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Site dependent reactivity of Pt single atoms on anatase TiO 2(101) in an aqueous environment
Abstract
The TiO 2–Pt–water interface is of great relevance in photocatalysis where Pt is widely used as a co-catalyst for The TiO 2–Pt–water interface is of great relevance in photocatalysis where Pt is widely used as a co-catalyst for enhancing hydrogen evolution in aqueous TiO 2. Using ab initio molecular dynamics, we investigated this interface focusing on Pt single atoms supported on anatase TiO 2(101) in a water environment. Based on recent experiments showing a broad distribution of Pt coordination sites in TiO 2, we examined six distinct single-Pt supported species with different nominal Pt oxidation states, namely: Pt, PtOH, and PtO 2 species adsorbed on the stoichiometric surface; Pt adsorbed at a surface oxygen vacancy (O v); and Pt substituting a surface Ti cation (PtTi), both without and with an accompanying O v (Pt Ti + O v). As found for the pristine anatase surface, interfacial water remained intact in the presence of a nearly neutral Pt adatom within the time duration of our simulations (~15 ps). Similarly, no (or only temporary) water dissociation was observed at the Pt Ti + O v and PtO 2 interfaces, due to the formation of very stable planar Pt coordination structures that interactmore »
- Authors:
-
[1];
[3];
- Beijing Computational Science Research Center, Beijing (China); Princeton Univ., NJ (United States)
- Hunan Univ. of Science and Technology, Xiangtan (China)
- Princeton Univ., NJ (United States)
- Beihang Univ., Beijing (China)
- Publication Date:
- Research Org.:
- Princeton Univ., NJ (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; National Natural Science Foundation of China (NNSFC); Tianhe-2JK
- OSTI Identifier:
- 1594492
- Grant/Contract Number:
- SC0007347; TZ20180; 51572016; U1930402; 11804090; 11847213; 51861130360; U1501501; NAFR1180242
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Chemistry Chemical Physics. PCCP (Print)
- Additional Journal Information:
- Journal Name: Physical Chemistry Chemical Physics. PCCP (Print); Journal ID: ISSN 1463-9076
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Wen, Bo, Yin, Wen-Jin, Selloni, Annabella, and Liu, Li-Min. Site dependent reactivity of Pt single atoms on anatase TiO2(101) in an aqueous environment. United States: N. p., 2019.
Web. doi:10.1039/C9CP05097C.
Wen, Bo, Yin, Wen-Jin, Selloni, Annabella, & Liu, Li-Min. Site dependent reactivity of Pt single atoms on anatase TiO2(101) in an aqueous environment. United States. doi:10.1039/C9CP05097C.
Wen, Bo, Yin, Wen-Jin, Selloni, Annabella, and Liu, Li-Min. Mon .
"Site dependent reactivity of Pt single atoms on anatase TiO2(101) in an aqueous environment". United States. doi:10.1039/C9CP05097C.
@article{osti_1594492,
title = {Site dependent reactivity of Pt single atoms on anatase TiO2(101) in an aqueous environment},
author = {Wen, Bo and Yin, Wen-Jin and Selloni, Annabella and Liu, Li-Min},
abstractNote = {The TiO2–Pt–water interface is of great relevance in photocatalysis where Pt is widely used as a co-catalyst for The TiO2–Pt–water interface is of great relevance in photocatalysis where Pt is widely used as a co-catalyst for enhancing hydrogen evolution in aqueous TiO2. Using ab initio molecular dynamics, we investigated this interface focusing on Pt single atoms supported on anatase TiO2(101) in a water environment. Based on recent experiments showing a broad distribution of Pt coordination sites in TiO2, we examined six distinct single-Pt supported species with different nominal Pt oxidation states, namely: Pt, PtOH, and PtO2 species adsorbed on the stoichiometric surface; Pt adsorbed at a surface oxygen vacancy (Ov); and Pt substituting a surface Ti cation (PtTi), both without and with an accompanying Ov (PtTi + Ov). As found for the pristine anatase surface, interfacial water remained intact in the presence of a nearly neutral Pt adatom within the time duration of our simulations (~15 ps). Similarly, no (or only temporary) water dissociation was observed at the PtTi + Ov and PtO2 interfaces, due to the formation of very stable planar Pt coordination structures that interact only weakly with water. In contrast, water dissociated with OH– (H+) on the Pt atom when this substituted a surface Ti (oxygen) ion as well as on PtOH. Lastly, the significant proton affinity of Pt atoms at surface oxygen vacancies suggests that negatively charged Pt species are particularly efficient at catalyzing hydrogen evolution in aqueous TiO2.hydrogen evolution in aqueous TiO2.},
doi = {10.1039/C9CP05097C},
journal = {Physical Chemistry Chemical Physics. PCCP (Print)},
number = ,
volume = ,
place = {United States},
year = {2019},
month = {10}
}
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DOI: 10.1039/C9CP05097C
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