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CN111029514B - 一种隔膜及包括该隔膜的高电压电池 - Google Patents

一种隔膜及包括该隔膜的高电压电池 Download PDF

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Publication number
CN111029514B
CN111029514B CN201911115315.XA CN201911115315A CN111029514B CN 111029514 B CN111029514 B CN 111029514B CN 201911115315 A CN201911115315 A CN 201911115315A CN 111029514 B CN111029514 B CN 111029514B
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parts
mass
ceramic particles
separator
diaphragm
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CN111029514A (zh
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张祖来
李素丽
李俊义
徐延铭
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Zhuhai Cosmx Battery Co Ltd
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Zhuhai Cosmx Battery Co Ltd
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Priority to CN201911115315.XA priority Critical patent/CN111029514B/zh
Publication of CN111029514A publication Critical patent/CN111029514A/zh
Priority to PCT/CN2020/128134 priority patent/WO2021093774A1/zh
Priority to CN202080077087.6A priority patent/CN114641890A/zh
Priority to EP20886697.0A priority patent/EP4050710B1/en
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Publication of CN111029514B publication Critical patent/CN111029514B/zh
Priority to US17/744,633 priority patent/US20220271329A1/en
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Abstract

本发明提供了一种隔膜及包括该隔膜的高电压电池。本发明是通过在无机陶瓷颗粒表面包覆一层改性层，所述改性层可以吸附电极材料析出的过渡金属离子，从而避免过渡金属离子在负极表面形成过渡金属析出物，提高电池的安全性、倍率性能和循环性能。同时，由于所述改性层是包覆在无机陶瓷颗粒表面的，因此并不会对电池的内阻产生明显的影响，从而不会降低电池的倍率、低温和循环性能。不仅如此，发明人还出人意料地发现所述改性材料的引入还可以实现对电池体系中产生的微量的HF的吸附，一方面可以抑制过渡金属离子的溶出，稳定正极表面结构，改善电池性能；另一方面可以降低HF对电池外包材料的腐蚀，改善电池安全性能。

Description

一种隔膜及包括该隔膜的高电压电池
技术领域
本发明属于锂离子电池技术领域，具体涉及一种适用于高电压电池体系的隔膜及包括该隔膜的电池。
背景技术
随着3C产品的普及和电动汽车市场的兴起，对锂离子二次电池的需求越来越高。由于在整个电池体系中不可避免的会掺入一些磁性金属颗粒或者金属离子，这些磁性金属颗粒或者金属离子在电池充放电过程中会在负极表面析出；另外，正极材料本身也存在过渡金属离子溶出的情况，该溶出的过渡金属离子也会在负极表面析出；尤其在高电压电池体系下，此类析出显得更加严重。
在负极表面析出的金属颗粒，一方面产生金属枝晶容易刺穿隔膜造成电池内部短路；另一方面影响锂离子的正常插入，影响电池长期循环等性能。
由于析出的磁性金属颗粒或者金属离子(包括过渡金属离子)存在上述问题，现有技术中曾报道过通过使用多孔陶瓷颗粒吸附的方式吸附过渡金属离子，此种方式由于使用多孔陶瓷颗粒，导致水分很高而对电性能产生不良影响。现有技术中还曾报道过在陶瓷隔膜表面增加一层过渡金属离子吸附层，此种方式不仅增加隔膜制造成本，同时也由于增加过渡金属离子吸附层恶化离子导通性，恶化电池的循环及倍率放电等性能。
发明内容
隔膜是锂离子二次电池中必不可少的元件，其主要作用是：一方面作为正负极之间的隔离物，防止正负极短路，保证电池的安全问题；另一方面作为正负极之间锂离子的通道，保证电池的正常工作。但是，本申请的发明人经过大量的实验研究，认为随着人们对电池性能的不断追求，作为电池的关键材料之一的隔膜，应该发挥更大的作用。
为了改善现有技术的不足，本发明的目的是提供一种陶瓷颗粒，以及包括所述陶瓷颗粒的隔膜和电池。
本发明是通过在无机陶瓷颗粒表面包覆一层改性层，所述改性层可以吸附电池体系中存在的金属离子(如正极材料析出的过渡金属离子，电池体系中掺入的金属离子或金属颗粒)，从而避免金属离子在负极表面形成金属析出物，提高电池的安全、倍率、循环等性能。同时，由于所述改性层是包覆在无机陶瓷颗粒表面的，因此并不会对电池的内阻产生明显的影响，从而不会降低电池的倍率、低温和循环性能。
本发明目的是通过如下技术方案实现的：
一种陶瓷颗粒，其中，所述陶瓷颗粒具有核壳结构，即包括壳层和核芯，形成所述壳层的材料包括改性材料，形成所述核芯的材料包括无机陶瓷材料；
所述改性材料选自取代的硅氧烷，形成取代基的化合物选自含有羧基的胺类化合物，或者选自含氮的杂环化合物。
根据本发明，所述含有羧基的胺类化合物例如选自含有至少两个羧基的多元胺类化合物，再例如选自乙二胺四乙酸、丙二胺四乙酸、羟乙基乙二胺三乙酸、乙二醇二乙醚二胺四乙酸中的一种或两种以上。
根据本发明，所述含氮的杂环化合物例如选自含有一个氮或两个氮的杂环化合物，例如选自吡啶、咪唑中的一种或两种以上。
