CN108064423B - 用于二次电池的包括磁性材料的粘合剂 - Google Patents
用于二次电池的包括磁性材料的粘合剂 Download PDFInfo
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- CN108064423B CN108064423B CN201680035921.9A CN201680035921A CN108064423B CN 108064423 B CN108064423 B CN 108064423B CN 201680035921 A CN201680035921 A CN 201680035921A CN 108064423 B CN108064423 B CN 108064423B
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Abstract
本发明提供一种用于二次电池的粘合剂,所述粘合剂包含在电极混合物中,所述粘合剂包括:对集电器和活性材料颗粒表现出粘合力的粘合剂分子;和对从外部施加的磁场显示出磁性的磁性材料。
Description
技术领域
本发明涉及一种用于二次电池的包括磁性材料的粘合剂。本申请要求于2015年8月31日提交的韩国专利申请第10-2015-0122799号的优先权,通过引用将上述专利申请的公开内容作为整体结合在此。
背景技术
近年来,随着因化石燃料的消耗导致的能源价格的上涨以及对环境污染的关注的加剧,环境友好型替代能源已经成为未来生活不可缺少的元素。因此,对使用核电、太阳能发电、风力发电、潮汐发电等各种发电技术的研究在不断地开展,且也对用于更有效地利用如此产生的能源的电力储存装置产生了极大兴趣。
具体地说,随着移动装置的不断发展和对这种移动装置的需求增加,对作为这种移动装置的能源的二次电池的需求也急剧增加。因此,已经对满足各种需要的电池进行了很多研究。
通常,就电池的形状而言,对足够薄以应用于诸如手机之类的产品的棱柱形二次电池或袋型二次电池的需求非常之高。另一方面,就电池的材料而言,对表现出高能量密度、放电电压和输出稳定性的诸如锂离子电池和锂离子聚合物电池之类的锂二次电池的需求也非常之高。
此外,二次电池可基于电极组件的结构进行分类,电极组件具有其中堆叠有正极、负极以及插置在正极和负极之间的隔板的结构。这样的电极组件的代表性实例包括包卷型(缠绕型)电极组件和堆叠型(层压型)电极组件,在包卷型(缠绕型)电极组件中,涂覆有活性材料的长片型正极和长片型负极在隔板插置在正极和负极之间的状态下一起缠绕,在堆叠型(层压型)电极组件中,每一个都被切割成预定尺寸单元的多个正极和负极在多个隔板分别插置在正极和负极之间的状态下顺序地堆叠。近年来,为了解决包卷型电极组件和堆叠型电极组件的问题,开发了一种堆叠/折叠型电极组件,其为包卷型电极组件和堆叠型电极组件的组合,具有以下改良的结构:其中预定数量的正极和预定数量的负极在预定数量的隔板分别设置在正极和负极之间的状态下顺序地堆叠以构成单元电池,之后多个单元电池在被置于隔膜上的状态下顺序地缠绕。
此外,根据电池的形状,二次电池可分为圆柱型电池或棱柱形电池、以及袋型电池,且在圆柱型电池和棱柱形电池中,电极组件内置于圆柱型或矩形金属容器内,在袋型电池中,电极组件内置于由铝层压片制成的袋型壳体内。
具体地说,近年来,具有其中堆叠型或堆叠/折叠型电极组件内置于由铝层压片制成的袋型电池壳体内的结构的袋型电池因制造成本低、重量小、易形变等引起极大的关注,并且袋型电池的使用也在逐渐增加。
一般而言,此类二次电池是通过以下方式制备的:将包含电极活性材料、导电剂、粘合剂等的电极混合物涂覆到电极集电器上,对涂覆的集电器进行干燥以制备电极,将电极与隔板一起层压,将电极与电解质溶液一起封闭在电池壳体中,然后将壳体密封。
