CN103828090A - 锂蓄电池 - Google Patents

锂蓄电池 Download PDF

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CN103828090A
CN103828090A CN201280033034.XA CN201280033034A CN103828090A CN 103828090 A CN103828090 A CN 103828090A CN 201280033034 A CN201280033034 A CN 201280033034A CN 103828090 A CN103828090 A CN 103828090A
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storage battery
electrode
lithium storage
lithium
collector
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CN103828090B (zh
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J·小普罗哈斯卡
J·波利夫卡
J·波斯特勒
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HE3DA sro
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Abstract

一种具有外壳的锂蓄电池，包括至少一个具有两个电极(2a，2b)的单元，所述电极设置有集流体(3a，3b)中并且由隔离物(4)分隔开，其中每个电极(2a，2b)，无需有机粘合剂地，被压制到集流体(3a，3b)的两侧上而，所述集流体由以金属网络、网状金属或打孔金属箔形式的打孔金属带制成。所述电极(2a，2b)的最小厚度是所述打孔金属带(3a，3b)的厚度的3倍。

Description

锂蓄电池
技术领域
本发明涉及一种具有外壳的锂蓄电池(accumulator)，其包括至少一个单元(cell)，所述单元包括设置有集流体且由隔离物分隔开的两个电极。
背景技术
锂电池已在过去二十年中受到大力的开发，使得许多便携式设备能够出现。对锂蓄电池的更高容量和安全性的增长需求是当前在许多应用开发中的限制因素，这些应用包括在汽车中将铅酸蓄电池更换为更高电压的锂蓄电池，或用于电动汽车的大型蓄电池。
目前生产的可充电锂蓄电池的主要部分是基于薄膜电极，其中活性材料、导电碳和有机粘合剂的混合物喷涂或层压在通常是用作集流体的铝或铜的导电材料的箔上以形成薄层。这样的平面电极的厚度范围通常从几微米到一百微米。正电极和负电极被叠置，且通过薄中间层彼此分隔开，所述薄中间层由非导电材料组成，典型地是有机聚合物的多孔箔一隔离物。由隔离物分隔开的叠置电极随后被压制，密封到壳中并且自由空间充满电解液。锂盐的非水溶液经常用于电解液。
EP1777761A2的目的提供了一个解决方案，其借助于两个隔离物层来增加薄膜平面蓄电池在较高温度下的安全性，其中一个层由电解液盐、粘合剂和有机粉末(1-40mm)构成，并且第二层包括陶瓷粉末(5-30mm)。电极的厚度只有几个微米，而其方案无法实现隔离物数量的进一步减少，因此增加了蓄电池单元的体积和容量。
US2008038638A1，JP2000090922公开了具有限定的孔隙率并且能够嵌入锂的复合基体的构造，这样的基体由能够形成锂合金的颗粒和非活性材料(共价无机化合物)构成。