根据本发明，所述硅氧烷选自含有氨基的硅氧烷；其中，通过硅氧烷中的氨基被上述化合物取代而得到所述取代的硅氧烷。所述含有氨基的硅氧烷例如为3-氨丙基三甲氧基硅烷、3-氨丙基三乙氧基硅烷、2-氨乙基三甲氧基硅烷、2-氨乙基三乙氧基硅烷中的一种或多种。
根据本发明，所述陶瓷颗粒可以用于锂离子电池领域。
根据本发明，所述无机陶瓷材料选自氧化铝、氧化镁、勃姆石、硫酸钡、钛酸钡、氧化锌、氧化钙、二氧化硅、碳化硅、氧化镍中的一种或两种以上。
根据本发明，所述壳层也称为改性层。
根据本发明，所述壳层的厚度为5nm-1000nm，优选为50nm-500nm。例如为5nm、10nm、50nm、100nm、200nm、500nm或1000nm。
根据本发明，所述无机陶瓷材料的平均粒径为0.01μm-20μm。例如为0.01μm、0.05μm、0.1μm、0.5μm、1μm、4μm、5μm、8μm、10μm、12μm、15μm、18μm或20μm。
根据本发明，所述陶瓷颗粒中，包覆于无机陶瓷材料表面的改性材料形成的改性层(即所述壳层)可以吸附从正极析出的过渡金属离子，从而避免过渡金属离子在负极表面形成过渡金属析出物，提高电池的安全、倍率、循环等性能。
本发明还提供上述陶瓷颗粒的制备方法，所述方法包括如下步骤：
采用硅烷化处理法，将包括改性材料的形成壳层的材料包覆在包括无机陶瓷材料的形成核芯的材料表面，制备得到所述陶瓷颗粒；其中，所述陶瓷颗粒具有核壳结构，即包括壳层和核芯，形成所述壳层的材料包括改性材料，形成所述核芯的材料包括无机陶瓷材料。
示例性地，所述硅烷化处理法包括如下步骤：
将形成壳层的材料通过搅拌方式加入到溶剂中形成含有形成壳层的材料的溶液；在前述溶液中加入形成核芯的材料，搅拌混合均匀；通过真空加热干燥或喷雾干燥等除去混合体系中的溶剂，得到所述陶瓷颗粒，其中，所述陶瓷颗粒具有核壳结构，即包括壳层和核芯，形成所述壳层的材料包括改性材料，形成所述核芯的材料包括无机陶瓷材料。
其中，所述溶剂选自醇类有机溶剂，具体的为甲醇、乙醇、丙醇、乙二醇、丙二醇、丙三醇的至少一种。
本发明还提供一种隔膜，所述隔膜包括隔膜基层和位于隔膜基层至少一侧表面的涂覆层，所述涂覆层由包括上述陶瓷颗粒的混合体系在隔膜基层至少一侧表面涂覆得到。
根据本发明，所述涂覆层的厚度为1-10μm，例如为2-5μm，如1μm、2μm、3μm、4μm、5μm、6μm、7μm、8μm、9μm、10μm，所述厚度的涂覆层可以是一次涂覆得到的，也可以是多次涂覆得到的。
根据本发明，若所述隔膜包括隔膜基层和位于隔膜基层两侧表面的涂覆层，则两侧表面的涂覆层的厚度相同或不同。
根据本发明，所述混合体系中还包括聚合物粘结剂和助剂中的至少一种。例如，所述混合体系中还包括聚合物粘结剂和助剂。
根据本发明，所述混合体系中各组分的质量份数如下所示：
50-95质量份的上述陶瓷颗粒、5-40质量份的聚合物粘结剂和0-10质量份的助剂。
例如，所述混合体系中各组分的质量份数如下所示：
60-95质量份的上述陶瓷颗粒、10-30质量份聚合物粘结剂和0-5质量份助剂。
示例性地，上述陶瓷颗粒的质量份为50、55、60、65、70、75、80、85、90或95质量份。
示例性地，上述聚合物粘结剂的质量份为5、6、7、8、9、10、15、20、25、30、35或40质量份。
示例性地，上述助剂的质量份为1、2、3、4、5、6、7、8、9或10质量份。
