CN1323852A - 具有永久抗雾性能的聚烯烃薄膜组合物 - Google Patents
具有永久抗雾性能的聚烯烃薄膜组合物 Download PDFInfo
- Publication number
- CN1323852A CN1323852A CN01121424A CN01121424A CN1323852A CN 1323852 A CN1323852 A CN 1323852A CN 01121424 A CN01121424 A CN 01121424A CN 01121424 A CN01121424 A CN 01121424A CN 1323852 A CN1323852 A CN 1323852A
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- Prior art keywords
- film
- phenyl
- hydroxyl
- tertiary butyl
- butyl
- Prior art date
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- Granted
Links
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Abstract
一种聚烯烃薄膜呈现极佳的长期持续抗雾性能,其中掺入分子式为CH3CH2(CH2CH2)aCH2CH2(OCH2H2)bOH的化合物,其中a为9-25,b为1-10。该聚烯烃薄膜用作潮湿产品的包装薄膜和用作农业应用的温室薄膜。
Description
本发明涉及一种新颖的抗生雾烯烃聚合物组合物,尤其是用作潮湿产品的包装薄膜和用作农业应用的温室薄膜的组合物。
大量用于温室栽培或隧道栽培的农业薄膜主要包括大约30-200微米厚的软乙烯树脂薄膜,其包括,作为基本树脂,聚氯乙烯(以下简称PVC)、支化低密度聚乙烯(以下简称LDPE)、乙烯-醋酸乙烯酯共聚物(EVA)、线性低密度聚乙烯(以下简称LLDPE),等等。对于农业薄膜所需要的各种性能,特别重要的是耐候性、抗雾性、保温性,和透明性。为了克服目前农业所面临的费用增加和劳力减少的情况,人们希望开发在更换之前具有延长使用寿命的薄膜。
在农业薄膜所环绕的温室或隧道内的空气是被从土壤和植物蒸发的水蒸气饱和的,该水蒸气冷凝滴落在冷薄膜的内表面形成雾。薄膜上的水滴由于不规则反射不仅大大降低入射的阳光而且滴落在植物上造成频繁出现病害。
为了避免起雾,已采用在农业薄膜内表面抗雾处理将薄膜变为抗沾水薄膜并防止水滴粘合,由此保证阳光透入温室或隧道,提高温室或隧道内的土壤温度和气温,促进植物的光合作用,促进植物健康生长,并且控制植物病害的发生。
目前采用的抗雾处理包括将抗雾剂(抗雾添加剂)掺入形成薄膜的乙烯树脂化合物和涂覆抗雾剂至薄膜上。
然而,通过用抗雾剂涂覆软塑料薄膜而得到的抗雾薄膜尚未作为农业薄膜而实际应用,这是由于以下原因。由于其表面能低,农业应用的软塑料薄膜当用表面活性剂或亲水高聚物(已被用作抗雾剂)涂覆时一般吸湿性和粘合性差。当用低极性的软乙烯树脂薄膜,例如LDPE、EVA、和LLDPE薄膜时这种趋势特别明显。因此,当用喷雾器将抗雾剂喷涂到软乙烯树脂薄膜时,需要使用大量的抗雾剂,从而提高了费用,而且喷射涂覆操作需要大量的时间。此外,喷射涂覆不能均匀地实施从而出现抗雾效果不充分。在用涂覆机等涂施抗雾剂时,消耗了大量涂料,而且不能提高涂覆速度,造成费用增加。在任何一种情况下,由于粘合力差,涂覆的抗雾剂可被水滴冲走,导致抗雾性能的寿命很短。此外,由于抗雾剂的粘着性使涂覆薄膜产生粘连。结果,不能以稳定的方式将抗雾效果保持长达至少1年,更希望几年。大多数现有技术农业薄膜呈现抗雾性能仅仅大约1个月的时间。
一般掺入薄膜的抗雾剂包括非离子的、阴离子的和阳离子的表面活性剂。
除了涂覆方法和掺入方法以外,提供给农业薄膜抗雾性能的其它方法包括乙烯基树脂的化学改性或乙烯树脂薄膜表面引入极性基,例如亲水基。然而,此技术目前需要费用高因此很难实施于农业薄膜。
另一方面,涂覆型抗雾剂主要包括一种无机亲水胶体物质和一种亲水有机化合物,其近年来已被开发,如在JP63-45432和JP63-45717中所揭示。适宜的无机亲水胶体物质包括胶态二氧化硅、胶态氧化铝、胶态Fe(OH)2、胶态Sn(OH)4、胶态TiO2、胶态BaSO4、和胶态硅酸锂,最常用的是胶态二氧化硅和胶态氧化铝。适宜的亲水有机化合物包括各种非离子、阴离子或阳离子表面活性剂;主要包括含羟基乙烯单体单元和0.1-40%重量含羧基乙烯单体单元接枝共聚物或其局部或全部中和产物,以及含硫聚酯树脂。
这种新型薄膜所用的涂覆型抗雾剂显著改善了湿润性和粘合性,涂覆的农业薄膜呈现抗雾性能大约半年至1年的时间。
在这些情况下,没有任何现有技术的聚烯烃基农业薄膜满足长期维持抗雾性能的要求。
在包装领域,其中聚合物薄膜用于包覆或封入商品,在此处希望薄膜透明或商品可视性,对于聚合物薄膜当其曝露于可在薄膜上产生冷凝水的温度和湿度条件下时需要其抗雾。当包装物内部含有足够水蒸气以致在薄膜内表面产生雾时此冷凝水特别麻烦。尽管与非食品也有关系,然而此处特别有关的是食品产品的包装,例如、肉食、面包、蔬菜、水果,等等。
