CN110724366A - 预浸物、积层板以及印刷电路板 - Google Patents

预浸物、积层板以及印刷电路板 Download PDF

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Publication number
CN110724366A
CN110724366A CN201911127763.1A CN201911127763A CN110724366A CN 110724366 A CN110724366 A CN 110724366A CN 201911127763 A CN201911127763 A CN 201911127763A CN 110724366 A CN110724366 A CN 110724366A
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Prior art keywords
dopo
prepreg
epoxy resin
weight
group
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CN201911127763.1A
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Inventor
刘明
翁宗烈
苑绍杰
陈凯杨
于达元
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Lianmao (wuxi) Electronic Technology Co Ltd
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Lianmao (wuxi) Electronic Technology Co Ltd
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Priority to CN201911127763.1A priority Critical patent/CN110724366A/zh
Publication of CN110724366A publication Critical patent/CN110724366A/zh
Priority to US16/822,013 priority patent/US20210147646A1/en
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Abstract

本发明公开一种预浸物，及其积层板与印刷电路板。本发明的预浸物包括无卤环氧树脂组成物以及含浸于其中且经部分固化的非织造强化材料。非织造强化材料具有1.5至4.8的介电强度以及在10GHz下低于0.003的耗损因子，无卤环氧树脂组成物包括：(a)100重量份的无卤萘型环氧树脂；(b)10至25重量份的DOPO改质硬化剂；(c)25至45重量份的氰酸酯树脂；(d)35至60重量份的双马来酰亚胺；(e)45至65重量份的非DOPO阻燃剂；以及(f)0.5至15重量份的硬化促进剂。本发明的预浸物有效改善延迟效应，且具有较高的玻璃转化温度、低介电损耗、高耐热性及高储存模数的特性。

Description

预浸物、积层板以及印刷电路板
技术领域
本发明涉及一种预浸物、积层板以及印刷电路板，特别是涉及一种使用无卤环氧树脂组成物的预浸物、积层板以及印刷电路板。
背景技术
印刷电路板(PCB)通常是以强化材料含浸于一高分子材料中形成一复合材料，再进一步在所述复合材料的一侧或两侧以金属层压合(clad)，以形成用于PCB应用中的积层板。
