CN1047604C - 聚烯烃组合物 - Google Patents
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Abstract
本发明揭示的聚烯烃组合物包含(A)一种丙烯聚合物材料和(B)一种由部分地交联的热塑性高弹体组合物,烯烃共聚物橡胶及其混合物组成的一个组中选出的聚合物材料。本发明的聚烯烃组合物具有低的光泽度。
Description
本发明涉及一种聚烯烃组合物,较具体地说,涉及一种含(A)丙烯聚合物材料和(B)烯烃聚合物材料的聚烯烃组合物,更具体地说,涉及一种含(A)丙烯聚合物材料和部分地交联的热塑性高弹性体组合物,乙烯-丙烯-共轭二烯三聚体橡胶或其混合物的烯烃聚合物材料的聚烯烃组合物。
烯烃聚合物材料,特别是丙烯聚合物材料,由于它们的优异物理和机械性能,已被广泛用于各个应用领域,例如纤维,膜,片和其它成型制品。然而,现已发现,某些烯烃聚合物材料在要求有低光泽度的应用中不能令人满意,例如在热成型,挤压贴胶,吹气模塑,注射模塑和片或膜的挤压等应用中,因为它们在加工后具有高的光泽度。
这样,工业上需要在经过加工后具有低光泽度且基本上仍保持其物理和机械性能的烯烃聚合物材料。
现已发现,通过将烯烃聚合物材料与部分交联的热塑性高弹体组合物,乙烯-丙烯-共轭二烯三聚体橡胶或其混合物共混,可得具有低光泽度的一种组合物。
如由可以提供一种聚烯烃组合物,主要包括(A)70一90%(重量)丙烯聚合物材料和(B)30—10%(重量)从部分交联的热塑性高弹体组合物,乙烯-丙烯-共轭二烯三聚体橡胶及其混合物组成的一组物质中选出的一种烯烃聚合物材料。
除另有说明外,用于本申请中的所有份数和百分数都以重量表示,环境温度或室温为约25℃。
用于本发明组合物的组份(A)为一种丙烯聚合物材料,主要由下述组份构成:
(1)10—50%,较好的为10—40%,最好为20—35%丙烯均聚物,其等规度为80—99%以上,较好的为85—99%,或为自下组中选出的一种共聚物:(a)丙烯和乙烯,(b)丙烯,乙烯和CH2=CHRα-烯烃,其中R为C2-8直链或支链烷基,和(C)丙烯和α-烯烃,其定义如上述(1)(b)中所述,其中所述的共聚物含85—99%,较好的为90—99%的丙烯,且其等规度为大于80—98%,较好的为大于85—98%。
(2)5—20%,较好的为7—15%半结晶的,基本为线型共聚物的组份,由差示扫描量热法(DSC)测得其结晶度约为20—60%,其中共聚物选自下列的一个组:(a)乙烯和丙烯,含乙烯大于55%;(b)乙烯,丙烯,和如上述(1)(b)中定义的α-烯烃,含1—10%的α-烯烃,和55%—98%,较好的为80—95%的乙烯和α-烯烃;和(c)乙烯和如(1)(b)中定义的α-烯烃,含55%—98%,较好的为80—95%的所述α-烯烃,在室温或环境温度下所述共聚物不溶于二甲苯,和
(3)40—80%,较好的为50—70%的共聚物部分,它选自下列共聚物构成的一个组:(a)乙烯和丙烯,其中共聚物含20%—40%,较好的为20—38%,最好为25—38%的乙烯;(b)乙烯,丙烯,和如(1)(b)中定义的α-烯烃,其中所存在的α-烯烃的量为1—10%,较好的为1—5%,所存在的乙烯和α-烯烃的量为20%—小于40%;和(c)乙烯和如(1)(b)中定义的α-烯烃,含20—40%,较好的为20—38%,最好为25—35%的α-烯烃,和任选的0.5—10%,较好的为1—5%的二烯,所述的共聚物组份在环境温度下能溶于二甲苯,其特性粘度较好的为1.7—3.0dl/g,其中在烯烃聚合物组合物中的乙烯单元或所述α-烯烃单元的总量或当烯烃聚合物组合物中存在着乙烯和所述α-烯烃单元时的两者的总量为15—35%,(2)和(3)部分的总量,以总的烯烃聚合物组合物为计算基准,较好的约为65%—80%,(2)/(3)的重量比较好的为0.1—约0.3,在(2+3)中的乙烯或C4—8α-烯烃或其结合体的总含量为小于50%,较好的为20—45%。
组份(A)的组合物,由DSC法测定,在高于120℃的温度处至少有一个熔融峰,且在-10℃—-35℃之间的温度处至少有一个相应于玻璃态转变的峰。另外,这些组合物有一个小于150MPa的弯曲模量,通常为20—100MPa;在屈服点处的抗拉强度为10—20MPa,在断裂点处的伸长率高于400%;在75%应变下的永久变形为20%—50%;Shore D硬度为20—35;浊度值小于40%,较好的为小于35%,当在-50℃时进行悬臂梁式冲击试验时不发生断裂(无脆性冲击断裂)。
所述组份(A)的量为总组合物的70—90%,较好地且最好为75—85%。
本发明的组份(B)为一种烯烃聚合物材料,选自主要由下列物质组成的组:
