CN1253387A - 无液体电解质电池 - Google Patents

无液体电解质电池 Download PDF

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CN1253387A
CN1253387A CN99123616A CN99123616A CN1253387A CN 1253387 A CN1253387 A CN 1253387A CN 99123616 A CN99123616 A CN 99123616A CN 99123616 A CN99123616 A CN 99123616A CN 1253387 A CN1253387 A CN 1253387A
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packaging material
exterior packaging
liquidless
electrolyte battery
heat
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CN1140936C (zh
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柴田启一
小幡享子
八田一人
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Murata Northeast China
Murata Manufacturing Co Ltd
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Sony Corp
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Abstract

一种无液体电解质电池可减小它在便携式电子设备中的伸出区域。一个单元电池装于多层膜的外封装材料中,由深拉法用一个间隔形成,并且其中电连接于单元电池各电极的电极终端引线是从外封装材料的里面引出到外面的。外封装材料是在由深拉法形成的间隔周围热熔的,除了从其引出所述电极终端引线的所述外封装材料的热熔部分之外,所述外封装材料的热熔部分是在其自身上折叠的。用介质片把折叠的外封装材料固定到外封装材料上。

Description

无液体电解质电池
本发明涉及一种无液体电解质电池，其中一个单元电池被装于一个由叠层膜组成的外封装材料中。更具体地说，它涉及一种无液体电解质电池，其中外封装材料的热熔融部分被折叠。
近来，主要以笔记本式个人计算机为代表的电子设备有一种向无塞绳性和便携性发展的趋势，并且还在一个接一个地研制小尺寸轻重量便携式电子设备。由于电子设备的多样性，正在试图减小蓄电池的厚度和尺寸。
已提出用一种聚合物锂离子蓄电池作上述的电池和蓄电池，它用一种以电解液溶胀的高聚合物凝胶作电解质。
至于聚合物锂离子蓄电池的结构，在由铝薄片组成的正电极集电器上敷设一层由LiCoO2和锌组成的活性材料，以构成一个正电极。在负电极集电器上敷设一层由例如碳、焦碳、石墨等组成的活性材料，以构成一个负电极。在负与正集电器之间，插入一个由聚丙烯或聚乙烯组成的多孔薄膜的隔板。在这些电极与隔板之间，装进一种高分子凝胶电解质，例如聚丙烯腈(PAN)、聚氧化乙烯(PEO)或聚偏氟乙烯(PVDF)，以提供一种整体夹层状结构。
夹层状结构的单元电池由一种用作密封容器的外封装材料封装，该容器由一个铝箔之类的软金属膜和一个耐纶、聚乙烯、聚丙烯或聚对苯二甲酸乙二酯的膜之类的塑料膜组成。
在其中单元电池是由上述外封装材料封装的无液体电解质电池中，外封装材料的边缘部分是在其中装入单元电池时用热熔法来密封的。这个外封装材料的热熔部分是无液体电解质电池防水所必需的，至少具有5mm的宽度。
这样，在无液体电解质电池中，单元电池的尺寸加上外封装材料热熔部分的尺寸就是电池的总尺寸。这样，在无液体电解质电池中，已经难以减小电池的外尺寸，尤其是它在电子设备中从平面方向伸出的区域的尺寸。
