CN1088227A - 可光降解的聚烯烃组合物 - Google Patents
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Abstract
本发明涉及可光降解聚烯烃组合物,它包括:
(A)80—99.9%(重量)的聚烯烃树脂;(B)0.01—
20%(重量)的至少一种选自改性离子型聚乙烯、用
烃属不饱和环酐接枝的聚烯烃和氧化聚乙烯的其它
聚合物;以及可选择性加入的(C)0.10重量份或更少
些的光敏剂,基于100份组分(A)和(B)的总和。
Description
本发明涉及可光降解的聚烯烃组合物;而且特别涉及含有聚烯烃树脂、可光降解的聚合组分及可选择地加入的光敏剂的可光降解的聚烯烃组合物。
聚烯烃树脂,特别是聚乙烯已被应用于各种用途,例如用于制造购物袋和农用薄膜。但是,由于树脂是非极性的聚合物,丢弃后长时间仍不能自行腐烂,因而引起了环境问题。
所以,人们已做了各种努力来开发可降解的塑料。但是,直到最近,这些努力主要是针对低密度聚乙烯(LDPE)的,因为LDPE比高密度聚乙烯更容易降解。因此,近来所做的研究旨在使较高密度的聚乙烯具有可降解性。
现有技术的方法通常针对合成一种聚合物,在它的主链中含有羰基;或者通过掺混可降解的聚合物和非降解的聚合物使之具有可降解性;或者通过将光降解促进剂掺入聚合物来提供可降解性。
制备含有羰基的聚合物的方法,例如乙烯和一氧化碳共聚物已在美国专利2495286;3676401;3853814等中有所披露。如此制得的聚乙烯薄膜,当暴露于太阳光的紫外光时将由于Norish-Ⅰ或Ⅱ降解机理而被降解。然而,为了制备这种薄膜,该方法需要昂贵的设备和材料。
美国专利3860538披露了一种使聚烯烃,例如聚乙烯和聚苯乙烯,具有可光降解性的方法,即用具有羰基的酮共聚物与聚烯烃掺混。但是,这种方法也需要相当高的生产成本而得到略有降解性的薄膜。
另外,英国专利1,356,107和美国专利3,880,952;3,888,804;4,028,480;4,121,025;4,191,320;4,461,853;4,519,161也描述了使聚烯烃树脂具有可降解性的类似方法,它包括将作为光敏剂的含过渡金属的化合物或芳香酮化合物加入树脂中。但是,这些方法存在各种问题:在降解过程中由于释放添加剂中的重金属而引起污染问题;由于所用的添加剂的性质造成的聚烯烃薄膜的着色;以及当这种树脂用作食物容器时由于芳香酮化合物所产生的健康问题。
因此,本发明的主要目的是开发可降解的聚烯烃组合物,该组合物用于以低成本制备具有良好的可光降解性、物理性能、可加工性、可印刷性以及透明的聚烯烃薄膜。
根据本发明,所提供的可降解的聚烯烃组合物包括:
(A)80-99.9%(重量)的聚烯烃树脂;和
(B)0.01-20%(重量)的至少一种选自改性的离子型聚乙烯、用烯属不饱和环酐接枝的聚烯烃、和氧化聚乙烯的另一种聚合物,以及可选择地加入的
(C)0.10份(重量)或更少些的光敏剂,以100份组分(A)和(B)的总和计。
可用作本发明组分(A)的典型的聚烯烃包括聚乙烯、聚丙烯、乙烯-乙酸乙烯酯共聚物等。优选熔融指数为0.01-8.0克/10分钟,更优选为0.03-6.0克/10分钟的聚乙烯树脂,按ASTM D-1238方法测定;优选比重为0.917-0.961克/厘米3,更优选为0.919-0.951克/厘米3,按ASTM D-1505方法测定;且在主链中有0-2个双键。本发明所用的聚丙烯优选具有熔融指数范围为1.4-16克/10分钟,在负荷2160克,230℃温度下测定;比重范围为0.890-0.910克/厘米3;而且可以是乙烯含量范围为2.5-8.5%(重量)的与乙烯的共聚物。乙烯-乙酸乙烯酯共聚物优选具有乙酸乙烯酯含量为3-18%(重量),熔融指数范围为0.3-4克/10分钟,在负荷2160克,190℃温度下测定;比重为0.925-0.943克/厘米3。
聚烯烃树脂的用量范围通常是组合物重量的80-99.9%,优选为93-99.9%。
可用作本发明组分(B)的改性离子型聚乙烯可以是由乙烯和含羧基单体合成的改性聚乙烯共聚物。这里可用的含羧基的单体最好可以是甲基丙烯酸。改性的聚乙烯可用以下方法制备,例如,用乙烯和含羧基的单体,如甲基丙烯酸共聚得到共聚物,然后用金属元素,如钠和锌与共聚物中所含的羧基反应。改性聚乙烯是部分离子型的,因为它的羧基与金属部分成盐。
