Citation: LI Lu, LI Yi, GUO Xin, ZHANG Yong-Fan, CHEN Wen-Kai. Adsorption and Dissociation of Water on HfO₂(111) and (110) Surfaces[J]. Acta Physico-Chimica Sinica, ;2013, 29(05): 937-945. doi: 10.3866/PKU.WHXB201303081 shu

Adsorption and Dissociation of Water on HfO₂(111) and (110) Surfaces

LI Lu ¹ ,
LI Yi ¹ ,
GUO Xin ² ,
ZHANG Yong-Fan ¹ ,
CHEN Wen-Kai ^1,3,

1.
1 Department of Chemistry, Fuzhou University, Fuzhou 350116, P. R. China;
2 States Key Laboratory of Coal combustion, Huazhong University of Science and Technology, Wuhan, Hubei, 410074, P. R. China;
3 Fujian Provincial Key Laboratory of Photocatalysis-State Key Laboratory Breeding Base, Fuzhou University, Fuzhou 350002, P. R. China

Received Date: 12 November 2012
Available Online: 8 March 2013
Fund Project: 福建省自然科学基金(2012J01032, 2012J01041) (2012J01032, 2012J01041)华中科技大学煤燃烧国家重点实验室开放基金(FSKLCC1110)资助项目 (FSKLCC1110)

First-principles calculations based on density functional theory (DFT) with the generalized gradient approximation (GGA-PW91) have been used to investigate the adsorption and dissociation of H₂O molecules on HfO₂(111) and (110) surfaces at different sites with different coverages. It was found that the surface hafnium atom was the active adsorption position of the (111) and (110) surfaces when compared different adsorption energies and various geometrical parameters. Adsorption energies of water on the HfO₂ (111) and (110) surfaces varied slightly as the coverage increased. It was shown that the most favorable configuration of H₂O on the HfO₂(111) and (110) surfaces corresponded to the coordination of H₂O via its oxygen to a surface hafnium atom. Adsorption geometries, Mulliken population charges, density of states, and frequency calculations for HfO₂-OH, HfO₂-O, and HfO₂-H at both surfaces were also carried out. The results showed that the hydroxyl group interacted with the surface by its oxygen atom to surface hafnium atoms. Isolated oxygen atoms bound to surface hafnium and oxygen atoms, while hydrogen atoms interact only with surface oxygen atoms to form hydroxyl groups. For the dissociation reaction, according to transition searching, H₂O→H (ads)+OH (ads). The energy barriers were endothermic by 9.7 and 17.3 kJ· mol^-1 for the (111) surfaces and exothermic by -59.9 and -47.6 kJ·mol^-1 for the (110) surfaces.
- Ddensity functional theory,
- HfO₂,
- H₂O molecule,
- Adsorption,
- Dissociation
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Adsorption and Dissociation of Water on HfO₂(111) and (110) Surfaces