因此，本发明之目的在于提供一种无液体电解质电池，它在便携式尺寸电子设备中的伸出区域是能够减小的。
根据本发明，提供一种无液体电解质电池，其中一个单元电池装于叠层膜的外封装材料中，该膜用深拉法以一定的间隔制成，并且其中电连接于单元电池各电极的电极终端引线是从外封装材料的内侧引导到外侧的。在此，外封装材料是围绕用深拉法形成的间隔而热熔的，除了从其引出电极终端引线的外封装材料热熔区以外，外封装材料的热熔部分是在其自身上折叠的。
在本发明的无液体电解质电池的情况下，外封装材料的叠合部分是用一个粘性转接带来固定。
在本发明的无液体电解质电池的情况下，热熔外封装材料是在其自身上折叠的，以便减小从电池平面侧看到的电池尺寸。
此外，在其中用粘性转接带固定叠合外封装材料的本发明无液体电解质电池中，有可能长时期保持减小的外尺寸。
图1是一个立体图，说明一个要插入外封装材料内的单元电池。
图2是一个无液体电解质电池的立体图。
图3A至3D是从底侧看的立体图，说明用于无液体电解质电池的外封装材料侧部的折叠状态。
图4是一个立体图，说明一个折叠模具。
图5A和5B是放大截面图，说明在其上调整无液体电解质电池的折叠模具的主要部分。
图6是一个固定模具的平面图，在该模具上调整无液体电解质电池。
图7是一个固定模具的截面图，取自图6的A-A线。
图8A至8C是放大截面图，说明在其上调整无液体电解质电池的固定模具的主要部分。
参照附图，详细说明根据本发明的无液体电解质电池的优选实施例。
如图1和图2所示，无液体电解质电池1例如是一个固态电解质电池或一个凝胶状电解质电池，由单元电池2和外封装材料3组成。单元电池2由置于正和负电极的活性材料层之间的一种固态电解质或一种凝胶状电解质组成，外封装材料3由一个在其本身上折起来的片状叠层膜组成。
电池单元2具有一个负终端引线4和一个正终端引线5，它们分别电连接于单元电池2的正电极和负电极。
用作单元电池2的高分子固态电解质的高分子材料只通过例子枚举如下：硅凝胶，丙稀酸凝胶，丙烯腈凝胶，聚磷腈改性聚合物，聚乙烯氧化物，聚丙烯氧化物，及其化合物，其交联或改性聚合物，氟基聚合物，例如聚(偏氟乙烯)，(偏氟乙烯-CO-六氟丙烯)，聚(偏氟乙烯-CO-三氟乙烯)，及其混合物。
在用一种由高分子化合物、电解质盐和溶剂组成的溶液(在凝胶状电极情况下用增塑剂)浸渍正电极活性材料或负电极活性材料层、去除其溶剂和固化所得物质时，可得到在正电极活性材料或负电极活性材料层上成层放置的固态电解质或凝胶状电解质。在正电极活性材料或负电极活性材料层上成层放置的固态电解质或凝胶状电解质，具有它的通过在正电极活性材料或负电极活性材料中浸渍而固化的部分。如果单元电池2的高分子材料是交联的，则随后用光或热在交联时固化。
凝胶状电解质由含增塑剂的锂盐和不少于2wt％到30wt％或30wt％以下的复合高分子材料组成。应当指出，酯-醚或碳酸酯可以单独使用，也可用作增塑剂的配料。
可以使用各种用于构成凝胶状电解质的高分子材料，作为用于在制备凝胶状电解质时胶凝这些碳酸酯的复合高分子材料。由还原/氧化稳定性来看，希望使用一种氟基高分子材料，例如聚(偏氟乙烯)或聚(偏氟乙烯-CO-六氟丙烯)。
高分子固态电解质由锂盐和用于溶解锂盐的高分子化合物组成。高分子化合物，醚基高分子化合物，例如聚(氧化乙烯)或它的交联化合物，聚(甲基丙烯酸酯)酯，丙烯酸酯，或氟基高分子化合物，例如聚(偏氟乙烯)或聚(偏氟乙烯-CO-六氟丙烯)，可以单独使用，也可作为混合物使用。由氧化/还原稳定性来看，可以优选地使用氟基高分子化合物，例如聚(偏氟乙烯)或聚(偏氟乙烯-CO-六氟丙烯)。
可以使用那些用于常规电池电解液中的锂盐，作为要含在凝胶状电解质或高分子固态电解质中的锂盐。只作为例子枚举一些锂化含物(盐)：氯化锂，溴化锂，碘化锂，氯酸锂，高氯酸锂，溴酸锂，碘酸锂，硝酸锂，四氟溴酸锂，六氟磷酸锂，醋酸锂，双(三氟甲烷磺酰)亚氨锂，LiAsF6，LiCF3SO3，LiCSO2CF3)3，LiAlCl4，和LiSiF6。
这些锂化合物可以单独使用，也可组合地使用。其中，从氧化稳定性来看，LiPF6和LiBF4是合乎需要的。