一般强化材料大多为织造玻璃材料，举例而言，如低介电常数(Dk)玻璃、E型玻璃、R型玻璃、ECR型玻璃、S型玻璃、C型玻璃以及Q型玻璃，然而，织造玻璃材料与高分子材料为异质材料，因而导致信号延迟的情况，此现象在数位工程领域已知为“传输延迟(skew)”。
此外，现有技术的高分子材料中常使用含卤素成份的阻燃剂(特别是溴系阻燃剂)，如四溴环己烷、六溴环癸烷以及2,4,6-三(三溴苯氧基)-1,3,5-三氮杂苯等，含卤素成份的阻燃剂具有阻燃性好且添加少的优点，然而，卤素产品在产品制造、使用，更甚至在回收或丢弃时易对环境造成污染，除此之外，含卤素的电子设备废弃物在燃烧时会产生腐蚀性、毒性气体及烟雾，且在燃烧后产物会检测出二恶英、二苯并呋喃等致癌物质。
综上所述，改良上述缺陷并维持积层板的耐热性、难燃性、低介电损耗、低吸湿性、高交联密度、高玻璃转化温度、高接合性、适当的热膨胀性等特性更是印刷电路板的开发及制造的重要课题。
发明内容
本发明所要解决的技术问题在于，针对现有技术的不足提供一种使用无卤环氧树脂组成物以及非织造强化材料的预浸物、积层板以及印刷电路板。
为了解决上述的技术问题，本发明所采用的其中一技术方案是，提供一种预浸物，其包括：一非织造强化材料以及一无卤环氧树脂组成物，且所述非织造强化材料是含浸于所述无卤环氧树脂组成物且经部分固化。其中，所述非织造强化材料具有自1.5至4.8的介电强度以及在10GHz下低于0.003的耗损因子，且所述无卤环氧树脂组成物包括：(a)100重量份的无卤萘型环氧树脂；(b)10至25重量份的DOPO改质硬化剂；(c)25至45重量份的氰酸酯树脂；(d)35至60重量份的双马来酰亚胺；(e)45至65重量份的非DOPO阻燃剂；以及(f)0.5至15重量份的硬化促进剂。
更进一步地，所述无卤萘型环氧树脂是选自双官能萘型环氧树脂、四官能萘型环氧树脂以及含恶唑烷酮双官能萘型环氧树脂所组成的群组的至少一者。
更进一步地，所述DOPO改质硬化剂是选自DOPO-对苯二酚树脂、DOPO-萘二醇树脂、DOPO-酚醛清漆树脂以及DOPO-双酚酚醛树脂所组成的群组；其中，所述DOPO-双酚酚醛树脂是选自DOPO-双酚A线型酚醛树脂、DOPO-双酚F线型酚醛树脂以及DOPO-双酚S线型酚醛树脂所组成的群组的至少一者。
更进一步地，所述双马来酰亚胺是选自双(4-马来酰亚胺基苯基)甲烷、2,2-双(4-(4-马来酰亚胺基苯氧基)-苯基)丙烷、双(3,5-二甲基-4-马来酰亚胺基苯基)甲烷、双(3-乙基-5-甲基-4-马来酰亚胺基苯基)甲烷和双(3,5-二乙基-4-马来酰亚胺基苯基)甲烷所组成的群组的至少一者。
更进一步地，所述非DOPO阻燃剂是选自结构式(Ⅰ)、结构式(Ⅱ)以及结构式(Ⅲ)的化合物所组成的群组：
Figure BDA0002277391140000021
Figure BDA0002277391140000022
以及
其中，R1是
Figure BDA0002277391140000032
Figure BDA0002277391140000041
其中，R2是
Figure BDA0002277391140000042
其中，R3是
Figure BDA0002277391140000043
或CH2CH2OCH＝CH2；
其中，n是0至500的整数；
其中，R4是
Figure BDA0002277391140000044
其中，m≧1；
其中，R5是
其中，R6是
Figure BDA0002277391140000051
Figure BDA0002277391140000052
更进一步地，所述预浸物还进一步包括：一阻燃性化合物，其是选自间苯二酚双二甲苯基磷酸盐、聚磷酸三聚氰胺、三(2-羧乙基)膦、三甲基磷酸盐、三(异丙基氯)磷酸盐、二甲基-甲基磷酸盐、双酚联苯磷酸盐、聚磷酸铵、对苯二酚-双-(联苯基磷酸盐)、双酚A-双-(联苯基磷酸盐)所组成的群组的至少一者。
