CN1210821C - 用于高能充电锂电池的隔板 - Google Patents

用于高能充电锂电池的隔板 Download PDF

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CN1210821C
CN1210821C CNB011163534A CN01116353A CN1210821C CN 1210821 C CN1210821 C CN 1210821C CN B011163534 A CNB011163534 A CN B011163534A CN 01116353 A CN01116353 A CN 01116353A CN 1210821 C CN1210821 C CN 1210821C
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Abstract

本发明涉及高能充电锂电池的隔板和相应的电池。该隔板包括陶瓷复合材料层和聚合物微孔层。陶瓷复合材料层包括无机颗粒和基质材料的混合物。陶瓷复合材料层适于至少阻挡枝晶生长并防止电子短路。聚合物层适于至少在热失控上升的情况下阻挡阳极和阴极之间的离子流动。

Description

用于高能充电锂电池的隔板
技术领域
在此披露了一种用于高能充电锂电池的隔板和高能充电锂电池。
背景技术
高能充电锂电池具有能量容量至少372毫安时/克(mAh/g)的阳极。该阳极包括例如锂金属、锂合金(如锂铝)、和锂金属或锂合金与如碳、镍和铜的材料的混合物。该阳极排除只具有锂嵌入或锂插入化合物的阳极。
由于长效安全问题，除一次电池外不能取得其它锂金属或锂合金电池的商业成功。
与使用上述阳极相关的困难主要源于重复充电-放电循环后发生的锂枝晶生长。(虽然枝晶生长对任何锂电池都是潜在问题，但对上述高能阳极来说，该问题的严重性远大于本领域公知的其它锂阳极(例如纯碳嵌入型阳极))。当锂枝晶生长并穿透隔板时，电池内部短路出现(阳极和阴极之间的任何直接接触都称为“电子”短路，并且由枝晶产生的接触是一种电子短路)。由很小的枝晶导致的一些短路(即软短路)可能仅仅降低电池的循环效率。其它短路可能导致锂电池的热失控上升，即充电锂电池的严重安全问题。
不能控制这类阳极的枝晶生长仍然是一问题，限制了具有那些阳极的电池，特别是具有液体有机电解质的那些电池的商业化。
因此，必须改进高能充电锂电池。
发明内容
本发明涉及高能充电锂电池的隔板和相应的电池。该隔板包括至少一个陶瓷复合材料层和至少一个聚合多孔层。陶瓷复合材料层包括无机颗粒和基质材料的混合物。使该陶瓷复合材料层至少适于阻挡枝晶生长并防止电子短路。使聚合物层，至少适于在热失控上升的情况下阻挡阳极和阴极之间的离子流动。
在一个技术方案中，本发明提供一种用于高能充电锂电池的隔板，包括：至少一个陶瓷复合材料层，所述陶瓷复合材料层包括无机颗粒和基质材料的混合物；所述陶瓷复合材料层至少阻挡枝晶生长并防止电子短路；和至少一个不含颗粒的聚合物微孔层，所述微孔层阻挡阳极和阴极之间的离子流动。
在又一个技术方案中，本发明提供一种用于高能充电锂电池的隔板，包括：至少一个陶瓷复合材料层或涂层，所述陶瓷复合材料层或涂层包括从SiO2、Al2O3、CaCO3、TiO2、SiS2、SiPO4和它们的混合物构成的组中选择的20-95wt％无机颗粒和从聚环氧乙烷、聚偏氟乙烯、聚四氟乙烯、它们的共聚物和它们的混合物构成的组中选择的5-80wt％基质材料的混合物；以及至少一个不含颗粒的聚烯烃微孔层，所述聚烯烃微孔层具有20-80％的孔隙率、在0.02-2微米范围内的平均孔径、以及在15-150秒范围内的Gurley Number，该Gurley number是在12.2英寸水压下使10cc空气通过1平方英寸材料所需的以秒计的时间。
在另一个技术方案中，本发明提供一种高能充电锂电池，包括：包含锂金属或锂合金、或锂金属和/或锂合金和另一种材料的混合物的阳极；阴极；位于所述阳极和所述阴极之间的根据权利要求1-10的隔板；以及经过所述隔板与所述阳极和所述阴极离子导通的电解质。
