KR940006470B1 - Polybuthylene terephthalate compositions - Google Patents
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Abstract
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Description
[발명의 명칭][Name of invention]
개량된 폴리부틸렌 테레프탈레이트 수지 조성물Improved Polybutylene Terephthalate Resin Composition
[발명의 상세한 설명]Detailed description of the invention
본 발명은 폴리부틸렌 테레프탈레이트(polybutylene terephthalate) 에 강화제, 난연제, 난연조제, 충격 강화제 및 에폭시 화합물과 모노옥사졸린을 첨가하여 가수분해를 억제시키고 내습열성이 우수하며, 충격강도및 인성을 향상시킨 개량된 폴리부틸렌 테레프탈레이트 수지 조성물에 관한 것이다.The present invention is a polybutylene terephthalate (polybutylene terephthalate) by adding a reinforcing agent, flame retardant, flame retardant aid, impact enhancer and epoxy compound and monooxazoline to inhibit hydrolysis, excellent heat and moisture resistance, improved impact strength and toughness An improved polybutylene terephthalate resin composition.
다시 말하면 본 발명은 폴리부틸렌 테레프탈레이트가 수분에 의해 가수분해가 일어나 기계적 성질이 저하되므로 이를 방지하면서 두께가 얇은 성형품들을 사출 성형할 수 있도록, 유도성의 개량 및 인성과 충격강도를 향상시킨 폴리부틸렌 테레프탈레이트 수지 조성물에 관한 것이다.In other words, in the present invention, polybutylene terephthalate is hydrolyzed by moisture, and mechanical properties are lowered, so that polybutylene terephthalate is improved in inducibility and toughness and impact strength so that injection molding of thin molded articles can be prevented. It relates to a len terephthalate resin composition.
일반적으로 폴리부틸렌 테레프탈레이트 수지는 결정성 수지로서 내열성, 전기특성, 기계적 강도, 내약품성이 우수하다. 그러나 결정 특성이 양호하기 때문에 오히려 아이조드 노치(izod notched) 충격강도가 부족하며, 유리섬유(glass fiber)로 강화된 폴리부틸렌 테레프탈레이트는 성형 수축율에 따른 이방성이 크기때문에 성형품의 왜곡이 발생하기 쉽고 두께가 얇은 성형품에서는 잘 깨지는 단점이 있을 뿐 아니라 표면광택성도 좋지 않았었다.In general, polybutylene terephthalate resin is a crystalline resin, excellent in heat resistance, electrical properties, mechanical strength, chemical resistance. However, Izod notched impact strength is insufficient because of good crystal characteristics, and polybutylene terephthalate reinforced with glass fiber tends to be easily distorted due to the large anisotropy according to the shrinkage rate. Thin molded parts not only had the disadvantage of breaking well but also had poor surface gloss.
또한, 폴리부틸렌 테레프랄레이트 수지는 고온에서 에스테르가 수분에 의해 가수분해 되는데 이때 말단의 카르복실기(carboxyl) 및 하이드록실(hydroxyl)기는 가수분해가 매우 빠르게 촉진된다.In addition, the polybutylene terephthalate resin is hydrolyzed ester at high temperature by water, wherein the carboxyl groups and hydroxyl groups at the terminal are accelerated very quickly.
따라서, 가수분해가 일어나면 폴리부릴렌 테레프탈레이트의 분자량이 감소되어 기계적 성질이 매우 감소되는 현상을 나타내는 결점이 있었다.Therefore, when hydrolysis occurs, there is a drawback that a phenomenon in which the molecular weight of polyburylene terephthalate is reduced and mechanical properties are greatly reduced.