(1)一种部分交联的热塑性高弹体组合物,它主要由以下物质组成:
(a)50份(重量)热塑性高弹体,它主要由以下物质组成:
(i)30—70%,较好的为20—50%的丙烯均聚物,其等规度大于90,较好的为大于98%,或者丙烯与乙烯和/或C4—8α-烯烃的结晶性共聚物,其丙烯含量大于85%,且等规度大于85%;
(ii)30—70%,较好的为30—50%的非结晶性乙烯-丙烯或丁烯共聚物部份,可任意地含1—10%,较好的为1—5%二烯,该部份在室温下可溶于二甲苯,且含30—70%乙烯;
(iii)10—30%,较好的为10—20%的半结晶性乙烯-丙烯或丁烯共聚物,该共聚物在室温下不溶于二甲苯,且含大于90%,较好的为大于95%乙烯;和
(iv)以100份(i)+(ii)+(iii)为基准,2—20重量份聚丁烯-1,其中聚丁烯-1与橡胶之比小于0.5;和
(b)55重量份烯烃橡胶组合物,它主要由以下物质构成;
(i)16.4%等规度大于90,较好的为大于98%的丙烯均聚物,和(ii)74.6%含30—70%乙烯的乙烯-丙烯共聚物橡胶;和
(2)乙烯-丙烯-共轭二烯三聚体橡胶,其乙烯含量为40—77%,较好的为45—75%,二烯含量为2—10%,较好的为3—8%。
在本发明的组合物中,组份(B)的量较好的为10—30%,更好的为20—15%。
当组份(B)为组份(B)(1)和(B)(2)的混合物时,所存在的组份(B)(1)的量为5—15%,组份(B)(2)的量为20—10%。
可用于制备上述丙烯聚合物材料和烯烃聚合物材料的组份(A)和(B)的C4—C10α-烯烃包括丁烯-1,戊烯-1,己烯-1,4-甲基戊烯-1和辛烯-1,丁烯-1则特别好。
当含有二烯时,典型的其为丁二烯,1,4-己二烯,1,5-己二烯或亚乙基降冰片烯二烯单体。
配合或熔融共混如上所述的本发明的组份(A)和组份(B)时,可在开放式辊上,在内混合机(例如Banbury或Haake混合机),以及单螺杆或双螺杆挤压机中进行。
本发明的聚烯烃组合物也可包含其它常规添加剂,例如,抗氧剂,稳定剂,增量油,如石蜡和环烷油;填料,如CaCO3,滑石和氧化锌;或阻燃剂。
本发明将结合下述本发明的实施例作更详细的描述,下列工作实施例和对比实施例的试验样品和光泽度性能按下法制备和测量:
光泽度45° ASTM D-523-85
熔融流动速率(MFR) ASTM D-1238, 条件L
实施例1
本发明的聚烯烃组合物用通常方法制备,包括共混如表1所列的聚合物(A)和聚合物(C),直至获得均匀混合物。
将配合好的混合物在常规的5盎司注射模塑机上进行注射模塑,筒温为420F,用水冷却,模塑温度为80F,制得40密耳,3″×3″的板。
光泽度性能列于表1中。
参照1
除了组合物中只含聚合物(A)外,按实施例1的通常方法制备聚烯烃组合物。
光泽度性能列于表1中。
实施例2
除了如表1所列,使用聚合物(B)代替聚合物(C)外,按实施例1的通常方法制备实施例2的组合物。
组合物的光泽度性能列于表1中。
实施例3和4
除了如表1所列使组合物含实施例1中的聚合物(A)和聚合物(C)之外还含聚合物(B)外,按实施例1的通常方法制备实施3—4的组合物。
组合物的光泽度性能列于表1中。
表1组份 参照1 实施例1 实施例2 实施例3 实施例4聚合物 100 75 75 75 75A,%聚合物 -- -- 25 20 10B,%聚合物 -- 25 -- 5 15C,%稳定剂1 0.2 0.2 0.2 0.2 0.2硬脂酸钙 0.1 0.1 0.1 0.1 0.1碳黑 4 4 4 4 4性能45°光泽度 44 27 37 32 32
聚合物A——一种烯烃聚合物组合物,含30%乙烯含量为3.3%的丙烯-乙烯无规共聚物,7%含51.9%乙烯的半结晶性乙烯-丙烯共聚物部份,和63%乙烯含量为31.1%的非结晶性乙烯-丙烯共聚物部分,该组合物的二甲苯可溶性成份含量为51%。
聚合物B——一种乙烯-丙烯-共轭二烯三聚体橡胶。
聚合物C——一种部分交联的热塑性高弹体组合物,含50份(重量)含40份丙烯均聚物、50份乙烯-丙烯共聚物橡胶、10份半结晶性乙烯-丙烯共聚物和10份聚丁烯-1的热塑性高弹体,与55份(重量)主要含16.4%丙烯均聚物和74.6%乙烯-丙烯共聚物橡胶的烯烃橡胶进行共混。
稳定剂1—Irganox B225-3,5-双(1,1-二甲乙基)-4-羟基苯丙酸2,2-双〔〔3-〔3,5-双(1,1-二甲乙基)-4-羟苯基〕-1-氧代丙氧基〕甲基〕-1,3-丙二基酯稳定剂和亚磷酸三(2,4-二叔丁苯基)酯以50∶50混合。
如表1所示,本发明的组合物与参照1相比,其光泽度至少减少20%。实施例5—8
