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

Research output: Contribution to Journal/Magazine › Journal article › peer-review

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Supported Pt enabled proton-driven NAD(P)+ regeneration for biocatalytic oxidation. / Burnett, Joseph; Chen, Hui; Li, Jianwei et al.
In: ACS Applied Materials and Interfaces, Vol. 14, No. 18, 11.05.2022, p. 20943-20952.

Research output: Contribution to Journal/Magazine › Journal article › peer-review

Harvard

Burnett, J, Chen, H, Li, J, Li, Y, Huang, S, Shi, J, McCue, AJ, Howe, R, Minteer, SD & Wang, X 2022, 'Supported Pt enabled proton-driven NAD(P)+ regeneration for biocatalytic oxidation', ACS Applied Materials and Interfaces, vol. 14, no. 18, pp. 20943-20952. https://doi.org/10.1021/acsami.2c01743

APA

Burnett, J., Chen, H., Li, J., Li, Y., Huang, S., Shi, J., McCue, A. J., Howe, R., Minteer, S. D., & Wang, X. (2022). Supported Pt enabled proton-driven NAD(P)+ regeneration for biocatalytic oxidation. ACS Applied Materials and Interfaces, 14(18), 20943-20952. https://doi.org/10.1021/acsami.2c01743

Vancouver

Burnett J, Chen H, Li J, Li Y, Huang S, Shi J et al. Supported Pt enabled proton-driven NAD(P)+ regeneration for biocatalytic oxidation. ACS Applied Materials and Interfaces. 2022 May 11;14(18):20943-20952. Epub 2022 Apr 28. doi: 10.1021/acsami.2c01743

Author

Burnett, Joseph ; Chen, Hui ; Li, Jianwei et al. / Supported Pt enabled proton-driven NAD(P)+ regeneration for biocatalytic oxidation. In: ACS Applied Materials and Interfaces. 2022 ; Vol. 14, No. 18. pp. 20943-20952.

Bibtex

@article{fe6e24612aa24ad89957d0235c178e6d,
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 NAD(P)+-dependent pathways utilizing a cooperative inorganic-enzymatic catalytic system.",
keywords = "hydrogen, heterogeneous Pt catalysis, dehydrogenase, biocatalytic oxidation, NAD(P)+ regeneration",
author = "Joseph Burnett and Hui Chen and Jianwei Li and Ying Li and Shouying Huang and Jiafu Shi and McCue, {Alan J} and Russell Howe and Minteer, {Shelley D} and Xiaodong Wang",
note = "This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Applied Materials and Interfaces, copyright {\textcopyright} 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",
year = "2022",
month = may,
day = "11",
doi = "10.1021/acsami.2c01743",
language = "English",
volume = "14",
pages = "20943--20952",
journal = "ACS Applied Materials and Interfaces",
issn = "1944-8244",
publisher = "American Chemical Society",
number = "18",

}

RIS

TY - JOUR

T1 - Supported Pt enabled proton-driven NAD(P)+ regeneration for biocatalytic oxidation

AU - Burnett, Joseph

AU - Chen, Hui

AU - Li, Jianwei

AU - Li, Ying

AU - Huang, Shouying

AU - Shi, Jiafu

AU - McCue, Alan J

AU - Howe, Russell

AU - Minteer, Shelley D

AU - Wang, Xiaodong

N1 - 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

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

KW - hydrogen

KW - heterogeneous Pt catalysis

KW - dehydrogenase

KW - biocatalytic oxidation

KW - NAD(P)+ regeneration

U2 - 10.1021/acsami.2c01743

DO - 10.1021/acsami.2c01743

M3 - Journal article

C2 - 35482431

VL - 14

SP - 20943

EP - 20952

JO - ACS Applied Materials and Interfaces

JF - ACS Applied Materials and Interfaces

SN - 1944-8244

IS - 18

ER -