CN102361938A - 具有改善的光学性能的(共)聚碳酸酯 - Google Patents
具有改善的光学性能的(共)聚碳酸酯 Download PDFInfo
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- CN102361938A CN102361938A CN2010800133770A CN201080013377A CN102361938A CN 102361938 A CN102361938 A CN 102361938A CN 2010800133770 A CN2010800133770 A CN 2010800133770A CN 201080013377 A CN201080013377 A CN 201080013377A CN 102361938 A CN102361938 A CN 102361938A
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Abstract
本发明涉及(共)聚碳酸酯组合物和成型物料,其特征在于更好的光学性能、良好的可流动性和高热变形稳定性。
Description
本发明涉及(共)聚碳酸酯组合物和成型物料,其特征在于改善的光学性能,良好的可流动性和高热变形稳定性。
(共)聚碳酸酯属于工业热塑性塑料。它们已被应用于电气和电子领域的各种各样应用中,作为灯罩材料;并应用于不仅要求特定的热和力学性能而且要求优良光学性能的应用中,如热风机,汽车领域应用,塑料盖板、漫射板和光导元件,以及灯罩,或灯镶框(Lampeneinfassung(bezel))。
所述应用实际上总是强制性要求好的热和力学性能,如维卡温度(Vikat-Temperatur) (热变形稳定性)和玻璃化转变温度。同时优异的光学性能特别重要。为了实现热变形稳定性,动用了特定的双酚。以该方式不能实现光学性能的同时改进。
已经知道,聚丙烯酸酯和(共)聚碳酸酯在共混物中不相容。这一点,从雾度增加直至不透明而表现出来。对于热和力学性能也有不利作用。
因此本发明的目的是研发具有改进光学性能而不改变核心性能,尤其力学和热性能,的芳族(共)聚碳酸酯。
已意外地发现,包含(共)聚碳酸酯和含特定丙烯酸酯结构的聚合物的组合物导致改进的光学性能。实现光学性能的有针对性提高及其调节的这种措施和对混入的聚合物的依赖性是迄今未知的。
本发明提供由以下组分组成的混合物:
A)99.98~99.5重量份,优选99.9~99.7重量份(基于组分A+B之和)分子量M(重均)为至少10 000 g·mol-1,优选20 000 g·mol-1~300 000 g·mol-1的高分子量热塑性芳族(共)聚碳酸酯,它包含式(Ⅰ)的结构单元
其中
R1和R2是氢、C1~C4-烷基,优选甲基,
k是0、1、2、3或4,优选2或3,
B)0.02~0.5重量份,优选0.1~0.3重量份(基于组分A+B之和)一种或多种包含至少一个通式(Ⅱ)或(Ⅲ)的结构单元的聚丙烯酸酯:
其中,
R3是C1~C8-烷基,优选甲基,
R4是C1~C6-烷基,优选甲基,
R5是氢、C1~C8-烷基,优选氢和甲基,和
R6是氢、C1~C4-烷基,优选甲基,
m和n是由分子量确定的整数
以及结构(Ⅱ)与(Ⅲ)的摩尔比为0 mol%~100 mol%,基于(Ⅱ)和(Ⅲ)的总摩尔数,而且结构(Ⅱ)和(Ⅲ)的总量为100 mol%,
其中,本申请中所有的重量份数据都已标准化到使组合物中组分A+B的总重量份为100。
任选地可以存在其它添加剂,如UV吸收剂、脱模助剂或热稳定剂,用量各为50~5000重量ppm,基于组分A+B之和。
由本发明的(共)聚碳酸酯和(共)聚碳酸酯组合物生产的注塑制品或挤出物具有显著改善的光学性能(黄度指数),而同时还具有几乎未改变的力学、热学和流变性能。这是对于注塑和挤出部件的光学、力学和热学行为的重要判据。