除了使用Lupersol101过氧化物以获得具有各种熔融流动速率(MFR)的组合物外,按实施例1组合物的通常方法制备实施例5—8的组合物。
光泽度性能列于表2中
表2组份 参照1 实施例5 实施例6 实施例7 实施例8聚合物 100 75 75 75 75A,%聚合物 -- 25 25 25 25B,%Lupersol -- 0.01 0.01 0.01 0.01101稳定剂1 0.2 0.2 0.2 0.2 0.2硬脂酸钙 0.1 0.1 0.1 0.1 0.1碳黑 4 4 4 4 4性能MFR -- 0.8 1.0 3.4 7.045°光泽 44 33 34 39 38度%
由此可见,与参照1的组合物相比,由本发明组合物制得的注射模塑板的光泽度至少减少20%。
对于那些从事本领域的一般熟练技术人员来说,在阅读上述内容后,本发明的其它特征,优点和具体实例都将是很明白的了,按照这一点,当本发明的特定具体实例已作相当详细的描述后,这些实例的变体和改进在不背离所述本发明及其权利要求书的精神和范围下都可以是有效的。
Claims (7)
1. 一种聚烯烃组合物,包含70—90重量%丙烯聚合物材料(A),它主要由下述组份构成:
(1)10—50重量%丙烯均聚物,其等规度为85—99%,或为自下组中选出的一种共聚物:(a)丙烯和乙烯,(b)丙烯,乙烯和CH2=CHRα-烯烃,其中R为C2-8直链或支链烷基,和(c)丙烯和α-烯烃,其定义如上述(1)(b)中所述,
(2)5—20重量%半结晶性的,基本为线型共聚物的组份,由差示扫描量热法测得其结晶度为20—60%,其中共聚物选自下列的一个组:(a)乙烯和丙烯,含乙烯大于55重量%;(b)乙烯,丙烯,和如上述(1)(b)中定义的α-烯烃,含1—10重量%的α-烯烃,和55—98重量%的乙烯和α-烯烃;和(c)乙烯和如(1)(b)中定义的α-烯烃,含55—98重量%的所述α-烯烃,在室温或环境温度下所述共聚物不溶于二甲苯,和
(3)40—80重量%共聚物部份,它选自下列共聚物构成的一个组:(a)乙烯和丙烯,其中共聚物含20—40重量%的乙烯;(b)乙烯,丙烯,和如(1)(b)中定义的α-烯烃,其中所存在的α-烯烃的量为1—10重量%,所存在的乙烯和α-烯烃的量为20—小于40重量%;和(c)乙烯和如(1)(b)中定义的α-烯烃,含20—40重量%的α-烯烃,和任选的0.5—10重量%的二烯,所述的共聚物组份在环境温度下能溶于二甲苯,其特性粘度为1.7—3.0dl/g,其中(2)和(3)组份的总量,以总的烯烃聚合物组合物为计算基准,为65%—80重量%,(2)/(3)的重量比为0.1—0.3,在(2)+(3)中的乙烯或C4-8α-烯烃或其结合体的总含量为小于50重量%,和
(B)30—10重量%的烯烃聚合物材料,它选自主要由下列物质构成的一个组:
(1)一种部分交联的热塑性烯烃高弹体组合物,它主要由以下物质组成:
(a)50重量份热塑性高弹体,它主要由以下物质组成:
(i)30—70重量%丙烯均聚物,其等规度大于90,或者丙烯与乙烯和/或C4-8α-烯烃的结晶性共聚物,其丙烯含量大于85重量%,且等规度大于85%;
(ii)30—70重量%的非结晶性乙烯-丙烯或丁烯共聚物部份,可任意地含1—10重量%二烯,该部份在室温下可溶于二甲苯,且含30—70重量%乙烯;
(iii)10—30重量%的半结晶性乙烯-丙烯或丁烯共聚物,该共聚物在室温下不溶于二甲苯,且含大于90重量%乙烯;和
(iv)以100份(i)+(ii)+(iii)为基准,2—20重量份聚丁烯-1,其中聚丁烯-1与橡胶之比小于0.5;和
(b)55重量份烯烃橡胶组合物,它主要由以下物质构成:
(i)16.4重量%等规度大于90的丙烯均聚物,和(ii)74.6重量%含30—70重量%乙烯的乙烯-丙烯共聚物橡胶;和
(2)乙烯-丙烯-共轭二烯三聚体橡胶,其乙烯含量为40—77重量%,二烯含量为2—10重量%;和
(3)它们的混合物。
2. 如权利要求1所述的组合物,其特征在于,其中组份(A)为一种丙烯聚合物材料,它主要由以下组份构成:
(1)10—50重量%自下组中选出的一种共聚物:(a)丙烯和乙烯,(b)丙烯,乙烯和CH2=CHRα-烯烃,其中R为C2-8直链或支链烷基,和(c)丙烯和α-烯烃,其定义如上述(1)(b)中所述,
(2)5—20重量%半结晶性的,基本为线型的共聚物的组份,由差示扫描量热法测得其结晶度为20—60%,其中共聚物选自下列的一个组:(a)乙烯和丙烯,含乙烯大于55重量%;(b)乙烯,丙烯,和如上述(1)(b)中定义的α-烯烃,含1—10重量%的α-烯烃,和55—98重量%的乙烯和α-烯烃;和(c)乙烯和如(1)(b)中定义的α-烯烃,含55—98重量%的所述α-烯烃,在室温或环境温度下所述共聚物不溶于二甲苯,和