图1是示出用于二次电池的传统正极的制造工艺的示意图。
参照图1,正极100是通过以下工艺形成的:其中将包括正极活性材料颗粒111和粘合剂112的正极混合物110以液体状态涂覆到正极集电器120的顶表面上,然后进行干燥工艺130。
在此,在用于正极混合物110的干燥工艺130中,包含在正极混合物110中的溶剂被干燥130,粘合剂112以溶解在溶剂中的状态被包含在正极混合物110中。因此,在对溶剂进行干燥的过程中,溶解在溶剂中的粘合剂112被转移到正极混合物110的上部。
因此,相对较小量的粘合剂组分置于正极混合物110和正极集电器120之间,从而降低了正极混合物110与正极集电器120之间的粘合力,并且也增加了正极100的电阻。因此,存在以下问题:包括正极100在内的二次电池的结构稳定性和电性能下降。
此外,这些问题作为增加电极制造工艺中的不合格率的因素,降低了电极制造工艺的可靠性,使整个工艺时间延迟,从而增加了制造成本。
因此,迫切需要能够从根本上解决这样的问题的技术。
发明内容
技术问题
本发明致力于解决上述问题和现有技术遇到的技术问题。
本发明人已进行了各种广泛而深入的研究和试验,并且已经发现,由于用于二次电池的粘合剂被配置为一并包括粘合剂分子以及如后面描述的对从外部施加的磁场显示出磁性的磁性材料,因此在对涂覆到集电器的一个表面上的电极混合物的干燥工艺中,通过设置在与集电器的所述一个表面相对的表面上的磁场施加单元,来抵制包含磁性材料的粘合剂随着溶剂的干燥而转移并位于电极混合物的上方的现象,提高了电极混合物对电极集电器的粘合力,改善了电极的结构稳定性,防止了电极的电阻增加,并且防止了电极的电性能下降,降低了产品的缺陷率,从而提高了工艺的稳定性。基于这些发现完成了本发明。
技术方案
根据本发明的一个方面,通过提供如下一种用于二次电池的粘合剂能够实现上述和其他目的,所述粘合剂是包含在电极混合物中的、用于二次电池的粘合剂,所述粘合剂包括:
对集电器和活性材料颗粒表现出粘合力的粘合剂分子;和
对从外部施加的磁场显示出磁性的磁性材料。
因此,在对涂覆到集电器的一个表面上的电极混合物的干燥工艺中,通过设置在与集电器的所述一个表面相对的表面上的磁场施加单元,来抵制包含磁性材料的粘合剂随着溶剂的干燥而转移并位于电极混合物的上方的现象,提高了电极混合物对电极集电器的粘合力,改善了电极的结构稳定性,防止了电极的电阻增加,并且防止了电极的电性能下降,降低了产品的缺陷率,从而提高了工艺的稳定性。
在本发明的一个实施方式中,磁性材料可以是金属,具体为选自由Al、Mg、Ni、Co、Fe、Cr、V、Ti、Cu、Zn、Zr、Nb、Mo、Sr、Sb、W和Ti构成的组中的至少一种。
然而,磁性材料的类型并不限于此。磁性材料的类型没有特别限制,只要磁性材料对从外部施加的磁场显示出磁性并且不影响电极的性能即可。
基于粘合剂的总重量,可包含的磁性材料的量的范围为0.1重量%至20重量%。
基于粘合剂的总重量,当所包含的磁性材料的量小于0.1%时,磁性材料的含量可能会太小而达不到预期的效果。另一方面,基于粘合剂的总重量,当所包含的磁性材料的量大于20%时,相较于相同重量的电极混合物,包括电极活性材料在内的其他组分的含量太过降低,导致电极的电性能下降。
此外,磁性材料可具有化学键合至粘合剂分子的结构。
在这种情况下,磁性材料可具有以离子形式结合至粘合剂分子的结构。
此外,磁性材料可具有通过离子键、共价键或配位键结合至粘合剂分子的结构。
因此,磁性材料以强结合力结合至粘合剂分子,且结合至对从外部施加的磁场具有预定磁力的磁性材料的粘合剂分子也保持固定或朝集电器转移,从而防止混合物的粘合力下降。
