Enzymatic C1 reduction using hydrogen in cofactor regeneration  

作　　者：Ruishuang Sun Chenqi Cao Qingyun Wang Hui Cao Ulrich Schwaneberg Yu Ji Luo Liu Haijun Xu 

机构地区：[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

出　　处：《Frontiers of Chemical Science and Engineering》2024年第7期33-40,共8页化学科学与工程前沿（英文版）

基　　金：funded by the National Key Research and Development Program of China(Grant No.2022YFC2105900);the National Natural Science Foundation of China(Grant Nos.22378015 and 52073022).

摘　　要：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 373.19μmol·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.

关 键 词：[NiFe]-hydrogenase SH formolase NADH regeneration C1 compound reduction thermodynamic calculation 

分 类 号：O64[理学—物理化学]