Self-carbon-thermal-reduction strategy for boosting the Fenton-like activity of single Fe-N(4) sites by carbon-defect engineering
Carbon-defect engineering in metal single-atom catalysts by simple and robust strategy, boosting their catalytic activity, and revealing the carbon defect-catalytic activity relationship are meaningful but challenging. Herein, we report a facile self-carbon-thermal-reduction strategy for carbon-defe...
Autores principales: | , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
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Nature Publishing Group UK
2023
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10662205/ https://www.ncbi.nlm.nih.gov/pubmed/37985662 http://dx.doi.org/10.1038/s41467-023-43040-5 |
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author | Wei, Shengjie Sun, Yibing Qiu, Yun-Ze Li, Ang Chiang, Ching-Yu Xiao, Hai Qian, Jieshu Li, Yadong |
author_facet | Wei, Shengjie Sun, Yibing Qiu, Yun-Ze Li, Ang Chiang, Ching-Yu Xiao, Hai Qian, Jieshu Li, Yadong |
author_sort | Wei, Shengjie |
collection | PubMed |
description | Carbon-defect engineering in metal single-atom catalysts by simple and robust strategy, boosting their catalytic activity, and revealing the carbon defect-catalytic activity relationship are meaningful but challenging. Herein, we report a facile self-carbon-thermal-reduction strategy for carbon-defect engineering of single Fe-N(4) sites in ZnO-Carbon nano-reactor, as efficient catalyst in Fenton-like reaction for degradation of phenol. The carbon vacancies are easily constructed adjacent to single Fe-N(4) sites during synthesis, facilitating the formation of C-O bonding and lowering the energy barrier of rate-determining-step during degradation of phenol. Consequently, the catalyst Fe-NCv-900 with carbon vacancies exhibits a much improved activity than the Fe-NC-900 without abundant carbon vacancies, with 13.5 times improvement in the first-order rate constant of phenol degradation. The Fe-NCv-900 shows high activity (97% removal ratio of phenol in only 5 min), good recyclability and the wide-ranging pH universality (pH range 3-9). This work not only provides a rational strategy for improving the Fenton-like activity of metal single-atom catalysts, but also deepens the fundamental understanding on how periphery carbon environment affects the property and performance of metal-N(4) sites. |
format | Online Article Text |
id | pubmed-10662205 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2023 |
publisher | Nature Publishing Group UK |
record_format | MEDLINE/PubMed |
spelling | pubmed-106622052023-11-20 Self-carbon-thermal-reduction strategy for boosting the Fenton-like activity of single Fe-N(4) sites by carbon-defect engineering Wei, Shengjie Sun, Yibing Qiu, Yun-Ze Li, Ang Chiang, Ching-Yu Xiao, Hai Qian, Jieshu Li, Yadong Nat Commun Article Carbon-defect engineering in metal single-atom catalysts by simple and robust strategy, boosting their catalytic activity, and revealing the carbon defect-catalytic activity relationship are meaningful but challenging. Herein, we report a facile self-carbon-thermal-reduction strategy for carbon-defect engineering of single Fe-N(4) sites in ZnO-Carbon nano-reactor, as efficient catalyst in Fenton-like reaction for degradation of phenol. The carbon vacancies are easily constructed adjacent to single Fe-N(4) sites during synthesis, facilitating the formation of C-O bonding and lowering the energy barrier of rate-determining-step during degradation of phenol. Consequently, the catalyst Fe-NCv-900 with carbon vacancies exhibits a much improved activity than the Fe-NC-900 without abundant carbon vacancies, with 13.5 times improvement in the first-order rate constant of phenol degradation. The Fe-NCv-900 shows high activity (97% removal ratio of phenol in only 5 min), good recyclability and the wide-ranging pH universality (pH range 3-9). This work not only provides a rational strategy for improving the Fenton-like activity of metal single-atom catalysts, but also deepens the fundamental understanding on how periphery carbon environment affects the property and performance of metal-N(4) sites. Nature Publishing Group UK 2023-11-20 /pmc/articles/PMC10662205/ /pubmed/37985662 http://dx.doi.org/10.1038/s41467-023-43040-5 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 Wei, Shengjie Sun, Yibing Qiu, Yun-Ze Li, Ang Chiang, Ching-Yu Xiao, Hai Qian, Jieshu Li, Yadong Self-carbon-thermal-reduction strategy for boosting the Fenton-like activity of single Fe-N(4) sites by carbon-defect engineering |
title | Self-carbon-thermal-reduction strategy for boosting the Fenton-like activity of single Fe-N(4) sites by carbon-defect engineering |
title_full | Self-carbon-thermal-reduction strategy for boosting the Fenton-like activity of single Fe-N(4) sites by carbon-defect engineering |
title_fullStr | Self-carbon-thermal-reduction strategy for boosting the Fenton-like activity of single Fe-N(4) sites by carbon-defect engineering |
title_full_unstemmed | Self-carbon-thermal-reduction strategy for boosting the Fenton-like activity of single Fe-N(4) sites by carbon-defect engineering |
title_short | Self-carbon-thermal-reduction strategy for boosting the Fenton-like activity of single Fe-N(4) sites by carbon-defect engineering |
title_sort | self-carbon-thermal-reduction strategy for boosting the fenton-like activity of single fe-n(4) sites by carbon-defect engineering |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10662205/ https://www.ncbi.nlm.nih.gov/pubmed/37985662 http://dx.doi.org/10.1038/s41467-023-43040-5 |
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