CN101048912A - 电池用非水电解液 - Google Patents
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Abstract
本发明涉及一种电池用非水电解液，更确切地说，涉及一种新型的电池用非水电解液，其中在传统的锂电池用非水电解液中添加呋喃酮类衍生物以抑制电解液的分解，因此，显著降低了高温下电池厚度的增长率，并且改善了高温下电池的容量存储特性。
Description
技术领域
本发明涉及一种电池用非水电解液，更确切地说，涉及一种新型的电池用非水电解液，其中，在传统的锂电池用非水电解液中添加呋喃酮类衍生物以抑制电解液的分解，因此，显著降低了高温下电池厚度的增长率，并且改善了高温下电池的容量存储特性。
背景技术
用于笔记本电脑、便携式摄像机、移动电话等的微型二次锂电池由阴极、阳极和电解液组成，所述阴极由能够嵌入与脱嵌锂离子的混合锂氧化物制成，所述阳极由碳材料或锂制成，所述电解液含有适量的溶解在混合有机溶剂中的锂盐。这种锂电池通常为硬币型、18650圆柱型或063048方型电池。锂电池的平均放电电压约为3.6-3.7伏特，因此，相对于其它碱性电池、Ni-MH电池或Ni-Cd电池，锂电池具有能量较高的优势。
为了提供这种高驱动电压，需要一种在0-4.2伏特范围内充电/放电时电化学稳定的电解液组合物，因此，为了增加碳酸酯类有机溶剂(例如碳酸乙烯酯(EC)、碳酸二甲酯(DMC)、碳酸二乙酯(DEC))与隔膜之间的吸收，在其中适当地加入氟苯(FB)并用作电解液的溶剂。关于电解液的溶质，一般使用锂盐例如LiPF6、LiBF4、LiClO4和LiN(C2F5SO3)2，所述锂盐在电池中提供锂离子的来源，以确保电池的基本运转。然而，相对于Ni-MH电池或Ni-Cd电池中所用的水性电解液，如此制备的非水电解液的离子电导率明显偏低，因此在高功率充电/放电方面的表现不好。
在锂电池首次充电时，锂离子从作为阴极的金属锂复合氧化物转移到作为阳极的石墨(晶态或非晶态)电极上，并且嵌入到石墨电极层间。同时，由于锂离子具有很高的活性，电解液与构成阳极的碳原子的反应，在石墨阳极表面形成化合物，例如Li2CO3、Li2O和LiOH。这些化合物在石墨阳极表面形成钝化层，称作固体电解质界面(Solid Electrolyte Interface，SEI)膜。SEI膜一旦形成，就起到离子通道的作用并且仅能通过锂离子。SEI膜通过这样的离子通道作用使锂离子溶剂化，并且因此防止电解液中随锂离子一起移动的大分子量的有机溶剂分子(例如，EC、DMC和DEC)嵌入到石墨阳极中破坏其结构。SEI膜一旦形成，锂离子不与石墨阳极或其它材料进行副反应，并且形成SEI膜所消耗电荷的量作为不可逆容量而释放掉，其具有不可逆反应的特性。因此，电解液不会出现进一步分解，并且通过稳定的充电/放电维护而可逆地维持电解液中锂离子的含量。(见J.Power Sources(1994)51：79-104)。
发明内容
同时，薄的方型电池的问题在于对其进行充电的过程中，在形成SEI膜的同时，碳酸酯类有机溶剂分解产生气体例如CO、CO2、CH4和C2H6，导致电池的厚度增加(见J.Power Sources(1998)72：66-70)。此外，当电池在充满电的状态下高温存放时(例如，充满电至4.2伏特后，在85℃下放置4小时)，随着时间的推移，由于电化学能量和热量的增加，所述SEI膜逐渐分解，因此，阴极暴露表面和周围的电解液不断进行副反应。因而，不断地产生气体，引起电池内部压力的增加，结果方型电池和锂离子聚合体(polymer lithium ion，PLI)电池的厚度增加，从而导致安装的困难。
本发明提供一种新型的锂电池用非水电解液，其中，在传统的锂电池用非水电解液中添加呋喃酮类衍生物以抑制电解液的分解，因此，显著降低了高温下电池厚度的增长率，并且改善了高温下电池的容量存储特性。
根据本发明的一个方面，本发明的以上和其它目的可以通过提供一种电池用非水电解液来实现，该非水电解液含有0.8-2M锂盐，其中，添加有0.01-20重量％的具有下式(I)的特窗酸：
(式I)
本发明提供一种新型的锂电池用非水电解液，其中，在传统的锂电池用非水电解液中添加呋喃酮类衍生物以抑制电解液的分解，因此，显著降低了高温下电池厚度的增长率，并且改善了高温下电池的容量存储特性。
附图说明
通过以下结合附图的详细描述，将更清楚地理解本发明的以上和其它目的、特点及其它优点，其中：