锂盐的深度是0.1到3.0摩尔每升增塑剂，最好是0.5到2.0摩尔每升增塑剂。
除了使用上述凝胶状电解质或固态电解质之外，可以通过与常规锂离子电池相同的方法，构造根据本发明一个实施例的无液体电解质电池1的单元电池2。
这就是说，这样一种能够掺入/不掺入锂的材料，能够用作一种锂离子电池的负电极材料。可以使用用于负电极的组成材料，例如碳材料，举例来说，难以石墨化的含碳材料或石墨材料。更准确地说，可以使用碳材料，包括热解碳，焦炭(沥青焦炭，针状焦炭或石油焦炭)，石墨，玻璃状碳，烧结的有机高分子化合物(酚醛树脂或焦炉树脂，以适当温度煅烧或焦化的)，碳纤维，和活性碳。其他能够掺入不掺入锂的材料包括高分子化合物，例如聚乙炔或聚吡咯，也可以使用SnO2之类的氧化物。在制备负电极时，如果需要，可以添加一些已知类型的粘合剂。
可以根据要制备的电池的类型，用金属氧化物或金属硫化物之类的高分子化合物或特殊高分子化合物作正电极活性材料，去构造正电极。如果例如要制备锂离子电池，则可以用下述材料作正电极的活性材料：无锂的金属硫化物或氧化物，例如TiS2，MoS2，NbSe2或V2O5，或主要由LiMxO2组成的复式锂氧化物，在此M表示至少一种过渡金属，且X通常为0.05至1.10，取决于电池的充电/放电状态。复式锂氧化物的过渡金属M最好是Co，Ni或Mn。复式锂氧化物的具体实例包括LiCoO2；LiNiO2；LiNiyCo1-yO2，在此0＜y＜1；或LiMn2O4。复式锂氧化物能够产生高电压，和用作具有高能量密度的正电极活性材料。有多种正电极活性材料可用于正电极。在制作正电极时，如果需要，可以添加已知类型的导电材料或粘合剂。
无液体电解质电池1中的单元电池2的结构可以任意地选自层状型，卷取型或折叠型。如果考虑到在外封装材料3中形成的和要在其中装入单元电池2的(如下文所述)间隔的形状，则希望采用具有弓形横侧的卷取型单元电池2。
外封装材料3由一个热密封式片状叠层膜形成，该膜包括三层，即一个外保护层，一个铝层和一个热熔层(最里面的叠层)。热熔层用于通过热熔来密封单元电池2，由塑料膜形成。塑料膜可以是任何适宜的热塑合成材料，例如聚乙烯，聚丙烯或聚对苯二甲酸乙二醇酯。
先用间隔6形成外封装材料，间隔深度的大小等于单元电池2的厚度。再沿着在间隔6侧面的一条线来在其自身折叠外封装材料3。于是在其自身上折起来的外封装材料3由一个外壳表面3a和一个底面3b组成。表面3a由深拉法用间隔6在其中部形成；底面3b面对外壳表面3a而安置，并且适合封闭在其中容纳单元电池2的间隔6。
沿着一个平行于折叠线的侧面和沿着两个垂直于折叠线的侧面，以预置宽度的热熔界限用热熔法来密封外封装材料3。即，在外封装材料3中，除了折叠侧面以外的三个外封装材料3的侧面代表预置宽度的热熔区，外壳表面3a和底面3b通过该区互相连接。
参照图2，从外壳表面3a和平行于折叠侧的底面3b的热熔区的侧面，把负电极终端引线4和负电极终端引线5引出到外面。此外，垂直于折叠侧的无液体电解质电池1两侧的热熔区的两个横侧面7，在底面3b折起来和在此固定。在无液体电解质电池1中，由于热熔横侧面7是在底面3b折叠的，从而能减小电子设备中电池的伸出区和电子设备的尺寸。此外，在无液体电解质电池1中，由于与外壳表面3a和底面3b在一起热熔的横侧面7是在底面3b折起来的，从而与常规电池相比，能够在防水方面改善电池。
横侧面7能够折叠成一种基本上V字形的截面。如果以基本上V字形截面形状折叠横侧面7倾向于损坏无液体电解质电池1的外封装材料3，则可考虑外封装材料3的材料类型，以某种曲率半径R折叠横侧面7，以防折叠部分损坏。
在无液体电解质电池1中，折叠于上述外封装材料3的底面3b上的横侧面7是例如使用一个双侧带8固定在一起的。这双侧带8只由约50μm厚的粘合层构成，没有衬底，用丙烯酸粘合剂作这个粘合层。在无液体电解质电池1中，因为用于固定底面3b上所折起来的横侧面7的双侧带8的厚度是直接添加到无液体电解质电池1自身厚度上的，故它在双侧带8的厚度超过50μm时变成难以减小电池的尺寸。
在无液体电解质电池1中，可以使用一种由Cemedine公司制造的Supex X这样的粘合剂，把横侧面固定到外封装材料3的底面3b上，其镀层厚度约为50μm，可代替使用双侧带。