具体地说,粘合剂分子可包含至少一个阴离子取代基,磁性材料可由阳离子金属组成,且该粘合剂分子和该磁性材料可具有形成螯合(chelate)键的结构。
如在此使用的,“螯合键”是指具有环状结构的化合物键,其在一个分子或离子中具有两个以上配位原子并且还被配位成如同围绕金属原子或离子。一般而言,当构成磁性材料的金属以离子形式存在时,其形成阳离子,相应地,粘合剂分子包含至少一个阴离子取代基。
因此,粘合剂分子可具有经由阴离子取代基与磁性金属离子形成螯合键的结构,因而粘合剂分子与对从外部施加的磁场显示磁性的金属一起沿着集电器的方向设置,从而表现出所期望的效果。
此外,粘合剂分子的类型没有特别限制,只要粘合剂分子能够与磁性材料化学键合并且对集电器和活性材料颗粒表现出粘合力即可。具体地说,粘合剂分子可包括选自由聚偏二氟乙烯、聚乙烯醇、羧甲基纤维素(CMC)、淀粉、羟丙基纤维素、再生纤维素、聚乙烯吡咯烷酮、四氟乙烯、聚乙烯、聚丙烯、乙烯-丙烯-二烯三元共聚物(EPDM)、磺化EPDM、丁苯橡胶、和氟橡胶、或它们的共聚物构成的组中的至少一种。
此外,本发明提供一种用于二次电池的电极混合物,所述电极混合物包括用于二次电池的粘合剂,其中所述电极混合物可以是正极混合物或负极混合物。
也就是说,根据本发明的用于二次电池的粘合剂能够应用于正极混合物和负极混合物二者,而与电极混合物的极性无关。
此外,本发明提供一种用于将电极混合物涂覆在电极集电器上的设备,所述设备包括:
传送单元,用于沿一个方向传送集电器;
电极混合物涂覆单元,用于将电极混合物涂覆到集电器的一个表面上;
干燥单元,用于对涂覆到集电器上的电极混合物进行干燥;和
磁场施加单元,用于向涂覆到集电器的一个表面上的电极混合物施加外部磁场。
在这种情况下,磁场施加单元可具有设置在与集电器的一个表面相对的另一表面处的干燥单元处、或者干燥单元和传送单元处的结构。因此,电极混合物的粘合剂可在集电器的一个表面上沿着邻近于磁场施加单元的方向设置。
如上所述,电极混合物可具有涂覆到集电器的一个表面上的结构。
因此,磁场施加单元能够设置在与集电器的一个表面相对的另一表面上,因而外部磁场可施加到电极混合物,并因此在电极混合物中所包括的粘合剂的磁性材料能够对外部磁场显示磁性。因而,可以防止包含磁性材料的粘合剂与待干燥的溶剂一起向上转移。因此,粘合剂藉由磁力在集电器的一个表面上沿着邻近于磁场施加单元的方向设置,从而能够提高电极混合物与集电器之间的粘合力。
此外,当将电极混合物涂覆到集电器的一个表面上时,粘合剂和活性材料均匀地分布,通过磁场施加单元设置在粘合剂的移动相对较容易的干燥单元中,或者设置在包括干燥单元在内的传送单元中,使得本发明的效果得以最大化。
在一个实施方式中,由磁场施加单元施加的外部磁场的强度可为0.05T(特斯拉)至100T。
当由磁场施加单元施加的外部磁场的强度远低于上述范围时,则可能不会展示出提高粘合力的期望效果。另一方面,当强度太高时,其可能会干扰电极混合物的均匀混合并且影响包含在电极混合物中的其他组分的电性能。
另一方面,本发明提供一种利用涂覆电极混合物的设备制成的电池单元。电池单元的类型没有特别限制,但电池的具体实例可包括具有诸如高能量密度、放电电压和输出稳定性之类的优异特性的诸如锂离子电池或锂离子聚合物电池等的锂二次电池。
一般而言,锂二次电池由正极、负极、隔板、和包含锂盐的非水电解质溶液组成。
正极例如通过以下方法制备:将正极活性材料、导电材料和粘合剂的混合物涂覆在正极集电器上,随后进行干燥,如果需要的话,进一步将填料添加至所述混合物。
