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Article(id=1193230866802504289, tenantId=1146029695717560320, journalId=1149653034449285133, issueId=1193230615618220608, articleNumber=null, orderNo=null, doi=10.16790/j.cnki.1009-9239.im.2025.02.006, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=research-article, receivedDate=1715529600000, receivedDateStr=2024-05-13, revisedDate=1718640000000, revisedDateStr=2024-06-18, acceptedDate=null, acceptedDateStr=null, onlineDate=1762418007803, onlineDateStr=2025-11-06, pubDate=1739980800000, pubDateStr=2025-02-20, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1762418007803, onlineIssueDateStr=2025-11-06, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1762418007803, creator=13701087609, updateTime=1762418007803, updator=13701087609, issue=Issue{id=1193230615618220608, tenantId=1146029695717560320, journalId=1149653034449285133, year='2025', volume='58', issue='2', pageStart='1', pageEnd='138', issueExtLink='null', onlineDate='null', pubDate='null', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=-1, specialIssue=null, createTime=1762417947916, creator=13701087609, updateTime=1762418457365, updator=13701087609, preIssue=null, nextIssue=null, ext={EN=IssueExt(id=1193232752444145866, tenantId=1146029695717560320, journalId=1149653034449285133, issueId=1193230615618220608, language=EN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1193232752444145867, tenantId=1146029695717560320, journalId=1149653034449285133, issueId=1193230615618220608, language=CN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null}, startPage=39, endPage=45, ext={EN=ArticleExt(id=1193230867012219491, articleId=1193230866802504289, tenantId=1146029695717560320, journalId=1149653034449285133, language=EN, title=Effect of micro-water on generation rate of C4F7N gas decomposition products, columnId=1193230616230588994, journalTitle=Insulating Materials, columnName=Special Issue on Eco-friendly Insulating Gas, runingTitle=null, highlight=

In order to explore the generation mechanism of perfluoroisobutyronitrile (C4F7N) gas decomposition products under the presence of micro-water, the decomposition process of C4F7N gas and the recombination process after decomposition were investigated when micro-water participated in the reaction. On the basis of density functional theory and transition state theory, the thermodynamic parameters of C4F7N gas under micro-water participation reaction conditions, as well as the generation paths and generation rates of some characteristic products, were calculated. The results show that when micro-water participates in the reaction, the activation energy required for the decomposition of C4F7N gas is lower than that required for the decomposition of dry C4F7N gas. The presence of micro-water makes the C4F7N decompose easier. The reaction rate constant of CHF3 gas is relatively high in the decomposition products of C4F7N gas, and its chemical properties are stable and detectable, which can be used as a characteristic product of C4F7N gas decomposition under the presence of micro-water.

, articleAbstract=

In order to explore the generation mechanism of perfluoroisobutyronitrile (C4F7N) gas decomposition products under the presence of micro-water, the decomposition process of C4F7N gas and the recombination process after decomposition were investigated when micro-water participated in the reaction. On the basis of density functional theory and transition state theory, the thermodynamic parameters of C4F7N gas under micro-water participation reaction conditions, as well as the generation paths and generation rates of some characteristic products, were calculated. The results show that when micro-water participates in the reaction, the activation energy required for the decomposition of C4F7N gas is lower than that required for the decomposition of dry C4F7N gas. The presence of micro-water makes the C4F7N decompose easier. The reaction rate constant of CHF3 gas is relatively high in the decomposition products of C4F7N gas, and its chemical properties are stable and detectable, which can be used as a characteristic product of C4F7N gas decomposition under the presence of micro-water.

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为了探索微水存在条件下全氟异丁腈（C4F7N）气体分解产物的生成机制，本文对微水参与反应时C4F7N气体的分解过程以及分解后重组的过程进行研究，基于密度泛函理论和过渡态理论计算得到C4F7N气体在微水参与反应条件下的热力学参数以及部分特征产物的生成路径和生成速率。结果表明：在微水参与反应时，C4F7N气体分解所需的活化能低于干燥C4F7N气体分解所需的能量，微水的存在使C4F7N气体更容易分解。C4F7N气体分解产物中CHF3气体的反应速率常数较大，化学性质稳定且具有可检性，可以作为微水存在条件下C4F7N气体分解的特征产物。

, articleAbstract=

为了探索微水存在条件下全氟异丁腈（C4F7N）气体分解产物的生成机制，本文对微水参与反应时C4F7N气体的分解过程以及分解后重组的过程进行研究，基于密度泛函理论和过渡态理论计算得到C4F7N气体在微水参与反应条件下的热力学参数以及部分特征产物的生成路径和生成速率。结果表明：在微水参与反应时，C4F7N气体分解所需的活化能低于干燥C4F7N气体分解所需的能量，微水的存在使C4F7N气体更容易分解。C4F7N气体分解产物中CHF3气体的反应速率常数较大，化学性质稳定且具有可检性，可以作为微水存在条件下C4F7N气体分解的特征产物。

