Production of Biobased Ethylbenzene by Cascade Biocatalysis with an Engineered Photodecarboxylase

Author:

Qin Zhaoyang1,Zhou Yi1ORCID,Li Zhi2ORCID,Höhne Matthias3ORCID,Bornscheuer Uwe T.4ORCID,Wu Shuke14ORCID

Affiliation:

1. National Key Laboratory of Agricultural Microbiology College of Life Science and Technology Huazhong Agricultural University No. 1 Shizishan Street Wuhan 430070 P. R. China

2. Department of Chemical and Biomolecular Engineering National University of Singapore 4 Engineering Drive 4 Singapore 117585 Singapore

3. Institute of Chemistry Technische Universität Berlin Müller-Breslau-Str. 10 10623 Berlin Germany

4. Department of Biotechnology and Enzyme Catalysis Institute of Biochemistry University of Greifswald Felix Hausdorff-Str. 4 17489 Greifswald Germany

Abstract

AbstractProduction of commodity chemicals, such as benzene, toluene, ethylbenzene, and xylenes (BTEX), from renewable resources is key for a sustainable society. Biocatalysis enables one‐pot multistep transformation of bioresources under mild conditions, yet it is often limited to biochemicals. Herein, we developed a non‐natural three‐enzyme cascade for one‐pot conversion of biobased l‐phenylalanine into ethylbenzene. The key rate‐limiting photodecarboxylase was subjected to structure‐guided semirational engineering, and a triple mutant CvFAP(Y466T/P460A/G462I) was obtained with a 6.3‐fold higher productivity. With this improved photodecarboxylase, an optimized two‐cell sequential process was developed to convert l‐phenylalanine into ethylbenzene with 82 % conversion. The cascade reaction was integrated with fermentation to achieve the one‐pot bioproduction of ethylbenzene from biobased glycerol, demonstrating the potential of cascade biocatalysis plus enzyme engineering for the production of biobased commodity chemicals.

Funder

National Natural Science Foundation of China

Natural Science Foundation of Hubei Province

Fundamental Research Funds for the Central Universities

Alexander von Humboldt-Stiftung

H2020 European Research Council

Publisher

Wiley

Subject

General Chemistry,Catalysis

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