CN101911370A - 袋状锂二次电池 - Google Patents
袋状锂二次电池 Download PDFInfo
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- CN101911370A CN101911370A CN2008801235257A CN200880123525A CN101911370A CN 101911370 A CN101911370 A CN 101911370A CN 2008801235257 A CN2008801235257 A CN 2008801235257A CN 200880123525 A CN200880123525 A CN 200880123525A CN 101911370 A CN101911370 A CN 101911370A
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- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 title claims abstract description 74
- 229910052744 lithium Inorganic materials 0.000 title claims abstract description 72
- -1 cyclic carbonate compound Chemical class 0.000 claims abstract description 29
- 239000011255 nonaqueous electrolyte Substances 0.000 claims abstract description 29
- 150000001875 compounds Chemical class 0.000 claims abstract description 27
- 239000000203 mixture Substances 0.000 claims abstract description 22
- 229910003002 lithium salt Inorganic materials 0.000 claims abstract description 10
- 159000000002 lithium salts Chemical class 0.000 claims abstract description 10
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 claims abstract description 9
- 229910001416 lithium ion Inorganic materials 0.000 claims abstract description 9
- JGFBQFKZKSSODQ-UHFFFAOYSA-N Isothiocyanatocyclopropane Chemical compound S=C=NC1CC1 JGFBQFKZKSSODQ-UHFFFAOYSA-N 0.000 claims abstract description 6
- PWLNAUNEAKQYLH-UHFFFAOYSA-N butyric acid octyl ester Natural products CCCCCCCCOC(=O)CCC PWLNAUNEAKQYLH-UHFFFAOYSA-N 0.000 claims abstract description 6
- YKYONYBAUNKHLG-UHFFFAOYSA-N n-Propyl acetate Natural products CCCOC(C)=O YKYONYBAUNKHLG-UHFFFAOYSA-N 0.000 claims abstract description 6
- UUIQMZJEGPQKFD-UHFFFAOYSA-N n-butyric acid methyl ester Natural products CCCC(=O)OC UUIQMZJEGPQKFD-UHFFFAOYSA-N 0.000 claims abstract description 6
- 229940090181 propyl acetate Drugs 0.000 claims abstract description 6
- NQPDZGIKBAWPEJ-UHFFFAOYSA-N valeric acid Chemical compound CCCCC(O)=O NQPDZGIKBAWPEJ-UHFFFAOYSA-N 0.000 claims abstract description 6
- 238000007599 discharging Methods 0.000 claims abstract description 5
