CN117203826A - 用于二次电池的铝软包膜 - Google Patents
用于二次电池的铝软包膜 Download PDFInfo
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- CN117203826A CN117203826A CN202180090906.5A CN202180090906A CN117203826A CN 117203826 A CN117203826 A CN 117203826A CN 202180090906 A CN202180090906 A CN 202180090906A CN 117203826 A CN117203826 A CN 117203826A
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- China
- Prior art keywords
- aluminum
- resin
- layer
- resin layer
- acid
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
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- -1 polypropylene Polymers 0.000 claims abstract description 118
- 229920005989 resin Polymers 0.000 claims abstract description 103
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- 229920000219 Ethylene vinyl alcohol Polymers 0.000 claims abstract description 34
- FPYJFEHAWHCUMM-UHFFFAOYSA-N maleic anhydride Chemical compound O=C1OC(=O)C=C1 FPYJFEHAWHCUMM-UHFFFAOYSA-N 0.000 claims abstract description 21
- 229920005672 polyolefin resin Polymers 0.000 claims abstract description 18
- 239000004715 ethylene vinyl alcohol Substances 0.000 claims abstract description 17
- 239000010410 layer Substances 0.000 claims description 114
- 239000012790 adhesive layer Substances 0.000 claims description 29
- 229920000098 polyolefin Polymers 0.000 claims description 24
- 229920001577 copolymer Polymers 0.000 claims description 18
- 239000007901 soft capsule Substances 0.000 claims description 13
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- 239000000126 substance Substances 0.000 claims description 10
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- VGGSQFUCUMXWEO-UHFFFAOYSA-N Ethene Chemical compound C=C VGGSQFUCUMXWEO-UHFFFAOYSA-N 0.000 claims description 4
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- 229910052742 iron Inorganic materials 0.000 description 6
- 229910052757 nitrogen Inorganic materials 0.000 description 6
- DVKJHBMWWAPEIU-UHFFFAOYSA-N toluene 2,4-diisocyanate Chemical compound CC1=CC=C(N=C=O)C=C1N=C=O DVKJHBMWWAPEIU-UHFFFAOYSA-N 0.000 description 6
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- SVTBMSDMJJWYQN-UHFFFAOYSA-N 2-methylpentane-2,4-diol Chemical compound CC(O)CC(C)(C)O SVTBMSDMJJWYQN-UHFFFAOYSA-N 0.000 description 4
