CN107735444B - 热塑性树脂膜与橡胶的叠层体、内衬层材料及充气轮胎 - Google Patents
热塑性树脂膜与橡胶的叠层体、内衬层材料及充气轮胎 Download PDFInfo
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- CN107735444B CN107735444B CN201680038137.3A CN201680038137A CN107735444B CN 107735444 B CN107735444 B CN 107735444B CN 201680038137 A CN201680038137 A CN 201680038137A CN 107735444 B CN107735444 B CN 107735444B
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Abstract
本发明涉及能够作为充气轮胎的内衬层材料使用的、由热塑性树脂或热塑性弹性体组合物的膜与橡胶组合物的层形成的叠层体,热塑性树脂或热塑性弹性体组合物的膜与橡胶组合物的层之间的界面的粘接强度得到改善。本发明涉及一种由热塑性树脂或热塑性弹性体组合物的膜与橡胶组合物的层形成的叠层体,其特征在于,橡胶组合物包含橡胶成分、酚类化合物与甲醛的缩合物、亚甲基供体以及硫化剂,橡胶成分的2.5~40质量%为丁基橡胶或卤化丁基橡胶,上述缩合物的配合量相对于橡胶成分100质量份为0.5~20质量份,亚甲基供体的配合量相对于橡胶成分100质量份为0.25~200质量份。
Description
技术领域
本发明涉及由热塑性树脂或热塑性弹性体组合物的膜与橡胶组合物的层形成的叠层体、由该叠层体构成的充气轮胎用内衬层材料以及将该叠层体作为内衬层材料使用的充气轮胎。
背景技术
已知一种充气轮胎,其包含由热塑性树脂或热塑性弹性体组合物的膜与橡胶组合物的层形成的叠层体,其特征在于,橡胶组合物包含橡胶成分、酚类化合物与甲醛的缩合物、亚甲基供体以及硫化剂,硫化剂为硫黄或有机过氧化物(日本特许第4858654号公报)。
现有技术文献
专利文献
专利文献1:日本特许第4858654号公报
发明内容
发明所要解决的课题
本发明的课题在于,对于可以作为充气轮胎的内衬层材料使用的、由热塑性树脂或热塑性弹性体组合物的膜与橡胶组合物的层形成的叠层体,进一步改善热塑性树脂或热塑性弹性体组合物的膜与橡胶组合物的层之间的界面的粘接强度。
用于解决课题的方法
本发明人发现,在由热塑性树脂或热塑性弹性体组合物的膜、与橡胶组合物的层形成的叠层体中,通过使构成橡胶组合物的橡胶成分的一部分使用丁基橡胶或卤化丁基橡胶,并且在橡胶组合物中配合酚类化合物与甲醛的缩合物和亚甲基供体,从而可以有效地改善热塑性树脂或热塑性弹性体组合物的膜与橡胶组合物的层之间的界面的粘接强度,由此完成了本发明。
本发明涉及一种充气轮胎用叠层体,是由热塑性树脂或热塑性弹性体组合物的膜与橡胶组合物的层形成的叠层体,其特征在于,橡胶组合物包含橡胶成分、式(1)所示的化合物与甲醛的缩合物、亚甲基供体以及硫化剂,橡胶成分的2.5~40质量%为丁基橡胶或卤化丁基橡胶,上述缩合物的配合量相对于橡胶成分100质量份为0.5~20质量份,亚甲基供体的配合量相对于橡胶成分100质量份为0.25~200质量份,
