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Title: Exceptionally High Rates of Biological Hydrogen Production by Biomimetic In Vitro Synthetic Enzymatic Pathways

Journal Article · · Chemistry - A European Journal
 [1];  [2];  [2];  [3]
  1. Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
  2. Univ. of Georgia, Athens, GA (United States)
  3. Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States); Chinese Academy of Sciences (CAS), Tianjin (China)

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.

Research Organization:
Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
Grant/Contract Number:
EE0006968
OSTI ID:
1533133
Journal Information:
Chemistry - A European Journal, Vol. 22, Issue 45; ISSN 0947-6539
Publisher:
ChemPubSoc EuropeCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 22 works
Citation information provided by
Web of Science

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Cited By (6)

A Recombinant 12‐His Tagged Pyrococcus furiosus Soluble [NiFe]‐Hydrogenase I Overexpressed in Thermococcus kodakarensis KOD1 Facilitates Hydrogen‐Powered in vitro NADH Regeneration journal October 2018
Building a Thermostable Metabolon for Facilitating Coenzyme Transport and In Vitro Hydrogen Production at Elevated Temperature journal August 2018
Engineering a thermostable highly active glucose 6-phosphate dehydrogenase and its application to hydrogen production in vitro journal February 2018
Biomanufacturing: history and perspective journal November 2016
Optimization of a reduced enzymatic reaction cascade for the production of L-alanine journal August 2019
Ultra-rapid rates of water splitting for biohydrogen gas production through in vitro artificial enzymatic pathways journal January 2018