- WSQZNZLOZXSBHA-UHFFFAOYSA-N 3,8-dioxabicyclo[8.2.2]tetradeca-1(12),10,13-triene-2,9-dione Chemical compound O=C1OCCCCOC(=O)C2=CC=C1C=C2 WSQZNZLOZXSBHA-UHFFFAOYSA-N 0.000 description 4
- NIXOWILDQLNWCW-UHFFFAOYSA-M Acrylate Chemical compound [O-]C(=O)C=C NIXOWILDQLNWCW-UHFFFAOYSA-M 0.000 description 4
- 239000005058 Isophorone diisocyanate Substances 0.000 description 4
- XMUZQOKACOLCSS-UHFFFAOYSA-N [2-(hydroxymethyl)phenyl]methanol Chemical class OCC1=CC=CC=C1CO XMUZQOKACOLCSS-UHFFFAOYSA-N 0.000 description 4
- 239000001361 adipic acid Substances 0.000 description 4
- 235000011037 adipic acid Nutrition 0.000 description 4
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- ZFSLODLOARCGLH-UHFFFAOYSA-N isocyanuric acid Chemical compound OC1=NC(O)=NC(O)=N1 ZFSLODLOARCGLH-UHFFFAOYSA-N 0.000 description 4
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Abstract
本发明提供了一种用于二次电池的铝软包膜,所述铝软包膜包括:铝膜层;沉积在所述铝膜层的一个表面上的外部树脂层;和沉积在所述铝膜层的另一表面上的内部树脂层,其中,所述内部树脂层包含聚烯烃树脂、乙烯乙烯醇共聚物(EVOH)和马来酸酐聚丙烯(MAHPP)树脂。
Description
技术领域
本申请要求于2020年12月18日提交的韩国专利申请No.10-2020-0179039和于2021年11月24日提交的韩国专利申请No.10-2021-0163362的优先权的权益,该两项专利申请的全部内容通过引用并入本说明书中。
本发明涉及一种用于二次电池的铝软包膜(aluminum pouch film)。
背景技术
锂二次电池是指通过锂离子迁移而产生电流的电池,并且使用用于二次电池的软包作为用于包装的外部材料以保护这种二次电池。这种用于二次电池的软包具有插设的铝薄膜,以便保护由电极组件和通过后续工艺填充在其中的电解质溶液形成的电池单体,并稳定地保持电池单体的电化学性能等。
在铝薄膜的一个表面上,将功能性聚合物膜层如聚对苯二甲酸乙二醇酯(PET)树脂、聚萘二甲酸乙二醇酯(PEN)树脂、尼龙树脂或液晶聚合物(LCP)树脂层压为外部树脂层,以便保护电池单体免受外界冲击的影响。
另外,在铝薄膜的另一表面上,内部树脂层由聚烯烃如聚乙烯(PE)、流延聚丙烯(cPP)或聚丙烯(PP)或它们的共聚物形成内部树脂层,以便用于上软包的下表面与下软包的上表面之间的粘合。
通常,形成用于二次电池的铝软包的上软包膜具有如图1中所示的其中顺序地层压了外部树脂层、粘合层、铝膜层、粘合层和内部树脂层的结构,并且下软包膜具有其中顺序地层压了内部树脂层、粘合层、铝膜层、粘合层和外部树脂层的结构。
具有上述结构的用于二次电池的铝软包可能由于各种过程中的各种原因而损坏。例如,在将电极组件存储在软包内的过程中,伸出部分如电极接头或电极引线引起诸如软包内的PP或CPP层上的裂纹的损坏,并且铝膜层会由于这种损坏而暴露。
如上所述的暴露于电解质溶液的铝膜层会通过与电解质溶液、氧气或水分发生化学反应而被腐蚀,并且可以通过其产生腐蚀气体,引起膨胀电池内部的膨胀现象。
此外,LiPF6等电解质溶液可以与水和氧气反应以产生腐蚀气体氢氟酸(HF),这种氢氟酸可以与铝反应以引起快速放热反应,并且可以吸附在铝表面上作为二次反应以在软包膜上引起裂纹。
因此,已经研究了各种铝表面改性技术以便防止如上所述的腐蚀性氢氟酸与铝接触。作为铝表面改性技术,可以包括热处理或其它化学转化处理、溶胶-凝胶涂覆、底漆处理、电晕处理、等离子体处理等。
然而,用这些现有技术解决上述问题似乎存在限制。
[现有技术文献]
[专利文献]
韩国特许专利公开No.10-2016-0077968
发明内容
技术问题
已经做出本发明以解决上述问题,并且本发明旨在提供一种用于二次电池的铝软包膜,该铝软包膜通过包括在防止氧气和水分透过的性能、粘合性能和防止HF气体透过的性能方面优异的内部树脂层,在高温和高湿度环境下具有优异的长期可靠性并具有优异的耐久性和安全性。
技术方案
为了实现上述目的,本发明提供了一种用于二次电池的铝软包膜,该铝软包膜包括:
铝膜层;
外部树脂层,该外部树脂层层压在所述铝膜层的一个表面上;和
内部树脂层,该内部树脂层层压在所述铝膜层的另一表面上,
