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Issue 23, 2021
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Chemo-bio catalysis using carbon supports: application in H2-driven cofactor recycling

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Abstract

Heterogeneous biocatalytic hydrogenation is an attractive strategy for clean, enantioselective C[double bond, length as m-dash]X reduction. This approach relies on enzymes powered by H2-driven NADH recycling. Commercially available carbon-supported metal (metal/C) catalysts are investigated here for direct H2-driven NAD+ reduction. Selected metal/C catalysts are then used for H2 oxidation with electrons transferred via the conductive carbon support material to an adsorbed enzyme for NAD+ reduction. These chemo-bio catalysts show improved activity and selectivity for generating bioactive NADH under ambient reaction conditions compared to metal/C catalysts. The metal/C catalysts and carbon support materials (all activated carbon or carbon black) are characterised to probe which properties potentially influence catalyst activity. The optimised chemo-bio catalysts are then used to supply NADH to an alcohol dehydrogenase for enantioselective (>99% ee) ketone reductions, leading to high cofactor turnover numbers and Pd and NAD+ reductase activities of 441 h−1 and 2347 h−1, respectively. This method demonstrates a new way of combining chemo- and biocatalysis on carbon supports, highlighted here for selective hydrogenation reactions.

Graphical abstract: Chemo-bio catalysis using carbon supports: application in H2-driven cofactor recycling

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Supplementary files

Article information


Submitted
15 Jan 2021
Accepted
30 Apr 2021
First published
07 May 2021

This article is Open Access
All publication charges for this article have been paid for by the Royal Society of Chemistry

Chem. Sci., 2021,12, 8105-8114
Article type
Edge Article

Chemo-bio catalysis using carbon supports: application in H2-driven cofactor recycling

X. Zhao, S. E. Cleary, C. Zor, N. Grobert, H. A. Reeve and K. A. Vincent, Chem. Sci., 2021, 12, 8105 DOI: 10.1039/D1SC00295C

This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. You can use material from this article in other publications without requesting further permissions from the RSC, provided that the correct acknowledgement is given.

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