图1为表示本发明实施例中制备的锂电池的充电/放电特性的曲线图；
图2为表示本发明实施例中制备的非水电解液的电化学特性的曲线图。
具体实施方式
在此，将对本发明进行更加详细的描述。
根据本发明，作为用于制备锂电池非水电解液的有机溶剂，可以提及环状碳酸酯类有机溶剂，例如碳酸乙烯酯(EC)和碳酸丙稀酯(PC)；和线型碳酸酯类有机溶剂，例如碳酸二甲酯(DMC)、碳酸二乙酯(DEC)、乙基甲基碳酸酯(EMC)、甲基丙基碳酸酯(MPC)和乙基丙基碳酸酯(EPC)。优选地，可以使用至少一种环状碳酸酯类有机溶剂和至少一种线型碳酸酯类有机溶剂的混合物，更优选地，使用碳酸乙烯酯、乙基甲基碳酸酯和碳酸二乙酯按照1∶1∶1的比例组成的混合物。另外，如果需要，可以另外混合、使用溶剂例如乙酸丙酯、乙酸甲酯、乙酸乙酯、乙酸丁酯、丙酸甲酯、丙酸乙酯和氟苯。各有机溶剂的混合比例没有特别的限制，只要不妨碍本发明的目的即可，可以按照制备常规锂电池非水电解液所用的混合比例。
根据本发明，作为所述非水电解液中所含锂盐的例子，可以提及LiPF6、LiClO4、LiAsF6、LiBF4、LiN(C2F5SO3)2等，这些锂盐可以单独使用也可以两种或两种以上混合使用。更优选使用LiPF6。锂盐的浓度范围为0.8-2.0M，当加入的锂盐的浓度低于0.8M时，离子电导率下降；当浓度超过2.0M时，电解液的粘度增加，因而离子电导率也下降。
根据本发明所述的非水电解液，其特征在于在其中添加有0.01-20重量％，优选为0.1-10重量％的具有下式(I)的特窗酸，该特窗酸为呋喃酮类衍生物。当上述提及的含量小于0.01重量％时，难以通过抑制电解液的分解来降低高温下电池厚度的增长率。另外，如果上述提及的含量超过20重量％时，电池的性能例如使用寿命将会降低。
(式I)
根据本发明所述的锂电池用非水电解液可以通过常规的方法用以制备锂电池。甚至所制备的电池在高温下放置时(80℃，10天)，抑制了由电解液分解引起的电池内部气体的产生，从而防止了电池厚度的膨胀，使高温下容量储存性能变得十分优良。
在此，结合以下实施例对本发明进行更加详细的描述。提供这些实施例仅仅为了解释本发明，而不应被理解为限制本发明的范围和精神。
实施例和对比例
将碳酸乙烯酯(EC)、乙基甲基碳酸酯(EMC)和碳酸二乙酯(DEC)按照1∶1∶1的体积比混合，并且将1M的LiPF6作为溶质溶解在其中，得到基础电解液。在得到的基础电解液中加入特窗酸，特窗酸的加入量如下表1所示，制得本发明的电解液(实施例1-5)。
制备的锂电池为方型423048电池。
石墨用作阳极活性材料，并且使用聚偏氟乙烯(PVDF)作为粘结剂。LiCoO2用作阴极活性材料，并且使用聚偏氟乙烯作为粘结剂。乙炔黑用作导电剂。
制备得到的锂电池在化成充电/放电和标准充电/放电过程后，电压为4.2伏特的充满电状态下，在高温下(80℃，10天)进行电池膨胀检测，结果如表1所示。同时进行使用寿命性能的检测(标准充电/放电，50个循环)，结果如图1所示。对添加有1.0重量％特窗酸的电解液(实施例2)和没有添加特窗酸的电解液(对比例)进行电化学性能检测，结果如图2所示。
表1
| 特窗酸的加入量 | 化成充电 | 化成放电 | 化成效率 | ΔIR(毫欧) | ΔV(伏特) | ΔT(毫米) | |
| 实施例1 | 0.1重量％ | 642.4 | 587.5 | 91.5 | 37.9 | -0.04 | 0.2 |
| 实施例2 | 1.0重量％ | 648.3 | 591.2 | 91.2 | 38.0 | -0.03 | 0.2 |
| 实施例3 | 3.0重量％ | 648.3 | 588.4 | 91.1 | 38.6 | -0.03 | 0.1 |
| 实施例4 | 5.0重量％ | 643.0 | 586.6 | 91.2 | 39.9 | -0.03 | 0.1 |
| 实施例5 | 10.0重量％ | 639.8 | 579.2 | 90.5 | 42.1 | -0.02 | 0.1 |
| 对比例 | - | 658.9 | 600.3 | 91.1 | 30.5 | -0.06 | 1.3 |
ΔIR(毫欧)：在高温条件下放置前和在高温条件下放置后，电池内阻的改变量；
ΔV(伏特)：在高温条件下放置前和在高温条件下放置后，电池电压的改变量；
ΔT(毫米)：在高温条件下放置前和在高温条件下放置后，电池厚度的改变量。
(高温条件为：80℃±2℃，10天)
