CN118126481A - 无卤素的阻燃丙烯酸类聚合物 - Google Patents
无卤素的阻燃丙烯酸类聚合物 Download PDFInfo
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- CN118126481A CN118126481A CN202311609922.8A CN202311609922A CN118126481A CN 118126481 A CN118126481 A CN 118126481A CN 202311609922 A CN202311609922 A CN 202311609922A CN 118126481 A CN118126481 A CN 118126481A
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- RNFJDJUURJAICM-UHFFFAOYSA-N 2,2,4,4,6,6-hexaphenoxy-1,3,5-triaza-2$l^{5},4$l^{5},6$l^{5}-triphosphacyclohexa-1,3,5-triene Chemical compound N=1P(OC=2C=CC=CC=2)(OC=2C=CC=CC=2)=NP(OC=2C=CC=CC=2)(OC=2C=CC=CC=2)=NP=1(OC=1C=CC=CC=1)OC1=CC=CC=C1 RNFJDJUURJAICM-UHFFFAOYSA-N 0.000 claims abstract description 70
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- 125000001997 phenyl group Chemical group [H]C1=C([H])C([H])=C(*)C([H])=C1[H] 0.000 claims description 2
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Abstract
本发明涉及无卤素的阻燃丙烯酸类聚合物。本发明涉及阻燃(甲基)丙烯酸酯组合物,其合并抗冲击(甲基)丙烯酸类聚合物(例如来自Trinseo的
Description
技术领域
本发明涉及阻燃(甲基)丙烯酸酯组合物,其合并(甲基)丙烯酸类聚合物与含有至少一种有机次膦酸盐和至少一种膦酸酯的协同阻燃共混物。所述(甲基)丙烯酸酯组合物可用作多层聚合物复合材料中的阻燃帽层(cap layer)。
背景技术
(甲基)丙烯酸类聚合物(PMMA),例如Trinseo 树脂,已广泛用作许多不同基材材料(例如ABS、PVC、HIPS)上的帽层,以在许多应用中,包括在盖板、窗型材和汽车内饰和外饰中改善耐候性、耐刮擦性和耐划伤性(mar resistance)、和美观性。
然而,PMMA是可燃的,限制了其在其中需要阻燃性的应用中的用途。在电气、建筑和施工以及汽车领域、电动车辆EV充电站和浴器壁覆盖物中对于具有好的可加工性和机械性质的阻燃(甲基)丙烯酸帽层存在增长的需求。
用于热塑性塑料中的阻燃化合物是公知的。这些中的大多数涉及碘和/或溴化合物,例如脂族溴化合物和芳族溴化合物,如在US 2012-0184638中所描述的苯乙烯树脂,或基于锑的化合物。对于这些阻燃剂而言的问题是,它们倾向于具有毒性问题,并且在使用5-30重量%的推荐使用水平的情况下,这些阻燃剂不利地影响聚合物的物理性质(例如拉伸强度)。