其中,所述内部树脂层包含聚烯烃树脂、乙烯乙烯醇共聚物(EVOH)和马来酸酐聚丙烯(MAHPP)树脂。
有益效果
根据本发明的用于二次电池的铝软包膜包括:在防止氧气透过的性能、粘合性能和防止HF气体透过的性能方面优异的内部树脂层,使得由于防止氧气和水分透过的效果而抑制在电池内部产生HF气体,防止在电池内部产生的HF气体透过并与铝膜层发生化学反应,并且显著地改善在高温和高湿度环境下的长期可靠性,从而提供显著地改善二次电池的耐久性和安全性的效果。
附图说明
图1是示出了用于二次电池的铝软包膜的结构的模拟图。
图2是通过测量具有本发明的实施例1至5的各自的组合物的内部树脂层膜的氧气透过率而得到的图。
图3是通过测量包括具有本发明的实施例3和比较例1的各自的组合物的内部树脂层的铝软包膜的粘合强度而得到的图。
图4是通过测量包括具有本发明的实施例3和比较例1的各自的组合物的内部树脂层的铝软包膜的HF气体阻隔能力而得到的图。
具体实施方式
在下文中,将参照附图详细描述本发明的实施方案,使得本领域技术人员可以容易地实施本发明。然而,本发明可以以各种不同的形式来实施,并且不限于本文中所描述的实施方案。另外,附图中相同的附图标记表示相同的组成,并且为了便于描述,可以放大各个组成的尺寸或厚度。
在本说明书中,特定构件被放置在另一构件“之上”的描述不仅包括特定构件与另一构件接触的情况,而且还包括在这两个构件之间还存在有又一构件的情况。
在本说明书中,一个部分“包含”特定成分的描述是指其可以进一步包含其它成分,而不是排除其它成分,除非相反地特别说明。
在下文中,将详细描述本发明的优选的实施方案。
本发明的用于二次电池的铝软包膜包括:铝膜层;外部树脂层,该外部树脂层层压在所述铝膜层的一个表面上;和内部树脂层,该内部树脂层层压在所述铝膜层的另一表面上,
其中,所述内部树脂层包含聚烯烃树脂、乙烯乙烯醇共聚物(EVOH)和马来酸酐聚丙烯(MAHPP)树脂。
第一粘合层可以层压在铝膜层与外部树脂层之间,并且第二粘合层可以层压在铝膜层与内部树脂层之间。
内部树脂层可以包含29重量%至90重量%的聚烯烃树脂、5重量%至70重量%的乙烯乙烯醇共聚物(EVOH)和1重量%至20重量%的马来酸酐聚丙烯树脂;
优选地35重量%至70重量%的聚烯烃树脂、25重量%至60重量%的乙烯乙烯醇共聚物(EVOH)和1.5重量%至15重量%的马来酸酐聚丙烯树脂;
更优选地,40重量%至55重量%的聚烯烃树脂、40重量%至55重量%的乙烯乙烯醇共聚物(EVOH)和3.5重量%至10重量%的马来酸酐聚丙烯树脂。
如果聚烯烃树脂的含量小于上述范围,则由于诸如热密封性、防湿性、耐热性和层压加工性能的性能会降低而不优选,如果聚烯烃树脂的含量超过上述范围,则由于出现诸如降低室温成型性和白化现象的问题而不优选。
如果乙烯乙烯醇共聚物(EVOH)的含量小于上述范围,则由于氧气和水分阻隔效果变得不足而不优选,如果乙烯乙烯醇共聚物(EVOH)的含量超过上述范围,则由于发生诸如降低热密封性和界面剥离的问题而不优选。
如果马来酸酐聚丙烯树脂的含量小于上述范围,则由于乙烯乙烯醇共聚物(EVOH)树脂在聚烯烃树脂中没有充分分散,降低了氧气透过率而不优选,如果离聚物树脂的含量超过上述范围,则由于发生诸如降低室温成型性和热密封性以及界面剥离的问题而不优选。
聚烯烃树脂可以优选为聚乙烯(PE)、聚丙烯(PP)或它们的共聚物。
上面使用的聚烯烃的具体实例可以包括:聚乙烯,如低密度聚乙烯、中密度聚乙烯、高密度聚乙烯和线性低密度聚乙烯;聚丙烯,如均聚丙烯、聚丙烯的嵌段共聚物(例如,丙烯和乙烯的嵌段共聚物)和聚丙烯的无规共聚物(例如,丙烯和乙烯的无规共聚物);乙烯-丁烯-丙烯的三元共聚物;等。在这些聚烯烃中,优选包括聚乙烯和聚丙烯。
同时,作为本发明中使用的聚烯烃,可以没有限制地使用本领域已知的聚烯烃。
当在内部树脂层中使用聚烯烃如聚乙烯或聚丙烯或它们的共聚物时,由于加工性能如层压是有利的,并且具有作为用于二次电池的包装材料所需要的性能如有利的热密封性、防潮性能和耐热性,因此是优选的。考虑到成型性能、绝缘性能、电解质溶液耐受性等,内部树脂层的聚合物层的厚度优选为20μm至100μm,并且更优选为30μm至80μm。如果不满足上述范围,则会出现诸如成型性能、绝缘性能和电解质溶液耐受性的劣化的问题。
聚烯烃树脂可以具有0.3至10并且更优选地1至5的熔体流动指数。
乙烯乙烯醇共聚物(EVOH)是由下面化学式1表示的共聚物,并且具有优异的材料阻隔性能,特别地,提供优异的阻隔氧气和水分的效果。
[化学式1]
其中,x和y是乙烯醇结构单元和乙烯结构单元的摩尔比,x可以是0.3至0.7,y可以是0.3至0.7,x+y是1。
更优选地,x可以是0.4至0.6,y可以是0.4至0.6,更优选地,x可以是0.5至0.6,y可以是0.4至0.5。
乙烯乙烯醇共聚物树脂可以具有0.5至50并且更优选地0.8至20的熔体流动指数。具体地,例如,可以使用由Kuraray Co.,Ltd.制造的EP-E105B(商品名),然而,乙烯乙烯醇共聚物树脂不限于该共聚物。
马来酸酐聚丙烯树脂用作用于增强乙烯乙烯醇共聚物与聚烯烃聚合物之间的分散性和粘合强度的增容剂,并且还起到吸附并固定在软包内产生的HF气体的作用。
作为马来酸酐聚丙烯树脂,可以使用由下面化学式2表示的树脂。
