Journal article
Chemo-bio catalysis using carbon supports: application in H2-driven cofactor recycling
- Abstract:
- Heterogeneous biocatalytic hydrogenation is an attractive strategy for clean, enantioselective C=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 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.
- Publication status:
- Published
- Peer review status:
- Peer reviewed
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(Preview, Version of record, 1.0MB, Terms of use)
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- Publisher copy:
- 10.1039/d1sc00295c
Authors
- Publisher:
- Royal Society of Chemistry
- Journal:
- Chemical Science More from this journal
- Volume:
- 12
- Issue:
- 23
- Pages:
- 8105-8114
- Publication date:
- 2021-05-07
- Acceptance date:
- 2021-04-30
- DOI:
- EISSN:
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2041-6539
- ISSN:
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2041-6520
- Language:
-
English
- Keywords:
- Pubs id:
-
1174879
- Local pid:
-
pubs:1174879
- Deposit date:
-
2021-05-07
Terms of use
- Copyright holder:
- Zhao et al.
- Copyright date:
- 2021
- Rights statement:
- ©2021 This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. Material from this article can be used in other publications provided that the correct acknowledgement is given with the reproduced material. All publication charges for this article have been paid for by the Royal Society of Chemistry.
- Licence:
- CC Attribution (CC BY)
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