用于热塑性塑料中的非卤化阻燃剂也是已知的,例如膦酸衍生物(WO2018/137883)、具有受阻胺的有机含磷化合物(EP3002311)和二烷基次膦酸盐(EP 1544206)。在这些参考文献中未将丙烯酸酯类描述为热塑性塑料。
EP1777257B1描述了次膦酸盐阻燃剂在(甲基)丙烯酸类聚合物中的用途,其中对于3.2mm厚度的样品获得UL-94V-1评级。该参考文献描述了阻燃(甲基)丙烯酸酯作为在丙烯腈-丁二烯-苯乙烯(ABS)上共挤出的顶层的用途。多层片材的总厚度为3mm,其具有0.3mm的阻燃(甲基)丙烯酸酯层厚度。所获得的多层片材的阻燃性能与基材材料相似。
增加阻燃剂的水平可以改善(甲基)丙烯酸热塑性塑料的阻燃性。然而,增加阻燃剂的水平倾向于不利地影响热塑性塑料的物理性质和机械性质,其包括熔体流动降低、断裂伸长率降低和黄度增加。
存在对于改善丙烯酸面料(capstock)中的阻燃性而不对(甲基)丙烯酸类聚合物的物理性质产生不利影响,并且不使用卤素或其它有毒添加剂的需要。
现在已令人意外地发现,有机次膦酸盐与低水平的膦酸酯化合物的共混物在PMMA中提供了协同效应,其中可以实现改善的阻燃性、可流动性和降低的黄度指数。在一个实施例中,配制物在1/8”厚度通过了UL94 V-0测试并在1/16”厚度通过了UL94 V-1测试。在PC/ABS基材上的新型阻燃PMMA组合物的共挤出片材通过了UL-94V-0测试。在一个实施例中,向PMMA组合物中的有机次膦酸盐中加入2%的膦酸酯意想不到地提供了等于额外4%的次膦酸盐的阻燃剂增加,而未损害物理性质和机械性质。
本发明提供了阻燃PMMA,其可以在热塑性基材上共挤出,以制备具有优异的阻燃性能(无卤化的阻燃剂)、抗冲击性、可流动性和耐候性的多层结构。所获得的多层结构可以进一步热成型为有用的型材和结构,例如EV充电站和洗车站的外部壳体、浴器壁覆盖物、汽车应用、卫生、航空航天以及建筑和施工应用。
发明内容
本发明的(甲基)丙烯酸阻燃组合物是一种或多种(甲基)丙烯酸类聚合物(PMMA)、一种或多种有机次膦酸盐、一种或多种膦酸酯、以及任选的其它添加剂的共混物。
(甲基)丙烯酸类聚合物
如本文所用,(甲基)丙烯酸类聚合物包括但不限于,包含(甲基)丙烯酸烷基酯类的均聚物、共聚物和三元共聚物(指多于两种不同的单体单元)。也考虑两种或更多种不同的(甲基)丙烯酸类聚合物的共混物。
甲基丙烯酸烷基酯单体优选是甲基丙烯酸甲酯,其占单体混合物的60至100%。0至40%的其它丙烯酸酯、甲基丙烯酸酯和/或其它乙烯基单体也可存在于该单体混合物中。共聚单体通常占(甲基)丙烯酸酯共聚物的0.5至40重量%,优选0.5至30重量%,并且优选2至20重量%。可用于单体混合物的其它甲基丙烯酸酯、丙烯酸酯和其它乙烯基单体包括但不限于丙烯酸甲酯、丙烯酸乙酯和甲基丙烯酸乙酯、丙烯酸丁酯和甲基丙烯酸丁酯、甲基丙烯酸异辛酯和丙烯酸异辛酯、丙烯酸乙基己酯和甲基丙烯酸乙基己酯、丙烯酸月桂酯和甲基丙烯酸月桂酯、丙烯酸硬脂酯和甲基丙烯酸硬脂酯、丙烯酸异冰片酯和甲基丙烯酸异冰片酯、丙烯酸甲氧基乙酯和甲基丙烯酸甲氧基乙酯、丙烯酸2-乙氧基乙酯和甲基丙烯酸2-乙氧基乙酯、丙烯酸二甲基氨基乙酯和甲基丙烯酸二甲基氨基乙酯单体、苯乙烯及其衍生物。烷基(甲基)丙烯酸例如(甲基)丙烯酸和丙烯酸可用于单体混合物。也可使用低水平的多官能单体作为交联剂。优选的丙烯酸类聚合物是甲基丙烯酸甲酯和2-16%的一种或多种C1-C4丙烯酸酯类的共聚物。