PCT申请WO2010031363提出了一种锂蓄电池，包括在其中压入相互隔离的电极的壳，或布置在彼此上方的金属框架的叠置，其中每个框架包括孔，在所述孔中放置厚壁的、所谓的三维(3D)电极。极性相反的电极通过隔离物隔开，并极性相反的框架彼此绝缘。该电极具有空间分布电子导电成分，所述成分具有在电解液存在下能吸收和释放锂的均匀混合的活性材料。锂蓄电池通过连续压紧第一电极层、隔离层和第二电极来制备，由此在壳体中填充电解液，密封并且相同电极的极(pole)相互连接。较高容量的蓄电池包括夹置的电极之间的额外的集流体。所描述的电极组合物、布置及其制备方法是非常适合3D电极，这使得蓄电池实现高体积容量。然而，这个优点伴随着更长的充电时间，也伴随着蓄电池增加的体积和重量，以及由于框架的原因而减小的活性区。
发明内容
技术问题
本发明的主要目的是提供一种锂蓄电池，其结合了上述压制3D电极的优点，所述锂蓄电池包括具有降低充放电周期的电极的优点的电子导电成分和活性材料，并同时保持蓄电池单元的高容量。本发明的另一个目的是提供一种可通过压制或轧制实现有效生产的电极结构。
解决问题的方案
技术解决方案
通过锂蓄电池实现本发明的目的和克服所描述的缺点，具有外壳的所述锂蓄电池包括至少一个单元，所述单元包括设置有集流体且由隔离物分隔开的两个电极，从而每个电极，无需有机粘合剂地，被压制在集流体的两侧上，所述集流体由呈现金属网络、网形金属或打孔金属箔的形式的打孔金属带制成。不同于已知的技术，各个电极或单元不利用粘合剂而施加在金属箔上。电极被直接并且无需有机粘合剂地压入集流体的打孔金属带的孔中，而无需使用框架的系统。
在下文中，描述了根据本发明的蓄电池的其他有益实施例，其进一步更详细地发展或详细说明其必要特征，但不限制本发明的范围。
单元被紧固在通过螺栓相互连接的两个边缘盖之间。
电极的最小厚度是在打孔金属带厚度的3倍。有利的，打孔金属带的厚度为30-500μm，并打孔金属带在其一个边缘上设置有突起接触。
至少一个电极由空间分布的电子导电成分形成，所述电子导电成分与活性材料混合并且被压缩，而无需有机粘合剂，并且具有最大壁厚为10微米的中空球体形态，或最大尺寸为30微米和孔隙率从25％至95％的聚集物或团聚物。有利地，所述电子导电成分以导电可压缩碳的形式存在。这种碳变型可以被压缩以形成固体片以及在集流体-网形金属的两侧上的致密层，并且当单元被组装时能够保持期望的电极形状。
所述活性材料选自能够迅速地嵌入锂的化合物的组中，有利地，组包括锂、锰、铬、钒、钛、钴、铝、镍、铁、镧、铌、硼、铈、钽、锡、镁、钇和锆的混合氧化物或磷酸盐。这种材料优选以纳米尺寸的颗粒存在，其可以将嵌入锂工序的时间减少到几秒钟。
第二负电极可以由石墨和电子导电碳构成，并且被压制以形成电极层。
可选地，第二电极可以由锂钛氧化物或相对于锂的电势比第一电极和电子导电碳低的其他材料组成。因此，石墨可以被相对于锂的电势比阴极低的另一活性化合物取代，通常低于2V。当其导电时，使用纯净的活性材料。
隔离物优选包括具有开放型孔隙率的热解产物或无纺玻璃或陶瓷纤维的非定向形态，并且可以通过将热解产物或陶瓷无纺纤维的粉末压制成主体层来制成。隔离物的厚度范围从0.1mm到10mm，并且隔离物可以通过将粉末直接压缩到电极上而制成，或者它可以单独压制成片，通常为小片，可选地进行热处理，然后布置到电极上。
本发明的有益效果
有益效果
根据本发明的隔离物的优点是它的安全性，这是基于它的总体热稳定性和以下事实，即电极材料，不含有机粘合剂，在蓄电池充放电过程中具有显著低的电阻和小体积释放的热量。不含有机粘结剂与内部电极形态一起提供了电极内部的锂离子的高迁移性。所描述的电极结构及其材料组成可以实现蓄电池的降低的充放电周期和高体积容量，甚至当使用传统类型的隔离物时。
