CN1424784A - 制造含有液体有机电解质的原电池的方法 - Google Patents

制造含有液体有机电解质的原电池的方法 Download PDF

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CN1424784A
CN1424784A CN02151588A CN02151588A CN1424784A CN 1424784 A CN1424784 A CN 1424784A CN 02151588 A CN02151588 A CN 02151588A CN 02151588 A CN02151588 A CN 02151588A CN 1424784 A CN1424784 A CN 1424784A
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electrolyte
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oxygen
primary cell
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F·比尔克-萨拉姆
P·比尔克
K·霍尔
H·施特尔茨格
D·伊利克
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VARTA Microbattery GmbH
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Abstract

一种制造包含有机电解质的原电池的方法，其中原电池包含具有至少一种锂嵌入电极的蓄电池电极隔板部件，该锂嵌入电极中不溶于聚合物基质的电化学活性的微细材料分布在所含的聚合物中，其中电解质包含2至15重量％具有一个中心碳原子的烃－氧化合物(碳酸酯)，一个氧原子通过双键而两个氧原子通过单键与该碳原子结合，通过其他的原子或基团使得单键的氧原子不饱和，而且具有四个碳原子或更短的烃链与那些单键的氧原子中的每一个结合，这两个链中区别在于至少一个、但不超过三个CH2－基团，首先用该电解质混合物浸透电极隔板部件，接着切割至其尺寸，然后插入到外壳中。在用液体有机电解质浸透电极隔板部件前将其层压在导体和/或反电极上，而且也可卷绕后再浸透该电极隔板部件。

Description

制造含有液体有机电解质的原电池的方法
技术领域
本发明涉及一种制造包含有机电解质的原电池的方法，其中原电池包含具有至少一种锂嵌入电极的蓄电池电极隔板部件，该锂嵌入电极中，不溶于聚合物基质的电化学活性微细材料分布在所含的聚合物中，并且涉及根据将描述的方法制造的原电池。
背景技术
通常首先将电极插入到被称为“半壳”的电池外壳中，接着加入电解质。但是，在涉及用于例如“智能卡”的具有小于0.5mm厚度的超平能量储存器件的情况下，上述过程就不再适用，因为在其杯(cup)和盖板上的密封附近容易发生污染，是由于在这类薄电池的外壳中没有电解质可渗回的凹陷，该凹陷可阻碍渗透电解质的糊剂的使用。
在使用锂金属和二氧化锰基阴极的3V一次回路中，通常电解质要么是高氯酸锂LiClO4，要么是三氟甲烷磺酸锂CF3SO3Li，它们溶解在碳酸丙烯酯(PC)中，如果需要可加入例如二甲氧基乙烷的减粘剂。例如，国际专利申请WO00/57504公开了一种薄膜电池，其阳极由二氧化锰，碳和电解质的糊剂混合物制成，其中所含的糊剂是在框架中制备。在含有碳阳极和LiMeO2阴极(Me＝Ni，Co或Mn)的可再充电4V系统中，使用由碳酸1，2-亚乙酯(EC)，碳酸丙烯酯(PC)，碳酸二甲酯(DMC)，碳酸乙基甲基酯(EMC)，碳酸二乙酯(DEC)，或其碳酸酯衍生物构成的混合物中的六氟磷酸锂LiPO4F6。美国专利US5296318中公开了用聚偏1，1-二氟乙烯-六氟丙烯共聚物和类似的混合物制成的膜所组成的聚合物电极的使用。
发明内容
本发明所要解决的问题是提出了一种制造含有液体有机电解质的原电池的方法，它特别适用于防止电解质对外壳部件的污染，而且其外壳的半壳被完全密封并且防止了渗漏。
本发明利用本说明书开始时所述类型的原电池解决了此问题，该电池具有在权利要求1中所述的特征。从属权利要求陈述了该方法和由该方法制造的原电池的有益实施方案。
在本发明的方法中，电解质包含2至15重量％具有一个中心碳原子的烃-氧化合物(碳酸酯)，一个氧原子通过双键而两个氧原子通过单键与该碳原子结合，通过其他的原子或基团使单键的氧原子不饱和，而且具有四个碳原子或更短的烃链与那些单键的氧原子中的每一个结合，这两个链中区别在于为至少一个、但不超过三个CH2-基团。首先用该电解质混合物浸透电极隔离部件，接着切割至其尺寸，然后插入到外壳中。
本发明的有机电解质在快速渗透到电极隔离元件中和缓慢从电极隔离元件中蒸发方面是特别有益的，该有机电解质含有缺少对称轴的开链碳酸酯，因为这种特殊的电解质包含能减少表面张力的不对称极性溶剂，并且允许电解质均匀快速地渗入到电池组件中。另外，由于电解质和蓄电池电极隔板部件之间的范得瓦力而导致增加的电解质的蒸气压被减少了，该范得瓦力是由于电解质溶剂混合物的至少一种成分的极性而产生的。
如果在用液体有机电解质浸透之前，将蓄电池电极隔板部件层压在导体或反电极上将是有益的，蓄电池电极隔板部件也可卷起后被浸透。
所包括的碳酸酯是在电解质混合物中的碳酸乙基甲基酯或碳酸丙基甲基酯，该电解质混合物优选包含高氯酸锂，碳酸丙基酯和碳酸乙基甲基酯。所讨论的导电盐是双(草酸)硼酸锂和三氟三(五氟乙基)磷酸锂，因为它们两者与水接触时，像高氯酸锂一样具有不释放盐酸作为预期的水解产物的有益特性。碳酸丙烯酯(PC)和碳酸乙烯酯(EC)是其它有前景的电解质成分。
如果本发明的方法用于制造小于0.5mm厚并且具有小于50mAh额定容量的平板电池将是特别有益的。
聚偏1，1-二氟乙烯(PVDF)和六氟丙烯(HFP)代表用于制造本发明电极隔离部件的聚合物的适宜选择。可以使用的溶剂是例如正-甲基吡咯烷2-吡咯烷酮或丙酮。多孔的隔离材料由聚烯烃组成，优选聚丙烯或聚乙烯，或由这些材料的各种组合构成的多层层压产品。
适宜制造负电极的材料包括金属锂或石墨化的碳，而且如果需要，可包括优选占所述材料65至85重量％的改性碳，以及具有适宜电压等级的混和氧化物的层间复合物，而正电极包含一种铁-氧或锰-氧化合物，如果需要，该化合物也可包含磷或锂作为插层的锂材料。
用于制造负电极箔的糊剂混合物包含55至95重量％，优选65至85重量％的前述类型材料用于制造正极的糊剂混合物含65至98重量％、优选为65至95重量％的正极材料。本发明糊剂混合物包含50至75重量％、优选55至65重量％的溶剂。正电极箔中PVDF/HFP的比例范围从最大99.5至最小0.5，优选从最大80至最小20。PVDF/HFP的分子量比例范围从3.2至2.8，或优选从2.3至2.5。
负电极箔中PVDF/HFP的比例范围为99.5至0.5，优选为85至15。PVDF/HFP的分子量比例范围从3.2至2.8，或优选从2.3至2.5。
将所含的糊剂制造成其初始混合物的粘度范围是从1帕斯卡·秒(Pa·s)至10帕斯卡·秒(Pa·s)，优选从3帕斯卡·秒至6帕斯卡·秒。
为了制造原电池，将其电极或是最初直接涂覆在导体或隔离体上，或是施加在载体箔上，接着在两步法中热层压。电池组件的其余部分涉及使电极隔离部件热层压至导体或使电极导体部件热层压至隔离层。
具体实施方式
通过完全混和丙酮中的在360℃下已热激活的77重量％褐锰矿(电解的MnO2)，6重量％的石墨(Timrex KS 6)、2重量％的导电碳黑(Erachem Super P)、7重量％的聚偏1，1-二氟乙烯-六氟丙烯(Elf Atochem Kynar FLEX2801)，和8重量％的碳酸丙烯酯来制备糊状材料(糊剂)，然后在聚烯烃(Calgard 2500聚丙烯)隔离层上涂覆所得的糊剂。蒸发溶剂并且在110℃下将所得的片真空干燥48小时，然后用有机锂电解质浸透该片，包含87体积％碳酸丙烯酯：13体积％碳酸乙烯酯的该电解质中已有0.96M的LiClO4。将电极隔离部件冲出1.6cm×2.3cm的孔，该孔中插入铜箔外壳，已预先在该外壳覆盖面上压制锂，而外壳的杯边已涂覆了石墨基导电增强剂，并且利用铜与铜接触时的绝缘层来将其杯和盖板进行超声波焊接。
对比实施例
在上述实施例的电解质中分别加入碳酸二甲酯和碳酸二乙酯来代替碳酸乙基甲基酯。在这两种情况下观察到更长的渗透时间，不完全的渗透和快速蒸发，这通过最初白片的变黑而后又恢复成白色而显示出来。