为了对食品产品提供卫生保护,为了提供比纸更易于和更经济的包裹材料,或提供食品产品更好的样式,食品产品常常被放入聚合物薄膜中包装以便顾客好拿。随着增塑的聚氯乙烯(PVC)广泛用于市场,各种聚合物材料,例如聚氯乙烯、聚(乙烯/醋酸乙烯酯)和辐射聚乙烯已被用于食品包装市场。新鲜的肉和蔬菜常常用这些薄膜包装,该薄膜的某些性能因能满足食品包装要求因此是所希望的。显然,在此应用中所用的薄膜具有良好的“透视”透明性,所以产品可被看到。对于顾客来说为了美学要求对包装加入高光泽性“闪光”是所希望的。当这些食品产品被包装时,它们一般经历从它们被包装处至它们被存储或出售处的温度变化。此温度变化可引起水滴在薄膜内表面的形成(通常称作“雾”)。这些水滴常常是令人讨厌的,因为它们妨碍顾客对食品产品的视线,并可造成腐败,特别是对某些蔬菜。为了防止冷凝水滴,常常对薄膜加入抗雾剂。此抗雾剂降低水的表面张力并因此使水形成连续的片状,因而是透明的。
在市场中对改进的包装薄膜有一种共同的需求,尤其是对食品产品的包装,其中广泛使用增塑的聚氯乙烯(PVC),需要用更加受欢迎的薄膜来替换。已经被使用的许多PVC薄膜是用添加剂,例如邻苯二甲酸二辛基酯增塑的,它们在市场上已经不太受欢迎。
美国专利5262233揭示了一种掺入抗雾剂的农业薄膜,其可以是一种长链醇的聚(环氧乙烷)。
WO91/04853揭示了一种具有增强表面能的聚合物组合物,包括,例如分子式为RO-(CH2CH2O)9R的化合物。
Atmer502,在1998年9月数据表中加以描述,其在LDPE农业薄膜中具有长效抗雾性能。Atmer502,一种乙氧基化醚,是ICI美国的商标。
本发明涉及一种具有抗雾性能的聚烯烃薄膜组合物,包括
(a)聚烯烃薄膜,和
(b)分子式为CH3CH2(CH2CH2)aCH2CH2(OCH2CH2)bOH的化合物,其中a为9-25,b为1-10。
在组分(b)的分子式CH3CH2(CH2CH2)aCH2CH2(OCH2CH2)bOH的化合物中,“a”是例如9、10、11、12、13、14、15、16、17、18、19、20、21、22、23、24或25。“b”是例如1、2、3、4、5、6、7、8、9或10。
聚烯烃的例子是
1.单烯烃和二烯烃聚合物,例如聚丙烯、聚异丁烯、聚丁烯-1、聚4甲基戊烯-1、聚异戊二烯或聚丁二烯,以及环烯烃聚合物,例如环戊烯或降冰片烯,聚乙烯(可选择被交联),例如高密度聚乙烯(HDPE)、高密度和高分子量聚乙烯(HDPE-HMW)、高密度和超高分子量聚乙烯(HDPE-UHMW)、中密度聚乙烯(MDPE)、低密度聚乙烯(LDPE)、线性低密度聚乙烯(LLDPE)、(VLDPE)和(ULDPE)。
聚烯烃,即在前段所例举的单烯烃聚合物,优选是聚乙烯和聚丙烯,可通过不同的方法,尤其是以下的方法来制备:
ⅰ)自由基聚合(即在高压下和高温下聚合)。
ⅱ)使用催化剂的催化聚合,该催化剂一般包含一种或一种以上的周期表Ⅳb、Ⅴb、Ⅵb或Ⅷ族金属。这些金属通常具有一种或一种以上的配位体,有代表性的是氧化物、卤化物、醇化物、酯、醚、胺、烷基、链烯基和/或芳基,它们可以是对位或对称配位。这些金属配位体可以是游离的形式或固定在基体上,代表性的是活化氯化镁、氯化钛(Ⅲ)、氧化铝或氧化硅。这些催化剂在聚合介质中是可溶解的或不可溶解的。该催化剂可在聚合中自身使用或进一步使用活化剂,代表性的是烷基金属、金属氢化物、烷基金属卤化物、烷基金属氧化物或金属烷基环氧乙烷,所说的金属是周期表Ⅰa、Ⅱa和/或Ⅲa族元素。活化剂可进一步用酯、醚、胺或甲硅烷基醚基常规改性。这些催化剂体系通常被称作Phillips,Standard Oil Indiana,Ziegler(-Natta),TNZ(DuPont),金属茂或单点催化剂(SSC)。
2.1.)所指聚合物的混合物,例如聚丙烯和聚异丁烯的混合物、聚丙烯和聚乙烯(例如PP/HDPE,PP/LDPE)的混合物以及不同类型聚乙烯(例如LDPE/HDPE)的混合物。
3.单烯烃和二烯烃相互间或与其它乙烯基单体的共聚物,例如乙烯/丙烯共聚物、线性低密度聚乙烯(LLDPE)和其与低密度聚乙烯(LDPE)的混合物、丙烯/丁烯1共聚物、丙烯/异丁烯共聚物、乙烯/丁烯-1共聚物、乙烯/己烯共聚物、乙烯/甲基戊烯共聚物、乙烯/庚烯共聚物、乙烯/辛烯共聚物、丙烯/丁二烯共聚物、异丁烯/异戊二烯共聚物、乙烯/丙烯酸烷基酯共聚物、乙烯/甲基丙烯酸烷基酯共聚物、乙烯/醋酸乙烯酯共聚物和它们与一氧化碳的共聚物或乙烯/丙烯酸共聚物和它们的盐(离聚物)以及乙烯与丙烯和一个二烯例如己二烯、二环戊二烯或亚乙基-降冰片烯的三聚物,和这种共聚物与另一共聚物及上述1)的聚合物的混合物,例如聚丙烯/乙烯-丙烯共聚物、LDPE/乙烯-醋酸乙烯共聚物(EVA)、LDPE/乙烯丙烯酸共聚物(EAA)、LLDPF/EVA、LLDPE/EAA和交替或无规聚亚烷基/一氧化碳共聚物和其与其它聚合物例如聚酰胺的混合物。
