CN101032043A - 非水电解质电池用引线和非水电解质电池 - Google Patents
非水电解质电池用引线和非水电解质电池 Download PDFInfo
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- XJUNLJFOHNHSAR-UHFFFAOYSA-J zirconium(4+);dicarbonate Chemical compound [Zr+4].[O-]C([O-])=O.[O-]C([O-])=O XJUNLJFOHNHSAR-UHFFFAOYSA-J 0.000 description 1
- LEHFSLREWWMLPU-UHFFFAOYSA-B zirconium(4+);tetraphosphate Chemical compound [Zr+4].[Zr+4].[Zr+4].[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O LEHFSLREWWMLPU-UHFFFAOYSA-B 0.000 description 1
- GFQYVLUOOAAOGM-UHFFFAOYSA-N zirconium(iv) silicate Chemical compound [Zr+4].[O-][Si]([O-])([O-])[O-] GFQYVLUOOAAOGM-UHFFFAOYSA-N 0.000 description 1
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Abstract
本发明提供非水电解质电池和引线,它们用无铬表面处理处理过并具有优良的耐氢氟酸性能。该引线包括(1)由镍、镀镍铜或铜制成的引线的金属部分;(2)复合涂层,其是在所述引线的金属部分的表面上所述封装体被密封粘着的部分处,通过涂布包含锆盐、钛盐或钼盐和包含聚丙烯酸的树脂组分的处理液体而形成的;和(3)布置在所述复合涂层外部并被封装体密封粘着的绝缘体。该非水电解质电池包括:由包含金属箔的层压膜制成的封装体;封装在封装体中的正极、负极和电解质溶液;和本发明的引线,其分别连接正极和负极并被布置为引出到封装体外部。
Description
技术领域
本发明涉及非水电解质电池用引线(lead),所述电池具有封装正极、负极和电解质溶液的封装体(package),所述引线与每个电极连接并从封装体引出到外部。本发明也涉及具有这种引线的非水电解质电池。
背景技术
随着电子器件的尺寸变得更小,也需要尺寸更小和重量更轻的电池用作所述电子器件的电源。而且,还需要更高能量密度和更高能量效率的电池。愈加希望锂离子电池和其它非水电解质电池满足这样的需求。日本专利3505905公开了一种非水电解质电池,其中正极、负极和电解质溶液封装在例如袋状封装体中,该袋状封装体由包含金属箔的层压膜和与电极连接并引出到封装体外部的引线制成。
与正极或负极连接的每个引线在连接至封装体的部分具有覆盖它的绝缘体,以防止引线和层压膜的金属箔之间电短路。同样,在这些部分处,引线被熔接到通过熔接层压膜而形成的封装体的边缘部分的规定位置上,从而该引线引出到封装体外部,同时保持封装体的密封状态。
用于覆盖每个引线的绝缘体由两层构成:内绝缘层和外绝缘层,外绝缘层的熔点比内绝缘层高,并且在热封(heat seal)层压膜的温度不会熔融。通过加热和熔融内绝缘层,使绝缘体在每个引线连接到封装体的部分处与每个引线的金属部分(metal portion of a lead)结合。将具有绝缘体的引线布置在封装体的引线通道部分上,从而将绝缘体置于层压膜的边缘的密封部分上。然后,通过热封来密封层压膜的边缘。绝缘体的外绝缘层在进行热封的温度不会熔融。因此,引线的金属部分在热封期间不会经由绝缘体而暴露出来。结果,引线的金属部分和层压膜内侧的金属箔之间不会发生电短路。所述引线的金属部分由铝、镍(包括镀镍)或铜制成。