(3)40—80重量%乙烯和丙烯的共聚物部份,其中所述共聚物含20—小于40重量%的乙烯;所述的共聚物组份在环境温度下能溶于二甲苯,其特性粘度为1.7—3.0dl/g,其中(2)和(3)组份的总量,以总的烯烃聚合物组合物为计算基准,为65—80重量%,(2)/(3)的重量比为0.1—0.3,在(2)+(3)中的乙烯或C4-8α-烯烃或其结合体的总含量为小于50重量%。
3. 如权利要求2所述的组合物,其特征在于,其中组份(B)为一种部分交联的热塑性高弹体组合物,它主要由以下组份构成:
(1)50重量份热塑性高弹体,它主要由以下物质组成:
(a)30—70重量%的丙烯均聚物,其等规度大于90,或者丙烯与乙烯和/或C4-8α-烯烃的结晶性共聚物,其丙烯含量大于85重量%,且等规度大于85%;
(b)30—70重量%的非结晶性乙烯-丙烯或丁烯共聚物部份,可任意地含1—10重量%二烯,该部份在室温下可溶于二甲苯,且含30—70重量%乙烯;
(c)10—30重量%的半结晶性乙烯-丙烯或丁烯共聚物,该共聚物在室温下不溶于二甲苯,且含大于90重量%乙烯;和
(d)以100份(a)+(b)+(c)为基准,2—20重量份聚丁烯-1,其中聚丁烯-1与橡胶之比小于0.5;和
(2)55重量份烯烃橡胶组合物,它主要由以下物质构成:
(a)16.4重量%等规度大于90的丙烯均聚物,和(b)74.6重量%含30—70重量%乙烯的乙烯-丙烯共聚物橡胶。
4. 如权利要求2所述的组合物,其特征在于,其中组份(B)为一种乙烯-丙烯-共轭二烯三聚体橡胶,其乙烯含量为40—77重量%,二烯含量为2—10重量%。
5. 如权利要求2所述的组合物,其特征在于,其中组份(B)为(B)(1)和(B)(2)的一种混合物。
6. 如权利要求5所述的组合物,其特征在于,其中组份(B)(1)的存在量为5—15重量%,组份(B)(2)的存在量为20—10重量%。
7. 如权利要求1所述的组合物,其特征在于,其中组份(A)的存在量为75—85重量%,组份(B)的存在量为25—15重量%。
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
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US139,963 | 1993-10-20 | ||
US08/139,963 US5338801A (en) | 1993-10-20 | 1993-10-20 | Compositions of propylene polymer materials and olefin polymer materials with reduced gloss |
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CN1106033A CN1106033A (zh) | 1995-08-02 |
CN1047604C true CN1047604C (zh) | 1999-12-22 |
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CN94117496A Expired - Fee Related CN1047604C (zh) | 1993-10-20 | 1994-10-20 | 聚烯烃组合物 |
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US (1) | US5338801A (zh) |
EP (1) | EP0649872B1 (zh) |
JP (1) | JP3406404B2 (zh) |
KR (1) | KR950011419A (zh) |
CN (1) | CN1047604C (zh) |
AT (1) | ATE158329T1 (zh) |
AU (1) | AU675874B2 (zh) |
BR (1) | BR9404160A (zh) |
CA (1) | CA2117859C (zh) |
DE (1) | DE69405676T2 (zh) |
DK (1) | DK0649872T3 (zh) |
TW (1) | TW276262B (zh) |
Families Citing this family (26)
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IT1271420B (it) * | 1993-08-30 | 1997-05-28 | Himont Inc | Composizioni poliolefiniche aventi un elevato bilancio di rigidita' e resilienza |
