CN103582966B - 二次电池用负极和具有其的二次电池 - Google Patents
二次电池用负极和具有其的二次电池 Download PDFInfo
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- 229910052751 metal Inorganic materials 0.000 claims description 19
- 239000002184 metal Substances 0.000 claims description 19
- 229910052759 nickel Inorganic materials 0.000 claims description 12
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 10
- 229910052799 carbon Inorganic materials 0.000 claims description 10
- 229910052744 lithium Inorganic materials 0.000 claims description 10
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- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 claims description 6
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- AMGQUBHHOARCQH-UHFFFAOYSA-N indium;oxotin Chemical compound [In].[Sn]=O AMGQUBHHOARCQH-UHFFFAOYSA-N 0.000 claims description 3
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- 229910002097 Lithium manganese(III,IV) oxide Inorganic materials 0.000 description 1
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- 239000004698 Polyethylene Substances 0.000 description 1
- 229910006145 SO3Li Inorganic materials 0.000 description 1
- UCKMPCXJQFINFW-UHFFFAOYSA-N Sulphide Chemical compound [S-2] UCKMPCXJQFINFW-UHFFFAOYSA-N 0.000 description 1
- BEKPOUATRPPTLV-UHFFFAOYSA-N [Li].BCl Chemical compound [Li].BCl BEKPOUATRPPTLV-UHFFFAOYSA-N 0.000 description 1
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- XGZVUEUWXADBQD-UHFFFAOYSA-L lithium carbonate Chemical compound [Li+].[Li+].[O-]C([O-])=O XGZVUEUWXADBQD-UHFFFAOYSA-L 0.000 description 1
- 229910052808 lithium carbonate Inorganic materials 0.000 description 1
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- HSZCZNFXUDYRKD-UHFFFAOYSA-M lithium iodide Inorganic materials [Li+].[I-] HSZCZNFXUDYRKD-UHFFFAOYSA-M 0.000 description 1