改性的离子型聚乙烯优选具有熔融指数为1.0-2.6克/10分钟,在负荷2160克,190℃温度下测定;比重范围为0.940-0.950克/厘米3;熔点为81-96℃,用差热分析(DTA)方法测得。改性聚乙烯对诱导降解时间有很大影响,而且可与本发明组分(A)聚烯烃相容。
改性离子型聚乙烯的用量范围为组合物重量的0.01-20%,优选为0.1-7.0%。
可被选为本发明组分(B)的烯属不饱和环酐接枝的聚烯烃可以由聚烯烃,如聚乙烯和聚丙烯和烯属不饱和环酐,如马来酐和邻苯二甲酸酐的溶液或熔融反应来制备;而且优选的熔融指数范围为1-1,300克/10分钟,在负荷为2160克,230℃温度下测定;比重范围为0.757-0.965克/厘米3;接枝率为0.01-10.0%。当暴露在紫外光下时,接枝聚烯烃作为断裂烯烃主链的游离基源。
接技聚烯烃的用量虽然可以随接枝程度而变化,但是当接枝率为5%时,其用量范围为组合物重量的0.1-10%,优选为0.1-4%。
此外,氧化聚乙烯,也可以用作组分(B),它可由用具有至少一个乙烯基的有机酸共聚或改性乙烯或丙烯来制备;优选比重范围为0.98-1.00克/厘米3;Brookfield粘度范围在150℃下为2,500-8,500厘泊;酸值范围为16-41毫克KOH/克。
氧化聚乙烯的用量虽然可随酸值变化,但是当酸值为16时一般用量范围为组合物重量的0.01-10%,优选为0.1-5%。
组分(B)本身可提供足够的光降解效果,而且当它与光敏剂一起使用时还会进一步产生协同效应。
因此,本发明的组合物还可含有作为非必要组分的光敏剂。
光敏剂的典型化合物为铁化合物,可包括乙酰丙酮化铁、二乙基氨荒酸铁、硬脂酸铁、棕榈酸铁,它们可单独或结合使用。光敏剂的用量,基于100份重量的组分(A)和(B)总和为0.10份或更少些,优选为0.005-0.05份。
本发明的可降解聚烯烃组合物可以通过分别或同时混合组分(A)的聚烯烃与组分(B)的其它聚合物以及组分(C)的光敏剂来制备。另一种方法是,每一种添加剂(B)和(C)可以上述比例预先与聚烯烃混合成母料,这些母料再混合生成最终组合物。
混合可以各种方法进行。例如,原料可在如Henschel混合器这样的混料器中干混,然后再在单或双螺杆挤出机中熔融混合,或者在例如Kneader的批料混合器中混合以提供粒料。
使用装有口模的单或双螺杆挤出机将本发明的组合物制成厚度为10-100μm的薄膜以便评价所生成薄膜的光降解性能。
给出下列实施例仅为了说明而不能限制本发明的范围。除非另有说明,以下给出的份数和百分数分别以重量计。
实施例中,本发明组合物所用组分的性能如下:
Ⅰ、聚烯烃树脂
PE(1):密度为0.945克/厘米3和熔融指数为0.19克/10分钟的高密度聚乙烯树脂。
PE(2):密度为0.945克/厘米3和熔融指数为0.10克/10分钟的高密度聚乙烯树脂。
PE(3):密度为0.946克/厘米3和熔融指数为0.62克/10分钟的高密度聚乙烯树脂。
PE(4):密度为0.951克/厘米3和熔融指数为0.03克/10分钟的高密度聚乙烯树脂。
PP(1):密度为0.910克/厘米3和熔融指数为2.0克/10分钟的均聚丙烯树脂。
PP(2):密度为0.910克/厘米3和熔融指数为8.0克/10分钟的均聚丙烯树脂。
EVA(1):乙酸乙烯酯含量为18%(重量),熔融指数为0.3克/10分钟,密度为0.940克/厘米3的乙烯-乙酸乙烯酯共聚物。
EVA(2):乙酸乙烯酯含量为15%(重量),熔融指数为1.7克/10分钟,密度为0.943克/厘米3的乙烯-乙酸乙烯酯共聚物。
Ⅱ、添加剂
Add. 1-1改性离子型聚乙烯,它可通过乙烯和甲基丙烯酸共聚,直到酸含量为15%,然后用钠离子与其中所含的羧基反应使之中和度为34%来制备;具有的熔点为92℃,密度为0.950克/厘米3,熔融指数为2.6克/10分钟。
Add. 1-2改性离子型聚乙烯,它可通过乙烯和甲基丙烯酸共聚,直到酸含量为15%,然后用钠离子与其中所含的羧基反应使之中和度为34%来制备;具有的熔点为95℃,密度为0.940克/厘米3,熔融指数为1.3克/10分。
Add. 2:用马来酐接枝的聚乙烯,通过溶液聚合制备,接枝率为5.0%,密度为0.8072克/厘米3,熔融指数为950克/10分钟。
