CN1068025C - 含有相容聚苯醚聚酰胺树脂掺混物的可挤塑的热塑性组合物 - Google Patents
含有相容聚苯醚聚酰胺树脂掺混物的可挤塑的热塑性组合物 Download PDFInfo
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- CN1068025C CN1068025C CN95103531A CN95103531A CN1068025C CN 1068025 C CN1068025 C CN 1068025C CN 95103531 A CN95103531 A CN 95103531A CN 95103531 A CN95103531 A CN 95103531A CN 1068025 C CN1068025 C CN 1068025C
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- acid
- polyamide resin
- polyphenylene oxide
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- 239000000203 mixture Substances 0.000 title claims abstract description 73
- 229920006122 polyamide resin Polymers 0.000 title claims abstract description 13
- 229920001955 polyphenylene ether Polymers 0.000 title claims abstract description 7
- 229920001169 thermoplastic Polymers 0.000 title claims abstract description 7
- 239000004416 thermosoftening plastic Substances 0.000 title claims abstract description 7
- -1 polyphenylene Polymers 0.000 claims abstract description 29
- YXFVVABEGXRONW-UHFFFAOYSA-N Toluene Chemical compound CC1=CC=CC=C1 YXFVVABEGXRONW-UHFFFAOYSA-N 0.000 claims abstract description 21
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 claims abstract description 13
- 229920005989 resin Polymers 0.000 claims abstract description 9
- 239000011347 resin Substances 0.000 claims abstract description 9
- 229920000265 Polyparaphenylene Polymers 0.000 claims abstract description 6
- 239000000654 additive Substances 0.000 claims abstract description 5
- 239000004721 Polyphenylene oxide Substances 0.000 claims description 41
- 229920006380 polyphenylene oxide Polymers 0.000 claims description 39
- 150000001408 amides Chemical class 0.000 claims description 31
- KRKNYBCHXYNGOX-UHFFFAOYSA-N citric acid Chemical compound OC(=O)CC(O)(C(O)=O)CC(O)=O KRKNYBCHXYNGOX-UHFFFAOYSA-N 0.000 claims description 18
- 239000002253 acid Substances 0.000 claims description 16
- 239000000126 substance Substances 0.000 claims description 8
- VZCYOOQTPOCHFL-OWOJBTEDSA-N Fumaric acid Chemical compound OC(=O)\C=C\C(O)=O VZCYOOQTPOCHFL-OWOJBTEDSA-N 0.000 claims description 6