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王璁（1980-），男（汉族），江西赣州人，高级工程师，博士，主要从事电气设备外绝缘、气体放电以及电气设备故障诊断的研究工作。
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崔光凯（2000-），男（汉族），山东济宁人，硕士生，主要从事高电压试验技术和气体放电方面的研究工作。

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崔光凯（2000-），男（汉族），山东济宁人，硕士生，主要从事高电压试验技术和气体放电方面的研究工作。

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崔光凯（2000-），男（汉族），山东济宁人，硕士生，主要从事高电压试验技术和气体放电方面的研究工作。

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Beijing:Chemical Industry Press,2002:195-334., articleTitle=null, refAbstract=null)], funds=[Fund(id=1193616221045227851, tenantId=1146029695717560320, journalId=1149653034449285133, articleId=1193230866802504289, awardId=3192038, language=CN, fundingSource=北京市自然科学基金面上项目(3192038), fundOrder=null, country=null)], companyList=[AuthorCompany(id=1193616217039667467, tenantId=1146029695717560320, journalId=1149653034449285133, articleId=1193230866802504289, xref=null, ext=[AuthorCompanyExt(id=1193616217043861772, tenantId=1146029695717560320, journalId=1149653034449285133, articleId=1193230866802504289, companyId=1193616217039667467, language=EN, country=null, province=null, city=null, postcode=null, companyName=null, departmentName=null, remark=Beijing Key Laboratory of High Voltage & EMC, North China Electric Power University, Beijing 102206, China), AuthorCompanyExt(id=1193616217052250381, tenantId=1146029695717560320, journalId=1149653034449285133, articleId=1193230866802504289, companyId=1193616217039667467, language=CN, country=null, province=null, city=null, postcode=null, companyName=null, departmentName=null, remark=华北电力大学 高电压与电磁兼容北京市重点实验室，北京 102206)])], figs=[ArticleFig(id=1193616219384283449, tenantId=1146029695717560320, journalId=1149653034449285133, articleId=1193230866802504289, language=EN, label=Fig.1, caption=Calculation process of quantum chemistry, figureFileSmall=XiBLJlNHXhRNW8HPqK/W3w==, figureFileBig=fQWUxqcPX4YQp/1qnYfL0w==, tableContent=null), ArticleFig(id=1193616219463975226, tenantId=1146029695717560320, journalId=1149653034449285133, articleId=1193230866802504289, language=CN, label=图1, caption=量子化学计算流程, figureFileSmall=XiBLJlNHXhRNW8HPqK/W3w==, figureFileBig=fQWUxqcPX4YQp/1qnYfL0w==, tableContent=null), ArticleFig(id=1193616219577221435, tenantId=1146029695717560320, journalId=1149653034449285133, articleId=1193230866802504289, language=EN, label=Fig.2, caption=Schematic diagram of molecular bond breaking positions, figureFileSmall=4K3AYkJcA4xsKMeXK5O21Q==, figureFileBig=Vivc3erLUlRKVnXdrYp1TQ==, tableContent=null), ArticleFig(id=1193616219635941692, tenantId=1146029695717560320, journalId=1149653034449285133, articleId=1193230866802504289, language=CN, label=图2, caption=分子键断裂位置示意图, figureFileSmall=4K3AYkJcA4xsKMeXK5O21Q==, figureFileBig=Vivc3erLUlRKVnXdrYp1TQ==, tableContent=null), ArticleFig(id=1193616219703050557, tenantId=1146029695717560320, journalId=1149653034449285133, articleId=1193230866802504289, language=EN, label=Fig.3, caption=Reaction process and energy changes (298.15K), figureFileSmall=yY7UmmSW864+qGnk8m4oZg==, figureFileBig=vsPxh2oWFJKK8iesKbhSIw==, tableContent=null), ArticleFig(id=1193616219778548030, tenantId=1146029695717560320, journalId=1149653034449285133, articleId=1193230866802504289, language=CN, label=图3, caption=反应过程及能量变化（298.15 