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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...

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Autores principales: Lu, Changhai, You, Daotong, Li, Juan, Wen, Long, Li, Baojun, Guo, Tuan, Lou, Zaizhu
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2022
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.
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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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