(式中,R1、R2、R3、R4和R5各自独立地为氢原子、羟基、碳原子数为1~8个的烷基或碳原子数为1~8个的烷氧基。)。
本发明包含以下方案。
[1]一种充气轮胎用叠层体,其特征在于,是由热塑性树脂或热塑性弹性体组合物的膜与橡胶组合物的层形成的叠层体,橡胶组合物包含橡胶成分、式(1)所示的化合物与甲醛的缩合物、亚甲基供体以及硫化剂,橡胶成分的2.5~40质量%为丁基橡胶或卤化丁基橡胶,上述缩合物的配合量相对于橡胶成分100质量份为0.5~20质量份,亚甲基供体的配合量相对于橡胶成分100质量份为0.25~200质量份,
(式中,R1、R2、R3、R4和R5各自独立地为氢原子、羟基、碳原子数为1~8个的烷基或碳原子数为1~8个的烷氧基。)。
[2]根据[1]所述的叠层体,其特征在于,亚甲基供体的配合量/上述缩合物的配合量之比为0.5~10。
[3]根据[1]或[2]所述的叠层体,其特征在于,热塑性树脂为选自聚乙烯醇、乙烯-乙烯醇共聚物、尼龙6、尼龙66、尼龙11、尼龙12、尼龙610、尼龙612、尼龙6/66、尼龙MXD6和尼龙6T中的至少1种。
[4]根据[1]~[3]中任一项所述的叠层体,其特征在于,热塑性弹性体组合物是使弹性体成分分散于热塑性树脂成分中而成的组合物,热塑性树脂成分为选自聚乙烯醇、乙烯-乙烯醇共聚物、尼龙6、尼龙66、尼龙11、尼龙12、尼龙610、尼龙612、尼龙6/66、尼龙MXD6和尼龙6T中的至少1种,弹性体成分为选自溴化异丁烯-对甲基苯乙烯共聚物、马来酸酐改性乙烯-α-烯烃共聚物、乙烯-甲基丙烯酸缩水甘油酯共聚物和马来酸酐改性乙烯-丙烯酸乙酯共聚物中的至少1种。
[5]根据[1]~[4]中任一项所述的叠层体,其特征在于,亚甲基供体为选自改性醚化羟甲基三聚氰胺、低聚甲醛、六亚甲基四胺、五亚甲基四胺和六甲氧基甲基三聚氰胺中的至少1种。
[6]一种充气轮胎用内衬层材料,其由[1]~[5]中任一项所述的叠层体构成。
[7]一种充气轮胎,其使用[1]~[5]中任一项所述的叠层体作为内衬层材料。
发明效果
对于本发明的由热塑性树脂或热塑性弹性体组合物的膜与橡胶组合物的层形成的叠层体而言,热塑性树脂或热塑性弹性体组合物的膜与橡胶组合物的层之间的界面的粘接强度优异。
具体实施方式
本发明涉及一种充气轮胎用叠层体,是热塑性树脂或热塑性弹性体组合物的膜与橡胶组合物的层形成的叠层体,其特征在于,橡胶组合物包含橡胶成分、式(1)所示的化合物与甲醛的缩合物、亚甲基供体以及硫化剂,橡胶成分的2.5~40质量%为丁基橡胶或卤化丁基橡胶,上述缩合物的配合量相对于橡胶成分100质量份为0.5~20质量份,亚甲基供体的配合量相对于橡胶成分100质量份为0.25~200质量份,
(式中,R1、R2、R3、R4和R5各自独立地为氢原子、羟基、碳原子数为1~8个的烷基或碳原子数为1~8个的烷氧基。)。
作为构成膜的热塑性树脂,可举出聚酰胺系树脂、聚酯系树脂、聚腈系树脂、聚甲基丙烯酸酯系树脂、聚乙烯基系树脂、纤维素系树脂、氟系树脂、酰亚胺系树脂、聚苯乙烯系树脂、聚烯烃系树脂等。
