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ThO+/0/-2不同电荷态对N2O氧化CO反应的影响
引用本文:夏婵娟,石锦豪,张惠孜,李大武,岳光辉. ThO+/0/-2不同电荷态对N2O氧化CO反应的影响[J]. 原子与分子物理学报, 2023, 40(1): 011007-72
作者姓名:夏婵娟  石锦豪  张惠孜  李大武  岳光辉
作者单位:湖南警察学院,湖南警察学院,湖南警察学院,中国刑警学院,湖南警察学院
基金项目:国家自然科学基金(21301030);
摘    要:本文采用密度泛函理论,对ThO+/0/-2团簇参与CO与N2O间氧化还原反应(CO+N2O→CO2+N2)的机理展开研究,探讨钍氧团簇所带的电荷对该反应的影响.研究表明:ThO+/0/-2在反应中主要起传输氧原子的作用,其中ThO+2与CO的反应以及ThO+/0/-与N2O的反应都为热力学上的放热反应,而ThO0/-2与CO的反应为热力学上的吸热反应.随着电荷态的改变,ThO+/0/-2与CO反应的总能垒(Eb)与总驱动力(-ΔG)有较大差异.因此,通过改变ThO2的电荷态能调节其对CO/N2O反应的催化活性,综合考虑,ThO+2对...

关 键 词:钍氧簇  密度泛函理论  电子结构  催化氧化反应  电荷
收稿时间:2021-11-05
修稿时间:2021-11-29

Oxidation Reactions of CO by N2O on ThO2+/0/- Clusters: The Effect of Charge States of ThO2
Xia Chan-Juan,Shi Jin-Hao,Zhang Hui-Zi,Li Da-Wu and Yue Guang-Hui. Oxidation Reactions of CO by N2O on ThO2+/0/- Clusters: The Effect of Charge States of ThO2[J]. Journal of Atomic and Molecular Physics, 2023, 40(1): 011007-72
Authors:Xia Chan-Juan  Shi Jin-Hao  Zhang Hui-Zi  Li Da-Wu  Yue Guang-Hui
Affiliation:Hunan Police Academy,hunan police academy,hunan police academy,Criminal Investigation Police University of China and hunan police academy
Abstract:Density functional theory (DFT) calculations at the B3LYP level are performed to investigate the redox reactions between CO and N2O in which ThO2+/0/- clusters participate. The reaction mechanisms are illustrated and the impacts of the charge states of ThO2+/0/- on the above reactions are evaluated as well. Our results show that ThO2+/0/- play the role of transporting O atom in the CO/N2O redox reaction. The reaction of ThO2+ with CO is exothermic, while those of ThO2-/0 with CO are endothermic. As for the reactions of ThO+/0/- with N2O, they are all exothermic. With the change of the charge state, the energy barriers (Eb) and the driving forces (-∆G) of the overall reactions show big differences for ThO2+, ThO2 and ThO2- reacting with CO, respectively. Therefore, by changing the charge state of ThO2, its redox ability can be regulated. In summary, the positively charged ThO2+ cluster shows the highest catalytic activity in the above CO/N2O redox reaction.
Keywords:Thorium oxide cluster   Density functional theory   Electronic structure   Catalytic oxidation reactions   Charge state
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