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Chemo-bio catalysis using carbon supports_application in H2-driven cofactor recycling.pdf (2.71 MB)

Chemo-Bio Catalysis Using Carbon Supports: Application in H2-Driven Cofactor Recycling

preprint
submitted on 11.12.2020, 10:27 and posted on 14.12.2020, 09:27 by Xu Zhao, Sarah Cleary, Ceren Zor, Nicole Grobert, Holly Reeve, Kylie Vincent
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 2,347 h-1,
respectively. This method demonstrates a new way of combining chemo- and biocatalysis on carbon supports, highlighted here for selective hydrogenation reactions.

Funding

EPSRC, IB Catalyst EP/N013514/1

History

Email Address of Submitting Author

sarah.cleary@chem.ox.ac.uk

Institution

University of Oxford

Country

United Kingdom

ORCID For Submitting Author

0000-0001-8876-1696

Declaration of Conflict of Interest

Authors declare no competing interests.

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