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Influence of Excess Charge on Water Adsorption on the BiVO(4)(010) Surface

[Image: see text] We present a combined computational and experimental study of the adsorption of water on the Mo-doped BiVO(4)(010) surface, revealing how excess electrons influence the dissociation of water and lead to hydroxyl-induced alterations of the surface electronic structure. By comparing...

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Autores principales: Wang, Wennie, Favaro, Marco, Chen, Emily, Trotochaud, Lena, Bluhm, Hendrik, Choi, Kyoung-Shin, van de Krol, Roel, Starr, David E., Galli, Giulia
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2022
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9501793/
https://www.ncbi.nlm.nih.gov/pubmed/36074011
http://dx.doi.org/10.1021/jacs.2c07501
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author Wang, Wennie
Favaro, Marco
Chen, Emily
Trotochaud, Lena
Bluhm, Hendrik
Choi, Kyoung-Shin
van de Krol, Roel
Starr, David E.
Galli, Giulia
author_facet Wang, Wennie
Favaro, Marco
Chen, Emily
Trotochaud, Lena
Bluhm, Hendrik
Choi, Kyoung-Shin
van de Krol, Roel
Starr, David E.
Galli, Giulia
author_sort Wang, Wennie
collection PubMed
description [Image: see text] We present a combined computational and experimental study of the adsorption of water on the Mo-doped BiVO(4)(010) surface, revealing how excess electrons influence the dissociation of water and lead to hydroxyl-induced alterations of the surface electronic structure. By comparing ambient pressure resonant photoemission spectroscopy (AP-ResPES) measurements with the results of first-principles calculations, we show that the dissociation of water on the stoichiometric Mo-doped BiVO(4)(010) surface stabilizes the formation of a small electron polaron on the VO(4) tetrahedral site and leads to an enhanced concentration of localized electronic charge at the surface. Our calculations demonstrate that the dissociated water accounts for the enhanced V(4+) signal observed in ambient pressure X-ray photoelectron spectroscopy and the enhanced signal of a small electron polaron inter-band state observed in AP-ResPES measurements. For ternary oxide surfaces, which may contain oxygen vacancies in addition to other electron-donating dopants, our study reveals the importance of defects in altering the surface reactivity toward water and the concomitant water-induced modifications to the electronic structure.
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spelling pubmed-95017932022-09-24 Influence of Excess Charge on Water Adsorption on the BiVO(4)(010) Surface Wang, Wennie Favaro, Marco Chen, Emily Trotochaud, Lena Bluhm, Hendrik Choi, Kyoung-Shin van de Krol, Roel Starr, David E. Galli, Giulia J Am Chem Soc [Image: see text] We present a combined computational and experimental study of the adsorption of water on the Mo-doped BiVO(4)(010) surface, revealing how excess electrons influence the dissociation of water and lead to hydroxyl-induced alterations of the surface electronic structure. By comparing ambient pressure resonant photoemission spectroscopy (AP-ResPES) measurements with the results of first-principles calculations, we show that the dissociation of water on the stoichiometric Mo-doped BiVO(4)(010) surface stabilizes the formation of a small electron polaron on the VO(4) tetrahedral site and leads to an enhanced concentration of localized electronic charge at the surface. Our calculations demonstrate that the dissociated water accounts for the enhanced V(4+) signal observed in ambient pressure X-ray photoelectron spectroscopy and the enhanced signal of a small electron polaron inter-band state observed in AP-ResPES measurements. For ternary oxide surfaces, which may contain oxygen vacancies in addition to other electron-donating dopants, our study reveals the importance of defects in altering the surface reactivity toward water and the concomitant water-induced modifications to the electronic structure. American Chemical Society 2022-09-08 2022-09-21 /pmc/articles/PMC9501793/ /pubmed/36074011 http://dx.doi.org/10.1021/jacs.2c07501 Text en © 2022 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Wang, Wennie
Favaro, Marco
Chen, Emily
Trotochaud, Lena
Bluhm, Hendrik
Choi, Kyoung-Shin
van de Krol, Roel
Starr, David E.
Galli, Giulia
Influence of Excess Charge on Water Adsorption on the BiVO(4)(010) Surface
title Influence of Excess Charge on Water Adsorption on the BiVO(4)(010) Surface
title_full Influence of Excess Charge on Water Adsorption on the BiVO(4)(010) Surface
title_fullStr Influence of Excess Charge on Water Adsorption on the BiVO(4)(010) Surface
title_full_unstemmed Influence of Excess Charge on Water Adsorption on the BiVO(4)(010) Surface
title_short Influence of Excess Charge on Water Adsorption on the BiVO(4)(010) Surface
title_sort influence of excess charge on water adsorption on the bivo(4)(010) surface
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9501793/
https://www.ncbi.nlm.nih.gov/pubmed/36074011
http://dx.doi.org/10.1021/jacs.2c07501
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