根据本发明的蓄电池的另一个优点在于通过压制或轧制以生产电极的可能性。该技术代替在集流体上层叠电极的相对复杂的工艺或甚至简单紧压电极材料到金属框架上。多功能边缘盖之间的各个蓄电池单元的固定提供了蓄电池的机械和耐振动性、通过盖的有效热交换、来自各个电极的最优电流收集和蓄电池的一个极的形成。
附图说明
通过参照相关示意图的示例的方式来进一步描述本发明的某些可能的实施例。在附图中：
图1是蓄电池的前剖视图；
图2示出图1中的蓄电池的电极布线系统；
图3是集流体与电极的平面图；
图3.1是集流体的详细视图；
图4是表示随着电压的台阶变化的充放电特性的曲线图；
图5是表示蓄电池的放电特性的曲线图；
图6是表示在恒定电压下蓄电池的充电特性的曲线图；
图7是表示蓄电池的循环稳定性的曲线
具体实施方式
示例1
由图1示意性剖视图的方式示出的蓄电池包括外壳10，在外壳10中各个蓄电池单元在边缘盖1a、1b之间以叠置体方式布置在彼此上方。蓄电池单元由螺栓11紧固在一起。每个单元由一个正电极2a、一个负电极2b和位于电极之间的隔离物4组成。每个正电极2a压入集流体3a并且每个负电极2b压入集流体3b。不含有机粘合剂的每个电极的材料被压入集流体中，而无需任何框架，但具有一定的突出部分以使得电极在集流体表面上方和下方延伸，以使得相对的外部电极表面之间的最小距离等于集流体3a、3b厚度的至少3倍。
蓄电池外壳10的内部空间与电极和隔离物的孔填充有电解液5。集流体3a、3b由金属网络、网状金属或打孔金属箔的带制成。集流体3a、3b的相互连接和它们各自的蓄电池极′+′和′-′在图2中呈现。
图3示出了装在电极2a中的集流体3a的示例。集流体3a由网状金属铝带制成，其在具有凸起31的一侧设置有非打孔的窄带，以形成到布线31、32的触点，以用于连接到各自的蓄电池极。相同尺寸和形状的集流体3b的网状金属条由铜制成。网状金属孔的最大尺寸的特征在于，如在图3a中详细示出的主对角线“a”为1.3mm。根据示例1的蓄电池单元的电极和隔离物的各种组合物和参数在下面的示例中进行描述。
示例2
锂蓄电池由通过隔离物4彼此分开的13个负电极2b和14个正电极2a组成。每个电极具有2×25毫米的面积，0.3至0.35毫米的厚度。正电极由重量比80％的LiFePO4(Life 
Figure BPA0000184829360000051
-P2(LFP))、进一步10wt％的电子导电碳和10wt％的在压缩时具有接合特性的导电可压缩碳的混合物构成，所述LiFePO4呈现具有约200nm的LFP颗粒的典型尺寸在2μm以下的小聚集物形态。这种类型的碳，以商品名Ketjen Black EC-300J分售，具有比表面积800m2/g，比孔体积为310-345ml/100g，团聚物尺寸主要在150nm以上和密度125-145kg/m3。另外，可以使用以商品名EC-600JD和EC-330JMA分售的碳。碳在约25kN/cm2的压力下紧压在网状铝金属集流体上，0.04毫米厚，且最大孔径尺寸′a′为1.3毫米。可替换地，可以使用以商品名EC-600JD和EC-330JMA分售的碳。
在金属带网络的一侧设置有突起31，用于电极的相互连接，并且一起形成集成的正极。压制的混合物的总量为2.8g且包括2.24g的活性LFP材料。
第二负电极由2.6g的混合物形成，所述混合物包括15wt％的电子导电碳-由Timcal公司分售的超级P-Li，以及85wt％的具有圆形聚集物形态(也是来自Timcal的Potatoe石墨)的石墨。将该混合物紧压到由0.05mm厚的具有2mm最大孔尺寸′a′的网状铜金属制成的集流体上。该网络还设置有突起31用于电极互连，并且形成集成的负极。以50％余量添加石墨。
