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邵先军,袁旭初,陈孝信,等. 基于过渡态理论及密度泛函理论的SF6主要分解产物生成路径的反应速率常数计算[J]. 科学技术与工程, 2020, 20(23): 9414-9420.
SHAO Xianjun,et al.Calculated Rate Constants of the Chemical Reactions Involving the Main Byproducts of SF6 Decomposition Based on Density Functional Theory and Transition State Theory[J].Science Technology and Engineering,2020,20(23):9414-9420.
基于过渡态理论及密度泛函理论的SF6主要分解产物生成路径的反应速率常数计算
Calculated Rate Constants of the Chemical Reactions Involving the Main Byproducts of SF6 Decomposition Based on Density Functional Theory and Transition State Theory
投稿时间:2019-09-10  修订日期:2020-05-03
DOI:
中文关键词:  SF6 分解组分分析 分解机理 化学反应速率常数 密度泛函理论 过渡态理论
英文关键词:SF6 decomposed components analysis decomposition mechanism chemical reaction rate constant density functional theory transition state theory
基金项目:国网浙江省电力公司科技项目(5211DS170012)
                       
作者单位
邵先军 State Grid Zhejiang Electric Power Co., Ltd. Electric Power Research Institute, Hangzhou
袁旭初 西安交通大学电力设备电气绝缘国家重点实验室
陈孝信 国网浙江省电力有限公司电力科学研究院
钱平 国网浙江省电力有限公司
何彦良 西安交通大学电力设备电气绝缘国家重点实验室
何毅帆 西安交通大学电力设备电气绝缘国家重点实验室
孙安邦 西安交通大学电力设备电气绝缘国家重点实验室
张冠军 西安交通大学电力设备电气绝缘国家重点实验室
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中文摘要:
      基于分解组分分析的SF6绝缘设备故障诊断方法不受电磁干扰,得到了广泛应用。专家学者建立了许多SF6分解模型以探究SF6分解的内部机理,但现有模型采用的反应速率常数为300 K温度下测量所得,并不适用于SF6的过热及电弧分解。本文对SF6分解过程中主要稳定分解产物SOF2、SO2F2、SO2的生成机理进行了研究,采用密度泛函理论(Density functional theory,DFT)结合B3LYP/6-311G*方法分析了主气室内SOF2、SO2F2、SO2的主要生成路径:SF4水解生成SOF2、SOF4水解生成SO2F2和SOF2水解生成SO2,得到了所涉及反应的反应物、生成物及过渡态结构;并采用高精度CCSD(T)方法结合aug-cc-pVTZ基组得到了各反应的势垒;再根据过渡态理论(Transition state theory, TST)从理论上计算了上述反应的反应速率常数。该反应速率常数考虑了温度变化的影响,适用范围更广,为研究SF6过热及电弧分解的内部机理提供了理论支撑。
英文摘要:
      Technology based on decomposed components analysis using for SF6 insulation equipment fault diagnosis is widely used in the fault diagnosis of power equipment for its advantage in anti-electromagnetic interference. Recently, some theoretical research focused on the formation of main SF6 derivatives have been carried out through chemical kinetics models, but the basic data (chemical reactions and their rate constants) adopted in the model are only appropriate for 300 K and not valid for the decomposition under partial over-thermal fault, as well as arc discharge. In this paper, the formation mechanism of SO2F2、SOF2 and SO2 have been investigated. The DFT-B3LYP method with 6-311G* basis set was used to calculate the optimized molecular geometries, as well as the transition states of hydrolysis reactions of SF4, SOF4 and SOF2. Those chemical reactions involve the main byproducts of SF6 decomposition. Energy of molecular geometries and transition states were calculated, using the sophisticated CCSD(T) ab-initio method with a large aug-cc-pVTZ basis set to obtain more accurate energies and barrier heights. Rate constants are estimated by TST based on the results obtained from DFT-B3LYP method mentioned above. The rate constants in this paper consider the influence of temperature and derived for a large temperature. This work is expected to lay a theoretical foundation for further study on SF6 decomposition mechanism under partial over-thermal fault and arc discharge.
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