CN1233058C - 聚合物锂离子电池及其制造方法 - Google Patents

聚合物锂离子电池及其制造方法 Download PDF

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CN1233058C
CN1233058C CNB031498655A CN03149865A CN1233058C CN 1233058 C CN1233058 C CN 1233058C CN B031498655 A CNB031498655 A CN B031498655A CN 03149865 A CN03149865 A CN 03149865A CN 1233058 C CN1233058 C CN 1233058C
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CN1487617A (zh
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付治国
王春生
高国鹏
司宏君
穆艳梅
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Harbin Zhong Qiang Energy Technology Co., Ltd.
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HEILONGJIANG ZHONGQIANG ENERGY SOURCE SCIENCE AND TECHNOLOGY Co Ltd
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Abstract

本发明涉及一种大容量锂离子聚合物电池制作方法及由该方法制得的电池。该方法以金属锂盐和金属钴的氧化物制成正极浆料，直接喷涂到铝集流体上制成正极，以两种嵌锂式材料碳制成负极浆料，直接喷涂到铜集流体上制成负极，将聚偏二氟乙烯和气相二氧化硅、邻苯二甲酸二丁酯与丙酮混合，制成浆料，然后涂布在聚酯薄膜上制成隔膜，将正极、隔膜、负极制成的电池单体，萃取、焊极耳、浸渍电解液、用铝塑复合膜包装、化成后制得大容量锂离子聚合物电池。由于本发明中采用特殊的电极浆料配方及特殊的制作工艺，从而使电池充放电性能得到提高，更加符合动力电源使用，单体电池厚度可以控制在3mm以下，特别适合于作电动车辆上的动力电源使用。

