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; Xiaodong Wang

doi:10.1021/acsami.2c01743

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

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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 via NAD(P)+-dependent pathways utilizing a cooperative inorganic-enzymatic catalytic system.

Original language	English
Pages (from-to)	20943-20952
Number of pages	10
Journal	ACS Applied Materials & Interfaces
Volume	14
Issue number	18
Early online date	28 Apr 2022
DOIs	https://doi.org/10.1021/acsami.2c01743
Publication status	Published - 11 May 2022

Bibliographical note

ACKNOWLEDGMENTS
This work was supported by the EPSRC New Horizons scheme (EP/V048635/1), Royal Society (ICA\R1\180317), and National Science Foundation Center for Synthetic Organic Electrochemistry (2002158). We are also grateful for support
from the U.K. Catalysis Hub funded by EPSRC grant reference EP/R026645/1.

Keywords

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

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This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Applied Materials and Interfaces, copyright © 2022 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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Cite this

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title = "Supported Pt Enabled Proton-Driven NAD(P)+ Regeneration for Biocatalytic Oxidation",

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.",

keywords = "NAD(P)+ regeneration, biocatalytic oxidation, dehydrogenase, heterogeneous Pt catalysis, hydrogen",

author = "Burnett, {Joseph W.H.} and Hui Chen and Jianwei Li and Ying Li and Shouying Huang and Jiafu Shi and McCue, {Alan J.} and Howe, {Russell F.} and Minteer, {Shelley D.} and Xiaodong Wang",

note = "ACKNOWLEDGMENTS This work was supported by the EPSRC New Horizons scheme (EP/V048635/1), Royal Society (ICA\R1\180317), and National Science Foundation Center for Synthetic Organic Electrochemistry (2002158). We are also grateful for support from the U.K. Catalysis Hub funded by EPSRC grant reference EP/R026645/1.",

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T1 - Supported Pt Enabled Proton-Driven NAD(P)+ Regeneration for Biocatalytic Oxidation

AU - Burnett, Joseph W.H.

AU - Chen, Hui

AU - Li, Jianwei

AU - Li, Ying

AU - Huang, Shouying

AU - Shi, Jiafu

AU - McCue, Alan J.

AU - Howe, Russell F.

AU - Minteer, Shelley D.

AU - Wang, Xiaodong

N1 - ACKNOWLEDGMENTS This work was supported by the EPSRC New Horizons scheme (EP/V048635/1), Royal Society (ICA\R1\180317), and National Science Foundation Center for Synthetic Organic Electrochemistry (2002158). We are also grateful for support from the U.K. Catalysis Hub funded by EPSRC grant reference EP/R026645/1.

PY - 2022/5/11

Y1 - 2022/5/11

N2 - 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.

AB - 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.

KW - NAD(P)+ regeneration

KW - biocatalytic oxidation

KW - dehydrogenase

KW - heterogeneous Pt catalysis

KW - hydrogen

U2 - 10.1021/acsami.2c01743

DO - 10.1021/acsami.2c01743

M3 - Article

SN - 1944-8244

VL - 14

SP - 20943

EP - 20952

JO - ACS Applied Materials & Interfaces

JF - ACS Applied Materials & Interfaces

IS - 18

ER -

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

Abstract

Bibliographical note

Keywords

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