摘要
采用广义梯度密度泛函理论研究了H2O分子在α-U(001)表面上的吸附、扩散和解离。结果表明,H2O分子在α-U(001)表面的最稳定构型为平行于表面的顶位吸附结构,吸附能为0.58 eV。吸附作用主要源于H2O分子1b1轨道与表面U原子6d轨道的空间交叠,同时伴有弱的H2O 3a1-U 6d轨道交叠。近邻顶位间H2O分子的扩散能垒为0.20～0.23 eV,预示H2O分子易于在α-U(001)表面发生扩散迁移。OH+H解离吸附较分子吸附在能量上高1.24～1.39 eV,解离能垒为0.56～0.62 eV,预示一定热激活条件下,吸附H2O分子趋向解离形成OH基团和H原子。
The adsorption, the diffusion and the dissociation of H20 molecule on a-U（001） surface have been studied using density functional theory （DFT） within generalized gradient approximation （GGA）. The calculation results indicate that H20 molecule is preferentially adsorbed on the top site in a fiat-lying configuration with the adsorption energy of 0.58 eV. The adsorption interaction is mainly contributed by the overlapping between the lbl orbital of H20 and the 6d orbital of the top-layer U atom, along with some weak H20 3al-U 6d mixing. The activation energy for H20 diffusion between two adjacent top sites is 0.20~0.23 eV, indicating that the on-surface diffusion is easy for H20 molecule. The OH＋H dissociative adsorption is about 1.24-1.39 eV higher in energy than molecular adsorption, together with the dissociation barrier of 0.56~0.62 eV, suggesting that the dissociation of adsorbed H20 into OH and H can occur under the certain heat activation condition.
出处
《稀有金属材料与工程》
SCIE
EI
CAS
CSCD
北大核心
2014年第1期85-90,共6页
Rare Metal Materials and Engineering
基金
国防基础科研课题基金(B1020110010)