更进一步地，所述硬化促进剂是选自三氟化硼胺复合物、2-乙基-4-甲基咪唑、2-甲基咪唑、2-苯基咪唑、氯化乙基三苯基鏻、三苯基膦、乙酰丙酮钴(Ⅱ)、4-二甲基胺基吡啶、端溴基液体丁二烯橡胶、双乙酰丙酮钴(Ⅱ)、三乙酰丙酮钴(Ⅲ)、三乙胺、三丁胺、二氮杂双环[2,2,2]辛烷所组成的群组的至少一者。
更进一步地，所述无机填料是选自二氧化硅、氧化铝、氢氧化铝、氧化镁、氢氧化镁、碳酸钙、氮化铝、氮化硼、碳化铝硅、碳化硅、二氧化钛、氧化锌、氧化锆、硫酸钡、碳酸镁、碳酸钡、云母、滑石以及石墨烯所组成的群组的至少一者。
更进一步地，所述预浸物还进一步包括：一溶剂，且所述溶剂是选自丙酮、丁酮、丙二醇甲醚、丙二醇甲醚醋酸酯、二甲基乙酰胺以及环己酮所组成的群组的至少一者。
更进一步地，所述非织造强化材料是选自聚四氟乙烯、液晶聚合物、石英以及玻璃所组成的群组的至少一者。
为了解决上述的技术问题，本发明所采用的另外一技术方案是，提供一种积层板，其包括：一树脂基板，其包括多个本发明所述的预浸物固化所制成；以及至少一金属箔层，其设置于所述树脂基板的至少一表面上。
为了解决上述的技术问题，本发明所采用的另外再一技术方案是，提供一种印刷电路板，其是将本发明的积层板的金属箔层图案化而形成。
本发明的其中一有益效果在于，本发明所提供的卷绕型固态电解电容器封装结构及其制作方法，其能通过“所述非织造强化材料具有自1.5至4.8的介电强度以及在10GHz下低于0.003的耗损因子”以及“45至65重量份的非DOPO阻燃剂”的技术方案，以提供较佳的玻璃转化温度，并消除传输延迟的现象。
为使能更进一步了解本发明的特征及技术内容，请参阅以下有关本发明的详细说明与图式，然而所提供的图式仅用于提供参考与说明，并非用来对本发明加以限制。
为使能更进一步了解本发明的特征及技术内容，请参阅以下有关本发明的详细说明与附图，然而所提供的附图仅用于提供参考与说明，并非用来对本发明加以限制。
附图说明
图1为本发明的预浸物的剖面示意图。
图2为本发明的积层板的剖面示意图。
图3为本发明的印刷电路板的剖面示意图。
具体实施方式
以下是通过特定的具体实施例来说明本发明所公开有关“预浸物、积层板以及印刷电路板”的实施方式，本领域技术人员可由本说明书所公开的内容了解本发明的优点与效果。本发明可通过其他不同的具体实施例加以施行或应用，本说明书中的各项细节也可基于不同观点与应用，在不悖离本发明的构思下进行各种修改与变更。另外，本发明的附图仅为简单示意说明，并非依实际尺寸的描绘，事先声明。以下的实施方式将进一步详细说明本发明的相关技术内容，但所公开的内容并非用以限制本发明的保护范围。
应当可以理解的是，本文中所使用的术语“或”，应视实际情况可能包括相关联的列出项目中的任一个或者多个的组合。
参阅图1所示，本发明提供一种预浸物1，其包括非织造强化材料11以及无卤环氧树脂组成物12，且非织造强化材料11是含浸于无卤环氧树脂组成物12且经部分固化。
参阅图2所示，本发明进一步提供一种积层板C，其包括：至少一树脂基板1以及至少一金属箔层2、2’，树脂基板1是如图1的预浸材1固化所制成；金属箔层2、2’设置于树脂基板1的表面，然后进行压合而形成。除此之外，于本发明的一实施例中，积层板C包括多个树脂基板1，依照金属箔层2、多个树脂基板1、金属箔层2’的顺序进行迭合，也就是说，多个树脂基板1是迭合并夹置于金属箔层2以及金属箔层2’之间。金属箔层2、2’可以是铜箔。压合的条件包括：压力200至220psi、温度200至250℃以及时间1至3小时。
参阅图3所示，本发明的积层板C可应用于印刷电路板P，印刷电路板P是将积层板C的金属箔层2、2’图案化而形成。举例来说，可以通过微影蚀刻制程将金属箔层2、2’图案化，进一步形成印刷电路线路层。
