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...

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Autores principales: Wei, Shengjie, Sun, Yibing, Qiu, Yun-Ze, Li, Ang, Chiang, Ching-Yu, Xiao, Hai, Qian, Jieshu, Li, Yadong
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2023
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.
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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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