Hydroxylation structure and proton transfer reactivity at the zinc oxide-water interface

David Raymand, Adri C.T. Van Duin, William A. Goddard, Kersti Hermansson, Daniel Spångberg

Research output: Contribution to journalArticle

64 Citations (Scopus)

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.

Original languageEnglish (US)
Pages (from-to)8573-8579
Number of pages7
JournalJournal of Physical Chemistry C
Volume115
Issue number17
DOIs
StatePublished - May 5 2011

Fingerprint

Zinc Oxide
Hydroxylation
Proton transfer
Zinc oxide
zinc oxides
reactivity
protons
Water
water
Adsorption
adsorption
dissociation
Energy barriers
Oxides
Free energy
metal oxides
Molecular dynamics
Protons
Monolayers
simulation

All Science Journal Classification (ASJC) codes

  • Electronic, Optical and Magnetic Materials
  • Energy(all)
  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films

Cite this

Raymand, David ; Van Duin, Adri C.T. ; Goddard, William A. ; Hermansson, Kersti ; Spångberg, Daniel. / Hydroxylation structure and proton transfer reactivity at the zinc oxide-water interface. In: Journal of Physical Chemistry C. 2011 ; Vol. 115, No. 17. pp. 8573-8579.
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Hydroxylation structure and proton transfer reactivity at the zinc oxide-water interface. / Raymand, David; Van Duin, Adri C.T.; Goddard, William A.; Hermansson, Kersti; Spångberg, Daniel.

In: Journal of Physical Chemistry C, Vol. 115, No. 17, 05.05.2011, p. 8573-8579.

Research output: Contribution to journalArticle

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