具体来说，半导体组件的热膨胀系数为3至6ppm/℃。萘型环氧树脂的热膨胀系数相较于一般半导体塑料封装用的印刷布线板小。因此，当半导体塑料封装经历热骤变时，由于在半导体组件与半导体塑料封装用的印刷布线板间的热膨胀系数差异，会造成半导体塑料封装发生翘曲，更甚至会造成连接瑕疵。
当具刚性的稠环结构引入环氧骨架时，可以减弱环氧树脂链段的运动、降低自由体积、增大高分子链段的刚性、提高环氧树脂固化物的堆积密度，大幅提高环氧固化物的耐热性能。而稠环结构环氧树脂按结构可分为萘系、蒽系、芘系环氧树脂，蒽系与芘系环氧树脂合成反应时间长、产率低、原料较贵、反应活性较低，且由于蒽环和芘环的体积较大，对树脂的交联密度影响较大，因此蒽环和芘环在提高环氧树脂的耐热性能方面有限。相较于此，萘环化合物具有较高的反应活性和耐热性，适于环氧树脂组成物。
具体而言，萘型环氧树脂的萘环结构具有高耐热性、低热膨胀系数(CTE)以及低吸湿性；较佳地，无卤萘型环氧树脂是选自双官能萘型环氧树脂、四官能萘型环氧树脂以及含恶唑烷酮双官能萘型环氧树脂所组成的群组。举例来说，如下列结构所示：
Figure BDA0002277391140000081
再者，9,10-二氢-9-氧杂-10-磷菲-10-氧化物(9,10-dihydro-9-oxa-10-phosphaphenanthrene-10-oxide，DOPO)改质硬化剂于本发明主要是做为与环氧树脂结合的硬化剂使用，改质硬化剂除了可提供良好的热稳定性和低介电性外，更可提升阻燃的功效，本发明的无卤环氧树脂组成物中DOPO改质硬化剂是选自DOPO-对苯二酚树脂、DOPO-萘二醇树脂、DOPO-酚醛清漆树脂以及DOPO-双酚酚醛树脂所组成的群组。更进一步而言，DOPO-双酚酚醛树脂是选自DOPO-双酚A线型酚醛树脂(DOPO-BPAN)、DOPO-双酚F线型酚醛树脂(DOPO-BPSN)以及DOPO-双酚S线型酚醛树脂(DOPO-BPSN)所组成的群组。
本发明所使用的氰酸酯树脂并无特别限定，氰酸酯树脂可增加树脂结构中的反应官能团，进而提高环氧固化物的交联密度，降低无卤环氧树脂组成物的自由体积，提高耐热性。举例而言，氰酸酯树脂可以是多官能脂肪族系异氰酸酯化合物、多官能脂环族系异氰酸酯、多官能芳香族系异氰酸酯化合物，如：三亚甲基二异氰酸酯、四亚甲基二异氰酸酯、六亚甲基二异氰酸酯、五亚甲基二异氰酸酯、1,2-伸丙基二异氰酸酯、1,3-伸丁基二异氰酸酯、十二亚甲基二异氰酸酯、2,4,4-三甲基六亚甲基二异氰酸酯等、1,3-环戊烯二异氰酸酯、1,3-环己烷二异氰酸酯、1,4-环己烷二异氰酸酯、异佛尔酮二异氰酸酯、氢化二苯基甲烷二异氰酸酯、氢化苯二亚甲基二异氰酸酯、氢化甲苯二异氰酸酯、氢化四甲基苯二亚甲基二异氰酸酯、伸苯基二异氰酸酯、2,4-甲苯二异氰酸酯、2,6-甲苯二异氰酸酯、2,2'-二苯基甲烷二异氰酸酯、4,4'-二苯基甲烷二异氰酸酯、4,4'-甲苯胺二异氰酸酯、4,4'-二苯基醚二异氰酸酯、4,4'-二苯基二异氰酸酯、1,5-萘二异氰酸酯、苯二亚甲基二异氰酸酯等。
本发明的双马来酰亚胺化合物并未特别的限制，主要是分子中含有两个马来酰亚胺基团的化合物，也可以使用双马来酰亚胺化合物的预聚物，或双马来酰亚胺化合物与胺化合物的预聚物。较佳地，双马来酰亚胺是选自双(4-马来酰亚胺基苯基)甲烷、2,2-双(4-(4-马来酰亚胺基苯氧基)-苯基)丙烷、双(3,5-二甲基-4-马来酰亚胺基苯基)甲烷、双(3-乙基-5-甲基-4-马来酰亚胺基苯基)甲烷和双(3,5-二乙基-4-马来酰亚胺基苯基)甲烷所组成的群组。
本发明无卤环氧树脂组成物的阻燃剂使用非DOPO阻燃剂，意即不含9,10-二氢-9-氧杂-10-磷杂菲-10-氧化物(DOPO)衍生物。详细而言，DOPO结构内的P-O-C键结容易水解为P-OH，会使材料介电常数及介电损耗上升，故选用非DOPO阻燃剂可避免提升材料的Dk以及Df，其中，Dk即为介电常数(Dielectric Constant，εr)，Df为介电损耗。
