基于密度泛函理论的SF_6潜在替代气体筛选
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摘要
目前在研的SF_6替代气体存在沸点θ_b过高、与缓冲气体混合后绝缘强度E_R降低等问题,仍需要寻找新型替代气体。为此,基于气体中载流子碰撞过程分析,找出第1电离能ε、分子电负性χ和分子直径D_w3个与气体绝缘强度相关的参数,并采密度泛函理论(DFT)下的B3LYP方法及6-311G+(d,p)基组对37种气体的上述参数进行计算。通过多元非线性拟合得到了气体绝缘强度预测模型,模型可决系数R~2达到0.90;并根据10个未代入拟合的气体绝缘强度数据对预测模型进行了校验。结果显示,在对弱极性非对称分子的D_w进行修正后,模型的准确性和适用性得到提高,R~2可达0.85。通过对θ_b已知的待选气体进行E_R的预测,并根据替代潜能因子Kp,从137种待选气体中筛选出了5种具有较高替代潜能的绝缘气体。
At present, the substitutes of SF_6 under investigation still have several problems such as possessing high boiling points θ_b and low insulation strengths E_R after being mixed with buffer gases. Hence the new substitutes are still need to be found. Consequently, the parameters such as the first ionization energy ε, electronegativity χ,and the molecule diameter D_w, which are highly correlated with the electric insulation strength, were selected by the analysis of different collision processes in the gas. Then, the parameters of 37 kinds of molecules were calculated and modified by the B3 LYP method in density functional theory with 6-311 G +(d, p) basic set. The predicting formula of insulation strength was fitted by a multivariate linear fitting method with the determination coefficient R~2 of 0.90. To verify the accuracy of predictions, the electrical insulation strengths of 10 kinds of gaseous molecules' without the adoption in regression were introduced for the verification of model accuracy. The result shows that, with rectifying molecule diameter D_w of weak polar asymmetric molecules, the prediction model has higher accuracy and applicability with R~2 of 0.85. The E_R of 137 candidates whose θ_b are experimentally tested are predicted, and five kinds of gases with high replacement potential were selected by the alternative potential factor Kp based on the compatibility between θ_b and E_R.
At present, the substitutes of SF_6 under investigation still have several problems such as possessing high boiling points θ_b and low insulation strengths E_R after being mixed with buffer gases. Hence the new substitutes are still need to be found. Consequently, the parameters such as the first ionization energy ε, electronegativity χ,and the molecule diameter D_w, which are highly correlated with the electric insulation strength, were selected by the analysis of different collision processes in the gas. Then, the parameters of 37 kinds of molecules were calculated and modified by the B3 LYP method in density functional theory with 6-311 G +(d, p) basic set. The predicting formula of insulation strength was fitted by a multivariate linear fitting method with the determination coefficient R~2 of 0.90. To verify the accuracy of predictions, the electrical insulation strengths of 10 kinds of gaseous molecules' without the adoption in regression were introduced for the verification of model accuracy. The result shows that, with rectifying molecule diameter D_w of weak polar asymmetric molecules, the prediction model has higher accuracy and applicability with R~2 of 0.85. The E_R of 137 candidates whose θ_b are experimentally tested are predicted, and five kinds of gases with high replacement potential were selected by the alternative potential factor Kp based on the compatibility between θ_b and E_R.
引文
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[12]MEURICE N,SANDRE E,ASLANIDES A,et al.Simple theoretical estimation of the dielectric strength of gases[J].IEEE Transactions on Dielectrics&Electrical Insulation,2004,11(6):946-948.
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[14]RABIE M,DAHL D A,DONALD S M A,et al.Predictors for gases of high electrical strength[J].IEEE Transactions on Dielectrics&Electrical Insulation,2013,20(3):856-863.
[15]林林,陈庆国,程嵩,等.基于密度泛函理论的SF6潜在可替代性气体介电性能分析[J].电工技术学报,2018,33(18):4382-4388.LIN Lin,CHEN Qingguo,CHENG Song,et al.The analysis of SF6potential alternative gas dielectric strength based on density functional theory[J].Transactions of China Electrotechnical Society,2018,33(18):4382-4388.
[16]YU X,HOU H,WANG B.Prediction on dielectric strength and boiling point of gaseous molecules for replacement of SF6[J].Journal of Computational Chemistry,2017,38(10):721-729.
[17]LU T,CHEN F.Multiwfn:a multifunctional wavefunction analyzer[J].Journal of Computational Chemistry,2012,33(5):580-592.