- 229920000098 polyolefin Polymers 0.000 claims description 6
- 230000035939 shock Effects 0.000 claims description 4
- 239000001530 fumaric acid Substances 0.000 claims description 3
- FPYJFEHAWHCUMM-UHFFFAOYSA-N maleic anhydride Chemical compound O=C1OC(=O)C=C1 FPYJFEHAWHCUMM-UHFFFAOYSA-N 0.000 claims description 3
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- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 claims 1
- 150000008064 anhydrides Chemical class 0.000 claims 1
- UJMDYLWCYJJYMO-UHFFFAOYSA-N benzene-1,2,3-tricarboxylic acid Chemical compound OC(=O)C1=CC=CC(C(O)=O)=C1C(O)=O UJMDYLWCYJJYMO-UHFFFAOYSA-N 0.000 claims 1
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- 239000004952 Polyamide Substances 0.000 abstract description 17
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- 125000000843 phenylene group Chemical group C1(=C(C=CC=C1)*)* 0.000 description 7
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- LYCAIKOWRPUZTN-UHFFFAOYSA-N Ethylene glycol Chemical compound OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 description 5
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- LIKMAJRDDDTEIG-UHFFFAOYSA-N 1-hexene Chemical compound CCCCC=C LIKMAJRDDDTEIG-UHFFFAOYSA-N 0.000 description 2
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- 229920003656 Daiamid® Polymers 0.000 description 2
- RTZKZFJDLAIYFH-UHFFFAOYSA-N Diethyl ether Chemical compound CCOCC RTZKZFJDLAIYFH-UHFFFAOYSA-N 0.000 description 2
- 150000001266 acyl halides Chemical class 0.000 description 2
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- 125000003545 alkoxy group Chemical group 0.000 description 2
- 150000001412 amines Chemical class 0.000 description 2
- UHOVQNZJYSORNB-UHFFFAOYSA-N benzene Substances C1=CC=CC=C1 UHOVQNZJYSORNB-UHFFFAOYSA-N 0.000 description 2
- IISBACLAFKSPIT-UHFFFAOYSA-N bisphenol A Chemical compound C=1C=C(O)C=CC=1C(C)(C)C1=CC=C(O)C=C1 IISBACLAFKSPIT-UHFFFAOYSA-N 0.000 description 2