(甲基)丙烯酸类聚合物可以是抗冲改性的。可用于本发明中的常见抗冲改性剂包括但不限于嵌段共聚物和核-壳抗冲改性剂。核-壳抗冲改性剂可以具有软-硬形态、硬核-软-硬形态或类似的其它形态。对于许多户外应用而言,非抗冲(甲基)丙烯酸类聚合物可对于使用而言过脆,并且抗冲改性的(甲基)丙烯酸将是优选的。
本发明的(甲基)丙烯酸类聚合物或抗冲改性的(甲基)丙烯酸类聚合物在230℃/3.8kg测试时的熔体流动速率(MFR)优选大于0.6g/10min,优选大于0.8g/10min,并且更优选大于1g/10min。本发明的(甲基)丙烯酸类聚合物或抗冲改性的(甲基)丙烯酸类聚合物进一步具有在10N下测试时优选大于90℃,优选大于95℃,并且更优选大于100℃的维卡温度,和在50N测试时大于85℃,优选大于90℃,并且更优选大于95℃的维卡温度。本发明的(甲基)丙烯酸类聚合物或抗冲改性的(甲基)丙烯酸类聚合物的Tg优选大于90℃,优选大于95℃,并且更优选大于102℃。
阻燃剂
本发明需要至少一种有机次膦酸盐阻燃剂和至少一种膦酸酯阻燃剂的阻燃共混物。
所述有机次膦酸盐阻燃剂具有下式的化合物:
其中:
R1和R2表示直链或支化C1-C6烷基和/或芳基。R1和R2可以相同或不同;
R3为直链或支化C1-C10亚烷基、C6-C10亚芳基、烷基亚芳基或芳基亚烷基;
M代表Mg、Ca、Al、Sb、Sn、Ge、Ti、Zn、Fe、Ze、Ce、Bi、Sr、Mn、Li、Na或K;
m是1至4的整数;
n是1至4的整数;
x是1至4的整数;
也可使用具有式[I]和/或[II]的两种或更多种不同的阻燃剂。
R1和R2优选为烷基,包括但不限于甲基、乙基、正丙基、正丁基、叔丁基、正戊基和/或苯基。
R3优选为亚甲基、亚乙基、正亚丙基、异亚丙基、正亚丁基、叔亚丁基、正亚戊基、正亚辛基或正亚十二烷基。它还可以是亚苯基、甲基亚苯基、乙基亚苯基、叔丁基亚苯基、甲基亚萘基、戊基亚乙基、苯基亚丙基或萘(naphalene)。
有利地,M表示Ca、Al或Zn,且优选M表示Al。
优选地,式(I)的有机次膦酸盐阻燃剂是其中M表示Al,且R1和R2二者都独立地表示C1-C6烷基的那种。优选R1和R2二者都是乙基,或乙基和甲基,如式[III]和[IV]中所示。
次膦酸盐阻燃剂中磷的重量%优选大于16%,更优选大于18%,更优选大于20%,并且最优选大于22%。
优选地,有机次膦酸盐阻燃剂具有0.5至10微米,有利地在1至5微米的重均粒度分布D50(其通过激光衍射在丙酮中测量)。该粒度范围提供了在(甲基)丙烯酸类聚合物中的好的分散。
有机次膦酸盐阻燃剂以20至45重量份,有利地25至45重量份,更有利地25至36重量份,并且优选29至32重量份存在于PMMA组合物中,基于(甲基)丙烯酸类聚合物基质的100份计。
本发明中所用的膦酸酯具有通式:
其中:
R1和R2相同或不同,并且选自直链或支化的C1-C4烷基。R1和R2可以相同或不同;
R3选自直链或支化的C1-C4烷基、亚烷基、烷基亚芳基或芳基亚烷基。
更短链R1、R2和R3倾向于提供更好的阻燃性,因为膦酸酯中磷的重量%更高。特别优选甲基和乙基。
膦酸酯的重量%磷含量优选大于16%,优选大于18%,更优选大于20%,并且最优选大于22%。
