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Full-spectrum nonmetallic plasmonic carriers for efficient isopropanol dehydration
Plasmonic hot carriers have the advantage of focusing, amplifying, and manipulating optical signals via electron oscillations which offers a feasible pathway to influence catalytic reactions. However, the contribution of nonmetallic hot carriers and thermal effects on the overall reactions are still...
Autores principales: | , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group UK
2022
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9666589/ https://www.ncbi.nlm.nih.gov/pubmed/36379947 http://dx.doi.org/10.1038/s41467-022-34738-z |
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author | Lu, Changhai You, Daotong Li, Juan Wen, Long Li, Baojun Guo, Tuan Lou, Zaizhu |
author_facet | Lu, Changhai You, Daotong Li, Juan Wen, Long Li, Baojun Guo, Tuan Lou, Zaizhu |
author_sort | Lu, Changhai |
collection | PubMed |
description | Plasmonic hot carriers have the advantage of focusing, amplifying, and manipulating optical signals via electron oscillations which offers a feasible pathway to influence catalytic reactions. However, the contribution of nonmetallic hot carriers and thermal effects on the overall reactions are still unclear, and developing methods to enhance the efficiency of the catalysis is critical. Herein, we proposed a new strategy for flexibly modulating the hot electrons using a nonmetallic plasmonic heterostructure (named W(18)O(49)-nanowires/reduced-graphene-oxides) for isopropanol dehydration where the reaction rate was 180-fold greater than the corresponding thermocatalytic pathway. The key detail to this strategy lies in the synergetic utilization of ultraviolet light and visible-near-infrared light to enhance the hot electron generation and promote electron transfer for C-O bond cleavage during isopropanol dehydration reaction. This, in turn, results in a reduced reaction activation barrier down to 0.37 eV (compared to 1.0 eV of thermocatalysis) and a significantly improved conversion efficiency of 100% propylene from isopropanol. This work provides an additional strategy to modulate hot carrier of plasmonic semiconductors and helps guide the design of better catalytic materials and chemistries. |
format | Online Article Text |
id | pubmed-9666589 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2022 |
publisher | Nature Publishing Group UK |
record_format | MEDLINE/PubMed |
spelling | pubmed-96665892022-11-17 Full-spectrum nonmetallic plasmonic carriers for efficient isopropanol dehydration Lu, Changhai You, Daotong Li, Juan Wen, Long Li, Baojun Guo, Tuan Lou, Zaizhu Nat Commun Article Plasmonic hot carriers have the advantage of focusing, amplifying, and manipulating optical signals via electron oscillations which offers a feasible pathway to influence catalytic reactions. However, the contribution of nonmetallic hot carriers and thermal effects on the overall reactions are still unclear, and developing methods to enhance the efficiency of the catalysis is critical. Herein, we proposed a new strategy for flexibly modulating the hot electrons using a nonmetallic plasmonic heterostructure (named W(18)O(49)-nanowires/reduced-graphene-oxides) for isopropanol dehydration where the reaction rate was 180-fold greater than the corresponding thermocatalytic pathway. The key detail to this strategy lies in the synergetic utilization of ultraviolet light and visible-near-infrared light to enhance the hot electron generation and promote electron transfer for C-O bond cleavage during isopropanol dehydration reaction. This, in turn, results in a reduced reaction activation barrier down to 0.37 eV (compared to 1.0 eV of thermocatalysis) and a significantly improved conversion efficiency of 100% propylene from isopropanol. This work provides an additional strategy to modulate hot carrier of plasmonic semiconductors and helps guide the design of better catalytic materials and chemistries. Nature Publishing Group UK 2022-11-15 /pmc/articles/PMC9666589/ /pubmed/36379947 http://dx.doi.org/10.1038/s41467-022-34738-z 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 Lu, Changhai You, Daotong Li, Juan Wen, Long Li, Baojun Guo, Tuan Lou, Zaizhu Full-spectrum nonmetallic plasmonic carriers for efficient isopropanol dehydration |
title | Full-spectrum nonmetallic plasmonic carriers for efficient isopropanol dehydration |
title_full | Full-spectrum nonmetallic plasmonic carriers for efficient isopropanol dehydration |
title_fullStr | Full-spectrum nonmetallic plasmonic carriers for efficient isopropanol dehydration |
title_full_unstemmed | Full-spectrum nonmetallic plasmonic carriers for efficient isopropanol dehydration |
title_short | Full-spectrum nonmetallic plasmonic carriers for efficient isopropanol dehydration |
title_sort | full-spectrum nonmetallic plasmonic carriers for efficient isopropanol dehydration |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9666589/ https://www.ncbi.nlm.nih.gov/pubmed/36379947 http://dx.doi.org/10.1038/s41467-022-34738-z |
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