为本发明的目的,热塑性芳族(共)聚碳酸酯是均聚碳酸酯或由不同二酚单元组成的共聚碳酸酯,这里,本申请中的术语(共)聚碳酸酯也包括由式(Ⅴ)的二酚单元组成的均聚碳酸酯。
适用于本发明的芳族(共)聚碳酸酯是从文献中已知的或能用从文献得知方法生产(关于芳族(共)聚碳酸酯的制备参见,例如,Schnell,“Chemistry and Physics of Polycarbonates(聚碳酸酯的化学与物理)”,Interscience出版社,1964以及DE-AS 1 495 626、DE-A 2 232 877、DE-A
2 703 376、DE-A 2 714 544、DE-A 3 000 610、DE-A
3 832 396)。
芳族(共)聚碳酸酯制备如下:根据相界面法,由,例如,二酚与碳酰卤,优选光气,反应而成,任选地,使用链终止剂,例如,一元酚,和任选地,使用三官能度或大于三官能度的支化剂,例如,三酚和四酚。同样可能的是经由熔体聚合法,由二酚与,例如,碳酸二苯酯反应而成。
适用于生产(共)聚碳酸酯的除式(Ⅴ)二酚
在其中,
R1和R2是氢、C1~C4烷基,优选甲基,
k是0,1,2,3或4,优选2或3,
以外的二羟基芳基化合物是式(Ⅵ)的那些化合物
其中,
A 是单键、C1~C5-亚烷基、C2~C5-烷叉基、C5~C6-环烷叉基、-O-、-SO-、-CO-、-S-、-SO2-、还能稠合任选地含杂原子的芳环的C6~C12-亚芳基
或式(Ⅶ)或(Ⅷ)的基团
B 在每一情况下是氢;C1~C12-烷基,优选甲基;卤素,优选氯和/或溴,
q 彼此独立地代表0,1或2,
p 是1或0,和
R7和R8 可独立地为每个X1选择,而且彼此独立地是氢或C1~C6-烷基,优选氢、甲基或乙基,
X1 是碳,和
r 是4~7的整数,优选4或5,条件是,在至少一个原子X1上,R7和R8同时是烷基。
优选用1,1-双(4-羟苯基)-3,3,5-三甲基环己烷(双酚TMC)作为衍生自式(Ⅴ)的二酚来生产本发明的(共)聚碳酸酯。
适用于生产本发明中所用(共)聚碳酸酯的式(Ⅵ)的二酚的实例是氢醌、间苯二酚、双(羟苯基)烷、双(羟苯基)硫醚、双(羟苯基)醚、双(羟苯基)酮、双(羟苯基)砜、双(羟苯基)亚砜、α,α’-双(羟苯基)二异丙基苯,还有这些的烷基化、环上烷基化和环上卤代的化合物。
优选的其它二酚是4,4’-二羟基联苯、2,2-双(4-羟苯基)-1-苯基丙烷、1,1-双-(4-羟苯基)苯基乙烷、2,2-双(4-羟苯基)丙烷、2,2-双(3-甲基-4-羟苯基)丙烷、2,4-双(4-羟苯基)-2-甲基丁烷、1,3-双[2-(4-羟苯基)2-丙基]苯(双酚M)、2,2-双(3-甲基-4-羟苯基)丙烷、双(3,5-二甲基-4-羟苯基)甲烷、2,2-双(3,5-二甲基-4-羟苯基)丙烷、双(3,5-二甲基-4-羟苯基)砜、2,4-双(3,5-二甲基-4-羟苯基)-2-甲基丁烷、1,3-双[2-(3,5-二甲基-4-羟苯基)-2-丙基]苯。
特别优选的二酚是2,2-双(4-羟苯基)丙烷(BPA)和2,2-双(3-甲基-4-羟苯基)丙烷(二甲基BPA)。
尤其优选由双酚A和双酚TMC制成的(共)聚碳酸酯。
二酚能单独或以任何所需混合物的形式使用。二酚是从文献已知的或能用从文献得知的方法获得。
上述和其它适用二酚可商业获得,并已描述在,例如,“H.Schnell, Chemistry and Physics of
Polycarbonates(聚碳酸酯的化学和物理),Interscience出版社,New
York 1964,从第28页起; 从第102页起”和“D.G.Legrand,
J.T.Bendler, Handbook of Polycarbonate Science and Technology(聚碳酸酯科学与技术手册), Marcel Dekker New York 2000, 从第72页起”中。
