六氟化硫替代气体的研究现状及未来发展趋势

doi:10.16085/j.issn.1000-6613.2023-0724

化工进展 ›› 2023, Vol. 42 ›› Issue (8): 4093-4107.DOI: 10.16085/j.issn.1000-6613.2023-0724

六氟化硫替代气体的研究现状及未来发展趋势

杨志强¹(), 曾纪珺¹(), 马义丁¹, 尉涛¹, 赵波¹, 刘英哲¹, 张伟¹, 吕剑¹(), 李兴文², 张博雅², 唐念³, 李丽³, 孙东伟³

^1.西安近代化学研究所氟氮化工资源高效开发与利用国家重点实验室，陕西西安 710065
^2.西安交通大学电力设备电气绝缘国家重点实验室，陕西西安 710049
^3.广东电网有限责任公司电力科学研究院，广东广州 510699

收稿日期:2023-05-04 修回日期:2023-08-10 出版日期:2023-08-15 发布日期:2023-09-19
通讯作者: 吕剑
作者简介:杨志强（1984—），男，博士，研究员，主要研究领域为含氟专用化学品的热物性及其应用基础。E-mail: zqyangs@stu.xjtu.edu.cn
曾纪珺（1984—），男，博士研究生，研究员，主要研究领域为环保氟代烃的催化反应合成及工程化技术。E-mail: huajun_8484@163.com。
基金资助:
国家自然科学基金(52277162);中国南方电网有限责任公司重点研发项目(GDKJXM20220361)

Research status and future trend of sulfur hexafluoride alternatives

YANG Zhiqiang¹(), ZENG Jijun¹(), MA Yiding¹, YU Tao¹, ZHAO Bo¹, LIU Yingzhe¹, ZHANG Wei¹, LYU Jian¹(), LI Xingwen², ZHANG Boya², TANG Nian³, LI Li³, SUN Dongwei³

^1.State Key Laboratory of Fluorine & Nitrogen Chemicals, Xi’an Modern Chemistry Research Institute, Xi’an 710065, Shaanxi，China
^2.State Key Laboratory of Electrical Insulation and Power Equipment, Xi’an Jiaotong University, Xi’an 710049, Shaanxi, China
^3.Electric Power Research Institute of Guangdong Power Grid Co. , Ltd. , Guangzhou 510080, Guangdong, China

Received:2023-05-04 Revised:2023-08-10 Online:2023-08-15 Published:2023-09-19
Contact: LYU Jian

摘要/Abstract

摘要：

六氟化硫（SF₆）是电力行业应用最为广泛的绝缘和灭弧介质。然而，SF₆具有极高的温室效应潜值（GWP = 23900），其引起的环境问题逐渐成为制约我国电网绿色发展的重要因素。本文首先回顾了SF₆替代气体试错法和计算机辅助法的筛选历程，综述了全氟酮、全氟异丁腈、三氟硫氮、氢氟烯烃等候选物在绝缘性能和制备方法两方面的研究成果。随后聚焦SF₆替代气体筛选中的核心问题，分别从物理定义、基团贡献、定量构效关系和机器学习的角度，回顾了绝缘气体各性能预测方法的研究进展，指出同时兼顾计算效率、精确性和泛用性的预测方法是未来的发展趋势。基于目前的研究现状，提出了高通量分子设计和共沸绝缘气体两种研发思路，以期为我国绝缘环保气体的研发提供有益的借鉴。

关键词: 六氟化硫, 环保绝缘气体, 分子设计, 共沸气体

Abstract:

Sulfur hexafluoride (SF₆) is the most widely used insulation and arc extinguishing medium in the power industry. However, SF₆ has a strong global warming potential (GWP=23900), and the environmental problems caused by it have gradually become an important factor restricting the green development of the power grid in China. This paper reviewed the screening history of SF₆ substitutes from the view of testing methods and computer-aided methods. The authors also summarized the research progress of perfluoroketone, perfluoroisobutyronitrile, trifluorosulfur nitrogen, hydrofluoroolefin, and other gases in both insulation properties and synthesis mothed. Focus on the core issues in the screening of SF₆ alternative gases, the research progress of various predictive methods for the performance of insulating gases was reviewed from the perspectives of physical definition, group contribution, quantitative structure-activity relationship, and machine learning, and authors pointed out that the prediction method that takes into account the calculation efficiency, accuracy, and versatility is the future development trend. Based on the current research status, two methods of high-throughput molecular design and azeotropic gas were proposed, which provided a useful references for the development of novel eco-friendly insulating gases.