US6686433B1 (en) | 1994-02-04 | 2004-02-03 | Exxonmobil Chemical Patents Inc. | Dual donor catalyst system for the polymerization of olefins |
WO1995021203A1 (en) * | 1994-02-04 | 1995-08-10 | Exxon Chemical Patents Inc. | Dual donor catalyst system for the polymerization of olefins |
AU696168B2 (en) * | 1995-04-28 | 1998-09-03 | Sumitomo Chemical Company, Limited | Thermoplastic resin composition |
JPH08302114A (ja) * | 1995-04-28 | 1996-11-19 | Sumitomo Chem Co Ltd | 熱可塑性樹脂組成物 |
MY114719A (en) | 1995-06-29 | 2002-12-31 | Mitsui Chemicals Inc | Olefin thermoplastic elastomer compositions |
US5552482A (en) * | 1995-09-08 | 1996-09-03 | Montell North America Inc. | Thermoplastic elastomers with improved extrusion performance |
IT1287179B1 (it) * | 1996-11-15 | 1998-08-04 | Montell North America Inc | Miscela polimerica per slush moulding |
EP0844278B1 (en) * | 1996-11-26 | 2003-05-28 | Basell North America Inc. | Polyolefin composition used for making embossed sheets with improved grain retention |
ATE258207T1 (de) * | 1996-11-26 | 2004-02-15 | Basell North America Inc | Polyolefinzusammensetzungen für die herstellugn von folien mit vertiefungen mit verbesserter erhaltung der kornstruktur |
US6013734A (en) * | 1997-04-29 | 2000-01-11 | Montell North America Inc. | Thermoplastic olefin composition containing an ethylene polymer for making molded parts having a good paint adhesion/durability balance |
WO1999020663A2 (en) * | 1997-10-17 | 1999-04-29 | Exxon Chemical Patents Inc. | High impact, flexural moduli polymeric materials formed using sequential donors |
US6087459A (en) * | 1998-05-14 | 2000-07-11 | Exxon Chemical Patents Inc. | Polymeric materials formed using blends of electron donors |
JP3634965B2 (ja) * | 1998-07-14 | 2005-03-30 | 日本ポリプロ株式会社 | プロピレン系樹脂組成物 |
US6020046A (en) * | 1998-10-23 | 2000-02-01 | Montell North America Inc. | Embossed sheets of polyolefin compositions with improved grain retention |