根据本发明，所述混合体系还包括100-5000质量份的溶剂，例如还包括500-2000质量份的溶剂。
根据本发明，所述聚合物粘结剂选自聚四氟乙烯、聚偏氟乙烯、聚偏氟乙烯-六氟丙烯、聚酰亚胺、聚丙烯腈、聚(甲基)丙烯酸甲酯、芳纶树脂、聚(甲基)丙烯酸、丁苯橡胶(SBR)、聚乙烯醇、聚醋酸乙烯酯、羧甲基纤维素(CMC)、羧甲基纤维素钠(CMC-Na)、羧乙基纤维素、聚丙烯酰胺、酚醛树脂、环氧树脂、水性聚氨酯、乙烯-醋酸乙烯共聚物、多元丙烯酸类共聚物、聚苯乙烯磺酸锂、水性有机硅树脂、丁腈-聚氯乙烯共混物、苯丙乳胶、纯苯乳胶等及由前述聚合物改性衍生的共混、共聚聚合物中的一种或多种组合。
根据本发明，所述助剂选自多支链醇、磷酸三乙酯、聚乙二醇、氟化聚氧化乙烯、聚氧化乙烯、硬脂酸、十二烷基苯磺酸钠、十六烷基磺酸钠、脂肪酸甘油酯，山梨坦脂肪酸酯和聚山梨酯中的至少一种。
根据本发明，所述溶剂选自水、甲醇、乙醇、丙酮、N-甲基-2-吡咯烷酮(NMP)、氯仿、二甲苯、四氢呋喃、邻氯苯甲醛、六氟异丙醇、N,N-二甲基甲酰胺、N,N-二甲基乙酰胺、丁酮和乙腈中的至少一种。
本发明还提供上述隔膜的制备方法，其中，所述方法包括如下步骤：
(a)将上述的陶瓷颗粒、任选地聚合物粘结剂和任选地助剂加入到溶剂中，混合，得到混合浆料；
(b)将步骤(a)的混合浆料涂覆在隔膜基层表面，经干燥后得到所述隔膜。
根据本发明，步骤(a)中，所述混合浆料中，上述陶瓷颗粒、任选地聚合物粘结剂、任选地助剂和溶剂的质量份数如下所示：
50-95质量份的上述陶瓷颗粒、5-40质量份的聚合物粘结剂、0-10质量份的助剂和100-5000质量份溶剂。
例如，所述混合体系中各组分的质量份数如下所示：
60-95质量份的上述陶瓷颗粒、10-30质量份聚合物粘结剂、0-5质量份助剂和500-2000质量份溶剂。
根据本发明，步骤(b)中，所述涂覆的方式例如为喷涂、浸涂、凹版印刷、挤压涂覆、转移涂覆等。
根据本发明，步骤(b)中，所述隔膜基层的孔隙率为20％-80％、厚度为5μm-50μm、平均孔径大小为D<80nm；所述隔膜基层的材料体系选自聚乙烯、聚丙烯、聚对苯二甲酸乙二酯、聚对苯二甲酸丁二酯、聚苯乙烯、聚萘体系聚合物、聚酰亚胺、聚酰胺、芳纶和聚对苯撑苯并二唑等中的至少一种。
本发明还提供一种锂离子电池，所述锂离子电池包括上述的隔膜。
根据本发明，所述锂离子电池还包括正极、负极和电解液。
根据本发明，所述锂离子电池为高电压锂离子电池。
本发明的有益效果：
本发明提供了一种隔膜及包括该隔膜的高电压电池。本发明是通过在无机陶瓷颗粒表面包覆一层改性层，所述改性层可以吸附电极材料析出的过渡金属离子，从而避免过渡金属离子在负极表面形成过渡金属析出物，提高电池的安全性、倍率性能和循环性能。同时，由于所述改性层是包覆在无机陶瓷颗粒表面的，因此并不会对电池的内阻产生明显的影响，从而不会降低电池的倍率、低温和循环性能。不仅如此，发明人还出人意料地发现所述改性材料的引入还可以实现对电池体系中产生的微量的HF的吸附，一方面可以抑制过渡金属离子的溶出，稳定正极表面结构，改善电池性能；另一方面可以降低HF对电池外包材料的腐蚀，改善电池安全性能。
附图说明
图1：本发明的陶瓷颗粒的改性反应示意图。
图2：本发明的陶瓷颗粒吸附过渡金属离子的示意图。
图3：本发明的锂离子电池的电芯结构示意图。
图4：使用实施例1和对比例1隔膜的电池循环测试结果图。