- FKRCODPIKNYEAC-UHFFFAOYSA-N ethyl propionate Chemical compound CCOC(=O)CC FKRCODPIKNYEAC-UHFFFAOYSA-N 0.000 claims description 56
- 239000000463 material Substances 0.000 claims description 25
- XBDQKXXYIPTUBI-UHFFFAOYSA-N dimethylselenoniopropionate Natural products CCC(O)=O XBDQKXXYIPTUBI-UHFFFAOYSA-N 0.000 claims description 24
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical group O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 claims description 23
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- 229910052799 carbon Inorganic materials 0.000 claims description 15
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- 235000019260 propionic acid Nutrition 0.000 claims description 12
- 229910052731 fluorine Inorganic materials 0.000 claims description 9
- 239000011737 fluorine Substances 0.000 claims description 9
- 229910013870 LiPF 6 Inorganic materials 0.000 claims description 8
- 230000004888 barrier function Effects 0.000 claims description 7
- 229910015645 LiMn Inorganic materials 0.000 claims description 6
- 239000000126 substance Substances 0.000 claims description 6
- SBLRHMKNNHXPHG-UHFFFAOYSA-N 4-fluoro-1,3-dioxolan-2-one Chemical compound FC1COC(=O)O1 SBLRHMKNNHXPHG-UHFFFAOYSA-N 0.000 claims description 5
- 229910013716 LiNi Inorganic materials 0.000 claims description 4
- 238000009413 insulation Methods 0.000 claims description 4
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 claims description 4
- ZZXUZKXVROWEIF-UHFFFAOYSA-N 1,2-butylene carbonate Chemical compound CCC1COC(=O)O1 ZZXUZKXVROWEIF-UHFFFAOYSA-N 0.000 claims description 3
- RJUFJBKOKNCXHH-UHFFFAOYSA-N Methyl propionate Chemical compound CCC(=O)OC RJUFJBKOKNCXHH-UHFFFAOYSA-N 0.000 claims description 3
- 229940017219 methyl propionate Drugs 0.000 claims description 3
- IUVKMZGDUIUOCP-BTNSXGMBSA-N quinbolone Chemical compound O([C@H]1CC[C@H]2[C@H]3[C@@H]([C@]4(C=CC(=O)C=C4CC3)C)CC[C@@]21C)C1=CCCC1 IUVKMZGDUIUOCP-BTNSXGMBSA-N 0.000 claims description 3
- 229910000314 transition metal oxide Inorganic materials 0.000 claims description 3
- DTQVDTLACAAQTR-UHFFFAOYSA-N trifluoroacetic acid Substances OC(=O)C(F)(F)F DTQVDTLACAAQTR-UHFFFAOYSA-N 0.000 claims description 3