- MHCFAGZWMAWTNR-UHFFFAOYSA-M lithium perchlorate Chemical compound [Li+].[O-]Cl(=O)(=O)=O MHCFAGZWMAWTNR-UHFFFAOYSA-M 0.000 description 1
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- 229910021437 lithium-transition metal oxide Inorganic materials 0.000 description 1
- HSFDLPWPRRSVSM-UHFFFAOYSA-M lithium;2,2,2-trifluoroacetate Chemical compound [Li+].[O-]C(=O)C(F)(F)F HSFDLPWPRRSVSM-UHFFFAOYSA-M 0.000 description 1
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- 150000003624 transition metals Chemical class 0.000 description 1
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Abstract
本发明涉及一种二次电池用负极以及包含所述负极的二次电池,所述负极包含相互平行并螺旋扭曲的至少两个负极线,且各个负极线具有涂布在线型集电器表面上的负极活性材料层。本发明的负极具有更大的在充电和放电过程中与Li离子反应的表面积,由此提高电池的倍率特性,并还能够释放在电池中由例如活性材料层的膨胀而施加的应力或压力,以防止所述电池变形并确保其稳定性,由此提高所述电池的寿命特征。
Description
技术领域
本发明涉及适用于二次电池中的负极和包含所述负极的二次电池。
本申请要求于2011年6月2日在韩国提交的韩国专利申请10-2011-0053351号的优先权,通过参考将其完整内容并入本文中。
背景技术
二次电池为能够以化学形式储存能量并在需要时能够产生电力的装置。也将所述二次电池称作充电电池,这是因为其能够反复充电。普通的二次电池包含铅蓄电池、NiCd电池、NiMH蓄电池、Li离子电池、Li离子聚合物电池等。当与一次性原电池相比时,二次电池不仅是经济更高效的,且是环境更友好的。
目前将二次电池用于需要低电力的应用,例如用于车辆启动的设备、移动装置、工具、不间断电源等。近来,随着无线通信技术的发展导致移动器件开始普及,甚至导致多种常规器件的可移动化,对二次电池的需求急剧增加。还将二次电池用于环境友好的下一代车辆如混合动力车辆和电动车辆中,以降低成本和重量并提高车辆的寿命。
通常,二次电池具有圆柱形、棱柱形或袋形。这与二次电池的制造方法相关,其中将由负极、正极和隔膜构成的电极组件安装在圆柱形或棱柱形金属壳或铝层压片的袋形壳中,且在所述壳中填充电解质。因为在这种方法中电极组件需要预定的安装空间,所以二次电池的圆柱形、棱柱形或袋形对于各种形状的移动器件的开发是一种限制。因此,需要具有形状易于适应的新结构的二次电池。为了满足这种需要,已经提出,开发长度与横断面直径之比非常大的柔性线型二次电池,下文中称作线缆型二次电池。
然而,柔性线缆型二次电池由于其结构特征如其扭曲而频繁经历外部物理冲击,这会导致短路。此外,当将Si或Sn用作负极活性材料时,所述活性材料会因为由于重复充电和放电造成的电极的膨胀和收缩而脱落。此外,当为了提高电池容量而使用由金属制成的负极活性材料层且所述负极活性材料层厚时,锂离子难以扩散入负极活性材料层中,由此大大限制了电池容量的发挥。
发明内容
技术问题
本发明设计用于解决现有技术的问题,因此,本发明的目的是提供一种用于二次电池并具有螺旋扭曲形式的负极,所述负极能够展示良好的电化学反应性,并对电池中施加的应力和压力具有优异的抵抗性。
技术方案
为了完成上述目的,根据本发明的一个方面,提供一种二次电池用负极,包含相互平行并螺旋扭曲的至少两个负极线,各个负极线具有涂布在线型集电器表面上的负极活性材料层。
优选地,负极线的扭曲率为每一个扭曲0.01~10mm。
在本发明中,所述线型集电器可以由如下材料制成:不锈钢、铝、镍、钛、烧结碳、铜;经碳、镍、钛或银进行表面处理的不锈钢;铝-镉合金;经导电材料进行表面处理的不导电聚合物;或导电聚合物,但不能特别地限制于此。