[化学式2]
其中,m和n是各个结构单元的摩尔比,m可以是0.3至0.7,n可以是0.3至0.7,x+y是1。
在上述化学式中,优选地,m可以是0.4至0.6,n可以是0.4至0.6,更优选地,m可以是0.5至0.6,n可以是0.4至0.5。
马来酸酐聚丙烯树脂可以具有50至300并且更优选地100至200的熔体流动指数。作为具体实例,可以使用由ExxonMobil制造的ExxonTM PO1015,然而,马来酸酐聚丙烯树脂不限于该共聚物。
在下文中,将示例性地描述本发明的用于二次电池的铝软包膜的其它组成。然而,本发明不限于以下组成,并且除了以下组成之外,还可以采用本领域已知的组成。
铝膜层
在本发明的用于二次电池的铝软包膜中,铝膜层用作用于防止氧气、水分等从外部渗透的阻挡层。作为铝的材料,铝或铝的合金是合适的。作为铝的合金,可以使用通过将各种金属和非金属加入到纯铝中得到的合金或不锈钢合金。作为铝膜层,可以优选使用软铝箔,并且更优选地,可以使用含铁铝箔以向铝箔提供成型性。关于铝箔,高纯度系列具有优异的加工性能,因此,1000系列或8000系列中的铝合金箔是优选的。此外,铝基体可以任选地是包含选自硅、硼、锗、砷、锑、铜、镁、锰、锌、锂、铁、铬、钒、钛、铋、钾、锡、铅、锆、镍、钴以及它们的组合的元素的合金。在含铁铝箔中,相对于总铝箔重量,可以优选包含0.1重量%至9.0重量%,更优选0.5重量%至2.0重量%的铁组分。如果在铝箔中铁含量小于0.1重量%,则铝膜层的柔软性降低,如果包含超过9.0重量%的铁含量,则引起成型性降低的问题。铝箔可以具有蚀刻的或脱脂的表面以增强与内部树脂层的粘合性,然而,可以省去处理以降低处理速度。铝膜层用于防止气体和水蒸气从外部渗透到电池中,并且要求铝薄膜没有针孔并具有加工适宜性(袋装、压花成型)。考虑到加工性能、氧气和水分阻隔性能等,厚度优选为10μm至100μm,并且更优选为30μm至50μm。如果厚度小于10μm,则铝膜层容易撕裂并具有降低的耐电解性和绝缘性能,如果厚度超过50μm,则铝膜层具有降低成型性的问题。
外部树脂层
在本发明的用于二次电池的铝软包膜中,外部树脂层对应于与硬件直接接触的部分,因此,优选为具有绝缘性能的树脂。因此,作为用作外部树脂层的树脂,优选使用聚酯树脂如聚对苯二甲酸乙二醇酯、聚对苯二甲酸丁二醇酯、聚萘二甲酸乙二醇酯、聚萘二甲酸丁二醇酯、共聚聚酯或聚碳酸酯,或尼龙膜。
聚酯树脂的具体实例可以包括:聚对苯二甲酸乙二醇酯(PET)、聚对苯二甲酸丁二醇酯(PBT)、聚萘二甲酸乙二醇酯(PEN)、聚萘二甲酸丁二醇酯(PBN)、共聚聚酯、聚碳酸酯(PC)等。此外,聚酯的具体实例可以包括:聚对苯二甲酸乙二醇酯、聚对苯二甲酸丁二醇酯、聚萘二甲酸乙二醇酯、聚萘二甲酸丁二醇酯、聚间苯二甲酸乙二醇酯、聚碳酸酯、采用对苯二甲酸乙二醇酯作为主要重复单元的共聚聚酯、采用对苯二甲酸丁二醇酯作为主要重复单元的共聚聚酯等。此外,采用对苯二甲酸乙二醇酯作为主要重复单元的共聚聚酯的具体实例可以包括:在采用对苯二甲酸乙二醇酯作为主要重复单元的同时与间苯二甲酸乙二醇酯聚合的共聚物聚酯、聚(对苯二甲酸/间苯二甲酸)乙二醇酯、聚(对苯二甲酸/己二酸)乙二醇酯、聚(对苯二甲酸/间苯二甲酸磺酸钠)乙二醇酯、聚(对苯二甲酸/间苯二甲酸钠)乙二醇酯、聚(对苯二甲酸/苯基二羧酸)乙二醇酯、聚(对苯二甲酸/癸烷二羧酸)乙二醇酯等。此外,采用对苯二甲酸丁二醇酯作为主要重复单元的共聚聚酯的实例可以包括:在采用对苯二甲酸丁二醇酯作为主要重复单元的同时与间苯二甲酸丁二醇酯聚合的共聚物聚酯、聚(对苯二甲酸/己二酸)丁二醇酯、聚(对苯二甲酸/癸二酸)丁二醇酯、聚(对苯二甲酸/癸烷二羧酸)丁二醇酯、聚萘二甲酸丁二醇酯等。这些聚酯可以作为一种类型单独使用,或者作为两种或更多种类型的组合使用。
聚酰胺树脂的具体实例可以包括:脂肪族类聚酰胺,如尼龙6、尼龙66、尼龙610、尼龙12、尼龙46以尼龙6和尼龙66的共聚物;包含芳香族基团的聚酰胺,如六亚甲基二胺-间苯二甲酸-对苯二甲酸共聚的聚酰胺,诸如包含来自对苯二甲酸和/或间苯二甲酸的结构单元的尼龙6I、尼龙6T、尼龙6IT和尼龙6I6T(I表示间苯二甲酸,T表示对苯二甲酸),和聚(己二酰间苯二甲胺)(MXD6);脂环族类聚酰胺,如聚氨基甲基环己基己二酰二胺(PACM6);或通过使内酰胺组分或异氰酸酯组分如4,4′-二苯甲烷-二异氰酸酯共聚得到的聚酰胺、聚酯酰胺共聚物或聚醚酯酰胺共聚物,其是共聚的聚酰胺和聚酯或聚亚烷基醚二醇的共聚物;它们的共聚物等。这些聚酰胺可以作为一种类型单独使用,或者作为两种或更多种类型的组合使用。
在如上所述的外部树脂层中,作为用于封装二次电池的膜,特别优选使用尼龙膜。尼龙膜通过具有优异的耐热性、耐寒性和机械强度以及具有优异的破坏强度、针孔耐受性、气体阻隔性能等而主要用作包装膜。尼龙膜的具体实例可以包括聚酰胺树脂,即,尼龙6、尼龙66、尼龙6和尼龙66的共聚物、尼龙610、聚己二酰间苯二甲胺(MXD6)等。当层压外部树脂层时,层压的外部树脂层的厚度优选为10μm至30μm以上,并且特别优选为12μm至25μm。如果不满足上述范围,则存在如下问题:当厚度小于10μm时,由于物理性能降低,外部树脂层容易撕裂,而当厚度超过30μm时,成型性降低。
第一粘合层
