KR20010075894A - Thermoplastic resin composition with highly impacted resistance - Google Patents
Thermoplastic resin composition with highly impacted resistance Download PDFInfo
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Abstract
Description
본 발명은 열가소성 수지조성물에 관한 것으로서, 더욱 상세하게는 폴리프로필렌계 수지를 기본수지로 하고, 여기에 보강제로서 스티렌-에틸렌-부틸렌-스티렌 블록공중합체(SEBS) 또는 스티렌-부타디엔-스티렌 블록공중합체와 같은 스티렌계 블록공중합체와 유기화된 몬모릴로나이트를 배합함으로써, 내충격성 및 기계적 물성을 향상시킨 열가소성 수지 조성물에 관한 것이다.The present invention relates to a thermoplastic resin composition, more specifically, a polypropylene-based resin as a base resin, styrene-ethylene-butylene-styrene block copolymer (SEBS) or styrene-butadiene-styrene block The present invention relates to a thermoplastic resin composition in which impact resistance and mechanical properties are improved by blending styrene-based block copolymers such as copolymerized with organic montmorillonite.
폴리프로필렌계 수지는 범용수지로 다른 수지와 비교하여 가격이 저렴함에도 불구하고 내열성, 내화학성 등이 우수하여 다양한 분야에서 적용되고 있다. 그러나, 치수안정성이 좋지 않으며, 기계적 물성에 한계가 있어 적용 범위에 제한이 있는 문제점이 있다.Polypropylene-based resin is a general-purpose resin, but has been applied in various fields due to its excellent heat resistance, chemical resistance, etc., despite being cheaper than other resins. However, there is a problem in that the dimensional stability is not good, there is a limit in the mechanical properties there is a limit to the application range.
한편, 폴리프로필렌 수지의 기계적 강도를 향상시키기 위해 탈크나 유리섬유와 같은 무기물을 첨가하는 방법이 이용되어 왔으나 이러한 무기물들은 폴리프로필렌의 충격강도를 저하시킨다는 문제점이 있다.On the other hand, in order to improve the mechanical strength of the polypropylene resin has been used a method of adding an inorganic material, such as talc or glass fiber, but these inorganic materials have a problem of lowering the impact strength of the polypropylene.
또 다른 폴리프로필렌의 충격강도를 향상시키는 방법으로는 고무성분을 첨가하는 방법이 이용되고 있는데 유연한 고무성분의 첨가로 인하여 기계적인 물성이 크게 저하된다.As a method of improving the impact strength of another polypropylene, a method of adding a rubber component is used, and mechanical properties are greatly reduced due to the addition of a flexible rubber component.
이러한 문제점을 해결하기 위하여 점토 일종인 유기화된 몬모릴로나이트(montmollilonite)와 폴리머를 혼합하여 몬모릴로나이트를 폴리머에 나노사이즈로 분산시키는 나노복합재라는 개념이 도입되었다.In order to solve this problem, the concept of nanocomposite is used to disperse montmorillonite in a nano-sized polymer by mixing a polymer of organic montmorillonite and clay.
몬모릴로나이트는 높은 축비(aspect ratio: 500∼1000)를 가진 대표적인 2:1 스멕타이트(smectite)계 층상점토이다. 몬모릴로나이트의 층간거리 1㎚ 미만 정도이나 양이온의 종류 및 수분함량에 따라 층간거리가 변하게 된다. 구체적으로는, 자연상태에서는 층 사이에 Na+나 Ca2+등이 수분과 같이 존재하며 층간거리가 대략 1㎚ 미만정도 인데, 탄소원자수 6∼18의 암모니윰 유기화제로 양이온 치환반응을 시키면 층간거리가 2∼3㎚인 유기화된 몬모릴로나이트가 생성된다. 이렇게 넓어진 층사이로 고분자가 삽입되어 나노복합재가 형성된다.(Journal of Applied Polymer Science, Vol. 67, 87- (1998)). 이와같이 제조된 나노복합재는 몬모릴리로나이트와 폴리머의 접촉면적이 매우 넓어져 충격강도의 감소없이 기계적강도를 향상시킨다고 알려져 있다. 그러나 몬모릴로나이트가 극성을 가지기 때문에 고분자를 유기화된 몬모릴로나이트의 층사이로 삽입하는 것은 나이론이나 폴리스티렌과 같은 극성고분자의 경우 용이하게 이루어지나, 폴리프로필렌이나 폴리에틸렌과 같은 무극성폴리머들은 삽입이 어렵다고 알려져 있다.