- HFZLSTDPRQSZCQ-UHFFFAOYSA-N 1-pyrrolidin-3-ylpyrrolidine Chemical compound C1CCCN1C1CNCC1 HFZLSTDPRQSZCQ-UHFFFAOYSA-N 0.000 claims description 2
- 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
- 229910015015 LiAsF 6 Inorganic materials 0.000 claims description 2
- 229910013063 LiBF 4 Inorganic materials 0.000 claims description 2
- 229910013684 LiClO 4 Inorganic materials 0.000 claims description 2
- 229910013733 LiCo Inorganic materials 0.000 claims description 2
- 229910012851 LiCoO 2 Inorganic materials 0.000 claims description 2
- 229910011281 LiCoPO 4 Inorganic materials 0.000 claims description 2
- 229910010707 LiFePO 4 Inorganic materials 0.000 claims description 2
- 229910014689 LiMnO Inorganic materials 0.000 claims description 2
- 229910013290 LiNiO 2 Inorganic materials 0.000 claims description 2
- 229910012513 LiSbF 6 Inorganic materials 0.000 claims description 2
- 229910052736 halogen Inorganic materials 0.000 claims description 2
- 150000002367 halogens Chemical class 0.000 claims description 2
- ACFSQHQYDZIPRL-UHFFFAOYSA-N lithium;bis(1,1,2,2,2-pentafluoroethylsulfonyl)azanide Chemical compound [Li+].FC(F)(F)C(F)(F)S(=O)(=O)[N-]S(=O)(=O)C(F)(F)C(F)(F)F ACFSQHQYDZIPRL-UHFFFAOYSA-N 0.000 claims description 2
- 230000037431 insertion Effects 0.000 claims 1
- 238000003780 insertion Methods 0.000 claims 1
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 abstract description 3
- 229910001290 LiPF6 Inorganic materials 0.000 abstract 1
- XBDQKXXYIPTUBI-UHFFFAOYSA-M Propionate Chemical compound CCC([O-])=O XBDQKXXYIPTUBI-UHFFFAOYSA-M 0.000 abstract 1
- 239000003575 carbonaceous material Substances 0.000 abstract 1
- 238000004090 dissolution Methods 0.000 abstract 1
- 238000010292 electrical insulation Methods 0.000 abstract 1
- 150000002500 ions Chemical class 0.000 abstract 1
- 230000008961 swelling Effects 0.000 abstract 1
- 239000003960 organic solvent Substances 0.000 description 14
- 230000000052 comparative effect Effects 0.000 description 12
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 description 10
- 238000002360 preparation method Methods 0.000 description 6
- 239000003792 electrolyte Substances 0.000 description 5