K）, figureFileSmall=yY7UmmSW864+qGnk8m4oZg==, figureFileBig=vsPxh2oWFJKK8iesKbhSIw==, tableContent=null), ArticleFig(id=1193616219858239807, tenantId=1146029695717560320, journalId=1149653034449285133, articleId=1193230866802504289, language=EN, label=Fig.4, caption=Generation pathways and structural diagrams of main characteristic products containing H element, figureFileSmall=Tjd5Z8nPVC/zSh3R8PaOzw==, figureFileBig=UD8lVG2zpCTldzwdG9m3DQ==, tableContent=null), ArticleFig(id=1193616219992457536, tenantId=1146029695717560320, journalId=1149653034449285133, articleId=1193230866802504289, language=CN, label=图4, caption=主要含H元素特征产物的生成路径及结构图, figureFileSmall=Tjd5Z8nPVC/zSh3R8PaOzw==, figureFileBig=UD8lVG2zpCTldzwdG9m3DQ==, tableContent=null), ArticleFig(id=1193616220105703745, tenantId=1146029695717560320, journalId=1149653034449285133, articleId=1193230866802504289, language=EN, label=Fig.5, caption=The variation of free energy of characteristic products containing H element with temperature, figureFileSmall=cIPO2YzoaLa3hgpn4tGxwQ==, figureFileBig=LH2RAZecIhQPEiZshs2kOA==, tableContent=null), ArticleFig(id=1193616220164424002, tenantId=1146029695717560320, journalId=1149653034449285133, articleId=1193230866802504289, language=CN, label=图5, caption=含氢元素特征产物的自由能随温度变化图, figureFileSmall=cIPO2YzoaLa3hgpn4tGxwQ==, figureFileBig=LH2RAZecIhQPEiZshs2kOA==, tableContent=null), ArticleFig(id=1193616220298641731, tenantId=1146029695717560320, journalId=1149653034449285133, articleId=1193230866802504289, language=EN, label=Fig.6, caption=Reaction rate lnk varies with temperature, figureFileSmall=X0g3fWlBCdzfrsGxzemXXg==, figureFileBig=WzHdGRYfNMnfbP+ys9k6PQ==, tableContent=null), ArticleFig(id=1193616220537717060, tenantId=1146029695717560320, journalId=1149653034449285133, articleId=1193230866802504289, language=CN, label=图6, caption=反应速率lnk随温度变化曲线, figureFileSmall=X0g3fWlBCdzfrsGxzemXXg==, figureFileBig=WzHdGRYfNMnfbP+ys9k6PQ==, tableContent=null), ArticleFig(id=1193616220592243013, tenantId=1146029695717560320, journalId=1149653034449285133, articleId=1193230866802504289, language=EN, label=Table 1, caption=Reaction process and energy changes（298.15 K）, figureFileSmall=null, figureFileBig=null, tableContent=
编号反应路径自由能/(kJ/mol)活化能/(kJ/mol)
A1C4F7N→(CF3)2CCN·+F·328.19—
A2C4F7N+H·→(CF3)2CCN·+HF-183.7997.93
A3C4F7N+H·→(CF3)2CHCN+F·-21.00126.04
B1C4F7N→CF3CFCN·+CF3·228.42—
B2C4F7N+H·→CF3CFCN·+CF3H-178.53149.65
B3C4F7N+H·→CF3CFHCN+CF3·-112.90139.15
B4C4F7N+HO·→CF3CFCN·+CF3OH-173.28131.28
C1C4F7N→(CF3)2CF·+CN·383.32—
C2C4F7N+H·→C3HF7+CN·-5.25133.90
C3C4F7N+H·→C3F7·+HCN-196.91217.92
C4C4F7N+HO·→C3F7OH+CN·28.88238.92
D1C4F7N→CF3CF2CFCN·+F·438.72—
D2C4F7N+H·→CF3CF2HCFCN+F·53.30244.17
D3C4F7N+H·→CF3CF2CFCN·+HF-73.25123.40
E1C4F7N→CF3CF2CFCN·+F·441.08—
E2C4F7N+H·→CF3CF2HCFCN+F·54.09249.42
E3C4F7N+H·→CF3CF2CFCN·+HF-71.15127.34
F1C4F7N→CF3CF2CFCN·+F·438.98—
F2C4F7N+H·→CF3CF2HCFCN+F·49.62240.32
F3C4F7N+H·→CF3CF2CFCN·+HF-72.99126.02
), ArticleFig(id=1193616220650963270, tenantId=1146029695717560320, journalId=1149653034449285133, articleId=1193230866802504289, language=CN, label=表1, caption=

