Citation: ZENG Xiu-Lin, HUANG Shan-Qi-Song, JU Xue-Hai. Density Functional Theory Study of the Gas-Phase Reaction of U⁺ with CO₂[J]. Acta Physico-Chimica Sinica, ;2013, 29(11): 2308-2312. doi: 10.3866/PKU.WHXB201309042 shu

Density Functional Theory Study of the Gas-Phase Reaction of U⁺ with CO₂

1.
1 Department of Chemistry and Chemical Engineering, Huainan Normal University, Huainan 232001, Anhui Province, P. R. China;
2 Department of Chemistry, Nanjing University of Science and Technology, Nanjing 210094, P. R. China

Received Date: 15 May 2013
Available Online: 4 September 2013
Fund Project: 国家自然科学基金(21101070)资助项目 (21101070)

The gas-phase reaction of U⁺ with CO₂ was investigated with B3LYP density functional theory (DFT) in conjunction with the relativistic effective core potential (ECP) of the SDD basis sets for Uand the 6-311 + G(d) basis set for C and O. The potential energy surfaces (PESs) of the reaction system were explored in detail for both doublet and quartet spin states. The geometries of reactants, intermediates, transition states, and products in the two reaction pathways were fully optimized. The reaction mechanism was analyzed using"two-state reactivity (TSR)."The calculations demonstrate that the reaction preferentially involves the high-spin state entrance channel and the low-spin state exit channel. The spin multiplicity transition from the quartet state to the doublet state enables the reaction system to find a lower energy pathway.
- Reaction mechanism,
- Density functional theory,
- Relativistic effective core potential,
- Potential energy surface,
- Spin state
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沈阳化工大学材料科学与工程学院沈阳 110142

Density Functional Theory Study of the Gas-Phase Reaction of U+ with CO2

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通讯作者: 陈斌, bchen63@163.com

Density Functional Theory Study of the Gas-Phase Reaction of U⁺ with CO₂