Key words: sulfur hexafluoride, eco-friendly insulating gas, molecular design, azeotropic gas

中图分类号:

O641.1

杨志强, 曾纪珺, 马义丁, 尉涛, 赵波, 刘英哲, 张伟, 吕剑, 李兴文, 张博雅, 唐念, 李丽, 孙东伟. 六氟化硫替代气体的研究现状及未来发展趋势[J]. 化工进展, 2023, 42(8): 4093-4107.

YANG Zhiqiang, ZENG Jijun, MA Yiding, YU Tao, ZHAO Bo, LIU Yingzhe, ZHANG Wei, LYU Jian, LI Xingwen, ZHANG Boya, TANG Nian, LI Li, SUN Dongwei. Research status and future trend of sulfur hexafluoride alternatives[J]. Chemical Industry and Engineering Progress, 2023, 42(8): 4093-4107.

图/表 14

图1 单质气体宏观性的固有矛盾

表1 常见绝缘气体的基本性质

绝缘气体	化学式	相对绝缘强度	标准大气压下的沸点/℃	GWP
六氟化硫	SF₆	1	-64	23900
全氟戊酮	C₅F₁₀O	约2	26.9	1
全氟已酮	C₆F₁₂O	>2	49	1
全氟异丁腈	C₄F₇N	约2.2	-4.7	2210
三氟硫氮	NSF₃	1.35	-27.1	916
四氟丙烯(E-HFO1234ze)	C₃H₂F₄	0.82	-18.9	4
六氟丁二烯(E-HFO1336mzz)	C₄H₂F₄	1.6	7.5	10
二氧化碳	CO₂	约0.3	-78.5	1
氮气	N₂		-196	0
空气	—		-194	0
氧气	O₂		-182	0

图2 三氟乙酰氟、六氟丙烯加成制备C5-PFK

图3 C6-PFK的制备方法

图4 C4-PFN的制备方法

图5 NSF3的主要制备方法

图6 HFO-1234ze(E)的主要制备方法

图7 HFO-1336mzz(E)的主要制备工艺

表2 基团贡献法预测气体沸点的模型

编号	年份	模型	参量	效果	文献
1	1987	$198.2 + Σ$	基团类型和数目	未考虑各基团所处的化学环境不同。对中等大小的分子描述较好（测试集中的标准偏差为17.9K），但对于较小或较大分子的预测误差较大	[82]
2	1994	模型1的改进版	基团类型和数目	根据基团所处的化学环境对其贡献进行了更细致的规定。考虑了基团间的协同作用。数据得到了明显扩充，达到4426种分子，计算标准偏差为24.6K	[83]
3	2004	$∑ N i C i n a + b + c$	分子的饱和度、芳香性、氢键等	训练集为2812种分子，对其测试集中199种分子预测的标准偏差为6.37K。基团拆分繁复，且在基团贡献中要同时考虑该基团α位和β位上的原子或基团，容易在计算过程中造成冲突	[84]
4	2016	$T 1 K + T 2 K$ $T 1 K = ∑ i N i t b i + (Q 1) ∑ j N j (t b i)$ $T 2 K = Q 2 a M w 3 + b M w 2 + c M w + d$	T₁反映了分子中的基团组成情况对沸点的影响；T₂反映了分子量对沸点的影响	模型包含122种基团和2036种有机分子沸点，较好地反映了含有36个以下碳原子、分子量小于555的有机分子沸点，平均偏差4.35K。但是方法非常复杂，通过复杂的查表计算才能获得多个模型系数，且该方法的基团并非以最小单位拆分，造成基团拆分方法不唯一，实际操作中难以达成最优效果	[85]