但是,如果层压膜的密封部分和引线与封装体连接的部分处的引线之间的密封粘合不充分,水分将从外部渗透到电池的内部并与电池内部的电解质酸反应,由此产生氢氟酸。在这种情况下,即使引线的金属部分的表面在封装体的引线通道部分上被绝缘体密封的,引线的金属部分的表面也将在长时间内逐渐被氢氟酸侵蚀,并且引线的金属部分上被绝缘体密封的部分将会崩溃。结果,封装体的密封性将被降级,并且会降低电池特性。
如日本专利申请公开2002-216741中所示,解决此问题的方法之一是用化学转化层(chemical conversion layer)覆盖引线的金属部分表面上被绝缘体密封的部分。日本专利申请公开2002-216741公开了典型的铬酸盐磷酸盐处理,其中使用包含磷酸盐的铬酸水溶液化学地产生涂层。它也公开了通过将引线浸在化学转化溶液中在引线上形成化学转化涂层,该化学转化溶液包括酚醛树脂的树脂,以及金属盐,例如钛盐、锆盐(zircon)或其它金属盐。以此方式,作为用于赋予耐氢氟酸性能的化学转化处理,基于铬的化学转化处理是有效的,并且已经被用于许多不同的领域。但是,由于对环境污染的考虑,在各个领域中正开发无铬化学转化处理。可以预期,将来会需要开发完全无铬的化学转化处理。
在非水电解质电池用引线领域之外的领域中,尝试过多次用包含金属如锆系和钛系的金属代替铬作为制造涂层的物质的实际应用。也尝试过使用这种盐和聚丙烯酸的混合物作为制造涂层的材料。据报道(基于2003年3月28日JPO网站主页上的文章),这种涂层当施涂在铝上时具有满意的粘合特性,并且从抗腐蚀性的观点来看也是有效的。
专利文献1:日本专利3505905
专利文献1:日本专利申请公开2002-216741
发明内容
本发明所要解决的问题
本发明的目的是提供非水电解质电池和引线,它们用无铬表面处液处理过的并具有优良的耐氢氟酸性能。
解决问题的方法
为了获得该目的,提供非水电解质电池用引线,其中正极、负极和电解质溶液封装在封装体中,该封装体由包含金属箔的层压膜制成。该引线包括:(1)由镍、镀镍铜(nickel plated copper)或铜制成的引线的金属部分;(2)复合涂层,其是在所述引线的金属部分的表面上所述封装体被密封粘着的部分处,通过涂布包含锆盐、钛盐或钼盐和包含聚丙烯酸的树脂组分的处理液体而形成的;和(3)布置在所述复合涂层外部并被封装体密封粘着的绝缘体。本发明也提供非水电解质电池,其具有:由包含金属箔的层压膜制成的封装体;封装在封装体中的正极、负极和电解质溶液;和本发明的引线,其分别连接正极和负极并被布置为引出到封装体外部。
发明效果
本发明使得可在引线表面上形成不包含六价铬(铬VI)或三价铬(铬III)的复合涂层,所述六价铬是已知的环境污染物质,所述三价铬的使用在将来将可能被限制。通过形成这种复合涂层,能够密封引线,从而具有优良的耐氢氟酸性能。而且,能够实现不泄漏并因此具有稳定特性和长期使用寿命的非水电解质电池。
附图说明
图1是本发明的非水电解质电池的实施方式的透视图。
图2说明图1中所示的非水电解质电池和引线。图2A是横截面图,图2B是沿着图2A的切线a-a的横截面图,和图2C是沿着图2A的切线b-b的横截面图。
附图标记说明
1---引线、2---引线的金属部分、3---封装体、3a---密封部分、4---层压膜、4a---金属箔、5---复合涂层、6---绝缘体、7---粘合层、8---绝缘层、9---正极、9’---负极、10---隔膜(separator)、11,11’---电极导体、12、12’---活性物质层
具体实施方式
下面将参考附图描述本发明的实施方式。出于说明本发明的目的而提供附图,并非限制本发明的范围。附图中,为了避免重复解释,相同的部件用相同的附图标记表示。附图并非必需按照比例绘制。
图1是本发明的非水电解质电池的实施方式的透视图。此非水电解质电池是薄型电池。将一对引线1布置成经过封装体3的密封部分3a引出到封装体外部,所述一对引线1中的每一根均由引线的金属部分2和绝缘体6构成,所述绝缘体6在引线1连接到封装体3的部分上覆盖所述引线的金属部分2。封装体3是袋状部件,其是通过热熔接所述封装体3的边缘形成所述密封部分3c而获得的。将单个电化学电池(eletrochemical cell)密封地封入封装体3中,所述电化学电池包括正极、负极、隔膜和包含溶解在非水溶剂(例如有机溶剂)中的电解质(例如锂化合物)的非水电解质溶液。
