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Hydroxylation Structure and Proton Transfer Reactivity at the Zinc Oxide-Water Interface

Raymand, David and van Duin, Adri C. T. and Goddard, William A., III and Hermansson, Kersti and Spångberg, Daniel (2011) Hydroxylation Structure and Proton Transfer Reactivity at the Zinc Oxide-Water Interface. Journal of Physical Chemistry C, 115 (17). pp. 8573-8579. ISSN 1932-7447. https://resolver.caltech.edu/CaltechAUTHORS:20110509-110054205

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Abstract

The hydroxylation structural features of the first adsorption layer and its connection to proton transfer reactivity have been studied for the ZnO-liquid water interface at room temperature. Molecular dynamics simulations employing the ReaxFF forcefield were performed for water on seven ZnO surfaces with varying step concentrations. At higher water coverage a higher level of hydroxylation was found, in agreement with previous experimental results. We have also calculated the free energy barrier for transferring a proton to the surface, showing that stepped surfaces stabilize the hydroxylated state and decrease the water dissociation barrier. On highly stepped surfaces the barrier is only 2 kJ/mol or smaller. Outside the first adsorption layer no dissociation events were found during almost 100 ns of simulation time; this indicates that these reactions are much more likely if catalyzed by the metal oxide surface. Also, when exposed to a vacuum, the less stepped surfaces stabilize adsorption beyond monolayer coverage.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1021/jp106144pDOIArticle
http://pubs.acs.org/doi/abs/10.1021/jp106144pPublisherArticle
ORCID:
AuthorORCID
van Duin, Adri C. T.0000-0002-3478-4945
Goddard, William A., III0000-0003-0097-5716
Additional Information:© 2011 American Chemical Society. Published In Issue May 05, 2011; Article ASAP April 12, 2011; Received: July 02, 2010; Revised: March 21, 2011. This work was supported by the Swedish Research Council (VR) and by NSF Grant #DMR 0427177. Computer time was provided by SNIC. The computations were performed on UPPMAX under Project s00707-54 and SweGRID under project 015/09-14. Useful discussions with professors Wim Briels (Twente University) and Philippe Bopp (Bordeaux University) are gratefully acknowledged.
Funders:
Funding AgencyGrant Number
Swedish Research CouncilUNSPECIFIED
NSFDMR-0427177
Issue or Number:17
Record Number:CaltechAUTHORS:20110509-110054205
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20110509-110054205
Official Citation:Hydroxylation Structure and Proton Transfer Reactivity at the Zinc Oxide−Water Interface David Raymand, Adri C.T. van Duin, William A. Goddard III, Kersti Hermansson, Daniel Spångberg The Journal of Physical Chemistry C 2011 115 (17), 8573-8579
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:23600
Collection:CaltechAUTHORS
Deposited By: Jason Perez
Deposited On:09 May 2011 22:44
Last Modified:03 Oct 2019 02:48

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