表2 基团贡献法预测气体沸点的模型

编号	年份	模型	参量	效果	文献
1	1987	$198.2 + Σ$	基团类型和数目	未考虑各基团所处的化学环境不同。对中等大小的分子描述较好（测试集中的标准偏差为17.9K），但对于较小或较大分子的预测误差较大	[82]
2	1994	模型1的改进版	基团类型和数目	根据基团所处的化学环境对其贡献进行了更细致的规定。考虑了基团间的协同作用。数据得到了明显扩充，达到4426种分子，计算标准偏差为24.6K	[83]
3	2004	$∑ N i C i n a + b + c$	分子的饱和度、芳香性、氢键等	训练集为2812种分子，对其测试集中199种分子预测的标准偏差为6.37K。基团拆分繁复，且在基团贡献中要同时考虑该基团α位和β位上的原子或基团，容易在计算过程中造成冲突	[84]
4	2016	$T 1 K + T 2 K$ $T 1 K = ∑ i N i t b i + (Q 1) ∑ j N j (t b i)$ $T 2 K = Q 2 a M w 3 + b M w 2 + c M w + d$	T₁反映了分子中的基团组成情况对沸点的影响；T₂反映了分子量对沸点的影响	模型包含122种基团和2036种有机分子沸点，较好地反映了含有36个以下碳原子、分子量小于555的有机分子沸点，平均偏差4.35K。但是方法非常复杂，通过复杂的查表计算才能获得多个模型系数，且该方法的基团并非以最小单位拆分，造成基团拆分方法不唯一，实际操作中难以达成最优效果	[85]

