引用本文格式: Xia Chan-Juan,Shi Jin-Hao,Zhang Hui-Zi,Li Da-Wu,Yue Guang-Hui. Oxidation Reactions of CO by N2O on ThO2+/0/- Clusters: The Effect of Charge States of ThO2 [J]. J. At. Mol. Phys., 2023, 40(1): 011007 (in Chinese) 夏婵娟,石锦豪,张惠孜,李大武,岳光辉. ThO2+/0/-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] |
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ThO2+/0/-不同电荷态对N2O氧化CO反应的影响 |
Oxidation Reactions of CO by N2O on ThO2+/0/- Clusters: The Effect of Charge States of ThO2 |
摘要点击 561 全文点击 205 投稿时间:2021-11-05 修订日期:2021-11-29 |
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DOI编号
10.19855/j.1000-0364.2023.011007 |
中文关键词
钍氧簇 密度泛函理论 电子结构 催化氧化反应 电荷 |
英文关键词
Thorium oxide cluster Density functional theory Electronic structure Catalytic oxidation reactions Charge state |
基金项目
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中文摘要
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本文采用密度泛函理论,对ThO2+/0/-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:ThO2+/0/-在反应中主要起传输氧原子的作用,其中ThO2+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ThO20/-与CO的反应为热力学上的吸热反应。随着电荷态的改变,ThO2+/0/-与CO反应的总能垒(Eb)与总驱动力(-∆G)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,ThO2+对于CO/N2O氧化还原反应的潜在催化活性最高。 |
英文摘要
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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. |