较佳地，非DOPO阻燃剂可选自结构式(Ⅰ)、结构式(Ⅱ)以及结构式(Ⅲ)的化合物所组成的群组：
Figure BDA0002277391140000101
以及
Figure BDA0002277391140000103
其中，R1是
Figure BDA0002277391140000104
Figure BDA0002277391140000111
其中，R2是
Figure BDA0002277391140000112
Figure BDA0002277391140000113
其中，R3是或CH2CH2OCH＝CH2；
其中，n是0至500的整数；
其中，R4是
Figure BDA0002277391140000121
Figure BDA0002277391140000122
其中，m≧1；
其中，R5是
Figure BDA0002277391140000123
其中，R6是
Figure BDA0002277391140000124
Figure BDA0002277391140000125
除此之外，本发明的无卤环氧树脂组成物视需求进一步包括阻燃性化合物，可选自磷酸盐化合物或含氮磷酸盐化合物，举例而言，可以是选自间苯二酚双二甲苯基磷酸盐(resorcinol dixylenylphosphate，RDXP(如PX-200))、聚磷酸三聚氰胺(melaminepolyphosphate)、三(2-羧乙基)膦(tri(2-carboxyethyl)phosphine，TCEP)、三甲基磷酸盐(trimethyl phosphate，TMP)、三(异丙基氯)磷酸盐、二甲基-甲基磷酸盐(dimethylmethyl phosphonate，DMMP)、双酚联苯磷酸盐(bisphenol diphenyl phosphate)、聚磷酸铵(ammonium polyphosphate)、对苯二酚-双-(联苯基磷酸盐)(hydroquinone bis-(diphenyl phosphate))、双酚A-双-(联苯基磷酸盐)(bisphenol A bis-(diphenylphosphate))所组成的群组。
较佳地，本发明硬化促进剂可选自咪唑、金属盐、三级胺或呱啶类化合物所组成的群组的至少一者或其混合，更进一步的可选自三氟化硼胺复合物、2-乙基-4-甲基咪唑(2-ethyl-4-methylimidazole，2E4MI)、2-甲基咪唑(2-methylimidazole，2MI)、2-苯基咪唑(2-phenyl-1H-imidazole，2PZ)、氯化乙基三苯基鏻(ethyltriphenyl phosphoniumchloride)、三苯基膦(triphenylphosphine，TPP)、乙酰丙酮钴(Ⅱ)(cobalt(Ⅱ)acetylacetonate)与4-二甲基胺基吡啶(4-dimethylaminopyridine，DMAP)、低分子量的端溴基液体丁二烯橡胶(terminal bromine-based liquid butadiene rubber，BTPB)，有机金属盐如双乙酰丙酮钴(Ⅱ)、三乙酰丙酮钴(Ⅲ)，三级胺类如三乙胺、三丁胺等以及二氮杂双环[2,2,2]辛烷等。更佳地，硬化促进剂是2-苯基咪唑以及双乙酰丙酮钴(Ⅱ)。具体而言，咪唑类化合物对树脂成分具有尤佳的兼容性，借此可获得均匀性高的硬化物。
另一方面，无机填料可增加无卤环氧树脂组成物的热传导性，改良其热膨胀性以及机械强度，较佳地，无机填料是均匀分布于无卤环氧树脂组成物中。较佳地，无机填料可经由硅烷偶合剂预先进行表面处理。较佳地，无机填料可为球型、片状、粒状、柱状、板状、针状或不规则状的无机填料。较佳地，无机填料选自二氧化硅(如熔融态、非熔融态、多孔质或中空型的二氧化硅)、氧化铝、氢氧化铝、氧化镁、氢氧化镁、碳酸钙、氮化铝、氮化硼、碳化铝硅、碳化硅、二氧化钛、氧化锌、氧化锆、硫酸钡、碳酸镁、碳酸钡、云母、滑石、石墨烯所组成的群组。
