Mimicking reductive dehalogenases for efficient electrocatalytic water dechlorination
Abstract 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 des...
| Main Authors: | , , , , , |
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2023-08-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-023-40906-6 |
| _version_ | 1797558042427916288 |
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| author | Yuan Min Shu-Chuan Mei Xiao-Qiang Pan Jie-Jie Chen Han-Qing Yu Yujie Xiong |
| author_facet | Yuan Min Shu-Chuan Mei Xiao-Qiang Pan Jie-Jie Chen Han-Qing Yu Yujie Xiong |
| author_sort | Yuan Min |
| collection | DOAJ |
| description | Abstract 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. |
| first_indexed | 2024-03-10T17:24:50Z |
| format | Article |
| id | doaj.art-e4e07ea5194440e6918e9f8922364f45 |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-03-10T17:24:50Z |
| publishDate | 2023-08-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-e4e07ea5194440e6918e9f8922364f452023-11-20T10:13:49ZengNature PortfolioNature Communications2041-17232023-08-0114111010.1038/s41467-023-40906-6Mimicking reductive dehalogenases for efficient electrocatalytic water dechlorinationYuan Min0Shu-Chuan Mei1Xiao-Qiang Pan2Jie-Jie Chen3Han-Qing Yu4Yujie Xiong5Department of Environmental Science and Engineering, University of Science and Technology of ChinaDepartment of Environmental Science and Engineering, University of Science and Technology of ChinaDepartment of Environmental Science and Engineering, University of Science and Technology of ChinaDepartment of Environmental Science and Engineering, University of Science and Technology of ChinaDepartment of Environmental Science and Engineering, University of Science and Technology of ChinaHefei National Research Center for Physical Sciences at the Microscale, Collaborative Innovative Center of Chemistry for Energy Materials (iChEM), School of Chemistry and Materials Science, University of Science and Technology of ChinaAbstract 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.https://doi.org/10.1038/s41467-023-40906-6 |
| spellingShingle | Yuan Min Shu-Chuan Mei Xiao-Qiang Pan Jie-Jie Chen Han-Qing Yu Yujie Xiong Mimicking reductive dehalogenases for efficient electrocatalytic water dechlorination Nature Communications |
| 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 |
| url | https://doi.org/10.1038/s41467-023-40906-6 |
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