表3 QSPR预测绝缘强度的模型

编号	年份	模型	参量	效果	文献
1	1982	$5.426 × 10 - 3 ε i α 1.5$	电离能ε_i 和极化率α	采用最小二乘法线性拟合了41种气体分子的绝缘强度与电离能、极化率之间的关系，模型相关系数R²=0.828，个别气体计算偏差较大，偏差最大达到了0.73	[86]
2	2004	$0.068 × I O A$	积分光吸收强度IOA	采用DFT方法在BLYP/DNP水平下计算43种分子IOA参数，模型的相关系数R仅为0.85（R²=0.7259），误差较大，且存在IOA计算量大、难计算的弊端	[87]
3	2013	$3.8 × 10 - 3 μ 0.3 N e 1.3 + 5.6 × 10 - 4 α 0.6 (ε i a) 2.8 - 1.05$ （极性） $1.2 × 10 - 3 α 1.5 (ε i a) 1.7 - 6.51 × 10 - 8 α 6.5 ε a V - ε a a 2.4 + 0.0173$ （非极性）	绝热电离能 $ε i a$ ，垂直电子亲和能 $ε a V$ ，绝热电子亲和能 $ε a a$ ，偶极矩μ，电子数N_e	采用DFT方法在BP86/def-TZVP和BP86/def2-QZVPP水平下计算了67种分子的描述符，建立了极性和非极性气体的两个构效关系模型，极性气体的模型相关系数R=0.84（R²=0.71），非极性气体的模型相关系数R=0.96（R²=0.71）。两个模型建模过程比较复杂，且样本量多的极性气体相关系数比样本量少的非极性分子相关系数更低	[88]
4	2016	$0.088 α + 0.08 ε a + 0.306$	极化率与电子亲合能	采用DFT方法在M06-2X/6-311+G(3df)水平下计算了24种分子的描述符，获得了相关系数R仅为0.78（R²=0.602）的线性模型	[19]
5	2016	$- 2.7 l g E v + 0.03 + 0.012 S - 1.6$	垂直电子亲和能E_v，等效截面积S	采用DFT方法计算了几种典型有机气体的描述符，模型样本量少，对外部气体的预测能力弱	[89]
6	2017	$0.36 A s 2 + 0.054 n S t o t 2 - 1.97 Π + 0.33 α χ + 0.36$	相互作用性质函数（GIPF）：A_s， $n$ ， $S t o t 2$ ， $Π$ ，电子参数 $α$ ， $χ$	采用DFT方法在M06-2X/6-31++G(d，p)水平下计算了43种分子的描述符，最优模型相关系数R²达到0.985	[89]
7	2018	$- 1.846 + 0.028 x m w - 0.062 x n e + 0.218 x E n + 0.139 x μ + 0.258 x a$	分子质量x_mw，电负性指数x_En，电子数x_ne，偶极矩x_μ，极化率x_a	采用DFT方法在B3LYP/6-311G++(d，p)水平下计算了104种气体分子的描述符，模型相关系数R=0.948	[90]
8	2018	$0.299 (A s + 0.783) 2 + 0.922 υ σ t o t 2 - 1.837 Π + 0.0391 (ρ A S, r +) 2$	表面积A_s，表面静电势分布情况 $υ σ t o t 2$ ，分子表面上静电势的统计平均偏差 $Π$ ，电子密度ρ，正静电势的分子表面积 $A S, r +$	采用DFT方法在M06-2X/6-31G+(d)水平下计算得到43种分子的描述符，模型相关系数R=0.993，平均绝对偏差MAD=0.0609，均方根误差σ=0.0802，最大偏差δ_max=0.28	[91]
9	2019	$0.004 × D 2 - 0.076 × ε i + ε a 1 + 1 + 32.598 ε i + ε a 0.004 × D 2 - 0.076 ε i - ε a$	第一电离能、第一电子亲和能、偶极矩和极化率等	用DFT方法在B3LYP/6-311G++(d,p)水平下计算了37种分子的描述符，相关系数R²=0.895	[92]
10	2021	$0.414 (A s + 0.9410) 2 + 1.0608 υ σ t o t 2 - 2.806 Π - 0.147 (ρ A s + / Ω) 2$	分子表面积A_s，正静电势面积 $A s +$ ，静电势统计方差 $σ t o t 2$ 正负静电势平衡度 $υ$ ，静电势统计平均偏差Π，分子椭圆度Ω，密度ρ	采用DFT方法在M06-2X/6-31G++(d，p)水平下计算得到65种分子的描述符，模型的相关系数0.844	[73]

