Copper oxide-based cathode for direct NADPH regeneration

Abstract Nearly a fourth of all enzymatic activities is attributable to oxidoreductases, and the redox reactions supported by this vast catalytic repertoire sustain cellular metabolism. In many biological processes, reduction depends on hydride transfer from either reduced nicotinamide adenine dinuc...

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Autores principales:	J. T. Kadowaki, T. H. Jones, A. Sengupta, V. Gopalan, V. V. Subramaniam
Formato:	article
Lenguaje:	EN
Publicado:	Nature Portfolio 2021
Materias:	Medicine R Science Q
Acceso en línea:	https://doaj.org/article/ad411539614147dc92701c9f044b2d36
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spelling	oai:doaj.org-article:ad411539614147dc92701c9f044b2d362021-12-02T11:46:07ZCopper oxide-based cathode for direct NADPH regeneration10.1038/s41598-020-79761-62045-2322https://doaj.org/article/ad411539614147dc92701c9f044b2d362021-01-01T00:00:00Zhttps://doi.org/10.1038/s41598-020-79761-6https://doaj.org/toc/2045-2322Abstract Nearly a fourth of all enzymatic activities is attributable to oxidoreductases, and the redox reactions supported by this vast catalytic repertoire sustain cellular metabolism. In many biological processes, reduction depends on hydride transfer from either reduced nicotinamide adenine dinucleotide (NADH) or its phosphorylated derivative (NADPH). Despite longstanding efforts to regenerate NADPH by various methods and harness it to support chemoenzymatic synthesis strategies, the lack of product purity has been a major deterrent. Here, we demonstrate that a nanostructured heterolayer Ni–Cu2O–Cu cathode formed by a photoelectrochemical process has unexpected efficiency in direct electrochemical regeneration of NADPH from NADP+. Remarkably, two-thirds of NADP+ was converted to NADPH with no measurable production of the inactive (NADP)2 dimer and at the lowest reported overpotential [− 0.75 V versus Ag/AgCl (3 M NaCl) reference]. Sputtering of nickel on the copper-oxide electrode nucleated an unexpected surface morphology that was critical for high product selectivity. Our results should motivate design of integrated electrolyzer platforms that deploy this heterogeneous catalyst for direct electrochemical regeneration of NADH/NADPH, which is central to design of next-generation biofuel fermentation strategies, biological solar converters, energy-storage devices, and artificial photosynthesis.J. T. KadowakiT. H. JonesA. SenguptaV. GopalanV. V. SubramaniamNature PortfolioarticleMedicineRScienceQENScientific Reports, Vol 11, Iss 1, Pp 1-12 (2021)
institution	DOAJ
collection	DOAJ
language	EN
topic	Medicine R Science Q
spellingShingle	Medicine R Science Q J. T. Kadowaki T. H. Jones A. Sengupta V. Gopalan V. V. Subramaniam Copper oxide-based cathode for direct NADPH regeneration
description	Abstract Nearly a fourth of all enzymatic activities is attributable to oxidoreductases, and the redox reactions supported by this vast catalytic repertoire sustain cellular metabolism. In many biological processes, reduction depends on hydride transfer from either reduced nicotinamide adenine dinucleotide (NADH) or its phosphorylated derivative (NADPH). Despite longstanding efforts to regenerate NADPH by various methods and harness it to support chemoenzymatic synthesis strategies, the lack of product purity has been a major deterrent. Here, we demonstrate that a nanostructured heterolayer Ni–Cu2O–Cu cathode formed by a photoelectrochemical process has unexpected efficiency in direct electrochemical regeneration of NADPH from NADP+. Remarkably, two-thirds of NADP+ was converted to NADPH with no measurable production of the inactive (NADP)2 dimer and at the lowest reported overpotential [− 0.75 V versus Ag/AgCl (3 M NaCl) reference]. Sputtering of nickel on the copper-oxide electrode nucleated an unexpected surface morphology that was critical for high product selectivity. Our results should motivate design of integrated electrolyzer platforms that deploy this heterogeneous catalyst for direct electrochemical regeneration of NADH/NADPH, which is central to design of next-generation biofuel fermentation strategies, biological solar converters, energy-storage devices, and artificial photosynthesis.
format	article
author	J. T. Kadowaki T. H. Jones A. Sengupta V. Gopalan V. V. Subramaniam
author_facet	J. T. Kadowaki T. H. Jones A. Sengupta V. Gopalan V. V. Subramaniam
author_sort	J. T. Kadowaki
title	Copper oxide-based cathode for direct NADPH regeneration
title_short	Copper oxide-based cathode for direct NADPH regeneration
title_full	Copper oxide-based cathode for direct NADPH regeneration
title_fullStr	Copper oxide-based cathode for direct NADPH regeneration
title_full_unstemmed	Copper oxide-based cathode for direct NADPH regeneration
title_sort	copper oxide-based cathode for direct nadph regeneration
publisher	Nature Portfolio
publishDate	2021
url	https://doaj.org/article/ad411539614147dc92701c9f044b2d36
work_keys_str_mv	AT jtkadowaki copperoxidebasedcathodefordirectnadphregeneration AT thjones copperoxidebasedcathodefordirectnadphregeneration AT asengupta copperoxidebasedcathodefordirectnadphregeneration AT vgopalan copperoxidebasedcathodefordirectnadphregeneration AT vvsubramaniam copperoxidebasedcathodefordirectnadphregeneration
_version_	1718395246232993792

Copper oxide-based cathode for direct NADPH regeneration

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