优选的聚烯烃是聚乙烯或聚丙烯和它们与单烯烃和二烯烃的共聚物。
本发明的乙烯聚合物是其特征为具有熔融指数或熔体流动值大约在0.01-20克/10分钟范围(以ASTM-D-1238,条件E测量),密度在大约0.9-0.96克/cc范围的聚合物。这些聚合物包括在高压下用自由基引发剂制备的支化聚合物和在低压、中压或高压用配位催化剂制备的线性聚合物(即基本上无支化的聚合物)的那些聚合物。用自由基引发剂(例如过氧化物)制备的那些聚合物是现有技术已知的“低密度聚乙烯”(LDPE),用配位催化剂(如齐格勒催化剂)制备的那些聚合物是现有技术已知的“高密度聚乙烯”(HDPE)。
最新开发的是商业上所称的“线性低密度聚乙烯”(LLDPE),其是通过配位催化剂制备的,但是,因为存在少量共聚合较高烯烃(尤其是4-10个碳原子的烯烃),因此其密度低于HDPE,而聚合分子单元的排列是线性类型。
在本发明范围内也打算使用含有其它共聚单体例如丙烯酸、甲基丙烯酸甲酯、丙烯酸烷基酯、乙烯基酯和一氧化碳的乙烯聚合物。这些含有氧原子类型的单体要使用自由基引发剂,但是当使用配位催化剂时不是很合适。配位催化剂一般含有金属-碳键,通常是有毒的或大量使用在共聚合中时被含有氧-碳键或氢-氧键化合物失活。另一方面,乙烯与较高烯烃的共聚合最好是使用配位催化剂进行。
在本发明中,优选的是乙烯聚合物为各种LLDPE,尤其是具有熔体流动指数在大约0.1-10范围和足够的共聚单体单元以得到大约0.9-0.935g/cc密度范围的那些聚合物,这种共聚单体单元是4-8个碳原子的脂族烃烯烃,包括在该范围中的异构体。这些LLDPE聚合物如落镖冲击和埃尔曼多夫撕裂所示的,在现有技术中被公认为具有极佳的强度、抗蔓延撕裂强度,并且当压抵着具有突起的制品时呈现良好的抗撕裂或抗穿孔性。此性能对于食品包装应用,最特别的是在鲜肉包装中的各种LLDPE是特别重要的。
本发明的抗雾薄膜是用生产薄膜的配制剂制备的,该配制剂包括在其中掺入A-B双嵌段共聚物抗雾剂的聚烯烃。这些共聚物具有以下的结构
CH3CH2(CH2CH2)aCH2CH2(OCH2CH2)bOH
其中a为9-25,b为1-10。优选的是组合物含有A-B双嵌段化合物,其中a是13,b是2.5。对于指数a和b这些数值是平均值。
本发明的聚合物配制剂优选包括大约0.1%-4%范围,更优选0.5%-3%范围的抗雾剂,基于配制剂的总重量。
此组合物可含有其它已知抗雾添加剂,例如烷氧基醚,例如Atmer502、脱水山梨糖醇酯,例如Atmer103、其它已知的如在前述美国专利中所揭示的非离子、阴离子和阳离子表面活性剂,例如聚氧化烯脂肪酸酯、烷氧基酚、混合的单、双或三甘油酯、多羟基醇的脂肪酸酯、其它聚烷氧基化的化合物,等等。Atmer是ICI美国商标。
2001年1月23日申请的PCT申请PCT/EP01/00694在此引作参考,揭示了用于食品保护的塑料薄膜,包括紫外线吸收剂。本发明具有抗雾性的聚烯烃薄膜也可进一步含有适宜的添加剂例如紫外线吸收剂、受阻胺光线稳定剂、抗氧化剂、加工助剂和如在PCT申请PCT/EP01/00694中揭示的其它添加剂。
例如,本发明的组合物也可选择含有大约0.01-10%,优选大约0.025-5%,并尤其是大约0.1-3%重量的各种常规稳定剂共添加剂,例如以下所列的材料或其混合物。
1.抗氧化剂
1.1烷基化单酚,例如
2,6-二-叔丁基-4-甲基酚
2-叔丁基-4,6-二甲基酚
2,6-二-叔丁基-4-乙基酚
2,6-二-叔丁基-4-正丁基酚
2,6-二-叔丁基-4-异丁基酚
2,6-二-环戊基-4-甲基酚
2-(α-甲基环己基)-4,6-二甲基酚
2,6-二-十八烷基-4-甲基酚
2,4,6-三-环己基酚
2,6-二-叔丁基-4-甲氧甲基酚
1.2烷基化氢醌,例如
2,6-二-叔丁基-4-甲氧基酚
2,5-二-叔丁基-氢醌
2,5-二-叔戊基-氢醌
2,6-二苯基-4-十八烷基羟基酚
1.3羟基化硫代二苯基醚,例如
2,2’-硫代-双-(6-叔丁基-4-甲基酚)
2,2’-硫代-双-(4-辛基酚)
4,4’-硫代-双-(6-叔丁基-3-甲基酚)
4,4’-硫代-双-(6-叔丁基2-甲基酚)
1.4亚烷基双酚,例如
2,2’-亚甲基-双-(6-叔丁基-4-甲基酚)
2,2’-亚甲基-双-(6-叔丁基-4-乙基酚)
2,2’-亚甲基-双-(4-甲基-6-(α-甲基环己基)-酚)
2,2’-亚甲基-双-(4-甲基-6-环己基酚)
2,2’-亚甲基-双-(6-壬基-4-甲基酚)
2,2’-亚甲基-双-[6-(α-甲基苄基)-4-壬基酚]
2,2’-亚甲基-双-[6-(α,α-二甲基苄基)-4-壬基酚]
2,2’-亚甲基-双-(4,6-二叔丁基酚)
2,2’-亚乙基-双-(4,6-二叔丁基酚)
2,2’-亚乙基-双-(6-叔丁基-4-异丁基酚)
4,4’-亚甲基-双-(2,6-二叔丁基酚)
4,4’-亚甲基-双-(6-叔丁基-2-甲基酚)
1,1-双-(5-叔丁基-4-羟基-2-甲基苯基)丁烷
2,6-二-(3-叔丁基5-甲基-2-羟苄基)-4-甲基酚