反应过程及能量变化（298.15 K）

, figureFileSmall=null, figureFileBig=null, tableContent=
编号反应路径自由能/(kJ/mol)活化能/(kJ/mol)
A1C4F7N→(CF3)2CCN·+F·328.19—
A2C4F7N+H·→(CF3)2CCN·+HF-183.7997.93
A3C4F7N+H·→(CF3)2CHCN+F·-21.00126.04
B1C4F7N→CF3CFCN·+CF3·228.42—
B2C4F7N+H·→CF3CFCN·+CF3H-178.53149.65
B3C4F7N+H·→CF3CFHCN+CF3·-112.90139.15
B4C4F7N+HO·→CF3CFCN·+CF3OH-173.28131.28
C1C4F7N→(CF3)2CF·+CN·383.32—
C2C4F7N+H·→C3HF7+CN·-5.25133.90
C3C4F7N+H·→C3F7·+HCN-196.91217.92
C4C4F7N+HO·→C3F7OH+CN·28.88238.92
D1C4F7N→CF3CF2CFCN·+F·438.72—
D2C4F7N+H·→CF3CF2HCFCN+F·53.30244.17
D3C4F7N+H·→CF3CF2CFCN·+HF-73.25123.40
E1C4F7N→CF3CF2CFCN·+F·441.08—
E2C4F7N+H·→CF3CF2HCFCN+F·54.09249.42
E3C4F7N+H·→CF3CF2CFCN·+HF-71.15127.34
F1C4F7N→CF3CF2CFCN·+F·438.98—
F2C4F7N+H·→CF3CF2HCFCN+F·49.62240.32
F3C4F7N+H·→CF3CF2CFCN·+HF-72.99126.02
), ArticleFig(id=1193616220726460743, tenantId=1146029695717560320, journalId=1149653034449285133, articleId=1193230866802504289, language=EN, label=Tab. 2, caption=Reaction process and energy change of characteristic products containing H element (298.15 K), figureFileSmall=null, figureFileBig=null, tableContent=
编号反应路径自由能/(kJ/mol)
R1F·+H·→HF-505.39
R2HO·+ F·→HOF-161.31
R3CF3·+ H·→CHF3-403.68
R4CF3·+ HO·→CHOF3-400.23
R5CN·+H·→HCN-488.00
R6CN·+ HO·→HOCN-446.32
R7(CF3)2CF·+ H·→C3HF7-383.28
R8(CF3)2CF·+ HO·→(CF3)2CHOF-346.19
R9(CF3)2CNC·+ H·→(CF3)2CHCN-342.25
R10(CF3)2CNC·+ HO·→(CF3)2CHOCN-262.00
R11CF3CFCNCF2·+ H·→CF3CHF2CFCN-508.51
R12CF3CFCNCF2·+ HO·→CF3CHOF2CFCN-505.31
R13CF3CNCF·+ H·→CF3CHFCN-336.24
R14(CF3)2CNC·+ HO·→(CF3)2CHOCN-261.99
), ArticleFig(id=1193616220780986696, tenantId=1146029695717560320, journalId=1149653034449285133, articleId=1193230866802504289, language=CN, label=表2, caption=

含H元素特征产物的反应过程及能量变化（298.15 K）

, figureFileSmall=null, figureFileBig=null, tableContent=
编号反应路径自由能/(kJ/mol)
R1F·+H·→HF-505.39
R2HO·+ F·→HOF-161.31
R3CF3·+ H·→CHF3-403.68
R4CF3·+ HO·→CHOF3-400.23
R5CN·+H·→HCN-488.00
R6CN·+ HO·→HOCN-446.32
R7(CF3)2CF·+ H·→C3HF7-383.28
R8(CF3)2CF·+ HO·→(CF3)2CHOF-346.19
R9(CF3)2CNC·+ H·→(CF3)2CHCN-342.25
R10(CF3)2CNC·+ HO·→(CF3)2CHOCN-262.00
R11CF3CFCNCF2·+ H·→CF3CHF2CFCN-508.51
R12CF3CFCNCF2·+ HO·→CF3CHOF2CFCN-505.31
R13CF3CNCF·+ H·→CF3CHFCN-336.24
R14(CF3)2CNC·+ HO·→(CF3)2CHOCN-261.99
), ArticleFig(id=1193616220848095561, tenantId=1146029695717560320, journalId=1149653034449285133, articleId=1193230866802504289, language=EN, label=null, caption=Table 3Reaction rate constants k of each reaction pathway under different temperature L·mol-1·s-1, figureFileSmall=null, figureFileBig=null, tableContent=
编号300 K1 500 K3 000 K
R11.439×101026.543×10286.504×1083
R21.753×10423.260×10164.388×1013
R39.310×10839.307×10236.008×1016
R46.799×10831.518×10231.757×1016
R51.460×101013.051×10272.722×1018
R67.213×10911.475×10252.323×1017
R74.177×10809.619×10232.330×1017
R81.846×10746.415×10205.167×1014
R91.835×10741.476×10221.017×1016
R102.654×10603.972×10175.300×1012
R113.250×10801.817×10232.718×1016
R128.311×10796.143×10211.507×1015
R138.028×10723.816×10213.149×1015
R141.608×10671.448×10196.422×1013
), ArticleFig(id=1193616220915204426, tenantId=1146029695717560320, journalId=1149653034449285133, articleId=1193230866802504289, language=CN, label=表3, caption=