表3 QSPR预测绝缘强度的模型

编号	年份	模型	参量	效果	文献
1	1982	$5.426 × 10 - 3 ε i α 1.5$	电离能ε_i 和极化率α	采用最小二乘法线性拟合了41种气体分子的绝缘强度与电离能、极化率之间的关系，模型相关系数R²=0.828，个别气体计算偏差较大，偏差最大达到了0.73	[86]
2	2004	$0.068 × I O A$	积分光吸收强度IOA	采用DFT方法在BLYP/DNP水平下计算43种分子IOA参数，模型的相关系数R仅为0.85（R²=0.7259），误差较大，且存在IOA计算量大、难计算的弊端	[87]
3	2013	$3.8 × 10 - 3 μ 0.3 N e 1.3 + 5.6 × 10 - 4 α 0.6 (ε i a) 2.8 - 1.05$ （极性） $1.2 × 10 - 3 α 1.5 (ε i a) 1.7 - 6.51 × 10 - 8 α 6.5 ε a V - ε a a 2.4 + 0.0173$ （非极性）	绝热电离能 $ε i a$ ，垂直电子亲和能 $ε a V$ ，绝热电子亲和能 $ε a a$ ，偶极矩μ，电子数N_e	采用DFT方法在BP86/def-TZVP和BP86/def2-QZVPP水平下计算了67种分子的描述符，建立了极性和非极性气体的两个构效关系模型，极性气体的模型相关系数R=0.84（R²=0.71），非极性气体的模型相关系数R=0.96（R²=0.71）。两个模型建模过程比较复杂，且样本量多的极性气体相关系数比样本量少的非极性分子相关系数更低	[88]
4	2016	$0.088 α + 0.08 ε a + 0.306$	极化率与电子亲合能	采用DFT方法在M06-2X/6-311+G(3df)水平下计算了24种分子的描述符，获得了相关系数R仅为0.78（R²=0.602）的线性模型	[19]
5	2016	$- 2.7 l g E v + 0.03 + 0.012 S - 1.6$	垂直电子亲和能E_v，等效截面积S	采用DFT方法计算了几种典型有机气体的描述符，模型样本量少，对外部气体的预测能力弱	[89]
6	2017	$0.36 A s 2 + 0.054 n S t o t 2 - 1.97 Π + 0.33 α χ + 0.36$	相互作用性质函数（GIPF）：A_s， $n$ ， $S t o t 2$ ， $Π$ ，电子参数 $α$ ， $χ$	采用DFT方法在M06-2X/6-31++G(d，p)水平下计算了43种分子的描述符，最优模型相关系数R²达到0.985	[89]
7	2018	$- 1.846 + 0.028 x m w - 0.062 x n e + 0.218 x E n + 0.139 x μ + 0.258 x a$	分子质量x_mw，电负性指数x_En，电子数x_ne，偶极矩x_μ，极化率x_a	采用DFT方法在B3LYP/6-311G++(d，p)水平下计算了104种气体分子的描述符，模型相关系数R=0.948	[90]
8	2018	$0.299 (A s + 0.783) 2 + 0.922 υ σ t o t 2 - 1.837 Π + 0.0391 (ρ A S, r +) 2$	表面积A_s，表面静电势分布情况 $υ σ t o t 2$ ，分子表面上静电势的统计平均偏差 $Π$ ，电子密度ρ，正静电势的分子表面积 $A S, r +$	采用DFT方法在M06-2X/6-31G+(d)水平下计算得到43种分子的描述符，模型相关系数R=0.993，平均绝对偏差MAD=0.0609，均方根误差σ=0.0802，最大偏差δ_max=0.28	[91]
9	2019	$0.004 × D 2 - 0.076 × ε i + ε a 1 + 1 + 32.598 ε i + ε a 0.004 × D 2 - 0.076 ε i - ε a$	第一电离能、第一电子亲和能、偶极矩和极化率等	用DFT方法在B3LYP/6-311G++(d,p)水平下计算了37种分子的描述符，相关系数R²=0.895	[92]
10	2021	$0.414 (A s + 0.9410) 2 + 1.0608 υ σ t o t 2 - 2.806 Π - 0.147 (ρ A s + / Ω) 2$	分子表面积A_s，正静电势面积 $A s +$ ，静电势统计方差 $σ t o t 2$ 正负静电势平衡度 $υ$ ，静电势统计平均偏差Π，分子椭圆度Ω，密度ρ	采用DFT方法在M06-2X/6-31G++(d，p)水平下计算得到65种分子的描述符，模型的相关系数0.844	[73]