Claims (8)

1.一种制造包含有机电解质的原电池的方法，其中原电池包含具有至少一种锂嵌入电极的蓄电池电极隔板部件，该锂嵌入电极中不溶于聚合物基质的电化学活性微细材料分布在所含的聚合物中，其中电解质包含2至15重量％的具有一个中心碳原子的烃-氧化合物(碳酸酯)，一个氧原子通过双键而两个氧原子通过单键与该碳原子结合，通过其他的原子或基团使得单键的氧原子不饱和，而且具有四个碳原子或更短的烃链与那些单键的氧原子中的每一个结合，这两个链中区别在于至少一个、但不超过三个CH2-基团，首先用该电解质混合物浸透电极隔板部件，接着切割至其尺寸，然后插入到外壳中。
2.根据权利要求1的方法，其特征在于在用液体有机电解质浸透电极隔板部件前将电极隔板部件层压在导体和/或反电极上。
3.根据权利要求1或2的方法，其特征在于可将该电极隔板部件卷起并且接着进行浸透。
4.根据权利要求1至3任一的方法，其特征在于所述碳酸酯是碳酸乙基甲基酯或碳酸丙基甲基酯。
5.根据权利要求1至4任一的方法，其特征在于电解质包含高氯酸锂、双(草酸)硼酸锂或三氟三(五氟乙基)磷酸锂中的至少一种导电盐，并且优选碳酸丙烯酯或碳酸乙烯酯中的至少一种开链(cyclic)的碳酸酯。
6.根据权利要求5的方法，其特征在于电解质包含碳酸乙基甲基酯。
7.根据前述任一种方法得到的原电池。
8.根据权利要求7的原电池，其特征在于原电池的厚度小于0.5mm并且电池容量小于50mAh。
CN02151588A 2001-12-03 2002-12-03 制造含有液体有机电解质的原电池的方法 Pending CN1424784A (zh)

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EP1317012A3 (de) 2005-04-13
US20030113637A1 (en) 2003-06-19

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