不同温度下各反应路径的反应速率常数k

, figureFileSmall=null, figureFileBig=null, tableContent=
编号300 K1 500 K3 000 K
R11.439×101026.543×10286.504×1083
R21.753×10423.260×10164.388×1013
R39.310×10839.307×10236.008×1016
R46.799×10831.518×10231.757×1016
R51.460×101013.051×10272.722×1018
R67.213×10911.475×10252.323×1017
R74.177×10809.619×10232.330×1017
R81.846×10746.415×10205.167×1014
R91.835×10741.476×10221.017×1016
R102.654×10603.972×10175.300×1012
R113.250×10801.817×10232.718×1016
R128.311×10796.143×10211.507×1015
R138.028×10723.816×10213.149×1015
R141.608×10671.448×10196.422×1013
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微水对C4F7N气体分解产物生成速率的影响
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崔光凯 , 徐焱 , 王璁 , 屠幼萍 , 陈庚 , 樊若岑 , 郑重
绝缘材料 | 环保绝缘气体专题 2025,58(2): 39-45
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绝缘材料 | 环保绝缘气体专题 2025, 58(2): 39-45
微水对C4F7N气体分解产物生成速率的影响
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崔光凯, 徐焱, 王璁, 屠幼萍, 陈庚, 樊若岑, 郑重
作者信息
  • 华北电力大学 高电压与电磁兼容北京市重点实验室，北京 102206

    • 崔光凯（2000-），男（汉族），山东济宁人，硕士生，主要从事高电压试验技术和气体放电方面的研究工作。

通讯作者:

王璁（1980-），男（汉族），江西赣州人，高级工程师，博士，主要从事电气设备外绝缘、气体放电以及电气设备故障诊断的研究工作。
Effect of micro-water on generation rate of C4F7N gas decomposition products
Guangkai CUI, Yan XU, Cong WANG, Youping TU, Geng CHEN, Ruocen FAN, Zhong ZHENG
Affiliations
  • Beijing Key Laboratory of High Voltage & EMC, North China Electric Power University, Beijing 102206, China
出版时间: 2025-02-20 doi: 10.16790/j.cnki.1009-9239.im.2025.02.006
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摘要
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为了探索微水存在条件下全氟异丁腈（C4F7N）气体分解产物的生成机制，本文对微水参与反应时C4F7N气体的分解过程以及分解后重组的过程进行研究，基于密度泛函理论和过渡态理论计算得到C4F7N气体在微水参与反应条件下的热力学参数以及部分特征产物的生成路径和生成速率。结果表明：在微水参与反应时，C4F7N气体分解所需的活化能低于干燥C4F7N气体分解所需的能量，微水的存在使C4F7N气体更容易分解。C4F7N气体分解产物中CHF3气体的反应速率常数较大，化学性质稳定且具有可检性，可以作为微水存在条件下C4F7N气体分解的特征产物。

全氟异丁腈（C4F7N）  /  微水  /  热力学参数  /  反应速率常数

In order to explore the generation mechanism of perfluoroisobutyronitrile (C4F7N) gas decomposition products under the presence of micro-water, the decomposition process of C4F7N gas and the recombination process after decomposition were investigated when micro-water participated in the reaction. On the basis of density functional theory and transition state theory, the thermodynamic parameters of C4F7N gas under micro-water participation reaction conditions, as well as the generation paths and generation rates of some characteristic products, were calculated. The results show that when micro-water participates in the reaction, the activation energy required for the decomposition of C4F7N gas is lower than that required for the decomposition of dry C4F7N gas. The presence of micro-water makes the C4F7N decompose easier. The reaction rate constant of CHF3 gas is relatively high in the decomposition products of C4F7N gas, and its chemical properties are stable and detectable, which can be used as a characteristic product of C4F7N gas decomposition under the presence of micro-water.

