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Enzymatic C1 reduction using hydrogen in cofactor regeneration |
Ruishuang Sun1, Chenqi Cao1, Qingyun Wang1, Hui Cao1, Ulrich Schwaneberg2, Yu Ji1,2, Luo Liu1( ), Haijun Xu1( ) |
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 |
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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.
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Keywords
[NiFe]-hydrogenase SH
formolase
NADH regeneration
C1 compound reduction
thermodynamic calculation
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Corresponding Author(s):
Luo Liu,Haijun Xu
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About author: #usheng Xing, Yannan Jian and Xiaodan Zhao contributed equally to this work.]]> |
Just Accepted Date: 28 February 2024
Issue Date: 29 May 2024
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