所述导电材料可以为聚乙炔、聚苯胺、聚吡咯、聚噻吩、聚氮化硫、铟锡氧化物(ITO)、铜、银、钯或镍。
此外,所述导电聚合物可以为聚乙炔、聚苯胺、聚吡咯、聚噻吩或聚氮化硫,但不能特别地限制于此。
所述负极活性材料层可包含:金属(Me)如Si、Sn、Li、Zn、Mg、Cd、Ce、Ni和Fe;包含所述金属的合金;所述金属的氧化物;或所述金属和碳的复合材料,但不能特别地限制于此。
此外,本发明提供一种包含正极、负极和电解质的二次电池,其中所述负极为上述负极。
有益效果
根据本发明,以螺旋扭曲形式包含几股负极线的上述负极具有负极活性层,所述负极活性层比涂布有相同负极活性材料的单股负极更薄以有助于锂离子的扩散,由此提供良好的电池性能。此外,本发明的负极具有更大的表面积以在充电和放电过程中与Li离子反应,由此提高电池的倍率特性。
此外,本发明的负极具有存在于几股负极线之间的空间,所述空间能够释放在充电和放电过程中电池中由例如活性材料层的膨胀而施加的应力或压力,以防止电池变形并确保其稳定性,由此提高电池的寿命特征。
附图说明
附图显示了本发明的优选实施方案,并与上述发明内容一起,用于进一步理解本发明的技术主旨。然而,不能将本发明解释为限于这些附图。
图1是示意性显示本发明优选实施方案的负极的透视图。
图2是图1的横截面视图。
图3是显示本发明一个优选实施方案的线缆型二次电池的横截面视图。
图4是显示本发明另一个优选实施方案的线缆型二次电池的横截面视图。
图5是本发明优选实施方案的负极的照片。
图6是显示在实施例1中制备的负极的充电/放电特性的图。
图7是显示在比较例1中制备的负极的充电/放电特性的图。
图8是显示在比较例2中制备的负极的充电/放电特性的图。
具体实施方式
下文中,将参考附图对本发明的优选实施方案进行详细说明。在说明之前,应理解,不能认为说明书和附属权利要求书中使用的术语限制为普通的词典意思,而是应在本发明人对术语进行适当定义以进行最好说明的原则的基础上,根据与本发明的技术方面相对应的意思和概念对所述术语进行解释。
图1和2示意性显示了本发明一个实施方案的负极。尽管在附图中显示了本发明的几个示例性实施方案并在本文中进行了描述,所述实施方案仅用于显示目的,且不用于限制本发明的技术主旨,但是在不背离本发明的主旨和范围的条件下对其可以完成各种等价物和变体。
参考图1和2,本发明的负极100的特征在于,包含相互平行并螺旋扭曲的至少两个负极线10,各个负极线具有涂布在线型集电器11的表面上的负极活性材料层12。
本发明的负极100被构造为具有螺旋扭曲的几个负极线10,且几个负极线的扭曲没有特别限制。例如,通过将几个负极线10相互平行地并排着放置并然后将其扭曲在一起,或通过类似于编长头发的方式一个接一个地使得几个负极线10交叉,可以得到扭曲的负极线。
通常,当将由于固有性质与Li离子形成合金或脱合金而展示电化学特性的金属如Si和Sn或含这种金属的化合物用作具有高容量的负极材料时,由于膨胀而存在非常大的体积变化,这会造成二次电池劣化。这种体积变化会减弱金属活性材料之间的电接触,由此抑制Li离子迁移入负极活性材料层而造成循环劣化。此外,如果负极活性材料层以高密度的方式包含金属并具有厚的厚度,则Li离子难以扩散入负极活性材料层中,由此难以提供足够的容量和良好的倍率特性。
然而,在本发明的负极100中,其中将负极活性材料12涂布在线型集电器11表面上的几个负极线10扭曲并呈螺旋形,以提高在充放电过程中与Li离子反应的表面积,由此提高电池的倍率特性。此外,本发明的负极在几股负极线之间存在空间,所述空间在充电和放电过程中能够释放电池中施加的应力或压力如活性材料层的膨胀,以防止电池的变形并确保其稳定性,由此提高电池的寿命特征。
优选地,负极线的扭曲率为每一个扭曲0.01~10mm。通过将负极线的长度除以扭曲数得到扭曲率。扭曲率的值越低,扭曲程度越高。当扭曲率大于每一个扭曲10mm时,负极线10之间的接触面积非常小且表面积的提高不足。当扭曲率小于每一个扭曲0.01mm时,扭曲程度变得过大,造成负极线10损伤,例如负极活性材料层脱落,以及集电器断裂。
用于本发明中的线型集电器11可以由如下材料制成:不锈钢、铝、镍、钛、烧结碳、铜;经碳、镍、钛或银进行表面处理的不锈钢;铝-镉合金;经导电材料进行表面处理的不导电聚合物;或导电聚合物,但不能特别地限制于此。