perfluoroisobutyronitrile (C4F7N)  /  micro-water  /  thermodynamic parameters  /  reaction rate constant
崔光凯, 徐焱, 王璁, 屠幼萍, 陈庚, 樊若岑, 郑重. 微水对C4F7N气体分解产物生成速率的影响. 绝缘材料, 2025 , 58 (2) : 39 -45 . DOI: 10.16790/j.cnki.1009-9239.im.2025.02.006
Guangkai CUI, Yan XU, Cong WANG, Youping TU, Geng CHEN, Ruocen FAN, Zhong ZHENG. Effect of micro-water on generation rate of C4F7N gas decomposition products[J]. Insulating Materials, 2025 , 58 (2) : 39 -45 . DOI: 10.16790/j.cnki.1009-9239.im.2025.02.006
正文
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0 引言
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全氟异丁腈（C4F7N）气体是一种具有高绝缘强度的环保气体绝缘介质，在0.1 MPa气压下，纯C4F7N气体的绝缘强度为SF6气体的两倍，且温室效应潜能值（global warming potential，GWP）仅为SF6的1/11，是目前最具潜力的SF6替代气体之一[1-4]。
近年来，以C4F7N及其他缓冲气体的混合气体作为绝缘介质的电气设备正在大力研发推广。气体绝缘设备在生产制造过程中因难以做到完全密封，其内部难免会存在微量水分[5]。目前，有关微水对绝缘气体分解特性的影响研究主要集中在SF6气体及其设备上[6-10]，微水的存在会促进SF6气体的分解，高含量的水分会导致硫化固体析出，进而导致设备内部的绝缘强度降低；微水的存在还会影响基于SF6气体分解组分的设备内部故障诊断方法的诊断效果，对气体绝缘设备的运行维护产生影响；当气体绝缘设备发生局部放电导致绝缘气体分解时，微水还会与绝缘气体的分解产物发生反应，生成具有毒性和腐蚀性的物质，进一步加速绝缘劣化。上述研究为SF6气体绝缘设备的应用提供了重要理论指导。
针对微水对环保绝缘气体分解特性影响的研究对于环保气体绝缘设备的应用同样具有工程价值。目前，研究人员主要从模拟试验和仿真计算两个角度开展微水对环保绝缘气体分解特性的影响研究。模拟试验方面，杨圆等[11]在不同微水含量条件下对C4F7N/CO2混合气体开展工频击穿和悬浮放电分解试验，研究发现随着微水含量的增大，C4F7N/CO2混合气体的工频击穿电压降低且部分放电分解产物的含量增加。仿真计算方面，张晓星等[12]利用密度泛函理论（density functional theory，DFT）以及过渡态理论（transition state theory，TST）仿真模拟了微水存在下三氟碘甲烷（CF3I）的放电分解过程，研究指出微水的存在会导致CF3I的放电分解过程更为复杂，且分解产物种类增加，从而影响CF3I分子本身的动态平衡，导致其绝缘性能降低。然而，有关微水对C4F7N环保气体分解特性影响的研究较少，微水对C4F7N气体分解的作用机制以及特征产物的生成机制尚不明确。
本研究基于密度泛函理论和过渡态理论探究微水的存在对C4F7N气体放电分解过程的影响规律，分析在微水存在条件下C4F7N气体的分解路径以及C4F7N气体放电分解过程中可能生成的特征产物，研究微水对C4F7N气体放电分解产物的影响规律，为进一步研究气体绝缘设备中C4F7N及其混合气体的分解过程及分解产物提供数据参考。
1 计算方法
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C4F7N气体在放电或过热条件下发生分解的过程是一种化学反应。为了探究微水对C4F7N气体分解特性的影响机制，可以利用量子化学理论从微观角度对微水存在条件下C4F7N气体分子分解过程中的热力学参数进行仿真计算。量子化学是利用量子力学基本原理解决化学问题的方法理论，其主要求解工具为薛定谔（Schrodinger）方程[13]，如式（1）所示。
H^ψ=Eψ
式（1）中：H^为Hamilton算符，对应于体系的波函数总能量；ψ为定态波函数；E为体系总能量。
Schrodinger方程的求解过程极其复杂，目前主流的求解方法为1964年P HOHENBERG和W KOHN以Thomas-Fermi模型为基础提出的密度泛函理论（DFT）方法[14]。DFT方法具有计算简便以及精度较高等优势，其中决定密度泛函计算精度的是泛函和基组的选择[15]。相较于普通泛函，B3LYP杂化泛函具有更高的计算精度以及较低的计算成本；DGDZVP基组适用的元素种类丰富且计算精度满足C4F7N气体的计算要求[16]，因此本研究选用B3LYP杂化泛函和DGDZVP基组进行量子化学仿真计算。