作为聚酰胺系树脂,可举出尼龙6(N6)、尼龙66(N66)、尼龙46(N46)、尼龙11(N11)、尼龙12(N12)、尼龙610(N610)、尼龙612(N612)、尼龙6/66(N6/66)、尼龙6/66/12(N6/66/12)、尼龙6/66/610(N6/66/610)、尼龙MXD6(MXD6)、尼龙6T、尼龙6/6T、尼龙9T、尼龙66/PP共聚物、尼龙66/PPS共聚物等。
作为聚酯系树脂,可举出聚对苯二甲酸乙二醇酯(PET)、聚对苯二甲酸丁二醇酯(PBT)、聚间苯二甲酸乙二醇酯(PEI)、PET/PEI共聚物、聚芳酯(PAR)、聚萘二甲酸丁二醇酯(PBN)、液晶聚酯、聚氧化烯二酰亚胺酸/聚丁酸酯对苯二甲酸酯共聚物等芳香族聚酯等。
作为聚腈系树脂,可举出聚丙烯腈(PAN)、聚甲基丙烯腈、丙烯腈/苯乙烯共聚物(AS)、甲基丙烯腈/苯乙烯共聚物、甲基丙烯腈/苯乙烯/丁二烯共聚物等。
作为聚甲基丙烯酸酯系树脂,可举出聚甲基丙烯酸甲酯(PMMA)、聚甲基丙烯酸乙酯等。
作为聚乙烯基系树脂,可举出聚乙酸乙烯酯(PVAc)、聚乙烯醇(PVA)、乙烯-乙烯醇共聚物(EVOH)、聚1,1-二氯乙烯(PVDC)、聚氯乙烯(PVC)、氯乙烯/1,1-二氯乙烯共聚物、1,1-二氯乙烯/丙烯酸甲酯共聚物等。
作为纤维素系树脂,可举出乙酸纤维素、乙酸丁酸纤维素等。
作为氟系树脂,可举出聚1,1-二氟乙烯(PVDF)、聚氟乙烯(PVF)、聚氯氟乙烯(PCTFE)、四氟乙烯/乙烯共聚物(ETFE)等。
作为酰亚胺系树脂,可举出芳香族聚酰亚胺(PI)等。作为聚苯乙烯系树脂,可举出聚苯乙烯(PS)等。
作为聚烯烃系树脂,可举出聚乙烯(PE)、聚丙烯(PP)等。
其中,从兼具耐疲劳性和空气阻隔性的观点出发,优选为聚乙烯醇、乙烯-乙烯醇共聚物、尼龙6、尼龙66、尼龙11、尼龙12、尼龙610、尼龙612、尼龙6/66、尼龙MXD6、尼龙6T。
为了改善加工性、分散性、耐热性、抗氧化性等,在不损害本发明的效果的范围内,在热塑性树脂中可以配合填充剂、增强剂、加工助剂、稳定剂、抗氧化剂等树脂组合物中通常所配合的配合剂。从空气阻隔性和耐热性的观点出发,最好不配合增塑剂,但是只要在不损害本发明的效果的范围内,也可以配合增塑剂。
构成膜的热塑性弹性体组合物是使弹性体成分分散于热塑性树脂成分中而成的组合物,热塑性树脂成分构成基体相,弹性体成分构成分散相。
作为构成热塑性弹性体组合物的热塑性树脂成分,可以使用与上述热塑性树脂相同的成分。
作为构成热塑性弹性体组合物的弹性体成分,可举出二烯系橡胶及其氢化物、烯烃系橡胶、含卤素橡胶、硅橡胶、含硫橡胶、氟橡胶等。
作为二烯系橡胶及其氢化物,可举出天然橡胶(NR)、异戊二烯橡胶(IR)、环氧化天然橡胶、丁苯橡胶(SBR)、丁二烯橡胶(BR)(高顺式BR和低顺式BR)、丙烯腈丁二烯橡胶(NBR)、氢化NBR、氢化SBR等。
作为烯烃系橡胶,可举出乙丙橡胶(EPM)、三元乙丙橡胶(EPDM)、马来酸改性乙丙橡胶(M-EPM)、马来酸酐改性乙烯-α-烯烃共聚物、乙烯-甲基丙烯酸缩水甘油酯共聚物、马来酸酐改性乙烯-丙烯酸乙酯共聚物(改性EEA)、丁基橡胶(IIR)、异丁烯与芳香族乙烯基系单体或二烯系单体共聚物、丙烯酸类橡胶(ACM)、离子交联聚合物等。