第一粘合层是增加外部树脂层-铝箔层之间的粘合性的层。粘合层由能够粘合基层和金属层的粘合树脂形成。用于形成粘合层的粘合树脂可以是双组分可固化粘合树脂或单组分可固化粘合树脂。此外,对用于形成粘合层的粘合树脂的粘合机理也没有特别限制,并且可以使用化学反应类型、溶剂挥发类型、热熔类型、热压类型等中的任意一种。
用于形成粘合层的粘合树脂的树脂组分的具体实例可以包括:聚酯类树脂,如聚对苯二甲酸乙二醇酯、聚对苯二甲酸丁二醇酯、聚萘二甲酸乙二醇酯、聚萘二甲酸丁二醇酯、聚间苯二甲酸乙二醇酯、聚碳酸酯和共聚聚酯;聚醚类粘合剂;聚氨酯类粘合剂;环氧类树脂;酚醛树脂类树脂;聚酰胺类树脂,如尼龙6、尼龙66、尼龙12和共聚聚酰胺;聚烯烃类树脂,如聚烯烃、酸改性聚烯烃和金属改性聚烯烃;聚乙酸乙烯酯类树脂;纤维素类粘合剂;(甲基)丙烯酸类树脂;聚酰亚胺类树脂;氨基树脂,如脲醛树脂和三聚氰胺树脂;橡胶,如氯丁二烯橡胶、丁腈橡胶和苯乙烯-丁二烯橡胶;硅类树脂;氟化乙烯丙烯共聚物等。这些粘合树脂成分可以作为一种类型单独使用,或者作为两种或更多种类型的组合使用。
对两种或更多种类型的粘合树脂组分的组合类型没有特别限制,然而,其实例可以包括:聚酰胺和酸改性聚烯烃的复合树脂、聚酰胺和金属改性聚烯烃的复合树脂、聚酰胺和聚酯、聚酯和酸改性聚烯烃的复合树脂、聚酯和金属改性聚烯烃的复合树脂等。其中,就具有优异的延展性、在高湿度条件下的耐久性或抗约束功能、或在热封过程中的抗劣化功能,以及通过抑制基层与金属层之间的层压强度的降低来有效地抑制分层的发生而言,可优选地包括聚氨酯类双组分可固化粘合树脂;聚酰胺、聚酯、或这些物质和改性聚烯烃的共混树脂。
第一粘合层是增加外部树脂层-铝膜层之间的粘合性的层。第一粘合层可以使用已知作为用于层压树脂膜和铝箔的粘合剂的材料形成。相应的粘合剂的实例可以包括包含主要试剂和固化剂的聚氨酯类粘合剂,所述主要试剂包括多元醇如聚酯多元醇、聚醚多元醇、丙烯酸类多元醇或碳酸酯多元醇,所述固化剂包括双官能以上的异氰酸酯化合物。聚氨酯类树脂通过使固化剂作用于主要试剂而形成。
首先,可以包含多元醇作为粘合剂的组分。
用于氨基甲酸乙酯型粘合剂的多元醇化合物的实例可以包括聚酯多元醇、聚酯聚氨酯多元醇、聚醚多元醇、聚醚聚氨酯多元醇等。对这些多元醇化合物的羟基当量和重均分子量没有特别限制,只要相对于要组合的异氰酸酯类化合物最终满足上述性能即可,然而,例如,羟基当量(数目/摩尔)可以是0.5至2.5,优选0.7至1.9,重均分子量可以是500至120000,优选1000至80000。在这些多元醇化合物中,优选包括聚酯多元醇、聚酯聚氨酯多元醇和聚醚聚氨酯多元醇。这些多元醇化合物可以作为一种类型单独使用,或者作为两种或更多种类型的组合使用。
作为聚酯多元醇,可以使用通过使至少一种类型的多元酸和至少一种类型的二醇反应得到的材料。多元酸的实例可以包括以下二元酸:脂肪族类二元酸如琥珀酸、戊二酸、己二酸、庚二酸、辛二酸、壬二酸、癸二酸和十三烷二酸,和芳香族类二元酸如间苯二甲酸、对苯二甲酸和萘二甲酸,等。二醇的实例可以包括:脂肪族类二醇,如乙二醇、丙二醇、丁二醇、新戊二醇、甲基戊二醇、己二醇、庚二醇、辛二醇、壬二醇、癸二醇和十二烷二醇;脂环族类二醇,如环己二醇和加氢的苯二甲醇;以及芳香族类二醇,如苯二甲醇,等。
另外,作为聚酯多元醇,可以包括通过使用异氰酸酯化合物的单一产物,或包含至少一种类型的异氰酸酯化合物的加合产物、缩二脲产物或异氰脲酸酯产物,在聚酯多元醇的两端扩链羟基而得到的聚酯聚氨酯多元醇等。异氰酸酯化合物的实例可以包括2,4-或2,6-甲苯二异氰酸酯、苯二甲基异氰酸酯、4,4′-二苯基甲烷二异氰酸酯、亚甲基二异氰酸酯、亚异丙基二异氰酸酯、赖氨酸二异氰酸酯、2,2,4-或2,4,4-三甲基六亚甲基二异氰酸酯、1,6-六亚甲基二异氰酸酯、甲基环己烷二异氰酸酯、异佛尔酮二异氰酸酯、4,4′-二环己基甲烷二异氰酸酯、亚异丙基二环己基-4,4′-二异氰酸酯等。
作为丙烯酸类多元醇,可以包括以聚(甲基)丙烯酸为主要组分的共聚物。相应的共聚物的实例可以包括由下面单体开始,通过共聚得到的材料:含羟基的单体,如2-羟乙基(甲基)丙烯酸酯或2-羟丙基(甲基)丙烯酸酯;(甲基)丙烯酸烷基酯类单体,其中的烷基是甲基、乙基、正丙基、异丙基、正丁基、异丁基、叔丁基、2-乙基己基或环己基;含酰胺基的单体,如(甲基)丙烯酰胺、N-烷基(甲基)丙烯酰胺、N,N-二烷基(甲基)丙烯酰胺(所述烷基是甲基、乙基、正丙基、异丙基、正丁基、异丁基、叔丁基、2-乙基己基、环己基等)、N-烷氧基(甲基)丙烯酰胺、N,N-二烷氧基(甲基)丙烯酰胺(所述烷氧基是甲氧基、乙氧基、丁氧基、异丁氧基等)、N-羟甲基(甲基)丙烯酰胺或N-苯基(甲基)丙烯酰胺;含缩水甘油基的单体,如(甲基)丙烯酸缩水甘油酯或烯丙基缩水甘油醚;含硅烷的单体,如(甲基)丙烯酰氧基丙基三甲氧基硅烷或(甲基)丙烯酰氧基丙基三乙氧基硅烷;以及含异氰酸酯基的单体,如(甲基)丙烯酰氧基丙基异氰酸酯。
作为碳酸酯多元醇,可以使用通过使碳酸酯化合物和二醇反应得到的材料。作为碳酸酯化合物,可以使用碳酸二甲酯、碳酸二苯酯、碳酸乙烯酯等。作为二醇,可以使用脂肪族二醇如乙二醇、丙二醇、丁二醇、新戊二醇、甲基戊二醇、己二醇、庚二醇、辛二醇、壬二醇、癸二醇和十二烷二醇;脂环族二醇,如环己二醇和加氢的苯二甲醇;芳香族二醇,如苯二甲醇,等。