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- 238000009833 condensation Methods 0.000 description 2
- 230000005494 condensation Effects 0.000 description 2
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- 125000000524 functional group Chemical group 0.000 description 2
- 125000005842 heteroatom Chemical group 0.000 description 2
- 125000004435 hydrogen atom Chemical group [H]* 0.000 description 2
- LVHBHZANLOWSRM-UHFFFAOYSA-N itaconic acid Chemical compound OC(=O)CC(=C)C(O)=O LVHBHZANLOWSRM-UHFFFAOYSA-N 0.000 description 2
- 238000004519 manufacturing process Methods 0.000 description 2
- OKKJLVBELUTLKV-UHFFFAOYSA-N methanol Natural products OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 2
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- 229920013636 polyphenyl ether polymer Polymers 0.000 description 2
- 125000002924 primary amino group Chemical group [H]N([H])* 0.000 description 2
- 125000004151 quinonyl group Chemical group 0.000 description 2
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- 125000000391 vinyl group Chemical group [H]C([*])=C([H])[H] 0.000 description 2
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- PUPZLCDOIYMWBV-UHFFFAOYSA-N (+/-)-1,3-Butanediol Chemical compound CC(O)CCO PUPZLCDOIYMWBV-UHFFFAOYSA-N 0.000 description 1
- JEFSTMHERNSDBC-UHFFFAOYSA-N 1,2-dimethylcyclohexa-2,4-dien-1-ol Chemical compound CC1=CC=CCC1(C)O JEFSTMHERNSDBC-UHFFFAOYSA-N 0.000 description 1
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- NGNBDVOYPDDBFK-UHFFFAOYSA-N 2-[2,4-di(pentan-2-yl)phenoxy]acetyl chloride Chemical group CCCC(C)C1=CC=C(OCC(Cl)=O)C(C(C)CCC)=C1 NGNBDVOYPDDBFK-UHFFFAOYSA-N 0.000 description 1
- ABGBGJXCHTWNJK-UHFFFAOYSA-N 2-[2-(dodecylamino)-2-oxoethyl]-2-hydroxybutanedioic acid Chemical compound CCCCCCCCCCCCNC(=O)CC(O)(C(O)=O)CC(O)=O ABGBGJXCHTWNJK-UHFFFAOYSA-N 0.000 description 1
- WSUBIRCPENZBDS-UHFFFAOYSA-N 2-carbonochloridoylpentanedioic acid Chemical compound OC(=O)CCC(C(O)=O)C(Cl)=O WSUBIRCPENZBDS-UHFFFAOYSA-N 0.000 description 1
