Supported Pt enabled proton-driven NAD(P)+ regeneration for biocatalytic oxidation

Burnett, Joseph and Chen, Hui and Li, Jianwei and Li, Ying and Huang, Shouying and Shi, Jiafu and McCue, Alan J and Howe, Russell and Minteer, Shelley D and Wang, Xiaodong (2022) Supported Pt enabled proton-driven NAD(P)+ regeneration for biocatalytic oxidation. ACS Applied Materials and Interfaces, 14 (18). pp. 20943-20952. ISSN 1944-8244

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Abstract

The utilization of biocatalytic oxidations has evolved from the niche applications of the early 21st century to a widely recognized tool for general chemical synthesis. One of the major drawbacks that hinders commercialization is the dependence on expensive nicotinamide adenine dinucleotide (NAD(P)+) cofactors, and so, their regeneration is essential. Here, we report the design of carbon-supported Pt catalysts that can regenerate NAD(P)+ by proton-driven NAD(P)H oxidation with concurrent hydrogen formation. The carbon support was modified to tune the electronic nature of the Pt nanoparticles, and it was found that the best catalyst for NAD(P) regeneration (TOF = 581 h-1) was electron-rich Pt on carbon. Finally, the heterogeneous Pt catalyst was applied in the biocatalytic oxidation of a variety of alcohols catalyzed by different alcohol dehydrogenases. The Pt catalyst exhibited good compatibility with the biocatalytic system. Its NAD(P)+ regeneration function successfully supported biocatalytic conversion from alcohols to corresponding ketone or lactone products. This work provides a promising strategy for chemical synthesis NAD(P)+-dependent pathways utilizing a cooperative inorganic-enzymatic catalytic system.

Item Type:
Journal Article
Journal or Publication Title:
ACS Applied Materials and Interfaces
Additional Information:
This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Applied Materials and Interfaces, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/acsami.2c01743
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ID Code:
173727
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Deposited On:
09 Aug 2022 10:50
Refereed?:
Yes
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Published
Last Modified:
09 Aug 2022 10:50