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Insights into Cell-Free Conversion of CO2 to Chemicals by a Multienzyme Cascade Reaction

Authors
Singh, Raushan KumarSingh, RanjithaSivakumar, DakshinamurthyKondaveeti, SanathKim, TaedooLi, JinglinSung, Bong HyunCho, Byung-KwanKim, Dong RipKim, Sun ChangKalia, Vipin C.Zhang, Yi-Heng P. JobZhao, HuiminKang, Yun ChanLee, Jung-Kul
Issue Date
12월-2018
Publisher
AMER CHEMICAL SOC
Keywords
cascade reaction; formaldehyde; methanol; multienzyme; CO2; FDH; FaldDH
Citation
ACS CATALYSIS, v.8, no.12, pp.11085 - 11093
Indexed
SCIE
SCOPUS
Journal Title
ACS CATALYSIS
Volume
8
Number
12
Start Page
11085
End Page
11093
URI
https://scholar.korea.ac.kr/handle/2021.sw.korea/71389
DOI
10.1021/acscatal.8b02646
ISSN
2155-5435
Abstract
Multienzymatic cascade reactions have garnered the attention of many researchers as an approach for converting CO, into methanol. The cascade reaction used in this study includes the following enzymes: a formate dehydrogenase (CIFDH), a formaldehyde dehydrogenase (BmFaldDH), and an alcohol dehydrogenase (YADH) from Clostridium ljungdahlii, Burkholderia multivorans, and Saccharomyces cerevisiae, respectively. Because this cascade reaction requires NADH as a cofactor, phosphite dehydrogenase (PTDH) was employed to regenerate the cofactor. The multienzymatic cascade reaction, along with PTDH, yielded 3.28 mM methanol. The key to the success of this cascade reaction was a novel formaldehyde dehydrogenase, BmFaldDH, the enzyme catalyzing the reduction of formate to formaldehyde. The methanol yield was further improved by incorporation of 1-ethyl-3-methylimidazolium acetate (EMIM-Ac), resulting in 7.86 mM of methanol. A 500-fold increase in total turnover number was observed for the CIFDH-BmFaldDH-YADH cascade system compared to the Candida boidinii FDH-Pseudomonas putida FaldDH-YADH system. We provided detailed insights into the enzymatic reduction of CO2 by determining the thermodynamic parameters (K-d and Delta G) using isothermal titration calorimetry. Furthermore, we demonstrated a novel time-dependent formaldehyde production from CO2. Our results will aid in the understanding and development of a robust multienzyme catalyzed cascade reaction for the reduction of CO2 to value-added chemicals.
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