CN1197301A - 层压式锂离子电池及其制造方法 - Google Patents

层压式锂离子电池及其制造方法 Download PDF

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CN1197301A
CN1197301A CN98107072A CN98107072A CN1197301A CN 1197301 A CN1197301 A CN 1197301A CN 98107072 A CN98107072 A CN 98107072A CN 98107072 A CN98107072 A CN 98107072A CN 1197301 A CN1197301 A CN 1197301A
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lithium
ion cell
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P·鲍尔莱恩
J·奥伯豪泽尔
H·W·普拉斯
H·舍曼
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VARTA Batterie AG
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Abstract

本发明涉及一种含有易弯曲层的层压式锂离子电池,其中该负极是金属锂、锂合金或金属粘着的纤维网或泡沫材料,其中含有嵌入锂材料如碳、石墨、二氧化钨、二氧化钛、二硫化钛、二氧化钼或五氧化二钒作为活性组分,该隔板是由一种多孔聚合物制成其中固定有一种非水电解质,并且作为活性物质的该正极含有锂锰二氧化物(lithiated manganesedioxide)、锰尖晶石、锂金属氧化物、锂金属的混合氧化物或锂金属硫化物。

Description

层压式锂离子电池及其制造方法
本发明涉及一种层压式锂离子电池及其制造方法。更具体地说，本发明涉及可再充电的锂离子电池，该电池包括一多孔聚合物材料的隔板。由于该聚合物基体中含有在有机溶剂中易解离的锂盐溶液而使之具有离子导电性。因此锂离子可以通过该隔板从一个电极迁移至另一个电极。
在美国专利US-A 5470357中公开了层压式锂离子电池。该电池的正极和负极以及隔板均具有一易弯曲的聚合物基体。用加热和加压的方法使其与具有聚合物涂层的集流器箔片相结合以形成易弯曲的层压式结构。所有用于电极、隔板和集流器箔片预涂层的聚合物必须是在该处理过程中相互可混溶的。在所有情况下，1，1-二氟乙烯和六氟环丙烯的共聚物(PVdF-HFP的共聚物)是优选的。因此该公知的锂离子电池需要一种用于制造电极层和隔板层的聚合物基体。
本发明的目的是详细说明锂离子电池及其制造方法，使得金属锂、锂合金或金属电极支撑材料可用于层压式电池中。
该新电池及其制造方法表示在权利要求1-10中。
该层压式锂离子电池通常包括易弯曲层，其中负极是金属锂、锂合金或金属粘着的纤维网或泡沫材料，其中含有嵌入锂材料如碳、石墨、二氧化钨、二氧化钛、二硫化钛、二氧化钼或五氧化二钒作为活性组分。该隔板是由一种多孔聚合物制成其中固定有一种非水电解质，并且作为活性物质的该正极含有含锂锰黑(lithiated manganese black manganese black)、锰尖晶石、锂金属氧化物、锂金属的混和氧化物或锂金属硫化物。
如果应用锂金属或锂合金，则用电化学稳定的金属栅或网层压在一起作为集流器。同样地，屏蔽负极的那部分聚合物材料可以在插入电池套筒前移除。该电池无需任何另外施加的压力。可选择地，该负极可含有粘着纤维网或泡沫体，由镍制成并且其中涂覆有锂嵌入化合物如碳材、石墨或金属氧化物如MoO2，WO2、TiO2、V2O5或金属硫化物如TiS2同时可加入导电添加剂如导电炭黑和粘结剂如聚四氟乙烯(PTFE)、聚环氧乙烷(PEO)或聚1，1-二氟乙烯(PVdF)的分散体。而后对这样获得的该负极带进行干燥并碾压使之压实。优选的是在负极上预涂覆聚环氧乙烷(PEO)分散体。在该PEO分散体中加入石墨使石墨具有预含锂(prelithiation)的性能。该集流器优选为多孔铜金属网或铜网。
该正极所使用的支撑材料可以粘着纤维网、多孔金属或网，它们是由镍或铝制成，其中涂覆有锰黑或含锂锰黑(lithiated manganese black)、尖晶石或锂金属氧化物如LiNiO2、LiCoO2以及导电炭黑和上述粘结剂的涂膏。
由正极、负极和隔板层压在一起的电极叠层构成的该新锂离子电池在层压后可以在干燥的室内甚或在一般湿度(如1-50％湿度)下进行处理。该电极叠层可以储存而没有任何容量损失。只有在引入了该非水电解质后才具有活性。这是由于将增塑剂提取和其后将电极叠层浸渍于在有机溶剂中的导电盐溶液造成的，或是由于增塑剂直接从电解质中进行转换造成的，即将该层压电极叠层在电解质中保存5-30分钟。这需要保护性气氛中的含水量在ppm数量级。该新层压式锂离子电池特别适用于制造非常薄且易弯曲的电池，其厚度在200μm至1mm之间。
以下本发明将结合附图和实施例进行详细描述，其中：
图1所示为依据实施例2制造的电池的放电曲线，放电是在室温下3mA恒电流放电，直到断路电压为1.8V下进行的，并且以1mA恒电流进行后期放电。
图2所示为依据实施例2的放电条件下制造的电池的放电曲线，在放电前在60℃温度保存了36天。
实施例1准备该负极材料22g  LiMnO2，5.9g PVdF，2.6g 导电炭黑，9g   邻苯二甲酸二丁酯，在75g  丙酮
将上述物质进行分散并用缝宽为850μm的刮涂装置拉制成薄膜，该薄膜在约10分钟内干燥。而后，在175℃温度下将该负极箔片用层压法压在多孔铝金属网上，配备一个集流器并将其分割为面积为24.75cm2的矩形片。
该正极物质是由辊镀了厚度约为250μm的锂箔的多孔铜金属网获得的，在其边缘部分不含锂或在该去除锂之处都不含有锂。
基本上由包括上述材料和PVdF隔板构成的该电池叠层由许多片上述材料一层叠一层而得到的，PVdF隔板的厚度约为110μm，该正极材料和第二PVdF隔板的厚度约为55μm并被置于该负极材料背向集流器的一面。基于此种设置该PVdF隔板的边缘伸出该正极材料所有的边约5mm。在约140℃温度下，在一个辊架上(该辊架与电池叠层接触的表面被加热)将这种电池叠层从两侧进行层压。获得的该电池叠层的总厚度为720μm。为去除该增塑剂，对该层压电池叠层用无水二乙醚进行三次提取，并进行搅拌，而后干燥。将这样处理过的电池叠层在一种含有溶剂为1∶1的碳酸乙烯酯(EC)和碳酸二乙酯(DEC)混合物的1M LiPF6溶液的电解质溶液中浸渍30分钟，移除多余的电解质，而后将其密封于多层金属箔中，该箔为一种金属化的聚乙烯/聚丙烯箔。
该电池在恒流放电电流密度为0.12mA/cm2下的比容量为120mAh。实施例2
负极材料与实施例1中的相同，所不同的是它含有磷酸三丁酯(TBP)作为增塑剂，将该负极材料用缝宽为900μm的刮涂工作台拉制成薄片。当该薄片干燥后，在158℃温度下，将其层压在多孔铝金属网上，该负极箔和该多孔金属网设置于两层特氟隆片之间。
所用的该正极材料为按照实施例1的方法在多孔铜金属网上所获得的锂金属箔。
所用的隔板为PVdF膜，该膜用缝宽为500μm的刮涂成形的，并且该膜含有20％wt的SiO2，30％wt的PVdF和50％wt的磷酸三丁酯。
该电池叠层是用与实施例1类似的方法将上述部件层压在一起并在含有1M LiClO4溶液的碳酸丙烯酯(PC)电解质中贮存15分钟，伴以搅拌而得到的。根据实施例1的方法将该含有电解质的电池叠层密封于金属化的多层箔片中。
图1所示为在室温以3mA恒流放电条件下开始放电直至断路电压为1.8V，而后以1mA进行后期放电，所得到的该电池电压(以伏特为单位)相对于容量降(单位为mAh)的分布。
图2所示为一个类似的电池的放电曲线，所不同的是该电池在放电前于60℃温度下贮存了36天。实施例3
用与实施例1类似的方法制备一种负极材料，所不同的是将锂尖晶石作为活性成分。
用与实施例1类似的方法制备正极，在其上涂覆碳酸亚乙酯和含有聚环氧乙烷的四氢呋喃悬浮液。
所用的隔板含有30wt％的聚1，1-二氟乙烯/六氟丙烯共聚物，还含有20wt％的SiO2和50wt％的邻苯二甲酸二丁酯。
由负极材料、隔板和正极材料组成的该电池叠层在70-100℃温度下层压在一起并浸渍于含有溶剂为2∶1的EC和DMC混合物的LiPF6电解质中。根据实施例1的方法通过将该电池叠层密封于金属化的多层箔片中所获得的该电池在9小时放电条件下的比容量为43.5mAh。实施例4
用与实施例1类似的方法制造电池，所不同的是将聚丙烯隔板与根据实施例1的隔板共层压在一起并且使用了含锂锰黑(lithiated manganeseblack)。
该制得的电池在恒定电流为3mA下放电时的电池比容量为25.5mAh。