US6548600B2 (en) | 2000-09-22 | 2003-04-15 | Dupont Dow Elastomers L.L.C. | Thermoplastic elastomer compositions rheology-modified using peroxides and free radical coagents |
US6566294B2 (en) | 2000-12-21 | 2003-05-20 | Exxonmobil Chemical Patents Inc. | Multi-donor catalyst system for the polymerization of olefins |
US7338994B2 (en) * | 2002-10-01 | 2008-03-04 | Dow Global Technologies Inc. | Rheology-modified thermoplastic elastomer compositions for extruded profiles |
US7259211B2 (en) * | 2003-12-12 | 2007-08-21 | Mitsui Chemicals, Inc. | Ethylene type ternary copolymer and propylene type resin composition |
US7041741B2 (en) * | 2004-01-08 | 2006-05-09 | Teknor Apex Company | Toughened polymer compositions |
US7557162B2 (en) * | 2004-01-08 | 2009-07-07 | Teknor Apex Company | Toughened polymer compositions |
CN101392083B (zh) * | 2004-04-19 | 2011-04-06 | 三井化学株式会社 | α-烯烃类聚合物组合物、由该组合物制成的成形体、新聚合物 |
JP4802503B2 (ja) * | 2005-01-21 | 2011-10-26 | マツダ株式会社 | 操作部材用熱可塑性エラストマー組成物及びその成形部材 |
CA2606584A1 (en) * | 2005-05-12 | 2006-11-23 | Dow Global Technologies Inc. | Thermoformed, extruded sheeting with reduced gloss |
KR101646437B1 (ko) * | 2015-01-23 | 2016-08-05 | 한화토탈 주식회사 | 저광택 및 플로우마크 외관 불량이 억제된 폴리프로필렌 수지 조성물 |
EP4251694A1 (en) * | 2020-11-26 | 2023-10-04 | Basell Poliolefine Italia S.r.l. | Polyolefin compositions obtained from recycled polyolefins |
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JPS62112644A (ja) * | 1985-11-11 | 1987-05-23 | Nippon Petrochem Co Ltd | 軟質ポリオレフイン系組成物 |
JPH0733460B2 (ja) * | 1987-06-23 | 1995-04-12 | 日産自動車株式会社 | 自動車バンパ−用樹脂組成物 |
IT1230133B (it) * | 1989-04-28 | 1991-10-14 | Himont Inc | Composizioni polipropileniche plasto-elastiche |
IT1243188B (it) * | 1990-08-01 | 1994-05-24 | Himont Inc | Composizioni poliolefiniche elastoplastiche |
US5143978A (en) * | 1990-08-28 | 1992-09-01 | Himont Incorporated | Dynamically partially crosslinked thermoplastic elastomer containing polybutene-1 |