Add. 3:密度为0.98克/厘米3、Brookfield粘度为8,500厘泊且酸值为16毫克KOH/克的氧化聚乙烯。
Add. 4:由乙酰丙酮和氯化铁的液相反应制备的乙酰丙酮化铁。
实施例1-27
组分PE(1)、Add. 1-1(或Add. 1-2)和Add. 4以表1和2中所示的量混合,然后在双螺杆挤出机中在温度范围为180-200℃和螺杆转数为200-350转/分下熔融掺合,该挤出机在六个位置上有温控。挤出的树脂混合物在冷水浴中冷却并切粒,然后用单螺杆吹塑薄膜机(由Brabender制造,L/D=19/25)在温度为170-200℃下使它们成型为厚度为10-100μm的薄膜。
通过将薄膜暴露于紫外光或户外环境下并测量降解膜的伸长来评价用本发明组合物制备的薄膜的可光降解性。
根据ASTM D-4329,通过在60℃紫外光辐射薄膜4小时,在40℃增湿薄膜4小时,并重复辐射和冷凝多次来进行暴露于紫外线下的薄膜的光降解作用。暴露于户外环境下的薄膜的光降解作用可根据ASTM D-1435进行。按照ASTM D-882在机器方向上测定降解膜的伸长。薄膜的伸长减小的愈多,薄膜的可降解性愈大。
评价结果示于表3中。
比较例1-5
除了不用添加剂1且其它组分按表4所示的量使用外,重复上述实施例所述的同样的步骤。
制得薄膜的评价结果示于表5中。
实施例28-33
除了使用表6所示的组分外,重复上述实施例1-27所述的同样的步骤。
制得薄膜的评价结果示于表7中。
实施例34-36
除了使用表8所示的组分外,重复实施例1-27所述的同样步骤。
制得薄膜的评价结果示于表9中。
实施例37和38
除了使用表10所示的组分外,重复实施例1-27所述的同样步骤。
制得薄膜的评价结果示于表11中。
实施例39-41
除了使用表12所示的组分外,重复实施例1-27所述的同样步骤。
制得薄膜的评价结果示于表13中。
实施例42和43
除使用表14所示的组分外,重复实施例1-27所述的同样步骤。
制得薄膜的评价结果示于表15中。
正如以下各表所表明的,与未用添加剂所制备的薄膜比较,本发明聚烯烃组合物所制备的薄膜的伸长是非常低的,清楚地表明本发明组合物所制备的聚烯烃薄膜可在短时间内降解。
Claims (15)
1、一种可光降解聚烯烃组合物,包括:(A)80-99.9%(重量)的聚烯烃树脂;和(B)0.01-20%(重量)的至少一种选自改性离子型聚乙烯、烯属不饱和环酐接枝的聚烯烃、和氧化聚乙烯的其它聚合物。
2、如权利要求1所述的组合物,其中聚烯烃树脂选自聚乙烯、聚丙烯和乙烯-乙酸乙烯酯共聚物。
3、如权利要求2所述的组合物,其中所述的聚乙烯树脂是低密度聚乙烯、中密度聚乙烯或高密度聚乙烯、或它们的混合物,且熔融指数范围为0.01-8.0克/10分钟,比重范围0.917-0.961克/厘米3。
4、如权利要求2所述的组合物,其中所述的聚丙烯的熔融指数范围为1.4-16克/10分钟,比重范围为0.890-0.910克/厘米3。
5、如权利要求4所述的组合物,其中所述的聚丙烯树脂具有的平均乙烯含量范围为2.5-8.5%(重量)。
6、如权利要求2所述的组合物,其中所述的乙烯-乙酸乙烯酯共聚物具有的乙酸乙烯酯含量范围为3-18%(重量),熔融指数范围为0.3-4克/10分钟且比重范围为0.925-0.943克/厘米3。
7、如权利要求1所述的组合物,其中所述的改性离子型聚乙烯具有的熔融指数范围为1.0-2.6克/10分钟且比重范围为0.940-0.950克/厘米3。
8、如权利要求1所述的组合物,其中所述的改性离子型聚乙烯的用量范围为组合物重量的0.01-20%。
9、如权利要求1所述的组合物,其中所述的用烯属不饱和环酐接枝的聚烯烃具有的熔融指数范围为1-1,300克/10分钟,比重范围为0.757-0.965克/厘米3,接枝率为0.01-10.0%。
10、如权利要求1所述的组合物,其中所述的用烯属不饱和环酐接枝的聚烯烃的用量范围为组合物重量的0.1-10.0%。
11、如权利要求1所述的组合物,其中所述的氧化聚乙烯具有的比重范围为0.98-1.00克/厘米3,150℃下Brookfield粘度范围为2,500-8,500厘泊,酸度范围为16-41毫克KOH/克。
