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

15 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

Fingerprint

glutathione-independent formaldehyde dehydrogenase
Methanol
Formaldehyde
formic acid
Formate Dehydrogenases
Clostridium
Candida
Alcohol Dehydrogenase
Calorimetry
Enzymes
Titration
NAD
Yeast
Thermodynamics
Oxidoreductases
Alcohols
NAD phosphite oxidoreductase

Keywords

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

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)

Cite this

Singh, R. K., Singh, R., Sivakumar, D., Kondaveeti, S., Kim, T., Li, J., ... 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

Insights into Cell-Free Conversion of CO2 to Chemicals by a Multienzyme Cascade Reaction. / Singh, Raushan Kumar; Singh, Ranjitha; Sivakumar, Dakshinamurthy; Kondaveeti, Sanath; Kim, Taedoo; Li, Jinglin; Sung, Bong Hyun; Cho, Byung Kwan; Kim, Dong Rip; Kim, Sun Chang; Kalia, Vipin C.; Zhang, Yi Heng P.Job; Zhao, Huimin; Kang, Yun Chan; Lee, Jung Kul.

In: ACS Catalysis, Vol. 8, No. 12, 07.12.2018, p. 11085-11093.

Research output: Contribution to journalArticle

Singh, RK, Singh, R, Sivakumar, D, Kondaveeti, S, Kim, T, Li, J, Sung, BH, Cho, BK, Kim, DR, Kim, SC, Kalia, VC, Zhang, YHPJ, Zhao, H, Kang, YC & Lee, JK 2018, 'Insights into Cell-Free Conversion of CO2 to Chemicals by a Multienzyme Cascade Reaction', ACS Catalysis, vol. 8, no. 12, pp. 11085-11093. https://doi.org/10.1021/acscatal.8b02646
Singh RK, Singh R, Sivakumar D, Kondaveeti S, Kim T, Li J et al. Insights into Cell-Free Conversion of CO2 to Chemicals by a Multienzyme Cascade Reaction. ACS Catalysis. 2018 Dec 7;8(12):11085-11093. https://doi.org/10.1021/acscatal.8b02646
Singh, Raushan Kumar ; Singh, Ranjitha ; Sivakumar, Dakshinamurthy ; Kondaveeti, Sanath ; Kim, Taedoo ; Li, Jinglin ; Sung, Bong Hyun ; Cho, Byung Kwan ; Kim, Dong Rip ; Kim, Sun Chang ; Kalia, Vipin C. ; Zhang, Yi Heng P.Job ; Zhao, Huimin ; Kang, Yun Chan ; Lee, Jung Kul. / Insights into Cell-Free Conversion of CO2 to Chemicals by a Multienzyme Cascade Reaction. In: ACS Catalysis. 2018 ; Vol. 8, No. 12. pp. 11085-11093.
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