Enzymatic C1 reduction using hydrogen in cofactor regeneration

  • Ruishuang Sun 1 ,
  • Chenqi Cao 1 ,
  • Qingyun Wang 1 ,
  • Hui Cao 1 ,
  • Ulrich Schwaneberg 2 ,
  • Yu Ji 1,2 ,
  • Luo Liu , 1 ,
  • Haijun Xu , 1
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  • 1. Beijing Bioprocess Key Laboratory, Beijing University of Chemical Technology, Beijing 100029, China
  • 2. Institute of Biotechnology, Rheinisch-Westfälische Technische Hochschale (RWTH) Aachen, Aachen 52074, Germany
liuluo@mail.buct.edu.cn
hjxu@mail.buct.edu.cn

Received date: 13 Dec 2023

Accepted date: 16 Feb 2024

Copyright

2024 Higher Education Press

Abstract

Carbon dioxide fixation presents a potential solution for mitigating the greenhouse gas issue. During carbon dioxide fixation, C1 compound reduction requires a high energy supply. Thermodynamic calculations suggest that the energy source for cofactor regeneration plays a vital role in the effective enzymatic C1 reduction. Hydrogenase utilizes renewable hydrogen to achieve the regeneration and supply cofactor nicotinamide adenine dinucleotide (NADH), providing a driving force for the reduction reaction to reduce the thermodynamic barrier of the reaction cascade, and making the forward reduction pathway thermodynamically feasible. Based on the regeneration of cofactor NADH by hydrogenase, and coupled with formaldehyde dehydrogenase and formolase, a favorable thermodynamic mode of the C1 reduction pathway for reducing formate to dihydroxyacetone (DHA) was designed and constructed. This resulted in accumulation of 373.19 μmol·L–1 DHA after 2 h, and conversion reaching 7.47%. These results indicate that enzymatic utilization of hydrogen as the electron donor to regenerate NADH is of great significance to the sustainable and green development of bio-manufacturing because of its high economic efficiency, no by-products, and environment-friendly operation. Moreover, formolase efficiently and selectively fixed the intermediate formaldehyde (FALD) to DHA, thermodynamically pulled formate to efficiently reduce to DHA, and finally stored the low-grade renewable energy into chemical energy with high energy density.

Cite this article

Ruishuang Sun , Chenqi Cao , Qingyun Wang , Hui Cao , Ulrich Schwaneberg , Yu Ji , Luo Liu , Haijun Xu . Enzymatic C1 reduction using hydrogen in cofactor regeneration[J]. Frontiers of Chemical Science and Engineering, 2024 , 18(7) : 75 . DOI: 10.1007/s11705-024-2431-3

Competing interests

The authors declare that they have no competing interests.

Acknowledgements

This study was funded by the National Key Research and Development Program of China (Grant No. 2022YFC2105900) and the National Natural Science Foundation of China (Grant Nos. 22378015 and 52073022).
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