1,1,3-三-(5-叔丁基-4-羟基2-甲基苯基)-丁烷
1,1-二-(5-叔丁基-4-羟基-2-甲基苯基)-3-正十二烷基巯基丁烷
1,2-亚乙基二醇双-[3,3-双-(3’-叔丁基-4’-羟苯基)-丁烷]
二-(3-叔丁基-4-羟基-5-甲基苯基)-二环戊二烯
二-[2-(3’-叔丁基2’-羟基-5’-甲基苄基)-6-叔丁基-4-甲基苯基]对苯二酸酯
1.5苄基化合物,例如
1,3,5-三-(3,5-二叔丁基-4-羟基苄基)-2,4,6-三甲基苯
二-(3,5-二叔丁基-4-羟基苄基)硫醚
3,5-二叔丁基-4-羟基苄基-巯基-乙酸异辛基酯
双-(4-叔丁基-3-羟基-2,6-二甲基苄基)二硫酚对苯二酸酯
1,3,5-三-(3,5-二叔丁基-4-羟基苄基)异氰脲酸酯
1,3,5-三-(4-叔丁基-3-羟基-2,6-二甲基苄基)异氰脲酸酯
3,5-二叔丁基-4-羟基苄基-磷酸二(十八烷基酯)
3,5-二叔丁基-4-羟基苄基-磷酸单乙基酯,钙盐
1.6酰胺基酚,例如
4-羟基-月桂酸苯胺
4-羟基-硬脂酸苯胺
2,4-双-辛基巯基-6-(3,5-叔丁基-4-羟基苯胺基)-对称-三嗪
辛基-N-(3,5-二叔丁基-4-羟基苯基)-氨基甲酸酯
1.7β-(3,5-二叔丁基-4-羟基苯基)-丙酸与一元或多元醇的酯,例如
甲醇 二甘醇
十八碳醇 三甘醇
1,6-己二醇 季戊四醇
新戊二醇 三-羟乙基异氰脲酸酯
硫代二甘醇 二-羟乙基草酸二酰胺
三乙醇胺 三异丙醇胺
1.8 β-(5-叔丁基-4-羟基-3-甲基苯基)-丙酸与一元或多元醇的酯,例如
甲醇 二甘醇
十八碳醇 三甘醇
1,6-己二醇 季戊四醇
新戊二醇 三-羟乙基异氰脲酸酯
硫代二甘醇 二-羟乙基草酸二酰胺
三乙醇胺 三异丙醇胺
1.9 β-(3.5-二-叔丁基-4-羟基苯基)-丙酸的酰胺例如,
N,N’-二-(3,5-二-叔丁基-4-羟基苯基丙基)-六亚甲基二胺
N,N’-二-(3,5-二-叔丁基-4-羟基苯基丙基)-三亚甲基二胺
N,N’-二-(3,5-二-叔丁基-4-羟基苯基丙基)-肼
2.UV吸收剂和光线稳定剂
2.1.2-(2’-羟基苯基)-苯并***,例如2-(2-羟基5-甲基苯基)-2H-苯并***、2-(3,5-二叔丁基-2-羟基苯基)-2H-苯并***、2-(2-羟基-5-叔丁基苯基)-2H-苯并***、2-(2-羟基-5-叔辛基苯基)-2H-苯并***、5-氯-2-(3,5-二叔丁基-2-羟基苯基)-2H-苯并***、5-氯-2-(3-叔丁基-2-羟基-5-甲基苯基)-2H-苯并***、2-(3-仲丁基-5-叔丁基-2-羟基苯基)-2H-苯并***、2-(2-羟基-4-辛基羟苯基)-2H-苯并***、2-(3,5-二叔戊基-2-羟基苯基)-2H-苯并***、2-(3,5-双-α-枯基-2-羟基苯基)-2H-苯并***、2-(3-叔丁基-2-羟基-5-(2-(ω-羟基-八-(乙氧基)羰基-乙基)-苯基)-2H-苯并***、2-(3-十二烷基-2-羟基-5-甲基苯基)-2H-苯并***、2-(3-叔丁基-2-羟基-5-(2-辛基氧代羰基)乙基苯基)-2H-苯并***、十二烷基化2-(2-羟基-5-甲基苯基)-2H-苯并***、2-(3-叔丁基-2-羟基-5-(2-辛基氧代羰基乙基)苯基)-5-氯-2H-苯并***、2-(3-叔丁基-5-(2-(2-乙基己基氧代)-羰基乙基)-2-羟基苯基)-5-氯-2H-苯并***、2-(3-叔丁基-2-羟基-5-(2-甲氧基羰基乙基)苯基)-5-氯-2H-苯并***、2-(3-叔丁基-2-羟基-5-(2-甲氧基羰基乙基)苯基)-2H-苯并***、2-(3-叔丁基-5-(2-(2-乙基己基氧代)羰基乙基)-2-羟基苯基)-2H-苯并***、2-(3-叔丁基-2-羟基5-(2-异辛基氧代羰基乙基)苯基)-2H-苯并***、2,2’-亚甲基-双(4-叔辛基-6-2H-苯并***-2-基-酚)、2-(2-羟基-3-α-枯基-5-叔辛基苯基)-2H-苯并***、2-(2-羟基-3-叔辛基-5-α-枯基苯基)-2H-苯并***、5-氟-2-(2-羟基-3,5-二-α-枯基苯基)-2H-苯并***、5-氯-2-(2-羟基-3,5-二-α-枯基苯基)-2H-苯并***、5-氯-2-(2-羟基-3-α-枯基-5-叔辛基苯基)-2H-苯并***、2-(3-叔丁基-2-羟基-5-(2-异辛基氧代羰基乙基)苯基)-5-氯-2H-苯并***、5-三氟甲基-2-(2-羟基-3-α-枯基-5-叔辛基苯基)-2H-苯并***、5-三氟甲基-2-(2-羟基-5-叔辛基苯基)-2H-苯并***、5-三氟甲基-2-(2-羟基-3,5-二叔辛基苯基)-2H-苯并***、甲基3-(5-三氟甲基-2H-苯并***-2-基)-5-叔丁基-4-羟基氢化肉桂酸酯、5-丁基磺酰基-2-(2-羟基-3-α-枯基-5-叔辛基苯基)-2H-苯并***、5-三氟甲基2-(2-羟基-3-α-枯基5-叔丁基苯基)-2H-苯并***、5-三氟甲基-2-(2-羟基-3,5-二-叔丁基苯基)-2H-苯并***、5-三氟甲基-2-(2-羟基-3,5-二-α-枯基苯基)-2H-苯并***、5-丁基磺酰基-2-(2-羟基-3,5-二叔丁基苯基)-2H-苯并***和5-苯基磺酰基-2-(2-羟基-3,5-二-叔丁基苯基)-2H-苯并***。
