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Atomistic insights into highly active reconstructed edges of monolayer 2H-WSe(2) photocatalyst
Ascertaining the function of in-plane intrinsic defects and edge atoms is necessary for developing efficient low-dimensional photocatalysts. We report the wireless photocatalytic CO(2) reduction to CH(4) over reconstructed edge atoms of monolayer 2H-WSe(2) artificial leaves. Our first-principles cal...
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/PMC8913837/ https://www.ncbi.nlm.nih.gov/pubmed/35273184 http://dx.doi.org/10.1038/s41467-022-28926-0 |
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author | Qorbani, Mohammad Sabbah, Amr Lai, Ying-Ren Kholimatussadiah, Septia Quadir, Shaham Huang, Chih-Yang Shown, Indrajit Huang, Yi-Fan Hayashi, Michitoshi Chen, Kuei-Hsien Chen, Li-Chyong |
author_facet | Qorbani, Mohammad Sabbah, Amr Lai, Ying-Ren Kholimatussadiah, Septia Quadir, Shaham Huang, Chih-Yang Shown, Indrajit Huang, Yi-Fan Hayashi, Michitoshi Chen, Kuei-Hsien Chen, Li-Chyong |
author_sort | Qorbani, Mohammad |
collection | PubMed |
description | Ascertaining the function of in-plane intrinsic defects and edge atoms is necessary for developing efficient low-dimensional photocatalysts. We report the wireless photocatalytic CO(2) reduction to CH(4) over reconstructed edge atoms of monolayer 2H-WSe(2) artificial leaves. Our first-principles calculations demonstrate that reconstructed and imperfect edge configurations enable CO(2) binding to form linear and bent molecules. Experimental results show that the solar-to-fuel quantum efficiency is a reciprocal function of the flake size. It also indicates that the consumed electron rate per edge atom is two orders of magnitude larger than the in-plane intrinsic defects. Further, nanoscale redox mapping at the monolayer WSe(2)–liquid interface confirms that the edge is the most preferred region for charge transfer. Our results pave the way for designing a new class of monolayer transition metal dichalcogenides with reconstructed edges as a non-precious co-catalyst for wired or wireless hydrogen evolution or CO(2) reduction reactions. |
format | Online Article Text |
id | pubmed-8913837 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2022 |
publisher | Nature Publishing Group UK |
record_format | MEDLINE/PubMed |
spelling | pubmed-89138372022-04-20 Atomistic insights into highly active reconstructed edges of monolayer 2H-WSe(2) photocatalyst Qorbani, Mohammad Sabbah, Amr Lai, Ying-Ren Kholimatussadiah, Septia Quadir, Shaham Huang, Chih-Yang Shown, Indrajit Huang, Yi-Fan Hayashi, Michitoshi Chen, Kuei-Hsien Chen, Li-Chyong Nat Commun Article Ascertaining the function of in-plane intrinsic defects and edge atoms is necessary for developing efficient low-dimensional photocatalysts. We report the wireless photocatalytic CO(2) reduction to CH(4) over reconstructed edge atoms of monolayer 2H-WSe(2) artificial leaves. Our first-principles calculations demonstrate that reconstructed and imperfect edge configurations enable CO(2) binding to form linear and bent molecules. Experimental results show that the solar-to-fuel quantum efficiency is a reciprocal function of the flake size. It also indicates that the consumed electron rate per edge atom is two orders of magnitude larger than the in-plane intrinsic defects. Further, nanoscale redox mapping at the monolayer WSe(2)–liquid interface confirms that the edge is the most preferred region for charge transfer. Our results pave the way for designing a new class of monolayer transition metal dichalcogenides with reconstructed edges as a non-precious co-catalyst for wired or wireless hydrogen evolution or CO(2) reduction reactions. Nature Publishing Group UK 2022-03-10 /pmc/articles/PMC8913837/ /pubmed/35273184 http://dx.doi.org/10.1038/s41467-022-28926-0 Text en © The Author(s) 2022, corrected publication 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 Qorbani, Mohammad Sabbah, Amr Lai, Ying-Ren Kholimatussadiah, Septia Quadir, Shaham Huang, Chih-Yang Shown, Indrajit Huang, Yi-Fan Hayashi, Michitoshi Chen, Kuei-Hsien Chen, Li-Chyong Atomistic insights into highly active reconstructed edges of monolayer 2H-WSe(2) photocatalyst |
title | Atomistic insights into highly active reconstructed edges of monolayer 2H-WSe(2) photocatalyst |
title_full | Atomistic insights into highly active reconstructed edges of monolayer 2H-WSe(2) photocatalyst |
title_fullStr | Atomistic insights into highly active reconstructed edges of monolayer 2H-WSe(2) photocatalyst |
title_full_unstemmed | Atomistic insights into highly active reconstructed edges of monolayer 2H-WSe(2) photocatalyst |
title_short | Atomistic insights into highly active reconstructed edges of monolayer 2H-WSe(2) photocatalyst |
title_sort | atomistic insights into highly active reconstructed edges of monolayer 2h-wse(2) photocatalyst |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8913837/ https://www.ncbi.nlm.nih.gov/pubmed/35273184 http://dx.doi.org/10.1038/s41467-022-28926-0 |
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