Electronic structure of aqueous two-dimensional photocatalyst

Abstract The electronic structure, in particular the band edge position, of photocatalyst in presence of water is critical for photocatalytic water splitting. We propose a direct and systematic density functional theory (DFT) scheme to quantitatively predict band edge shifts and their microscopic or...

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Autores principales:	Dawei Kang, Xianghua Kong, Vincent Michaud-Rioux, Ying-Chih Chen, Zetian Mi, Hong Guo
Formato:	article
Lenguaje:	EN
Publicado:	Nature Portfolio 2021
Materias:	Materials of engineering and construction. Mechanics of materials TA401-492 Computer software QA76.75-76.765
Acceso en línea:	https://doaj.org/article/dabbe38067e446e3b253f6b2172d78da
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spelling	oai:doaj.org-article:dabbe38067e446e3b253f6b2172d78da2021-12-02T18:15:28ZElectronic structure of aqueous two-dimensional photocatalyst10.1038/s41524-021-00516-62057-3960https://doaj.org/article/dabbe38067e446e3b253f6b2172d78da2021-04-01T00:00:00Zhttps://doi.org/10.1038/s41524-021-00516-6https://doaj.org/toc/2057-3960Abstract The electronic structure, in particular the band edge position, of photocatalyst in presence of water is critical for photocatalytic water splitting. We propose a direct and systematic density functional theory (DFT) scheme to quantitatively predict band edge shifts and their microscopic origins for aqueous 2D photocatalyst, where thousands of atoms or more are able to be involved. This scheme is indispensable to correctly calculate the electronic structure of 2D photocatalyst in the presence of water, which is demonstrated in aqueous MoS2, GaS, InSe, GaSe and InS. It is found that the band edge of 2D photocatalysts are not rigidly shifted due to water as reported in previous studies of aqueous systems. Specifically, the CBM shift is quantitatively explained by geometric deformation, water dipole and charge redistribution effect while the fourth effect, i.e., interfacial chemical contact, is revealed in the VBM shift. Moreover, the revealed upshift of CBM in aqueous MoS2 should thermodynamically help carriers to participate in hydrogen evolution reaction (HER), which underpin the reported experimental findings that MoS2 is an efficient HER photocatalyst. Our work paves the way to design 2D materials in general as low-cost and high-efficiency photocatalysts.Dawei KangXianghua KongVincent Michaud-RiouxYing-Chih ChenZetian MiHong GuoNature PortfolioarticleMaterials of engineering and construction. Mechanics of materialsTA401-492Computer softwareQA76.75-76.765ENnpj Computational Materials, Vol 7, Iss 1, Pp 1-9 (2021)
institution	DOAJ
collection	DOAJ
language	EN
topic	Materials of engineering and construction. Mechanics of materials TA401-492 Computer software QA76.75-76.765
spellingShingle	Materials of engineering and construction. Mechanics of materials TA401-492 Computer software QA76.75-76.765 Dawei Kang Xianghua Kong Vincent Michaud-Rioux Ying-Chih Chen Zetian Mi Hong Guo Electronic structure of aqueous two-dimensional photocatalyst
description	Abstract The electronic structure, in particular the band edge position, of photocatalyst in presence of water is critical for photocatalytic water splitting. We propose a direct and systematic density functional theory (DFT) scheme to quantitatively predict band edge shifts and their microscopic origins for aqueous 2D photocatalyst, where thousands of atoms or more are able to be involved. This scheme is indispensable to correctly calculate the electronic structure of 2D photocatalyst in the presence of water, which is demonstrated in aqueous MoS2, GaS, InSe, GaSe and InS. It is found that the band edge of 2D photocatalysts are not rigidly shifted due to water as reported in previous studies of aqueous systems. Specifically, the CBM shift is quantitatively explained by geometric deformation, water dipole and charge redistribution effect while the fourth effect, i.e., interfacial chemical contact, is revealed in the VBM shift. Moreover, the revealed upshift of CBM in aqueous MoS2 should thermodynamically help carriers to participate in hydrogen evolution reaction (HER), which underpin the reported experimental findings that MoS2 is an efficient HER photocatalyst. Our work paves the way to design 2D materials in general as low-cost and high-efficiency photocatalysts.
format	article
author	Dawei Kang Xianghua Kong Vincent Michaud-Rioux Ying-Chih Chen Zetian Mi Hong Guo
author_facet	Dawei Kang Xianghua Kong Vincent Michaud-Rioux Ying-Chih Chen Zetian Mi Hong Guo
author_sort	Dawei Kang
title	Electronic structure of aqueous two-dimensional photocatalyst
title_short	Electronic structure of aqueous two-dimensional photocatalyst
title_full	Electronic structure of aqueous two-dimensional photocatalyst
title_fullStr	Electronic structure of aqueous two-dimensional photocatalyst
title_full_unstemmed	Electronic structure of aqueous two-dimensional photocatalyst
title_sort	electronic structure of aqueous two-dimensional photocatalyst
publisher	Nature Portfolio
publishDate	2021
url	https://doaj.org/article/dabbe38067e446e3b253f6b2172d78da
work_keys_str_mv	AT daweikang electronicstructureofaqueoustwodimensionalphotocatalyst AT xianghuakong electronicstructureofaqueoustwodimensionalphotocatalyst AT vincentmichaudrioux electronicstructureofaqueoustwodimensionalphotocatalyst AT yingchihchen electronicstructureofaqueoustwodimensionalphotocatalyst AT zetianmi electronicstructureofaqueoustwodimensionalphotocatalyst AT hongguo electronicstructureofaqueoustwodimensionalphotocatalyst
_version_	1718378425238945792

Electronic structure of aqueous two-dimensional photocatalyst

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