12、如权利要求1所述的组合物,其中所述的氧化聚乙烯的用量范围为组合物重量的0.01-10.0%。
13、如权利要求1所述的组合物,其中还进一步含有基于每100份组分(A)和组分(B)总和的0.001-0.10重量份的光敏剂。
14、如权利要求13所述的组合物,其中所述的光敏剂是铁化合物。
15、如权利要求14所述的组合物,其中所述的铁化合物选自乙酰丙酮化铁、二乙基氨荒酸铁、硬脂酸铁、棕榈酸铁或它们的混合物。
Applications Claiming Priority (4)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
KR21095/92 | 1992-11-11 | ||
KR920021095 | 1992-11-11 | ||
KR1019930004329A KR960007311B1 (ko) | 1992-11-11 | 1993-03-20 | 광분해성 폴리올레핀 필름 조성물 |
KR4329/93 | 1993-03-20 |
Publications (1)
Publication Number | Publication Date |
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CN1088227A true CN1088227A (zh) | 1994-06-22 |
Family
ID=26629352
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
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CN93121069A Pending CN1088227A (zh) | 1992-11-11 | 1993-11-11 | 可光降解的聚烯烃组合物 |
Country Status (5)
Country | Link |
---|---|
JP (1) | JP2621012B2 (zh) |
KR (1) | KR960007311B1 (zh) |
CN (1) | CN1088227A (zh) |
GB (1) | GB2272902B (zh) |
TW (1) | TW253900B (zh) |
Cited By (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
WO2003014199A1 (en) * | 2001-08-09 | 2003-02-20 | Hubei Guanghe Environmental Protection Science & Technology Co., Ltd. | Light-degradable material for producing disposable medical appliances |
CN101381530B (zh) * | 2007-09-03 | 2011-06-15 | 中国科学院化学研究所 | 对凹凸棒石进行表面处理的方法 |
Families Citing this family (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN114395190B (zh) * | 2022-01-26 | 2022-07-29 | 岳阳兴长石化股份有限公司 | 一种可光降解的聚丙烯材料及其制备方法 |
Family Cites Families (6)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
BE789277A (fr) * | 1971-09-27 | 1973-03-26 | Union Carbide Corp | Composition de polymere d'ethylene degradable sous l'action desintemperies |
US3901838A (en) * | 1972-07-28 | 1975-08-26 | Union Carbide Corp | Environmentally degradable biodegradable blends of a dialkanoyl polymer and an environmentally degradable ethylene polymer |