Claims (10)

1、一种含有易弯曲层的层压式锂离子电池，其中该负极为金属锂、锂合金或金属粘着的纤维网或泡沫材料，其中含有嵌入锂材料如碳、石墨、二氧化钨、二氧化钛、二硫化钛、二氧化钼或五氧化二钒作为活性组分，该隔板是由一种多孔聚合物制成，其中固定有一种非水电解质，并且作为活性物质的该正极含有含锂锰黑(lithiated manganese black)、锰尖晶石、锂金属氧化物、锂金属的混合氧化物或锂金属硫化物。
2、根据权利要求1的层压式锂离子电池，其中该负极由锂金属或锂合金制得，在该负极背向该隔板的一面用一个聚合物箔片屏蔽。
3、根据权利要求2的层压式锂离子电池，其中该负极用一种聚环氧乙烷分散剂预涂覆。
4、根据权利要求2和/或3的层压式锂离子电池，其中该聚环氧乙烷分散剂中含有石墨。
5、根据权利要求2-4中的一项或多项的层压式锂离子电池，其中将金属栅或网作为集流器共层压在至少一个电极中。
6、根据权利要求1-5中的一项或多项的层压式锂离子电池，其中该隔板材料包括聚丙烯、聚乙烯、聚环氧乙烷、聚1，1-二氟乙烯、聚四氟乙烯、聚酰胺或它们的共聚物或其三元共聚物。
7、根据权利要求1-6中的一项或多项的层压式锂离子电池，其中该层状电极和该隔板的面积高达50cm2并且厚度高达1mm。
8、权利要求1-7中的一项或多项的层压式锂离子电池的制造方法，其中在层压前适当的时候，该正极的隔板材料和屏蔽该负极的该聚合物材料与一种增塑剂相混。
9、根据权利要求8的方法，其中该增塑剂在电池使用前转变为一种非水电解质。
10、根据权利要求8和9的方法，其中屏蔽该负极的一部分聚合物材料被移除。
CN98107072A 1997-03-10 1998-03-09 层压式锂离子电池及其制造方法 Pending CN1197301A (zh)

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