此外，本发明的无卤环氧树脂组成物更进一步包括适量的溶剂，举例而言，酮类、酯类、醚类、醇类等，更具体而言，本发明的溶剂是选自丙酮、丁酮、丙二醇甲醚、丙二醇甲醚醋酸酯、二甲基乙酰胺以及环己酮所组成的群组。
此外，本发明的预浸物包括：非织造强化材料，举例来说，可以是选自聚四氟乙烯、液晶聚合物、石英以及玻璃所组成的群组的至少一者，更详细来说，可以是非织造PTFE垫/纸、非织造石英垫/纸或是液晶聚合物等片状型材料，且其成分可以包括短纤(chopped)PTFE纤维、短纤(chopped)玻璃纤维。更详细来说，玻璃可以选自非织造E型玻璃纤维布、D型玻璃纤维布、S型玻璃纤维布、T型玻璃纤维布、L型玻璃纤维布或NE玻璃纤维布。
举体来说，非织造材料与传统的织造材料有较大的差异。非织造材料工艺的基本要求是力求避免或减少将纤维形成纱线这样的纤维集合体、再将纱线组合成一定的几何结构，而是让纤维呈单纤维分布状态后形成纤维网这样的集合体。典型的非织造材料都是由纤维组成的网络状结构形成的。同时为了进一步增加其强力，达到结构的稳定性，所形成的纤网还视需求通过施加黏合剂、热黏合、纤维与纤维的缠结、外加纱线缠结等方法予以加固。因此，大多数非织造材料的结构就是由纤维网与加固系统所共同组成的基本结构。
实施例E1至E6
实施例E1至E6的组成如以下表1所示。实施例E1至E6以非织造PTFE垫作强化材料，使其连续地通过一系列滚轮进入上胶槽，槽里装载本发明的无卤环氧树脂组成物(如表1所示)。在上胶槽中强化材料被无卤环氧树脂组成物充分浸润，然后经过计量辊刮除多余的无卤环氧树脂组成物，进入上胶炉烘烤100至180分钟，使溶剂蒸发并使树脂固化，再经过冷却、收卷，形成树脂基板。将上述树脂基板与两张18μm铜箔，依铜箔、树脂基板、铜箔的顺序进行迭合，再于真空条件下经由220℃压合2小时形成铜箔基板。
表1
Figure BDA0002277391140000141
*NPTE4000萘环环氧树脂：
*HP-6000(购自日本DIC公司)萘型(Naphthalene)环氧树脂
比较例C1至C5
比较例C1至C5的组成如以下表1所示。比较例C1至C5以织造E级玻璃(编织过的E级玻璃纤维布)作强化材料，使其连续地通过一系列滚轮进入上胶槽，槽里装载树脂组成物(如表2所示)。在上胶槽中强化材料被树脂组成物充分浸润，然后经过计量辊刮除多余的树脂组成物，进入上胶炉烘烤120至180分钟，使溶剂蒸发并使树脂固化，再经过冷却、收卷，形成树脂基板。将上述树脂基板与两张18μm铜箔，依铜箔、树脂基板、铜箔的顺序进行迭合，再于真空条件下经由220℃压合2小时形成铜箔基板。
表2
Figure BDA0002277391140000161
Figure BDA0002277391140000171
物性测试
分别将上述实施例E1至E6及比较例C1至C5的铜箔积层板进行物性测试，并纪录测试结果于表3：
玻璃转化温度(Tg)：根据差示扫描量热法(DSC)，依据IPC-TM-650 2.4.25所规定的DSC方法进行测定。
铜箔积层板耐热性(T288)：亦称“漂锡结果”，耐热实验是依据产业标准IPC-TM-650 2.4.24.1，将铜箔积层板浸泡于288℃锡炉至爆板所需时间。
含铜箔积层板吸湿后浸锡测试：使用含铜箔层的半固化胶片进行耐热性(T288)测试，依据产业标准IPC-TM-650 2.4.24.1，将铜箔积层板浸泡于288℃锡炉至爆板所需时间。
吸水率：由于覆铜基板会受环境的温度及湿度影响而膨胀变形或吸附水气，且在覆铜基板含水量、含湿度过高的情况下，易产生爆板的问题或其他电路板的缺陷等等，因此须测定吸水率以判定覆铜基板的吸水特性。传统上，可针对该材料进行IR光谱分析或热重量损失法分析，以确认该覆铜基板的吸水性。