종래의 폴리부틸렌 테레프탈레이트의 용도는 전기, 전자부품 및 자동차 부품에 국한되었지만 특히 현재는 자동차 수요가 신장세에 있는 데다가 특수 용도로 개발된 것으로는 전기, 전자용도로서 용제비축출성, 금속접점 부식성 방지 빛 난연화된 폴리부틸렌 테레프탈레이트와, 자동차 부품에서는 앞으로 내열성, 내습열성, 내구성이 향상 된 것들이 요구되고 있다. 그러나 폴리부틸렌 테레프탈레이트는 가수분해로 인한 분자량 감소로 기계적 성질중 강도, 인성, 충격성이 현저히 저하되는 현상이 있었다. 따라서 이러한 단점들을 해결하기 위해서 폴리부틸렌 테레프탈레이트에 특수한 첨가제의 채용함으로써 말단기를 감소시키며 또한 타수지와 알로이(Alloy)를 하는 경우도 있었다.Conventional use of polybutylene terephthalate has been limited to electric, electronic parts and automotive parts, but the current demand for automobiles is on the rise, and special applications have been developed for electric and electronic applications. Light flame-retardant polybutylene terephthalate and automotive parts are required to have improved heat resistance, heat resistance, heat resistance, and durability. However, polybutylene terephthalate has a phenomenon that the strength, toughness and impact properties of the mechanical properties are significantly reduced due to the decrease in molecular weight due to hydrolysis. Therefore, in order to solve these shortcomings, the use of special additives in polybutylene terephthalate reduces the end groups, and in some cases, the resin and alloy (Alloy).
일본 공개 특허 51-91958에서는 폴리부틸렌 테레프탈레이트와 α-올레핀 초산 비닐 공중합체에 에폭시기 1∼2개를 도입하여 혼련 제조함으로서 내습열성을 향상시킨 것으로 나타나 있으며, 일본 공개 특허 51-5865에서는 폴리부틸렌 테레프탈레이트와 데카브로모 디페닐(Decabromo dlphenyl) 및 헥사브로모 디페널에테르(Hexabromo diphenylether)를 난연제로 사용하여 컴파운딩 했을 때 신도가 저하되어 이를 해결하기위해 에폭시기가 1∼2개인 에폭시 화합물을 첨가하여 인성 및 신도를 향상시킨 것으로 공개되어 있다.Japanese Patent Laid-Open Publication No. 51-91958 has shown that the heat-and-moisture resistance has been improved by kneading a polybutylene terephthalate and α-olefin vinyl acetate copolymer by introducing 1 to 2 epoxy groups to produce kneading. To solve this problem, when compounding with ethylene terephthalate, decabromo phenyl, and hexabromo diphenylether as a flame retardant, elongation is lowered. It is disclosed that the addition improves toughness and elongation.
일본 공개 특허 61-221459는 폴리에스테르(polyester)에 에폭시기가 포함된 스타일렌(styrene) 수지를 사용하여 기계적 성질 및 표면 특성을 향상시킨 것으로 나타나 있다.Japanese Laid-Open Patent Publication No. 61-221459 shows that the mechanical properties and the surface properties are improved by using a styrene resin containing an epoxy group in a polyester.
일본 공개 특허 55-82148에서는 폴리에스테르에 유리섬유, 에스테르(ester)형 에폭시화합물을 혼련하여 강도 및 유동성을 향상시킨 것으로 공개되어 있다.Japanese Patent Laid-Open No. 55-82148 discloses that polyester is blended with a glass fiber and an ester epoxy compound to improve strength and fluidity.
일본 공개 특허 55-52340에서는 폴리에스테르에 에폭시화합물로 표면 처리된 유리섬유를 사용하여 강도를 향상시킨 것으로 되어 있다. 또한, 폴리머 알로이에서는 올레핀 혹은 폴리아미드를 폴리부딜렌 테레프랄레이트와 혼련하여 내습열성을 개량하기도 하지만 상용성 문제에 의한 물성 저하 등이 발생한다.In Japanese Patent Laid-Open No. 55-52340, the strength is improved by using glass fibers surface-treated with an epoxy compound in polyester. In addition, in the polymer alloy, the olefin or the polyamide is kneaded with the polybutylene terephthalate to improve the moisture and heat resistance, but a decrease in physical properties due to compatibility problems occurs.
