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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...

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Autores principales: 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
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2022
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.
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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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