电极通过由聚烯烃多孔箔制成的30μm厚的隔离物分隔开。具有插入的隔离物的电极被压紧在两个铝盖1a、1b之间，所述铝盖覆盖边缘正电极的极和同时整个单元的正极。
3.3V正规电压的蓄电池单元充满电解液1M LiPF6+EC/DME(1摩尔LiPF6在碳酸乙烯酯-碳酸二甲酯中)并且以受控的电势梯级进行电化学循环。图4中的图表显示了在恒定电压下的充电周期和以下面顺序的多个(4个)电势梯级的放电周期：充电3.6Và3.8Và4.1V和放电3.5Và3Và2.5Và2V。
整个蓄电池模块的比容量为280Wh/升。经过数十次循环中，当过渡层(SEI)形成在石墨表面时，该模块被完全充电，并随后通过低电阻电路放电。蓄电池容量的52％在10分钟过程中释放，而其温度升高不超过0.5C。在重复充电和低电阻电路放电时，蓄电池容量的38％在5分钟过程中释放，如图5所示。
示例3
锂蓄电池由通过隔离物4彼此分开的12个负电极2b和13个正电极2a组成。隔离物由陶瓷粉末Al2O3和玻璃纤维的混合物制得，具有80μm的厚度。正电极的活性材料是LiCo1/3Mn1/3Ni1/3O2(NMC)并且负电极的活性材料是纳米颗粒形式的Li4Ti5O12(LTS)。每个电极的面积为2×25mm，其厚度0.3-0.35mm。蓄电池模块的体积为3.25cm3及其比容量162Wh/升。
正电极由80wt％的NMC和另外20wt％的电子导电碳组成，所述NMC具有中空球形态，尺寸在40μm以下，具有5μm以下典型壁厚和250nm的平均NMC颗粒大小。该混合物如示例2中那样紧压在0.05mm厚的集流体-网状铝金属上，具有2mm的最大孔尺寸′a′。正电极的NMC材料的60％过量与LTS结合使用，当以比化学计量更少的量存在时，这能够以不会发生蓄电池过充的方式容易地控制充放电过程。紧压的混合物的总量为2.6g，包括2.08g的活性NMC材料。
负电极由2.04g混合物组成，所述混合物为21wt％的电子导电碳、20wt％的可压缩碳(Ketjen Black300J)和59wt％的纳米颗粒Li4Ti5O12。所述混合物被压制到由0.05mm厚的网状铜金属制成的具有最大孔大小′a′为2mm的集流体。集流体还设置有用于电极互连的突起31。LTS的量等于NMC容量的60％，其导致相对于333mAh的化学计量容量更小的210mAh容量。蓄电池正规电压为2.5V。
由隔离物分隔开的电极在两个铝盖1a、1b之间压紧，由此所述盖形成整个单元的正极并且同时边缘正电极的极。以电解液1M LiPF6vEC-DMC蓄电池浸泡一夜后，蓄电池单元已充满电至2.9V的恒定电压。如图6所示，900秒后单元被充电至其总容量的77％，并在1800秒后达到其总容量的96％以上。
并且，蓄电池以1800秒的间隔，在2.7V充电和在2.4V放电之间循环。电流特性的历史被显示在图7并说明了蓄电池良好的循环稳定性。
工业实用性
根据本发明的蓄电池可用于生产能够在高于100℃的高温下工作的锂蓄电池。该蓄电池适于取代在汽车工业中当今具有较高电压系统的铅酸蓄电池，适于手持电动工具和便携式电气及电子产品和设备。
权利要求书(按照条约第19条的修改)
1.一种具有外壳的锂蓄电池，包括至少一个单元、集流体(3a，3b)以及由有机溶剂中的锂盐的溶液构成的电解液，所述单元具有两个电极(2a，2b)，所述两个电极由隔离物(4)分隔开，其特征在于，每个电极(2a，2b)，无需有机粘合剂地，被压制到所述集流体(3a，3b)的两侧上，所述集流体由呈现金属网络、网状金属或打孔金属箔形式的打孔金属带制成。
2.根据权利要求1所述的锂蓄电池，其中所述单元被紧固在由螺栓(11)相互连接的两个边缘盖(1a，1b)之间。