特别优选包含如下结构单元(Ⅸ)和(Ⅹ)的无规(共)聚碳酸酯:
其中端基含下列结构(Ⅺ)和(Ⅻ)中至少之一:
其中
R9和R10彼此独立地是氢或C1~C6-烷基。结构(Ⅸ)或(Ⅹ)的摩尔比是0 mol%~100 mol%,优选1 mol%~99 mol%,特别优选2 mol%~98 mol%,非常特别优选3 mol%~97 mol%,基于(Ⅸ)和(Ⅹ)的总摩尔数。
非常特别优选其中R10是甲基的无规(共)聚碳酸酯。
适用于生产热塑性芳族(共)聚碳酸酯的链终止剂的实例是苯酚、对-叔丁基苯酚或枯基苯酚。
链终止剂的用量一般是0.5 mol%~10
mol%,基于在每一情况下所用二酚的总摩尔数。
热塑性芳族(共)聚碳酸酯能以已知方式,并具体地优选通过加入相对于二酚总用量为0.05~2.0 mol%的三官能或多于三官能的化合物,如带3或更多个酚属基团的化合物,而被支化。
在本发明的一个优选实施方案中,芳族(共)聚碳酸酯的重均分子量(Mw,用,例如,GPC、超离心或光散射法测定)大于10 000 g·mol-1,特别优选20
000 g·mol-1~300 000 g·mol-1。
热塑性芳族(共)聚碳酸酯能单独或以任何所需混合物,优选与其它芳族聚碳酸酯一起使用。
所用的二酚会因各二酚的合成、处理和储存所带来的污染物而被污染,对于加进合成的所有其它化学品和助剂也是这样。但是,合意的是用尽可能纯的原材料操作。
所用的具体聚丙烯酸酯可以是聚甲基丙烯酸甲酯或热变形稳定性的聚甲基丙烯酰亚胺,如聚(N-甲基甲基丙烯酰亚胺)(PMMI,也称做Pleximid; Röhm GmbH & Co KG, Darmstadt)或其混合物或共聚物。它们兼具高热变形稳定性和很好的透光率、很高的强度和刚度以及良好的耐侯性。
组合物可包含其它市售常规聚合物添加剂,如阻燃剂、阻燃增效剂、防滴剂(如来自下列物质类的化合物:氟化聚烯烃、硅酮和芳纶纤维)、润滑剂和脱模剂(如四硬脂酸季戊四醇酯)、成核剂、稳定剂、抗静电剂(如导电炭黑,碳纤维、碳纳米管、以及有机抗静电剂,如聚亚烷基醚、烷基磺酸盐或含聚酰胺的聚合物)以及染料和颜料,用量要使组合物力学性能的降低程度不致于不再符合所要求的性能范围(避免在-10℃脆性断裂失效)。
作为阻燃剂优选使用含磷阻燃剂,尤其选自下面各组:单-和寡聚磷酸酯和膦酸酯、膦酸酯胺和膦腈(Phosphazene),但这里也可以用选自其中一组或多组的多种组分的混合物作为阻燃剂。也可以用此处尚未具体提及的、优选不含卤素的磷化合物,单独或以与其它、优选不含卤素的磷化合物的任何所需组合使用。适用磷化合物的实例是:磷酸三丁酯、磷酸三苯酯、磷酸三甲苯酯、磷酸二苯基甲苯酯、磷酸二苯基辛酯、磷酸二苯基2-乙基甲苯酯、磷酸三(异丙基苯基)酯、间苯二酚桥连的二-或低聚磷酸酯以及双酚A桥连的二-或低聚磷酸酯。特别优选用衍生自双酚A的低聚磷酸酯。适合作阻燃剂的磷化合物是已知的(参考,例如,EP-A
0363 608,EP-A 0 640 655)或能用已知方法(例如,Ullmanns
Enzyklopädie der technischen Chemie,第18卷, 从第301页起1979; Houben-Weyl, Methoden der organischen Chemie, 第12/1卷, 第43页; Beilstein 第6卷, 第177页)类似地制造。
加入添加剂用以延长使用寿命或着色(稳定剂),简化加工(如脱模剂、流动助剂、抗静电剂),或为特定负荷类型适配聚合物的性能(冲击改性剂,如橡胶;阻燃剂、着色剂、玻璃纤维)。
所述添加剂可以在所谓配混步骤中,单独地或以任何所需混合物或以多种不同混合物,在聚合物分离期间直接地或在粒料熔化之后,加进聚合物熔体。这类添加剂或其混合物能以固体形式,即以粉末形式,或以熔体形式,加进聚合物熔体。其它计量类型是使用添加剂或添加剂混合物的母料或母料的混合物。
适用的添加剂已描述在,例如,“Additives for Plastics Handbood, John Murphy,
