First-principles study of the water adsorption on Anatase(101) as a function of the coverage
File(s)
Accepted version
Author(s)
Martinez-Casado, Ruth
Mallia, Giuseppe
Harrison, Nicholas M
Perez, Ruben
Type
Journal Article
Abstract
An understanding of the interaction of water with the anatase(101) surface is crucial for developing strategies to improve the efficiency of the photocatalytic reaction involved in solar water splitting. Despite a number of previous investigations, it is still not clear if water preferentially adsorbs in its molecular or dissociated form on anatase(101). With the aim of shedding some light on this controversial issue, we report the results of periodic screened-exchange density functional theory calculations of the dissociative, molecular, and mixed adsorption modes on the anatase(101) surface at various coverages. Our calculations support the suggestion that surface-adsorbed OH groups are present, which has been made on the basis of recently measured X-ray photoelectron spectroscopy, temperature-programmed desorption, and scanning tunneling microscopy data. It is also shown that the relative stability of water adsorption on anatase(101), at different configurations, can be understood in terms of a simple model based on the number and nature of the hydrogen bonds formed as well as the adsorbate-induced atomic displacements in the surface layers. These general conclusions are found to be insensitive to the specific choice of approximation for electronic exchange and correlation within the density functional theory. The simple model of water–anatase interactions presented here may be of wider validity in determining the geometry of water–oxide interfaces.
Date Issued
2018-09-13
Date Acceptance
2018-08-12
Citation
Journal of Physical Chemistry C, 2018, 122 (36), pp.20736-20744
ISSN
1932-7447
Publisher
American Chemical Society
Start Page
20736
End Page
20744
Journal / Book Title
Journal of Physical Chemistry C
Volume
122
Issue
36
Copyright Statement
© 2018 American Chemical Society. This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of Physical Chemistry C, after peer review and technical editing by the publisher. To access the final edited and published work see https://dx.doi.org/10.1021/acs.jpcc.8b05081.
Identifier
http://gateway.webofknowledge.com/gateway/Gateway.cgi?GWVersion=2&SrcApp=PARTNER_APP&SrcAuth=LinksAMR&KeyUT=WOS:000444920900019&DestLinkType=FullRecord&DestApp=ALL_WOS&UsrCustomerID=1ba7043ffcc86c417c072aa74d649202
Subjects
Science & Technology
Physical Sciences
Technology
Chemistry, Physical
Nanoscience & Nanotechnology
Materials Science, Multidisciplinary
Chemistry
Science & Technology - Other Topics
Materials Science
HYBRID DENSITY FUNCTIONALS
HYDROGEN-BOND
TIO2
SURFACES
RUTILE
DISSOCIATION
TIO2(110)
CRYSTALS
Publication Status
Published
Date Publish Online
2018-08-13