膦酸酯阻燃剂以0.1至17重量份,有利地0.2至12重量份存在于PMMA组合物中,基于(甲基)丙烯酸类聚合物基质的100份计。
在一个优选的实施方案中,膦酸酯具有式[VI],其具有约24重量%的磷含量。
膦酸酯可以是粒状或粉末状形式。它以0.1至10重量%,优选0.5至5重量%,并且更优选0.5至3重量%用于PMMA组合物中,基于组合物的总重量计。
在PMMA组合物中,膦酸酯与有机次膦酸盐的重量比为1:100至1:2,优选1:48至1:8。
任选地,其它非卤化的阻燃剂可以以总PMMA组合物的0至5重量%,并且优选0.1至3重量%的低水平存在。有用的其它阻燃剂包括但不限于选自以下的一种或多种化合物:
-单体或聚合物N-烷氧基受阻胺,包括但不限于NOR116(CAS#191680-81-6),
-三嗪衍生物,
-其它磷化合物例如有机磷酸酯和膦氧化物,
-硅化合物,包括但不限于硅酸盐、沸石、二氧化硅、硅氧烷,
-镁化合物,包括但不限于氢氧化镁、碳酸镁、镁氧化物、水滑石(hydrotalcite)、二水滑石(dihydrotalcite),
-钙化合物,包括但不限于氢氧化钙、钙氧化物、碳酸钙,
-锌化合物,包括但不限于锌氧化物、氢氧化锌、水合氧化锌,
-铝化合物,包括但不限于铝氧化物、氢氧化铝、磷酸铝,
-钛化合物,包括但不限于钛氧化物,
-锑化合物,包括但不限于三氧化锑、四氧化锑、酒石酸锑,和
-非卤化聚合物,包括但不限于聚碳酸酯和聚偏二氟乙烯。
优化在(甲基)丙烯酸组合物中使用的阻燃剂和添加剂的水平以平衡所需阻燃性的水平,却使阻燃剂的量最小化,以减少组合物的物理性质和机械性质的降解。本发明的组合物令人意外地允许了在阻燃性上的提高,而无物理性质和机械性质的典型损失。
其它添加剂
本发明的(甲基)丙烯酸类聚合物组合物可以任选在一个或多个层中包含用于以通常有效量使用的聚合物组合物的一种或多种的典型添加剂,包括但不限于加工助剂例如硬脂酸锌、硬脂醇和硬脂酸,稳定剂,增塑剂,填料,着色剂,颜料,抗氧化剂,抗静电剂,表面活性剂,调色剂,折射率匹配添加剂,具有特定光衍射、光吸收或光反射特性的添加剂,分散助剂,辐射稳定剂,羧酸例如乳酸、草酸和乙酸,以及光改性添加剂例如具有0.5微米至1,000微米的粒度的聚合物或无机球形颗粒。
本发明的阻燃(甲基)丙烯酸组合物可以通过本领域中已知的方式共混,例如在双螺杆挤出机中。
如表1-5中所示,本发明的阻燃(甲基)丙烯酸组合物提供了改善的可流动性(MFR提高)、改善的可燃性和降低的黄度。
阻燃(甲基)丙烯酸类聚合物基质,无论是否进行了抗冲改性,当在230℃/3.8kg测试时,都具有大于0.4g/10min,优选大于0.8g/10min,并且更优选大于1g/10min的熔体流动速率(MFR)。所述聚合物基质,无论是否经过抗冲改性,进一步具有在10N下测试时大于90℃,优选大于95℃,并且更优选大于100℃的维卡温度,和在50N下测试时大于85℃,优选大于90℃,并且更优选大于95℃的维卡温度。阻燃(甲基)丙烯酸类聚合物的Tg优选大于90℃,优选大于95℃,并且更优选大于100℃。
热塑性阻燃(甲基)丙烯酸组合物可以通过典型方式,例如但不限于挤出成型和注射成型,而转化为有用的物体、型材和片材。组合物的有用的物体包括用于电气装置、型材、汽车部件和可热成型片材的覆盖物。
多层复合材料
本发明的阻燃(甲基)丙烯酸组合物也可以应用于热塑性聚合物,改善多层复合材料对环境因素的耐性,例如提供耐刮擦性和耐划伤性以及耐UV性。