在层压膜4被密封粘着的至少部分表面上,对引线的金属部分2进行化学转化处理,形成复合涂层5,并且用绝缘体6覆盖绝缘复合涂层5的外表面。在绝缘体6的外表面上密封粘着层压膜4。
图2是说明图1中所示的非水电解质电池和引线的视图。图2A是在与非水电解质电池的厚度方向相垂直的方向上观察的非水电解质电池的横截面图。封装体3由层压膜4制成,层压膜4包含位于树脂膜内的金属箔4a。更具体地,层压膜4包括内层膜、外层膜和夹在内层膜和外层膜之间的金属箔4a,由此增加对封装在封装体3中的电解质溶液的密封性质,所述金属箔4a由铝、铜、不锈钢或其它金属制成。
层压膜4可以是由3~5层制成的层压材料。层压膜4的最内层(innermostlayer)由不溶于电解质溶液并且防止电解质溶液通过密封部分泄漏的材料,例如酸改性的聚烯烃(例如马来酸酐改性的聚乙烯)制成。最外膜层由保护内部金属箔4a不受外部损害的材料,例如聚对苯二甲酸乙二酯制成。
封装在封装体3内部的电解液是溶于有机溶剂中的LiClO4、LiBF4、LiPF6、LiAsF6或其它材料的非水电解质溶液,该有机溶剂例如碳酸亚丙酯(propylene carbonate)、碳酸亚乙酯(ethylene carbonate)、碳酸二乙酯、碳酸二甲酯、1,2-二甲氧基乙烷或四氢呋喃。该电解质也可以是锂离子导电性的固体电解质。
每个电极包括称为“集电体”的金属基材和设置在该基材上的活性物质层,该金属基材由金属箔或多孔金属网(expanded metal)制成。更具体地,正极9包括铝电极导体11和活性物质层12,该活性物质层12由还原的氧化物粉末、碳粉末和粘合剂制成,并被设置在电极导体11上。负极9’包括铜或者镍的电极导体11’和活性物质层12’,该活性物质层12’由碳粉末和粘合剂制成,并被设置在电极导体11’上。隔膜10被布置在正极9和负极9’之间。隔膜10是电绝缘和粒子导电性的聚烯烃系多孔膜。
连接片(connection piece)由电极导体11、11’一体化形成的,从而用点焊或超声波焊将每个连接片连接到相应的引线的金属部分2。这样将正极9和负极9’电连接到外部。由于连接到正极9的引线的金属部分2到达高正电势,所以它优选由铝(类似于电极导体11)或铝合金制成,以防止它溶于接触它的电解质溶液。连接到负极9’的引线的金属部分2优选由铜或镍(类似于电极导体11’)、或铜或镍的合金制成,以使它能抵抗锂的腐蚀、阻止与锂成合金和防止在高电势下溶解,这是因为过度放电导致锂在其上沉积(deposition),并且由于过度充电,它达到高电势。
单股圆形导体或扁平矩形导体能够被用作引线的金属部分2。但是,当圆形导体用于大容量电池中时,导体的直径必须大,并且存在危害引线连接到封装体上的部分处的密封性的可能性。因此,甚至当电池容量大时,宽度可以增加而厚度没有显著增加的扁平矩形导体,也能够穿过封装体3而不危害密封性。此外,考虑到电极导体11、11’到引线的金属部分2的焊接,通过使用具有扁平矩形导体的引线,由于能够获得更大的接触面,所以能够获得具有优良可靠性的连接。
图2B是沿着图2A的切线a-a的横截面图,和图2C是沿着图2A的切线b-b的横截面图。如图2B和图2C所示,绝缘体6优选由两层即粘合层7和绝缘层制成,该绝缘体6在引线1连接到封装体3的部分上覆盖每个引线的金属部分2,并用来使引线的金属部分2与层压膜4的金属箔4a之间电绝缘。粘合层7由具有相对低的熔融温度(melting temperature)的树脂材料制成,并熔接到复合涂层5上(这将在后面讨论),从而密封地将绝缘层8连接到形成于引线的金属部分2表面上的复合涂层5上。粘合层7由例如热塑性聚烯烃树脂制成,并被热熔接到形成于引线的金属部分2表面上的复合涂层5上,所述热塑性聚烯烃树脂优选为低密度聚乙烯或酸改性的低密度聚乙烯(其具有例如40μm的厚度和110℃的熔点)。