- 239000011149 active material Substances 0.000 description 4
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 4
- 230000008859 change Effects 0.000 description 4
- 229920001577 copolymer Polymers 0.000 description 4
- 238000003860 storage Methods 0.000 description 4
- WEVYAHXRMPXWCK-UHFFFAOYSA-N Acetonitrile Chemical compound CC#N WEVYAHXRMPXWCK-UHFFFAOYSA-N 0.000 description 3
- VGGSQFUCUMXWEO-UHFFFAOYSA-N Ethene Chemical compound C=C VGGSQFUCUMXWEO-UHFFFAOYSA-N 0.000 description 3
- 239000005977 Ethylene Substances 0.000 description 3
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- 229920003048 styrene butadiene rubber Polymers 0.000 description 3
- RTZKZFJDLAIYFH-UHFFFAOYSA-N Diethyl ether Chemical compound CCOCC RTZKZFJDLAIYFH-UHFFFAOYSA-N 0.000 description 2
- 239000004743 Polypropylene Substances 0.000 description 2
- 239000002174 Styrene-butadiene Substances 0.000 description 2
- 239000011230 binding agent Substances 0.000 description 2
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 description 2
- 239000011302 mesophase pitch Substances 0.000 description 2
- 229910052751 metal Inorganic materials 0.000 description 2
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- 238000011160 research Methods 0.000 description 2
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- SHJWFIDAWODQSR-UHFFFAOYSA-N 3,3-difluoropropanoic acid Chemical compound OC(=O)CC(F)F SHJWFIDAWODQSR-UHFFFAOYSA-N 0.000 description 1
- 229920000049 Carbon (fiber) Polymers 0.000 description 1
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 description 1
- 229910012820 LiCoO Inorganic materials 0.000 description 1
- 229910013872 LiPF Inorganic materials 0.000 description 1
- 101150058243 Lipf gene Proteins 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
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
-
- 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
- H01M10/0568—Liquid materials characterised by the solutes
-
- 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
- H01M10/0569—Liquid materials characterised by the solvents
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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
- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/10—Primary casings; Jackets or wrappings
- H01M50/102—Primary casings; Jackets or wrappings characterised by their shape or physical structure
- H01M50/105—Pouches or flexible bags
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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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- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
- H01M4/583—Carbonaceous material, e.g. graphite-intercalation compounds or CFx
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Abstract
一种袋状锂二次电池,包括一个这样的电极组,该电极组具有由能够吸藏或释放锂离子的碳材料制成的阳极、由含锂的氧化物制成的阴极,以及插入所述阴极和所述阳极之间的用于使其间电绝缘的隔膜;一个由薄片制成的袋状壳体,用于提供容纳电极组的空间;以及一种注入所述电极组中的非水电解质。所述非水电解质为一种基于非线性碳酸酯的非水电解质,含有一种锂盐、(a)一种环状碳酸酯化合物和(b)一种选自基于丙酸酯的化合物、丁酸甲酯和乙酸丙酯或其混合物的线性酯类化合物。溶解1M LiPF6时,所述非水电解质在约23℃时的离子电导率为9mS/cm或更高。该袋状锂二次电池确保了良好的高速放电性能,并解决了袋状锂二次电池的膨胀问题。
Description
技术领域
本发明涉及一种具有由薄片形成的袋状壳体的袋状锂二次电池。
背景技术
近来,人们对能量储存技术的关注不断增加。随着能量储存技术延及至手机、可携式摄像机和笔记本电脑,并进一步延及电动车,对用作这些电子设备能源的高能量密度电池的需求增加。锂离子二次电池是最令人满意的电池之一,大量针对改进进行的研究目前也在活跃进行中。
锂二次电池可制成多种形状。代表性的实例包括角状锂二次电池、柱状锂二次电池和袋状锂二次电池。
如图1所示,袋状锂二次电池10通常包括一个电极组11和一个限定用于容纳电池组11的空间的壳体12。所述电极组11包括由能够吸藏或释放锂离子的碳材料制成的阳极、由含锂的氧化物制成的阴极,以及插入所述阴极和所述阳极之间以使它们电绝缘的隔膜。阴极和阳极接头分别从所述电极组11的阴极和阳极的一个边缘引出,形成接头单元13,其彼此电连接并集中在每个电极板上。接头单元13各自与电极端子焊接,电极端子可与外部端子相连。
袋状锂二次电池10包括由薄片制成的袋状壳体12,所述薄片通过将聚合物膜层压至由例如铝制成的金属薄片上而形成。所述壳体12具有其中可放置电极组11的空间,并且通常上部壳体与下部壳体可拆卸地彼此连接。在如上所形成的袋状锂二次电池10中,电极组11被安装在具有一个空间的袋状壳体11中,然后电解质被注入所述空间内。然后,在袋状壳体12周围加热并加压,以牢固地密封所述袋状壳体12,由此制成袋状锂二次电池10。
如上所述,袋状锂二次电池采用一种由薄片制成的袋状壳体,从而可通过简单的制造方法制作出具有多种形状的轻质的锂二次电池。但是,由于使用袋状壳体,其中的锂二次电池与柱状或角状电池相比更易于因内部压力的增加而膨胀。伴随着膨胀,电池的厚度增加,引起电子设备如手机或笔记本电脑中的问题,并且还对电池的稳定性和性能产生严重的影响。
电池的这种膨胀在注入含有碳酸二甲酯的非水电解质的锂二次电池中更为严重。
例如,日本专利No.3,032,338公开了一种含有三元有机溶剂体系的非水电解质二次电池,所述三元有机溶剂体系由碳酸亚乙酯、碳酸二甲酯和丙酸甲酯组成。具有碳酸二甲酯作为线性碳酸酯的非水电解质具有良好的高速放电特性。但是,由于碳酸二甲酯具有低沸点,如果电池过热或处于高温中时会显著膨胀。如果碳酸甲乙酯或碳酸二甲酯作为线性碳酸酯被加入或者仅有少量的碳酸二甲酯被加入,电池的膨胀问题会得以改进,但高速放电特性劣化。
发明内容
【技术问题】
本发明旨在解决现有技术中的问题,因此本发明的一个目的是提供一种袋状锂二次电池,其具有良好的高速放电性能,并解决了电池的膨胀问题,由此克服了袋状电池的弱点。
【技术方案】