2.2 2-羟基-二笨酮,例如,4-羟基-、4-甲氧基、4-辛氧基-、4-癸氧基-、4-十二烷氧基-、4-苄氧基、4,2’,4’-三羟基-和2’-羟基-4,4’-二甲氧基衍生物。
2.3可任选被取代的苯甲酸的酯,例如,苯基水杨酸酯、4-叔丁基苯基水杨酸酯、辛基苯基水杨酸酯、二苯甲酰基间苯二酚、双-(4-叔丁基-苯甲酰基)-间苯二酚、苯甲酰基间苯二酚、3,5-二-叔丁基-4-羟基苯甲酸2,4-二-叔丁基苯基酯和3,5二-叔丁基-4-羟基苯甲酸十六烷基酯。
2.4丙烯酸酯和丙二酸酯,例如,α-氰基-β,β-二苯基丙烯酸乙基酯或异辛基酯、α-甲酯基-肉桂酸甲基酯、α-氰基-β-甲基-p-甲氧基肉桂酸甲基酯或丁基酯、α-甲酯基-p-甲氧基肉桂酸甲基酯、N-(β-甲酯基-β-氰基乙烯基)-2-甲基-二氢吲哚、SanduvorPR25和PR31。
2.5空间位阻胺,例如,双-(2,2,6,6-四甲基哌啶基)癸二酸酯、双-(1,2,2,6,6-五甲基哌啶基)癸二酸酯、正-丁基-3,5-二-叔丁基-4-羟基苄基丙二酸双-(1,2,2,6,6-五甲基哌啶基)酯、1-羟基乙基-2,2,6,6-四甲基-4-羟基哌啶与琥珀酸的缩聚产物、N,N’-(2,2,6,6-四甲基哌啶基)-六甲基二胺与4-叔辛基氨-2,6-二氯-s-三嗪的缩聚产物、三-(2,2,6,6-四甲基哌啶基)-次氮基三乙酸酯、四重-(2,2,6,6-四甲基-4-哌啶基)1,2,3,4-丁烷四羧酸酯、1,1’(1,2-乙烷联基)-双-(3,3,5,5-四甲基哌嗪酮)、双(1-辛氧基-2,2,6,6-四甲基哌啶-4-基)癸二酸酯。
2.6在N-原子上由羟基取代的烷氧基取代的空间位阻胺,例如,在共同申请的No.09/257711中揭示的化合物,其相关部分也在此引作参考,例如1-(2-羟基-2-甲基丙氧基)-4-十八烷酰基氧代-2,2,6,6-四甲基哌啶、1-(2-羟基2-甲基丙氧基)-4-羟基-2,2,6,6-四甲基哌啶、1-(2-羟基-2-甲基丙氧基)-4-氧代-2,2,6,6-四甲基哌啶、双(1-(2-羟基-2-甲基丙氧基)-2,2,6,6-四甲基哌啶-4-基)癸二酸酯、双(1-(2-羟基-2-甲基丙氧基)-2,2,6,6-四甲基哌啶-4-基)己二酸酯、双(1-(2羟基2-甲基丙氧基)-2,2,6,6-四甲基哌啶-4-基)琥珀酸酯、双(1-(2-羟基-2-甲基丙氧基)-2,2,6,6-四甲基哌啶-4-基)戊二酸酯和2,4-双{N-[1-(2-羟基-2-甲基丙氧基)-2,2,6,6-四甲基哌啶-4-基]-N-丁基氨}-6-(2-羟乙基氨)-s-三嗪。
2.7草酸二酰胺,例如,4,4’-二-辛氧基-N,N’-草酰二苯胺、2,2'-二-辛氧基-5,5’-二-叔丁基-N,N’-草酰二苯胺、2,2’-二-十二烷氧基5,5’-二-叔丁基-N,N’-草酰二苯胺、2-乙氧基-2’-乙基-N,N’-草酰二苯胺、N,N’-双(3-二甲基氨基丙基)-N,N’-草酰二苯胺、2-乙氧基-5-叔丁基-2’-乙基N,N’-草酰二苯胺和其与2-乙氧基-2’-乙基-5,4’-二-叔丁基N,N’-草酰二苯胺的混合物和邻位-与对位-甲氧基-以及o-或p-乙氧基-双取代的N,N'-草酰二苯胺的混合物。
2.8羟基苯基-s-三嗪,例如,4,6-双-(2,4-二甲基苯基)-2-(2-羟基-4-辛基氧代苯基)-s-三嗪、Cyasorb1164,Cytec Corp.、4,6-双-(2,4-二甲基苯基)-2-(2,4-二羟基氧代苯基)-s-三嗪、2,4-双-(2,4-二羟基苯基)-6-(4-氯苯基)-s-三嗪、2,4-双[2-羟基-4-(2-羟基乙氧基)苯基]-6-(4氯苯基)-s-三嗪、2,4-双[2-羟基-4-(2-羟基-4-(2-羟基乙氧基)苯基]-6-(2,4-二甲基苯基)-s-三嗪、2,4-双[2-羟基-4-(2-羟基乙氧基)苯基]-6-(4-溴苯基)-s-三嗪、2,4-双[2-羟基-4-(2-乙酸基乙氧基)苯基]-6-(4-氯苯基)-s-三嗪、2,4-双(2,4-二羟基苯基)-6-(2,4-二甲基苯基)-s-三嗪、2,4-双(4-联苯基)-6-(2-羟基-4-辛基氧代羰基亚乙基氧代苯基)-s-三嗪、2-苯基-4-[2-羟基-4-(3-仲丁基氧基-2-羟基丙氧基)苯基]-6-[2-羟基-4-(3-仲戊基氧基-2-羟基丙氧基)苯基]-s-三嗪、2,4-双(2,4-二甲基苯基)-6-[2-羟基-4-(3-苄氧基-2-羟基丙氧基)苯基]-S-三嗪、2,4-双(2-羟基-4-正丁基苯基)-6-(2,4-二-正丁氧基苯基]-s-三嗪、2,4-双(2,4-二甲基苯基)-6-[2-羟基-4-(3-壬氧基*-2-羟基丙氧基)-5-α-枯基苯基]-s-三嗪(*表示辛氧基、壬氧基和十二烷氧基的混合物)、亚甲基双-{2,4-双(2,4