图5：使用实施例1和对比例1隔膜的电池倍率测试结果图。
具体实施方式
下文将结合具体实施例对本发明的制备方法做更进一步的详细说明。应当理解，下列实施例仅为示例性地说明和解释本发明，而不应被解释为对本发明保护范围的限制。凡基于本发明上述内容所实现的技术均涵盖在本发明旨在保护的范围内。
下述实施例中所使用的实验方法如无特殊说明，均为常规方法；下述实施例中所用的试剂、材料等，如无特殊说明，均可从商业途径得到。
实施例1
将20份改性材料通过搅拌方式溶解于乙醇中，形成混合溶液，加入200份三氧化二铝，搅拌混合均匀后，通过真空加热干燥技术除去混合物中的溶剂，得到改性材料包覆陶瓷材料的颗粒，所述改性材料选自乙二胺四乙酸取代的3-氨丙基三甲氧基硅烷。
制备得到的陶瓷颗粒中，壳层为包含乙二胺四乙酸取代的3-氨丙基三甲氧基硅烷的改性材料，核芯为三氧化二铝；壳层和核芯的质量比为20:200，壳层的厚度为10nm，陶瓷颗粒的平均粒径约为0.8μm。
将80份上述制备得到的陶瓷颗粒、20份聚偏氟乙烯-六氟丙烯和2份聚乙二醇加入到900份N,N-二甲基乙酰胺中，均匀混合后得到混合浆料，将混合浆料通过微凹版涂覆在隔膜基层表面，经干燥后得到所述隔膜。
所述隔膜为厚度为9μm的湿法基材隔膜，单面涂覆，涂层厚度为3μm，隔膜总面密度为10.6g/m2。
将上述隔膜与正极、负极采用叠片或卷绕等方法，制备锂离子电池电芯，经烘烤、注液、化成、封装后得到高安全锂离子电池。
实施例2
将20份改性材料通过搅拌方式溶解于乙醇中，形成混合溶液，加入200份勃姆石，搅拌混合均匀后，通过真空加热干燥技术除去混合物中的溶剂，得到改性材料包覆陶瓷材料的颗粒，所述改性材料选自羟乙基乙二胺三乙酸取代的3-氨丙基三甲氧基硅烷。
制备得到的陶瓷颗粒中，壳层为包含羟乙基乙二胺三乙酸取代的3-氨丙基三甲氧基硅烷的改性材料，核芯为勃姆石；壳层和核芯的质量比为20:200，壳层的厚度为10nm，陶瓷颗粒的平均粒径约为0.8μm。
隔膜和锂离子电池的制备方法同实施例1，区别在于使用上述制备得到的陶瓷颗粒。
实施例3
将20份改性材料通过搅拌方式溶解于乙二醇中，形成混合溶液，加入200份三氧化二铝，搅拌混合均匀后，通过真空加热干燥技术除去混合物中的溶剂，得到改性材料包覆陶瓷材料的颗粒，所述改性材料选自吡啶取代的3-氨丙基三甲氧基硅烷。
制备得到的陶瓷颗粒中，壳层为包含吡啶取代的3-氨丙基三甲氧基硅烷的改性材料，核芯为三氧化二铝；壳层和核芯的质量比为20:200，壳层的厚度为10nm，陶瓷颗粒的平均粒径约为0.8μm。
隔膜和锂离子电池的制备方法同实施例1，区别在于使用上述制备得到的陶瓷颗粒。
实施例4
将20份改性材料通过搅拌方式溶解于丙二醇中，形成混合溶液，加入200份三氧化二铝，搅拌混合均匀后，通过真空加热干燥技术除去混合物中的溶剂，得到改性材料包覆陶瓷材料的颗粒，所述改性材料选自咪唑取代的3-氨丙基三甲氧基硅烷。
制备得到的陶瓷颗粒中，壳层为包含咪唑取代的3-氨丙基三甲氧基硅烷的改性材料，核芯为三氧化二铝；壳层和核芯的质量比为50:200，壳层的厚度为20nm，陶瓷颗粒的平均粒径约为0.9μm。
隔膜和锂离子电池的制备方法同实施例1，区别在于使用上述制备得到的陶瓷颗粒。
实施例5
将20份改性材料通过搅拌方式溶解于丙二醇中，形成混合溶液，加入200份氧化镁，搅拌混合均匀后，通过真空加热干燥技术除去混合物中的溶剂，得到改性材料包覆陶瓷材料的颗粒，所述改性材料选自咪唑取代的3-氨丙基三甲氧基硅烷。
