CN113793984A - 一种双离子电池用电解液及其制备方法 - Google Patents
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- 159000000002 lithium salts Chemical class 0.000 claims abstract description 13
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- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims description 11
- 229910052744 lithium Inorganic materials 0.000 claims description 11
- PFKFTWBEEFSNDU-UHFFFAOYSA-N carbonyldiimidazole Chemical class C1=CN=CN1C(=O)N1C=CN=C1 PFKFTWBEEFSNDU-UHFFFAOYSA-N 0.000 claims description 9
- MBABOKRGFJTBAE-UHFFFAOYSA-N methyl methanesulfonate Chemical compound COS(C)(=O)=O MBABOKRGFJTBAE-UHFFFAOYSA-N 0.000 claims description 8
- 238000003756 stirring Methods 0.000 claims description 8
- UHOPWFKONJYLCF-UHFFFAOYSA-N 2-(2-sulfanylethyl)isoindole-1,3-dione Chemical compound C1=CC=C2C(=O)N(CCS)C(=O)C2=C1 UHOPWFKONJYLCF-UHFFFAOYSA-N 0.000 claims description 2
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- MHCFAGZWMAWTNR-UHFFFAOYSA-M lithium perchlorate Chemical compound [Li+].[O-]Cl(=O)(=O)=O MHCFAGZWMAWTNR-UHFFFAOYSA-M 0.000 claims description 2
- 229910001486 lithium perchlorate Inorganic materials 0.000 claims description 2
- 229910001496 lithium tetrafluoroborate Inorganic materials 0.000 claims description 2
- IGILRSKEFZLPKG-UHFFFAOYSA-M lithium;difluorophosphinate Chemical compound [Li+].[O-]P(F)(F)=O IGILRSKEFZLPKG-UHFFFAOYSA-M 0.000 claims description 2
- 239000007773 negative electrode material Substances 0.000 claims description 2
- 229920001343 polytetrafluoroethylene Polymers 0.000 claims description 2
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- 125000001424 substituent group Chemical group 0.000 claims description 2
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- SYRDSFGUUQPYOB-UHFFFAOYSA-N [Li+].[Li+].[Li+].[O-]B([O-])[O-].FC(=O)C(F)=O Chemical compound [Li+].[Li+].[Li+].[O-]B([O-])[O-].FC(=O)C(F)=O SYRDSFGUUQPYOB-UHFFFAOYSA-N 0.000 claims 1
- 238000007599 discharging Methods 0.000 abstract description 4
- PQXKHYXIUOZZFA-UHFFFAOYSA-M lithium fluoride Chemical compound [Li+].[F-] PQXKHYXIUOZZFA-UHFFFAOYSA-M 0.000 abstract description 4
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- 125000001495 ethyl group Chemical group [H]C([H])([H])C([H])([H])* 0.000 description 2
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- 238000012360 testing method Methods 0.000 description 2