Elsevier, Oxford 1999”或“Plastics
Additives Handbook, Hans Zweifel, Hanser, Munich,2001”或WO 99/55772,第15~25页中。
作为热稳定剂合适的优选是亚磷酸三(2,4-二叔丁基苯基)酯(Irgafos 168)、[1,1-联苯基]-4,4’-二基双亚膦酸四(2,4-二叔丁基苯基)酯、磷酸三辛酯、3-(3,5-二叔丁基-4-羟苯基)丙酸十八烷基酯(Irganox 1076)、二亚磷酸双(2,4-二枯基苯基)季戊四醇酯(Doverphos S-9228-PC)、二亚磷酸双(2,6-二叔丁基-4-甲基苯基)季戊四醇酯(ADK STAB PEP-36)或三苯膦。它们单独或以混合物使用(例如,Irganox B900或Doverphos
S-9228-PC与Irganox B900或Irganox 1076)。
优选的适用脱模剂是四硬脂酸季戊四醇酯、一硬脂酸甘油酯、硬脂酸硬脂酯或一或二硬脂酸丙二醇酯。它们单独或以混合物使用。
优选的适用UV稳定剂是2-(2’-羟苯基)苯并三唑、2-羟基二苯甲酮、取代或未取代苯甲酸的酯、丙烯酸酯、空间受阻胺、草酰胺、2-(2-羟苯基)-1,3,5-三嗪,且特别优选取代的苯并三唑类,如Tinuvin
360、 Tinuvin 350、Tinuvin 234、Tinuvin
329或UV CGX 006(Ciba)。
还可加入着色剂,实例是有机染料或颜料,或无机颜料或IR吸收剂,单独地,以混合物,或以与稳定剂、与(空心)玻璃珠、或与无机填料的组合加入;其它实例是有机或无机散射颜料。
本发明的热塑性成型物料(Formmass)生产如下:用已知方式混合各组分,和在200℃~340℃,优选240℃~300℃的温度,在常规装置内,如在内捏和机、挤出机和双螺杆体系内,将它们熔体配混和熔体挤出。
各组分的混合能用已知方式相继或同时进行,具体地,在约20℃(室温)或更高温度下。
本发明还提供包含至少一个通式(Ⅱ)或(Ⅲ)的结构单元的聚丙烯酸酯在生产包含至少一个式(Ⅰ)二酚单元的(共)聚碳酸酯的方法中的应用,
其中
R1和R2是氢、C1~C4-烷基,
k是0、1、2、3或4
在其中,将所述一种或多种所述聚丙烯酸酯混入所述(共)聚碳酸酯中。
本发明还提供生产成型物料的方法,以及成型物料在生产成型体(Formkörper)中的应用。
本发明的成型物料可用来生产任何类型的成型体。成型体可以由,例如,注塑、挤出和吹塑工艺生产。另一类加工形式是用深拉法从预先制成的板材或薄膜生产成型体。
本发明的(共)聚碳酸酯和(共)聚碳酸酯组合物可以在常规机械中,例如,在挤出机或注塑机中,用常规方式加工,以形成任何所需的成型体或成型件,或形成薄膜和薄膜层压制件,或板材,或瓶子。
如此所得(共)聚碳酸酯可用来生产挤出物(板材、薄膜和它们的层合制件;例如,用于卡片应用和管道)和成型体(瓶子),尤其用于透明领域,特别在光学应用领域的挤出物,如板材、夹心板(Stegplatte)、窗玻璃、漫射板或防尘盖、灯罩、塑料防尘盖、光导元件,或光数据存贮器,如以仅可读或可单次写入、有时还可多次写入的多种实施方案的音频CD、CD-R(W)、DVD、DVD-R(W)、微型光盘,还有数据载体。它们也能用来生产电气/电子领域和IT领域的制品。
(共)聚碳酸酯组合物尤其适用于生产其中利用光学、热学和力学性能的复合物、共混物和部件,如外壳;电气/电子领域的制品,如插头、开关、板、灯座、灯罩;汽车领域的制品,如灯座和灯罩,以及窗玻璃;医疗领域的制品,如透析仪、接头、龙头;包装,如瓶子、容器;透镜、准直仪;发光二极管,或显示器的漫射板,和其它应用。
本申请还提供由本发明的聚合物制成的挤出物和成型体或成型件。