作为含卤素橡胶,可举出溴化丁基橡胶(Br-IIR)、氯化丁基橡胶(Cl-IIR)等卤化丁基橡胶、溴化异丁烯-对甲基苯乙烯共聚物(BIMS)、卤化异丁烯-异戊二烯共聚橡胶、氯丁橡胶(CR)、氯醇(hydrin)橡胶(CHR)、氯磺化聚乙烯(CSM)、氯化聚乙烯(CM)、马来酸改性氯化聚乙烯(M-CM)等。
作为硅橡胶,可举出甲基乙烯基硅橡胶、二甲基硅橡胶、甲基苯基乙烯基硅橡胶等。作为含硫橡胶,可举出聚硫橡胶等。作为氟橡胶,可举出1,1-二氟乙烯系橡胶、含氟乙烯基醚系橡胶、四氟乙烯-丙烯系橡胶、含氟硅系橡胶、含氟磷腈系橡胶等。
其中,从空气阻隔性的观点出发,优选为溴化异丁烯-对甲基苯乙烯共聚物、马来酸酐改性乙烯-α-烯烃共聚物、乙烯-甲基丙烯酸缩水甘油酯共聚物、马来酸酐改性乙烯-丙烯酸乙酯共聚物。
在弹性体成分中,可以在不损害本发明的效果的范围内配合炭黑、二氧化硅等其它增强剂(填料)、软化剂、防老化剂、加工助剂等橡胶组合物中通常所配合的配合剂。
构成热塑性弹性体组合物的弹性体成分与热塑性树脂成分的组合不受限定,可举出卤化丁基橡胶与聚酰胺系树脂、溴化异丁烯-对甲基苯乙烯共聚橡胶与聚酰胺系树脂、丁二烯橡胶与聚苯乙烯系树脂、异戊二烯橡胶与聚苯乙烯系树脂、氢化丁二烯橡胶与聚苯乙烯系树脂、乙丙橡胶与聚烯烃系树脂、三元乙丙橡胶与聚烯烃系树脂、非晶性丁二烯橡胶与间规聚(1,2-聚丁二烯)、非晶性异戊二烯橡胶与反式聚(1,4-异戊二烯)、氟橡胶与氟树脂等,但优选为空气阻隔性优异的丁基橡胶与聚酰胺系树脂的组合,其中,从兼具耐疲劳性和空气阻隔性这样的观点出发,特别优选作为改性丁基橡胶的溴化异丁烯-对甲基苯乙烯共聚橡胶与尼龙6/66或尼龙6的组合、或者尼龙6/66与尼龙6的共混树脂的组合。
热塑性弹性体组合物可以如下制造:利用例如双螺杆混炼挤出机等将热塑性树脂成分和弹性体成分进行熔融混炼,在形成基体相的热塑性树脂成分中使弹性体成分作为分散相分散。热塑性树脂成分与弹性体成分的质量比率不受限定,但优选为10/90~90/10,更优选为15/85~90/10。
在不损害本发明的效果的范围内,热塑性树脂或热塑性弹性体组合物可以包含各种添加剂。
构成橡胶组合物的层的橡胶组合物包含橡胶成分、式(1)所示的化合物与甲醛的缩合物、亚甲基供体以及硫化剂。
橡胶组合物包含橡胶成分,橡胶成分的2.5~40质量%为丁基橡胶或卤化丁基橡胶。
所谓丁基橡胶,是异丁烯-异戊二烯共聚物,具有式(4)的结构,简称为IIR。可以使用弗瑞德克来福特催化剂(Friedel-Crafts catalyst),使异丁烯与少量的异戊二烯在氯甲烷溶剂中、在-95℃左右的低温下进行共聚来制造。
式(4)中,m和n表示正整数。
所谓卤化丁基橡胶,是将丁基橡胶卤化而得的橡胶,可以通过使丁基橡胶在己烷溶液中与气态或液态的卤素进行加成反应(丁基橡胶中的异戊二烯单元结合约1原子的卤素,产生1分子的卤化氢。)来制造。作为卤化丁基橡胶,可举出氯化丁基橡胶、溴化丁基橡胶,优选为溴化丁基橡胶。
丁基橡胶或卤化丁基橡胶需要占构成橡胶组合物的橡胶成分中的2.5~40质量%。在橡胶成分包含丁基橡胶和卤化丁基橡胶这两者的情况下,丁基橡胶和卤化丁基橡胶的合计量需要为橡胶成分的2.5~40质量%。优选橡胶成分的2.5~20质量%为丁基橡胶或卤化丁基橡胶,更优选橡胶成分的2.5~10质量%为丁基橡胶或卤化丁基橡胶。如果丁基橡胶或卤化丁基橡胶的含量过少,则得不到粘接性提高的效果。如果丁基橡胶或卤化丁基橡胶的含量过多,则混合或成型时易于与树脂发生反应,使加工性降低。
