水在HfO2(111)和(110)表面的吸附与解离

doi:10.3866/PKU.WHXB201303081

Abstract

Abstract:

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.

Key words: Ddensity functional theory, HfO₂, H₂O molecule, Adsorption, Dissociation

MSC2000:

O647

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 Phys. -Chim. Sin., 2013, 29(05): 937-945.

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

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

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