US5212246A (en) * | 1990-09-28 | 1993-05-18 | Himont Incorporated | Olefin polymer films |
US5196462A (en) * | 1991-05-16 | 1993-03-23 | Himont Incorporated | Zinc-salts of certain mercapto compounds as antioxidants for high temperature aging of thermoplastic elastomers |
EP0714948B1 (en) * | 1992-06-04 | 1998-07-15 | Tonen Chemical Corporation | Resin composition having excellent paint coatability |
-
1993
- 1993-10-20 US US08/139,963 patent/US5338801A/en not_active Expired - Lifetime
-
1994
- 1994-05-24 TW TW083104714A patent/TW276262B/zh active
- 1994-10-11 DE DE69405676T patent/DE69405676T2/de not_active Expired - Lifetime
- 1994-10-11 EP EP94116000A patent/EP0649872B1/en not_active Expired - Lifetime
- 1994-10-11 DK DK94116000.4T patent/DK0649872T3/da active
- 1994-10-11 CA CA002117859A patent/CA2117859C/en not_active Expired - Fee Related
- 1994-10-11 AT AT94116000T patent/ATE158329T1/de not_active IP Right Cessation
- 1994-10-14 AU AU75833/94A patent/AU675874B2/en not_active Ceased
- 1994-10-19 KR KR1019940026705A patent/KR950011419A/ko active IP Right Grant
- 1994-10-19 BR BR9404160A patent/BR9404160A/pt not_active IP Right Cessation
- 1994-10-20 CN CN94117496A patent/CN1047604C/zh not_active Expired - Fee Related
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Also Published As
Publication number | Publication date |
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DE69405676T2 (de) | 1998-02-26 |
AU7583394A (en) | 1995-05-11 |
JP3406404B2 (ja) | 2003-05-12 |
BR9404160A (pt) | 1995-06-20 |
ATE158329T1 (de) | 1997-10-15 |
AU675874B2 (en) | 1997-02-20 |
CA2117859A1 (en) | 1995-04-21 |
DE69405676D1 (de) | 1997-10-23 |
TW276262B (zh) | 1996-05-21 |
CA2117859C (en) | 2000-09-19 |
EP0649872B1 (en) | 1997-09-17 |
CN1106033A (zh) | 1995-08-02 |
KR950011419A (ko) | 1995-05-15 |
JPH07157607A (ja) | 1995-06-20 |
EP0649872A3 (en) | 1995-06-14 |
DK0649872T3 (da) | 1998-02-02 |
US5338801A (en) | 1994-08-16 |
EP0649872A2 (en) | 1995-04-26 |
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