所述导电材料可以为聚乙炔、聚苯胺、聚吡咯、聚噻吩、聚氮化硫、铟锡氧化物(ITO)、铜、银、钯或镍。
此外,所述导电聚合物可以为聚乙炔、聚苯胺、聚吡咯、聚噻吩或聚氮化硫,但不能特别地限制于此。
所述负极活性材料层可包含:金属(Me)如Si、Sn、Li、Zn、Mg、Cd、Ce、Ni和Fe;包含所述金属的合金;所述金属的氧化物;或所述金属和碳的复合材料。
另外,本发明的负极可以为具有可以使用电镀法或阳极氧化法在集电器表面上形成的多孔负极活性材料层的负极。在集电器表面上形成活性材料层的过程中使用电镀法,其中会产生氢气气泡。通过调节产生的氢气气泡的量和大小,可以形成具有期望孔径的三维孔结构的活性材料层。在集电器表面上形成金属氧化物类活性材料层的过程中可以使用阳极氧化法。在此情况中,通过调节在阳极氧化条件下会产生的氧气气泡的产生量和大小,可以形成一维通道状孔结构的金属氧化物类活性材料层。
将如上所述本发明的负极与正极一起使用以形成电极组件,其中引入电解质,从而制备锂二次电池。用于构成电极组件的正极和电解质可以为常规用于制备锂二次电池中的任意一种。
具体地,可以用于本发明中的负极活性材料优选为含锂的过渡金属氧化物,例如选自如下物质中的任意一种物质或其混合物:LiCoO2、LiNiO2、LiMnO2、LiMn2O4、Li(NiaCobMnc)O2(0<a<1,0<b<1,0<c<1,a+b+c=1)、LiNi1-yCoyO2、LiCo1-yMnyO2、LiNi1-yMnyO2(O≤y<1)、Li(NiaCobMnc)O4(0<a<2,0<b<2,0<c<2,a+b+c=2)、LiMn2-zNizO4、LiMn2-zCozO4(0<z<2)、LiCoPO4和LiFePO4。此外,可以使用含锂的过渡金属的硫化物、硒化物或卤化物以及含锂的过渡金属氧化物。
可以用于本发明中的所述电解质包括:聚环氧乙烷(PEO)、聚偏二氟乙烯(PVdF)、PVdF-六氟丙烯(HFP)、聚甲基丙烯酸甲酯(PMMA)、聚丙烯腈(PAN)或聚乙酸乙烯酯(PVAc)的胶凝聚合物电解质;以及PEO、聚环氧丙烷(PPO)、聚乙烯酰亚胺(PEI)、聚硫化乙烯(PES)或PVAc的固体聚合物电解质。
电解质层还可包含锂盐如LiCl、LiBr、LiI、LiClO4、LiBF4、LiB10Cl10、LiPF6、LiCF3SO3、LiCF3CO2、LiAsF6、LiSbF6、LiAlCl4、CH3SO3Li、CF3SO3Li、(CF3SO2)2NLi、氯硼烷锂、低级脂族碳酸锂和四苯基硼酸锂。
下文中,参考图3和4,对包含本发明负极的线缆型二次电池关于其具体结构进行简要说明,其中相同的参考符号表示相同或等价的组件。
参考图3,根据本发明的线缆型二次电池200具有:包含至少一个负极线210的内电极;包围所述内电极并充当离子通道的电解质层215;通过包含形成在管型集电器217内部的正极活性材料层216而包围所述电解质层215并充当正极的外电极;以及包围所述外电极的保护涂层218。
根据本发明,提供多个内电极210和管型外电极216、217以提高接触面积,由此提高电池倍率,且还可以对内电极的数量进行调节以容易地控制内电极与外电极之间的容量平衡。在这种线缆型二次电池中,优选通过使用挤出机将电极浆料挤出涂布在集电器上,从而得到具有施加到集电器217的活性材料层216的正极。此外,通过用外围的电解质电极215涂布扭曲的负极线210或通过将扭曲的负极线210插入电解质电极215中可以得到内电极。因此,通过形成内电极和电解质电极215,然后在电解质电极215的表面上形成外电极216、217和保护涂层218,可以制备线缆型二次电池。或者,通过形成包含电解质层215和保护涂层218的外电极216、217,并将内电极插入电解质层215中,或者通过形成外电极216、217和保护涂层218、插入内电极,然后填充电解质层215,可以制备线缆型二次电池。
在本发明中,将保护涂层218形成在电池外表面上,并充当绝缘体以保护电极免受空气中的水汽和外部冲击的影响。所述保护涂层可以由典型的聚合物树脂如PVC、高密度聚乙烯(HDPE)或环氧树脂制成。
另外,如图4中所示,可以以几组的方式使用根据本发明的负极线310以制备线缆型二次电池300。