为实现上述目的,本发明提供一种袋状锂二次电池,其包括一个这样的电极组,该电极组具有由能够吸藏或释放锂离子的碳材料制成的阳极、由含锂的氧化物制成的阴极、以及插入所述阴极和所述阳极之间的用于使其间电绝缘的隔膜;一个由薄片制成的袋状壳体,用于提供容纳电极组的空间;以及一种注入电极组中的非水电解质,其中所述非水电解质为一种基于非线性碳酸酯的非水电解质,含有一种锂盐、(a)一种环状碳酸酯化合物和(b)一种选自基于丙酸酯的化合物、丁酸甲酯和乙酸丙酯或其混合物的线性酯类化合物,并且其中溶解1M LiPF6时,所述非水电解质在约23℃时的离子电导率为9mS/cm或更高。
在本发明的袋状锂二次电池中,(a)组分——即环状碳酸酯化合物——和(b)组分——即线性酯类化合物——的体积比(a∶b)优选为约2∶8至约4∶6。
在本发明的袋状锂二次电池中,环状碳酸酯化合物可为选自碳酸亚乙酯、碳酸亚丙酯、氟代碳酸亚乙酯和碳酸亚丁酯的任意一种物质或至少两种物质的混合物。另外,基于丙酸乙酯的化合物为选自丙酸乙酯、3-氟丙酸乙酯、3,3-二氟丙酸乙酯、3,3,3-三氟丙酸乙酯、丙酸2-氟乙酯、丙酸2,2-二氟乙酯、丙酸2,2,2-三氟乙酯、3-氟丙酸2,2,2-三氟乙酯、3,3-二氟丙酸2,2,2-三氟乙酯,和3,3,3-三氟丙酸2,2,2-三氟乙酯的任意一种物质或至少两种物质的混合物。
附图说明
图1是示意性示出一般袋状锂二次电池的截面图;
图2是示出将1M LiPF6溶解于碳酸亚乙酯与其它有机溶剂(x)的混合有机溶剂中获得的非水电解质的离子电导率的图,所述电导率根据混合有机溶剂的组成比(%)在23℃测定。
具体实施方式
下文将参照附图详细描述本发明的优选实施方案。在描述之前,应理解,说明书和所附权利要求书中使用的术语不应被理解为被限制在一般含义和词典中的含义,而应在允许发明人为进行最佳解释而对术语作适当定义的原则基础上,基于与本发明技术方案相应的含义和概念来解释。
如上所述,本发明的袋状锂二次电池实质上采用了一种具有高离子电导率的预定混合有机溶剂,而不是使用线性碳酸酯化合物。也即,注入本发明的袋状锂二次电池中的非水电解质是一种基于非线性碳酸酯的非水电解质,其含有一种锂盐、(a)一种环状碳酸酯化合物和(b)一种诸如基于丙酸酯的化合物、丁酸甲酯和乙酸丙酯及其混合物的线性酯类化合物。在溶解1M LiPF6时,所述非水电解质在约23℃时的离子电导率为9mS/cm或更高。
环状碳酸酯化合物易于使电解质中的锂盐解离,这有利于提高电池的充电/放电容量。环状碳酸酯化合物可为选自碳酸亚乙酯、碳酸亚丙酯、氟代碳酸亚乙酯和碳酸亚丁酯的任意一种物质或至少两种物质的混合物。特别地,碳酸亚乙酯(或氟代碳酸亚乙酯)或者碳酸亚乙酯(或氟代碳酸亚乙酯)与碳酸亚丙酯的混合物具有高介电常数,从而更易于使电解质中的锂盐解离。
用于本发明中的基于丙酸酯的化合物可为由以下化学式1表示的基于丙酸酯的酯类化合物:
化学式1
其中R1和R2独立地为一种线性或支化的C1-6烷基,且R1和R2各自可为未取代的或可被至少一个卤素取代。
由化学式1表示的基于丙酸酯的酯类化合物的非限制性实例包括选自基于丙酸甲酯的化合物、基于丙酸乙酯的化合物、基于丙酸丙酯的化合物和基于丙酸丁酯的化合物中的至少一种化合物。基于丙酸乙酯的酯类化合物是优选的。
基于丙酸乙酯的化合物、丁酸甲酯和乙酸丙酯是具有低凝固点和较高沸点、并具有出色低温特性的线性酯类化合物。此外,它们对碳材料阳极具有较低的反应性。特别是,这种线性酯类化合物与上述环状碳酸酯化合物混合有利于提高锂二次电池的高速放电特性。也即,所述线性酯类化合物在常温和低温时通过适当调节锂离子而具有高离子电导率,从而改进电池的高速放电特性。此外,所述线性酯类化合物对电池充电过程中阴极上电解质的分解反应具有高的抗性,从而抑制电池的膨胀,并改进电池的循环寿命。另外,与单独使用酯类碳酸酯溶剂作为非水电解质的情形不同,由于提高了对电极的可润湿性,锂树突状物在电极表面的形成受到抑制,从而提高电池的安全性。线性酯类化合物可单独使用或结合使用。基于丙酸乙酯的化合物可采用丙酸乙酯、3-氟丙酸乙酯、3,3-二氟丙酸乙酯、3,3,3-三氟丙酸乙酯、丙酸2-氟乙酯、丙酸2,2-二氟乙酯、丙酸2,2,2-三氟乙酯、3-氟丙酸2,2,2-三氟乙酯、3,3-二氟丙酸2,2,2-三氟乙酯,和3,3,3-三氟丙酸2,2,2-三氟乙酯,它们可单独使用或结合使用。
如上所述,本发明的非水电解质在溶解1M LiPF6时在约23℃的离子电导率为9mS/cm或更高。也即,如图2所示,在含有(a)一种环状碳酸酯化合物和(b)一种特定的线性酯类化合物的非水电解质中,控制它们的比例以使溶解1M LiPF6时在23℃的离子电导率为9mS/cm或更高,以提高高速放电特性。当所述非水电解质的离子电导率超过9mS/cm时,应理解,离子电导率基本上与含有碳酸二甲酯的混合有机溶剂处于相同水平,这与其它种类的线性碳酸酯不同。在这个方面,(a)组分——即环状碳酸酯化合物——与(b)组分——即线性酯类化合物——的体积比(a∶b)优选为2∶8至4∶6。
本发明的锂二次电池的非水电解质采用一种环状碳酸酯化合物作为碳酸酯化合物,以及一种非线性酯类化合物,即一种基于非线性碳酸酯的有机溶剂。因此,未加入线性碳酸酯化合物来提高锂二次电池的充电/放电效率,但在不偏离本发明目的的前提下可含有少量的线性碳酸酯化合物。