따라서, 본 발명은 충격강도, 인성, 내습열성 및 유동성이 우수한 개량된 폴리부틸렌 테레프탈레이트 수지 조성물을 제공코저 하는 것으로 이를 상세히 설명하면 다음과 같다.Accordingly, the present invention is to provide an improved polybutylene terephthalate resin composition excellent in impact strength, toughness, heat and moisture resistance, and fluidity will be described in detail as follows.
본 발명은, 고유점도 1.2인 폴리부틸렌 테레프탈레이트를 기재로 하여, 여기에 강화제로서 유리섬유, 난연제로서 페녹시 터미네이티드 테트라브로모 비스페놀 A 카보네이트올리고머((phenoxy ternnnatedterabromo bisphenol A carbonate oligomer), 난연조제로서 삼산화안티몬, 충격 강화제로서 디엔(diene)계 고무 존재하에서 아크릴산 에스테르나 메타크릴산 에스테르 중에서 선택된 1종 이상의 모노머와 방향족 비닐 화합물을 공중합시킨 코아-쉘(core-shell) 형태의 공중합체, 에폭시기가 2∼3개인 에폭시 화합물 및 모노옥사졸린을 혼련하여 된 개량된 폴리부틸렌 테레프탈레이트 수지 조성물에 관한 것이다.The present invention is based on polybutylene terephthalate having an inherent viscosity of 1.2, and as a reinforcing agent therein, glass fiber as a reinforcing agent, phenoxy-terminated tetrabromo bisphenol A carbonate oligomer (retardant) Core-shell copolymer and epoxy group copolymerized with an aromatic vinyl compound with at least one monomer selected from acrylic acid esters and methacrylic acid esters in the presence of antimony trioxide as a preparation and a diene rubber as an impact modifier. An improved polybutylene terephthalate resin composition obtained by kneading an epoxy compound having 2 to 3 and a monooxazoline.
상기한 본원 발명에서 사용되는 폴리부틸렌 테레프탈레이트는 1,4-부탄디올과 테레프탈산으로 이루어져 있으며 고유점도가 1.2인 선상 폴리에스테르를 의미한다.The polybutylene terephthalate used in the present invention described above means a linear polyester composed of 1,4-butanediol and terephthalic acid and having an intrinsic viscosity of 1.2.
또한 충격강화제로는 디엔계 고무 존재하에서 탄소수 5∼14인 아크릴산 에스테르 및 메타크릴산 에스테르에서 선택된 1종 이상의 모노머 및 방향족 비닐 화합물을 공중합시킨 코아-켈 형태의 공중합물인데 여기에서 디엔계 고무로서는 폴리부타디엔, 폴리이소프렌에서 아크릴산 에스테르 및 메타크릴산 에스테르는 아크릴산 메틸, 아크릴산 부틸, 메타크릴산 메틸, 메타크릴산 부릴 등에서 선택하는 것이 바람직하며, 방향족비닐 화합물로서는 스타일렌, α-메틸스타일렌에서 선택될 수 있다. 본원 발명 조성물에서 충격강화제의 함량은 폴리부틸렌 테레프탈레이트 100중량%에 대하여 1∼20중량%, 더욱 좋기로는 5∼10중량%이다In addition, the impact modifier is a copolymer of coa-kel type in which at least one monomer selected from acrylic acid ester and methacrylic acid ester having 5 to 14 carbon atoms and aromatic vinyl compound is copolymerized in the presence of diene rubber. In the butadiene and polyisoprene, the acrylic acid ester and the methacrylic acid ester are preferably selected from methyl acrylate, butyl acrylate, methyl methacrylate, buryl methacrylate, and the like, and the aromatic vinyl compound may be selected from styrene and α-methyl styrene. . The content of the impact modifier in the composition of the present invention is 1 to 20% by weight, more preferably 5 to 10% by weight based on 100% by weight of polybutylene terephthalate.