本发明的阻燃(甲基)丙烯酸类聚合物组合物可用作热塑性基材上的帽层。帽层通常比结构塑料薄得多,通常为包含面料和结构塑料层的多层结构的总厚度的约5至25%。例如,面料的厚度可为约0.05至约3mm,优选0.1至1mm,而结构热塑性层的厚度可为约0.5至约20mm,且优选1至10mm。
用于多层复合材料的有用热塑性基材包括但不限于饱和聚酯(聚对苯二甲酸乙二醇酯、聚对苯二甲酸丁二醇酯)、丙烯腈/丁二烯/苯乙烯(ABS)、苯乙烯/丙烯腈共聚物、丙烯酸/苯乙烯/丙烯腈(ASA)共聚物、聚苯乙烯(PS)、聚碳酸酯(PC)、聚环氧丙烷(PPO)、聚砜、聚氯乙烯(PVC)、氯化聚氯乙烯(CPVC)、膨胀PVC、聚丙烯、聚乙烯、高抗冲聚苯乙烯(HIPS)。热塑性基材也可以是两种或更多种热塑性塑料(例如但不限于PPO/PS、PC/ABS)的混合物或合金。
在优选的实施方案中,基材层是PC/ABS。发现PC/ABS可以提供比单独的ABS更高的耐热性,以及更好的机械性质、增加的韧性、强度和尺寸稳定性。
阻燃(甲基)丙烯酸组合物和热塑性基材组合物可通过本领域中已知的方式,例如但不限于共挤出(或多次挤出)成型、热压缩成型、多次注射成型,而合并为多层结构片材或型材。
任选地,可以在(甲基)丙烯酸层和热塑性基材之间施加结系层(tie layer),例如以改善层的粘附。中间层比热塑性基材薄,通常为10至700微米。
用途
本发明的多层复合材料可用于通过共挤出生产可热成型的片材。所述片材可以热成型为有用的物体,包括但不限于电动车辆(EV)充电站壳体、洗车站、汽车应用、汽车装饰、航空航天应用以及建筑和施工应用,例如浴室墙壁覆盖物和淋浴间。
具体实施方式
实施例
材料:
HFI-10:由Trinseo市售的抗冲改性PMMA(包含多层颗粒型抗冲改性剂),其具有1.0ft-lb/in的切口悬梁臂冲击和在230℃/3.8kg的3.3g/10min的熔体流动速率(MFR)。维卡温度为在10N下101.1℃和在50N下92.9℃。
DR-101:由Trinseo市售的抗冲改性PMMA(包含多层颗粒型抗冲改性剂),其具有1.1ft-lb/in的切口悬梁臂冲击和在230℃/3.8kg的1.0g/10min的熔体流动速率(MFR)。维卡温度为在10N下105.1℃和在50N下97.2℃。
OP935:由Clariant市售的二乙基次膦酸铝。磷含量为约24重量%。密度为1.35g/cm3。粒度D50为约2微米。
PCO900:由Thor市售的有机磷阻燃剂。磷含量为约24重量%。
PCO960:由Thor市售的有机磷阻燃剂。磷含量为约24重量%。PCO960是PCO900的非微粉化版本。
硬脂酸锌:CAS号557-05-1。由Sigma-Aldrich市售。
116:CAS号191680-81-6。FlameStab 116是由BASF市售的三嗪衍生物。它是单体N-烷氧基受阻胺,其具有108-123℃的熔化范围和1.06g/cm3的比重。
126:由BASF市售的有机亚磷酸酯。CAS号26741-53-7。磷含量10.3重量%。
168:由BASF市售的有机亚磷酸酯。CAS号31570-04-4。磷含量4.8重量%。
7740:UL-94V-0评级的阻燃剂PC/ABS不含卤化的阻燃剂。MFR在230℃/3.8kg为4.5g/10min。
测试方法
MFR:阻燃丙烯酸类聚合物的熔体流动速率在230℃在3.8kg的负载下测量。(ASTMD1238-20)
