Fang Yiyu, Kong Xianggang, Yu You, Zhang Xiaotong, Chen Xiaojun, Gao Tao, Xiao Chengjian, Lu Tiecheng
Institute of Atomic and Molecular Physics, Sichuan University Chengdu 610065 People's Republic of China
College of Optoelectronic Technology, Chengdu University of Information Technology Chengdu 610225 China.
RSC Adv. 2019 Mar 13;9(15):8490-8497. doi: 10.1039/c9ra00830f. eCollection 2019 Mar 12.
We investigated the effect of Pd and Ni dopants on the formation and desorption of tritiated water (TO) molecules from the LiTiO (001) surface using first-principles calculations coupled with the climbing-image nudged elastic band method. We calculated the energy barriers for TO production and desorption on the pure LiTiO surface to be 0.94 and 0.64 eV, respectively. The Pd and Ni dopants enhanced TO formation by reducing the formation energy of O vacancies, and TO generated spontaneously on the dopant surface. Moreover, we found that dopant atoms affect the charge transfer of neighboring atoms, which leads to orbital hybridization and the generation of a chemical bond between the O and T on the doped LiTiO surface. In addition, desorption of TO from the doped LiTiO surface requires a relatively low energy (<0.50 eV). This theoretical study suggests that doping the LiTiO surface with metal atoms is an effective strategy for producing TO molecules and is beneficial to T release.
我们采用第一性原理计算结合爬山图像推挤弹性带方法，研究了钯（Pd）和镍（Ni）掺杂剂对氚化水（TO）分子在LiTiO(001)表面形成和解吸的影响。我们计算得出，在纯LiTiO表面上TO生成和解吸的能垒分别为0.94电子伏特和0.64电子伏特。Pd和Ni掺杂剂通过降低氧空位的形成能来增强TO的形成，并且TO在掺杂剂表面自发生成。此外，我们发现掺杂原子会影响相邻原子的电荷转移，这导致轨道杂化以及在掺杂的LiTiO表面上氧（O）和氚（T）之间形成化学键。另外，TO从掺杂的LiTiO表面解吸需要相对较低的能量（<0.50电子伏特）。这项理论研究表明，用金属原子掺杂LiTiO表面是生产TO分子的有效策略，并且有利于氚的释放。