本发明通过并用丁基橡胶或卤化丁基橡胶、式(1)所示的化合物与甲醛的缩合物、以及亚甲基供体,从而能够通过较少量的丁基橡胶或卤化丁基橡胶而发挥有效地提高热塑性树脂或热塑性弹性体组合物的膜与橡胶组合物的层之间的界面的粘接强度这样显著的协同效果。
在构成橡胶组合物的橡胶成分中,作为丁基橡胶和卤化丁基橡胶以外的橡胶成分,不受特别限定,可举出二烯系橡胶及其氢化物、烯烃系橡胶、含卤素橡胶、硅橡胶、含硫橡胶、氟橡胶等。
作为二烯系橡胶及其氢化物,可举出天然橡胶(NR)、异戊二烯橡胶(IR)、环氧化天然橡胶、丁苯橡胶(SBR)、丁二烯橡胶(BR)(高顺式BR和低顺式BR)、丙烯腈丁二烯橡胶(NBR)、氢化NBR、氢化SBR等。
作为烯烃系橡胶,可举出乙丙橡胶(EPM)、三元乙丙橡胶(EPDM)、马来酸改性乙丙橡胶(M-EPM)、马来酸酐改性乙烯-α-烯烃共聚物、乙烯-甲基丙烯酸缩水甘油酯共聚物、马来酸酐改性乙烯-丙烯酸乙酯共聚物(改性EEA)、异丁烯与芳香族乙烯基系单体或二烯系单体共聚物、丙烯酸类橡胶(ACM)、离子交联聚合物等。
作为含卤素橡胶,可举出溴化异丁烯-对甲基苯乙烯共聚物(BIMS)、卤化异丁烯-异戊二烯共聚橡胶、氯丁橡胶(CR)、氯醇橡胶(CHR)、氯磺化聚乙烯(CSM)、氯化聚乙烯(CM)、马来酸改性氯化聚乙烯(M-CM)等。
作为硅橡胶,可举出甲基乙烯基硅橡胶、二甲基硅橡胶、甲基苯基乙烯基硅橡胶等。作为含硫橡胶,可举出聚硫橡胶等。
作为氟橡胶,可举出1,1-二氟乙烯系橡胶、含氟乙烯基醚系橡胶、四氟乙烯-丙烯系橡胶、含氟硅系橡胶、含氟磷腈系橡胶等。
其中,优选为二烯系橡胶、烯烃系橡胶、含卤素橡胶,从与相邻橡胶材料的共交联性的观点出发,特别优选为二烯系橡胶。优选的二烯系橡胶为天然橡胶、丁苯橡胶、丁二烯橡胶、异戊二烯橡胶、它们的混合物,进一步优选为天然橡胶与丁苯橡胶的组合、天然橡胶与丁二烯橡胶的组合。
橡胶组合物包含式(1)所示的化合物与甲醛的缩合物。
式(1)中,R1、R2、R3、R4和R5各自独立地为氢原子、羟基、碳原子数为1~8个的烷基或碳原子数为1~8个的烷氧基。
式(1)所示的化合物的一个优选例是R1、R2、R3、R4和R5中的至少1个是碳原子数为1~8个的烷基,且其余是氢原子或碳原子数为1~8个的烷基的化合物。式(1)所示的化合物的优选的具体例为甲酚。
式(1)所示的化合物的另一个优选例是R1、R2、R3、R4和R5中的至少1个是羟基,且其余是氢原子或碳原子数为1~8个的烷基的化合物。式(1)所示的化合物的优选的具体例的另一个是间苯二酚(也称为“resorcin”。)。
作为式(1)所示的化合物与甲醛的缩合物,可举出甲酚-甲醛缩合物、间苯二酚-甲醛缩合物等。此外,这些缩合物可以在不损害本发明的效果的范围内被改性。例如,被环氧化合物改性了的改性间苯二酚-甲醛缩合物也可以在本发明中使用。这些缩合物有市售,本发明可以使用市售品。
式(1)所示的化合物与甲醛的缩合物优选为式(2)或式(3)所示的化合物。
式(2)中,n为1~20的整数,优选为1~10的整数,更优选为1~5的整数。
式(3)中,m为1~20的整数,优选为1~10的整数,更优选为1~3的整数。