切口悬梁臂:使用Instron Ceast Resil Impactor在室温下进行切口悬梁臂测试。(ASTM D256-10(2018))。“C”表示完全断裂。
拉伸性质(拉伸强度、断裂伸长率和拉伸模量):拉伸测试使用Instron工作站进行。十字头速度:0.2”/min。(ASTM D638)
在10N(和50N)下维卡温度:使用Instron HV6M工作站测量维卡软化温度。(ASTMD1525-17e1)。在测试前,将样品在80℃退火过夜,然后冷却至室温。
弯曲应力/弯曲模量:使用Instron 4201工作站进行测试。测试速度0.054in/min。(ASTM D790-17)
燃烧:根据UL94标准(第6版,2013年3月28日,2022年4月1日ANSI批准)在ATLASHUVL水平/垂直燃烧室中进行阻燃性测试。V-0、V-1和V-2标准描述于下表中。NR(无评级)指示阻燃性能比V-2差。
落镖:用BYK 5513Gardner Impact Tester进行测试。(ASTM D4226-19e1)
YI-E313:通过来自X-Rite的台式分光光度计来测量黄度指数。型号颜色i7。(ASTME313-20)
实施例1:配制物和性质:
使用27mm双螺杆挤出机混合和配混下表1中所列出的配制物。用Demag注射成型机在360°F至445°F制备测试试样。对样品进行测试,其中所得的性质在下表1中示出:
表1
实施例说明:
1)比较实施例A、B和C,或D、E和F,使用相同的负载PCO960(0%或2%),/>OP935负载越高,则MFR和切口悬梁臂冲击越低,并且燃烧性能越好并且黄度指数越高。
2)比较实施例A和D,或B和E,或C和F,使用相同的OP935的负载,PCO960的添加导致更好的可流动性(更高的MFR)、更好的燃烧性能和更低的黄色指数。
3)比较实施例D与B,或E与C,当4%OP935被2%/>PCO960代替时,燃烧性能保持相同或改善(在1/16”厚度实施例C vs E),并且可流动性和黄度显著改善(高得多的MFR和较低的黄度指数)。
实施例2:配制物和性质:
使用27mm双螺杆挤出机混合和配混下表2中所列出的配制物。用Demag注射成型机在360°F至445°F制备测试试样。对样品进行测试,其中所得的性质在下表2中示出:
表2
实施例说明:
1)比较实施例G和H,添加0.5%PCO900改善了可流动性并降低了黄度(更高的MFR和更低的黄度指数)。燃烧性能未显著地改善。
2)然而,通过向配制物H添加额外的1%硬脂酸锌,在1/8”厚度,燃烧性能从V-1改善至V-0。同时,MFR进一步提高,且黄度指数降低。这证明硬脂酸锌可以与PCO900和/>OP935组合使用以增强可流动性和燃烧性能并降低黄度指数。
与配制物I相比,使用额外的0.25%116,MFR进一步提高。然而,燃烧性能保持相同,且黄度指数快速提高。
实施例3:配制物和性质:
使用27mm双螺杆挤出机混合和配混下表3中所列出的配制物。HFI-10(商业级)和/>DR101(商业级)来自Trinseo Altuglas。用Demag注射成型机在360°F至445°F制备测试试样。对样品进行测试,其中所得的性质在下表3中示出:
表3
实施例说明:
1)比较实施例K和L,当向在DR101PMMA基质中含有24%/>OP935的配制物中添加2%PCO900时,MFR从0.4提高至0.9g/10min,这意味着可加工性得到了显著改善。此外,UL94垂直燃烧测试结果在1/16”厚度从NR增加至V-1。
