Enhanced P450 fatty acid decarboxylase catalysis by glucose oxidase coupling and co-assembly for biofuel generation

Libo Zhang; Olivia M Manley; Dumei Ma; Yingwu Yin; Thomas M Makris; Qian Wang

doi:10.1016/j.biortech.2020.123538

Enhanced P450 fatty acid decarboxylase catalysis by glucose oxidase coupling and co-assembly for biofuel generation

Bioresour Technol. 2020 Sep:311:123538. doi: 10.1016/j.biortech.2020.123538. Epub 2020 May 15.

Authors

Libo Zhang¹, Olivia M Manley¹, Dumei Ma², Yingwu Yin³, Thomas M Makris¹, Qian Wang⁴

Affiliations

¹ Department of Chemistry and Biochemistry, University of South Carolina, 631 Sumter Street, Columbia, SC 29208, USA.
² Department of Chemistry and Biochemistry, University of South Carolina, 631 Sumter Street, Columbia, SC 29208, USA; Department of Chemical and Biochemical Engineering, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian, China.
³ Department of Chemical and Biochemical Engineering, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian, China.
⁴ Department of Chemistry and Biochemistry, University of South Carolina, 631 Sumter Street, Columbia, SC 29208, USA. Electronic address: wang263@mailbox.sc.edu.

PMID: 32485602
DOI: 10.1016/j.biortech.2020.123538

Abstract

Cytochrome P450 OleT is a fatty acid decarboxylase that uses hydrogen peroxide (H₂O₂) to catalyze the production of terminal alkenes, which are industrially important chemicals with biofuel and synthetic applications. Despite its requirement for large turnover levels, high concentrations of H₂O₂ may cause heme group degradation, diminishing enzymatic activity and limiting broad application for synthesis. Here, we report an artificial enzyme cascade composed of glucose oxidase (GOx) and OleT_SA from Staphylococcus aureus for efficient terminal alkene production. By adjusting the ratio of GOx to OleT_SA, the GOx-based tandem catalysis shows significantly improved product yield compared to the H₂O₂ injection method. Moreover, the co-assembly of the GOx/OleT_SA enzymes with a polymer, forming polymer-dual enzymes nanoparticles, displays improved activity compared to the free enzyme. This dual strategy provides a simple and efficient system to transform a naturally abundant feedstock to industrially important chemicals.

Keywords: Co-assembly; Enhanced activity; Enzyme cascade; Glucose oxidase; P450 OleT; Terminal alkenes.

MeSH terms

Biofuels
Carboxy-Lyases*
Catalysis
Cytochrome P-450 Enzyme System
Glucose
Glucose Oxidase*
Hydrogen Peroxide

Substances

Biofuels
Cytochrome P-450 Enzyme System
Hydrogen Peroxide
Glucose Oxidase
Carboxy-Lyases
Glucose