本发明的(共)聚碳酸酯成型物料的其它可能应用是:已知在建筑物、车辆和飞机上很多领域都需要的安全板,还有头盔的护板形式的安全板;生产显示器或电机的挤出或溶液薄膜,及滑雪板膜;生产吹塑制品,如水瓶(见,例如,US专利2 964 794);生产半透明板材,尤其空心板,例如,建筑物,如火车站、温室和照明系统的防护板;生产交通信号罩或交通标志;生产泡沫(见,例如,DE-B 1 031 507),生产丝和线(见,例如,DE-B 1 137 167和DE-A
1 785 137),以含玻璃纤维的半透明塑料的形式用于照明(见,例如,DE-A 1 554 020),以及生产精密注塑零件,如镜头架。这里所用的(共)聚碳酸酯含玻璃纤维,而且任选地,包含约1 重量%~10 重量%MoS2,基于总重量。其它光学应用的实例是光学存储器(CD、DVD),防护眼镜以及照相机和摄影机的透镜(见,例如,DE-A 2 701 173),光传播载体,尤其以光导线缆形式(见,例如,EP-A1 0 089 801),以电绝缘材料形式,用于电导体和插头外壳以及插塞连接器,以载体材料形式,用于有机光导体;生产灯,如前大灯,作为人们所称的头灯,或以光漫射板或灯罩形式,或用于医疗应用,如充氧器和透析仪;或用于食品应用,如瓶子、炊具和巧克力模具;或用于汽车领域会与燃料和润滑剂接触的应用;或用于运动器具,例如,障碍滑雪杆;或用于家庭用品,如厨房水槽和邮箱外壳,或用于壳体,如配电箱,电气设备,家用设备;家庭用品、电气设备和电子设备的零部件;或生产摩托车头盔和防护头盔;或汽车零件,如窗玻璃、仪表板、车身零件、和减震器。下面的实施例用来进一步解释本发明。
实施例
下列原材料用来生产复合材料:
●A 2000 nat:由双酚TMC和BPA制成的共聚碳酸酯,来自Bayer
Material-Science AG,Leverkusen, 其MVR为5.3 cm3/10 min(330℃,2.16 kg),维卡温度为205℃。
●Pleximid 8813:聚(N-甲基丙烯酰亚胺),来自Röhm GmbH &
Co KG, Darmstadt,其MVR为20 cm3/10 min(260℃,10 kg),维卡温度为130℃。
●Pleximid 8817:聚(N-甲基丙烯酰亚胺),来自Röhm GmbH &
Co KG, Darmstadt,其MVR为1 cm3/10 min(260℃,10
kg),维卡温度为170℃。
用多螺杆挤出机制造2种Pleximid类型与基础共聚碳酸酯Apec 2000的各种试验混合物(见表1)。
用所得共混物注塑成彩色样板(厚4 mm),并表征下列光学特性:透光率、雾度和YI(黄度指数)。对共混物作力学和热性能的常规试验,如维卡温度、HDT、拉伸试验、弹性模量和抗冲击性,用不含添加剂的Apec
2000作为对照。下表1对照对比实施例(不含添加剂的样品)汇总了所有的性能。
Pleximid在Apec中的含量至多0.25重量%时,Pleximid对复合材料光学性能的有利作用明显可见,而力学、热学和流变性能基本没变。相反,当浓度超过0.25 重量%时,光学性能又变差,这一点,从透光率的减小及雾度和YI的增大上,表现出来。本领域的技术人员未曾料到,Pleximid产品在Apec中非常特定的浓度范围内会有利于提高光学性能。
Claims (12)
1.组合物,由以下组分组成:
A) 99.98~99.5重量份(基于组分A+B之和)分子量M(重均)为至少10 000 g·mol-1的高分子量热塑性芳族(共)聚碳酸酯,其包含式(Ⅰ)的结构单元
其中
R1和R2是氢、C1~C4-烷基,
k是0、1、2、3或4,
B) 0.02~0.5重量份(基于组分A+B之和)一种或多种包含至少一个通式(Ⅱ)或(Ⅲ)的结构单元的特定聚丙烯酸酯:
其中,
R3是C1~C8-烷基,优选甲基,
R4是C1~C6-烷基,优选甲基,
R5是氢、C1~C8-烷基,优选氢和甲基,和
R6是氢、C1~C4-烷基,优选甲基,
m和n是由分子量确定的整数
