CN86102718A - 固态锂电池阴极的组成及制备方法 - Google Patents
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Abstract
一种固态锂电池的阴极,包括聚合物球体层。每一个聚合物球体包含一个封装在离子和导电聚合物材料中的氧化钒芯。
Description
本发明旨在提供用于全固态锂电化学电解槽的新型阴极及其制造方法,本发明尤其涉及多层电化学锂电解槽的阴极层,该种电解槽具有聚合物电解质层,含有氧化钒的阴极层,和锂或锂铝合金的阳极层。
电化学电解槽一直为多种材料制造。其电极及非导电层一直是由塑料,金属及其他材料制造的。电解质通常都是液体,但是现在人们都希望用固态物质,比如聚合物来制造锂电池。
固态电池将避免由液态电解质电解槽带来的许多问题,比如电解液渗漏,干枯,阳极钝化,结晶等。另外,由于所有组件均为固态,所以简化了电解槽的制造并使之成了一个机械性的坚固的装置。适宜的操作温度可克服高温熔盐电解质或熔化的电极带来的腐蚀,密封等严重问题。很清楚,固态电池比液态电解质或糊状电解质电池可取之处更多。
制造锂电池时最好用聚合物/无机复合材料做阴极层和电解质层。这些夹层通过连续浇注和溶剂蒸发形成薄膜状,用这种方法可以通过常规方法生产出25-50微米厚的大面积薄片。这一技术通常称为“刮片”技术,它导致产生了电解质层,该电解质层无小孔,多次使用后仍保持完好,并有极好的界面特性。
最近,哈威尔(Harwell)试验室和欧旦斯(odense)大学能源研究试验室对锂电池共同进行了研究,重点是关于由各种锂盐和聚环氧乙烷复合而成的聚合物电解质问题。这种电解槽阴极的材料主要是V6O13,阳极最理想的是用锂金属箔或者是锂/铝箔。具体说,阴极是将磨碎的氧化钒与乙炔黑在电解质溶液里直接混合而形成的合成结构。电解质溶液含有聚环氧乙烷,当合成的阴极层淀积为薄膜时,它含有不规则的聚合物、碳和氧化钒的颗粒结块。据说这样制造的锂电解槽在电流密度,材料利用及再生性方面都有所改进。人们建议这些电解槽可用于牵引车辆的电池之中,可参见胡波(Hoper,A,et al.,)写的“先进电池发展”一文(一九八四年欧旦斯大学学报)。
现已发现,使用新颖的阴极结构可使锂电解槽的特性大幅度提高。特别是本发明旨在提供一个以V6O13为基础的复合阴极,它可增大表面积,提高性能特点,延长寿命。
通过以聚合物封装的氧化钒球体层做固态电池阴极层,可达到上述目的。理想的聚合物,聚环氧乙烷,含有更多的锂盐和活性碳。这些球体呈乳胶状,可做为导电衬底层。
结合本文下列附图说明,很容易理解本发明的性质和特点。
图1表明,该发明的聚合物球体存在于夹层中,即每一球体与其邻近球体接触而形成电子网络。
图2表明以聚合物球体层做阴极的固态锂电池。
当然,应当知道本文的附图和叙述只是一个图解,在不改变本发明基本精神的前提下,对于所公开的结构可做多种改型和变更。
固态锂电池包括一个阳极层,一个阴极层和一个聚合物非导电层。由片、卷、带等形式组成的这种三层结构体构成了一个简单的电解槽或电池。这种结构可以应用各种不同的附加层,包括引导电流底层、绝缘层和/或双相电极连接。这种简单电池可以连接组合在一起形成多电解槽电化学装置。
尤其是电化学电解槽被制成活性面积为0.75平方厘米的夹层盘式。然而,也可在中心轴上采用“瑞士绕法”(swiss-roll)技术制得其面积约为85~200平方厘米的大面积电解槽,或采用“六角手风琴式”(concertina)结构,在两块不锈钢板之间夹入上述大面积电解槽。这两种方法在本领域是广为人知的。
层状结构的阴极层和电解质层是将所谓“刮片”技术用于某种聚合物薄膜来生产的。按这一方法,在适当的溶剂中制备聚合物(或者与无机材料复合的聚合物)溶液并在垫板上浇制成膜状,如同腊纸通过安在平台一端的容器下方一样。容器正面的高低可以调整。刮片和纸之间的间隙决定了浇制薄膜的厚度。溶剂的挥发可使薄膜厚度均匀减少,减薄的程度取决于溶液的浓度。这一制造薄膜片的技术对于本领域的工作人员是很熟悉的。用此方法可产生25-50微米厚的薄膜。
锂电池的阳极层包括有一个锂金属箔或者锂/铝合金箔。电池等级为350微米厚的锂箔以前曾在电化学锂电解槽中使用过。使用这种箔需用大大超量的锂。最好是用锂铝合金的薄阳极。该合金是通过把铝箔在锂盐溶液里进行阴极还原制成的。淀积在箔表面的锂可在铝箔表面达到10-20微米厚,使铝箔厚度的一多半保持不改变,可以使阳极层结构的完整性得以保持。在铜箔上压焊上铝、比如80微米的铜箔和20微米的铝箔,同样可做阳极。然后,通过在含有锂盐非水液态电解质里把铝箔进行电化学转换的办法来制造阳极。两种阳极结构都适用于制造大面积薄膜电池。
聚合物电解质合成物是由锂盐和聚合物质,如聚环氧乙烷复合而成的。通过把高氯酸锂晶体和加热的聚合物相研磨,从而得到均匀混合的聚环氧乙烷和锂盐复合物。另外的办法是将聚合物和溶剂结合以提高薄膜形成的质量,并把盐加入溶液中的聚合物。得到的混合物做为薄膜直接淀积在电解槽的阴极层上。上述刮片技术被用于混合物。这样可提高电解质层的再生性,电解质层约为25微米。
按本发明制造的阴极层包括一个聚合物球体薄层。在聚合物球体中心处是活性阴极材料,即氧化钒。理想的氧化钒复合物V6O13是通过对偏钒酸铵加热分解而制备的。而且其颗粒结块平均尺寸为100-500微米。结块可进一步研磨以缩小至几毫米。
精磨的V6O13颗粒密封在导电聚合物里形成球体,如图1所示,参阅图1,聚合物球体10含有封装在导电聚合物材料12中的氧化钒芯13。理想的导电聚合物包括含有无机盐的聚环氧乙烷和炭黑,聚环氧乙烷具有离子导电性,而炭黑具有聚合物导电性。
