CN1695261A - 薄锂膜电池 - Google Patents
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Abstract
本发明提供一种可充电薄膜锂电池(10),该电池具有夹在两个晶化的阴极(12)之间的铝阴极集流体(11)。每个阴极具有在其上沉积的电解质(13),用锂阳极(14)覆盖该电解质。阳极集流体(15)连接阳极,并基本上包住阴极集流体、阴极、电解质和阳极。
Description
技术领域
本发明一般涉及薄膜电池,尤其涉及薄膜、可再充电的锂离子电池。
发明背景
通常来说,现有的罐型电池包括有毒材料,例如镉、汞、铅和酸性电解质。这些化学品目前正面临着政府的法令或禁令禁止作为生产原料,从而限制使用其作为电池成分。与它们相关的另一限制是由这些电池所存储和释放的能量的多少与电池的尺寸和重量直接相联系。较大的电池,例如用在汽车上的电池,产生大量的电流但能量密度(瓦时/升)和比能量(瓦时/克)却很低。正因如此,它们需要很长的再充电时间,这就致使它们在许方方面不太实用。
为了致力于满足更高的能量密度和比能量的需要,电池工业现在已朝锂基电池方向发展。电池工业的主要焦点已经集中于液体和聚合物电解质体系。但是,由于电解质溶剂的易挥发性,这些体系存在固有的安全性问题。相对于用于阳极和阴极的活性能量储存材料,这些类型电池的惰性材料组分具有比较高的比率,例如集流体、隔膜和基底。此外,它们相对高的内阻导致低的比容量(瓦/千克),多次使用后,这就致使它们在许方方面不太实用。
现已生产的薄膜锂电池具有从惰性陶瓷基底开始的膜的叠层结构,其上放置了阴极集流体和阴极。固态电解质沉积在阴极上,依次将阳极沉积在电解质上,阳极集流体放置在阳极上。典型地,在整个单元电池上提供保护层。在专利号为5,569,520和5,597,660的美国专利中详细地描述了这种类型的锂电池,这些专利所公开的内容引于此作为参考。这些电池的锂化(lithiated)阴极材料具有锂单元电池的(003)排列,如图1所示,它产生很高的电池内阻,导致大量的容量损失。
近来,已经发现在适当条件下在基底上的锂化(lithiated)阴极材料的退火引起了电池性能的显著增强,这是由于退火使得已锂化的材料晶化。这种已晶化的材料具有六边形层状结构,在这种结构中,含有Li和Co离子的交替排列平面被紧密堆积的氧层分开。现已发现通过磁电管喷射沉积在铝基底上并通过在700℃退火而晶化的LiCoO2膜具有高度的优选取向度,或者具有氧、钴和锂层结构的LiCoO2膜基本上标准地取向到基底,例如图2所示的(101)平面。由于锂平面与电流方向平行排列,这种取向是优选的,因为其提供了高的锂离子通过阴极的扩散。因为在退火过程中过度的加热产生了与下面的刚性基底表面基本平行取向的大体积应变能量,所以可以认为形成了优选取向。正如晶体的形成,它们自然地沿最小能量应变的方向生长,正如退火过程那样,由此而产生的体积应变能量促进了晶体在基本上朝着下面的基底表面的方向上生长,这也就是离子通过晶体扩散的优选取向。
然而,这些电池的局限性在于上面放置有活性材料层的基底的厚度和重量。由于基底的尺寸,这些电池在能量密度和比能量方面与其它的构型设计相比不具竞争力。未能成功地制得高能量密度的单元电池。支撑基底由比较厚的铝、刚玉、硅石玻璃和各种其它类型的陶瓷材料的薄片组成。集流体和这些电池的基底一般占几乎总重量的70%及甚至更大的体积百分比,因此只有电池重量和体积一小部分是由活性材料构成的。活性材料与电池全部重量和体积之比限制了它们的使用。
以低于600℃的退火温度,锂材料在微观结构上没有显著的变化,因此锂的取向仍是无序的,正如在the Joural of The ElectrochemicalSociety第143卷第10期由B.wang、J.B.Bates、F.X.Hart、B.C.Sales、R.A.Zuhr和J.D.Robertson所著的“具有氧化钴锂阴极的薄膜可充电锂电池的特点”(Characterization of Thin-Film Rechargeable LithiumBatleries with Lithium Cobalt Oxide Cathodes)一文中所讲述的。这种无序状态限制了锂离子通过氧和钴层的扩散,因此产生了很高的电池内阻,致使大的容量损失。
