CN103618109B - 电解液用阻燃添加剂及阻燃型锂离子电池电解液 - Google Patents
电解液用阻燃添加剂及阻燃型锂离子电池电解液 Download PDFInfo
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- 239000003063 flame retardant Substances 0.000 title claims abstract description 36
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- NKDDWNXOKDWJAK-UHFFFAOYSA-N dimethoxymethane Chemical compound COCOC NKDDWNXOKDWJAK-UHFFFAOYSA-N 0.000 claims description 4
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 claims description 4
- VUPKGFBOKBGHFZ-UHFFFAOYSA-N dipropyl carbonate Chemical compound CCCOC(=O)OCCC VUPKGFBOKBGHFZ-UHFFFAOYSA-N 0.000 claims description 4
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- 230000015572 biosynthetic process Effects 0.000 claims description 2
- JKJWYKGYGWOAHT-UHFFFAOYSA-N bis(prop-2-enyl) carbonate Chemical compound C=CCOC(=O)OCC=C JKJWYKGYGWOAHT-UHFFFAOYSA-N 0.000 claims description 2
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- 229910001496 lithium tetrafluoroborate Inorganic materials 0.000 claims description 2
- VDVLPSWVDYJFRW-UHFFFAOYSA-N lithium;bis(fluorosulfonyl)azanide Chemical compound [Li+].FS(=O)(=O)[N-]S(F)(=O)=O VDVLPSWVDYJFRW-UHFFFAOYSA-N 0.000 claims description 2
- MCVFFRWZNYZUIJ-UHFFFAOYSA-M lithium;trifluoromethanesulfonate Chemical compound [Li+].[O-]S(=O)(=O)C(F)(F)F MCVFFRWZNYZUIJ-UHFFFAOYSA-M 0.000 claims description 2
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- 150000004651 carbonic acid esters Chemical class 0.000 claims 1
- 125000000118 dimethyl group Chemical group [H]C([H])([H])* 0.000 claims 1
- 125000005678 ethenylene group Chemical group [H]C([*:1])=C([H])[*:2] 0.000 claims 1
- QSZMZKBZAYQGRS-UHFFFAOYSA-N lithium;bis(trifluoromethylsulfonyl)azanide Chemical compound [Li+].FC(F)(F)S(=O)(=O)[N-]S(=O)(=O)C(F)(F)F QSZMZKBZAYQGRS-UHFFFAOYSA-N 0.000 claims 1
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- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 abstract description 9
- 229910052744 lithium Inorganic materials 0.000 abstract description 9
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- 229910002097 Lithium manganese(III,IV) oxide Inorganic materials 0.000 description 1