[18]LU T,CHEN F.Quantitative analysis of molecular surface based on improved marching tetrahedra algorithm[J].Journal of Molecular Graphics&Modelling,2012,38(9):314-323.
[2]YAMAMOTO O,TAKUMA T,HAMADA S,et al.Appling a gas mixture containing c-C4F8 as an insulation medium[J].IEEE Transactions on Dielectrics and Electrical Insulation,2001,8(6):1071-1085.
[3]KATAGIRI H,KASUYA H,MIZOGUCHI H,et al.Investigation of the performance of CF3I gas as a possible substitute for SF6[J].IEEETransactions on Dielectrics&Electrical Insulation,2008,15(5):1424-1429.
[4]KIEFFEL Y.Characteristics of g3-an alternative to SF6[C]∥IEEEInternational Conference on Dielectrics.Montpellier,France:IEEE,2016:880-884.
[5]ZHAO H,LI X,TANG N,et al.Dielectric properties of fluoronitriles/CO2 and SF6/N2 mixtures as a possible SF6-substitute gas[J].IEEE Transactions on Dielectrics&Electrical Insulation,2018,25(4):1332-1339.
[6]ZHANG X,LI Y,CHEN D,et al.Dissociative adsorption of environment-friendly insulating medium C3F7CN on Cu(111)and Al(111)surface:a theoretical evaluation[J].Applied Surface Science,2018,434:549-560.
[7]肖登明,焦俊韬,YAN Jiudun.环保型绝缘气体的灭弧能力分析[J].高电压技术,2016,42(6):1681-1687.XIAO Dengming,JIAO Juntao,YAN Jiudun.Arc quenching characteristics analysis of environmental-friendly insulation gases[J].High Voltage Engineering,2016,42(6):1681-1687.
[8]王小华,傅熊雄,韩国辉,等.C5F10O/CO2混合气体的绝缘性能[J].高电压技术,2017,43(3):715-720.WANG Xiaohua,FU Xiongxiong,HAN Guohui,et al.Insulation performance of C5F10O/CO2 gas mixture[J].High Voltage Engineering,2017,43(3):715-720.
[9]李兴文,邓云坤,姜旭,等.环保气体C4F7N和C5F10O与CO2混合气体的绝缘性能及其应用[J].高电压技术,2017,43(3):708-714.LI Xingwen,DENG Yunkun,JIANG Xu,et al.Insulation performance and application of environment-friendly gases mixtures of C4F7N and C5F10O with CO2[J].High Voltage Engineering,2017,43(3):708-714.
[10]周文俊,郑宇,高克利,等.环保型绝缘气体电气特性研究进展[J].高电压技术,2018,44(10):3114-3124.ZHOU Wenjun,ZHENG Yu,GAO Keli,et al.Progress in researching electrical characteristics of environment-friendly insulating gases[J].High Voltage Engineering,2018,44(10):3114-3124.
[11]BRAND K P.Dielectric strength,boiling point and toxicity of gases-different aspects of the same basic molecular properties[J].IEEETransactions on Electrical Insulation,1982,17(5):451-456.
[12]MEURICE N,SANDRE E,ASLANIDES A,et al.Simple theoretical estimation of the dielectric strength of gases[J].IEEE Transactions on Dielectrics&Electrical Insulation,2004,11(6):946-948.
[13]KAZAKOV A,MCLINDEN M O,FRENKEL M.Computational design of new refrigerant fluids based on environmental,safety and thermodynamic characteristics[J].Industrial&Engineering Chemistry Research,2012,51(38):12537-12548.
[14]RABIE M,DAHL D A,DONALD S M A,et al.Predictors for gases of high electrical strength[J].IEEE Transactions on Dielectrics&Electrical Insulation,2013,20(3):856-863.
[15]林林,陈庆国,程嵩,等.基于密度泛函理论的SF6潜在可替代性气体介电性能分析[J].电工技术学报,2018,33(18):4382-4388.LIN Lin,CHEN Qingguo,CHENG Song,et al.The analysis of SF6potential alternative gas dielectric strength based on density functional theory[J].Transactions of China Electrotechnical Society,2018,33(18):4382-4388.
[16]YU X,HOU H,WANG B.Prediction on dielectric strength and boiling point of gaseous molecules for replacement of SF6[J].Journal of Computational Chemistry,2017,38(10):721-729.
[17]LU T,CHEN F.Multiwfn:a multifunctional wavefunction analyzer[J].Journal of Computational Chemistry,2012,33(5):580-592.
[18]LU T,CHEN F.Quantitative analysis of molecular surface based on improved marching tetrahedra algorithm[J].Journal of Molecular Graphics&Modelling,2012,38(9):314-323.
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