绝缘层8由在热封封装体3的温度不熔融的树脂材料制成。将绝缘层8熔接到封装体3上,从而引线的金属部分2以密封的方式引出到封装体3之外。绝缘层8由例如交联的聚烯烃制成,所述交联的聚烯烃优选为交联的低密度聚乙烯或乙烯-乙烯醇聚合物(其具有例如44%的乙烯比例,100μm的厚度和165℃的熔点)。如果封装体3的最内层由酸改性的低密度聚乙烯制成,将在约110℃热封密封部分3a,但是在此热封温度时绝缘层8将不会熔融。因此,引线的金属部分2能够在引线1连接到封装体3的部分上与层压膜4的金属箔4a电绝缘。
在此实施方式中,为了防止引线的金属部分2被氢氟酸腐蚀,用复合涂层处理用来制造每个引线的金属部分2的镍、镀镍铜或铜的表面,所述复合涂层包括由聚丙烯酸构成的树脂组分或包含聚丙烯酸的树脂组分,以及锆、钛或钼的金属盐。该复合涂层增加了引线的耐氢氟酸性能。此处的金属盐不包含铬--已知的环境污染物质。锆盐可为氟化锆、碳酸锆或磷酸锆。有机钛螯合物可用作钛盐。钼酸盐可用作钼盐。
已确定,当通过使用不仅包含聚丙烯酸还包含聚丙烯酸酰胺(polyacrylicacid amide)的处理液体获得复合涂层5的树脂组分时,该复合涂层5比通过使用仅包含聚丙烯酸的处理液体获得的复合涂层,具有更好的耐氢氟酸性能,并且更加有用。
复合涂层5优选包含1~200mg/m2的树脂组分和0.5~50mg/m2的锆盐、钛盐或钼盐。如果树脂组分含量低于1mg/m2,复合涂层5的柔韧性将降低,并且更加易于发生断裂。相反,如果树脂组分含量超过200mg/m2,复合涂层5和绝缘体6(绝缘层7)之间的粘合性将降低。同时,如果金属盐含量低于0.5mg/m2,耐氢氟酸性能将不够,而且如果金属盐含量超过50mg/m2,涂层将是脆性的。
对于复合涂层5,树脂组分含量与锆盐、钛盐或钼盐的含量之比优选为1∶3至6∶1。如果树脂组分含量与金属盐含量之比低于1∶3,则树脂组分将包封金属盐,导致粘合强度降低,并且使得难以获得足够的耐氢氟酸性。相反,如果该比值大于6∶1,复合涂层5中的金属盐的相对量将少,又将不可能获得足够的耐氢氟酸性。
引线的金属部分2通常由铝、镍、镀镍铜或铜制成。已确定,本发明的复合涂层有效地适合于由镍、镀镍铜或铜制成的引线的金属部分2。
表1示出了本发明的实施例1~5和对比例1~5的数据。更具体地,该表示出了每个实施例和对比例的引线材料、用来制造复合涂层的化学处理液体的组成和树脂组分含量与金属盐含量之比,所述化学处理液体包括树脂组分和金属盐。在所有这些实施例中,具有80μm厚的金属箔用作引线的金属部分。在实施例1~5和对比例4和5中,用凹槽辊涂布机(gravure coater),将具有表1中所示的组成比的化学转化处理液体,以5g/m2(湿)的厚度施涂到金属箔的两面上。然后通过加热使金属表面变成100℃来干燥处理液体。在对比例1~3中,在金属箔上没有设置复合涂层。在实施例1~5和对比例4和5中,化学转化处理液体的树脂组分是聚丙烯酸和聚丙烯酸酰胺,金属盐是锆盐(碱式碳酸锆((NH4)3Zr(OH)(CO3)3))或钛盐(有机钛螯合物)。
表1
引线材料 | 树脂组分mg/m2 | 金属盐mg/m2 | 比 | |
实施例1 | 铝 | 20 | 锆盐20 | 1/1 |
实施例2 | 镍 | 100 | 锆盐20 | 5/1 |
实施例3 | 镍 | 20 | 钛盐20 | 1/1 |
实施例4 | 镀镍铜 | 20 | 锆盐20 | 1/1 |
实施例5 | 铜 | 20 | 锆盐20 | 1/1 |
对比例1 | 铝 | - | - | - |
对比例2 | 镀镍铜 | - | - | - |
对比例3 | 铜 | - | - | - |
对比例4 | 镍 | 0.5 | 锆盐20 | 1/40 |
对比例5 | 镍 | 3.0 | 锆盐0.4 | 7/1 |
接下来,将每个实施例的金属箔切成5mm的宽度。然后,将绝缘体热熔接到金属箔上,从而形成引线,所述绝缘体具有热塑性聚烯烃树脂的粘合层和交联的聚烯烃树脂的绝缘层。然后将引线浸入电解质溶液(其中向含有1∶1∶1比例的碳酸亚乙酯、碳酸二乙酯和碳酸二甲酯的液体中加入1mol六氟磷酸盐)并在80℃的恒温容器中储存四周。用肉眼观察引线,检查绝缘体从引线的金属部分上的剥落。