3.根据权利要求1或2所述的锂蓄电池，其中所述电极(2a，2b)的最小厚度是所述集流体的打孔金属带(3a，3b)的厚度的3倍。
4.根据权利要求1至3中的任一项所述的锂蓄电池，其中所述打孔金属带的厚度为30-500μm，并且所述打孔金属带在其一个边缘上设置有突起(31)。
5.根据权利要求1至4中的任一项所述的锂蓄电池，其中至少一个电极(2a，2b)包括空间分布的电子导电成分，所述电子导电成分与活性材料混合并被压缩而无需有机粘合剂，并且所述电子导电成分具有壁厚最大为10微米的中空球体形态，或最大尺寸为30微米以及孔隙率从25-95％的聚集物或团聚物形态。
6.根据权利要求5所述的蓄电池，其中所述电子导电成分选自于包括以下各项的组：导电可压缩碳及其变型、导电金属、导电性氧化物、金属碳化物和氮化物。
7.根据权利要求5所述的锂蓄电池，其中所述活性材料选自于由锂、锰、铬、钒、钛、钴、铝、镍、铁、镧、铌、硼、铈、钽、锡、镁、钇和锆的混合氧化物或磷酸盐的化合物构成的组。
8.根据权利要求1至7中的任一项所述的锂蓄电池，其中所述第二负电极包括石墨和电子导电碳，并且被压制以形成电极层。
9.根据权利要求1至8中的任一项所述的锂蓄电池，其中第二负电极由锂钛氧化物或相对于锂的电势比第一电极和电子导电碳低的材料制成。
10.根据权利要求1至8中的任一项所述的锂蓄电池，其中所述隔离物选自于由纳米纤维、纤维或有机多孔箔形式的压缩的无机陶瓷材料Al2O3、SiO2、玻璃、ZrO2构成的材料组。

Claims (10)

1.一种具有外壳的锂蓄电池，包括至少一个单元，所述单元具有两个电极(2a，2b)，所述两个电极设置有集流体(3a，3b)并且由隔离物(4)分隔开，其特征在于，每个电极(2a，2b)，无需有机粘合剂地，被压制到所述集流体(3a，3b)的两侧上，所述集流体由呈现金属网络、网状金属或打孔金属箔形式的打孔金属带制成。
2.根据权利要求1所述的锂蓄电池，其中所述单元被紧固在由螺栓(11)相互连接的两个边缘盖(1a，1b)之间。
3.根据权利要求1或2所述的锂蓄电池，其中所述电极(2a，2b)的最小厚度是所述集流体的打孔金属带(3a，3b)的厚度的3倍。
4.根据权利要求1至3中的任一项所述的锂蓄电池，其中所述打孔金属带的厚度为30-500μm，并且所述打孔金属带在其一个边缘上设置有突起(31)。
5.根据权利要求1至4中的任一项所述的锂蓄电池，其中至少一个电极(2a，2b)包括空间分布的电子导电成分，所述电子导电成分与活性材料混合并被压缩而无需有机粘合剂，并且所述电子导电成分具有壁厚最大为10微米的中空球体形态，或最大尺寸为30微米以及孔隙率从25-95％的聚集物或团聚物形态。
6.根据权利要求5所述的蓄电池，其中所述电子导电成分选自于包括以下各项的组：导电可压缩碳及其变型、导电金属、导电性氧化物、金属碳化物和氮化物。
7.根据权利要求5所述的锂蓄电池，其中所述活性材料选自于由锂、锰、铬、钒、钛、钴、铝、镍、铁、镧、铌、硼、铈、钽、锡、镁、钇和锆的混合氧化物或磷酸盐的化合物构成的组。
8.根据权利要求1至7中的任一项所述的锂蓄电池，其中所述第二负电极包括石墨和电子导电碳，并且被压制以形成电极层。
9.根据权利要求1至8中的任一项所述的锂蓄电池，其中第二负电极由锂钛氧化物或相对于锂的电势比第一电极和电子导电碳低的材料制成。
10.根据权利要求1至8中的任一项所述的锂蓄电池，其中所述隔离物选自于由纳米纤维、纤维或有机多孔箔形式的压缩的无机陶瓷材料Al2O3、SiO2、玻璃、ZrO2构成的材料组。
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