또한 본 발명에 사용된 에폭시기가 2∼3개인 에폭시 화합물을 일반식으로 표시하면 다음과 같다.In addition, when the epoxy compound having 2 to 3 epoxy groups used in the present invention is represented by the general formula is as follows.
R1, R3는 C원자 6∼7개인 아릴기이고 R2는 C원자 7∼8개인 방향촉이며, R4, R6는 수소 혹은 알킬기이고 R5는 에테르(ether)기 및 에스테르기를 함유한 알킬렌, 아릴렌기이며 n은 3∼6의 정수이다.R 1 and R 3 are aryl groups having 6 to 7 C atoms, R 2 are aromatic atoms having 7 to 8 C atoms, R 4 and R 6 are hydrogen or alkyl groups and R 5 contains ether and ester groups. One alkylene and arylene group and n is an integer of 3-6.
이 에폭시 화합물의 함량은 폴리부틸렌 테레프탈레이트 100중량%에 대하여 0.1∼10중량%이며, 더욱 좋기로는 0.5∼5중량%이다.The content of this epoxy compound is 0.1 to 10 wt% with respect to 100 wt% of polybutylene terephthalate, and more preferably 0.5 to 5 wt%.
특히 일반식(I )과 (II)의 비는 10 : 90∼90 : 10이고, 더욱 좋기로는 30:70∼70:30이다.Especially the ratio of general formula (I) and (II) is 10: 90-90: 10, More preferably, it is 30: 70-70: 30.
또한, 상기한 모노옥사졸린은로서 R은 수소 및 알킬기이고, 이 모노옥사졸린의 함량은 폴리부틸렌 테레프탈레이트 100중량%에 대하여 0.1∼1중량%가 좋다. 이 모노옥사졸린은 말단기 -COOH와 반응하여 ∼COONHCOR로 반응이 진행된다.In addition, the above-mentioned monooxazoline R is hydrogen and an alkyl group, and the content of this monooxazoline is preferably 0.1 to 1% by weight relative to 100% by weight of polybutylene terephthalate. The monooxazoline reacts with the terminal group -COOH and proceeds to -COONHCOR.
상기한 난연제인 페녹시 터미네이트 테트라브로모 비스페놀 A 카보네이트 올리고머는 폴리부틸렌 테레프달레이트 100중량%에 대하여 10∼30중량%, 더욱 좋기로는 15∼25중량%이다.The above-described flame retardant phenoxy-terminated tetrabromo bisphenol A carbonate oligomer is 10 to 30% by weight, more preferably 15 to 25% by weight based on 100% by weight of polybutylene terephalate.
상기힌 난연조제인 삼산화안티몬은 상기 폴리부틸렌 테레프탈레이트 수지 100중량%에 대하여 3∼15중량%, 더욱 좋기로는 5∼10중량%이다. 강화제인 유리섬유는 직경이 10∼13μm, 길이가 3∼4mm인 단유리성유를 사용하였으며 함량은 상기 폴리부틸렌 테레프탈레이트 수지 100중량%에 대하여 30∼60중량%를 사용하였다.The antimony trioxide, which is the flame retardant aid, is 3 to 15% by weight, more preferably 5 to 10% by weight, based on 100% by weight of the polybutylene terephthalate resin. As glass fiber as a reinforcing agent, mono-glass oil having a diameter of 10 to 13 μm and a length of 3 to 4 mm was used, and the content thereof was 30 to 60 wt% based on 100 wt% of the polybutylene terephthalate resin.
기타 안정제, 산화 안정제, 이형제, 안료, 무기첨가물 등도 첨가할 수 있다. 이때 함량은 수지 100중량%에 대하여 0.1∼1중량%가 바람직하다.Other stabilizers, oxidation stabilizers, mold release agents, pigments, inorganic additives and the like can also be added. At this time, the content is preferably 0.1 to 1% by weight relative to 100% by weight of the resin.
