摘要
为了从电子层面揭示δ相Pu中化学吸附原子与Pu原子间的化合过程,提出相应的Pu金属表面抗腐蚀技术。采用局域密度近似(LDA)+U(Hubbard U参数是对Coulomb排斥相互作用的修正)方法研究了PuH2、PuH3、PuC、PuN、PuO、β-Pu2O3、PuO2、PuS的偏态密度(PDOS)和差分电荷密度,通过PDOS分析了Pu 5f、6d状态和H 1s、C 2p、N 2p、O 2p、S 3p状态间的杂化和混合效应,以及Pu原子与化合物原子间的化学成键行为。计算结果表明:PuH2具有金属特性,PuH3中Pu—H化学键本质上是离子性的,Pu—C化学键具有共价行为,Pu—O、Pu—N和Pu—S化学键具有离子性行为,β-Pu2O3和PuO2中Pu—O化学键具有共价行为,研究结果与其他研究结果一致。
To understand chemisorption atoms react with Pu atoms inδphase plutonium from the electronic scale,and propose the anti-corrosion techniques for plutonium metal,electronic structures of PuH2,PuH3,PuC,PuN,PuO,β-Pu2O3,PuO2 and PuS compounds were calculated within the framework of LAD+U(Hubbard U parameter represents a correction to Coulomb repulsion interaction)method using the PerdewBurke-Ernzerhof(PBE)exchange-correlation functional at the spin-polarized(SP)level.The hybridization and mixing effects of Pu 5f,6dstates with H 1s,C 2p,N 2p,O 2pand S 3pstates were analyzed in terms of partial density of states(PDOS).The chemical bonding behaviors of Pu atom with the valence atoms were investigated.The results show that PuH2 compound has the metallic character,Pu—H bonds in PuH3 compound,Pu—O bond in PuO compound,Pu—N bond in PuN compound and Pu—Sbond in PuS compound are essentially ionic in character.Pu—C bond in PuC compound,Pu—O bond in Pu2O3 compound and Pu—O bond in PuO2 compound are covalent in character,which are in agreement with the obtainable results.
出处
《原子能科学技术》
EI
CAS
CSCD
北大核心
2014年第S1期43-49,共7页
Atomic Energy Science and Technology
基金
国家自然科学基金资助项目(51401237
51271198
11474358)
第二炮兵工程大学青年基金资助项目(2014QNJJ018
YX2012cxpy06)
关键词
密度泛函理论
化学吸附
态密度
电子密度差分
density functional theory
chemisorption
density of state
electron density difference