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Mimicking reductive dehalogenases for efficient electrocatalytic water dechlorination
Electrochemical technology is a robust approach to removing toxic and persistent chlorinated organic pollutants from water; however, it remains a challenge to design electrocatalysts with high activity and selectivity as elaborately as natural reductive dehalogenases. Here we report the design of hi...
Autores principales: | , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group UK
2023
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10447495/ https://www.ncbi.nlm.nih.gov/pubmed/37612275 http://dx.doi.org/10.1038/s41467-023-40906-6 |
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author | Min, Yuan Mei, Shu-Chuan Pan, Xiao-Qiang Chen, Jie-Jie Yu, Han-Qing Xiong, Yujie |
author_facet | Min, Yuan Mei, Shu-Chuan Pan, Xiao-Qiang Chen, Jie-Jie Yu, Han-Qing Xiong, Yujie |
author_sort | Min, Yuan |
collection | PubMed |
description | Electrochemical technology is a robust approach to removing toxic and persistent chlorinated organic pollutants from water; however, it remains a challenge to design electrocatalysts with high activity and selectivity as elaborately as natural reductive dehalogenases. Here we report the design of high-performance electrocatalysts toward water dechlorination by mimicking the binding pocket configuration and catalytic center of reductive dehalogenases. Specifically, our designed electrocatalyst is an assembled heterostructure by sandwiching a molecular catalyst into the interlayers of two-dimensional graphene oxide. The electrocatalyst exhibits excellent dechlorination performance, which enhances reduction of intermediate dichloroacetic acid by 7.8 folds against that without sandwich configuration and can selectively generate monochloro-groups from trichloro-groups. Molecular simulations suggest that the sandwiched inner space plays an essential role in tuning solvation shell, altering protonation state and facilitating carbon−chlorine bond cleavage. This work demonstrates the concept of mimicking natural reductive dehalogenases toward the sustainable treatment of organohalogen-contaminated water and wastewater. |
format | Online Article Text |
id | pubmed-10447495 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2023 |
publisher | Nature Publishing Group UK |
record_format | MEDLINE/PubMed |
spelling | pubmed-104474952023-08-25 Mimicking reductive dehalogenases for efficient electrocatalytic water dechlorination Min, Yuan Mei, Shu-Chuan Pan, Xiao-Qiang Chen, Jie-Jie Yu, Han-Qing Xiong, Yujie Nat Commun Article Electrochemical technology is a robust approach to removing toxic and persistent chlorinated organic pollutants from water; however, it remains a challenge to design electrocatalysts with high activity and selectivity as elaborately as natural reductive dehalogenases. Here we report the design of high-performance electrocatalysts toward water dechlorination by mimicking the binding pocket configuration and catalytic center of reductive dehalogenases. Specifically, our designed electrocatalyst is an assembled heterostructure by sandwiching a molecular catalyst into the interlayers of two-dimensional graphene oxide. The electrocatalyst exhibits excellent dechlorination performance, which enhances reduction of intermediate dichloroacetic acid by 7.8 folds against that without sandwich configuration and can selectively generate monochloro-groups from trichloro-groups. Molecular simulations suggest that the sandwiched inner space plays an essential role in tuning solvation shell, altering protonation state and facilitating carbon−chlorine bond cleavage. This work demonstrates the concept of mimicking natural reductive dehalogenases toward the sustainable treatment of organohalogen-contaminated water and wastewater. Nature Publishing Group UK 2023-08-23 /pmc/articles/PMC10447495/ /pubmed/37612275 http://dx.doi.org/10.1038/s41467-023-40906-6 Text en © The Author(s) 2023 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 licence, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons licence 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 licence, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) . |
spellingShingle | Article Min, Yuan Mei, Shu-Chuan Pan, Xiao-Qiang Chen, Jie-Jie Yu, Han-Qing Xiong, Yujie Mimicking reductive dehalogenases for efficient electrocatalytic water dechlorination |
title | Mimicking reductive dehalogenases for efficient electrocatalytic water dechlorination |
title_full | Mimicking reductive dehalogenases for efficient electrocatalytic water dechlorination |
title_fullStr | Mimicking reductive dehalogenases for efficient electrocatalytic water dechlorination |
title_full_unstemmed | Mimicking reductive dehalogenases for efficient electrocatalytic water dechlorination |
title_short | Mimicking reductive dehalogenases for efficient electrocatalytic water dechlorination |
title_sort | mimicking reductive dehalogenases for efficient electrocatalytic water dechlorination |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10447495/ https://www.ncbi.nlm.nih.gov/pubmed/37612275 http://dx.doi.org/10.1038/s41467-023-40906-6 |
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