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Unbiased biocatalytic solar-to-chemical conversion by FeOOH/BiVO(4)/perovskite tandem structure

Redox enzymes catalyze fascinating chemical reactions with excellent regio- and stereo-specificity. Nicotinamide adenine dinucleotide cofactor is essential in numerous redox biocatalytic reactions and needs to be regenerated because it is consumed as an equivalent during the enzymatic turnover. Here...

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Autores principales: Lee, Yang Woo, Boonmongkolras, Passarut, Son, Eun Jin, Kim, Jinhyun, Lee, Sahng Ha, Kuk, Su Keun, Ko, Jong Wan, Shin, Byungha, Park, Chan Beum
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2018
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6181951/
https://www.ncbi.nlm.nih.gov/pubmed/30310064
http://dx.doi.org/10.1038/s41467-018-06687-z
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author Lee, Yang Woo
Boonmongkolras, Passarut
Son, Eun Jin
Kim, Jinhyun
Lee, Sahng Ha
Kuk, Su Keun
Ko, Jong Wan
Shin, Byungha
Park, Chan Beum
author_facet Lee, Yang Woo
Boonmongkolras, Passarut
Son, Eun Jin
Kim, Jinhyun
Lee, Sahng Ha
Kuk, Su Keun
Ko, Jong Wan
Shin, Byungha
Park, Chan Beum
author_sort Lee, Yang Woo
collection PubMed
description Redox enzymes catalyze fascinating chemical reactions with excellent regio- and stereo-specificity. Nicotinamide adenine dinucleotide cofactor is essential in numerous redox biocatalytic reactions and needs to be regenerated because it is consumed as an equivalent during the enzymatic turnover. Here we report on unbiased photoelectrochemical tandem assembly of a photoanode (FeOOH/BiVO(4)) and a perovskite photovoltaic to provide sufficient potential for cofactor-dependent biocatalytic reactions. We obtain a high faradaic efficiency of 96.2% and an initial conversion rate of 2.4 mM h(−1) without an external applied bias for the photoelectrochemical enzymatic conversion of α-ketoglutarate to l-glutamate via l-glutamate dehydrogenase. In addition, we achieve a total turnover number and a turnover frequency of the enzyme of 108,800 and 6200 h(−1), respectively, demonstrating that the tandem configuration facilitates redox biocatalysis using light as the only energy source.
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spelling pubmed-61819512018-10-15 Unbiased biocatalytic solar-to-chemical conversion by FeOOH/BiVO(4)/perovskite tandem structure Lee, Yang Woo Boonmongkolras, Passarut Son, Eun Jin Kim, Jinhyun Lee, Sahng Ha Kuk, Su Keun Ko, Jong Wan Shin, Byungha Park, Chan Beum Nat Commun Article Redox enzymes catalyze fascinating chemical reactions with excellent regio- and stereo-specificity. Nicotinamide adenine dinucleotide cofactor is essential in numerous redox biocatalytic reactions and needs to be regenerated because it is consumed as an equivalent during the enzymatic turnover. Here we report on unbiased photoelectrochemical tandem assembly of a photoanode (FeOOH/BiVO(4)) and a perovskite photovoltaic to provide sufficient potential for cofactor-dependent biocatalytic reactions. We obtain a high faradaic efficiency of 96.2% and an initial conversion rate of 2.4 mM h(−1) without an external applied bias for the photoelectrochemical enzymatic conversion of α-ketoglutarate to l-glutamate via l-glutamate dehydrogenase. In addition, we achieve a total turnover number and a turnover frequency of the enzyme of 108,800 and 6200 h(−1), respectively, demonstrating that the tandem configuration facilitates redox biocatalysis using light as the only energy source. Nature Publishing Group UK 2018-10-11 /pmc/articles/PMC6181951/ /pubmed/30310064 http://dx.doi.org/10.1038/s41467-018-06687-z Text en © The Author(s) 2018 Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.
spellingShingle Article
Lee, Yang Woo
Boonmongkolras, Passarut
Son, Eun Jin
Kim, Jinhyun
Lee, Sahng Ha
Kuk, Su Keun
Ko, Jong Wan
Shin, Byungha
Park, Chan Beum
Unbiased biocatalytic solar-to-chemical conversion by FeOOH/BiVO(4)/perovskite tandem structure
title Unbiased biocatalytic solar-to-chemical conversion by FeOOH/BiVO(4)/perovskite tandem structure
title_full Unbiased biocatalytic solar-to-chemical conversion by FeOOH/BiVO(4)/perovskite tandem structure
title_fullStr Unbiased biocatalytic solar-to-chemical conversion by FeOOH/BiVO(4)/perovskite tandem structure
title_full_unstemmed Unbiased biocatalytic solar-to-chemical conversion by FeOOH/BiVO(4)/perovskite tandem structure
title_short Unbiased biocatalytic solar-to-chemical conversion by FeOOH/BiVO(4)/perovskite tandem structure
title_sort unbiased biocatalytic solar-to-chemical conversion by feooh/bivo(4)/perovskite tandem structure
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6181951/
https://www.ncbi.nlm.nih.gov/pubmed/30310064
http://dx.doi.org/10.1038/s41467-018-06687-z
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