이상과 같은 조성물의 컴파운딩(compounding)은 이중 나사 압출기(twin extruder, 직경 30mm)를 이용하여 240∼250℃에서, 250rpm으로 압출시켜 펠렛(pellet)을 제조하였다. 이때 폴리부틸렌 테레프탈레이트는 120℃에서 3시간 전조하여 사용하였으며 다른 첨가제들은 건조하지 않고 그대로 사용하였다.Compounding of the composition as described above (compounding) using a twin extruder (twin extruder, diameter 30mm) at 240-250 ° C, extruded at 250rpm to produce a pellet (pellet). At this time, polybutylene terephthalate was used for 3 hours at 120 ℃ and other additives were used as it is without drying.
제조된 펠렛은 5 OZ성형기에서 실린더 온도 245∼255℃로 하고 60∼70kg/㎠의 사출압으로 하여 금형온도는 80℃에서 시편을 성형하였다.The prepared pellets were molded at a temperature of 80 ° C. with a cylinder temperature of 245 to 255 ° C. and an injection pressure of 60 to 70 kg / cm 2 in a 5 OZ molding machine.
제조된 시편으로 인장강도, 신도, 충격강도, 유동성, 내습열성 시험을 하였다.The prepared specimens were tested for tensile strength, elongation, impact strength, fluidity, and heat and moisture resistance.
이상의 컴파운딩 방법에 따라 다음과 같이 본원 발명의 실시예 및 비교예의 수지 조성물대로 실시하여 표 1에 나타난 바와 같은 물성 시험결과를 얻었다.According to the compounding method described above was carried out according to the resin composition of the Examples and Comparative Examples of the present invention as follows to obtain the physical property test results as shown in Table 1.
[실시예 및 비교예][Examples and Comparative Examples]
● 폴리부틸렌 테레프탈레이트 : 제일합섬(주), 고유점도 1.2인 PBT● Polybutylene terephthalate: Cheil Synthetic Co., Ltd., PBT with an inherent viscosity of 1.2
● 난연제 : Great lake사● Flame retardant: Great lake company
● 충격강화제 : 오우화학 KCA 301● Impact Enhancer: OW Chemical KCA 301
● 에폭시(1) : Nippon Kayaku사 EOCN 1020● Epoxy (1): Nippon Kayaku's EOCN 1020
● 에폭시(2) : 금호-shell 화학 Epikote 815● Epoxy (2): Kumho-shell Chemical Epikote 815
● 안정제 CIBA-GEIGY사 B 215● Stabilizer CIBA-GEIGY company B 215
● 이형제 에틸렌 비스스테아린마이드● Release agent ethylene bis stearinamide
[표 1]TABLE 1
* 유동성 측정은 Spira1 시험으로 측정하였다·* Fluidity measurement was measured by Spira1 test
△ : 불량 ○ : 양호 ◎ : 우수△: poor ○: good ◎: excellent
* 내습열성 시험은 120℃, 2atm, 100hrs 후의 물성(인장강도)* Moisture and heat resistance test after 120 ℃, 2atm, 100hrs (tensile strength)
Claims (7)
Priority Applications (1)
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KR1019910009773A KR940006470B1 (en) | 1991-06-13 | 1991-06-13 | Polybuthylene terephthalate compositions |
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KR1019910009773A KR940006470B1 (en) | 1991-06-13 | 1991-06-13 | Polybuthylene terephthalate compositions |
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KR930000602A KR930000602A (en) | 1993-01-15 |
KR940006470B1 true KR940006470B1 (en) | 1994-07-20 |
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KR20040001572A (en) * | 2002-06-28 | 2004-01-07 | 주식회사 삼양사 | Thermoplastic polybutylene terephthalate resinous compositions |
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KR20010107032A (en) * | 2000-05-24 | 2001-12-07 | 김정희 | Functional beverage and aromatic composition containing extracts from Korean medicine, products and manufacturing process thereof |
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KR20040001572A (en) * | 2002-06-28 | 2004-01-07 | 주식회사 삼양사 | Thermoplastic polybutylene terephthalate resinous compositions |
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