可用下述方法制备上述结构的无液体中解质电池1。
单元电池2的制备。
通过混合90wt％的石墨粉末和10wt％的用作粘合剂的聚(偏氟乙烯-CO-六氟丙烯)，制备负电极混合物。使所得到的物料分散于N-甲基替-2-吡咯烷酮中以形成一种浆料，然后在一个用作负电极集电器的条形铜箔的一侧上均匀地涂上一层10μm厚度的浆料，并且干燥之。使所得到的物料在轧机中模压，以形成负电极。
另一方面，制备一个正电极如下：
为了得到一种用于正电极的活性材料(LiCoO2)，以5比1的分子比混合碳酸锂和碳酸钴，然后以900℃在空气中烧5小时，再把91份重量的所产生的LiCoO2、6份重量的用作导电提供剂的石墨和10份重量的聚(偏氟乙烯-CO-六氟丙烯)混合在一起，以制备一种正电极混合物，然后把它分散于N-甲基替-2-吡咯烷酮中，以形成浆料。在一个用作正电极集电器的20μm厚度的条形铝箔的一侧上，均匀地涂复这种浆料，并且干燥之。在轧机中模压所得到的物料，以形成一个正电极。
凝胶状电解质也制备如下：
由42.5份重量的碳酸乙烯(EC)、42.5份重量的碳酸丙烯(PC)和16份重量的LiPF6构成一种增塑剂，把30份重量的这种增塑剂、10份重量的加权平均分子量为600,000的聚(偏氟乙烯-CO-六氟丙烯)和60份重量的碳酸二乙酯加以混合和溶解而得到一种溶液，然后在负和正电极上均匀地涂复这种溶液，经浸渍，并在室温下经历8小时，以挥发掉碳酸二甲酯，从而产生一种凝胶状电解质。
涂以凝胶状电解质的负和正电极是在凝胶状电解质的侧面互相面对着的情况下安置的，并且压制结合在一起，以形成一个扁平板型凝胶状电解质电池，其面积为2.5cm×4.0cm，厚度为0.3mm。
把一个铝制正电极终端引线和一个镍制负电极终端引线焊接到未涂以活性材料的电极板部分上，以制备一个单元电池2。该电极板分别是正电极和负电极上的铝箔和铜箔。
然后在外封装材料3的外壳表面3a上用深拉法形成的间隔6中，装入单元电池2。然后把外封装材料3自身折起来，使底面3b面对外壳表面3a，以闭合间隔6。然后围绕间隔6，在除3折叠侧面以外的三个侧面，把外壳表面3a和底面3b熔化在一起，以闭合外封装材料3。为修整而切除热密封部分3c外面的外封装材料的任何多余部分。
如图3A所示，通过切除多余材料而修整的无液体电解质电池1，具有在图3b中箭头指示的方向上弯曲的横侧面7。
用图4所示的弯曲模具20来弯曲横侧面7。
弯曲模具20由下列部件组成：一个架23，它在底块21上旋转地支承一个T形杠杆22；一个刀25，它在由图4中箭头D指示的方向上用一个圈簧24偏置，并且安排成可在图4中箭头C和D指示的方向上进行提升和下降移动；一个V形槽块27，它直接在刀25下用V形槽26形成；和一个导板28，它安置于V形槽块27附近，适用于引导无液体电解质电池1的设置位置。
当杠杆22在图4中箭头C指示的方向上被推动时，装在弯曲模具20上的刀25就经过一个装在刀25上的凸轮随动器29而向下推动，从而在图4中箭头C指示的方向下降。当刀25下降时，刀25的远端适配于直接在刀25下的在V形槽块27中形成的槽。使刀25的远端制成一个具有V字形两侧的基本上三角形截面形状，以适配槽26的形状。
下面说明用上述构造的弯曲模具20弯曲横侧面7。
首先，在通过弯曲模具20上导板28和V形槽块27匹配的位置，放置无液体电解质电池1。这时，无液体电解质电池1被放置得使它的一个横侧面7定位于V形槽块27的槽26上方。
然后在图4中箭头C指示的方向上，向下推动杠杆22，直至刀25变成停止。如此下降的刀25接触装于槽26上的无液体电解质电池1的横侧面7，从而推动横侧面进入槽26中。当横侧面7由刀25推入槽26内时，无液体电解质电池1就弯成一个基本上V字形状。
用弯曲模具20同样地弯曲相对的横侧面7，使无液体电解质电池1弯曲成基本上U字形状。当两个横侧面都被弯曲时，就从弯曲模具中拆卸无液体电解质电池1。
通过改变槽26和刀25的形状，可把横侧面7弯成一种期望的角度。在本优选实施例中，横侧面7用槽26和刀25变成基本上V字形状。另一方在，横侧面7可弯成在横截面7上提供一个曲率半径R。弯曲模具20具有一个槽和一个刀，槽具有横侧面7中的半径R，刀具有的远端被制成具有曲率半径R，以适应槽的形状。