另外,可以使用通过使用上述异氰酸酯化合物在碳酸酯多元醇的末端扩链羟基而得到的聚碳酸酯氨基甲酸乙酯多元醇。
接下来,可以包括异氰酸酯作为粘合剂的组分。
用于氨基甲酸乙酯型粘合剂的异氰酸酯类化合物的实例可以包括聚异氰酸酯、其加合产物、其异氰脲酸酯改性产物、其碳二亚胺改性产物、其脲基甲酸酯改性产物、其缩二脲改性产物等。聚异氰酸酯的具体实例可以包括:芳香族二异氰酸酯,如二苯基甲烷二异氰酸酯(MDI)、聚苯基甲烷二异氰酸酯(聚合的MDI)、甲苯二异氰酸酯(TDI)、六亚甲基二异氰酸酯(HDI)、双(4-异氰酸酯环己基)甲烷(H12MDI)、异佛尔酮二异氰酸酯(IPDI)、1,5-萘二异氰酸酯(1,5-NDI)、3,3′-二甲基-4,4′-二亚苯基二异氰酸酯(TODI)和二甲苯二异氰酸酯(XDI);脂肪族二异氰酸酯,如三亚甲基二异氰酸酯、六亚甲基二异氰酸酯、三甲基六亚甲基二异氰酸酯和异佛尔酮二异氰酸酯;脂环族二异氰酸酯,如4,4′-亚甲基双(环己基异氰酸酯)和异佛尔酮二异氰酸酯等。加合产物的具体实例可以包括通过向聚异氰酸酯中加入三羟甲基丙烷、乙二醇等而得到的那些产物。在这些异氰酸酯类化合物中,可以优选包括聚异氰酸酯及其加合产物;更优选地,芳香族二异氰酸酯、其加合产物和其异氰脲酸酯改性产物;还更优选地,MDI、聚合的MDI、TDI、它们的加合产物和它们的异氰脲酸酯改性产物;并且特别优选地,MDI的加合产物、TDI的加合产物、聚合的MDI和TDI的异氰脲酸酯改性产物。这些异氰酸酯类化合物可以作为一种类型单独使用,或者作为两种或更多种类型的组合使用。
作为用作固化剂的双官能以上异氰酸酯化合物,可以使用用作扩链剂的异氰酸酯化合物的类型,并且尽管重复,可以使用选自2,4-或2,6-甲苯二异氰酸酯、苯二甲基二异氰酸酯、4,4′-二苯基甲烷二异氰酸酯、亚甲基二异氰酸酯、亚异丙基二异氰酸酯、赖氨酸二异氰酸酯、2,2,4-或2,4,4-三甲基六亚甲基二异氰酸酯、1,6-六亚甲基二异氰酸酯、甲基环己烷二异氰酸酯、异佛尔酮二异氰酸酯、4,4′-二环己基甲烷二异氰酸酯和亚异丙基二环己基-4,4′-二异氰酸酯中的异氰酸酯化合物的单一产物,或包括选自上述异氰酸酯化合物中的至少一种类型的异氰酸酯化合物的加合产物、缩二脲产物或异氰脲酸酯产物。
作为固化剂的混合量,相对于100质量份的主剂,优选1质量份至100质量份,更优选5质量份至50质量份。如果固化剂的含量小于1质量份,则粘合性或电解质溶液耐受性方面的性能不会表达。如果固化剂的含量超过100质量份,则存在过量的异氰酸酯基,其会通过剩余的未反应的材料而影响粘合膜质量,或会影响硬度。
为了促进粘合,也可以将碳二亚胺化合物、噁唑啉化合物、环氧化合物、磷化合物、硅烷偶联剂等混合至聚氨酯类粘合剂。
碳二亚胺化合物的实例可以包括N,N′-二-邻甲苯甲酰基碳二亚胺、N,N′-二苯基碳二亚胺、N,N′-二-2,6-二甲基苯基碳二亚胺、N,N′-双(2,6-二异丙基苯基)碳二亚胺、N,N′-二辛基癸基碳二亚胺、N-三基-N′-环己基碳二亚胺、N,N′-二-2,2-二叔丁基苯基碳二亚胺、N-三基-N′-苯基碳二亚胺、N,N′-二-对硝基苯基碳二亚胺、N,N′-二-对氨基苯基碳二亚胺、N,N′-二-对羟基苯基碳二亚胺、N,N′-二环己基碳二亚胺、N,N′-二-对甲苯甲酰基碳二亚胺等。
噁唑啉化合物的实例可以包括:单噁唑啉化合物,如2-噁唑啉、2-甲基-2-噁唑啉、2-苯基-2-噁唑啉、2,5-二甲基-2-噁唑啉和2,4-二苯基-2-噁唑啉;以及二噁唑啉化合物,如2,2′-(1,3-亚苯基)-双(2-噁唑啉)、2,2′-(1,2-亚乙基)-双(2-噁唑啉)、2,2′-(1,4-亚丁基)-双(2-噁唑啉)和2,2′-(1,4-亚苯基)-双(2-噁唑啉)。
环氧化合物的实例可以包括:脂肪族二醇如1,6-己二醇、新戊二醇和聚亚烷基二醇的二缩水甘油醚;脂肪族多元醇如山梨糖醇、脱水山梨糖醇、聚甘油、季戊四醇、二甘油、甘油和三羟甲基丙烷的聚缩水甘油醚;脂环族多元醇如环己烷二甲醇的聚缩水甘油醚;脂肪族或芳香族多元羧酸如对苯二甲酸、间苯二甲酸、萘二甲酸、偏苯三甲酸、己二酸和癸二酸的二缩水甘油酯或聚缩水甘油酯;多元酚如间苯二酚、双-(对羟基苯基)甲烷、2,2-双-(对羟基苯基)丙烷、三-(对羟基苯基)甲烷和1,1,2,2-四(对羟基苯基)乙烷的二缩水甘油醚或聚缩水甘油醚;胺如N,N′-二缩水甘油基苯胺、N,N,N-二缩水甘油基甲苯胺和N,N,N′,N′-四缩水甘油基-双-(对氨基苯基)甲烷的N-缩水甘油基衍生物;氨基苯酚、三缩水甘油基三(2-羟乙基)异氰脲酸酯、三缩水甘油基异氰脲酸酯、邻甲酚型环氧树脂、苯酚酚醛清漆型环氧树脂等的三缩水甘油基衍生物。
磷类化合物的实例可以包括:三(2,4-二叔丁基苯基)亚磷酸酯、四(2,4-二叔丁基苯基)-4,4′-亚联苯基亚膦酸酯、双(2,4-二叔丁基苯基)季戊四醇-二亚磷酸酯、双(2,6-二叔丁基-4-甲基苯基)季戊四醇二亚磷酸酯、2,2-亚甲基双(4,6-二叔丁基苯基)辛基亚磷酸酯、4,4′-亚丁基-双(3-甲基-6-叔丁基苯基-二-十三烷基)亚磷酸酯、1,1,3-三(2-甲基-4-二(十三烷基)亚磷酸酯-5-叔丁基-苯基)丁烷、三(混合的单-和二-壬基苯基)亚磷酸酯、三(壬基苯基)亚磷酸酯、4,4′-亚异丙基双(苯基-二烷基亚磷酸酯)等。
