Affiliation:
1. Beijing Key Laboratory of Ionic Liquids Clean Process CAS Key Laboratory of Green Process and Engineering State Key Laboratory of Mesoscience and Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 P. R. China
2. Sino‐Danish College University of Chinese Academy of Sciences Beijing 101408 P. R. China
3. Longzihu New Energy Laboratory Zhengzhou Institute of Emerging Industrial Technology Henan University Zhengzhou 450000 P. R. China
Abstract
AbstractMulti‐enzymatic cascade reaction provides a new avenue for C─C coupling directly from CO2 under mild conditions. In this study, a new pathway with four enzymes including formate dehydrogenase (PaFDH), formaldehyde dehydrogenase (BmFADH), glycolaldehyde synthase (PpGALS), and alcohol dehydrogenase (GoADH) is developed for directly converting CO2 gas molecules to ethylene glycol (EG) in vitro. A rhodium‐based NADH regeneration electrode is constructed to continuously provide the proton and electron of this multi‐enzymatic cascade reaction. The prepared electrode can reach the Faradaic Efficiency (FE) of 82.9% at −0.6 V (vs. Ag/AgCl) and the NADH productivity of 0.737 mM h−1. Shortening the reaction path is crucial for multi‐enzymatic cascade reactions. Here, a hydrogen‐bonded organic framework (HOF) nano‐reactor is successfully developed to immobilize four enzymes in one pot with a striking enzyme loading capacity (990 mg enzyme g−1 material). Through integrating and optimization of NADH electro‐regeneration and enzymatic catalysis in one pot, 0.15 mM EG is achieved with an average conversion rate of 7.15 × 10−7 mmol CO2 min−1 mg−1 enzymes in 6 h. These results shed light on electro‐driven multi‐enzymatic cascade conversion of C─C coupling from CO2 in the nano‐reactor.
Funder
National Key Research and Development Program of China