本发明聚合物球体的基本优点是可以大幅度增大阴极的活性表面积。也即,氧化钒阴极材料可在球体中机械地固定,这样可增加阴极层的活性寿命。另外,既然每一个球体和另外的导电性球体相接触,这样就有一个电子网络横跨并通过阴极,如图1所示。球体之间的空隙可使阴极每一部分都能扩散接触。
以乳胶液用聚环氧乙烷聚合物做粘合剂可制得球体。聚合物加入乳胶液之前与锂盐和炭黑合成。在锂电池电解质层中最好采用无机盐类,它包括LiClO4、NaClO4、L1F3CSO3和L1BF4。炭或乙炔黑以5%的重量比加入聚合物以提供导电率。
合成的聚合物和精细分解了的V6O13溶解于适合的有机溶液中,结果,每一个颗粒或氧化钒结块都为聚合物所封装并在乳胶液中保持球状。因此,当去掉溶剂,乳胶液呈薄膜状使用时,球体层即淀积于衬底之上。由“刮片”法制作的薄膜其厚度可任意选择。
图2所示意的是使用了本发明的固态锂电池结构。层14相当于阳极,所前所述,它含有锂或锂/铝箔。层16相当于电解质层,按需要含有聚环氧乙烷和无机盐。如这里所公开的,层10是由各种含氧化钒的聚合物的球体形成的阴极。层18是聚合电流的底层,可含例如镍或铜箔。
图2所示的四个叠层可由连续板或卷制备,最好是以连续工艺逐层从下至上进行。
本发明的最佳实施例中,是在球体层中使用离子导电聚环氧乙烷以在球体周围形成基体并充于其间的空隙之中。这将增加该层的机械稳定性并提供改善的扩散特性。
据发现,最好使用相当于阴极和基体总体积的50%的氧化钒。
当制取锂电池时,应将阴极层直接淀积在电流聚集底层上。依照本发明,聚合物球体的乳胶液可直接以薄膜状用在箔底上。
Claims (7)
1、一种固态锂电池,包括一个锂或锂/铝阳极,一种聚合物电解质和一个以氧化钒为基础的阴极,其中,该阴极包括多个球体,每一个球体包括一个封装在聚合物薄膜里的氧化钒芯,所提到的聚合物薄膜含无机盐和活性炭。
2、权利要求1中所说的聚合物薄膜含聚环氧乙烷。
3、权利要求2中所说的电池,其中无机盐选自LiClO4、NaClO4、LiF3CSO3和LiBF4。
4、权利要求2中所说的电池,其中,通过把氧化钒粉置于用聚环氧乙烷作粘合剂的有机溶液中进行乳化,可制备球体。
5、权利要求1中所提的电池,其阴极含体积为50%的氧化钒。
6、在固态锂电池中形成阴极层的方法包括如下步骤:
a)在有机溶液中乳化氧化钒粉末,用包含一种无机盐和活性炭的聚环氧乙烷做粘合剂,以便在乳胶中提供多个球体,所说的球体包含封装在所提到的粘合剂薄膜里的氧化钒芯;
b)乳胶液以薄膜状用于电流聚集衬底上,并
c)使所提到的溶剂蒸发,从而使球体层淀积在所说的衬底上。
7、权利要求6中所说的方法,包括把淀积的球体层作为离子导电材料以形成包含球体的基体的步骤。
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US06/729,643 US4576883A (en) | 1985-05-02 | 1985-05-02 | Cathode composition and method for solid state lithium battery |
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US (1) | US4576883A (zh) |
JP (1) | JPS61256564A (zh) |
CN (1) | CN86102718A (zh) |
AU (1) | AU576948B2 (zh) |
BR (1) | BR8601185A (zh) |
CA (1) | CA1268809C (zh) |
DE (1) | DE3608643A1 (zh) |
DK (2) | DK155477C (zh) |
GB (1) | GB2175126B (zh) |
NZ (1) | NZ215394A (zh) |
Families Citing this family (23)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US4847174A (en) * | 1985-12-17 | 1989-07-11 | Combustion Engineering, Inc. | Thermally actuated hydrogen secondary battery |
JP2504428B2 (ja) * | 1986-10-17 | 1996-06-05 | 昭和電工株式会社 | 二次電池 |
US4808496A (en) * | 1987-03-13 | 1989-02-28 | Mhb Joint Venture | Electrode construction for solid state electrochemical cell |
US4720910A (en) * | 1987-06-16 | 1988-01-26 | Mhb Joint Venture | Method for preparing encapsulated cathode material |
US4794059A (en) * | 1988-02-29 | 1988-12-27 | Hope Henry F | Lightweight solid state rechargeable batteries |
US4911996A (en) * | 1988-03-11 | 1990-03-27 | Eic Laboratories, Inc. | Electrochemical cell |