下文中,通过具体实例对本发明进行详细说明。然而,本文中提出的说明只是仅用于显示目的的优选实例,不用于限制本发明的范围,从而应理解,提供所述实例是为了对本领域技术人员进行更好地说明。
实施例
实施例1:制备具有六个扭曲股的负极
在具有150μm直径的线型Cu集电器的表面上,形成具有2.5μm厚度的Sn-Ni层,以得到具有负极活性材料涂层的负极线。实施相同程序以得到总共六股负极线。将六股负极线扭曲以制备负极(如图5中所示)。
比较例1:制备具有单股的负极(负极活性材料层的厚度:2.5μm)
在具有150μm直径的线型Cu集电器表面上,形成具有2.5μm厚度的Sn-Ni层以得到具有负极活性材料涂层的负极线。
比较例2:制备具有单股的负极(负极活性材料层的厚度:5μm)
在具有150μm直径的线型Cu集电器表面上,形成具有5μm厚度的Sn-Ni层以得到具有负极活性材料涂层的负极线。
实验例
<制备硬币型半电池电池>
将锂箔用作正极,并将实施例1和比较例1和2中制备的各个负极用作负极,并将聚乙烯隔膜插入正极和负极,以得到电极组件。将电极组件插入电池壳中,向所述电池壳中引入电解质溶液以制备硬币型半电池电池,所述电解质溶液包含溶于碳酸亚乙酯和碳酸二乙酯的混合溶剂(1:2(体积比))中的1M LiPF6。
<电池充电/放电特征的评价>
在0.1C恒定电流下对使用实施例1和比较例1和2中制备的各种负极的各种电池进行充电,直至5mV,然后在5mV的恒定电压下充电,并在充电电流达到0.005C时完成各种电池的充电过程。在0.1C的恒定电流下对各种电池进行放电,直至1.5V。在相同条件下将充电/放电重复30次,然后测量各种电池的容量并示于表1和图6~8中。
表1
在电池容量方面,在比较例1和2的情况中,使用比较例1的负极的电池展示了几乎是使用比较例2的负极的电池的两倍的电池容量。这是因为比较例2的负极具有更厚的负极活性材料层和更高的密度,这使得锂离子更难以扩散入负极活性材料层中,由此劣化了锂离子的存储效率。
在比较实施例1和比较例1时,使用实施例1的负极的电池比使用比较例1的负极的电池展示了大大提高的初始效率,且还展示了良好的寿命特征。推断这是由于如下原因:实施例1中制备的具有六股负极线的负极具有薄的负极活性材料层,以及更高的表面积和存在于几股负极线之间的空间以有助于锂离子的扩散,由此提高了初始效率,此外认为,扭曲的负极线的内部结构能够释放在充电和放电过程中在电池内部由于例如活性材料层的膨胀施加的应力和压力,由此提高电池的寿命特征。
Claims (6)
1.一种线缆型二次电池,包含:
具有至少一个负极的内电极,所述负极具有包含相互平行并螺旋扭曲的至少两个负极线,各个负极线具有涂布在线型集电器表面上的负极活性材料层,所述负极具有存在于所述至少两个负极线之间的空间;
电解质层,其中以包围所述内电极的方式填充所述电解质层,且所述电解质层充当离子通道;
外电极,所述外电极包围所述电解质层的表面并充当正极,所述正极具有形成在管型集电器内部的正极活性材料层;以及
保护涂层,所述保护涂层形成在所述外电极周围。
2.如权利要求1所述的线缆型二次电池,其中所述负极线的扭曲率为每一个扭曲0.01mm~10mm,其中通过将所述负极线的长度除以扭曲数得到所述扭曲率。
3.如权利要求1所述的线缆型二次电池,其中所述线型集电器由如下材料制成:不锈钢、铝、镍、钛、烧结碳、铜;经碳、镍、钛或银进行表面处理的不锈钢;铝-镉合金;经导电材料进行表面处理的不导电聚合物;或导电聚合物。
4.如权利要求3所述的线缆型二次电池,其中所述导电材料选自如下物质:聚乙炔、聚苯胺、聚吡咯、聚噻吩、聚氮化硫、铟锡氧化物(ITO)、铜、银、钯、镍及它们的混合物。
5.如权利要求3所述的线缆型二次电池,其中所述导电聚合物选自如下物质:聚乙炔、聚苯胺、聚吡咯、聚噻吩、聚氮化硫及它们的混合物。
6.如权利要求1所述的线缆型二次电池,其中所述负极活性材料层包含选自如下物质的活性材料:金属(Me),所述金属(Me)选自Sn、Li、Zn、Mg、Cd、Ce、Ni和Fe;包含所述金属的合金;所述金属的氧化物;所述金属和碳的复合材料;Si;包含Si的合金;Si的氧化物;Si和碳的复合材料;及它们的混合物。
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