铜箔与基板间拉力(peeling strength,half ounce copper foil,P/S)：依据IPC－TM－650 2.4.1检测规范进行测定。
介电常数(Dk)：依据IPC－TM－650 2.5.5检测规范进行测定，介电常数代表所制胶片的电子绝缘特性，数值越低代表电子绝缘特性越好。
介电损耗(Df)：依据IPC－TM－650 2.5.5检测规范进行测定，介电损耗表示物质在一定温度下吸收某一频率的微波的能力，通常在通讯产品的规范里，介电损耗数值需越低越好。
耐燃性(flaming test，UL94)：依据UL94垂直燃烧法测定，其以塑料材料标准试片经火焰燃烧后的自燃时间、自燃速度、掉落的颗粒状态来订定塑料材料的耐燃等级。而依耐燃等级优劣，依次是HB、V-2、V-1、V-0、最高为5V等级。而UL 94测试方法是指塑料材料以垂直方式在火焰上燃烧。以每十秒为一测试周期，其步骤如下：步骤一：将试片放进火焰中十秒再移开，测定移开之后该试片继续燃烧时间(T1)；步骤二：当试片火焰熄灭后，再放进火焰中十秒再移开，再测定移开之后该试片继续燃烧时间(T2)；步骤三：重复数次实验并取其平均值；步骤四：计算T1+T2的总合。而UL 94 V-0等级的要求是为在试片单一燃烧时间T1的平均及T2的平均皆不得超过10秒，且其T1与T2的总合不得超过50秒方符合UL 94V-0要求。
基板绝缘层的X或Y轴热膨胀系数(CTE)：依IPC-TM-650-2.4.24测试标准量测。
基板绝缘层的储存模数(storage modulus，以DMA仪器量测，依IPC-TM-650-2.4.24.2测试标准)于约250℃的条件下是大于或等于5000MPa。
实施例的有益效果
本发明的其中一有益效果在于，本发明所提供的卷绕型固态电解电容器封装结构及其制作方法，其能通过“所述非织造强化材料具有自1.5至4.8的介电强度以及在10GHz下低于0.003的耗损因子”以及“45至65重量份的非DOPO阻燃剂”的技术方案，以提供较佳的玻璃转化温度，并消除传输延迟的现象。
更进一步来说，本发明借由萘型环氧树脂大幅提高无卤环氧树脂组成物的耐热性能，更降低热膨胀系数。DOPO改质硬化剂不仅提供良好的热稳定性及低介电性，更提升阻燃的功效，而使用非DOPO阻燃剂可避免提升材料的Dk以及Df。
以上所公开的内容仅为本发明的优选可行实施例，并非因此局限本发明的权利要求书的保护范围，所以凡是运用本发明说明书及附图内容所做的等效技术变化，均包含于本发明的权利要求书的保护范围内。

Claims (12)

1.一种预浸物，其特征在于，所述预浸物包括：
一非织造强化材料，其具有自1.5至4.8的介电强度以及在10GHz下低于0.003的耗损因子；以及
一无卤环氧树脂组成物，其包括；
(a)100重量份的无卤萘型环氧树脂；
(b)10至25重量份的DOPO改质硬化剂；
(c)25至45重量份的氰酸酯树脂；
(d)35至60重量份的双马来酰亚胺；
(e)45至65重量份的非DOPO阻燃剂；以及
(f)0.5至15重量份的硬化促进剂；
其中，所述非织造强化材料是含浸于所述无卤环氧树脂组成物且经部分固化。
2.根据权利要求1所述的预浸物，其特征在于，所述无卤萘型环氧树脂是选自双官能萘型环氧树脂、四官能萘型环氧树脂以及含恶唑烷酮双官能萘型环氧树脂所组成的群组的至少一者。
3.根据权利要求1所述的预浸物，其特征在于，所述DOPO改质硬化剂是选自DOPO-对苯二酚树脂、DOPO-萘二醇树脂、DOPO-酚醛清漆树脂以及DOPO-双酚酚醛树脂所组成的群组；其中，所述DOPO-双酚酚醛树脂是选自DOPO-双酚A线型酚醛树脂、DOPO-双酚F线型酚醛树脂以及DOPO-双酚S线型酚醛树脂所组成的群组的至少一者。