2)比较使用相同阻燃剂负载的实施例K和F(表1)或L和C(表1),当将基质PMMA从HFI-10切换到DR101时,维卡温度提高约5℃,并且Tg提高约4℃。这是由于与HFI-10相比,/>DR101的高热稳定性。
3)所有这些改善使得实施例K为可加工的高耐热性阻燃PMMA,其具有在1/8”厚度的V-0评级和在1/16”厚度的V-1评级。
实施例4:配制物和性质:
使用27mm双螺杆挤出机混合和配混下表4中所列出的配制物。用Demag注射成型机在360°F至445°F制备测试试样。对样品进行测试,其中所得的性质在下表4中示出:
表4
实施例说明:
比较实施例M和N或O,使用相同的OP935的负载,通用亚磷酸酯例如126和/>168并未像/>PCO900那般改善化合物的MFR和燃烧性能。这可能是由于/>PCO900的独特化学结构和高磷含量。
实施例5:配制物和性质,多层复合材料:
使用三个挤出机(两个用于阻燃PMMA,和一个用于PC/ABS)和三歧管模头在PC/ABS上共挤出FR PMMA,以制备多层片材样品。来自每个挤出机的挤出物在模头处铺展然后合并,并以通过具有三个辊的冷却站来最终完成。精细调节每个挤出机的挤出速率,以使获得的多层片材满足所需的层厚度(对于PMMA或阻燃PMMA层而言为0.6mm,和对于PC/ABS层而言为2.4mm)。然后切割这些片材样品以制造用于测试的试样。
表5
实施例说明:
实施例Q证明共挤出的具有PC/ABS的阻燃PMMA是成功的(该配制物可加工)。与实施例P(具有非阻燃PMMA帽层的相同PC/ABS)相比,片材的阻燃性能从NR改善至V-0。同时,弯曲性和冲击抗性仅略微降低,因此其仍适合用于热成型并用于EV充电站壳体、浴室墙壁覆盖物等。
Claims (21)
1.一种阻燃(甲基)丙烯酸类聚合物组合物,其每100重量份的(甲基)丙烯酸类聚合物包含:
a.20至45重量份的式[I]或[II]的一种或多种有机次膦酸盐阻燃剂:
其中:
R1和R2表示直链或支化的C1-6烷基和/或芳基,并且其中R1和R2可以相同或不同;
R3为直链或支化的C1-C10亚烷基、C6-C10亚芳基、烷基亚芳基或芳基亚烷基;
M代表Mg、Ca、Al、Sb、Sn、Ge、Ti、Zn、Fe、Ze、Ce、Bi、Sr、Mn、Li、Na或K;
m是1至4的整数;
n是1至4的整数;
x是1至4的整数;
b.0.1至17重量份的具有式[V]的一种或多种膦酸酯阻燃剂:
其中:
R1和R2相同或不同,并且选自直链或支化的C1-C6烷基,并且其中R1和R2可以相同或不同;
R3选自直链或支化的C1-C10烷基、亚烷基、C6-C10亚芳基、烷基亚芳基或芳基亚烷基。
并且其中所述(甲基)丙烯酸类聚合物包含至少60重量%的甲基丙烯酸甲酯单体单元。
2.根据权利要求1所述的阻燃(甲基)丙烯酸类聚合物组合物,其中式[I]和/或式[II]的所述有机次膦酸盐阻燃剂的R1和R2独立选自甲基、乙基、正丙基、正丁基、叔丁基、正戊基和苯基。
3.根据权利要求1所述的阻燃(甲基)丙烯酸类聚合物组合物,其中在式[I]的所述有机次膦酸盐阻燃剂中,R1为乙基且R2为甲基或乙基,M为Al,并且所述阻燃剂具有式[III]或[IV]的化合物:
4.根据权利要求1所述的阻燃(甲基)丙烯酸类聚合物组合物,其中所述有机次膦酸盐阻燃剂具有0.5至10微米的重均粒径(D50)。