在本发明的锂二次电池的非水电解质中,其中所含的作为电解质的锂盐可采用任意一种常用于锂二次电池的电解质中的锂盐。锂盐的非限制性的典型实例还可包括LiPF6、LiBF4、LiSbF6、LiAsF6、LiClO4、LiN(C2F5SO2)2、LiN(CF3SO2)2、CF3SO3Li和LiC(CF3SO2)3。此外,在不偏离本发明目的的前提下,可向锂二次电池的非水电解质中添加其它化合物,如内酯、醚、酯、乙腈、内酰胺和酮。
本发明的袋状锂二次电池具有如图1所示的结构。也即,本发明的袋状锂二次电池包括一个电极组,其具有由能够吸藏或释放锂离子的碳材料制成的阳极、由含锂的氧化物制成的阴极、以及插入所述阴极和所述阳极之间的用于使它们之间电绝缘的隔膜;一个由薄片制成的袋状壳体,电极组被放置于其中;以及一种注入电极组中的非水电解质。注入电极组中的非水电解质已在上文中描述。
由能够吸藏或释放锂离子的碳材料制成的阳极和由含锂的氧化物制成的阴极可采用任何通常用于制造锂二次电池的材料。
例如,能够吸藏或释放锂离子的碳材料可为低晶态碳或高晶态碳。低晶态碳包括软质碳或硬质碳,高晶态碳包括天然石墨、漂浮石墨、热解碳、中间相沥青基碳纤维、中间相碳微球、中间相沥青和高温烧结碳,如来源于石油或煤焦油沥青的焦炭,但不限于此。阳极可具有一种粘合剂,其可使用多种粘合剂聚合物,如PVDF-共-HFP HFP(聚偏氟乙烯-共-六氟丙烯)、聚偏氟乙烯、聚丙烯腈、聚甲基丙烯酸甲酯、SBR(苯乙烯-丁二烯橡胶)共聚物,以及改性的SBR共聚物。
此外,由含锂的氧化物制备的阴极活性材料优选地采用一种含锂的过渡金属氧化物,例如选自LiCoO2、LiNiO2、LiMnO2、LiMn2O4、Li(NiaCobMnc)O2(0<a<1,0<b<1,0<c<1,a+b+c=1)、LiNi1-yCoyO2、LiCo1-yMnyO2、LiNi1-yMnyO2(0≤y<1)、Li(NiaCobMnc)O4(0<a<2,0<b<2,0<c<2,a+b+c=2)、LiMn2-zNizO4、LiMn2-zCozO4(0<z<2)、LiCoPO4和LiFePO4的任意一种物质或至少两种物质的混合物。
本发明的袋状锂二次电池的电极可根据常规方法制备,例如所述方法包括向溶剂中加入电解质活性材料颗粒和一种粘合剂聚合物,以及一种导电材料和分散剂(如果需要),然后用浆料涂布集电器,最后将其压制并干燥。此外,插入所述阴极和所述阳极之间的隔膜可采用用作常规隔膜的常见多孔聚合物膜,例如使用一种乙烯均聚物、丙烯均聚物、乙烯/丁烯共聚物、乙烯/己烯共聚物或乙烯/甲基丙烯酸酯共聚物制备的单层或层压形式的多孔聚合物膜。在其它情形下,隔膜可为一种常见的多孔非织造物,例如由具有高熔点的玻璃纤维或聚对苯二甲酸乙二醇酯纤维制备的非织造物,但不限于此。
此外,容纳电极组的袋状壳体可使用一种常见的薄片制备,例如一种通过将聚合物膜层压至一个由诸如铝制成的金属片上制得的薄片,例如一种通过将聚乙烯片层压至铝片的两个表面上制得的薄片。
下文中,基于几个实施例更详细地描述本发明。但是,以下实施例可以多种方式变化,且本发明不应被理解为受其限制。提供以下实施例以使本领域普通技术人员更好地理解本发明。
实施例1
将1M LiPF6加入碳酸亚乙酯(EC)与丙酸乙酯(EP)以3∶7的体积比混合的混合有机溶剂中,以制备非水电解质。
然后,电极组通过将聚乙烯多孔膜插入使用LiCoO2作为阴极活性材料的阴极和使用人造石墨作为阳极活性材料的阳极之间,然后将电极组放置并密封于由聚丙烯/铝/聚丙烯薄膜制成的袋状壳体中。向壳体中注入如上制备的非水电解质以制得袋状锂二次电池。
实施例2
以与实施例1相同的方式制备袋状锂二次电池,不同在于使用丁酸甲酯代替丙酸乙酯。
实施例3
以与实施例1相同的方式制备袋状锂二次电池,不同在于使用乙酸丙酯代替丙酸乙酯。
实施例4
以与实施例1相同的方式制备袋状锂二次电池,不同在于碳酸亚乙酯与丙酸乙酯的组成改变为体积比2∶8。
实施例5
以与实施例1相同的方式制备袋状锂二次电池,不同在于碳酸亚乙酯与丙酸乙酯的组成改变为体积比4∶6。
对比例1
以与实施例1相同的方式制备袋状锂二次电池,不同在于混合有机溶剂的组成和种类改变为碳酸亚乙酯∶碳酸二甲酯=3∶7(体积比)。
对比例2
以与实施例1相同的方式制备袋状锂二次电池,不同在于混合有机溶剂的组成和种类改变为碳酸亚乙酯∶碳酸甲乙酯=3∶7(体积比)。
对比例3
以与实施例1相同的方式制备袋状锂二次电池,不同在于混合有机溶剂的组成和种类改变为碳酸亚乙酯∶碳酸二乙酯=3∶7(体积比)。高速充电/放电试验
将根据实施例1-5和对比例1-3制备的袋状电池以0.2C速率充电/放电3次,随后以0.2C速率充电并以2C速率放电。测定的0.2C放电容量、2C放电容量及其容量比列于下表1中。
高温储存的膨胀试验
将根据实施例1-5和对比例1-3制备的袋状电池用1小时的时间从常温加热至90℃。然后在90℃储存4小时。在90℃储存4小时的时间内厚度的增加列于表1中。
【表1】
溶剂组成 | 0.2C放电容量(mAh) | 2C放电容量(mAh) | 2C/0.2C容量比(%) | 高温储存时的厚度增加(mm) | |