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- UCVQOIPQDBZRMG-UHFFFAOYSA-N [C].COC(C=1C(C(=O)OC)=CC=CC1)=O Chemical group [C].COC(C=1C(C(=O)OC)=CC=CC1)=O UCVQOIPQDBZRMG-UHFFFAOYSA-N 0.000 description 1
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
- H01M10/0566—Liquid materials
- H01M10/0567—Liquid materials characterised by the additives
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- H—ELECTRICITY
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- H01M6/00—Primary cells; Manufacture thereof
- H01M6/14—Cells with non-aqueous electrolyte
- H01M6/16—Cells with non-aqueous electrolyte with organic electrolyte
- H01M6/162—Cells with non-aqueous electrolyte with organic electrolyte characterised by the electrolyte
- H01M6/168—Cells with non-aqueous electrolyte with organic electrolyte characterised by the electrolyte by additives
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0025—Organic electrolyte
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
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Abstract
本发明属于电化学和化学电源产品的技术领域，具体为一种电解液用阻燃添加剂及阻燃型锂离子电池电解液，具体为含有氟代嗪环类化合物作为阻燃添加剂。此电解液含有氟代嗪类化合物，具有很高效阻燃效能；这种电解液不仅对正负极具有良好的相容性，也对电池的性能影响很小，且大幅提高电池的燃烧安全性，具有更广的应用前景。上述的阻燃型电解质溶液可应用于锂一次电池、锂二次电池以及锂离子电池中。
Description
技术领域
本发明属于电化学和化学电源产品的技术领域，具体为一种电解液用阻燃添加剂及阻燃型锂离子电池电解液，具体为含有氟代嗪环类化合物作为阻燃添加剂。
背景技术
锂电池具有比能量高、自放电率低、绿色等显著优点,是目前最有希望的未来能源体系。然而，目前锂电池使用的电解液组分为易燃的酯或者醚的混合溶剂体系，虽然其电化学性能优良，但是极易燃烧甚至引起爆炸,造成人员和财产损失，因此，开发具有不燃或者耐燃的锂电池电解液具有非常重要的应用价值。
目前开发的主要阻燃剂为磷酸酯（美国专利US2005277027-A1）和氟代醚（中国专利200910249883.9）等，但是这些化合物具有阻燃性能低以及负极稳定性差等缺点。
发明内容
本发明的目的在于提供一种电解液用阻燃添加剂及阻燃型锂离子电池电解液，此电解液含有氟代嗪类化合物，具有很高效阻燃效能；这种电解液不仅对正负极具有良好的相容性，也对电池的性能影响很小，且大幅提高电池的燃烧安全性，具有更广的应用前景。
本发明采用的具体技术方案是：
一种电解液用阻燃添加剂，其特征在于，所述的阻燃添加剂为式Ⅰ的化合物，结构式如下所示：
一种阻燃型锂离子电池电解液，其特征在于：该电解液由四类成份组成：(A)锂盐，(B)碳酸酯类和/或醚类有机溶剂，(C)阻燃添加剂和(D)其他功能添加剂；
其中，(A)锂盐在此电解液中的摩尔浓度范围是：0.001-3摩尔/升；
(C)阻燃添加剂在此电解液中所占的质量比例范围是：0.1％-60％；
(D)其他功能添加剂在此电解液中的摩尔浓度范围是：0-2摩尔/升；
所述的(C)阻燃添加剂选自式Ⅰ的化合物，名称为三氟均三（TFT），结构式如下所示：
作为优选，其中，(A)锂盐在此电解液中的摩尔浓度范围是：0.5-1.5摩尔/升；
(C)阻燃添加剂在此电解液中所占的质量比例范围是：10％-35％；
(D)其他功能添加剂在此电解液中的摩尔浓度范围是：0.1-1摩尔/升。
作为优选，所述的(B)碳酸酯类和/或醚类有机溶剂，为两种或三种组分的组合，为两种组分时各个组分的用量比例为2:1-1:2；为三种组分时各个组分的用量比例为1:（1-2）:（1-2）。