因此,为了给锂化的阴极材料退火以达到最有效取向,人们认为必须将阴极结合到刚性的基底上、以更长的时间周期加热到接近700℃。由于这样过度的加热,人们认为只有具有高熔点的特定金属才能用作阴极集流体。与这些金属相关的问题在于不能与基底材料结合,这是由于这些金属”完全不润湿”,从而在基底表面上形成小坑(pool)。这样,阴极集流体由钴构成,表面覆盖有金或铂层。在退火过程中,钴变成迁移离子(transition ion),穿过金或铂进入到阴极材料中,由此留下金或铂层作为集流体。
有人认为重量轻、低熔点的金属例如铝经受不住退火处理,因此在具有晶化阴极的薄膜锂电池中不能用作集流体。虽然这样的金属在用于锂阴极具有化学相容性,但上述观点仍是人们的普遍看法。
由此可以看出,仍然存在对高性能可充薄膜锂电池的要求,那就是希望这种电池比原有技术的更小、更轻。所以,本发明的主要目的就是提供这样的电池。
发明概要
在本发明的优选形式中,薄膜锂电池包括铝阴极集流体、沉积在铝阴极集流体上的晶化锂嵌入化合物阴极、阳极、放置在锂嵌入化合物阴极和阳极之间的电解质以及与阳极结合的阳极集流体。
附图的简要说明
图1是沿着(003)平面取向的锂嵌入化合物。
图2是沿着优选(101)平面取向的锂嵌入化合物。
图3是阐明本发明优选实施例的薄膜锂电池原理的平面图。
图4是沿着平面4-4得到的图3的薄膜锂电池的截面图。
图6是显示图3的薄膜锂电池的铝阴极集流体和锂化阴极照片的照相复制本。
发明详述
接下来参考附图,其说明在优选形式中本发明的可充电薄膜锂电池的单元电池10的实施原理。电池的单元电池10具有夹在两个阴极12之间的铝阴极集流体11。阴极12是由锂嵌入化合物构成的,最好是金属氧化物例如LiNiO2、V2O5、LixMn2O4、LiCoO2或TiS2。每个阴极12具有在其上形成的固态电解质13。电解质13最好是由锂磷氧氮化物,LixPOyNz构成。依次,每个电解质13具有在其上沉积的阳极14。当用在锂离子电池中时,阳极14最好由硅锡氧氮化物,SiTON构成,或由其它适合的材料例如锂金属、氮化锌或氮化锡构成。最后,阳极集流体16最好由铜或镍构成,将两个阳极14连接以基本上包住阴极集流体11、阴极12、电解质13和阳极14。可以以与在阴极集流体11电连接的方式设置可软焊触点16。
电池的单元电池10最好按下面的方法制造。将大约4微米厚的铝箔坯料通过等离子处理站以从金属箔上除去所有残留的油。将铝箔通过阴极Leybold室,该阴极Leybold室装备有两个大的低温泵和一系列rf或dc磁控管喷涂或二极管喷涂阴极,上述阴极在足够纯的氧气气氛中在旋转的磁鼓周围设置。喷涂阴极沉积在金属箔片的一面上约3微米厚。接下来,将铝箔翻过来以便磁控管在金属箔片的反面上沉积3微米厚的阴极。
接着将涂覆后的箔片从喷涂室移出,并分割成许多块,这些块夹在铝框架上。这些框架既在加工过程中作为用于处理材料的装置,又在材料沉积过程中作为用于提供精确的掩模对准的装置。然后将涂覆-后的箔片在约600℃下烧结约8小时以使阴极材料晶化。
接下来,通过在氮气气氛下喷涂正磷酸锂Li5PO4以生成锂磷氧氮层电解质13沉积在阴极12上。同样,通过喷涂将每个阳极14提供到相应的电解质13上。之后通过喷涂铜或镍,在阳极上沉积阳极集流体16。