- WOGWYSWDBYCVDY-UHFFFAOYSA-N 2-chlorocyclohexa-2,5-diene-1,4-dione Chemical class ClC1=CC(=O)C=CC1=O WOGWYSWDBYCVDY-UHFFFAOYSA-N 0.000 description 1
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- VEORPZCZECFIRK-UHFFFAOYSA-N 3,3',5,5'-tetrabromobisphenol A Chemical compound C=1C(Br)=C(O)C(Br)=CC=1C(C)(C)C1=CC(Br)=C(O)C(Br)=C1 VEORPZCZECFIRK-UHFFFAOYSA-N 0.000 description 1
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Abstract
本发明涉及一种含有相容聚苯醚-聚酰胺树脂掺混物的可挤塑的热塑组合物。通过使用特性粘度大于45毫升/克(在甲苯中于25℃在0.6克/100毫升的条件下测定)的聚苯醚的比浓粘度大于175毫升/克(按ISO 307方法在硫酸中测定)的聚酰胺，证明可以得到一种容易挤塑的掺混物。掺混物中如果这两种树脂中只有一种树脂，即聚苯醚或聚酰胺具有所要求的粘度值，则不太适于用挤塑法加工。该组合物还可含有其它常用的添加剂。
Description
本发明涉及含有适于挤塑的相容聚苯醚-聚酰胺树脂掺混物的热塑性组合物。
本发明也涉及由本发明的组合物形成的物品。
市售的聚苯醚和聚酰胺的掺混物不太适用于通过挤塑模制成所需形状：这种掺混物是通过混料-挤塑步骤，然后切粒而制造的。然后通常用注塑法将所得到的丸粒加工成所需形状。
通常知道，可以通过增加热塑性树脂的分子量从而增加其粘度的方法来使其更适于挤塑。使用高粘度热塑性树脂的结果是可获得较高的挤塑所需的熔体强度值。
商业上最感兴趣的聚苯醚和聚酰胺掺混物包含聚酰胺的连续相，而聚苯醚则分散在其中。因此可以预料增加聚酰胺的粘度只会使该掺混物更适于挤塑。组合使用高粘度聚酰胺与标准粘度的聚苯醚确实可以增加熔体粘度。然后不幸的是，一般聚苯醚的这种掺混物显示出很不理想的效果：在制造步骤中挤塑时所发生的所谓离模膨胀达到如此的程度，以致使得产品厚度不均匀且加工性不好。
现已发现，使用具有特定粘度(比通常的高)的聚苯醚和具有特定粘度(比通常的高)的聚酰胺的组合物可以得到的一种具有满意的熔体粘度而不发生离模膨胀现象的掺混物。
在本发明的热塑性组合物中，聚苯醚的特性粘度高于45毫升/克，这是在甲苯中于25℃，浓度为0.6克/100毫升的条件下测定的；聚酰胺的比浓粘度高于175毫升/克，这是在硫酸中按ISO 307标准测定的。
在本发明的掺混物中，聚苯醚的特性粘度较好为至少50毫升/克，聚酰胺的比浓粘度较好为至少190毫升/克。
下面叙述较好的聚苯醚对脂(PPE)和聚酰胺树脂以及提供其相容组合物的方法。
通常，较好是，聚酰胺组分构成掺混物的连续相。因此，聚酰胺组分一般至少应占PPE-聚酰胺组合物总重量的35％。
聚苯醚是一类众所周知的化合物，有时也称为聚苯氧。适用的聚苯醚及其制备方法的实例可参见美国专利3,306,874、3,306,875、3,257,357和3,257,358。本发明的组合物包含由酚类化合物的氧化偶联反应所制得的均聚物，共聚物和接枝共聚物。在本发明的组合物中用作基材树脂的较好的聚苯醚是由2,6-二甲基苯酚衍生得到的聚苯醚。含有由2,6-二甲基苯酚和2,3,6-三甲基苯酚衍生得到的聚苯醚共聚物也包括在内。
特别有用的聚苯醚是特性粘度(I.V)高于50毫升/克的聚(2,6-二甲基-1,4-亚苯基醚)，其I.V.是在甲苯中于25℃在0.6克100毫升的浓度下测定的。
可用于实施本发明的聚酰胺树脂是一类被称为尼龙的树脂，其特征是存在酰胺基团(-CONH-)。尼龙6和尼龙6,6通常是较好的聚酰胺，可从各种商业渠道得到，但是，其也聚酰胺，如尼龙-4、尼龙-12、尼龙-6,10，尼龙-6,9或其它尼龙，如非结晶尼龙也可用于特定的聚苯醚-聚酰胺用途。对本发明的掺混物而言，最好的聚酰胺是聚酰胺-6,6。
聚酰胺可用许多熟知的方法制得。例如，尼龙-6是己内酰胺的聚合产物。尼龙-6,6是己二酸和己二胺的缩合产物。按照ISO 307标准在硫酸中测定的比浓粘度高于175毫升/克，较好至少190毫升/克的尼龙-6,6是最好的一类聚酰胺。
在本发明的掺混物中，制备组合物时必须使用相容剂。使用相容剂有两个目的，总的来说是改善聚苯醚-聚酰胺树脂掺混物的物理性能，并使得能够使用较大比例的聚酰胺组分。这里所使用的术语“相容剂”是指能与聚苯醚、聚酰胺或这两者相互作用的那些多官能化合物。这种相互怍用可以是化学的(如接枝)或物理的(如影响分散相的表面特性)。无论是哪种情况，所得到的聚苯醚-聚酰胺组合物似乎都具有改善的相容性(可混性)，尤其如由提高的冲击强度、模塑汇合线强度和/或伸长率所证实的那样。这里所使用的术语“相容的聚苯醚-聚酰胺基树脂”是指在物理上或化学上已经与上述一种试剂相容了的那些组合物，以及不用US-A-3,379,792中公开的那试剂就是在物理上可相容的那些组合物。