量子化学仿真计算使用美国GAUSSIAN公司推出的Gaussian 09W专业量子化学仿真软件。Gaussian 09W软件内涵盖了现阶段可能使用到的所有量子化学计算理论及计算方法，可以为本研究提供所需的计算工具。由于针对C4F7N气体分解的研究已较为全面，本研究仅针对有、无微水两种情况下C4F7N气体的分解反应过程进行分析。首先采用B3LYP杂化泛函和DGDZVP基组对分子结构进行优化，并对每条反应路径的吉布斯自由能进行计算，再使用过渡态理论（TST）方法进行过渡态结构的搜索，其中TST方法是通过计算搜索化学反应过程中存在的过渡态结构，来解释反应物和生成物之间化学反应的机理[13]。然后对搜索结果进行频率分析，测试是否只含有1个虚频，并结合内禀反应坐标（intrinsic reaction coordinate，IRC）法分析获得的过渡态结构，最终求得反应过程中的自由能变化以及活化能。量子化学计算流程如图1所示，计算方法如式（2）所示。
ΔG=∑G1-∑G0
式（2）中：G0为反应物自由能；若G1为生成物自由能时，ΔG则为反应过程中的自由能变化值，若G1为过渡态自由能时，ΔG则为反应过程的活化能。
反应速率常数是化学反应快慢的量化表征参数，使用TST方法可以计算各反应的反应速率[17]。反应速率常数（kTST(T)）的计算公式如式（3）所示。
kTST(T)=σkBTh(RTP0)Δnexp[-ΔG0,≠(T)kBT]
式（3）中：σ是反应路径简并度；kB是玻尔兹曼常数；T是反应体系温度；h是普朗克常量；R是理想气体常数；P0是标准大气压；Δn=n-1，n是分子数量；∆G0,≠(T)是标准态吉布斯自由能。反应路径简并度（σ）的计算公式如式（4）所示。
σ=σ(R)n(R)σ(TS)n(TS)
式（4）中：σ(R)、σ(TS)分别是反应物和过渡态的转动对称数，可根据优化后的分子结构得到；n(R)、n(TS)分别是反应物和过渡态手性异构体的数量。
2 微水对C4F7N气体分解的影响
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C4F7N气体在放电故障以及高温过热情况下会发生分解生成各种分解产物，根据文献[18]中C4F7N气体的分解产物生成路径可知，C2F4、CF4、C3F8、CF3CN、CNCN等分解产物的最终生成数量主要取决于混合气体中CF2·、CF3·、F·、(CF3)2CF·、CN·自由基的含量。而这5种自由基均由C4F7N分子分解产生，因此C4F7N气体分子的分解过程以及分解率将会影响自由基含量，即影响产物的最终生成量。在C4F7N气体分解过程中，气体中存在的微水会与C4F7N气体分子发生反应，生成一系列产物，从而对C4F7N气体分子的分解过程及分解率产生影响。
在故障条件作用下，C4F7N分子和H2O分子中共价键可能的断裂情况如图2所示。考虑到CN共价三键的键能较高且不易断裂，本研究不考虑其断裂的情况。
从图2可以看出，C4F7N分子在初步裂解反应中可以生成CF3·、F·、CN·、(CF3)2CF·等自由基，H2O分子的共价键断裂后可以得到H·和HO·自由基。
有、无微水情况下，C4F7N气体的分解过程及反应过程中的能量变化（298.15 K）如表1和图3所示，在图3中给出了反应物、产物以及过渡态的物质结构，由于D和F系列的反应过程及计算能量大致相同，图中只给出了D系列的反应过程及计算能量。
由计算结果可知，C4F7N分子的初步分解路径A1、B1、C1、D1没有过渡态的反应。A1和B1分解路径的自由能相对较小，C1分解路径的自由能相对较大，因此在外部故障条件下CN·自由基相对CF3·和F·自由基不易产生。相应地由CN·、CF3·生成的CF3CN气体相对由CF3·和F·生成的CF4气体含量更低，而由两个CN·结合生成的CNCN产物更不易产生，即相同故障条件下，干燥的C4F7N气体分解产物的含量从高到低应为CF4、CF3CN、CNCN，与文献[11]的试验结果相符。
在H·和HO·自由基参与下，C4F7N气体分解过程中虽存在过渡态，但所需的活化能均低于干燥C4F7N分解所需的能量，且吉布斯自由能由正变负，反应过程由吸热反应转变为放热反应，分解过程的热力学方向和自发性发生了变化，从而使得分解反应更容易进行。因此，微水促进了C4F7N气体的分解过程。随着微水含量的增加，混合气体中H·和HO·自由基的数量增多，C4F7N气体的分解率相应升高，从而使得分解产物的生成量与微水含量呈正相关关系。
微水存在条件下，A1、B1、C1、D1、E1、F1反应路径中生成F·、CF3·、CN·、F·、F·、CF3CF2CFCN·自由基所需要的最小能量，分别是无微水条件下的0.38、0.61、0.35、0.56、0.57和0.55倍。可以看出，混合气体中存在微水时，C1路径的反应能量降低最显著，从而促进了含CN基团的分解产物生成。
3 微水存在下C4F7N气体的特征产物生成分析
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C4F7N气体在外界故障条件下可以分解生成多种自由基且分解反应过程复杂，C4F7N气体分解后主要产生CF3·、CF3CNCF·、F·、CN·、(CF3)2CF·以及(CF3)2CNC·等自由基[18]，为了进一步研究微水存在条件下C4F7N气体的分解特性，对C4F7N气体分解产生的自由基进行结构分析并给出自由基进行复合反应生成含H元素特征产物的路径。C4F7N气体在故障条件下分解产生的自由基与水分子分解产生的H·和HO·自由基互相组合，可以生成HF、HCN、CHF3以及C3HF7等物质，图4为主要含H元素特征产物的生成路径及结构图（298.15 K），表2给出了含H元素特征产物的生成路径及能量变化（298.15 K）。