人们已经发现在铝集流体上沉积并在600℃退火的晶化锂材料具有优选的(101)晶体生长平面取向,如图2所示。人们认为由于铝阴极集流体和锂嵌入化合物阴极之间在热膨胀系数上的差异,通过在晶体生成期间减少体积应变能量和增加表面能量来获得这种取向。铝阴极集流体的热膨胀系数是13.3×10-6/°F,而阴极材料(LiCoO2)的热膨胀系数是4.5×10-6/°F。在系数上的差异导致在锂嵌入材料的晶格内强度或压缩应变。这种在铝和阴极之间的体积应变能引起锂化材料的重新取向,从无序状态到结晶(101)平面。在图6中解释了锂化材料的排列,其中显示了一般朝下面的铝集流体11正规地排列的锂化阴极12,由阴极的纹理表示。这种在铝膜上600℃下的有效退火极大地提高了在电池制造过程中的效率。在铝基底上成功的退火是显著的,因为600℃的退火温度非常接近铝的熔点温度648℃。在这个温度铝几乎没有结构强度,因此以其自身的能力将所需的应变能量施加到沉积在其上的阴极材料上是非常有限的。
正如在图3和4中所示,将阴极集流体的端面露置以便电池的单元电池可以按照惯例与其它相似的单元电池以串联或者并联的方式连接。
以约为10平方厘米的表面积、约为5.4×10-2克的重量和约为14微米的厚度制备前述电池的单元电池。这种结构具有82.4毫安时的容量。以82.4毫安作为1C充电或放电速率,在以超过10C即824.0毫安的速率放电时,这些单元电池降低量低于20%。以阴极、电解质、集流体和阳极的联合质量为基准,单元电池的能量密度约为293瓦时每千克。应该注意的是单元电池没有先前在薄膜锂电池的制造过程中所要求的初始基底。现有技术的薄膜锂电池使用其它较重和较厚的基底,与之相比,这有益地减少了重量和厚度。
图5所示为本发明的锂离子电池(MLI Li-Ion)和本发明的金属锂电池MLI(Li Metal)与锂聚合物电池(Li Poly)、液体锂离子电池(LLI)、镍金属氢化物电池(NiMH)和镍镉电池(NiCd)的比较。图5的表说明了本发明的电池在能量密度(Whr/kg)上具有相当大的提高,在功率(W/kg)、体积能量密度(Whr/l)和电池充放电循环次数上显著提高。单元电池尺寸和重量的降低使电池可以在不降低容量和输出功率的条件下制造的比现有技术的电池更小、更轻。作为选择,由于单元电池的厚度降低,在电池中单元电池的数目可以提高,这样在不增加电池尺寸和重量的情况下获得比先前制造的采用下部基底的薄膜锂电池更高的容量。
可以相信铝箔可以在阴极材料沉积前预退火以限制铝箔的变形。
应理解可以采用绝缘体18例如聚对苯二甲基来填充这些部件和阳极集流体16之间的任何空间。
应理解铝箔不一定是纯铝。也可以采用某些铝合金,因此这里使用的术语铝也指铝合金。同样,铝箔可以包括由通常的喷涂方法沉积的钴或钛的薄涂层。
因此,可以看到现在提供了比现有技术的电池更轻和更小的高速率容量电池。当然可以理解,在不偏离下面的权利要求中提出的本发明的宗旨和范围的情况下可以对这里所叙述的具体优选实施例进行许多修改。
Claims (16)
1.一种薄膜锂电池,包括:
铝阴极集流体;
沉积在所述的铝阴极集流体上的晶化锂嵌入化合物;
阳极;
设置在所述的锂嵌入化合物阴极和所述的阳极之间的电解质;和
与所述的阳极结合的阳极集流体。
2.根据权利要求1的薄膜锂电池,其特征在于所述的铝阴极集流体具有钴涂层。
3.根据权利要求1的薄膜锂电池,其特征在于所述的铝阴极集流体具有钛涂层。
4.根据权利要求1的薄膜锂电池,其特征在于所述的阴极包括设置在所述的阴极集流体的相对面上的两层。
5.根据权利要求4的薄膜锂电池,其特征在于所述的电解质包括夹设有所述阴极层的两层。
6.根据权利要求5的薄膜锂电池,其特征在于所述的阳极包括夹设有所述电解质层的两层。
7.根据权利要求6的薄膜锂电池,其特征在于所述的阳极集流体包括夹设有所述电解质层的两层。
8.一种薄膜锂电池,包括:
铝阴极集流体;
夹设有所述集流体的锂嵌入化合物阴极;
覆盖所述阴极的电解质;
覆盖所述电解质的阳极;和
与所述的阳极结合的阳极集流体。
9.根据权利要求8的薄膜锂电池,其特征在于所述的阴极包括设置在所述阴极集流体相对面上的两层。
10.根据权利要求9的薄膜锂电池,其特征在于所述电解质包括夹设有所述阴极层的两层。