在另一个技术方案中，本发明提供一种用于能量存储系统的隔板，包括：至少一个陶瓷复合材料层或涂层，所述陶瓷复合材料层或涂层包括从SiO2、Al2O3、CaCO3、TiO2、SiS2、SiPO4和它们的混合物构成的组中选择的20-95wt％无机颗粒和从聚环氧乙烷、聚偏氟乙烯、聚四氟乙烯、它们的共聚物和它们的混合物构成的组中选择的5-80wt％基质材料的混合物，所述陶瓷复合材料层或涂层至少阻挡枝晶生长并防止电子短路；以及至少一个不含颗粒的聚烯烃微孔层，所述聚烯烃微孔层具有20-80％的孔隙率、在0.02-2微米范围内的平均孔径、以及在15-150秒范围内的Gurley Number，所述微孔层阻挡阳极和阴极之间的离子流动，其中所述Gurley number是在12.2英寸水压下使10cc空气通过1平方英寸材料所需的以秒计的时间。
附图说明
为示意说明本发明，在附图中示出目前的优选形式，然而，应当理解本发明不限于所示的精确布置和方式。
图1是锂金属电池的横截面图。
图2是隔板的横截面图。
具体实施方式
参照附图，其中相同的数字表示相同的部件，图1中示出了锂金属电池10。锂金属电池10包括锂金属阳极12、阴极14、和位于阳极12和阴极14之间的隔板16，它们全部装在外壳20内。所示电池10是圆柱形电池或“胶卷”形电池，但本发明不限于此。其它结构，例如还包括棱柱形电池、钮扣电池或聚合物电池。此外，没有示出电解质。电解质可以是液体(有机或无机)、或凝胶(或聚合物)。为方便起见，参照具有液体有机电解质的圆柱形电池描述本发明，但本发明不限于此，并可以在其它电池类型(例如能量存储系统、组合电池和电容器)和结构中使用。
阳极12的能量容量应当大于或等于372mAh/g，优选≥700mAh/g，最好≥1000mAh/g。阳极12可由锂金属箔或锂合金箔(例如锂铝合金)、或锂金属和/或锂合金与如碳(例如焦碳、石墨)、镍、铜的材料的混合物构成。阳极12不是仅仅由含锂的嵌入化合物或含锂的插入化合物构成。
阴极14可以是与阳极匹配的任何阴极并且包括嵌入化合物、插入化合物或电化学活性聚合物。适当的嵌入材料包括例如MoS2、FeS2、MnO2、TiS2、NbSe3、LiCoO2、LiNiO2、LiMn2O4、V6O13、V2O5和CuCl2。适当的聚合物包括例如聚乙炔、聚吡咯、聚苯胺和聚噻吩(polythiopene)。
电解质可以是液体或凝胶(或聚合物)。通常，电解质基本由盐和介质(例如在液体电解质中，介质称为溶剂；在胶体电解质中，介质可以是聚合物基质)构成。盐可以是锂盐。锂盐可以包括例如LiPF6、LiAsF6、LiCF3SO3、LiN(CF3SO3)3、LiBF6和LiClO4、BETTE电解质(从3MCorp.of Minneapolis，MN购买)和它们的组合物。溶剂可以包括例如碳酸亚乙酯(EC)、碳酸亚丙酯(PC)、EC/PC、2-MeTHF(2-甲基四氢呋喃)/EC/PC、EC/DMC(碳酸二甲酯)、EC/DME(二甲基乙烷)、EC/DEC(碳酸二乙酯)、EC/EMC(碳酸甲乙酯)、EC/EMC/DMC/DEC、EC/EMC/DMC/DEC/PE、PC/DME和DME/PC。聚合物基质包括例如PVDF(聚偏氟乙烯)、PVDF:THF(PVDF:四氢呋喃)、PVDF:CTFE(PVDF:三氟氯乙烯)PAN(聚丙烯腈)、和PEO(聚环氧乙烷)。
参照图2，示出隔板16。隔板16包括陶瓷复合材料层22和聚合物多孔层24。陶瓷复合材料层至少适用于防止电子短路(例如，阳极和阴极的直接或物理接触)并阻挡枝晶生长。聚合物多孔层在热失控上升的情况下至少适用于阻挡(或断开)阳极和阴极之间的离子传导(或流动)。隔板16的陶瓷复合材料层22必须有足够的传导性以实现阳极和阴极之间离子流动，这样电池能产生所需大小的电流。层22和24应当很好地相互粘合在一起，即不出现分离。层22和24由层压、共挤压、或涂覆工艺形成，陶瓷复合材料层22可以是涂层或单独的层，其厚度范围从0.001微米-50微米，优选在0.01微米-25微米的范围内。聚合物多孔层24优选是不连续的膜，具有5微米-50微米范围的厚度，优选厚度在12微米-25微米的范围内。隔板16的总厚度在5-100微米的范围内，优选在12-50微米的范围内。