由表2可以看出，在外部故障条件下，C4F7N气体分解产生的自由基与微水分解产生的H·和HO·自由基进行复合反应，生成含H元素特征产物的过程均释放热量，这表明H·和HO·自由基的存在可以阻碍C4F7N气体分解后再复原。微水存在条件下C4F7N气体分解产物中，氟化氢（HF）、次氟酸（HOF）以及氰化氢（HCN）等都具有腐蚀性和毒性，会降低C4F7N设备的绝缘性能。
为了进一步研究故障条件下C4F7N气体分解并生成含H元素特征产物的特性，计算了300～3 000 K温度范围内R1～R14反应路径复合过程的自由能，并根据式（3）计算出各个反应路径的反应速率常数k。图5为各反应路径自由能随温度变化曲线图，表3为各产物生成路径在300、1 500、3 000 K温度下的反应速率常数k。
由于各反应路径的反应速率常数在不同温度下的差值较大，为方便比较各反应路径反应的快慢，计算了反应速率常数的lnk值[17]，图6为反应速率常数的lnk值随温度的变化曲线。
由于微水存在条件下H·和HO·自由基的数量较少，H·和HO·自由基与C4F7N气体一次分解产生的自由基复合反应在理论上不会存在竞争关系，但是H·和HO·自由基会与更易发生反应的碳氟自由基进行复合。由表3和图6可知，生成HF、HCN、CHF3以及C3HF7等产物的复合反应速率较大，且在高温下仍为放热反应，这些产物理论上更易形成。但是HF和HCN的化学性质极不稳定[19]，不易被检测，而CF3CHF2CFCN和CF3CHOF2CFCN物质的检测手段较为困难，以上物质不能作为判别C4F7N气体分解是否涉及微水的特征产物。三氟甲烷（CHF3）的熔点为-160℃，沸点为84℃，常温常压下是无色、无味气体，不易燃且化学性质稳定，具有良好的介电特性以及较高的热稳定性，可以通过氦离子化脉冲放电检测器气相色谱仪（gas chromatography-pulsed discharge helium ionization detector，GC-PDHID）进行定量检测[11,20]。路径R3给出298.15 K温度下CF3·和H·自由基复合反应生成CHF3气体的自由能为-403.68 kJ/mol，且在不同温度下该复合反应的反应速率常数k大于大多数含H元素特征产物的复合反应。文献[12]通过试验研究了微水存在条件下C4F7N/CO2混合气体的悬浮放电分解特性，指出低微水含量（小于321 μL/L）下CHF3气体基本不产生，随着微水含量的增加，CHF3气体的生成量呈线性增长趋势，表明CHF3可以作为微水存在条件下C4F7N气体分解的特征产物。
4 结论
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本文研究了微水存在条件下环保型C4F7N气体的分解过程，基于密度泛函理论和过渡态理论计算得到了C4F7N分子在水分子参与分解反应时的热力学参数以及部分特征产物的生成路径、能量变化、反应速率常数，主要得到以下结论：
（1）微水会加速C4F7N气体分解，在外部故障条件下，微水分解产生的H·和HO·自由基参与C4F7N气体的分解，使C4F7N气体分解所需的活化能降低，部分反应路径的自由能由正变负，反应过程由吸热反应转变为放热反应，分解过程的热力学方向和自发性发生了变化，从而使得C4F7N气体的分解反应更容易进行。
（2）微水含量越高，C4F7N气体的分解率越高，微水存在条件下C4F7N气体分解生成CF3·、F·、(CF3)2CF·、CN·等自由基所需要的能量变少，是无微水条件下的0.3～0.6倍。
（3）微水条件下C4F7N气体一次分解产生的自由基与H·和HO·自由基的复合反应为放热反应，复合生成的部分产物具有腐蚀性和毒性，会降低设备绝缘性能，破坏C4F7N气体的动态平衡。生成CHF3气体的复合反应速率常数k高于大多数含H元素特征产物的复合反应，且CHF3化学性质稳定，具有可检性，可以作为微水存在条件下C4F7N气体分解的特征产物。
基金
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  • 北京市自然科学基金面上项目(3192038)
文献
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doi: 10.16790/j.cnki.1009-9239.im.2025.02.006
  • 接收时间：2024-05-13
  • 首发时间：2025-11-06
  • 出版时间：2025-02-20
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  • 收稿日期：2024-05-13
  • 修回日期：2024-06-18
基金
北京市自然科学基金面上项目(3192038)
作者信息
    华北电力大学 高电压与电磁兼容北京市重点实验室，北京 102206

通讯作者:

王璁（1980-），男（汉族），江西赣州人，高级工程师，博士，主要从事电气设备外绝缘、气体放电以及电气设备故障诊断的研究工作。
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