表2
3天后的剥落% | 1周后的剥落% | 2周后的剥落% | 3周后的剥落% | 4周后的剥落% | |
实施例1 | 0 | 0 | 0 | 0 | 0 |
实施例2 | 0 | 0 | 0 | 0 | 0 |
实施例3 | 0 | 0 | 0 | 0 | 0 |
实施例4 | 0 | 0 | 0 | 0 | 0 |
实施例5 | 0 | 0 | 0 | 0 | 0 |
对比例1 | 0 | 80 | 100 | 100 | 100 |
对比例2 | 0 | 80 | 100 | 100 | 100 |
对比例3 | 0 | 100 | 100 | 100 | 100 |
对比例4 | 0 | 0 | 10 | 50 | 80 |
对比例5 | 0 | 0 | 25 | 80 | 100 |
结果如表2所示,实施例1~5都获得无剥落的优良结果。相反,一周之后,对比例1~3中没有设置复合涂层的引线的80%以上发生了绝缘体的剥落。两周之后,所有这些对比例的引线发生剥落。此结果清楚地证明,当绝缘体以密封的方式单独被密封粘着至引线的金属部分上,不使用任何方式处理该金属时,耐氢氟酸性能不够。而且,在对比例4和5中,两周之后引线的10%~25%发生绝缘体的剥落,四周之后引线的80%以上发生绝缘体的剥落。此结果说明,即使设置有复合涂层,如果复合涂层中的树脂组分含量与金属盐含量之比低于或高于规定值,则在长期使用之后,也能够发生由氢氟酸导致的腐蚀所导致的电解液泄漏。
日本专利申请2004-286740(2004年9月30日申请)的说明书、权利要求、附图和摘要中所做的所有公开在此引入,作为参考。
工业实用性
本发明使得可在引线表面上形成不包含六价铬(铬VI)和三价铬(铬III)的复合涂层,所述六价铬是已知的环境污染物质,所述三价铬的使用在将来将可能被限制。通过形成这种复合涂层,能够以这种方式密封引线,即获得优选的耐氢氟酸性,而且能够实现不泄漏、具有稳定特性和长期使用寿命的非水电解质电池。
Claims (6)
1.非水电解质电池用引线,其中正极、负极和电解质溶液封装在封装体中,所述封装体由包含金属箔的层压膜制成,所述引线包括:
(1)由镍、镀镍铜或铜制成的引线的金属部分;
(2)复合涂层,其是在所述引线的金属部分的表面上所述封装体被密封粘着的部分处,通过涂布包含锆盐、钛盐或钼盐和包含聚丙烯酸的树脂组分的处理液体而形成的;和
(3)布置在所述复合涂层外部并被封装体密封粘着的绝缘体。
2.权利要求1的非水电解质电池用引线,其中
所述树脂组分包含聚丙烯酸和聚丙烯酸酰胺。
3.权利要求1或2的非水电解质电池用引线,其中
所述复合涂层包含1~200mg/m2的树脂组分和0.5~50mg/m2的锆盐、钛盐或钼盐。
4.权利要求3的非水电解质电池用引线,其中
所述树脂组分与锆盐、钛盐或钼盐之比为1∶3至6∶1。
5.非水电解质电池,其包括:
由包含金属箔的层压膜制成的封装体;
封装在封装体中的正极、负极和电解质溶液;和
分别连接正极和负极并被布置为引出到封装体外部的引线,
至少一个所述引线包括:
(1)由镍、镀镍铜或铜制成的引线的金属部分;
(2)复合涂层,其是在所述引线的金属部分的表面上所述封装体被密封粘着的部分处,通过涂布包含锆盐、钛盐或钼盐和包含聚丙烯酸的树脂组分的处理液体而形成的;和
(3)布置在所述复合涂层外部并被封装体密封粘着的绝缘体。
6.权利要求5的非水电解质电池,其中
所述树脂组分包含聚丙烯酸和聚丙烯酸酰胺。
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PCT/JP2005/017589 WO2006035691A1 (ja) | 2004-09-30 | 2005-09-26 | 非水電解質電池用リード線及び非水電解質電池 |
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