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

Raushan Kumar Singh, Ranjitha Singh, Dakshinamurthy Sivakumar, Sanath Kondaveeti, Taedoo Kim, Jinglin Li, Bong Hyun Sung, Byung Kwan Cho, Dong Rip Kim, Sun Chang Kim, Vipin C. Kalia, Yi Heng P.Job Zhang, Huimin Zhao, Yun Chan Kang, Jung Kul Lee

Research output: Contribution to journalArticle

23 Citations (Scopus)

Abstract

Multienzymatic cascade reactions have garnered the attention of many researchers as an approach for converting CO2 into methanol. The cascade reaction used in this study includes the following enzymes: a formate dehydrogenase (ClFDH), 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 ClFDH-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 (Kd and ΔG) 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.

Original languageEnglish
Pages (from-to)11085-11093
Number of pages9
JournalACS Catalysis
Volume8
Issue number12
DOIs
Publication statusPublished - 2018 Dec 7

Keywords

  • cascade reaction
  • CO
  • FaldDH
  • FDH
  • formaldehyde
  • methanol
  • multienzyme

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)

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    Singh, R. K., Singh, R., Sivakumar, D., Kondaveeti, S., Kim, T., Li, J., Sung, B. H., Cho, B. K., Kim, D. R., Kim, S. C., Kalia, V. C., Zhang, Y. H. P. J., Zhao, H., Kang, Y. C., & Lee, J. K. (2018). Insights into Cell-Free Conversion of CO2 to Chemicals by a Multienzyme Cascade Reaction. ACS Catalysis, 8(12), 11085-11093. https://doi.org/10.1021/acscatal.8b02646