以及结构(Ⅱ)与(Ⅲ)的摩尔比是0 mol%~100 mol%,基于(Ⅱ)和(Ⅲ)的总摩尔数,而且结构(Ⅱ)和(Ⅲ)的总量为100 mol%。
2.权利要求1所述的组合物,其特征在于,所述(共)聚碳酸酯A)的分子量为20000 g·mol-1~300000 g·mol-1。
3.权利要求1或2所述的组合物,其特征在于,组分A)的用量是99.9~99.7重量份,以及组分B的用量是 0.1~0.3重量份(基于组分A+B之和)。
4.前述权利要求中任何一项所述的组合物,其特征在于,其它添加剂,如UV吸收剂、脱模助剂或热稳定剂的存在量各为50~5000 重量ppm,基于组分A+B之和。
7.权利要求6中所述的组合物,其中R9是叔丁基或氢和R10是甲基,以及结构(Ⅸ)或(Ⅹ)的摩尔比为2 mol%~98 mol%,基于(Ⅸ)和(Ⅹ)的总摩尔数计,而且结构(Ⅸ)和(Ⅹ)之和为100 mol%。
8.用于生产权利要求1~7中任何一项所述的组合物的方法:其中混合各组分,和在升高温度将它们熔体配混或熔体挤出。
10.权利要求9中所述的一种或多种聚丙烯酸酯的应用,其特征在于混合各组分,和将它们熔体配混或熔体挤出。
11.权利要求1~7中任何一项所述的组合物在生产成型件中的应用。
12.能从权利要求1~7中任何一项所述的组合物得到的成型件。
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CN111511834A (zh) * | 2017-12-20 | 2020-08-07 | 科思创德国股份有限公司 | 滑石填充的聚碳酸酯组合物 |
CN113614171A (zh) * | 2019-03-28 | 2021-11-05 | 科思创知识产权两合公司 | 具有小的热膨胀的填充聚碳酸酯组合物 |
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CN105209543B (zh) * | 2013-04-04 | 2017-10-13 | 科思创德国股份公司 | 具有改善的流变性能的耐高温(共)聚碳酸酯 |
WO2014161830A1 (de) * | 2013-04-04 | 2014-10-09 | Bayer Materialscience Ag | Hochtemperaturbeständige phthalimid-haltige (co)polycarbonate mit verbesserten rheologischen eigenschaften |
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CN111465654A (zh) * | 2017-12-20 | 2020-07-28 | 科思创德国股份有限公司 | 稳定化的经填充的聚碳酸酯组合物 |
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DE102009015040A1 (de) | 2010-09-30 |
US9139730B2 (en) | 2015-09-22 |
KR20110135946A (ko) | 2011-12-20 |
US20120022204A1 (en) | 2012-01-26 |
EP2411473B1 (de) | 2013-11-20 |
KR101727335B1 (ko) | 2017-04-26 |
WO2010108626A1 (de) | 2010-09-30 |
CN105462226A (zh) | 2016-04-06 |
EP2411473A1 (de) | 2012-02-01 |
JP2012521447A (ja) | 2012-09-13 |
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