硅烷偶联剂的实例可以包括各种硅烷偶联剂,如乙烯基三乙氧基硅烷、乙烯基三(β-甲氧基乙氧基)硅烷、γ-甲基丙烯酰氧基丙基三甲氧基硅烷、乙烯基三乙酰氧基硅烷、γ-缩水甘油氧基丙基三甲氧基硅烷、γ-缩水甘油氧基丙基三乙氧基硅烷、β-(3,4-环氧环己基)乙基三甲氧基硅烷、γ-氯丙基甲氧基硅烷、乙烯基三氯硅烷、γ-巯基丙基三甲氧基硅烷、γ-氨基丙基三乙氧基硅烷和N-β-(氨乙基)-γ-氨基丙基三甲氧基硅烷。
用于形成满足本发明的用于二次电池的包装膜的性能的粘合层的粘合剂可以优选地包括氨基甲酸乙酯型粘合剂,所述氨基甲酸乙酯型粘合剂包含选自聚酯多元醇、聚酯聚氨酯多元醇、聚醚多元醇和聚醚聚氨酯多元醇中的至少一种类型的多元醇化合物,和选自芳香族二异氰酸酯、其加合产物和其异氰脲酸酯改性产物中的至少一种类型的异氰酸酯类化合物;更优选地包括氨基甲酸乙酯型粘合剂,所述氨基甲酸乙酯型粘合剂包含选自聚酯多元醇、聚酯聚氨酯多元醇、聚醚多元醇和聚醚聚氨酯多元醇中的至少一种类型的多元醇化合物,以及选自MDI、聚合的MDI、TDI、它们的加合产物和它们的异氰脲酸酯改性产物中的至少一种类型的异氰酸酯类化合物。
另外,在包含多元醇化合物(主剂)和异氰酸酯类化合物(固化剂)的粘合剂中,它们的比例根据待在粘合层中提供的性能而适当地设定,然而,例如,多元醇化合物的每1摩尔的羟基,异氰酸酯类化合物的异氰酸酯基的比例可以为1摩尔至30摩尔,并且优选地为3摩尔至20摩尔。
考虑到与外部树脂层的粘合性和成型后的厚度,第一粘合层优选具有2μm至10μm,更优选3μm至5μm的厚度。如果厚度小于2μm,则粘合性降低,如果厚度超过10μm,则会出现诸如产生裂纹等的问题。
第二粘合层
第二粘合层是增加内部树脂层-铝膜层之间的粘合性的层。
在本发明的用于二次电池的铝软包膜中,可以使用聚氨酯、酸改性的聚烯烃树脂、环氧树脂等作为第二粘合层。第二粘合剂的具体实例可以包括马来酸酐聚丙烯(MAHPP)等。
热粘合烯烃类树脂的实例可以包括:聚乙烯、乙烯-α-烯烃共聚物、乙烯-丙烯酸共聚物、乙烯-甲基丙烯酸共聚物、乙烯-丙烯酸酯共聚物、乙烯-甲基丙烯酸酯共聚物、乙烯-乙酸乙烯酯共聚物、离聚物、聚丙烯、马来酸酐改性的聚丙烯、乙烯-丙烯共聚物、丙烯-1-丁烯-乙烯共聚物等,并且可以优选地包括选自聚丙烯、乙烯-丙烯共聚物和丙烯-1-丁烯-乙烯共聚物中的一种或多种类型的烯烃类树脂。
用于形成第二粘合层的酸改性的聚烯烃是通过将聚烯烃与不饱和羧酸接枝聚合而改性的聚合物。所述酸改性的聚烯烃的具体实例可以包括:聚乙烯,如低密度聚乙烯、中密度聚乙烯、高密度聚乙烯或线性低密度聚乙烯;结晶或非晶聚丙烯,如均聚丙烯、聚丙烯的嵌段共聚物(例如,丙烯和乙烯的嵌段共聚物)和聚丙烯的无规共聚物(例如,丙烯和乙烯的无规共聚物);乙烯-丁烯-丙烯的三元共聚物;等。在这些聚烯烃中,优选包括至少具有丙烯作为形成单体的聚烯烃,并且就耐热性而言,可以更优选包括乙烯-丁烯-丙烯的三元共聚物和丙烯-乙烯的无规共聚物。用于改性的不饱和羧酸的实例可以包括马来酸、丙烯酸、衣康酸、巴豆酸、马来酸酐、衣康酸酐等。在这些不饱和羧酸中,优选包括马来酸和马来酸酐。所述酸改性的聚烯烃可以作为一种类型单独使用,或者作为两种或更多种类型的组合使用。
考虑到与内部树脂层的粘合性和成型后的厚度,第二粘合层优选具有2μm至10μm,更优选3μm至5μm的厚度。如果厚度小于2μm,则粘合性降低,如果厚度超过5μm,则会出现诸如产生裂纹等的问题。
当在第二粘合层上层压内层和铝膜层时,对方法没有特别限制,然而,可以优选使用干式层压法、热层压法或挤出层压法进行层压。
制造用于二次电池的铝软包膜的方法
可以使用包括以下步骤的方法制造本发明的用于二次电池的铝软包膜:a)制备铝膜层;b)在铝膜层的第一表面上形成外部树脂层;c)制备包含其中含氟聚合物树脂、聚烯烃和功能性树脂化学键合的化合物的内部树脂层;和d)将所述内部树脂层粘合至所述铝膜层的第二表面。
a)制备铝膜层
铝膜材料与上面描述的相同。
作为铝膜,可以使用铝箔。可以使用未经预处理的未处理的铝箔,然而,就提供电解液体耐受性、电解质溶液耐受性等而言,更优选使用脱脂铝箔。作为脱脂处理方法,可以包括湿式或干式处理方法。
湿式脱脂处理的实例可以包括酸脱脂或碱脱脂。用于酸脱脂的酸的实例可以包括无机酸如硫酸、乙酸、磷酸和氢氟酸,并且该酸可以作为一种类型单独使用,或者作为两种或更多种类型的组合使用。另外,当需要时,可以向其中混合各种金属盐,以便增强铝箔的蚀刻效果。用于碱脱脂的碱的实例可以包括强碱如氢氧化钠,并且也可以使用具有弱碱类或混合有表面活性剂的那些。
干式脱脂处理的实例可以包括采用在高温下对铝退火处理的脱脂方法。
b)在铝膜层的第一表面上形成外部树脂层;
在步骤a)中制备的铝膜层上涂覆第一粘合层。此处,考虑到与外部树脂层的粘合性和成型后的厚度,涂覆的第一粘合层的厚度优选为2μm至10μm,更优选3μm至5μm。如果不满足上述范围,当厚度小于2μm时,粘合性会降低,当厚度超过10μm时,会出现裂纹。
在如上涂覆的第一粘合层上,层压外部树脂层,并且通过使用干式层压法或挤出层压法的层压来形成外部树脂层。
c)制备内部树脂层
内部树脂层可以通过混合40重量份至90重量份的聚烯烃树脂、5重量份至70重量份的乙烯乙烯醇共聚物(EVOH)和1重量份至20重量份的马来酸酐聚丙烯树脂来制备。
d)将内部树脂层粘合至铝膜层的第二表面