表4 QSPR预测气体沸点的模型

编号	年份	模型	参量	效果	文献
1	1982	$3.703 ε i α$	电离能ε_i 和极化率α	训练集依托于实验值，拟合度不高，只能用作定性、半定量分析	[86]
2	1993	$a A s + β υ σ t o t 2 - γ$	分子范德华表面积A_s，分子表面的静电势分布情况 $υ σ t o t 2$ ，对应的拟合系数α、β、γ	使用量子化学方法对C、H、O、N、Cl、Br类化合物的分子表面静电势进行计算。由99种化合物组成的测试集的平均误差为36.5K	[93]
3	2013	模型按照极性、非极性和全集合	垂直电子亲和能、极化率、分子偶极矩、分子量、电子数等	对67种绝缘气体组成的数据集拟合得到一系列构效关系模型。对于非极性分子，模型拟合度R²最高达到了0.92。但对于极性分子，模型拟合度较低，对全集合分子的拟合度更低，不足0.5，难以达到实用要求	[88]
4	2013	$1000 × (3.37 + 0.27 α 0.23 μ 0.04 - 2.83 ε i 0.07 m 0.01$	垂直电子亲和能、极化率、分子偶极矩、分子量、电子数等	对含3~5个碳原子的羰基化合物沸点进行拟合，结果表明对这一分子集合，沸点预测的标准偏差为28K，但是模型中各个变量的阶数都很低，难以理解其物理意义，且不能排除过拟合可能	[94]
5	2017	$2.7364 A s + 33.31 υ σ t o t 2 - 72.05$	分子范德华表面积、分子表面静电势分布、正负电荷分离程度和通用相互作用函数	模型2的改进版。54种气体沸点的拟合度R²=0.985，与实验数据的相对偏差σ=0.08。应用此模型对其之前研究中涉及的气体分子进行预测并比较发现相关系数低于0.9，标准偏差最大达到0.27，显示出该模型高度依赖数据集的选择，泛用能力较低	[6]
6	2017	$125.3 Π 2 - 143.2 / A s + 194.7 η 3 - 27.0$	分子范德华表面积、分子表面正负电势分布的平均偏差、化学硬度	模型5修正版，以代替了描述分子表面正负电势面积乘积的电荷平衡度，同时引入化学硬度参数用以描述分子失电子的难易程度。修正后的模型在其测试集内的拟合度R²=0.985	[6]

表4 QSPR预测气体沸点的模型

编号	年份	模型	参量	效果	文献
1	1982	$3.703 ε i α$	电离能ε_i 和极化率α	训练集依托于实验值，拟合度不高，只能用作定性、半定量分析	[86]
2	1993	$a A s + β υ σ t o t 2 - γ$	分子范德华表面积A_s，分子表面的静电势分布情况 $υ σ t o t 2$ ，对应的拟合系数α、β、γ	使用量子化学方法对C、H、O、N、Cl、Br类化合物的分子表面静电势进行计算。由99种化合物组成的测试集的平均误差为36.5K	[93]
3	2013	模型按照极性、非极性和全集合	垂直电子亲和能、极化率、分子偶极矩、分子量、电子数等	对67种绝缘气体组成的数据集拟合得到一系列构效关系模型。对于非极性分子，模型拟合度R²最高达到了0.92。但对于极性分子，模型拟合度较低，对全集合分子的拟合度更低，不足0.5，难以达到实用要求	[88]
4	2013	$1000 × (3.37 + 0.27 α 0.23 μ 0.04 - 2.83 ε i 0.07 m 0.01$	垂直电子亲和能、极化率、分子偶极矩、分子量、电子数等	对含3~5个碳原子的羰基化合物沸点进行拟合，结果表明对这一分子集合，沸点预测的标准偏差为28K，但是模型中各个变量的阶数都很低，难以理解其物理意义，且不能排除过拟合可能	[94]
5	2017	$2.7364 A s + 33.31 υ σ t o t 2 - 72.05$	分子范德华表面积、分子表面静电势分布、正负电荷分离程度和通用相互作用函数	模型2的改进版。54种气体沸点的拟合度R²=0.985，与实验数据的相对偏差σ=0.08。应用此模型对其之前研究中涉及的气体分子进行预测并比较发现相关系数低于0.9，标准偏差最大达到0.27，显示出该模型高度依赖数据集的选择，泛用能力较低	[6]
6	2017	$125.3 Π 2 - 143.2 / A s + 194.7 η 3 - 27.0$	分子范德华表面积、分子表面正负电势分布的平均偏差、化学硬度	模型5修正版，以代替了描述分子表面正负电势面积乘积的电荷平衡度，同时引入化学硬度参数用以描述分子失电子的难易程度。修正后的模型在其测试集内的拟合度R²=0.985	[6]

图8 高通量分子设计筛选策略

表5 具有应用潜力的亚胺化合物

序号	绝缘强度	沸点/K
1	0.87	209
2	1.09	250
3	1.17	273

图9 共沸气体的协同作用

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六氟化硫替代气体的研究现状及未来发展趋势

Research status and future trend of sulfur hexafluoride alternatives

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