US4902589A (en) * | 1988-06-08 | 1990-02-20 | Moli Energy Limited | Electrochemical cells, electrodes and methods of manufacture |
ATE99077T1 (de) * | 1988-09-09 | 1994-01-15 | Hydro Quebec | Verfahren zur herstellung einer von einem streifen getragenen duennen elektrode. |
US4960655A (en) * | 1989-01-27 | 1990-10-02 | Hope Henry F | Lightweight batteries |
US5124508A (en) * | 1990-08-14 | 1992-06-23 | The Scabbard Corp. | Application of sheet batteries as support base for electronic circuits |
US5147985A (en) * | 1990-08-14 | 1992-09-15 | The Scabbard Corporation | Sheet batteries as substrate for electronic circuit |
DE69318766T2 (de) * | 1992-07-10 | 1998-10-08 | Nippon Oil Co Ltd | Zinkelektrode für alkalische Speicherbatterie |
US5330856A (en) * | 1993-06-08 | 1994-07-19 | Valence Technology, Inc. | Method of making a cathode for use in an electrolytic cell |
US5360686A (en) * | 1993-08-20 | 1994-11-01 | The United States Of America As Represented By The National Aeronautics And Space Administration | Thin composite solid electrolyte film for lithium batteries |
US5418089A (en) * | 1993-12-06 | 1995-05-23 | Valence Technology, Inc. | Curable cathode paste containing a conductive polymer to replace carbon as the conductive material and electrolytic cells produced therefrom |
JPH09245836A (ja) * | 1996-03-08 | 1997-09-19 | Fuji Photo Film Co Ltd | 非水電解質二次電池 |
EP0958627B1 (en) | 1996-05-22 | 2002-02-27 | Moltech Corporation | Composite cathodes, electrochemical cells comprising novel composite cathodes, and processes for fabricating same |
US7214446B1 (en) | 1997-07-21 | 2007-05-08 | Nanogram Corporation | Batteries with electroactive nanoparticles |
US5952125A (en) * | 1997-07-21 | 1999-09-14 | Nanogram Corporation | Batteries with electroactive nanoparticles |
US6132904A (en) * | 1997-07-24 | 2000-10-17 | Sanyo Electric Co., Ltd. | Polyelectrolytic battery having a polyelectrolyte based on a polystyrene main chain and polyethylene oxide side chain |
US6673130B2 (en) * | 2001-06-15 | 2004-01-06 | The Regents Of The University Of California | Method of fabrication of electrodes and electrolytes |
CN1260848C (zh) * | 2002-03-28 | 2006-06-21 | Tdk株式会社 | 锂二次电池 |
US10411252B2 (en) * | 2016-02-09 | 2019-09-10 | GM Global Technology Operations LLC | Positive electrode composition, a positive electrode of a lithiumion electrochemical cell, and a method of forming the positive electrode |