工业适用性
根据本发明，提供了一种新型的锂电池用非水电解液，其中，在传统的锂电池用非水电解液中添加呋喃酮类衍生物以抑制电解液的分解，因此，显著降低了高温下电池厚度的增长率，并且改善了高温下电池的容量存储特性。
虽然，为了说明的目的公开了本发明的优选实施方式，但是在不背离本发明权利要求所公开的范围和精神的情况下，本领域技术人员可以进行各种修改、补充和替换。
Claims (4)
1、一种电池用非水电解液，该电解液含有溶解在其中的0.8-2.0M的锂盐，其中，添加有0.01-20重量％的具有下式I的特窗酸：
(式I)。
2、根据权利要求1所述的非水电解液，其中，所述锂盐为选自由LiPF6、LiClO4、LiAsF6、LiBF4和LiN(C2F5SO3)2所组成的组中的至少一种物质。
3、根据权利要求1所述的非水电解液，其中，至少一种环状碳酸酯类有机溶剂和至少一种线型碳酸酯类有机溶剂的混合物用作溶剂。
4、一种二次锂电池，该电池包括如权利要求1所述的电池用非水电解液。
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| PCT/KR2004/002728 WO2006046785A1 (en) | 2004-10-27 | 2004-10-27 | Nonaqueous electrolyte for battery |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| CN101048912A true CN101048912A (zh) | 2007-10-03 |
| CN100454654C CN100454654C (zh) | 2009-01-21 |
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| Application Number | Title | Priority Date | Filing Date |
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| CNB2004800442961A Expired - Fee Related CN100454654C (zh) | 2004-10-27 | 2004-10-27 | 电池用非水电解液 |
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| Country | Link |
|---|---|
| US (1) | US20090226820A1 (zh) |
| EP (1) | EP1807899A4 (zh) |
| JP (1) | JP2008518392A (zh) |
| CN (1) | CN100454654C (zh) |
| TW (1) | TWI259597B (zh) |
| WO (1) | WO2006046785A1 (zh) |
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| KR102431845B1 (ko) * | 2017-04-28 | 2022-08-10 | 삼성에스디아이 주식회사 | 리튬 이차 전지용 전해질 및 이를 포함하는 리튬 이차 전지 |
| US11824160B2 (en) * | 2018-03-12 | 2023-11-21 | Tesla, Inc. | Battery systems based on two-additive electrolyte systems including 2-furanone, and method of formation process of same |
Family Cites Families (13)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH0770326B2 (ja) * | 1986-06-09 | 1995-07-31 | 松下電器産業株式会社 | 有機電解質電池 |
| JPH0763023B2 (ja) * | 1986-06-09 | 1995-07-05 | 松下電器産業株式会社 | 有機電解質電池 |
| JPH0763015B2 (ja) * | 1987-11-18 | 1995-07-05 | 松下電器産業株式会社 | 有機電解質電池 |