- DKQPXAWBVGCNHG-UHFFFAOYSA-N 2,2,4,4,6,6-hexafluoro-1,3,5-triaza-2$l^{5},4$l^{5},6$l^{5}-triphosphacyclohexa-1,3,5-triene Chemical compound FP1(F)=NP(F)(F)=NP(F)(F)=N1 DKQPXAWBVGCNHG-UHFFFAOYSA-N 0.000 description 1
- BTBUEUYNUDRHOZ-UHFFFAOYSA-N Borate Chemical compound [O-]B([O-])[O-] BTBUEUYNUDRHOZ-UHFFFAOYSA-N 0.000 description 1
- 229910019142 PO4 Inorganic materials 0.000 description 1
- 125000002915 carbonyl group Chemical group [*:2]C([*:1])=O 0.000 description 1
- HRYZWHHZPQKTII-UHFFFAOYSA-N chloroethane Chemical compound CCCl HRYZWHHZPQKTII-UHFFFAOYSA-N 0.000 description 1
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Classifications
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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
- H01M10/0561—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of inorganic materials only
- H01M10/0563—Liquid materials, e.g. for Li-SOCl2 cells
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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
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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- H—ELECTRICITY
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- 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
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- 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
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- 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
- H01M10/0569—Liquid materials characterised by the solvents
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Abstract
本发明公开了一种双离子电池用电解液及其制备方法，包括锂盐、氟盐、溶剂与添加剂；所述溶剂为直链或支链羧酸酯；所述氟盐包括六氟环三磷腈。由于上述组分之间的协同作用，降低了电解液的粘度，而较低的电解液粘度，又能够加快放电过程中氟盐中的氟离子与锂盐中的锂离子形成氟化锂，从而形成双离子电池，并提升电池的循环性能。
Description
技术领域
本发明属于电解液技术领域，具体涉及一种双离子电池用电解液及其制备方法。
背景技术
锂离子电池是一种充电电池，它主要依靠锂离子在正极和负极之间移动来工作。在充放电过程中，Li+在两个电极之间往返嵌入和脱嵌：充电时，Li+从正极脱出，经过电解质嵌入负极，负极处于富锂状态；放电时则相反。锂离子电池具有高比能量、高充放电效率和长寿命等优点，是目前最具有应用前景的化学电源之一。
但是，上述锂离子电池中的电解液，存在价格昂贵、粘度较大、电池倍率特性较差等缺点，而利用溶性液体如氟化醚类与TFSI的共同作用降低粘度的方法，热稳定性差且易胀气，也无法有效解决电解液粘度大而影响电池性能的问题。
发明内容
本发明所要解决的第一个技术问题是：
提供一种双离子电池用电解液。
本发明所要解决的第二个技术问题是：
提供一种上述双离子电池用电解液的制备方法。
本发明所要解决的第三个技术问题是：
上述双离子电池用电解液的应用。
为了解决上述第一个技术问题，本发明采用的技术方案为：
一种双离子电池用电解液，
包括锂盐、氟盐、溶剂与添加剂；
所述溶剂为直链或支链羧酸酯；
所述氟盐包括六氟环三磷腈；
所述双离子电池用电解液粘度为0.8-1.50mpa·s。
根据本发明的一种实施方式，上述锂盐浓度为0.05-0.10mol/L。
根据本发明的一种实施方式，上述锂盐包括六氟磷酸锂、二氟磷酸锂、二氟草酸磷酸锂和四氟硼酸锂、二氟草酸硼酸锂、双三氟甲磺酰基酰亚胺锂、双三氟甲基亚胺锂、双氟磺酰亚胺锂、高氯酸锂中的至少一种。
根据本发明的一种实施方式，上述添加剂包括改性N,N'-羰基二咪唑。
上述改性N,N'-羰基二咪唑的制备方法为：
混合N’N-羰基二咪唑缓与氯乙烷，搅拌，得到乙基接枝N’N-羰基二咪唑的氯盐；
将上述乙基接枝N’N-羰基二咪唑的氯盐与二氰氨钠和丙酮共混，搅拌，加入乙醇胺，通过羰基与羟基发生亲核加成反应，得到上述改性N,N'-羰基二咪唑。