式(1)所示的化合物与甲醛的缩合物(以下也简称为“缩合物”。)的配合量相对于橡胶成分100质量份为0.5~20质量份,优选为1~10质量份。如果缩合物的配合量过少,则获得良好的粘接所需要的热量、时间增加,因此硫化效率恶化,相反地如果缩合物的配合量过多,则获得的橡胶组合物的硫化伸长率受损,易于断裂。
橡胶组合物包含亚甲基供体。
所谓亚甲基供体,是指通过加热等产生甲醛的碱化合物,可举出例如,六亚甲基四胺、五亚甲基四胺、六亚甲基二胺、羟甲基三聚氰胺、醚化羟甲基三聚氰胺、改性醚化羟甲基三聚氰胺、酯化羟甲基三聚氰胺、六甲氧基羟甲基三聚氰胺、六羟甲基三聚氰胺、六(乙氧基甲基)三聚氰胺、六(甲氧基甲基)三聚氰胺、N,N’,N”-三甲基-N,N’,N”-三羟甲基三聚氰胺、N,N’,N”-三羟甲基三聚氰胺、N-羟甲基三聚氰胺、N,N’-双(甲氧基甲基)三聚氰胺、N,N’,N”-三丁基-N,N’,N”-三羟甲基三聚氰胺、低聚甲醛等。其中,从甲醛的释放温度的观点出发,优选为改性醚化羟甲基三聚氰胺。
亚甲基供体的配合量相对于橡胶成分100质量份为0.25~200质量份,优选为0.5~80质量份,进一步优选为1~40质量份。如果亚甲基供体的配合量过少,则亚甲基供体在橡胶组合物体系内的树脂反应中被消耗,界面反应处的反应不进行,粘接恶化。相反地如果亚甲基供体的配合量过多,则橡胶组合物体系内的反应被过度促进,或者诱发被粘接对象树脂体系内的交联反应,粘接恶化。
亚甲基供体的配合量/缩合物的配合量之比优选为0.5~10,更优选为1~4质量份,进一步优选为1~3。如果该比过小,则供体在橡胶组合物体系内的树脂反应中被消耗,界面反应处的反应不进行,粘接恶化。相反地如果该比过大,则橡胶组合物体系内的反应被过度促进,或诱发被粘接对象树脂体系内的交联反应,粘接恶化。
橡胶组合物包含硫化剂。
作为硫化剂,有无机系硫化剂和有机系硫化剂,作为无机系硫化剂,可举出硫黄、一氯化硫、硒、碲、氧化锌、氧化镁、一氧化铅等,作为有机系硫化剂,可举出含硫有机化合物、二硫代氨基甲酸盐、肟类、四氯对苯醌、二亚硝基化合物、改性酚树脂、多胺、有机过氧化物等。其中,优选为硫黄、1,3-双(叔丁基过氧化异丙基)苯这样的有机过氧化物、溴化烷基酚-甲醛缩合物这样的改性酚树脂、氧化锌、含硫有机化合物。
硫化剂的配合量相对于橡胶成分100质量份优选为0.5~10质量份,更优选为0.5~8质量份,进一步优选为0.5~5质量份。如果硫化剂的配合量过少,则橡胶的强度降低,结果是不显示良好的粘接性。如果硫化剂的配合量过多,则阻碍橡胶与膜的粘接反应。
橡胶组合物可以进一步包含硫化促进剂。
作为硫化促进剂,可举出醛-氨系、醛-胺系、硫脲系、胍系、噻唑系、次磺酰胺系、秋兰姆系、二硫代氨基甲酸盐系、黄原酸盐系,优选为噻唑系、次磺酰胺系、秋兰姆系。
噻唑系硫化促进剂是具有噻唑结构的化合物,可举出例如,二-2-苯并噻唑基二硫化物、巯基苯并噻唑、苯并噻唑基二硫化物、巯基苯并噻唑的锌盐、(二硝基苯基)巯基苯并噻唑、(N,N-二乙基硫代氨基甲酰基硫代)苯并噻唑等,其中优选为二-2-苯并噻唑基二硫化物。
次磺酰胺系硫化促进剂是具有次磺酰胺结构的化合物,可举出例如,N-环己基苯并噻唑次磺酰胺、N-叔丁基苯并噻唑次磺酰胺、N-氧基二亚乙基苯并噻唑次磺酰胺、N,N-二环己基苯并噻唑次磺酰胺、(吗啉基二硫代)苯并噻唑等,其中优选为N-叔丁基-2-苯并噻唑次磺酰胺。