制备得到的陶瓷颗粒中，壳层为包含咪唑取代的3-氨丙基三甲氧基硅烷的改性材料，核芯为氧化镁；壳层和核芯的质量比为100:200，壳层的厚度为40nm，陶瓷颗粒的平均粒径约为1.0μm。
隔膜和锂离子电池的制备方法同实施例1，区别在于使用上述制备得到的陶瓷颗粒。
实施例6
改性材料包覆陶瓷材料的颗粒的制备同实施例1。
将60份上述制备得到的陶瓷颗粒、40份聚(甲基)丙烯酸甲酯和4份聚乙二醇加入到900份N,N-二甲基乙酰胺中，均匀混合后得到混合浆料，将混合浆料通过微凹版涂覆在隔膜基层表面，经干燥后得到所述隔膜。
所述隔膜为厚度为9μm的湿法基材隔膜，单面涂覆，涂层厚度为3μm，隔膜总面密度为10.6g/m2。
将上述隔膜与正极、负极采用叠片或卷绕等方法，制备锂离子电池电芯，经烘烤、注液、化成、封装后得到高安全锂离子电池。
实施例7
改性材料包覆陶瓷材料的颗粒的制备同实施例1。
将95份上述制备得到的陶瓷颗粒、5份丁苯橡胶加入到900份N-甲基-2-吡咯烷酮(NMP)中，均匀混合后得到混合浆料，将混合浆料通过微凹版涂覆在隔膜基层表面，经干燥后得到所述隔膜。
所述隔膜为厚度为9μm的湿法基材隔膜，单面涂覆，涂层厚度为3μm，隔膜总面密度为10.6g/m2。
将上述隔膜与正极、负极采用叠片或卷绕等方法，制备锂离子电池电芯，经烘烤、注液、化成、封装后得到高安全锂离子电池。
对比例1
将80份氧化铝的陶瓷颗粒、20份聚偏氟乙烯-六氟丙烯和2份聚乙二醇加入到900份N,N-二甲基乙酰胺中，均匀混合后得到混合浆料，将混合浆料通过微凹版涂覆在隔膜基层表面，经干燥后得到所述隔膜。
所述隔膜为厚度为9μm的湿法基材隔膜，单面涂覆，涂层厚度为3μm，隔膜总面密度为10.6g/m2。
将上述隔膜与正极、负极采用叠片或卷绕等方法，制备锂离子电池电芯，经烘烤、注液、化成、封装后得到高安全锂离子电池。
对比例2
将20份包含乙二胺四乙酸、80份氧化铝的陶瓷颗粒、20份聚偏氟乙烯-六氟丙烯和2份聚乙二醇加入到900份N,N-二甲基乙酰胺中，均匀混合后得到混合浆料，将混合浆料通过微凹版涂覆在隔膜基层表面，经干燥后得到所述隔膜。
所述隔膜为厚度为9μm的湿法基材隔膜，单面涂覆，涂层厚度为3μm，隔膜总面密度为10.6g/m2。
将上述隔膜与正极、负极采用叠片或卷绕等方法，制备锂离子电池电芯，经烘烤、注液、化成、封装后得到高安全锂离子电池。
测试例1
将实施例1-7、对比例1-2制备的锂离子电池进行电压测试和内阻测试，测试过程是将实施例1-7、对比例1-2制备的锂离子电池充满电后置于25℃、50％湿度的环境中，用电压内阻仪(安柏-Applent，型号AT526B)测试电池满电状态下的电压和内阻，结果如表1所示。
表1实施例1-7、对比例1-2的锂离子电池的电压测试和内阻测试结果
样品编号 锂电池平均电压 锂离子电池内阻
实施例1 4.2016V 12.18mΩ
实施例2 4.2011V 12.32mΩ
实施例3 4.2012V 11.98mΩ
实施例4 4.2008V 12.21mΩ
实施例5 4.2011V 11.97mΩ
实施例6 4.2009V 11.87mΩ
实施例7 4.2003V 12.05mΩ
对比例1 4.2010V 12.36mΩ
对比例2 4.2017V 18.35mΩ