11.根据权利要求10的薄膜锂电池,其特征在于所述的阳极包括夹设有所述电解质层的两层。
12.根据权利要求11的薄膜锂电池,其特征在于所述的阳极集流体包括夹设有所述电解质层的两层。
13.根据权利要求8的薄膜锂电池,其特征在于所述的阴极是晶化锂嵌入化合物。
14.一种制造薄膜锂电池的方法,包括步骤:
提供铝阴极集流体;
在铝阴极集流体上沉积锂嵌入化合物;
在选定的温度下将集流体和阴极进行选定的时间期限的退火,以使集流体和阴极之间的表面应变取向于阴极晶化;
将电解质放在晶化的阴极上;
将阳极放在电解质上;以及
将阳极集流体放在阳极上。
15.根据权利要求14的制造薄膜电池的方法,其特征在于在铝阴极集流体的相对面上沉积锂嵌入化合物。
16.根据权利要求15的制造薄膜电池的方法,其特征在于电解质、阳极和阳极集流体夹设有铝集流体和阴极。
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US09/286,112 US6242129B1 (en) | 1999-04-02 | 1999-04-02 | Thin lithium film battery |
US09/286,112 | 1999-04-02 |
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US6982132B1 (en) * | 1997-10-15 | 2006-01-03 | Trustees Of Tufts College | Rechargeable thin film battery and method for making the same |
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-
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- 2000-03-31 CN CNB008070768A patent/CN100365851C/zh not_active Expired - Fee Related
- 2000-03-31 WO PCT/US2000/008576 patent/WO2000060682A1/en not_active Application Discontinuation
- 2000-03-31 MX MXPA01010004A patent/MXPA01010004A/es active IP Right Grant
- 2000-03-31 CA CA002368425A patent/CA2368425A1/en not_active Abandoned
- 2000-03-31 AU AU39315/00A patent/AU763305B2/en not_active Ceased
- 2000-03-31 NZ NZ514966A patent/NZ514966A/xx not_active IP Right Cessation
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EP1177589A1 (en) | 2002-02-06 |
ZA200108166B (en) | 2002-10-04 |
WO2000060682A1 (en) | 2000-10-12 |
CN100365851C (zh) | 2008-01-30 |
NZ514966A (en) | 2003-02-28 |
CA2368425A1 (en) | 2000-10-12 |
AU3931500A (en) | 2000-10-23 |
EP1177589A4 (en) | 2002-09-25 |
AU763305B2 (en) | 2003-07-17 |
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