5.根据权利要求1所述的阻燃(甲基)丙烯酸类聚合物组合物,其中所述膦酸酯具有式[VI]
6.根据权利要求1所述的阻燃(甲基)丙烯酸类聚合物组合物,其中PMMA组合物中的膦酸酯与有机次膦酸盐的重量比在1:100至1:2。
7.根据权利要求1所述的阻燃(甲基)丙烯酸类聚合物组合物,其中所述(甲基)丙烯酸类聚合物进一步包含抗冲改性剂。
8.根据权利要求1所述的阻燃(甲基)丙烯酸类聚合物组合物,其中当在230℃/3.8kg下测试时,所述(甲基)丙烯酸类聚合物的熔体流动速率(MFR)大于0.6g/10min。
9.根据权利要求1所述的阻燃(甲基)丙烯酸类聚合物组合物,其中当在10N下测试时,所述(甲基)丙烯酸类聚合物的维卡温度大于90℃,和当在50N下测试时,所述(甲基)丙烯酸类聚合物的维卡温度大于85℃。
10.根据根据权利要求1所述的阻燃(甲基)丙烯酸类聚合物组合物,其中所述组合物进一步包含另外的阻燃剂和添加剂,所述阻燃剂和添加剂选自NOR 116、硬脂酸锌、硬脂醇和硬脂酸。
11.根据权利要求1所述的阻燃(甲基)丙烯酸类聚合物组合物,其中所述组合物在1/8英寸厚度样品上以V-0评级通过了UL94测试。
12.根据权利要求1所述的阻燃(甲基)丙烯酸类聚合物组合物,其中所述组合物在1/16英寸厚度样品上以V-1评级通过了UL94测试。
13.根据权利要求1所述的阻燃(甲基)丙烯酸类聚合物组合物,其中所述组合物是物体、型材或片材的形式。
14.根据权利要求13所述的阻燃(甲基)丙烯酸类聚合物组合物,其中物体、型材或片材通过挤出成型或注射成型而形成。
15.一种多层聚合物复合材料,其包括:
a.至少一层的权利要求1所述的阻燃(甲基)丙烯酸类聚合物组合物,
b.至少一层的热塑性塑料,其选自:饱和聚酯、聚对苯二甲酸乙二醇酯、聚对苯二甲酸丁二醇酯、丙烯腈/丁二烯/苯乙烯(ABS)、苯乙烯/丙烯腈共聚物、丙烯酸/苯乙烯/丙烯腈(ASA)共聚物、聚苯乙烯(PS)、聚碳酸酯(PC)、聚环氧丙烷(PPO)、聚砜、聚氯乙烯(PVC)、氯化聚氯乙烯(CPVC)、膨胀PVC、聚乙烯、聚丙烯、高抗冲聚苯乙烯(HIPS)、及其共混物,
其中暴露于环境的层包含层a)阻燃(甲基)丙烯酸类聚合物组合物。
16.根据权利要求15所述的多层聚合物复合材料,其中所述热塑性塑料是PC/ABS共混物。
17.根据权利要求15所述的多层聚合物复合材料,其中所述阻燃(甲基)丙烯酸类聚合物组合物层具有0.05至3.0mm的厚度,和所述热塑性层具有0.5至20mm的厚度。
18.根据权利要求15所述的多层聚合物复合材料,其中所述复合材料进一步包括在所述阻燃(甲基)丙烯酸类聚合物组合物层和所述热塑性层之间的中间结系层(tielayer)。
19.根据权利要求15所述的多层聚合物复合材料,其中所述复合材料通过包括以下各项的方法而形成:共挤出(或多次挤出)成型、热压缩成型或多次注射成型。
20.根据权利要求15所述的多层聚合物复合材料,其中所述复合材料在具有0.6mm的阻燃(甲基)丙烯酸类聚合物层厚度的3mm的总厚度通过UL94 V-0测试。
21.根据权利要求15所述的多层聚合物复合材料,其中所述多层复合材料是电动车辆(EV)充电站、洗车站、汽车应用、汽车装饰、航空航天应用、建筑和施工应用、浴室墙壁覆盖物、浴缸或淋浴间的一部分。
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