4.根据权利要求1所述的预浸物，其特征在于，所述双马来酰亚胺是选自双(4-马来酰亚胺基苯基)甲烷、2,2-双(4-(4-马来酰亚胺基苯氧基)-苯基)丙烷、双(3,5-二甲基-4-马来酰亚胺基苯基)甲烷、双(3-乙基-5-甲基-4-马来酰亚胺基苯基)甲烷和双(3,5-二乙基-4-马来酰亚胺基苯基)甲烷所组成的群组的至少一者。
5.根据权利要求1所述的预浸物，其特征在于，所述非DOPO阻燃剂是选自结构式(Ⅰ)、结构式(Ⅱ)以及结构式(Ⅲ)的化合物所组成的群组：
以及
Figure FDA0002277391130000022
其中，R1是
Figure FDA0002277391130000023
Figure FDA0002277391130000031
其中，R2是
Figure FDA0002277391130000032
Figure FDA0002277391130000033
其中，R3是
Figure FDA0002277391130000034
或CH2CH2OCH＝CH2；
其中，n是0至500的整数；
其中，R4是
Figure FDA0002277391130000041
其中，m≥1；
其中，R5是
Figure FDA0002277391130000042
其中，R6是
Figure FDA0002277391130000043
Figure FDA0002277391130000044
6.根据权利要求1所述的预浸物，其特征在于，所述预浸物还进一步包括：一阻燃性化合物，其是选自间苯二酚双二甲苯基磷酸盐、聚磷酸三聚氰胺、三(2-羧乙基)膦、三甲基磷酸盐、三(异丙基氯)磷酸盐、二甲基-甲基磷酸盐、双酚联苯磷酸盐、聚磷酸铵、对苯二酚-双-(联苯基磷酸盐)、双酚A-双-(联苯基磷酸盐)所组成的群组的至少一者。
7.根据权利要求1所述的预浸物，其特征在于，所述硬化促进剂是选自三氟化硼胺复合物、2-乙基-4-甲基咪唑、2-甲基咪唑、2-苯基咪唑、氯化乙基三苯基鏻、三苯基膦、乙酰丙酮钴(II)、4-二甲基胺基吡啶、端溴基液体丁二烯橡胶、双乙酰丙酮钴(II)、三乙酰丙酮钴(III)、三乙胺、三丁胺、二氮杂双环[2，2，2]辛烷所组成的群组的至少一者。
8.根据权利要求1所述的预浸物，其特征在于，所述无机填料是选自二氧化硅、氧化铝、氢氧化铝、氧化镁、氢氧化镁、碳酸钙、氮化铝、氮化硼、碳化铝硅、碳化硅、二氧化钛、氧化锌、氧化锆、硫酸钡、碳酸镁、碳酸钡、云母、滑石以及石墨烯所组成的群组的至少一者。
9.根据权利要求1所述的预浸物，其特征在于，所述预浸物还进一步包括：一溶剂，且所述溶剂是选自丙酮、丁酮、丙二醇甲醚、丙二醇甲醚醋酸酯、二甲基乙酰胺以及环己酮所组成的群组的至少一者。
10.根据权利要求1所述的预浸物，其特征在于，所述非织造强化材料是选自聚四氟乙烯、液晶聚合物、石英以及玻璃所组成的群组的至少一者。
11.一种积层版，其特征在于，所述积层版包括：
一树脂基板，其包括多个如权利要求1所述的预浸物固化所制成；以及
至少一金属箔层，其设置于所述树脂基板的至少一表面上。
12.一种印刷电路板，其特征在于，所述印刷电路板是将如权利要求11所述的积层板的所述金属箔层图案化而形成。
CN201911127763.1A 2019-11-18 2019-11-18 预浸物、积层板以及印刷电路板 Pending CN110724366A (zh)

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TWI675063B (zh) * 2018-01-02 2019-10-21 聯茂電子股份有限公司 無鹵環氧樹脂組成物、積層板以及印刷電路板

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