正极活性材料的实例包括:诸如锂钴氧化物(LiCoO2)、锂镍氧化物(LiNiO2)等的层状化合物、或由一种或多种过渡金属取代的化合物;诸如Li1+xMn2-xO4(其中x为0至0.33)、LiMnO3、LiMn2O3、LiMnO2等的锂锰氧化物;锂铜氧化物(Li2CuO2);钒氧化物,诸如LiV3O8、LiFe3O4、V2O5、Cu2V2O7等;化学式为LiNi1-xMxO2(其中M=Co、Mn、Al、Cu、Fe、Mg、B或Ga,且x=0.01至0.3)的Ni-位型锂镍氧化物;化学式为LiMn2-xMxO2(其中M=Co、Ni、Fe、Cr、Zn或Ta,且x=0.01~0.1)或Li2Mn3MO8(其中M=Fe、Co、Ni、Cu或Zn)的锂锰复合氧化物;LiMn2O4,其中化学式中Li部分地被碱土金属离子取代;二硫化合物;Fe2(MoO4)3和类似物,但并不限于此。
以包含正极活性材料在内的混合物的总重量计,导电材料一般添加的量为1重量%至30重量%。所述导电材料没有特别限制,只要其具有导电性同时不会在电池中引起化学变化即可。本发明中使用的导电材料的实例包括:石墨,诸如天然石墨或人工石墨;炭黑,诸如炭黑、乙炔黑、ketjen黑、槽法炭黑、炉法炭黑、灯黑、夏黑等;导电纤维,诸如碳纤维、金属纤维等;金属粉末,诸如氟化碳、铝和镍粉等;导电晶须,诸如氧化锌、钛酸钾等;导电金属氧化物,诸如钛氧化物;诸如聚苯撑衍生物之类的导电材料;和类似物。
填料被可选地用作抑制正极膨胀的成分,且填料没有特别限制,只要其是纤维材料同时不会在电池中引起化学变化即可。填料的实例包括:烯烃基聚合物,诸如聚乙烯、聚丙烯等;和纤维材料,诸如玻璃纤维和碳纤维等。
负极通过以下方法制备:将负极活性材料涂覆在负极集电器上,随后进行干燥,如果需要的话,负极可进一步可选地包括如上所述的组分。
本发明中使用的负极活性材料的实例包括:碳,诸如非石墨化碳和石墨碳;金属复合氧化物,诸如LixFe2O3(0≤x≤1)、LixWO2(0≤x≤1)、SnxMe1-xMe’yOz(其中Me为Mn、Fe、Pb或Ge;Me’为Al、B、P、Si、元素周期表第1、2、3族元素、或卤素;0≤x≤1;1≤y≤3;1≤z≤8)等;锂金属;锂合金;硅系合金;锡系合金;金属氧化物,诸如SnO、SnO2、PbO、PbO2、Pb2O3、Pb3O4、Sb2O3、Sb2O4、Sb2O5、GeO、GeO2、Bi2O3、Bi2O4、和Bi2O5等;导电聚合物,诸如聚乙炔;Li-Co-Ni系材料;和类似物。
隔板和隔膜插置在正极和负极之间,且使用具有高离子渗透性和机械强度的绝缘薄膜。隔板的孔径和厚度一般分别为0.01μm至10μm和5μm至120μm。作为这样的隔板,例如使用由耐化学腐蚀的和疏水性的烯烃基聚合物制成的片材或无纺布、玻璃纤维、聚乙烯或类似者。当使用诸如聚合物之类的固体电解质作为电解质时,固体电解质也可充当隔板。
此外,在一个具体实例中,为了提高电池的安全性,隔板和/或隔膜可以是有机/无机复合多孔SRS(安全加强隔板)隔板。
SRS隔板是通过利用位于聚烯烃基隔板基体物质上的无机颗粒和粘合剂聚合物作为活性层成分来制备的,其中隔板具有藉由作为活性层成分的无机颗粒中的间隙体积(interstitial volume)形成的均匀的孔结构以及包含在隔板基板本身中的孔结构。
相较于使用传统隔板的情形,使用这样的有机/无机复合多孔隔板具有以下优点:可以抑制电池形成(Formation)时由于膨胀(swelling)导致的电池厚度的增加,且当在用液体电解质浸渍粘合剂聚合物组分中使用能够凝胶化的聚合物时,所述隔板可被用作电解质。
此外,由于有机/无机复合多孔隔板能够通过控制隔板中的无机颗粒和粘合剂聚合物的含量而表现出优异的粘结性能,因此能够容易地执行组装电池的工序。
