High Reactivity of the ZnO(0001) Polar Surface: The Role of Oxygen Adatoms

Liu, Yang; Xu, Wangping; Shan, Yueyue; Xu, Hu

2017-07-27

10.1021/acs.jpcc.7b03326

Journal of Physical Chemistry C   影响因子和分区

1932-7447

Understanding the mechanism of water dissociation on metal oxide surfaces is of particular interest in catalytic reactions. In this work, the interaction of water with the ZnO(0001) polar surface is investigated, and the role of oxygen adatoms in water splitting is uncovered. The individual surface energies and electronic properties of ZnO polar surfaces are investigated on the basis of density functional theory calculations. The oxygen adatoms on the ZnO(0001) surface introduce in-gap surface states, resulting in a direct-to-indirect band gap transition. Water strongly interacts with oxygen adatoms to spontaneously form hydroxyl groups, recovering the direct band-gap characteristics of ZnO polar surfaces. Furthermore, water prefers to adsorb at the step edges of cavities after all of the oxygen adatoms are consumed, and the hydrogen-bonded network among water molecules triggers the dissociation of water at the edge sites, which is also confirmed by molecular dynamics calculations. Our results provide atomic-scale insight into the interactions of water with the ZnO(0001) surface.

SCI ; EI

英语

第一 ; 通讯

Basic Research Program of Science, Technology, and Innovation Commission of Shenzhen Municipality[JCYJ20160531190054083]

Chemistry ; Science & Technology - Other Topics ; Materials Science

Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary

WOS:000406726200025

AMER CHEMICAL SOC

20173104013298

Adatoms ; Catalysis ; Density functional theory ; Dissociation ; Electronic properties ; Energy gap ; Hydrogen bonds ; Metals ; Molecular dynamics ; Molecular oxygen ; Molecules ; Reaction kinetics ; Zinc oxide

Physical Chemistry:801.4 ; Chemical Reactions:802.2 ; Inorganic Compounds:804.2 ; Atomic and Molecular Physics:931.3

Web of Science

Southern Univ Sci & Technol, Dept Phys, Shenzhen 518055, Peoples R China

Liu, Yang,Xu, Wangping,Shan, Yueyue,et al. High Reactivity of the ZnO(0001) Polar Surface: The Role of Oxygen Adatoms[J]. Journal of Physical Chemistry C,2017,121(29):15711-15718.

Liu, Yang,Xu, Wangping,Shan, Yueyue,&Xu, Hu.(2017).High Reactivity of the ZnO(0001) Polar Surface: The Role of Oxygen Adatoms.Journal of Physical Chemistry C,121(29),15711-15718.

Liu, Yang,et al."High Reactivity of the ZnO(0001) Polar Surface: The Role of Oxygen Adatoms".Journal of Physical Chemistry C 121.29(2017):15711-15718.