其中，所述的(A)锂盐可以是具有如下分子式的化合物中的一种或几种的混合物：LiBF4，LiPF6，LiN(SO2CF3)2，LiFSI,LiBOB,LiSO3CF3。
所述的(B)碳酸酯类有机溶剂为环状碳酸酯类和/或链状碳酸酯类化合物。
所述的醚类有机溶剂选自四氢呋喃(THF)、2-甲基四氢呋喃(2-Methyl-THF)、1，3-二氧环戊烷(DOL)、二甲氧基甲烷(DMM)、1，2-二甲氧基乙烷(DME)和二甘醇二甲醚(dimethyl carbitol)中的一种或几种的混合物。
所述的环状碳酸酯类化合物优选自碳酸乙烯酯(EC)、碳酸丙烯酯(PC)、γ-丁内酯(GBL)和碳酸亚丁酯(BC)中的一种或几种的混合物；所述的链状碳酸酯类化合物优选自碳酸二甲酯(DMC)、碳酸二乙酯(DEC)、碳酸二丙酯(DPC)、碳酸甲基乙基酯(EMC)、以及碳数为3-8的直链或支链脂肪单醇与碳酸合成的碳酸酯衍生物中的一种或几种的混合物。
所述的(D)其他功能添加剂可以是下列化合物中的一种或几种的混合物：联苯(BP)，碳酸亚乙烯酯(VC)，碳酸乙烯亚乙酯(VEC)，氟代碳酸乙烯酯(FEC)，1、3-丙磺酸内酯(PS)，1、4-丁磺酸内酯(BS)，1、3-(1-丙烯)磺内酯(PST)，亚硫酸乙烯酯(ES)，硫酸乙烯酯(ESA)，环己基苯(CHB)，叔丁基苯(TBB)，叔戊基苯(TPB)和丁二氰(SN)。
本发明所述的阻燃型锂离子电池电解液应用于锂一次电池、锂二次电池以及锂离子电池中。
本发明的有益效果是：本专利采用了新型的阻燃剂组分-氟代嗪类，氟代嗪类化合物同时含有氮和氟两类阻燃元素，氮、氟元素都具有具有阻燃作用，并且氟的存在大大增加了这种溶剂对负极的稳定性以及电解液的粘度，氟代嗪类化合物的添加将可以大大提高电解液的安全性能。
经研究发现，三氟均三嗪具有很高效阻燃效能；氟的存在不但提高了阻燃性能而且提高了嗪类化合物对电极材料的相容性。这种电解液对电池的循环性能影响很小，且安全性大幅提高，具有广阔的应用前景。
附图说明
图1是使用含有17%TFT EC/DMC/EMC(1:1:1)的锰酸锂/石墨的商业化电池的循环性能以及与空白电池对比图。
具体实施方式
下面通过具体实施例对本发明作进一步的描述，但这些实施例不构成对本发明的任何限制。阻燃型
本发明以表格的形式例举了24种阻燃型电解液的成份组成、以及各电解液自熄时间的测试数据，详见下表1。
表1阻燃性电解液自熄时间的测试数据
实施例25
在含有1M LiPF6的体积比1:1:1的碳酸乙烯酯、碳酸二甲酯和碳酸二乙酯的电解液中加入17%TFT。该电解液可以达到完全不可燃。图1是使用该电解液的石墨/锰酸锂电池的1C倍率下的循环性能。从图中可以看出，使用这种这种电解液对电池的容量和循环性能影响不超过10%。
Claims (4)
1.一种阻燃型锂离子电池电解液，其特征在于：该电解液由四类成份组成：(A)锂盐，(B)碳酸酯类和/或醚类有机溶剂，(C)阻燃添加剂和(D)其他功能添加剂；
其中，(A)锂盐在此电解液中的摩尔浓度范围是：0.5-1.5摩尔/升；
(C)阻燃添加剂在此电解液中所占的质量比例范围是：10％-35％；
(D)其他功能添加剂在此电解液中的摩尔浓度范围是：0.1-1摩尔/升；
所述的(C)阻燃添加剂选自式Ⅰ的化合物，名称为三氟均三(TFT)，结构式如下所示：
所述的(A)锂盐是具有如下分子式的化合物中的一种或几种的混合物：LiBF4，LiPF6，LiN(SO2CF3)2，LiFSI,LiBOB,LiSO3CF3；
所述的(B)碳酸酯类有机溶剂为环状碳酸酯类和/或链状碳酸酯类化合物。
2.根据权利要求1所述的阻燃型锂离子电池电解液，其特征在于：
所述的醚类有机溶剂选自四氢呋喃(THF)、2-甲基四氢呋喃(2-Methyl-THF)、1，3-二氧环戊烷(DOL)、二甲氧基甲烷(DMM)、1，2-二甲氧基乙烷(DME)和二甘醇二甲醚(dimethylcarbitol)中的一种或几种的混合物。
3.根据权利要求1所述的阻燃型锂离子电池电解液，其特征在于：
所述的环状碳酸酯类化合物选自碳酸乙烯酯(EC)、碳酸丙烯酯(PC)、γ-丁内酯(GBL)和碳酸亚丁酯(BC)中的一种或几种的混合物；所述的链状碳酸酯类化合物选自碳酸二甲酯(DMC)、碳酸二乙酯(DEC)、碳酸二丙酯(DPC)、碳酸甲基乙基酯(EMC)、以及碳数为3-8的直链或支链脂肪单醇与碳酸合成的碳酸酯衍生物中的一种或几种的混合物。
4.根据权利要求1所述的阻燃型锂离子电池电解液，其特征在于：
所述的(D)其他功能添加剂可以是下列化合物中的一种或几种的混合物：联苯(BP)，碳酸亚乙烯酯(VC)，碳酸乙烯亚乙酯(VEC)，氟代碳酸乙烯酯(FEC)，1、3-丙磺酸内酯(PS)，1、4-丁磺酸内酯(BS)，1、3-(1-丙烯)磺内酯(PST)，亚硫酸乙烯酯(ES)，硫酸乙烯酯(ESA)，环己基苯(CHB)，叔丁基苯(TBB)，叔戊基苯(TPB)和丁二氰(SN)。
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