrogen Production by Biomimetic In Vitro Synthetic Enzymatic Pathways. United States: N. p., 2016.
Web. doi:10.1002/chem.201604197.
Kim, Eui-Jin, Wu, Chang-Hao, Adams, Michael W. W., & Zhang, Y. -H. Percival. Exceptionally High Rates of Biological Hydrogen Production by Biomimetic In Vitro Synthetic Enzymatic Pathways. United States. https://doi.org/10.1002/chem.201604197
Kim, Eui-Jin, Wu, Chang-Hao, Adams, Michael W. W., and Zhang, Y. -H. Percival. Fri .
"Exceptionally High Rates of Biological Hydrogen Production by Biomimetic In Vitro Synthetic Enzymatic Pathways". United States. https://doi.org/10.1002/chem.201604197. https://www.osti.gov/servlets/purl/1533133.
@article{osti_1533133,
title = {Exceptionally High Rates of Biological Hydrogen Production by Biomimetic In Vitro Synthetic Enzymatic Pathways},
author = {Kim, Eui-Jin and Wu, Chang-Hao and Adams, Michael W. W. and Zhang, Y. -H. Percival},
abstractNote = {Hydrogen production by water splitting energized by biomass sugars is one of the most promising technologies for distributed green H2 production. Direct H2 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 H2 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 H2 generation rates using this biomimetic chain increased by approximately five-fold compared to those catalysed only by SH1. The peak volumetric H2 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 H2/L h-1, the highest rate yet reported. The concept of biomimetic electron transport chains could be applied to both in vitro and in vivo H2 production biosystems and artificial photosynthesis.},
doi = {10.1002/chem.201604197},
journal = {Chemistry - A European Journal},
number = 45,
volume = 22,
place = {United States},
year = {Fri Sep 30 00:00:00 EDT 2016},
month = {Fri Sep 30 00:00:00 EDT 2016}
}
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Works referencing / citing this record:
A Recombinant 12‐His Tagged Pyrococcus furiosus Soluble [NiFe]‐Hydrogenase I Overexpressed in Thermococcus kodakarensis KOD1 Facilitates Hydrogen‐Powered in vitro NADH Regeneration
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