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Gas‐phase water activation by Th atom: Reaction mechanisms and topological analysis
Author(s) -
Li Peng,
Niu Wenxia,
Gao Tao,
Wang Hongyan
Publication year - 2014
Publication title -
international journal of quantum chemistry
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.484
H-Index - 105
eISSN - 1097-461X
pISSN - 0020-7608
DOI - 10.1002/qua.24651
Subject(s) - isomerization , exothermic reaction , chemistry , electron localization function , atom (system on chip) , density functional theory , reaction mechanism , reactivity (psychology) , molecule , computational chemistry , natural bond orbital , chemical physics , electron , catalysis , organic chemistry , physics , medicine , alternative medicine , pathology , quantum mechanics , computer science , embedded system
Density functional theory calculations were performed to investigate the gas‐phase reaction of Th atom with water. Three reaction pathways were identified, which leads to the formation of ThOH + H, ThO + H 2 , and H 2 ThO. The latter two are generated via the intermediate HThOH, and the H 2 ThO specie is generated from the isomerization of the HThOH intermediate. A thorough description of the reaction mechanism taking into account different possible spin states together with analysis of the electronic factors offer insights into the reactivity of the actinides atom. The obtained results are compared with the available experimental data. The three reaction pathways were found to be exothermic, in which the isomerization channel was observed with best thermochemical conditions around 123.9 kcal/mol. The nature of the chemical bonding evolution along the reaction pathways was studied using topological analysis including electron localization function, atoms‐in‐molecules, and natural bond orbital. © 2014 Wiley Periodicals, Inc.