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Title: Water Dissociates at the Aqueous Interface with Reduced Anatase TiO 2 (101)

Abstract

Elucidating the structure of the interface between natural (reduced) anatase TiO 2 (101) and water is an essential step toward understanding the associated photoassisted water splitting mechanism. In this work we present surface X-ray diffraction results for the room temperature interface with ultrathin and bulk water, which we explain by reference to density functional theory calculations. We find that both interfaces contain a 25:75 mixture of molecular H 2O and terminal OH bound to titanium atoms along with bridging OH species in the contact layer. This is in complete contrast to the inert character of room temperature anatase TiO 2 (101) in ultrahigh vacuum. A vital difference between the ultrathin and bulk water interfaces is that in the latter water in the second layer is also ordered. These molecules are hydrogen bonded to the contact layer, modifying the bond angles.

Authors:
 [1];  [2];  [3]; ORCiD logo [4];  [2];  [5];  [5];  [6];  [7];  [8]; ORCiD logo [3];  [8];  [2]; ORCiD logo [5]
  1. Univ. College London (UCL) (United Kingdom); Science and Technology Facilities Council (STFC), Harwell Campus, Oxford (United Kingdom). Diamond Light Source, Ltd.
  2. Univ. of Manchester (United Kingdom)
  3. Princeton Univ., NJ (United States)
  4. Institut de Ciència de Materials de Barcelona (CSIC) (Spain)
  5. Univ. College London (UCL) (United Kingdom)
  6. Sorbonne Université, Paris (France). Centre National de la Recherche Scientifique (CNRS)
  7. Univ. of Warwick (United Kingdom); European Synchrotron Radiation Facility (ESRF), Grenoble (France)
  8. Science and Technology Facilities Council (STFC), Harwell Campus, Oxford (United Kingdom). Diamond Light Source, Ltd.
Publication Date:
Research Org.:
Princeton Univ., NJ (United States); Univ. of California, Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division
OSTI Identifier:
1546605
Grant/Contract Number:  
[SC0007347; AC02-05CH11231]
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
[ Journal Volume: 9; Journal Issue: 11]; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Nadeem, Immad M., Treacy, Jon P. W., Selcuk, Sencer, Torrelles, Xavier, Hussain, Hadeel, Wilson, Axel, Grinter, David C., Cabailh, Gregory, Bikondoa, Oier, Nicklin, Christopher, Selloni, Annabella, Zegenhagen, Jörg, Lindsay, Robert, and Thornton, Geoff. Water Dissociates at the Aqueous Interface with Reduced Anatase TiO2 (101). United States: N. p., 2018. Web. doi:10.1021/acs.jpclett.8b01182.
Nadeem, Immad M., Treacy, Jon P. W., Selcuk, Sencer, Torrelles, Xavier, Hussain, Hadeel, Wilson, Axel, Grinter, David C., Cabailh, Gregory, Bikondoa, Oier, Nicklin, Christopher, Selloni, Annabella, Zegenhagen, Jörg, Lindsay, Robert, & Thornton, Geoff. Water Dissociates at the Aqueous Interface with Reduced Anatase TiO2 (101). United States. doi:10.1021/acs.jpclett.8b01182.
Nadeem, Immad M., Treacy, Jon P. W., Selcuk, Sencer, Torrelles, Xavier, Hussain, Hadeel, Wilson, Axel, Grinter, David C., Cabailh, Gregory, Bikondoa, Oier, Nicklin, Christopher, Selloni, Annabella, Zegenhagen, Jörg, Lindsay, Robert, and Thornton, Geoff. Wed . "Water Dissociates at the Aqueous Interface with Reduced Anatase TiO2 (101)". United States. doi:10.1021/acs.jpclett.8b01182. https://www.osti.gov/servlets/purl/1546605.
@article{osti_1546605,
title = {Water Dissociates at the Aqueous Interface with Reduced Anatase TiO2 (101)},
author = {Nadeem, Immad M. and Treacy, Jon P. W. and Selcuk, Sencer and Torrelles, Xavier and Hussain, Hadeel and Wilson, Axel and Grinter, David C. and Cabailh, Gregory and Bikondoa, Oier and Nicklin, Christopher and Selloni, Annabella and Zegenhagen, Jörg and Lindsay, Robert and Thornton, Geoff},
abstractNote = {Elucidating the structure of the interface between natural (reduced) anatase TiO2 (101) and water is an essential step toward understanding the associated photoassisted water splitting mechanism. In this work we present surface X-ray diffraction results for the room temperature interface with ultrathin and bulk water, which we explain by reference to density functional theory calculations. We find that both interfaces contain a 25:75 mixture of molecular H2O and terminal OH bound to titanium atoms along with bridging OH species in the contact layer. This is in complete contrast to the inert character of room temperature anatase TiO2 (101) in ultrahigh vacuum. A vital difference between the ultrathin and bulk water interfaces is that in the latter water in the second layer is also ordered. These molecules are hydrogen bonded to the contact layer, modifying the bond angles.},
doi = {10.1021/acs.jpclett.8b01182},
journal = {Journal of Physical Chemistry Letters},
number = [11],
volume = [9],
place = {United States},
year = {2018},
month = {5}
}

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Cited by: 11 works
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