CN1505198B - 锂离子二次电池以及制造该电池的方法 - Google Patents

锂离子二次电池以及制造该电池的方法 Download PDF

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CN1505198B
CN1505198B CN2003101246513A CN200310124651A CN1505198B CN 1505198 B CN1505198 B CN 1505198B CN 2003101246513 A CN2003101246513 A CN 2003101246513A CN 200310124651 A CN200310124651 A CN 200310124651A CN 1505198 B CN1505198 B CN 1505198B
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印田靖
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Abstract

锂离子二次电池以及制造该电池的方法。一种锂离子二次电池，包括正电极，负电极和包括锂离子导电无机物质的薄膜固体电解质。薄膜固体电解质的厚度为20微米或更小，且直接形成在用于正和/或负电极的电极材料上。薄膜固体电解质具有锂离子导电率为10-5Scm-1或更高的锂离子导电率，并且在聚合体介质中包含重量比为40％或是更多的锂离子导电无机物质粉末。无机物质粉末的平均颗粒直径为0.5μm或更小。根据一种制造锂离子二次电池的方法，通过直接在用于正电极和/或负电极的电极材料上覆盖锂离子导电无机物质而形成薄膜固体电解质。

Description

锂离子二次电池以及制造该电池的方法
技术领域
本发明涉及一种采用薄膜固体电解质的锂离子二次电池和一种制造该电池的方法。
背景技术
以前通常使用非水的电解溶液作为锂离子二次电池的电解溶液。由日本专利申请公开出版物第2000-067917中公开的采用聚合体制成的聚合体电解质的锂离子二次电池，与采用液体电解溶液的此类电池相比，最近更加得到了工业上的关注。
采用聚合体电解质的锂离子二次电池在聚合体电解质内保持有液体电解溶液，因此具有以下优点：液体泄漏可能性小，腐蚀可能性小，以及避免了由枝状晶体形式的锂的沉淀引起的电极间的短路，并且因为电池结构非常简单而使得电池的组装非常容易。
由于此类聚合体电解质的锂离子的导电率低于仅包含有一种电解溶液的电解质，因此实际中会发生聚合体电解质厚度减小这样的情况。但是在其厚度被减小的聚合体电解质中出现这样一个问题，由于其机械强度降低，因此聚合体电解质容易被削弱或是在电池生产过程中出现有孔，导致正负电极之间发生短路。据报道凝胶聚合体电解质具有从30μm到80μm的厚度。
为了提高机械强度，在日本专利申请公开出版物第2001-015164中提出了一种包含有锂离子导电玻璃陶瓷粉末的复合电解质。但是该方案并不能实现厚度为20μm或是20μm以下的薄膜电解质。
还提出有许多方案，例如日本专利申请公开出版物第Hei07-326373中公开了一种不采用电解溶液的固体电解质电池。由于采用固体电解质的锂离子二次电极与现有技术相同，不需要有机电解溶液，因而不会有溶液泄漏和燃烧的危险，因此能够提供安全性高的电池。在采用有机电解溶液的现有技术的电池中，正电极和负电极通过靠固体电解质的有机电解溶液的方式彼此接触，因此接触面上的离子运动中的阻抗不会引起严重的问题。但是如果电池的正电极，负电极以及电解质都是由固体制成，则正电极与电解质之间的接触面上的接触，和负电极与电解质之间的接触面上的接触就会成为包括在接触面的一些部分上进行点接触的固体之间的接触，由此产生了与采用电解溶液的现有技术的电池相比，非常大的接触阻抗。因此，固体电解质电池在接触面上具有非常大的阻抗，其容易引起极化并且由此限制了接触面内的锂离子的运动，结果是很难用该固体电解质电池实现具有高容量和高输出的电池。
因此本发明的一个目的是提供一种锂离子二次电池，其尽管采用了固体电解质，但该电池仍能够解决以上问题并且具有稀薄的电解质，并且由此具有较小的阻抗，因此具有较高的电池容量和较高输出以及良好的充-放电特性，并且由此确保电池在长时间使用中的稳定性。
发明内容
作为详细研究和试验的结果，本发明的发明人发现导致了本发明产生的以下内容，包含某一晶体的无机物质具有较高的锂离子导电率，其锂离子传送数量是1，并且通过采用该物质作为锂离子二次电池中薄膜形式的固体电解质，能够实现电池的高性能。
根据本发明的锂离子二次电池包含有正电极，负电极以及固体电解质，所述固体电解质制成为包含锂离子导电无机物质的薄膜形式。
薄膜固体电解质最好应该包含一种具有高锂离子导电率的无机物质，更好的是包含一种锂离子导电晶体，玻璃或玻璃陶瓷。在用于本发明的锂离子二次电池的薄膜固体电解质中，薄膜固体电解质越薄，锂离子运动的距离就越短，因此电池的输出就越高。所以在锂离子二次电池中，薄膜固体电解质的厚度最好为20μm或更小，较佳的是10μm或更小，最佳的是5μm或更小。
在本发明的锂离子二次电池充放电期间的锂离子的迁移，是由固体电解质的锂离子的导电率以及锂离子的传送数量决定的。因此，在本发明的锂离子二次电池中，薄膜固体电解质的锂离子导电率最好为10-5Scm-1或更多。
附图说明
在附图中，图1是示出了本发明的锂离子二次电池内部结构的横截面图；
图2是示出了实施例1和比较实施例1的锂离子二次电池的伴随充放电循环的放电容量的变化的曲线图。
图3是示出了实施例4和比较实施例4的锂离子二次电池伴随充放电循环的放电容量的变化的曲线图。
具体实施方式
在本发明的最佳实施例中，薄膜固体电解质最好应该具有40％重量百分比或是更多的无机物质。该无机物质最好应该是离子导电晶体，玻璃或是玻璃陶瓷。无机物质最好应该为无机物质的粉末。薄膜固体电解质中无机物质的粉末的平均颗粒直径最好应该为1.0μm或更小，较佳的是0.5μm或更小，最佳的是0.3μm或更小。
在本发明的锂离子二次电池中，薄膜固体电解质可以在聚合体介质中包含锂离子导电无机物质粉末。薄膜固体电解质最好应该具有锂无机盐和锂离子导电玻璃陶瓷粉末。
在本发明的锂离子二次电池中，薄膜固体电解质可以通过直接覆盖在用于正电极和/或负电极的电极材料上而形成。
根据本发明，制造具有包含有锂离子导电无机物质的薄膜固体电解质的锂离子二次电池的方法包括，通过在用于正和/负电极的电极材料上直接覆盖锂离子导电无机物质而形成薄膜固体电解质的步骤。
如上所述，固体电解质越薄，电阻就越小，并且离子的运动距离就越短，因此电池的输出就越高。但是，在独立且与电池的其他元件分离地生产固体电解质的情况下，由于强度，操作以及制造工艺方面的原因，因此对于把固体电解质作薄方面就存在有限制。根据本发明的用于制造锂离子二次电池的方法，固体电解质直接在用于正电极和/或负电极的电极材料上形成，因此不会出现由处理单独的固体电解质而引发的问题，由此可以将固体电解质作得足够薄。
薄膜固体电解质可以通过将包含有锂离子导电晶体，玻璃或玻璃陶瓷的浆制备为无机物质，并且将该浆直接覆盖在用于正和/或负电极的电极材料上而形成。
为了把浆直接覆盖在用于正电极和/或负电极的电极材料上，可以采用浸渍，丝网涂层或是磁带浇铸的方法，或是采用诸如喷墨或屏幕印刷之类的印刷工艺。可以采用无机物质的锂离子导电粉末与粘合剂一起分散在介质物中形成浆。优选的无机物质为晶体，玻璃以及玻璃陶瓷。薄膜固体电解质最好应该包含40％重量比或是更多的无机物质。
本发明中使用的锂离子导电粉末最好应该具有较高的锂离子导电率，并且较