-二甲基苯基)-6-[2-羟基-4-(3-丁氧基-2羟基丙氧基)苯基]-s-三嗪}、在3∶5’、5∶5’和3∶3’位置以5∶4∶1的比例桥联的亚甲基桥基二聚物混合物、2,4,6-三(2-羟基-4-异丁氧基羰基异亚丙氧基苯基)-s-三嗪、2,4-双(2,4-二甲基苯基)-6-(2-羟基-4-己氧基-5-α-枯基苯基)-s-三嗪、2-(2,4,6-三甲基苯基)4,6-双[2-羟基-4-(3-丁氧基-2-羟基丙氧基)苯基]-s-三嗪、2,4,6-三(2-羟基-4-(3-仲丁氧基-2羟基丙氧基)苯基]-s-三嗪、4,6-双-(2,4-二甲基苯基)-2-(2-羟基-4-(3-十二烷氧基-2-羟基丙氧基)-苯基)-s-三嗪和4,6-双-(2,4-二甲基苯基)-2-(2-羟基-4-(3-十三烷氧基-2-羟基丙氧基)-苯基)-s-三嗪的混合物。Tinuvin400,Ciba Specialty Chemicals Corp.、4,6-双-(2,4-二甲基苯基)-2-(2-羟基-4-(3-(2-乙基己氧基)-2-羟基丙氧基)-苯基)-s-三嗪和4,6-二苯基-2-(4-己氧基-2-羟基丙氧基)-苯基)-s-三嗪。
3.亚磷酸酯和亚膦酸酯,例如,三苯基亚磷酸酯、二苯烷基亚磷酸酯、苯基二烷基亚磷酸酯、三-(壬基苯基)亚磷酸酯、三月桂基亚磷酸酯、三-十八烷基亚磷酸酯、二-硬脂基-季戊四醇二亚磷酸酯、三-(2,4-二-叔丁基苯基)亚磷酸酯、二异癸基季戊四醇二亚磷酸酯、二-(2,4,6-三-叔丁基苯基)-季戊四醇二亚磷酸酯、二-(2,4-二-叔丁基-6-甲基苯基)-季戊四醇二亚磷酸酯、二-(2,4-二-叔丁基苯基)-季戊四醇二亚磷酸酯、三硬脂基-山梨糖醇三亚磷酸酯、四-(2,4-二-叔丁基苯基)-4,4’-二亚苯基二亚膦酸酯。
4.破坏过氧化物的化合物,例如,β-硫代二丙酸的酯,例如,月桂基、硬脂基、肉豆蔻基或十三烷基酯、巯基苯并咪唑或2-巯基苯并咪唑的锌盐、二丁基二硫代氨基甲酸锌、二(十八烷基)二硫醚、季戊四醇四-(β-十二烷基巯基)-丙酸酯。
5.羟基胺,例如,N,N-二苄基羟基胺、N,N-二乙基羟基胺、N,N-二辛基羟基胺、N,N-二月桂基羟基胺、N,N-双十四烷基羟基胺、N,N-双十六烷基羟基胺、N,N-双十八烷基羟基胺、N-十六烷基-N-十八烷基-羟基胺、N-十七烷基-N-十八烷基-羟基胺、由氢化的牛脂胺衍生的N,N-二烷基羟基胺。
6.硝酮,例如,N-苄基-α-苯基硝酮、N-乙基-α-甲基硝酮、N-辛基-α-庚基硝酮、N-月桂基-α-十一烷基硝酮、N-十四烷基-α-十三烷基硝酮、N-十六烷基-α-十五烷基硝酮、N-十八烷基-α-十七烷基硝酮、N-十六烷基-α-十七烷基硝酮、N-十八烷基-α-十五烷基硝酮、N-十七烷基-α-十七烷基硝酮、N-十八烷基-α-十六烷基硝酮、由氢化的牛脂胺衍生的N,N-二烷基羟基胺衍生的硝酮、
7.氧化胺,例如,在美国专利5844029和5880191中所揭示的氧化胺衍生物、十二烷基甲基氧化胺、十三烷基氧化胺、三(十二烷基)氧化胺和三(十六烷基)氧化胺。
8.聚酰胺稳定剂,例如,与碘化物和/或磷化合物结合的铜盐和二价锰的盐。
9.碱性共稳定剂,例如,蜜胺、聚乙烯吡咯烷酮、双氰胺、三烯丙基氰尿酯、脲衍生物、肼衍生物、胺、聚酰胺、聚氨酯、高脂肪酸的碱金属盐和碱土金属盐例如硬脂酸钙、硬脂酸锌、硬脂酸镁、蓖麻醇酸钠和棕榈酸钾、焦邻苯二酚锑或焦邻苯二酚锌。
10.成核剂,例如,无机物例如滑石、金属氧化物例如二氧化钛或氧化镁、或优选碱土金属的磷酸盐、碳酸盐或硫酸盐;有机化合物例如一或多羧酸及其盐,例如4-叔丁基-苯甲酸、己二酸、二苯基乙酸、琥珀酸钠或苯甲酸钠;聚合物化合物例如离子共聚物(离聚物)。
11.填料和增强剂,例如,碳酸钙、硅酸钙、玻璃纤维、石棉、滑石、高岭土、云母、硫酸钡、金属氧化物和氢氧化物、碳黑、石墨。
12.其它添加剂,例如,增塑剂、润滑剂、乳化剂、颜料、流变学添加剂、催化剂、流动控制剂、荧光增白剂、澄清剂例如取代的和未取代的二亚苄基山梨糖醇、阻燃剂、抗静电剂、发泡剂和硫代协合剂例如二月桂基硫代二丙酸酯或二硬脂酸硫代二丙酸酯。
13.苯并呋喃酮和二氢吲哚酮,例如,在美国专利US4325863、US4338244或US5175312中所揭示的那些,或3-[4-(2-乙酸基乙氧基)苯基]-5,7-二-叔丁基苯并呋喃-2-酮、5,7-二-叔丁基3-[4-(2-硬脂酰氧基乙氧基)苯基]苯并呋喃-2-酮、3,3’-双[-5,7-二-叔丁基-3-(4-[2-羟基乙氧基]苯基]苯并呋喃-2-酮]、5,7-二-叔丁基-3-(4-乙氧基苯基)苯并呋喃-2-酮、3-(4-乙酸基-3,5-二甲基苯基)-5,7-二-叔丁基-苯并呋喃-2-酮、3-(3,5-二甲基-4-新戊酰氧基苯基)-5,7-二-叔丁基苯并呋喃-2-酮。
14.镍化合物,例如,2,2’-硫代-双-[4-(1,1,3,3-四甲基丁基)苯酚]的镍络合物,例如1∶1或1∶2络合物,带有或不带有附加的配位体例如正丁胺、三乙醇胺或N-环己基二乙醇胺,二丁基二硫代氨基甲酸镍、4-羟基-3,5-二-叔丁基苄基膦酸的一烷基酯的镍盐,例如甲基或乙基酯的镍盐,酮肟的镍络合物,例如2-羟基-4-甲基苯基十一酮肟的镍络合物,1-苯基-4-月桂酰-5-羟基吡唑的镍络合物,带有或不带有附加的配位体。
