The complex interplay of chemo- and bio-catalysis for one-pot oxidation cascades – indole oxidation in focus

Stenner, Alex, Lewis, Richard J., Pask, Johnathan, Morgan, David J. ORCID: https://orcid.org/0000-0002-6571-5731, Davies, Thomas E. and Hutchings, Graham J. ORCID: https://orcid.org/0000-0001-8885-1560 2025. The complex interplay of chemo- and bio-catalysis for one-pot oxidation cascades – indole oxidation in focus. Green Chemistry 10.1039/d5gc05367f

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Abstract

The combination of chloroperoxidase (CPO), derived from the marine fungus Caldariomyces fumago, in combination with supported AuPd nanoalloys, has been demonstrated as a highly efficient one-pot system for the selective oxidation of indole to 2-oxindole. Peroxy-enzymatic oxygen transfer is driven via chemo-catalytic in situ H2O2 generation from H2 and O2 over AuPd surfaces, with the continuous supply of the oxidant at low-concentration essential in maintaining enzymatic activity. Indeed, coupling CPO and an optimised 1% Au1Pd1/TiO2 formulation achieved 33 000 TTN for indole oxidation, which is among the highest reported when compared to alternative systems utilizing in situ generated H2O2, including electrochemical and co-enzymatic approaches. Exceptional tandem performance has been achieved upon adopting a holistic approach toward design and optimisation of the system, thus deconvoluting the complex array of parameters governing chemo- and bio-catalytic performance under operational conditions; including metal nanoparticle speciation, morphology, electronic structure, and leaching, in addition to enzyme deactivation and in situ physisorption. We consider such an approach to offer a case study and guide to the community, facilitating efficient optimisation of complex chemo-enzymatic systems for potential industrial applications.

Item Type:	Article
Date Type:	Published Online
Status:	In Press
Schools:	Schools > Chemistry
Additional Information:	License information from Publisher: LICENSE 1: URL: https://creativecommons.org/licenses/by/3.0/, Start Date: 2025-12-02
Publisher:	Royal Society of Chemistry
ISSN:	1463-9262
Date of First Compliant Deposit:	22 December 2025
Date of Acceptance:	27 November 2025
Last Modified:	23 Dec 2025 02:30
URI:	https://orca.cardiff.ac.uk/id/eprint/183405

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