可用来实施本发明的各种相容剂的例子包括：a)液态二烯聚合物，b)环氧化合物，c)氧化聚烯烃腊，d)醌类，e)有机硅烷化合物，f)多官能化合物和官能化聚苯醚，如下面所述由一种或多种前述的相容剂与聚苯醚反应所制得的那些化合物。
适用于本发明的液态二烯聚合物a)包括共轭二烯的均聚物及其与选自下列的至少一种单体的共聚物：其它共轭二烯；乙烯基单体，如苯乙烯和α-甲基苯乙烯：烯烃，如乙烯、丙烯、1-丁烯、异丁烯、1-己烯、1-辛烯和1-十二碳烯，以及它们的混合物，这种聚合物的数均分子量应为150-10,000，较好是150-5,000。这些均聚物和共聚物可按例如US-A-4,054,612、3,876,721和3,428,699中所述方法制备，这些聚合物包括，其中有聚丁二烯、聚异戊二烯、聚(1,3-戊二烯)、聚(丁二烯-异戊二烯)、聚(苯乙烯-丁二烯)、聚氯丁二烯、聚(丁二烯-α-甲基苯乙烯)、聚(丁二烯-苯乙烯-异戊二烯)、聚(丁烯-丁二烯)等。
适用于实施本发明的环氧化合物(b)包括：(1)由多元酚(例如双酚-A、四溴双酚-A、间苯二酚和对苯二酚)和表氯醇缩合所制得的环氧对脂：(2)由多元醇(例如乙二醇、丙二醇、丁二醇、聚乙二醇、聚丙二醇、季戊四醇和三羟甲基乙烷等)和表氯醇缩合所制得的环氧树脂：(3)一元醇和一元酚的缩水甘油基醚化产物，包括苯基缩水甘油醚、丁基缩水甘油醚和甲苯基缩水甘油醚：(4)氨基化合物的缩水甘油基衍生物：例如苯胺的二缩水甘油基衍生物：和(5)较高级的烯烃或环状链烯、或天然不饱和油(如豆油)以及上述液态二烯聚合物等的环氧化产物。
氧化聚烯烃腊(c)是众所周知的，关于这类化合物的说明及制备方法可参见US-A-3,822,227和3,756,999及德国专利公告3,047,915和2,201,862。
一般地说，这类化合物可由聚烯烃氧化或悬浮氧化制得。一种特别优选的聚烯烃腊是“Hoechst Wachs”。
适用于本发明的醌化合物(d)的特征是在未取代衍生物的分子中含有至少一个6元碳环；在环结构中至少含有2个羰基，这两个羰基可以在同一环中，或者，如果环的数目大于1，则可在不同的环中，其条件是它们必须占据相应于该单环醌的1,2-或1,4-的定向位置；且在环结构中至少含有两个碳-碳双键，所述碳-碳双键和环结构中的羰基碳-碳双键，所述碳-碳双键和羰基碳-氧双键均为相互共轭。当未取代的醌中存在的环数大于1时，这些环可以是稠合的、非稠合的，或两者皆有，非稠合的环可由一个碳-碳双键直接按键合或由一个含有诸如=C-C=的共轭不饱和部分的烃基连接。
取代的醌类也是在本发明的范围之内。当希望取代时，取代度可为1至可取代的氢原子的最大数目。可存在未取代醌结构上的各种取代基的例子包括卤素，例如氯、溴、氟等，烃基，包括支化和非支化的，饱和及不饱和的烷基、芳基、烷芳基和环烷基及其卤代衍生物：以及其中含有杂原子的类似的烃类，这些杂原子是起连接作用的氧、硫或磷，其中靠这些原子将上述基团连接到醌环上(例如氧键)。
可以举出各种醌化合物的例子：1,2-和1,4-苯醌，2,6-二苯基苯醌，四甲基二醌，2,2＇-和4,4＇-联苯醌，1,2-、1,4-和1,6-萘醌，氯醌，2-氯-1,4-苯醌，2,6-二甲基苯醌等。
适合用作相容剂的有机硅烷化合物(e)的特征是在分子中含有(a)至少一个通过氧键连接到碳上的硅原子和(b)至少一个碳-碳双键或碳-碳三键和/或一个选自胺基或巯基的官能基团，其条件是该官能基团不是直接连接到该硅原子上。
在这种化合物中，C-O-Si部分通常以直接连接到硅原子上的烷氧基或乙酰氧基的形式存在，其中该烷氧基或乙酰氧基一般含有15个碳原子，且也可含有杂原子(如氧)。此外，在该化合物中也可以有一个以上的硅原子，如果有的话，这些多硅原子可以通过氧键(如硅氧烷)、硅键、或二官能有机基(如亚甲基或亚苯基基团)连接起来。
适用的有机硅烷的例子包括：γ-氨基丙基三乙氧基硅烷、2-(3-环己烯基)乙基三甲氧基硅烷、1,3-二乙烯基四乙氧基硅烷、乙烯基三-(2-甲氧基乙氧基)硅烷、5-二环庚烯基三乙氧基硅烷和γ-巯基丙基三甲氧基硅烷。