陶瓷复合材料层22包括其中分散有无机颗粒28的基质材料26。陶瓷复合材料层22是无孔的(应当明白，一旦与电解质接触，可能会形成一些孔，但层22的离子传导率主要取决于基质材料26和颗粒28的选择)。层22的基质材料26至少在功能方面不同于上述聚合物基质(即，如上所讨论过的电解质的介质)。即，基质材料26是通过防止枝晶生长来部分防止电子短路的隔板组分；反之，聚合物基质限于载有解离盐的介质，利用该盐发生电池内导电。此外，基质材料26还与上述聚合物基质执行相同功能(例如携带电解质盐)。基质材料26包括约5-80wt％的陶瓷复合材料层22，并且无机颗粒28构成层22的约20-95wt％。优选地，复合层22包含30-75wt％的无机颗粒。最优选地，复合层22包含40-60wt％的无机颗粒。
基质材料26可以是离子传导的或非离子传导的，因此能使用用于锂聚合物电池或固体电解质电池中的任何凝胶形式的聚合物。基质材料26可以从例如聚环氧乙烷(PEO)、聚偏氟乙烯(PVDF)、聚四氟乙烯(PTFE)、聚氨酯、聚丙烯腈(PAN)、聚甲基丙烯酸甲酯(PMMA)、聚四甘醇二丙烯酸酯(polytetraethylene glycol diacrylate)、其共聚物和其混合物中选择。优选的基质材料是PVDF和/或PEO和它们的共聚物。PVDF共聚物包括PVDF:HFP(聚偏氟乙烯:六氟丙烯)和PVDF:CTFE(聚偏氟乙烯:三氟氯乙烯)。最优选的基质材料包括具有少于23wt％CTFE的PVDH:CTFE，少于28wt％HFP的PVDH:HFP，任何种类的PEO，和它们的混合物。
通常认为无机颗粒28是不导电的，然而，当这些颗粒与电解质接触时，似乎产生改进隔板16传导性(降低电阻)的超导表面，然而本发明人不希望局限于此。无机颗粒28可以从例如二氧化硅(SiO2)、氧化铝(Al2O3)、碳酸钙(CaCO3)、二氧化钛(TiO2)、SiS2、SiPO4等、或它们的混合物中选择。优选的无机颗粒是SiO2、Al2O3和CaCO3。该颗粒的平均粒径在0.001微米-25微米的范围内，最好在0.01微米-2微米的范围内。
微孔聚合物层24由任何市售微孔膜(例如单层或多层)构成，例如，由Celgard Inc.of Charlotte，North Carolina，Asahi Chemical ofTokyo，Japan和Tonen of Tokyo，Japan制造的产品。层24的孔隙率在20-80％的范围内，优选在28-60％的范围内。层24的平均孔径在0.02-2微米的范围内，优选在0.08-0.5微米的范围内。层24的Gurley Number在15-150秒的范围内，最好在30-80秒。(Gurley Number指在12.2英寸水压下10cc空气通过1平方英寸材料(隔膜)的时间(秒)。)层24优选是聚烯烃类的。优选的聚烯烃包括聚乙烯和聚丙烯。聚乙烯是最适宜的。
主要为在高能充电锂电池中使用而设计的上述隔板可以用于其它有枝晶生长问题的电池系统。
将根据下面非限定性例子进一步描述上述情况。
                         例子
把60份碳酸钙细颗粒、40份PVDF:HFP(Kynar2801)在35℃下溶解在100份丙酮中，高剪切混合3小时。把溶液浇铸成15微米膜。在室温下丙酮蒸发后，把该复合膜与2层(8微米)Celgard2801膜热层压。所得复合截止隔板具有PE/复合膜/PE的结构并且厚度为30微米。
把30份二氧化硅、30份碳酸钙、40份PVDF:HFP(Kynar2801)在35℃下溶解在100份丙酮中，高剪切混合3小时。把该溶液浇注或涂覆在Celgard Inc.制造的23微米聚乙烯微孔层上。在室温下丙酮蒸发后，聚乙烯/复合膜具有38微米的厚度。
在不脱离本发明精神或实质特点的情况下，能以其它形式实施本发明，因此参照附属权利要求而非上述说明书，作为指示本发明的范围。

