Supported Pt Enabled Proton-Driven NAD(P)+ Regeneration for Biocatalytic Oxidation

Joseph W.H. Burnett, Hui Chen, Jianwei Li, Ying Li, Shouying Huang, Jiafu Shi, Alan J. McCue, Russell F. Howe, Shelley D. Minteer* (Corresponding Author), Xiaodong Wang* (Corresponding Author)

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

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 via NAD(P)+-dependent pathways utilizing a cooperative inorganic-enzymatic catalytic system.
Original languageEnglish
Pages (from-to)20943-20952
Number of pages10
JournalACS Applied Materials & Interfaces
Volume14
Issue number18
Early online date28 Apr 2022
DOIs
Publication statusPublished - 11 May 2022

Keywords

  • NAD(P)+ regeneration
  • biocatalytic oxidation
  • dehydrogenase
  • heterogeneous Pt catalysis
  • hydrogen

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