在实施本发明中可用作相容剂的多官能化合物(f)有三种类型。第一种类型的多官能化合物是在分子中既含有(a)碳-碳双键或碳-碳三键又含有(b)至少一个羧酸、酸酐、酰基卤、酐、酰基卤酐、酰胺、酸酯、酰亚胺、氨基、或羟基的那些化合物。这类多官能化合物的例子包括：马来酸、马来酸杆、富马酸、柠康酸、衣康酸、马来酰亚胺、马来酰肼：由二胺和马来酸酐、马来酸、富马酸等反应得到的产物：二氯马来酸酐、马来酰胺、不饱和羧酸(如丙烯酸、丁烯酸、甲基丙烯酸、t-乙基丙烯酸、戊烯酸)：壬烯二酸、十一碳烯酸、十二碳烯酸、亚油酸等：上述不饱和羧酸的酯类、酰胺或酐：不饱和醇类(如烷基醇、巴豆醇、甲基乙烯基甲醇、4-戊烯-1-醇、1,4-己二烯-3-醇、3-丁烯-1,4-二醇、2,5-二甲基-3-己烯-2,5-二醇以及通式为CnH2n-5OH、CnH2n-7OH和CnH2n-8OH的醇类，其中n为不大于30的正整数，用NH2基取代上述不饱和醇中的-OH而得到的不饱和胺类；以及多官能二烯聚合物和共聚物。在这些化合物中，用于本发明组合物的优选相容剂之一的马来酐。
适用于本发明的第二种类型的多官能相容剂化合物的特征是含有下述(a)和(b)的基团的那些化合物：(a)通式(OR)所示的基团，其中R代表氢或烷基、芳基、酰基或碳酰二氧基：(b)至少两个选自下列的相同或不同的基团：羧酸、酰基卤、酸酐、酐、酰基卤酐、酸酯、酰胺、亚氧基、氨基及其盐类。这类相容剂的代表是脂族多元酸、酸酯及酰胺，可用下面通式表示：(RⅠO)mR(COORⅡ)n(CONRⅢ R Ⅳ)s其中R是含有2-20个，较好2-10个碳原子的直链或支链的饱和脂族烃基；RⅠ选自氢或含有1-10个，较好1-6个，更好1-4个碳原子的烷基、芳基、酰基可碳酰二氧基，特别优选氢；每个RⅡ独立地选自氢或者含有1-20个，较好1-10个碳原子的烷基或芳基：每个RⅢ和RⅣ独立地选自氢或者含有1-10个，较好1-6个，更好1-4个碳原子的烷基或芳基；m等于1，(n+s)大于或等于2，较好等于2或3,n和s各大于或等于0，而且式中(ORⅠ)是在羰基的α和β位置，而且至少可有2个羰基被2-6个碳原子隔开。显然，当各取代基所含碳原子数小于6时RⅠ,RⅡ、RⅢ和RⅣ不可能是芳基。
说明适用的多元酸的例子可以举出：柠檬酸、苹果酸和松蕈(三)酸；包括其各种商品形式，例如，无水的和水合的酸。其中，柠檬酸是另一种优选的相容剂。可用于本发明的酸酯的例子包括例如柠檬酸乙酰酯和柠檬酸一和/或二硬脂酰酯等。这里适用的酰胺包括例如N,N＇-二乙基柠檬酰胺：N-苯基柠檬酰胺；N-十二烷基柠檬酰胺：N,N＇-双十二烷基柠檬酰胺和N-十二烷基苹果酰胺。特别优选的衍生物是它们的盐，包括与胺和/或较好是碱形成的盐，以及碱金属盐。适合的盐的例子包括苹果酸钙、柠檬酸钙、苹果酸钾和柠檬酸钾。
适用于本发明第三种类型的相容剂化合物的特征是分子中含有(a)一种酰卤基，最好是酰氯基和(b)至少一种羧酸，羧酸酐、酸酯或酰胺基团，较好是羧酸或羧酸酐基团。这类相容剂的例子可以举出：1,2,4-苯三酸酐酰氯、氯甲酰基琥珀酸酐、氯甲酰基琥珀酸、氯甲酰基戊二酸酐、氯甲酰基戊二酸、氯乙酰基琥珀酸酐、氯乙酰基琥珀酸、1,2,4-苯三酰氯和氯乙酰基戊二酸。其中较佳者是1,2,4-苯三酸酐酰氯。此外，特别推荐的作法是将这种类型的相容剂与至少一部分聚苯醚进行预反应，从而使该相容剂成为PPE官能化的化合物。
上述各种相容剂详见US-A-4,315,086和4,642,358：及欧洲专利申请No.04640。
上述各种相容剂可以单独使用或以任何互相组合的形式使用。此外，它们可以直接加入到熔融的掺混物中或与聚苯醚和聚酰胺中的任何一种或两种以及在制备本发明的组合物中所用的其它树脂状物料进行预混。对于前述多种相容剂，尤其对多官能化合物来说，当至少一部分相容剂与全部或部分聚苯醚预混时，可以发现相容性有更大的改进。可以认为这种预混作用可以促使该相容剂与聚合物发生反应，并因此使这种聚合物象上面所指出的那样官能化，例如聚苯醚可用1,2,4-苯三酐酰氯进行预混生成一种酐官能化的聚苯醚，这种聚苯醚未官能化的醚比较，其与聚酰胺的相容性有所改善。
如果在制备本发明的组合物时使用相容剂，则其初始用量将取决于所选用的具体相容剂和具体要加进去的聚合物体系。
在本发明的组合物中也可以使用任何其它已知的相容化体系。其它体系可参见例如US-4,866,114。
可以在本发明的组合物中掺入一种或多种冲击改性剂。通常用于含有聚苯醚、聚酰胺或聚苯醚和聚酰胺的组合的组合物的所有冲击改性剂均可使用。特别适用的是所谓的嵌段共聚物，如三嵌段共聚物和二嵌段共聚物。
可以提供包含有不同含量冲击改性剂的各种有用的聚苯醚-聚酰胺组合物。一般地说，当每100重量份聚苯醚和聚酰胺组分的总和使用1-30重量份冲击改性剂时，就观察到改进的性质，尤其有关塑料的延性。
可用在本发明组合物中的二嵌段或三嵌段共聚物橡胶添加剂是一种由一个或两个链烯基芳族嵌段，通常是苯乙烯嵌段，和橡胶嵌段如可以是部分加氢的丁二烯嵌段构成的热塑性橡胶。
本发明的热塑性组合物可以包含下述任何添加剂：增强纤维、稳定剂、染料、颜料、聚烯烃、阻火剂等。