| FR2673769B1 (fr) * | 1991-03-07 | 1993-06-18 | Centre Nat Rech Scient | Materiaux polymeriques a conduction ionique. |
| JPH0582168A (ja) * | 1991-09-25 | 1993-04-02 | Sanyo Electric Co Ltd | 非水系電解液電池 |
| US5432029A (en) * | 1993-05-14 | 1995-07-11 | Sharp Kabushiki Kaisha | Lithium secondary battery |
| JP3663897B2 (ja) * | 1998-03-20 | 2005-06-22 | 宇部興産株式会社 | リチウム二次電池用電解液およびそれを用いたリチウム二次電池 |
| JP3730491B2 (ja) * | 1999-07-28 | 2006-01-05 | 三菱化学株式会社 | 制御電極表面を有する電池 |
| JP4474715B2 (ja) * | 1999-10-13 | 2010-06-09 | パナソニック株式会社 | 非水電気化学装置およびその電解液 |
| JP2003163031A (ja) * | 2001-09-12 | 2003-06-06 | Daicel Chem Ind Ltd | 電解液及び非水電気化学装置、並びにα−置換オキシ−γ−ブチロラクトン誘導体 |
| JP2003243031A (ja) * | 2002-02-19 | 2003-08-29 | Japan Storage Battery Co Ltd | 非水電解質二次電池 |
| KR100467696B1 (ko) * | 2002-08-31 | 2005-01-24 | 삼성에스디아이 주식회사 | 유기 전해액 및 이를 채용한 리튬 전지 |
| KR100611462B1 (ko) * | 2003-10-08 | 2006-08-09 | 제일모직주식회사 | 전지용 비수 전해액 |
-
2004
- 2004-10-27 WO PCT/KR2004/002728 patent/WO2006046785A1/en active Application Filing
- 2004-10-27 EP EP04793586A patent/EP1807899A4/en not_active Withdrawn
- 2004-10-27 CN CNB2004800442961A patent/CN100454654C/zh not_active Expired - Fee Related
- 2004-10-27 US US11/718,031 patent/US20090226820A1/en not_active Abandoned
- 2004-10-27 JP JP2007537788A patent/JP2008518392A/ja active Pending
- 2004-10-29 TW TW093133152A patent/TWI259597B/zh not_active IP Right Cessation
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| Publication number | Publication date |
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| CN100454654C (zh) | 2009-01-21 |
| US20090226820A1 (en) | 2009-09-10 |
| WO2006046785A1 (en) | 2006-05-04 |
| JP2008518392A (ja) | 2008-05-29 |
| EP1807899A1 (en) | 2007-07-18 |
| EP1807899A4 (en) | 2009-11-11 |
| TW200614561A (zh) | 2006-05-01 |
| TWI259597B (en) | 2006-08-01 |
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