实施例1-7采用的改性材料包覆陶瓷材料的颗粒应用在隔膜中并组装成锂离子电池，通过表1的数据得知，实施例1-7和对比例1-2制备的锂离子电池分选后，电压正常，但对比例2内阻明显增加，这主要是由于在浆料中直接加入改性材料会影响锂离子的通透性；
将实施例1、对比例1制备的锂离子电池进行充放电循环和倍率性能测试，充放电循环测试采用1C充电/1C放电的制度进行测试；倍率性能测试采用0.2C充电/0.2C、0.5C、1C、3C、5C放电的制度进行测试，结果如图4和图5所示，从图4和图5中可以看出，实施例1的电池不仅在循环后期能保持良好的容量保持率，而且在电池高倍率放电下能保持很好的容量保持率。
通过对比实施例1-7、对比例1-2的实验结果，得出以下结论：
1、直接将改性材料加入到涂层中，应用在锂离子电池隔膜中，改性材料会影响锂离子电池中锂离子的通透性，导致锂离子电池的内阻增加；
2、实施例1-7中采用改性材料包覆陶瓷材料的颗粒并应用在锂离子电池隔膜中，不影响锂离子电池内阻、不影响锂离子电池电压、不影响锂离子电池充放电循环，满足应用需求。
测试例2
将实施例1-7、对比例1-2制备的锂离子电池隔膜进行金属离子测试，测试过程如下：
取100mm*100mm大小的实施例1-7、对比例1-2制备的隔膜片，分别放置于装有100mL的0.1wt％含量CoCl2水溶液烧杯中，再将烧杯置于150℃的加热板上放置30min，待冷却后取出隔膜，对其进行ICP测试分析。
ICP测试结果如下：
样品编号 Co含量(PPM)
实施例1 177
实施例2 181
实施例3 183
实施例4 205
实施例5 227
实施例6 178
实施例7 182
对比例1 126
对比例2 183
通过以上数据可以看出：加入改性陶瓷颗粒后的隔膜对金属离子的吸附能力有显著的提升。
测试例3
将实施例1、对比例1制备的锂离子电池循环后进行拆解，对其隔膜和负极进行ICP检测，检测结果如下：
样品编号 隔膜(ppm) 负极(ppm)
实施例1 1275 336
对比例1 267 1130
通过以上数据可以看出：加入改性陶瓷颗粒后的隔膜对金属离子的吸附能力有显著的提升，从而保证电池的循环性能。
以上，对本发明的实施方式进行了说明。但是，本发明不限定于上述实施方式。凡在本发明的精神和原则之内，所做的任何修改、等同替换、改进等，均应包含在本发明的保护范围之内。

Claims (18)

1.一种用于隔膜涂覆层中的陶瓷颗粒，其中，所述陶瓷颗粒具有核壳结构，即包括壳层和核芯，形成所述壳层的材料包括改性材料，形成所述核芯的材料包括无机陶瓷材料；
所述改性材料选自取代的硅氧烷，形成取代基的化合物选自含有羧基的胺类化合物，或者选自含氮的杂环化合物；
所述含有羧基的胺类化合物选自含有至少两个羧基的多元胺类化合物，所述含有至少两个羧基的多元胺类化合物选自乙二胺四乙酸、丙二胺四乙酸、羟乙基乙二胺三乙酸、乙二醇二乙醚二胺四乙酸中的一种或两种以上；
所述含氮的杂环化合物选自吡啶、咪唑中的一种或两种；
所述硅氧烷选自含有氨基的硅氧烷，所述含有氨基的硅氧烷选自3-氨丙基三甲氧基硅烷、3-氨丙基三乙氧基硅烷、2-氨乙基三甲氧基硅烷、2-氨乙基三乙氧基硅烷中的一种或多种。
2.根据权利要求1所述的陶瓷颗粒，其中，所述无机陶瓷材料选自氧化铝、氧化镁、勃姆石、硫酸钡、钛酸钡、氧化锌、氧化钙、二氧化硅、碳化硅、氧化镍中的一种或两种以上。
3.根据权利要求1所述的陶瓷颗粒，其中，所述壳层的厚度为5nm-1000nm。