相容的聚苯醚-聚酰胺树脂组合物的玻璃增强等级在要求各种物理性质如冲击强度、刚性和模量，尺寸稳定性，高的耐热性以及耐化学性等的独特组合的热塑性应用中极为重要。原则上讲，玻璃填充的本发明的PPE-聚酰胺组合物能提供良好的物理性能。一般可用10-30％重量的切短的玻璃纤维来改进这些组合物。这些重量百分率基于聚苯醚树脂、聚酰胺对脂以及玻璃等的总重量。在某些情况下也可使用或多或少(例如5-45％(重量))的玻璃。当玻璃纤维含量小于5％时就开始呈现象未增强产品的性能。当玻璃纤维含量大于45％重量时就开始影响树脂涂布和有效粘结玻璃的能力。
上述所有专利及专利申请均列为本申请的参考文献。本发明由下列实例进一步说明。
实例
在实例中使用下列材料：
PPE-1：一种特性粘度为40毫升/克的聚(2,6-二甲基-1,4-亚苯基醚)，测定条件：在甲苯中，25℃，浓度为0.6克/100毫升，(PPO 803)：
PPE-2：一种特性粘度为45毫升/克的聚(2,6-二甲基-1,4-亚苯基醚)，测定条件：在甲苯中，25℃，浓度为0.6克/100毫升，(PPO 800)：
PPE-3：一种特性粘度为57毫升/克的聚(2,6-二甲基-1,4-亚苯基醚)，测定条件：在甲苯中，25℃，浓度为0.6克/100毫升，(PPO 805)：
PA-1：一种按ISO 307标准在硫酸中测定的比浓粘度为145毫升/克的聚酰胺-6,6,(A3Q44)；
PA-2：一种按ISO 307标准在硫酸中测定的比浓粘度为205毫升/克的聚酰胺-6,6,(A4)；
PA-3：一种按ISO 307标准在硫酸中测定的比浓粘度为270毫升/克的聚酰胺-6,6,(A5)：
CA：柠檬酸；
ST：标准碘基稳定剂
PETS：季戊四醇四硬脂酸酯：
CB：炭黑。
各成分按下表中指明的量在一台双螺杆挤塑机中进行混料，在该挤塑机长度方向上有6个不同的温度设定值，可从280-310℃改变。螺杆转速为300转/分，挤出容量为10千克/小时。除聚酰胺外，所有成分均在挤塑机的进料口喂入，而聚酰胺则在挤塑机中部附近顺流喂入。挤塑机模口直径为4毫米。以挤塑机出来的部分掺混物会因离模膨胀而受损，即挤出的线料直径远大于4毫米。这是一种完全不希望的效应，因为这种效应会引起极大的不稳定性。这会使得该掺混物不适于采用挤塑方法模制由该掺混物形成的制品。也不适于用通常的生产工艺进行切粒。
从挤塑机出来的线料在实验室设备中进行切粒，然后在110℃干燥3小时。
干燥后的粒料送入到一台挤塑机中，该挤塑机装有一台Goettfert-Feinwerk公司制造的Rheotene熔体粘度测定仪。该设备包括一台带有模头直径为4毫米的挤塑机头的挤塑机和两个安放在该挤塑机头下面彼此相距120毫米的轮子。线料通过这两个高速转动的导料轮之间。对拉伸速度和拉伸力进行监测。当出现不稳定现象时就测得这些值，根据所测得的这些值计算以牛顿表示的熔体强度。在下面的表中也给出了这些结果。
表实例： A* B* C* Ⅰ Ⅱ Ⅲ Ⅳ组合物(重量份)PPE-1: 58.9 58.9 - - - - -PPE-2: - - - - - - 58.9PPE-3: - - 58.9 58.9 58.9 53.9 -PA-1: 40 - 40 - - - -PA-2: - 40 - 40 - 45 40PA-3: - - - - 40 - -CA: 0.7 0.7 0.7 0.7 0.7 0.7 0.7ST: 0.1 0.1 0.1 0.1 0.1 0.3 0.1PETS: 0.3 0.3 0.3 0.3 0.3 0.3 0.3CB: 0.1 0.1 0.1 0.1 0.1 0.1 0.1性能离模膨胀 无 有 无 无 无 无 极小熔体强度 未测定 26 22 26 35 未测定 未测定*A、B和C是对比实例。
从表中的结果可以看出：普通的聚苯醚和聚酰胺的掺混物(实例A)很容易从混料机中挤出。但是，其熔体强度不足以用挤塑法将这种公知的掺混物模塑成形为制品。
实例B的掺混物含有一种标准聚苯醚和一种高粘度聚酰胺，确实显示出良好的熔体强度，这是可以预料的，因为聚酰胺形成了连续相。出人意料的是对比掺混物显示出强烈的离模膨胀，使得这种掺混物不适于挤塑用途。
上述结果非常令人惊奇，因为如对比实例B中所用的高粘度聚酰胺本身，即不与聚苯醚掺混时，是特别适于挤塑用途的。
使用高粘度聚苯醚和标准聚酰胺(掺混物C)的结果是掺混物不产生离模膨胀，但熔体强度相当低。
只有通过组合使用高粘度聚苯醚和高粘度聚酰胺(实例Ⅰ、Ⅱ、Ⅲ和Ⅳ)才能得到一种熔体强度好、没有离模膨胀，或只有极少离模膨胀的材料。
Claims (12)
1．一种含有相容聚苯醚-聚酰胺树脂掺混物的可挤塑热塑性组合物，其中聚苯醚的特性粘度高于45毫升/克，其测定条件是在甲苯中25℃，浓度为0.6克/100毫升，且其中聚酰胺的比浓粘度按照ISO 307标准在硫酸中测定时高于175毫升/克，其中所述的聚酰胺是聚酰胺6,6。
