First-Principles Study of Water Reaction and H-2 Formation on UO2 (111) and (110) Single Crystal Surfaces

	First-Principles Study of Water Reaction and H-2 Formation on UO2 (111) and (110) Single Crystal Surfaces
	Bo T(薄涛); Lan JH(兰建慧); Wang CZ(王聪芝); Bo, T; Lan, JH; Wang, CZ; Zhao, YL; He, CH; Zhang, YJ; Chai, ZF
刊名	JOURNAL OF PHYSICAL CHEMISTRY C
	2014
卷号	118 期号:38 页码:21935-21944
英文摘要	Molecular and dissociative adsorption behavior of H2O along with the accompanying H-2 formation mechanism on the UO2 (111) and (110) surfaces have been investigated by using DFT+U calculations. According to our calculations, the higher stability of the (111) surface leads to higher oxygen vacancy formation energy compared to the (110) surface. On the stoichiometric (111) and (110) surfaces, the first hydrogen atom of water molecule can dissociate readily with very small or no energy barrier. On the contrary, dissociation of the second one becomes the rate-determining step, and water-catalysis leads to the decrease of energy barrier from 0.92 to 0.70 eV and from 2.36 to 1.21 eV on the stoichiometric (111) and (110) surfaces, respectively. H-2 formation resulting from water dissociation may undergo two pathways in the presence of surface oxygen vacancy on the reduced UO2 (111) surface. One is characterized by direct combination of two hydrogen atoms of one water molecule, and the other is characterized by dissociation of the first hydrogen atom and its combination with a neighboring surface hydrogen atom. The above two formation pathways possess the energy barriers of 0.56 and 0.53 eV, corresponding to the large reaction energies of -2.62 and -2.64 eV, respectively.
学科主题	Chemistry; Science & Technology - Other Topics; Materials Science
收录类别	SCI
WOS记录号	WOS:000342396300023
公开日期	2016-05-03
内容类型	期刊论文
源URL	[http://ir.ihep.ac.cn/handle/311005/225148]
专题	高能物理研究所_院士高能物理研究所_多学科研究中心
推荐引用方式 GB/T 7714	Bo T,Lan JH,Wang CZ,et al. First-Principles Study of Water Reaction and H-2 Formation on UO2 (111) and (110) Single Crystal Surfaces[J]. JOURNAL OF PHYSICAL CHEMISTRY C,2014,118(38):21935-21944.
APA	薄涛.,兰建慧.,王聪芝.,Bo, T.,Lan, JH.,...&石伟群.(2014).First-Principles Study of Water Reaction and H-2 Formation on UO2 (111) and (110) Single Crystal Surfaces.JOURNAL OF PHYSICAL CHEMISTRY C,118(38),21935-21944.
MLA	薄涛,et al."First-Principles Study of Water Reaction and H-2 Formation on UO2 (111) and (110) Single Crystal Surfaces".JOURNAL OF PHYSICAL CHEMISTRY C 118.38(2014):21935-21944.