Family Cites Families (6)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
FR2485274A1 (fr) * | 1980-03-31 | 1981-12-24 | France Etat | Electrolyte solide a base de materiau macromoleculaire a conduction ionique |
US4520086A (en) * | 1980-11-18 | 1985-05-28 | The United States Of America As Represented By The United States Department Of Energy | Rechargeable solid polymer electrolyte battery cell |
JPS58169769A (ja) * | 1982-03-30 | 1983-10-06 | Toshiba Corp | 固体電解質電池 |
US4471037A (en) * | 1982-04-16 | 1984-09-11 | United Kingdom Atomic Energy Authority | Solid state electrochemical cell |
US4570086A (en) * | 1983-06-27 | 1986-02-11 | International Business Machines Corporation | High speed complementary NOR (NAND) circuit |
US4496633A (en) * | 1983-11-01 | 1985-01-29 | Union Carbide Corporation | High density load bearing insulation peg |
-
1985
- 1985-05-02 US US06/729,643 patent/US4576883A/en not_active Expired - Fee Related
-
1986
- 1986-03-06 NZ NZ215394A patent/NZ215394A/xx unknown
- 1986-03-07 AU AU54482/86A patent/AU576948B2/en not_active Ceased
- 1986-03-07 GB GB08605673A patent/GB2175126B/en not_active Expired
- 1986-03-14 CA CA504129A patent/CA1268809C/en not_active Expired
- 1986-03-14 DE DE19863608643 patent/DE3608643A1/de not_active Withdrawn
- 1986-03-14 JP JP61055135A patent/JPS61256564A/ja active Pending
- 1986-03-17 BR BR8601185A patent/BR8601185A/pt unknown
- 1986-03-17 DK DK122386A patent/DK155477C/da active
- 1986-04-23 CN CN86102718A patent/CN86102718A/zh active Pending
-
1988
- 1988-04-08 DK DK195088A patent/DK195088A/da not_active Application Discontinuation
Also Published As
Publication number | Publication date |
---|---|
DK195088D0 (da) | 1988-04-08 |
US4576883A (en) | 1986-03-18 |
JPS61256564A (ja) | 1986-11-14 |
AU576948B2 (en) | 1988-09-08 |
BR8601185A (pt) | 1987-01-13 |
DK155477C (da) | 1989-09-11 |
DK155477B (da) | 1989-04-10 |
GB2175126B (en) | 1988-03-02 |
GB2175126A (en) | 1986-11-19 |
CA1268809A (en) | 1990-05-08 |
DK122386D0 (da) | 1986-03-17 |
NZ215394A (en) | 1989-04-26 |
DE3608643A1 (de) | 1987-09-17 |
AU5448286A (en) | 1986-11-06 |
GB8605673D0 (en) | 1986-04-16 |
DK195088A (da) | 1988-04-08 |
DK122386A (da) | 1986-11-03 |
CA1268809C (en) | 1990-05-08 |
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