Description

聚合物锂离子电池及其制造方法
技术领域
本发明属电化学技术领域，具体涉及一种大容量聚合物锂离子电池及其制造方法。
背景技术
大容量化学电源主要在动力方面使用，主要应用品种以铅酸电池、镍氢电池和锂离子电池为主，目前的大容量化学电池存在的问题是能量密度低、质量及体积大，这给其应用带来的很多不便。
发明内容
本发明的目的在于提供一种高能轻薄电池。本发明的另一目的还在于提供这种电池的制作方法。
本发明所涉及的是一种聚合物锂离子电池的制造方法，包括如下步骤：
1、正极的制备
(1)正极浆料的制备
本发明所涉及的大容量聚合物锂离子电池的正极应用的是金属锂盐和金属钴的氧化物，两种材料相互搀杂；将它与聚偏二氟乙烯(PVDF)、导电碳黑、邻苯二甲酸二丁酯充分混合后，溶解在丙酮中制成浆料；具体的重量比例如下：
锰酸锂或镍酸锂和钴氧化物的掺杂混合物49.89％-50.32％
聚偏二氟乙烯(PVDF)     8.99％-9.07％
导电碳黑               29.98％-30.24％
邻苯二甲酸二丁酯       10.7％-10.8％
(2)集流体的预处理
利用乙烯丙烯酸共聚物(EAA)、导电碳黑与丙酮混合制成集流体预处理浆料，将该浆料均匀的涂在铝集流体上，以增加与正极材料的粘合力，降低电池的内阻；
(3)正极的最后制备
将正极浆料均匀的涂敷在铝集流体上，然后再将涂敷后的正极放到平压机上，在一定的温度及压力下进行压制，制成正极；
2、负极的制备
(1)负极浆料的制备
本发明所涉及的大容量聚合物锂离子电池的负极应用的是两种嵌锂式材料碳相互掺杂；将它与聚偏二氟乙烯(PVDF)、导电碳黑、邻苯二甲酸二丁酯充分混合后，溶解在丙酮中制成浆料。具体的重量比例如下：
掺杂嵌锂式碳材料         53.19％-53.85％
聚偏二氟乙烯             6.99％-7.1％
导电碳黑                 24.47％-24.82％
邻苯二甲酸二丁酯         14.69％-14.89％
(2)负极的制备
将负极浆料均匀的涂敷在同样经过处理的铜集流体上，然后再将涂敷后的负极放到平压机上，在一定的温度及压力下进行压制，制成负极；
3、隔膜的制备
本发明所涉及的大容量聚合物锂离子电池的隔膜应用的是聚偏二氟乙烯(PVDF)膜，将聚偏二氟乙烯(PVDF)和气相二氧化硅、邻苯二甲酸二丁酯与丙酮混合，制成浆料，然后涂布在聚酯薄膜上，烘干后揭下聚酯薄膜，厚度在0.03mm以内；具体的重量比例如下：
聚偏二氟乙烯                    65.54％
气相二氧化硅                    21.35％
邻苯二甲酸二丁酯                13.11％
4、电池单体的制作
将一片正极、一片隔膜和一片负极层叠在一起，在平压机上进行热压，制成电池，厚度在3mm以内；
5、增塑剂的去除
将4中提到的电池单元用无水甲醇进行3次萃取，然后烘干；
6、焊集流体
用超声波焊接机将正、负极的铜、铝集流体与镍极耳焊在一起，作为电池的两极。
7、电解液的浸渍
将6中的电池浸渍在电解液中；
8、电池的包装
用铝塑复合膜将电池包装起来；
9、电池的化成
将8中的电池按适当的化成制度进行原始充放电试验。
将上述得到的单体电池可以按照使用要求进行适当的串并联，组装成实用的大容量电池组。
本发明还提供了采用上述方法制作的大容量聚合物锂离子电池，包括包装在铝塑复合膜内的电池单体，电池单体的正极与负极之间之间有隔膜，其特征在于：正极的集流体上涂敷的正极浆料组成为锰酸锂或镍酸锂和钴氧化物的掺杂混合物49.89％-50.32％、聚偏二氟乙烯8.99％-9.07％、导电碳黑29.98％-30.24％、邻苯二甲酸二丁酯10.7％-10.8％；负极的集流体上涂敷的负极浆料为掺杂嵌锂式碳材料53.19％-53.85％、聚偏二氟乙烯6.99％-7.1％、导电碳黑24.47％-24.82％、邻苯二甲酸二丁酯14.69％-14.89％。。
由于本发明中采用特殊的电极浆料配方及特殊的制作工艺，从而使电池充放电性能得到提高，更加符合动力电源使用，单体电池厚度可以控制在3mm以下，电池组整体体积仅为同容量铅酸电池的1/7，镍氢矿灯电池的1/4；重量仅为铅酸矿灯电池的1/3，镍氢矿灯电池的1/2，这种电池可用于多种领域，特别适合于作电动车辆上的动力电源使用。
具体实施方式
以下将本发明结合实例进行详细描述。
实例一
1、准备正极材料
(1)正极浆料的制备
锰酸(LiMn2O4)             182g
三氧化二钴(Co2O3)         49g
聚偏二氟乙烯(PVDF)           42g
邻苯二甲酸二丁酯             50g
导电碳黑                     140g
丙酮                         4340g
将上述材料在搅拌机里均匀搅拌制成浆料，搅拌速度6000r/min，时间120分钟。
(2)集流体预处理浆料的制备
导电碳黑                     45.5g
乙烯丙烯酸共聚物(EAA)        14g
丙酮                         560g
将以上材料在搅拌机里均匀搅拌制成浆料，搅拌速度6000r/min，时间30分钟。然后用喷网机将浆料喷在集流体上。
(3)正极的最后制备
将制备好的正极浆料放到喷涂机内，调整喷涂压力为3个大气压，距离为0.4m，出料孔径为0.017mm.均匀的涂在集流体上，然后放到烘干箱内烘干30分钟，烘干温度为55℃。
将烘干后的正极放到平压机上进行热压，热压温度100℃，然后分割成尺寸为100×180mm的矩形片。
2、准备负极材料
(1)负极浆料的制备：
中间相碳微球(MCMB)          84g
石墨                        70g
聚偏二氟乙烯(PVDF)          20g
邻苯二甲酸二丁酯            42g
导电碳黑                    70g
丙酮                        4270g