JPS5213596B2 (zh) * | 1973-12-03 | 1977-04-15 | ||
US4176145A (en) * | 1977-02-01 | 1979-11-27 | Guillet James E | Photodegradable polymer compositions comprising blends of polymers with ketone-containing block or graft copolymers |
GB2187193B (en) * | 1986-02-27 | 1989-11-08 | Gerald Scott | Controllably and swiftly degradable polymer compositions and films and other products made therefrom |
US4990568A (en) * | 1987-01-29 | 1991-02-05 | Copolymer Rubber & Chemical Corporation | Thermoplastic polyolefin and ethylene copolymers with oxidized polyolefin |
-
1993
- 1993-03-20 KR KR1019930004329A patent/KR960007311B1/ko not_active IP Right Cessation
- 1993-11-09 GB GB9323095A patent/GB2272902B/en not_active Expired - Fee Related
- 1993-11-11 JP JP5307354A patent/JP2621012B2/ja not_active Expired - Lifetime
- 1993-11-11 CN CN93121069A patent/CN1088227A/zh active Pending
- 1993-11-15 TW TW082109535A patent/TW253900B/zh active
Cited By (3)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
WO2003014199A1 (en) * | 2001-08-09 | 2003-02-20 | Hubei Guanghe Environmental Protection Science & Technology Co., Ltd. | Light-degradable material for producing disposable medical appliances |
US7045557B2 (en) | 2001-08-09 | 2006-05-16 | Hua Jin | Light-degradable material for producing disposable medical appliances |
CN101381530B (zh) * | 2007-09-03 | 2011-06-15 | 中国科学院化学研究所 | 对凹凸棒石进行表面处理的方法 |
Also Published As
Publication number | Publication date |
---|---|
GB2272902A (en) | 1994-06-01 |
JPH07300541A (ja) | 1995-11-14 |
KR960007311B1 (ko) | 1996-05-30 |
GB9323095D0 (en) | 1994-01-05 |
GB2272902B (en) | 1996-07-17 |
JP2621012B2 (ja) | 1997-06-18 |
KR940011554A (ko) | 1994-06-21 |
TW253900B (zh) | 1995-08-11 |
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