2．如权利要求1的组合物，其中聚苯醚的特性粘度为至少50毫升/克，聚酰胺的比浓粘度为至少190毫升/克。
3．如权利要求1的组合物，其中以聚苯醚和聚酰胺的总重量为基准，该相容聚苯醚-聚酰胺树脂掺混物中含有5-95％重量聚苯醚树脂和95-5％重量聚酰胺树脂。
4．如权利要求3的组合物，其中所述聚酰胺树脂构成一个连续相，其量大于该相容聚苯醚-聚酰胺树脂掺混物重量的35％。
5．如权利要求1的组合物，其中所述相容聚苯醚-聚酰胺树脂掺混物与选自下述的一种相容剂相容：马来酐、富马酸、柠檬酸、苹果酸，以及聚苯醚和苯三酸酐酰基氯的反应产物。
6．如权利要求1的组合物，其中所述聚苯醚树脂是一种包含由选自2,6-二甲基苯酚单元和2,3,6-三甲基苯酚单元的单元衍生出来的一种或多种单元的聚合物或共聚物。
7．如权利要求6的组合物，其中所述聚苯醚是聚(2,6-二甲基-1,4-亚苯基醚)。
8．如权利要求1的组合物，其中该组合物还包含一种能提高抗冲击强度的添加剂。
9．如权利要求1的组合物，其中该组合物还包含选自下列的一种添加剂：增强纤维、稳定剂、染料、颜料、聚烯烃、阻火剂及其它们的混合物。
10．由权利要求1的组合物形成的物品。
11．如权利要求5的组合物，其中所述的相容剂是柠檬酸。
12．如权利要求9的组合物，其中所述的能提高抗冲击强度的添加剂是一种嵌段共聚物。
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| EP94104746A EP0675165A1 (en) | 1994-03-25 | 1994-03-25 | Extrudable thermoplastic composition comprising a compatibilized polyphenylene ether polyamide resin blend |
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1994
- 1994-03-25 EP EP94104746A patent/EP0675165A1/en not_active Withdrawn
- 1994-08-23 US US08/294,705 patent/US5534600A/en not_active Expired - Lifetime
-
1995
- 1995-03-20 JP JP7059587A patent/JPH0834917A/ja active Pending
- 1995-03-23 ES ES95200729T patent/ES2132516T3/es not_active Expired - Lifetime
- 1995-03-23 DE DE69510479T patent/DE69510479T2/de not_active Expired - Lifetime
- 1995-03-25 CN CN95103531A patent/CN1068025C/zh not_active Expired - Lifetime
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| EP0270796A1 (en) * | 1986-10-23 | 1988-06-15 | Mitsubishi Petrochemical Co., Ltd. | Process for the preparation of Polyphenylene ether-polyamide resin compositions |
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| EP0501175A1 (de) * | 1991-02-28 | 1992-09-02 | BASF Aktiengesellschaft | Faserverstärkte thermoplastische Formmassen |
Also Published As
| Publication number | Publication date |
|---|---|
| CN1126224A (zh) | 1996-07-10 |
| DE69510479T2 (de) | 2000-03-09 |
| US5534600A (en) | 1996-07-09 |
| JPH0834917A (ja) | 1996-02-06 |
| EP0675165A1 (en) | 1995-10-04 |
| DE69510479D1 (de) | 1999-08-05 |
| ES2132516T3 (es) | 1999-08-16 |
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