然后，如图3C所示，在无液体电解质电池1的底面3b的横侧面7上，粘接两个双侧带8。
在双侧带8粘接于外封装材料3的底面3b的情况下，横侧面7被折叠，并固定于外封装材料3的底侧面3b上。
使用图6所示的固定模具30来固定横侧面7。
固定模具30包括一对旋转地装在基块31上的折叠块32，和一对支承支承轴34的支承块33，如图6和7所示。
折叠块32由装在折叠块32纵向端上的成对支承轴34旋转地支承，以便在图7中箭头E和F指示的方向转动。固定模具30通过操作员手持旋钮35来打开或闭合折叠块32之间的间隙，以便在由图7中箭头E和F指示的方向上转动支承轴34的中心。同时，固定模具30由圈簧36在图7中箭头F指示的方向上来偏置。
下面说明固定方式，其中由上述固定模具30在底面3b上固定横侧面7。
在置于固定模具30的折叠块32下的支承块33上，安置无液体电解质电池1。这时，无液体电解质电池1被设置成，使由弯曲模具20弯曲的横侧面7平放，以便沿着弯曲块32的垂直延伸侧32a延伸，如图8a所示。
然后，操作员在图7中箭头E指示的方向上转动装在折叠块32上的旋钮35，以闭合折叠块32。这时，固定模具30被设置成，使无液体电解质电池1横侧面7近端附近处位于折叠块32的转动中心G，如图8B所示。在折叠块32转动时，在折叠块32产生的推动下，在底面3b上折叠横侧面7，横侧面7被设置成沿着弯曲块32的垂直延伸侧32a延伸。
转动折叠块32，直至横侧面7接触粘合于底面3b的双侧带8为止，如图8C所示。由于横侧面7是通过双侧带8推动的，故无液体电解质电池1的横侧面7和底面3b是通过粘合到双侧带8上来固定的。
然后，在图7中箭头F指示的方向上，用偏置折叠块32的圈簧36，把折叠块32恢复到它的原始位置。从一个介于两个折叠块32之间的空间中取出无液体电解质电池1，电池1具有折叠于底面3b上和固定于此处的横侧面7。
可以在导板28、V形槽块27或在折叠块32之间距离等方面，根据无液体电解质电池1的尺寸，修改弯曲模具20和固定模具30，以便用于各种尺寸的无液体电解质电池。

Claims (9)

1.一种无液体电解质电池，其中单元电池被装于一个多层膜外封装材料内，是由深拉法用间隔形成的，并且其中电连接于单元电池各电极的电极终端引线是从外封装材料的里面引出到外面的，
其中
所述的外封装材料是在由深拉法形成的间隔周围热熔的，除了从其引出所述电极终端引线的所述外封装材料热熔部分之外，所述外封装材料的热熔部分是在其自身上折叠的。
2.根据权利要求1的无液体电解质电池，其中：
所述的外封装材料的热熔部分，除了从其引出所述电极终端引线的所述外封装材料的热熔部分之外，是在对着携带深拉法形成的所述间隔的表面的外封装材料表面上进行折叠的。
3.根据权利要求1的无液体电解质电池，其中：
外封装材料的折叠部分是用一个粘合转接带来固定的。
4.根据权利要求3的无液体电解质电池，其中：
所述的粘合转接带是一种聚丙烯粘合带。
5.一种无液体电解质电池，包括：
一个多层膜的外封装材料，它具有用于安装单元电池的间隔；
一些电极终端引线，它们从所述外封装材料的里面引出到外面，以便电连接于所述单元电池的电极；
一个热熔部分，它位于所述外封装材料的凸缘上；和
一个除了从其把所述电极终端引线引出到外面的热熔部分之外的所述热熔部分的折叠部分。
6.根据权利要求5的无液体电解质电池，其中：
所述的单元电池是用深拉法形成的。
7.根据权利要求5的无液体电解质电池，其中：
在对着携带所述间隔的侧面的外封装材料表面上折叠所述的外封装材料，所述间隔位于除了从其把所述电极终端引线引出到外面的热熔部分之外的热熔部分中。
8.根据权利要求5的无液体电解质电池，其中：所述外封装材料的折叠部分是用一个粘合转接带固定的。
9.根据权利要求8的无液体电解质电池，其中：所述的粘合转接带包括一个聚丙烯粘合层。
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