4.根据权利要求1-3任一项所述的陶瓷颗粒，其中，所述无机陶瓷材料的平均粒径为0.01μm-20μm。
5.权利要求1-4任一项所述的用于隔膜涂覆层中的陶瓷颗粒的制备方法，所述方法包括如下步骤：
采用硅烷化处理法，将包括改性材料的形成壳层的材料包覆在包括无机陶瓷材料的形成核芯的材料表面，制备得到所述用于隔膜涂覆层中的陶瓷颗粒；其中，所述用于隔膜涂覆层中的陶瓷颗粒具有核壳结构，即包括壳层和核芯，形成所述壳层的材料包括改性材料，形成所述核芯的材料包括无机陶瓷材料。
6.根据权利要求5所述的用于隔膜涂覆层中的陶瓷颗粒的制备方法，其中，所述硅烷化处理法包括如下步骤：
将形成壳层的材料通过搅拌方式加入到溶剂中形成含有形成壳层的材料的溶液；在前述溶液中加入形成核芯的材料，搅拌混合均匀；通过真空加热干燥或喷雾干燥除去混合体系中的溶剂，得到所述用于隔膜涂覆层中的陶瓷颗粒，其中，所述用于隔膜涂覆层中的陶瓷颗粒具有核壳结构，即包括壳层和核芯，形成所述壳层的材料包括改性材料，形成所述核芯的材料包括无机陶瓷材料。
7.一种隔膜，所述隔膜包括隔膜基层和位于隔膜基层至少一侧表面的涂覆层，所述涂覆层由包括权利要求1-4任一项所述用于隔膜涂覆层中的陶瓷颗粒的混合体系在隔膜基层至少一侧表面涂覆得到。
8.根据权利要求7所述的隔膜，其中，所述涂覆层的厚度为1-10μm；所述厚度的涂覆层是一次涂覆得到的，或者是多次涂覆得到的。
9.根据权利要求7或8所述的隔膜，其中，若所述隔膜包括隔膜基层和位于隔膜基层两侧表面的涂覆层，则两侧表面的涂覆层的厚度相同或不同。
10.根据权利要求7所述的隔膜，其中，所述混合体系中还包括聚合物粘结剂和助剂中的至少一种。
11.根据权利要求10所述的隔膜，其中，所述混合体系中各组分的质量份数如下所示：
50-95质量份的用于隔膜涂覆层中的陶瓷颗粒、5-40质量份的聚合物粘结剂和0-10质量份的助剂。
12.根据权利要求11所述的隔膜，其中，所述混合体系中各组分的质量份数如下所示：
60-95质量份的用于隔膜涂覆层中的陶瓷颗粒、10-30质量份聚合物粘结剂和0-5质量份助剂。
13.根据权利要求10所述的隔膜，其中，所述混合体系还包括100-5000质量份的溶剂。
14.权利要求7-13任一项所述的隔膜的制备方法，其中，所述方法包括如下步骤：
(a)将权利要求1-4任一项所述的用于隔膜涂覆层中的陶瓷颗粒、聚合物粘结剂和助剂加入到溶剂中，混合，得到混合浆料；
(b)将步骤(a)的混合浆料涂覆在隔膜基层表面，经干燥后得到所述隔膜。
15.根据权利要求14所述的隔膜的制备方法，其中，步骤(a)中，所述混合浆料中，用于隔膜涂覆层中的陶瓷颗粒、聚合物粘结剂、助剂和溶剂的质量份数如下所示：
50-95质量份的用于隔膜涂覆层中的陶瓷颗粒、5-40质量份的聚合物粘结剂、0-10质量份的助剂和100-5000质量份溶剂。
16.根据权利要求15所述的隔膜的制备方法，其中，所述混合体系中各组分的质量份数如下所示：
60-95质量份的用于隔膜涂覆层中的陶瓷颗粒、10-30质量份聚合物粘结剂、0-5质量份助剂和500-2000质量份溶剂。
17.一种锂离子电池，所述锂离子电池包括权利要求7-13任一项所述的隔膜。
18.根据权利要求17所述的锂离子电池，其中，所述锂离子电池还包括正极、负极和电解液。
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