实施例1 | EC/EP=3/7 | 901 | 752 | 83.5 | 0.18 |
实施例2 | EC/MB=3/7 | 897 | 746 | 83.2 | 0.14 |
实施例3 | EC/PA=3/7 | 898 | 748 | 83.3 | 0.16 |
实施例4 | EC/EP=2/8 | 897 | 729 | 81.3 | 0.25 |
实施例5 | EC/EP=4/6 | 900 | 743 | 82.6 | 0.15 |
对比例1 | EC/DMC=3/7 | 905 | 758 | 83.8 | 5.56 |
对比例2 | EC/EMC=3/7 | 903 | 634 | 70.2 | 0.22 |
对比例3 | EC/DEC=3/7 | 897 | 503 | 56.1 | 0.03 |
如表1所示,应理解:根据实施例1-5的袋状锂二次电池具有良好的2C放电容量,其基本上与使用碳酸亚乙酯和碳酸二甲酯的混合有机溶剂的对比例1处于相同水平,但不同于对比例2和3。同时,对比例1的袋状锂二次电池在高温储存时厚度增加很大,并因而具有严重的膨胀问题。另一方面,本发明实施例1-5的袋状锂二次电池与对比例2和3一样具有小的厚度变化。
【产业实用性】
本发明的袋状锂二次电池采用具有高离子电导率的预定混合有机溶剂,而不使用线性碳酸酯化合物,以确保出色的高速放电特性,并解决了与具有袋状壳体的电池相关的膨胀问题。
Claims (12)
1.一种袋状锂二次电池,包括:
一个电极组,其含有阳极、阴极和插入所述阴极和所述阳极之间的用于使其间电绝缘的隔膜;
一个由薄片制成的袋状壳体,用于提供容纳所述电极组的空间;以及
一种注入所述电极组中的非水电解质,
其中所述非水电解质是一种基于非线性碳酸酯的非水电解质,包括一种锂盐、(a)一种环状碳酸酯化合物和(b)一种选自基于丙酸酯的化合物、丁酸甲酯、乙酸丙酯及其混合物的线性酯类化合物,并且
其中,溶解1M LiPF6时,所述非水电解质在约23℃时的离子电导率为9mS/cm或更高。
2.权利要求1的袋状锂二次电池,其中(a)组分与(b)组分的体积比(a∶b)为约2∶8至约4∶6。
3.权利要求1的袋状锂二次电池,其中所述环状碳酸酯化合物包括选自碳酸亚乙酯、碳酸亚丙酯、氟代碳酸亚乙酯和碳酸亚丁酯的任意一种物质或至少两种物质的混合物。
5.权利要求4的袋状锂二次电池,其中所述由化学式1表示的基于丙酸酯的酯类化合物包括选自基于丙酸甲酯的化合物、基于丙酸乙酯的化合物、基于丙酸丙酯的化合物和基于丙酸丁酯的化合物中的至少一种化合物。
6.权利要求5的袋状锂二次电池,其中所述基于丙酸乙酯的化合物为选自丙酸乙酯、3-氟丙酸乙酯、3,3-二氟丙酸乙酯、3,3,3-三氟丙酸乙酯、丙酸2-氟乙酯、丙酸2,2-二氟乙酯、丙酸2,2,2-三氟乙酯、3-氟丙酸2,2,2-三氟乙酯、3,3-二氟丙酸2,2,2-三氟乙酯,和3,3,3-三氟丙酸2,2,2-三氟乙酯的任意一种物质或至少两种物质的混合物。
7.权利要求1的袋状锂二次电池,其中所述锂盐包括选自LiPF6、LiBF4、LiSbF6、LiAsF6、LiClO4、LiN(C2F5SO2)2、LiN(CF3SO2)2、CF3SO3Li和LiC(CF3SO2)3的任意一种物质或至少两种物质的混合物。
8.权利要求1的袋状锂二次电池,其中所述阳极由能够吸藏或释放锂离子的碳材料制成。
9.权利要求8的袋状锂二次电池,其中所述能够吸藏或释放锂离子的碳材料为一种低晶态碳或高晶态碳。
10.权利要求1的袋状锂二次电池,其中所述阴极由含锂的氧化物制成。
11.权利要求10的袋状锂二次电池,其中所述含锂的氧化物为一种含锂的过渡金属氧化物。
12.权利要求11的袋状锂二次电池,其中所述含锂的过渡金属氧化物为选自LiCoO2、LiNiO2、LiMnO2、LiMn2O4、Li(NiaCobMnc)O2(0<a<1,0<b<1,0<c<1,a+b+c=1)、LiNi1-yCoyO2、LiCo1-yMnyO2、LiNi1-yMnyO2(0≤y<1)、Li(NiaCobMnc)O4(0<a<2,0<b<2,0<c<2,a+b+c=2)、LiMn2-zNizO4、LiMn2-zCozO4(0<z<2)、LiCoPO4和LiFePO4的任意一种物质或至少两种物质的混合物。
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US8741473B2 (en) | 2014-06-03 |
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JP2011508956A (ja) | 2011-03-17 |
CN101911370B (zh) | 2017-02-08 |
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WO2009084928A3 (en) | 2009-10-15 |
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