Claims (12)

1.一种锂离子二次电池，包括正电极，负电极和固体电解质，其中所述固体电解质制成为包含有锂离子导电玻璃陶瓷的薄膜形式，所述薄膜固体电解质直接形成在用于正电极和/或负电极的电极材料上，并且在所述正电极、所述固体电解质和所述负电极的覆盖过程中没有干燥过程。
2.如权利要求1中限定的锂离子二次电池，其中所述薄膜固体电解质的厚度为20微米或更小。
3.如权利要求1中限定的锂离子二次电池，其中所述薄膜固体电解质具有10-5Scm-1或以上的锂离子导电率。
4.如权利要求1中限定的锂离子二次电池，其中所述薄膜固体电解质具有重量比为40％或以上的玻璃陶瓷。
5.如权利要求1中限定的锂离子二次电池，其中所述锂离子导电玻璃陶瓷是粉末。
6.如权利要求5中限定的锂离子二次电池，其中玻璃陶瓷粉末的平均颗粒直径为1.0μm或更小。
7.如权利要求5中限定的锂离子二次电池，其中所述薄膜固体电解质在聚合体介质中具有锂离子导电玻璃陶瓷粉末。
8.如权利要求5中限定的锂离子二次电池，其中所述薄膜固体电解质在聚合体介质中具有锂无机盐和锂离子导电玻璃陶瓷粉末。
9.如权利要求1中限定的锂离子二次电池，其中所述薄膜固体电解质是通过直接覆盖在用于正电极和/或负电极的电极材料上而形成的。
10.如权利要求1中限定的锂离子二次电池，其中所述正和/或负电极具有锂离子导电玻璃陶瓷粉末。
11.如权利要求10中限定的锂离子二次电池，其中所述正和/或负电极中的所述玻璃陶瓷粉末的平均颗粒直径为3微米或更小。
12.一种制造具有薄膜固体电解质的锂离子二次电池的方法，该薄膜固体电解质包括锂离子导电玻璃陶瓷，该方法包括：制备包含有该锂离子导电玻璃陶瓷的浆的步骤，通过直接在用于正和/或负电极的电极材料上覆盖该浆而形成该薄膜固体电解质的步骤，其中在所述正电极、所述固体电解质和所述负电极的覆盖过程中没有干燥过程。
CN2003101246513A 2002-11-29 2003-12-01 锂离子二次电池以及制造该电池的方法 Expired - Fee Related CN1505198B (zh)

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US8383268B2 (en) 2013-02-26
HK1065649A1 (en) 2005-02-25
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CA2451181C (en) 2013-04-02
EP1424743A1 (en) 2004-06-02
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DE60309815D1 (de) 2007-01-04
JP2004185862A (ja) 2004-07-02
KR100580442B1 (ko) 2006-05-15
CA2698567A1 (en) 2004-05-29
JP4777593B2 (ja) 2011-09-21
US20090274832A1 (en) 2009-11-05
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CN1505198A (zh) 2004-06-16
ATE346392T1 (de) 2006-12-15

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