根据本发明的一种实施方式，上述直链或支链羧酸酯含有以下结构式：
其中，R1、R2各自独立选自取代或未取代的C1-7烷基，取代基选自卤素；
根据本发明的一种实施方式，上述锂盐、氟盐、溶剂与添加剂的质量份比为2.3-4.6：1.5-2.5：50-78：0.7-1.5。
根据本发明的一种实施方式，上述添加剂还包括聚四氟乙烯、乙炔黑和丙酸丙酯中的至少一种。
据本发明的一种实施方式，上述添加剂还包括磺酸二甲酯。
磺酸二甲酯能够抑制直链或支链羧酸酯在高电压下在正极持续发生氧化反应，以弥补直链或支链羧酸酯的缺点，使得本发明电解液循环性能得到了提高。
为了解决上述第二个技术问题，本发明采用的技术方案为：
一种制备上述双离子电池用电解液方法，包括以下步骤：
将锂盐、氟盐与添加剂分散在溶剂中，搅拌得到所述双离子电池用电解液。
本发明的再一个方面，还提供一种锂离子电池，包括含有正极活性材料的正极片、含有负极活性材料的负极片、锂电池隔膜和上述的双离子电池用电解液。
上述技术方案中的一个技术方案至少具有如下优点或有益效果之一：
1.上述改性N,N'-羰基二咪唑和六氟环三磷腈降低了上述双离子电池用电解液的粘度，提高了电解液的离子电导率；
2.上述直链或支链羧酸酯作为低凝固点、低粘度、高介电常数的溶剂，有助于降低上述双离子电池用电解液的粘度以及提高锂离子电池大倍率充电性能；
3.上述磺酸二甲酯能够抑制直链或支链羧酸酯在高电压下在正极持续发生氧化反应；
4.由于上述组分之间的协同作用，降低了电解液的粘度，而较低的电解液粘度，又能够加快放电过程中氟盐中的氟离子与锂盐中的锂离子形成氟化锂，从而形成双离子电池。此外，低粘度的电解液在放电过程中的副反应也会大幅度减少，从而提升电池的循环性能。
具体实施方式
为详细说明本发明的技术内容、所实现目的及效果，以下结合实施方式予以说明。
实施例1
将2.3g六氟磷酸锂、1.5g六氟环三磷腈与0.6g改性N,N'-羰基二咪唑、0.1g磺酸二甲酯分散在50mL的CH3CH2CH2COOCHF溶剂中，搅拌得到所述双离子电池用电解液，上述双离子电池用电解液粘度为0.8-1.50mpa·s。
实施例2
将4.6g六氟磷酸锂、2.5g六氟环三磷腈与1.0g改性N,N'-羰基二咪唑、0.5g磺酸二甲酯分散在50mL的CH3CH2CH2COOCHF溶剂中，搅拌得到所述双离子电池用电解液。
对比例1
将2.3g六氟磷酸锂、1.5g六氟环三磷腈与0.6g改性N,N'-羰基二咪唑、0.1g磺酸二甲酯分散在50mL的水中，搅拌得到所述双离子电池用电解液。
对比例2
将2.3g六氟磷酸锂、0.6g改性N,N'-羰基二咪唑、0.1g磺酸二甲酯分散在50mL的CH3CH2CH2COOCHF溶剂中，搅拌得到所述双离子电池用电解液。
对比例3
将2.3g六氟磷酸锂、1.5g六氟环三磷腈分散在50mL的CH3CH2CH2COOCHF溶剂中，搅拌得到所述双离子电池用电解液。
性能测试：
一种Li2MnSiO4电池包括正极、负极、PE隔膜，以及按照本发明制备的电解液。
将实验例1-2与对比例1-3分别进行放电比容量和粘度的测试，测试结果如下：
用基于Poiseuille定律的乌氏毛细管黏度测试电解液的粘度：依据Poiseuille定律，液体流经毛细管黏度计的黏度为η＝A·ρ·t-(B·ρ)/t，其中，A、B为黏度计的仪器常数，ρ为液体密度，t为液体流经黏度计上两刻度线的时间。
表1
| 粘度(mPa·s) | 放电比容量(mAh/g) | |
| 实施例1 | 0.8 | 768.3 |
| 实施例2 | 1.5 | 718.2 |
| 对比例1 | 2.6 | 694.1 |
| 对比例2 | 4.8 | 618.2 |
| 对比例3 | 2.5 | 688.4 |
以上仅为本发明的实施例，并非因此限制本发明的专利范围，凡是利用本发明说明书内容所作的等同变换，或直接或间接运用在相关的技术领域，均同理包括在本发明的专利保护范围内。
Claims (10)
1.一种双离子电池用电解液，其特征在于：
包括锂盐、氟盐、溶剂与添加剂；
所述溶剂为直链或支链羧酸酯；
所述氟盐包括六氟环三磷腈；
所述双离子电池用电解液粘度为0.8-1.50mpa·s。
2.根据权利要求1所述的一种双离子电池用电解液，其特征在于：
所述锂盐浓度为0.05-0.10mol/L。
3.根据权利要求1所述的一种双离子电池用电解液，其特征在于：
所述锂盐包括六氟磷酸锂、二氟磷酸锂、二氟草酸磷酸锂和四氟硼酸锂、二氟草酸硼酸锂、双三氟甲磺酰基酰亚胺锂、双三氟甲基亚胺锂、双氟磺酰亚胺锂、高氯酸锂中的至少一种。
4.根据权利要求1所述的一种双离子电池用电解液，其特征在于：
所述添加剂包括改性N,N'-羰基二咪唑。
5.根据权利要求1所述的一种双离子电池用电解液，其特征在于：
所述直链或支链羧酸酯含有以下结构式：
其中，R1、R2各自独立选自取代或未取代的C1-7烷基，取代基选自卤素；
6.根据权利要求1所述的一种双离子电池用电解液，其特征在于：
所述锂盐、氟盐、溶剂与添加剂的质量份比为2.3-4.6：1.5-2.5：50-78：0.7-1.5。
7.根据权利要求1所述的一种双离子电池用电解液，其特征在于：
所述添加剂还包括聚四氟乙烯、乙炔黑和丙酸丙酯中的至少一种。
8.根据权利要求1所述的一种双离子电池用电解液，其特征在于：
所述添加剂还包括磺酸二甲酯。
9.一种制备如权利要求1至7任一项所述的一种双离子电池用电解液的方法，其特征在于：包括以下步骤：
将锂盐、氟盐与添加剂分散在溶剂中，搅拌得到所述双离子电池用电解液。
10.一种锂离子电池，其特征在于，包括含有正极活性材料的正极片、含有负极活性材料的负极片、锂电池隔膜和权利要求1-7中任一项所述的双离子电池用电解液。
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