Melling, Benjamin, Mielke, Tamara, Whitwood, Adrian C. et al. (5 more authors) (2024) Complementary specificity of unspecific peroxygenases enables access to diverse products from terpene oxygenation. CHEM: Catalysis. 100889. ISSN 2667-1093
Abstract
Unspecific peroxygenases (UPOs) have emerged as attractive biocatalysts for selective oxygenations because, unlike cytochromes P450, they can be employed as easy-to-use lyophilized powders and depend only upon hydrogen peroxide as the external oxidant. The application of UPOs to a range of synthetic challenges relies on the characterization of activity and specificity of complementary enzymes. Here, we show that two UPOs, artUPO and rAaeUPO-PaDa-I-H, which are representative members of the “short” family I and “long” family II UPOs, display complementary activity in a series of scalable, preparative biotransformations of a diverse array of terpenes. The UPOs were also applied to the biotransformation of chrysanthemic-acid-derived fragments relevant in the agrichemical industry, culminating in the highly diastereoselective and enantioselective oxidation of a racemic synthetic pyrethroid derivative via kinetic resolution.
Metadata
Item Type: | Article |
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Authors/Creators: |
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Copyright, Publisher and Additional Information: | Funding Information: We thank the UK Engineering and Physical Sciences Research Council ( EPSRC ) and Syngenta for the award of a studentship to B.M. (project 2602946 ) and the Industrial Affiliates of the Center of Excellence for Biotransformations, Bioprocessing, and Biomanufacturing ( CoEBio3 ) for the award of a studentship to T.M. Publisher Copyright: © 2023 The Authors |
Keywords: | cytochromes P450,C–H activation,oxygenation,SDG9: Industry, innovation, and infrastructure,terpenes,unspecific peroxygenases,UPOs |
Dates: |
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Institution: | The University of York |
Academic Units: | The University of York > Faculty of Sciences (York) > Chemistry (York) |
Depositing User: | Pure (York) |
Date Deposited: | 23 Jan 2024 17:30 |
Last Modified: | 02 Apr 2025 23:26 |
Published Version: | https://doi.org/10.1016/j.checat.2023.100889 |
Status: | Published |
Refereed: | Yes |
Identification Number: | 10.1016/j.checat.2023.100889 |
Related URLs: | |
Open Archives Initiative ID (OAI ID): | oai:eprints.whiterose.ac.uk:208197 |
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