| Cite this article as: 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.(原子与分子物理学报), 2023, 40: 011007 (in Chinese) |
| Oxidation Reactions of CO by N2O on ThO2+/0/- Clusters: The Effect of Charge States of ThO2 |
| Hits 427 Download times 149 Received:November 05, 2021 Revised:November 29, 2021 |
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| Key Words
Thorium oxide cluster Density functional theory Electronic structure Catalytic oxidation reactions Charge state |
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| Abstract
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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. |
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