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Heat-fueled enzymatic cascade for selective oxyfunctionalization of hydrocarbons

Heat is a fundamental feedstock, where more than 80% of global energy comes from fossil-based heating process. However, it is mostly wasted due to a lack of proper techniques of utilizing the low-quality waste heat (<100 °C). Here we report thermoelectrobiocatalytic chemical conversion systems fo...

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Autores principales: Yoon, Jaeho, Jang, Hanhwi, Oh, Min-Wook, Hilberath, Thomas, Hollmann, Frank, Jung, Yeon Sik, Park, Chan Beum
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9243031/
https://www.ncbi.nlm.nih.gov/pubmed/35768427
http://dx.doi.org/10.1038/s41467-022-31363-8
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author Yoon, Jaeho
Jang, Hanhwi
Oh, Min-Wook
Hilberath, Thomas
Hollmann, Frank
Jung, Yeon Sik
Park, Chan Beum
author_facet Yoon, Jaeho
Jang, Hanhwi
Oh, Min-Wook
Hilberath, Thomas
Hollmann, Frank
Jung, Yeon Sik
Park, Chan Beum
author_sort Yoon, Jaeho
collection PubMed
description Heat is a fundamental feedstock, where more than 80% of global energy comes from fossil-based heating process. However, it is mostly wasted due to a lack of proper techniques of utilizing the low-quality waste heat (<100 °C). Here we report thermoelectrobiocatalytic chemical conversion systems for heat-fueled, enzyme-catalyzed oxyfunctionalization reactions. Thermoelectric bismuth telluride (Bi(2)Te(3)) directly converts low-temperature waste heat into chemical energy in the form of H(2)O(2) near room temperature. The streamlined reaction scheme (e.g., water, heat, enzyme, and thermoelectric material) promotes enantio- and chemo-selective hydroxylation and epoxidation of representative substrates (e.g., ethylbenzene, propylbenzene, tetralin, cyclohexane, cis-β-methylstyrene), achieving a maximum total turnover number of rAaeUPO (TTN(rAaeUPO)) over 32000. Direct conversion of vehicle exhaust heat into the enantiopure enzymatic product with a rate of 231.4 μM h(−1) during urban driving envisions the practical feasibility of thermoelectrobiocatalysis.
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spelling pubmed-92430312022-07-01 Heat-fueled enzymatic cascade for selective oxyfunctionalization of hydrocarbons Yoon, Jaeho Jang, Hanhwi Oh, Min-Wook Hilberath, Thomas Hollmann, Frank Jung, Yeon Sik Park, Chan Beum Nat Commun Article Heat is a fundamental feedstock, where more than 80% of global energy comes from fossil-based heating process. However, it is mostly wasted due to a lack of proper techniques of utilizing the low-quality waste heat (<100 °C). Here we report thermoelectrobiocatalytic chemical conversion systems for heat-fueled, enzyme-catalyzed oxyfunctionalization reactions. Thermoelectric bismuth telluride (Bi(2)Te(3)) directly converts low-temperature waste heat into chemical energy in the form of H(2)O(2) near room temperature. The streamlined reaction scheme (e.g., water, heat, enzyme, and thermoelectric material) promotes enantio- and chemo-selective hydroxylation and epoxidation of representative substrates (e.g., ethylbenzene, propylbenzene, tetralin, cyclohexane, cis-β-methylstyrene), achieving a maximum total turnover number of rAaeUPO (TTN(rAaeUPO)) over 32000. Direct conversion of vehicle exhaust heat into the enantiopure enzymatic product with a rate of 231.4 μM h(−1) during urban driving envisions the practical feasibility of thermoelectrobiocatalysis. Nature Publishing Group UK 2022-06-29 /pmc/articles/PMC9243031/ /pubmed/35768427 http://dx.doi.org/10.1038/s41467-022-31363-8 Text en © The Author(s) 2022 https://creativecommons.org/licenses/by/4.0/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/ (https://creativecommons.org/licenses/by/4.0/) .
spellingShingle Article
Yoon, Jaeho
Jang, Hanhwi
Oh, Min-Wook
Hilberath, Thomas
Hollmann, Frank
Jung, Yeon Sik
Park, Chan Beum
Heat-fueled enzymatic cascade for selective oxyfunctionalization of hydrocarbons
title Heat-fueled enzymatic cascade for selective oxyfunctionalization of hydrocarbons
title_full Heat-fueled enzymatic cascade for selective oxyfunctionalization of hydrocarbons
title_fullStr Heat-fueled enzymatic cascade for selective oxyfunctionalization of hydrocarbons
title_full_unstemmed Heat-fueled enzymatic cascade for selective oxyfunctionalization of hydrocarbons
title_short Heat-fueled enzymatic cascade for selective oxyfunctionalization of hydrocarbons
title_sort heat-fueled enzymatic cascade for selective oxyfunctionalization of hydrocarbons
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9243031/
https://www.ncbi.nlm.nih.gov/pubmed/35768427
http://dx.doi.org/10.1038/s41467-022-31363-8
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