无机颗粒没有特别限制,只要它们是电化学稳定的即可。也就是说,本发明中使用的无机颗粒没有特别限制,只要在应用电池的工作电压范围(例如,基于Li/Li+为0V至5V)下不发生氧化和/或还原反应即可。具体地,当使用具有离子传输能力的无机颗粒时,能够提高电化学装置中的离子导电性以改善性能,因而具有尽可能高的离子导电性的无机颗粒是优选的。此外,当无机颗粒具有高密度时,在涂覆时很难分散,且在电池生产中存在重量增加的问题。因此,优选的是无机颗粒具有尽可能小的密度。此外,在无机颗粒具有高介电常数的情形中,有助于增加电解质盐(例如液体电解质中的锂盐)的解离,从而能够提高电解质溶液的离子导电性。
含锂盐的非水电解质溶液由极性有机电解质溶液和锂盐组成。作为电解质溶液,使用非水液体电解质溶液、有机固体电解质、无机固体电解质等。
作为非水液体电解质溶液,例如,可使用以下非质子有机溶剂:N-甲基-2-吡咯烷酮、碳酸丙烯酯、碳酸乙烯酯、碳酸丁烯酯、碳酸二甲酯、碳酸二乙酯、γ-丁内酯、1,2-二甲氧基乙烷、四氢呋喃、2-甲基四氢呋喃、二甲亚砜、1,3-二氧戊环、甲酰胺、二甲基甲酰胺、二氧戊环、乙腈、硝基甲烷、甲酸甲酯、乙酸甲酯、磷酸三酯、三甲氧基甲烷、二氧戊环衍生物、环丁砜、甲基环丁砜、1,3-二甲基-2-咪唑烷酮、碳酸丙烯酯衍生物、四氢呋喃衍生物、醚、丙酸甲酯、丙酸乙酯和类似物。
作为有机固体电解质,例如,可使用以下聚合物:聚乙烯衍生物、聚环氧乙烷衍生物、聚环氧丙烷衍生物、磷酸酯聚合物、多聚赖氨酸(polyagitationlysine)、聚酯硫化物、聚乙烯醇、聚偏二氟乙烯、包括离子解离基团的聚合物和类似物。
作为无机固体电解质,例如,可使用以下化合物:锂的氮化物、卤化物和硫酸盐,诸如Li3N、LiI、Li5NI2、Li3N-LiI-LiOH、LiSiO4、LiSiO4-LiI-LiOH、Li2SiS3、Li4SiO4、Li4SiO4-LiI-LiOH、Li3PO4-Li2S-SiS2等。
锂盐可溶解于非水电解质中。作为锂盐,例如,可使用以下化合物:LiCl、LiBr、LiI、LiClO4、LiBF4、LiB10Cl10、LiPF6、LiCF3SO3、LiCF3CO2、LiAsF6、LiSbF6、LiAlCl4、CH3SO3Li、CF3SO3Li、(CF3SO2)2NLi、氯硼烷锂、低级脂族羧酸锂、四苯基硼酸锂、酰亚胺和类似物。
为了提高充电-放电特性和阻燃性,例如,非水电解质溶液可包括吡啶、亚磷酸三乙酯、三乙醇胺、环醚、乙二胺、n-乙二醇二甲醚、六磷酸三酰胺、硝基苯衍生物、硫、醌亚胺染料、N-取代的恶唑烷酮、N,N-取代的咪唑烷、乙二醇二烷基醚、铵盐、吡咯、2-甲氧基乙醇、三氯化铝和类似物。如果需要的话,在一些情况下,可进一步添加诸如四氯化碳、三氟乙烯或类似的含卤溶剂,以赋予不燃性,或者,可进一步添加二氧化碳气体,以改善高温存储特性。
本发明还提供一种包括一个或多个单元电池的装置。装置的实例包括手机、平板电脑、笔记本电脑、动力工具、可佩戴式电子装置、电动汽车、混合电动汽车、插电式混合电动汽车和电力储存装置。
由于这些装置是本领域众所周知的,因此本文将省略对它们的详细描述。
附图说明
图1是示出用于二次电池的传统正极的制造工艺的示意图。
图2是示出根据本发明的一个实施方式用于二次电池的包括粘合剂在内的正极混合物的构造的示意图。
图3是示出将图2的正极混合物涂覆在集电器上的工艺的示意图。
具体实施方式
下文中,将根据本发明的实施方式参照附图详细地描述本发明,但是本发明的范围并不限于此。
图2是示出根据本发明的一个实施方式用于二次电池的包括粘合剂在内的正极混合物的构造的示意图。
参照图2,正极混合物210包括正极活性材料颗粒211和粘合剂212。