Claims (12)

1.一种用于高能充电锂电池的隔板，包括：
至少一个陶瓷复合材料层，所述陶瓷复合材料层包括无机颗粒和基质材料的混合物；所述陶瓷复合材料层至少阻挡枝晶生长并防止电子短路；和
至少一个不含颗粒的聚合物微孔膜层，所述微孔膜层在热失控时阻挡阳极和阴极之间的离子流动。
2.根据权利要求1的隔板，其中所述混合物包括20wt％-95wt％的所述无机颗粒和5wt％-80wt％的所述基质材料。
3.根据权利要求1的隔板，其中所述无机颗粒从SiO2、Al2O3、CaCO3、TiO2、SiS2、SiPO4和它们的混合物构成的组中选择。
4.根据权利要求1的隔板，其中所述基质材料从聚环氧乙烷、聚偏氟乙烯、聚四氟乙烯、聚氨酯、聚丙烯腈、聚甲基丙烯酸甲酯、聚四甘醇二丙烯酸酯、它们的共聚物和它们的混合物构成的组中选择。
5.根据权利要求1的隔板，其中所述聚合物微孔层是聚烯烃膜。
6.根据权利要求5的隔板，其中所述聚烯烃膜是聚乙烯膜。
7.一种用于能量存储系统的隔板，包括：
至少一个陶瓷复合材料层或涂层，所述陶瓷复合材料层或涂层包括从SiO2、Al2O3、CaCO3、TiO2、SiS2、SiPO4和它们的混合物构成的组中选择的20-95wt％无机颗粒和从聚环氧乙烷、聚偏氟乙烯、聚四氟乙烯、它们的共聚物和它们的混合物构成的组中选择的5-80wt％基质材料的混合物；以及
至少一个不含颗粒的聚烯烃微孔膜层，所述聚烯烃微孔膜层具有20-80％的孔隙率、在0.02-2微米范围内的平均孔径、以及在15-150秒范围内的Gurley Number，该Gurley number是在12.2英寸水压下使10cc空气通过1平方英寸材料所需的以秒计的时间。
8.根据权利要求7的隔板，其中所述无机颗粒具有在0.001-24微米范围内的平均粒径。
9.根据权利要求7的隔板，其中所述无机颗粒从SiO2、Al2O3、CaCO3、和它们的混合物构成的组中选择。
10.根据权利要求7的隔板，其中所述基质材料从聚偏氟乙烯和/或聚环氧乙烷、它们的共聚物、和它们的混合物构成的组中选择。
11.一种高能充电锂电池，包括：
包含锂金属或锂合金、或锂金属和/或锂合金和另一种材料的混合物的阳极；
阴极；
位于所述阳极和所述阴极之间的根据权利要求1-10中任一项的隔板；以及
经过所述隔板与所述阳极和所述阴极离子导通的电解质。
12.根据权利要求7的隔板，包括：
至少一个陶瓷复合材料层或涂层，所述陶瓷复合材料层或涂层包括从SiO2、Al2O3、CaCO3、TiO2、SiS2、SiPO4和它们的混合物构成的组中选择的20-95wt％无机颗粒和从聚环氧乙烷、聚偏氟乙烯、聚四氟乙烯、它们的共聚物和它们的混合物构成的组中选择的5-80wt％基质材料的混合物，所述陶瓷复合材料层或涂层至少阻挡枝晶生长并防止电子短路；以及
至少一个不含颗粒的聚烯烃微孔膜层，所述聚烯烃微孔膜层具有20-80％的孔隙率、在0.02-2微米范围内的平均孔径、以及在15-150秒范围内的Gurley Number，所述微孔层在热失控时阻挡阳极和阴极之间的离子流动，其中所述Gurley number是在12.2英寸水压下使10cc空气通过1平方英寸材料所需的以秒计的时间。
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CN106159160A (zh) * 2010-12-08 2016-11-23 索尼公司 层压微孔膜、电池隔膜和非水电解质电池
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CN103579564B (zh) * 2013-11-18 2016-02-10 番禺南沙殷田化工有限公司 一种陶瓷隔膜及其制备方法和应用

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CN1325145A (zh) 2001-12-05
TW507392B (en) 2002-10-21
KR20100038350A (ko) 2010-04-14
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US6432586B1 (en) 2002-08-13
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