将抗雾剂的混合物加入聚烯烃是通过常规使用的技术,例如辊炼,在班伯里密炼机中混合或在挤出机料筒中混合等等,将其混入到熔体聚合物中。加热历程(维持高温的时间)可通过混入抗雾剂和未加热聚合物颗粒而缩短从而实现抗雾剂在聚合物中基本上均匀分布,从而减少在熔融温度充分混合所需时间。
按照常规,抗雾剂也可以基本上同时或顺序地与任何其它添加剂(着色剂、增粘剂、增滑剂、封端剂、等等)加入,这些添加剂是在某些情况下所需要的。抗雾剂也可与其它添加剂预混合,然后将该混合体加入聚合物。在某些情况下设想这些抗雾剂具有辅助其它添加剂更容易或更均匀分散或溶解在聚烯烃中的额外的优点。为了更易于控制分批的质量,优选应用聚合物/抗雾剂混合母料,其随后作为一部分混入另外的聚合物中实现最终所希望的配方。该母料,或纯净的添加剂可被注入新近制备的聚合物中而该聚合物在离开聚合釜或一组聚合釜之后仍为熔融体,在将熔融体聚合物冷却固化或进一步加工之前使其混合。在本发明范围之内使用混合物或烯烃聚合物合金,不管它们是上述的LDPE、LLDPE、HDPE还是用自由基引发剂或配位催化剂制备的其它烯烃聚合物或共聚物。聚丙烯是用配位催化剂制备的烯烃聚合物之一例(例如,熟知的齐格勒或纳塔催化剂或其变体)其固有地显示比聚乙烯低的密度。
本领域众所周知聚丁烯或聚异丁烯当与聚乙烯混合时是有效的增粘剂或粘接剂。在包装工序中,在某些情况下良好的粘接性能是所希望的,其中预料薄膜自身粘接直至被拉开或直至被热密封,视情况而定。通常用于此目的的聚丁烯或聚异丁烯的用量一般很少只占总重量很小的百分比,它们常常是低分子量或相对低的分子量,重均分子量在几百至几千的范围。这种增粘剂的使用在本发明范围内某些预期的配方中是优选的,尤其是在肉食(等等)的包装方面是所希望的,在包装操作过程中直至热密封,或在运输、储存,和热密封之后的加工过程中其基本上不会出现液体泄漏。
聚烯烃薄膜的制造是众所周知的,包括流延薄膜技术(作为薄片穿过窄缝形模头),和吹塑薄膜技术,其中挤出的管状熔融聚合物在被冷却和收集或进一步加工之前被膨胀到希望的“膜泡”直径和-或薄膜厚度。目前的这些配方也适宜共挤出生产薄膜,其中两层或多层薄膜含有多层结构。本发明的抗雾剂可透过不含抗雾剂的相邻薄膜层渗出,从而使相邻层抗雾。
在优选的情况下,本发明包括一种聚烯烃树脂和添加剂的组合物形成适用于鲜肉包装的薄膜。聚烯烃树脂具有此市场所要求的所需要的强度、光学性能和透气性能。然而它们没有防止在低温包装中形成水滴所需的吸湿性。为了解决吸湿问题,将通常在增塑的PVC薄膜中使用的抗雾剂(例如单-和二脂酰甘油脂)尝试用于聚烯烃树脂。这些添加剂在聚烯烃树脂中不象在增塑的PVC薄膜中那样有效。聚烯烃薄膜中没有增塑剂可能成为所观察到的抗雾剂性能差别原因之一。抗雾剂必须能渗到薄膜可起作用的表面,而不磨损薄膜表面。可从薄膜表面用水容易地除去或擦掉的抗雾剂是不理想的因为该抗雾剂将会使肉食串味,而且该薄膜也将不抗雾。因此本发明包括一种聚烯烃树脂和有效量的抗雾剂的独特组合物,该抗雾剂不易从薄膜表面擦掉。这种聚烯烃树脂和抗雾剂的混合物的用途可以用在食品包装(肉食、蔬菜,等等)、温室薄膜,或其它需要透明薄膜具有吸湿性或无雾的应用中。
本发明不同于广泛使用的PVC鲜肉包装和生产包装纸,即基本树脂是聚烯烃而不是聚氯乙烯树脂。聚烯烃树脂的优点是不需要象PVC薄膜所需要和使用的增塑剂(例如对苯二甲酸二辛酯)。抗雾剂在两种不同类别的树脂中作用不同。由于PVC薄膜中存在的增塑剂,抗雾剂不易于从薄膜表面洗掉。因此,不是所有能在增塑PVC薄膜中应用的抗雾剂都能用于聚烯烃薄膜。
还有,本发明在树脂内掺入抗雾剂而不是将其作为涂层应用。在树脂中掺入添加剂价格不贵,劳动强度不大,比施于薄膜表面的涂层更坚固。因此,本发明应用抗雾剂,甚至薄膜已经经历了磨损时也维持了其在薄膜表面的抗雾性能。这在食品产品的包装过程中是重要的从而防止食品产品吸收抗雾剂又保持了包装薄膜的吸湿性。
此外,本发明可使抗雾剂掺入树脂,该树脂用一般技术不需要附加处理制成薄膜。不需要辐射或热老化来使抗雾剂渗出到薄膜的表面并在那里起作用。在生产之后大约48小时之内抗雾剂渗出到薄膜表面。
本发明的具有抗雾性能的烯烃薄膜用于温室薄膜和用于食品包装应用是有利的。
以下的例子说明一些特殊的实施方案,本发明不受这些特例的限制。
例1
为了评价所要求保护的化合物在LDPE薄膜中的抗雾性能,按照以下程序将其掺入该聚合物。为了得到含有每种化合物1、1.5或2%的配方,将每种化合物称重适宜的量加入LDPE粒料中(Riblene FF29,由Polimeri Europa Milan,Italy提供),该颗粒料的特征在于密度为0.921g/cm3和熔体流动指数(190℃,2.16kg)为0.6,将如此得到的颗粒在半工业Dolci吹塑挤出机中以最高210℃的温度吹塑得到150μm厚的薄膜。
抗雾测试方法