将上述材料在搅拌机里均匀搅拌制成浆料，搅拌速度5500r/min，时间100分钟。
(2)集流体预处理浆料的制备
导电碳黑                   45.5g
乙烯丙烯酸共聚物(EAA)      28g
丙酮                       210g
将以上材料在搅拌机里均匀搅拌制成浆料，搅拌速度6000r/min，时间30分钟。然后用喷网机将浆料喷在集流体上。
(3)负极的最后制备
将制备好的负极浆料放到喷涂机内，调整喷涂压力为3个大气压，距离为0.4m，出料孔径为0.015mm.均匀的涂在集流体上，然后放到烘干箱内烘干15分钟，烘干温度为55℃。
将烘干后的负极放到平压机上进行热压，热压温度100℃，然后分割成尺寸为100×180mm的矩形片。
3、准备隔膜材料
聚偏二氟乙烯(PVDF)            175g
气相二氧化硅                  57g
邻苯二甲酸二丁酯              35g
丙酮                          2450g
将上述材料在搅拌机内均匀混合，搅拌速度8000r/min，时间60分钟，然后在涂布机上进行涂布，涂布间隙为0.01mm，最终涂布厚度为0.005mm。
4、电池单元的合成
将上面方法制成的正极、负极、隔膜进行层叠，然后在热压机上进行热合，热合温度110℃，热合后厚度为2.65mm。
5、萃取
将合成后的电池放到甲醇中进行萃取，以提取电池中的增塑剂，分3次，每次30分钟，磁力搅拌器搅拌，然后在烘箱中进行烘干45分钟，温度50℃。
6、极耳的焊接
分别用镍条和铝条将电池的正、负极的集流体焊接在一起，形成电池的两个引出极。
7、电解液的浸渍与电池的包装
将电池在一种含有机溶剂为1∶1的碳酸乙烯酯和碳酸二乙酯混合物的1M六氟磷锂(LiPF6)溶液的电解质溶液中浸渍20分钟，除去多余的电解液，用铝塑复合膜包装材料将电池包装好。
8、电池的化成
将电池用0.5C放电制度进行化成，测试结果如下：
首次放电容量为15Ah，经0.5C500次循环后放电容量为14Ah。
9、电池组的组装
将8个上述单体电池并联组装成120Ah的电池块，而后根据电动车实际使用要求将88块这样的电池组串联，从而构成了动力车用电池组。
实例二
1、准备正极材料
(1)正极浆料的制备
镍酸锂(LiNiO2)            190g
四氧化三钴(Co3O4)       45g
聚偏二氟乙烯(PVDF)         42g
邻苯二甲酸二丁酯           50g
导电碳黑                   140g
丙酮                       4300g
将上述材料在搅拌机里均匀搅拌制成浆料，搅拌速度6000r/min，时间120分钟。
(2)集流体预处理浆料的制备
导电碳黑                    45.5g
乙烯丙烯酸共聚物(EAA)       14g
丙酮                        560g
将以上材料在搅拌机里均匀搅拌制成浆料，搅拌速度6000r/min，时间30分钟，然后用喷网机将浆料喷在集流体上。
(3)正极的最后制备
将制备好的正极浆料放到喷涂机内，调整喷涂压力为3个大气压，距离为0.4m，出料孔径为0.017mm.均匀的涂在集流体上，然后放到烘干箱内烘干30分钟，烘干温度为55℃。
将烘干后的正极放到平压机上进行热压，热压温度100℃，然后分割成尺寸为100×180mm的矩形片。
4、准备负极材料
(1)负极浆料的制备：
中间相碳微球(MCMB)        75g
石墨                      75g
聚偏二氟乙烯(PVDF)        20g
邻苯二甲酸二丁酯          42g
导电碳黑                  70g
丙酮                      4270g
将上述材料在搅拌机里均匀搅拌制成浆料，搅拌速度5500r/min，时间100分钟。
(2)集流体预处理浆料的制备
导电碳黑                    45.5g
乙烯丙烯酸共聚物(EAA)       28g
丙酮                        210g
将以上材料在搅拌机里均匀搅拌制成浆料，搅拌速度6000r/min，时间30分钟。然后用喷网机将浆料喷在集流体上。
(3)负极的最后制备
将制备好的负极浆料放到喷涂机内，调整喷涂压力为3个大气压，距离为0.4m，出料孔径为0.015mm.均匀的涂在集流体上，然后放到烘干箱内烘干15分钟，烘干温度为55℃。
将烘干后的负极放到平压机上进行热压，热压温度100℃，然后分割成尺寸为100×180mm的矩形片。
5、准备隔膜材料
聚偏二氟乙烯(PVDF)        175g
气相二氧化硅              57g
邻苯二甲酸二丁酯          35g
丙酮                      2450g
将上述材料在搅拌机内均匀混合，搅拌速度8000r/min，时间60分钟，然后在涂布机上进行涂布，涂布间隙为0.01mm，最终涂布厚度为0.005mm。
4、电池单元的合成
将上面方法制成的正极、负极、隔膜进行层叠，然后在热压机上进行热合，热合温度110℃，热合后厚度为2.7mm。
5、萃取
将合成后的电池放到甲醇中进行萃取，以提取电池中的增塑剂，分3次，每次30分钟，磁力搅拌器搅拌，然后在烘箱中进行烘干45分钟，温度50℃。
6、极耳的焊接
分别用镍条和铝条将电池的正、负极的集流体焊接在一起，形成电池的两个引出极。
7、电解液的浸渍与电池的包装
将电池在一种含有机溶剂为1∶1的碳酸乙烯酯和碳酸二乙酯混合物的1M六氟磷锂(LiPF6)溶液的电解质溶液中浸渍20分钟，除去多余的电解液，用铝逆复合膜包装材料将电池包装好。
8、电池的化成
将电池用0.5C放电制度进行化成，测试结果如下：
首次放电容量为15Ah，经0.5C500次循环后放电容量为14.3Ah。
9、电池组的组装
将8个上述单体电池并联组装成120Ah的电池块，而后根据电动车实际使用要求将86块这样的电池组串联，从而构成了动力车用电池组。