秋兰姆系硫化促进剂是具有秋兰姆结构的化合物,可举出例如,四(2-乙基己基)秋兰姆二硫化物、四甲基秋兰姆二硫化物、四甲基秋兰姆单硫化物、四乙基秋兰姆二硫化物、四丁基秋兰姆二硫化物、双五亚甲基秋兰姆六硫化物等,其中优选为四(2-乙基己基)秋兰姆二硫化物。
硫化促进剂的配合量相对于橡胶成分100质量份优选为0.5~10质量份,更优选为0.5~8质量份,进一步优选为0.5~5质量份。如果硫化促进剂的配合量过少,则硫化反应不能在所期望的硫化时间以内完成,因此橡胶强度降低,结果是不显示良好的粘接性。如果硫化促进剂的配合量过多,则阻碍橡胶与膜的粘接反应。
本发明的叠层体可以通过对热塑性树脂或热塑性弹性体组合物的膜叠层橡胶组合物来制造。不进行限定,但更具体地可以如下操作来制造。首先,将热塑性树脂或热塑性弹性体组合物利用吹胀成型装置、T型模挤出机等成型装置成型成膜状,制作热塑性树脂或热塑性弹性体组合物的膜。接下来,利用T型模挤出机等将橡胶组合物挤到上述膜上,同时进行叠层,制造叠层体。
本发明的充气轮胎可以通过常规方法来制造。例如,可以将作为内衬层材料的本发明的叠层体以热塑性树脂或热塑性弹性体组合物的膜侧朝向轮胎成型用鼓的方式置于轮胎成型用鼓上,在其上依次贴合由未硫化橡胶形成的胎体层、带束层、胎面层等通常的轮胎制造所使用的构件,成型后,去掉鼓,制成生胎,接着,按照常规方法将该生胎加热硫化,从而制造充气轮胎。
实施例
(1)橡胶组合物的调制
以表1和表2所示的配合比率配合下述原料,调制出橡胶组合物。
丁苯橡胶:日本ゼオン株式会社制“Nipol 1502”
溴化丁基橡胶:エクソンモービルケミカル社制“ブロモブチル2255”
丁基橡胶:エクソンモービルケミカル社制“Butyl 268”
天然橡胶:SIR-20
炭黑:东海カーボン株式会社制“シーストV”
硬脂酸:工业用硬脂酸
芳香油:昭和シェル石油株式会社制“デソレックス3号”
氧化锌:正同化学工业株式会社制“氧化锌3号”
改性间苯二酚-甲醛缩合物:田冈化学工业株式会社制“スミカノール620”
亚甲基供体:改性醚化羟甲基三聚氰胺(田冈化学工业株式会社制“スミカノール507AP”)
硫黄:5%充油处理硫黄
硫化促进剂:二-2-苯并噻唑基二硫化物(大内新兴化学工业株式会社制“ノクセラーDM”)
(2)热塑性弹性体组合物膜的制作
将溴化异丁烯-对甲基苯乙烯共聚物(エクソンモービルケミカル社制“EXXPRO”(注册商标)3035)100质量份、氧化锌(正同化学工业株式会社制“氧化锌3号”)0.5质量份、硬脂酸(工业用硬脂酸)0.2质量份、硬脂酸锌(日油株式会社制“硬脂酸锌”)1质量份、尼龙6/66(宇部兴产株式会社制“UBE尼龙”5033B)100质量份、马来酸酐改性乙烯-丙烯酸乙酯共聚物(アルケマ社制“リルサン”(注册商标)BESN O TL)10质量份以及增塑剂(大八化学工业株式会社制N-丁基苯磺酰胺“BM-4”)20质量份配合在一起,调制热塑性弹性体组合物,将该热塑性弹性体组合物利用吹胀成型装置成型,制作出厚0.1mm的热塑性弹性体组合物膜。以下将制作的热塑性弹性体组合物膜也称为“膜A”。
(3)热塑性树脂膜的制作