根据热雾测试方法评价薄膜:250ml玻璃烧杯,其中含有50ml水并用要评价的薄膜覆盖,将其高度的大约1/2浸入60℃的水浴中。从试验开始以限定的间隔观察薄膜,确定A-E的范围作常规标记。结果列于表1。
热雾测试标定值
说明 性能 标定值 评定
小雾滴不透明层 无 A 零能见度,透光性差
大雾滴不透明层 无 B 零能见度,透光性差完全是大的雾滴构成的层 差 C 能见度差,镜片效果
透明液滴无规分散的大的透明液滴 中等 D 不连续的水膜几乎没有小的或大的透明液滴 好 D/E 水的盘、膜,基本上透明透明薄膜显示无可见水 极佳 E 完全透明
表1添加剂 分子量 a b 在D/E热雾测试中的小时
数
无 - - - (恒定的B/C比值)1%Atmer103 430 - - 5001%98-0218 575 13 2.5 6501%98-0216 875 23 4 11001.5%Atmer502 344 7 2 3501.5%98-0218 575 13 2.5 19502%Atmer103 430 - - 7502%98-0218 575 13 2.5 24002%98-0216 875 23 4 1500
添加剂具有如下分子式CH3CH2(CHCH2)aCH2CH2(OCH2CH2)bOH,指数a和b表示此分子式中a、b的平均值。
D/E的抗雾比值小时数高是所希望的。可以看出本发明的抗雾添加剂提供了优良的长期持续结果。
例2
重复例1得到含有1或2%重量表2的添加剂的配方,由此得到大约75μm的薄膜。
根据例1中所述的热雾测试方法评价其薄膜。结果示于下表
表2
添加剂 分子量 a b 在D/E热雾测试中的小时
数1%Atmer103 430 - - 1751%98-0218 575 13 2.5 11001%98-0216 875 23 4 3501%98-0222 920 13 10.5 1501%98-0224 1100 18 12.5 502%Atmer103 430 - - 2002%98-0218 575 13 2.5 1200
添加剂具有如下分子式CH3CH2(CH2CH2)aCH2CH2(OCH2CH2)bOH,指数a和b表示此分子式中a、b的平均值。
D/E的抗雾比值小时数高是所希望的。可以看出本发明的抗雾添加剂提供了优良的长期持续结果。
Claims (6)
1.一种抗雾聚烯烃薄膜组合物,包括
(a)聚烯烃薄膜,和
(b)分子式为CH3CH2(CH2CH2)aCH2CH2(OCH2CH2)bOH的化合物,其中a为9-25,b为1-10。
2.根据权利要求1的组合物,其中聚烯烃是聚乙烯。
3.根据权利要求1的组合物,其中组分(b)是分子式为CH2CH2(CH2)13CH2CH2(OCH2CH2)2.5OH的化合物。
4.根据权利要求1的组合物,其中聚烯烃薄膜是温室薄膜。
5.根据权利要求1的组合物,其中聚烯烃薄膜是食品包装薄膜。
6.根据权利要求1的组合物作为鲜肉包装的用途。
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JP2005538200A (ja) * | 2002-09-06 | 2005-12-15 | チバ スペシャルティ ケミカルズ ホールディング インコーポレーテッド | 永続的な防霧性、防靄性及び防曇性を有するフィルム組成物 |
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KR20010102933A (ko) | 2001-11-17 |
US20010047046A1 (en) | 2001-11-29 |
US20040234801A1 (en) | 2004-11-25 |
JP2002012712A (ja) | 2002-01-15 |
EP1152027A1 (en) | 2001-11-07 |
BR0101691A (pt) | 2001-12-18 |
BR0101691B1 (pt) | 2010-09-21 |
DE60105484D1 (de) | 2004-10-21 |
CN1171938C (zh) | 2004-10-20 |
MX235508B (es) | 2006-04-05 |
EP1152027B1 (en) | 2004-09-15 |
US7037964B2 (en) | 2006-05-02 |
US6784235B2 (en) | 2004-08-31 |
DE60105484T2 (de) | 2005-10-13 |
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AR035997A1 (es) | 2004-08-04 |
CA2346198C (en) | 2009-12-22 |
TWI293974B (en) | 2008-03-01 |
KR100716601B1 (ko) | 2007-05-10 |
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