作为用于粘合铝膜层和内部树脂层的第二粘合层,可以使用聚氨酯、酸改性的聚烯烃树脂、环氧树脂等,并且其具体实例可以包括马来酸酐聚丙烯(MAHPP)等。
考虑到与内部树脂层的粘合性和成型后的厚度,第二粘合层的厚度优选为2μm至30μm,更优选3μm至15μm。如果不满足上述范围,当厚度小于2μm时,粘合性会降低,当厚度超过30μm时,会出现裂纹。
当在铝膜层上层压内部树脂层时,尽管没有特别地限制,但是可以优选使用干式层压法或挤出层压法来层压内部树脂层。
在上文中,已经详细描述了本发明的优选的实施方案,然而,本发明的权利范围不限于此,本领域技术人员利用权利要求书中限定的本发明的基本概念所作的各种修改和改进形式也落入本发明的权利范围内。
实施例和比较例:软包膜的制造
为了在厚度为40μm的铝箔(Dong-il Aluminum Co.,Ltd.的产品)的第一表面上层压外部树脂层,使用凹版辊法涂布厚度为4μm的聚氨酯粘合树脂(Hi-chem Co.,Ltd.的产品),然后干式层压厚度为25μm的尼龙6膜(Hyosung的产品),以将尼龙膜层压在铝层上。之后,为了在铝箔的第二表面上层压内部树脂层,以下面表1的重量比混合相应的组分,并使用多层层压挤出机(多层头块的挤出机)制备内部树脂层。将内部树脂层挤出至40μm的厚度,然后使用粘合剂(ADME)层压在铝上,以制造软包膜。
[表1]
EVOH | MAHPP | 聚氟乙烯 | PP | |
比较例1 | 0 | 5 | 6 | 89 |
比较例2 | 50 | 0 | 0 | 50 |
实施例1 | 50 | 2 | 0 | 50 |
实施例2 | 50 | 4 | 0 | 50 |
实施例3 | 50 | 6 | 0 | 50 |
实施例4 | 50 | 8 | 0 | 50 |
实施例5 | 50 | 10 | 0 | 50 |
(单位:重量份)PP:cPP,Hanwha Total Company的产品
EVOH:由Kuraray Company制造,EP-E105B(商品名)
MAHPP:马来酸酐聚丙烯(ExxonTM,PO1015)
试验例1:氧气透过率的测量(OTR:cc/m2天)
使用在用于制造铝软包膜的工艺过程中在实施例1至5的各自的组合物中制备的内部树脂层膜来测量氧气透过率,并将结果示于图2中。
从图2可以确认,随着MAHPP树脂含量的增加,EVOH在PP中的分散程度提高,这降低了氧气透过率。
试验例2:粘合强度的测量
使用在实施例3和比较例1的各自的组合物中制造的铝软包膜来测量粘合强度,并将结果示于图3中。在85℃/85RH%的恒定温度和湿度环境下进行试验,用于长期可靠性评估。
如从图3确认的,在270小时之前,比较例1的铝软包膜(包括含氟聚合物)具有比实施例3的铝软包膜更高的粘合强度,然而,在270小时之后,实施例3的铝软包膜的粘合强度被更好地保持,因为在比较例1的铝软包膜(包括含氟聚合物)中,由于氟和聚烯烃之间的相分离而导致粘合强度降低。
试验例3:HF气体浓度的测量
使用在实施例3或比较例1的组合物中制造的铝软包膜来制备虚拟电池,并在经过一定时间之后,测量电解质溶液中包含的HF气体的浓度,并将结果示于图4中。在85℃/85RH%的恒定温度和湿度环境下进行试验,用于长期可靠性评估。
如从图4确认的,在250小时之前,比较例1的铝软包膜(包括含氟聚合物)中包含的电解质溶液具有较低的HF浓度,然而,在250小时之后,实施例3的铝软包膜的电解质溶液保持较低的HF浓度,因为在比较例1的铝软包膜中,性能降低(界面之间的粘合强度降低)。
实施例3中在250小时之后HF浓度降低的趋势被认为是由于MAHPP树脂的-COONa官能团和HF形成NaF键,从而以“中和键”的形式将HF吸附并固定在离聚物树脂中。换言之,由此认为HF扩散的量减少。
Claims (7)
1.一种用于二次电池的铝软包膜,所述铝软包膜包括:
铝膜层;
外部树脂层,所述外部树脂层层压在所述铝膜层的一个表面上;
内部树脂层,所述内部树脂层层压在所述铝膜层的另一表面上,
其中,所述内部树脂层包含聚烯烃树脂、乙烯乙烯醇共聚物(EVOH)和马来酸酐聚丙烯树脂。
2.根据权利要求1所述的铝软包膜,其中,所述内部树脂层包含29重量%至90重量%的聚烯烃树脂、5重量%至70重量%的乙烯乙烯醇共聚物(EVOH)和1重量%至20重量%的马来酸酐聚丙烯树脂。
3.根据权利要求1所述的铝软包膜,其中,所述聚烯烃是聚乙烯(PE)、聚丙烯(PP)或它们的共聚物。
4.根据权利要求1所述的铝软包膜,其中,所述乙烯乙烯醇共聚物(EVOH)是由下面化学式1表示的共聚物:
[化学式1]
其中,x和y是乙烯醇结构单元和乙烯结构单元的摩尔比,x是0.3至0.7,y是0.3至0.7,x+y是1。
5.根据权利要求1所述的铝软包膜,其中,所述马来酸酐聚丙烯树脂是由下面化学式2表示的共聚物:
[化学式2]
其中,m和n是各结构单元的摩尔比,m是0.3至0.7,n是0.3至0.7,x+y是1。
6.根据权利要求1所述的铝软包膜,其中,所述外部树脂层由尼龙膜形成。
7.根据权利要求1所述的铝软包膜,其中,第一粘合层层压在所述铝膜层与所述外部树脂层之间;并且第二粘合层层压在所述铝膜层与所述内部树脂层之间。
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