将宇部兴产(株)制的UBE尼龙(注册商标)5033B利用吹胀成型装置成型,制作出厚0.1mm的热塑性树脂膜。以下将制作的热塑性树脂膜也称为“膜B”。
(4)叠层体的制作
使用挤出机,将由上述(1)调制的橡胶组合物以0.7mm的厚度挤出叠层在由上述(2)和(3)制作的膜上,制作出叠层体。
(5)叠层体的评价
关于制作的叠层体,评价了剥离强度。将热塑性弹性体组合物膜与橡胶组合物的叠层体的评价结果示于表1中,将热塑性树脂膜与橡胶组合物的叠层体的评价结果示于表2中。另外,剥离强度的评价方法如下所述。
[剥离强度]
将叠层体的试样硫化,然后切成宽25mm,按照JIS-K6256来测定该长条状试验片的膜与橡胶之间的界面的剥离强度。在表1和表2中,以相对于各自的比较例的剥离强度的比率(以下称为“剥离强度指数”。)来表示各实施例的剥离强度。另外,比较例1的剥离强度为160N/25mm,比较例2的剥离强度为200N/25mm。
产业可利用性
本发明的叠层体可以很好地用作充气轮胎的内衬层材料。
Claims (9)
2.根据权利要求1所述的叠层体,其特征在于,亚甲基供体的配合量/所述缩合物的配合量之比为0.5~10。
3.根据权利要求1或2所述的叠层体,其特征在于,热塑性树脂为选自聚乙烯醇、乙烯-乙烯醇共聚物、尼龙6、尼龙66、尼龙11、尼龙12、尼龙610、尼龙612、尼龙6/66、尼龙MXD6和尼龙6T中的至少1种。
4.根据权利要求1或2所述的叠层体,其特征在于,热塑性弹性体组合物是使弹性体成分分散于热塑性树脂成分而得的组合物,热塑性树脂成分为选自聚乙烯醇、乙烯-乙烯醇共聚物、尼龙6、尼龙66、尼龙11、尼龙12、尼龙610、尼龙612、尼龙6/66、尼龙MXD6和尼龙6T中的至少1种,弹性体成分为选自溴化异丁烯-对甲基苯乙烯共聚物、马来酸酐改性乙烯-α-烯烃共聚物、乙烯-甲基丙烯酸缩水甘油酯共聚物和马来酸酐改性乙烯-丙烯酸乙酯共聚物中的至少1种。
5.根据权利要求1或2所述的叠层体,其特征在于,亚甲基供体为选自改性醚化羟甲基三聚氰胺、低聚甲醛、六亚甲基四胺、五亚甲基四胺和六甲氧基甲基三聚氰胺中的至少1种。
6.根据权利要3所述的叠层体,其特征在于,亚甲基供体为选自改性醚化羟甲基三聚氰胺、低聚甲醛、六亚甲基四胺、五亚甲基四胺和六甲氧基甲基三聚氰胺中的至少1种。
7.根据权利要求4所述的叠层体,其特征在于,亚甲基供体为选自改性醚化羟甲基三聚氰胺、低聚甲醛、六亚甲基四胺、五亚甲基四胺和六甲氧基甲基三聚氰胺中的至少1种。
8.一种充气轮胎用内衬层材料,由权利要求1~7中任一项所述的叠层体构成。
9.一种充气轮胎,使用了权利要求1~7中任一项所述的叠层体作为内衬层材料。
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Address after: Kanagawa Prefecture, Japan Patentee after: THE YOKOHAMA RUBBER Co.,Ltd. Country or region after: Japan Address before: Tokyo, Japan Patentee before: THE YOKOHAMA RUBBER Co.,Ltd. Country or region before: Japan |