粘合剂212包括:对集电器和正极活性材料颗粒211表现出粘合力的粘合剂分子212a;和化学键合至粘合剂分子212a的磁性材料212b。
磁性材料212b对从外部施加的磁场显示磁性,用于施加外部磁场的磁场施加单元设置在与集电器的其上涂覆正极混合物210的一个表面相对的另一表面上。因此,磁性材料212b置于涂覆有正极混合物210的集电器的朝向邻近于磁场施加单元的方向的一侧上。因此,可以防止在干燥工艺期间化学键合的粘合剂分子212a与溶剂一起沿正极混合物210的向上方向转移。
图3是示出将图2的正极混合物涂覆在集电器上的工艺的示意图。
参照图3,正极200是通过将包括正极活性材料颗粒211和粘合剂212在内的正极混合物210以液体状态涂覆在正极集电器220的顶表面上,然后对其进行干燥来制备的。
在正极混合物210的干燥工艺230中,用于施加外部磁场的磁场施加单元240位于与正极集电器220的涂覆有正极混合物210的一个表面相对的另一表面上。
因此,磁性材料212b对从磁场施加单元240施加的外部磁场显示磁性,且置于集电器220的朝向邻近于磁场施加单元240的方向的一侧上。
因此,可以防止在溶剂的干燥工艺期间化学键合至磁性材料212b的粘合剂分子212a沿正极混合物210的向上方向转移,且提高了正极混合物210对正极集电器220的粘合力。
对本领域的技术人员显而易见的是,在不脱离本发明的精神和范围的情况下,可在上述描述的基础上做出各种修改和变化。
如上所述,由于用于二次电池的粘合剂一并包括粘合剂分子以及对从外部施加的磁场显示磁性的磁性材料,因此在对涂覆到集电器的一个表面上的电极混合物的干燥工艺中,通过设置在与集电器的所述一个表面相对的表面上的磁场施加单元,来抵制包含磁性材料的粘合剂随着溶剂的干燥而转移并位于电极混合物的上方的现象,提高了电极混合物对电极集电器的粘合力,改善了电极的结构稳定性,防止了电极的电阻增加,并且防止了电极的电性能下降,降低了产品的缺陷率,从而提高了工艺的稳定性。
Claims (7)
1.一种用于二次电池的粘合剂,所述粘合剂包含在电极混合物中,所述粘合剂包括:
对集电器和活性材料颗粒表现出粘合力的粘合剂分子;和
对从外部施加的磁场显示出磁性的磁性材料,
其中所述磁性材料为金属阳离子,所述金属选自由Al、Mg、Ni、Co、Fe、Cr、V、Cu、Zn、Zr、Nb、Mo、Sr、Sb、W和Ti构成的组中的至少一种;
其中所述磁性材料是化学键合至所述粘合剂分子,其中所述粘合剂分子和所述磁性材料形成螯合键。
2.根据权利要求1所述的用于二次电池的粘合剂,其中,所述磁性材料以基于所述粘合剂的总重量的0.1重量%至20重量%的量被包含。
3.根据权利要求1所述的用于二次电池的粘合剂,其中所述粘合剂分子选自由聚偏二氟乙烯、聚乙烯醇、羧甲基纤维素(CMC)、淀粉、羟丙基纤维素、再生纤维素、聚乙烯吡咯烷酮、四氟乙烯、聚乙烯、聚丙烯、乙烯-丙烯-二烯三元共聚物(EPDM)、磺化EPDM、丁苯橡胶和氟橡胶或它们的共聚物构成的组中的至少一种。
4.一种用于二次电池的电极混合物,包括根据权利要求1所述的用于二次电池的粘合剂。
5.根据权利要求4所述的用于二次电池的电极混合物,其中所述电极混合物是正极混合物或负极混合物。
6.一种用于二次电池的电极,所述电极包括集电器和权利要求4所述的用于二次电池的电极混合物,其中所述的用于二次电池的电极混合物是被涂覆在所述集电器的表面上,并且所述粘合剂的所述磁性材料置于在所述电极混合物的涂层内、与涂覆有所述电极混合物的所述集电器的所述表面相邻。
7.一种二次电池,所述二次电池包括权利要求6所述用于二次电池的电极。
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