Claims (8)

1、一种聚合物锂离子电池的制作方法，包括以下步骤：
(1)正极的制备
将下述重量配比的原料混合后以丙酮为溶剂制备正极浆料：
锰酸锂或镍酸锂和钴氧化物的掺杂混合物49.89％-50.32％
聚偏二氟乙烯                8.99％-9.07％
导电碳黑                    29.98％-30.24％
邻苯二甲酸二丁酯            10.7％-10.8％
用乙烯丙烯酸共聚物、导电碳黑与丙酮混合制成铝集流体预处理浆料，将该浆料均匀的涂在铝集流体上，进行铝集流体的预处理；然后将正极浆料均匀的涂敷在铝集流体上，再将涂敷后的正极放到平压机上，在一定的温度及压力下进行压制，制成正极；
(2)负极的制备
将下述重量配比的原料混合后以丙酮为溶剂制备负极浆料：
掺杂嵌锂式碳材料            53.19％-53.85％
聚偏二氟乙烯                6.99％-7.1％
导电碳黑                    24.47％-24.82％
邻苯二甲酸二丁酯            14.69％-14.89％
用乙烯丙烯酸共聚物、导电碳黑与丙酮混合制成铜集流体预处理浆料，将该浆料均匀的涂在铜集流体上进行预处理，将负极浆料均匀的涂敷在经过处理的铜集流体上，然后再将涂敷后的负极放到平压机上，在一定的温度及压力下进行压制，制成负极；
(3)隔膜的制备
将下述原料按如下重量配比与丙酮混合制成浆料，然后涂布在聚酯薄膜上制备隔膜：
聚偏二氟乙烯                65.54％
气相二氧化硅                21.35％
邻苯二甲酸二丁酯            13.11％
(4)电池单体的制作
将一片正极、一片隔膜和一片负极层叠在一起，在平压机上进行热压，制成电池；
(5)增塑剂的去除
将上述电池单元用无水甲醇进行3次萃取，然后烘干；
(6)焊集流体
用超声波焊接机将正、负极的铜、铝集流体与镍极耳焊在一起，作为电池的两极；
(7)电解液的浸渍
将电池在电解质溶液中浸渍；
(8)用铝塑复合膜将电池包装起来；然后进行化成。
2、如权利要求1所述的聚合物锂离子电池的制作方法，其特征在于：所述的锰酸锂或镍酸锂在混合物中所占重量比例为78.79-80.85％；钴氧化物指的是三氧化二钴或四氧化三钴，在混合物中所占重量比例为21.21-19.15％。
3、如权利要求1所述的聚合物锂离子电池的制作方法，其特征在于：所述的掺杂嵌锂式碳材料指的是中间相碳微球或石墨或二者混合物。
4、如权利要求1所述的聚合物锂离子电池的制作方法，其特征在于：
所述的电解液指六氟磷锂的有机溶液，溶剂是碳酸乙烯酯和碳酸二乙酯的混合物。
5、如权利要求1所述的聚合物锂离子电池的制作方法，其特征在于：
所述的将正极浆料涂敷于铝集流体的过程是将正极材料直接喷涂到铝集流体上制得。
6、如权利要求1所述的聚合物锂离子电池的制作方法，其特征在于：
所述的将负极浆料涂敷于铜集流体的过程是将负极材料直接喷涂到铜集流体上制得。
7、如权利要求1所述的聚合物锂离子电池的制作方法，其特征在于：
所述的单体电池隔膜厚度在0.03mm以内。
8、一种由权利要求1所述的方法制得的聚合物锂离子电池，包括包装在铝塑复合膜内的电池单体，电池单体的正极与负极之间有隔膜，其特征在于：正极的集流体上涂敷的正极浆料组成为锰酸锂或镍酸锂和钴氧化物的掺杂混合物49.89％-50.32％、聚偏二氟乙烯8.99％-9.07％、导电碳黑29.98％-30.24％、邻苯二甲酸二丁酯10.7％-10.8％；负极的集流体上涂敷的负极浆料为掺杂嵌锂式碳材料53.19％-53.85％、聚偏二氟乙烯6.99％-7.1％、导电碳黑24.47％-24.82％、邻苯二甲酸二丁酯14.69％-14.89％。
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