Shi H, Hussain T, Ahuja R, Kang T W, Luo W
School of Physics, Beijing Institute of Technology, 100081, Beijing, P. R. China.
Centre for Theoretical and Computational Molecular Science, Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, Brisbane, Qld 4072, Australia.
Sci Rep. 2016 Aug 24;6:31345. doi: 10.1038/srep31345.
The magnetic properties and electronic structures of pure, doped and defective cerium oxide (CeO2) have been studied theoretically by means of ab initio calculations based on the density function theory (DFT) with the hybrid HF/DFT technique named PBE0. Carbon (C), nitrogen (N), phosphorus (P), sulphur (S), lanthanum (La) and praseodymium (Pr) doped in CeO2 and CeO2 containing oxygen vacancies (Ov) were considered. Our spin-polarized calculations show that C, N, Pr dopants and Ov defects magnetize the non-magnetic CeO2 in different degree. The optical band gap related to photocatalysis for pure CeO2, corresponding to the ultraviolet region, is reduced obviously by C, N, S, Pr impurities and oxygen vacancies, shifting to the visible region and even further to the infrared range. Especially, N-, S- and Pr-doped CeO2 could be used to photocatalytic water splitting for hydrogen production. As the concentration of Ov increasing up to 5%, the CeO2 exhibits a half-metallic properties.
利用基于密度泛函理论（DFT）的从头算方法，并采用名为PBE0的杂化HF/DFT技术，从理论上研究了纯的、掺杂的和有缺陷的氧化铈（CeO2）的磁性和电子结构。考虑了碳（C）、氮（N）、磷（P）、硫（S）、镧（La）和镨（Pr）掺杂在CeO2中以及含有氧空位（Ov）的CeO2。我们的自旋极化计算表明，C、N、Pr掺杂剂和Ov缺陷会使非磁性的CeO2产生不同程度的磁化。与纯CeO2光催化相关的光学带隙对应于紫外区域，由于C、N、S、Pr杂质和氧空位，其明显减小，向可见光区域甚至进一步向红外范围移动。特别是，N、S和Pr掺杂的CeO2可用于光催化水分解制氢。当Ov浓度增加到5%时，CeO2呈现半金属性质。
