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

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dc.contributor.authorSingh, Raushan Kumarko
dc.contributor.authorSingh, Ranjithako
dc.contributor.authorSivakumar, Dakshinamurthyko
dc.contributor.authorKondaveeti, Sanathko
dc.contributor.authorKim, Taedooko
dc.contributor.authorLi, Jinglinko
dc.contributor.authorSung, Bong Hyunko
dc.contributor.authorCho, Byung-Kwanko
dc.contributor.authorKim, Dong Ripko
dc.contributor.authorKim, Sun Changko
dc.contributor.authorKalia, Vipin C.ko
dc.contributor.authorZhang, Yi-Heng P. Jobko
dc.contributor.authorZhao, Huiminko
dc.contributor.authorKang, Yun Chanko
dc.contributor.authorLee, Jung-Kulko
dc.identifier.citationACS CATALYSIS, v.8, no.12, pp.11085 - 11093-
dc.description.abstractMultienzymatic 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.-
dc.publisherAMER CHEMICAL SOC-
dc.titleInsights into Cell-Free Conversion of CO2 to Chemicals by a Multienzyme Cascade Reaction-
dc.citation.publicationnameACS CATALYSIS-
dc.contributor.localauthorCho, Byung-Kwan-
dc.contributor.localauthorKim, Sun Chang-
dc.contributor.nonIdAuthorSingh, Raushan Kumar-
dc.contributor.nonIdAuthorSingh, Ranjitha-
dc.contributor.nonIdAuthorSivakumar, Dakshinamurthy-
dc.contributor.nonIdAuthorKondaveeti, Sanath-
dc.contributor.nonIdAuthorKim, Taedoo-
dc.contributor.nonIdAuthorLi, Jinglin-
dc.contributor.nonIdAuthorSung, Bong Hyun-
dc.contributor.nonIdAuthorKim, Dong Rip-
dc.contributor.nonIdAuthorKalia, Vipin C.-
dc.contributor.nonIdAuthorZhang, Yi-Heng P. Job-
dc.contributor.nonIdAuthorZhao, Huimin-
dc.contributor.nonIdAuthorKang, Yun Chan-
dc.contributor.nonIdAuthorLee, Jung-Kul-
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