(Macromolecules, Vol. 28, 8080-(1995))Montmorillonite is a representative 2: 1 smectite-based layered clay with a high aspect ratio (500-1000). The interlaminar distance of montmorillonite is less than 1 nm, but the interlaminar distance varies depending on the type of cation and water content. Specifically, in the natural state, Na + or Ca 2+ is present between the layers as moisture and the interlayer distance is less than about 1 nm. If the cation substitution reaction is carried out with an ammonia organizing agent having 6 to 18 carbon atoms, Organized montmorillonite with a distance of 2-3 nm is produced. The polymer is intercalated between these widened layers to form a nanocomposite (Journal of Applied Polymer Science, Vol. 67, 87- (1998)). The nanocomposites thus prepared are known to improve the mechanical strength without reducing the impact strength by increasing the contact area between montmorillonite and the polymer. However, because montmorillonite is polar, the insertion of polymers between layers of organicized montmorillonite is easy for polar polymers such as nylon and polystyrene, but it is known that nonpolar polymers such as polypropylene and polyethylene are difficult to insert (Macromolecules, Vol. 28, 8080- (1995))
이에, 본 발명자들은 폴리프로필렌계 수지를 포함하는 열가소성 수지에 있어서, 이들의 내충격성과 기계적물성을 동시에 향상시킬 수 있는 새로운 수지조성물을 제공하고자 예의 연구한 결과, 폴리스티렌이 유기화된 몬모릴로나이트에 용이하게 삽입이 되며, 스티렌-에틸렌-부틸렌-스티렌 블록공중합체(SEBS)나 스티렌-부타디엔-스티렌 블록공중합체와 같은 스티렌계 블록공중합체가 폴리프로필렌의 충격강도를 향상시킨다는 사실로부터, 스티렌-에틸렌-부틸렌-스티렌 블록공중합체(SEBS)와 유기화된 몬모릴로나이트를 1차 혼합한 후 이를 폴리프로필렌에 2차로 배합하는 경우 상기한 목적을 달성할 수 있음을 발견하고 본 발명을 완성하게 되었다.Accordingly, the present inventors have diligently studied to provide a new resin composition capable of simultaneously improving their impact resistance and mechanical properties in a thermoplastic resin including a polypropylene resin. As a result, the polystyrene is easily inserted into the organic montmorillonite. From the fact that styrene-based block copolymers such as styrene-ethylene-butylene-styrene block copolymers (SEBS) or styrene-butadiene-styrene block copolymers improve the impact strength of polypropylene, styrene-ethylene-butylene The present invention has been accomplished by discovering that the first purpose of mixing styrene block copolymer (SEBS) and organicized montmorillonite and then blending it in polypropylene in a second manner can achieve the above object.
따라서, 본 발명의 목적은 내충격성 및 기계적강도가 향상된 폴리프로필렌을 기본수지로 하는 열가소성 수지 조성물을 제공하는 것이다.Accordingly, an object of the present invention is to provide a thermoplastic resin composition based on polypropylene having improved impact resistance and mechanical strength.
이와같은 목적을 달성하기 위한 본 발명의 열가소성 수지조성물은 폴리프로필렌계 수지 100중량부, 스티렌계 블록공중합체 5∼10중량부 및 유기화된 몬모릴로나이트 1∼5중량부를 포함하는 것을 그 특징으로 한다.The thermoplastic resin composition of the present invention for achieving the above object is characterized in that it comprises 100 parts by weight of polypropylene resin, 5 to 10 parts by weight of styrene block copolymer and 1 to 5 parts by weight of organic montmorillonite.
본 발명의 열가소성 수지 조성물에 있어서 기본수지인 폴리프로필렌계 수지는, 그 종류가 특별히 한정되지 않는 바, 예를 들면, 용융흐름지수가 2~15g/10분인폴리프로필렌 수지를 사용할 수 있다.In the thermoplastic resin composition of the present invention, the type of the polypropylene resin that is the basic resin is not particularly limited. For example, a polypropylene resin having a melt flow index of 2 to 15 g / 10 minutes may be used.
본 발명에 따른 열가소성 수지 조성물에서 충격보강제로는 스티렌-에틸렌-부틸렌-스티렌 블록공중합체를 사용한다. 이는 고무성분이므로 충격강도를 향상시킬 수 있고 스티렌블록이 유기화제의 층사이로 용이하게 침투 할 수 있다. 그 종류는 스티렌 함량이 블록공중합체 내에서 20∼40중량부인 것으로 하며 특별히 한정되지 않는다. 스티렌-에틸렌-부틸렌-스티렌 블록공중합체를 보강제로서 지나치게 과량 사용하면 오히려 기본수지의 물성을 저하시킬 우려가 있으므로 폴리프로필렌 수지 100중량부에 대하여 5∼10중량부 되도록 사용하는 것이 바람직하다. 본 발명에서는 스틸렌-에틸렌-부틸렌-스틸렌 블록공중합체 외에도 스티렌-부타디엔-스티렌 블록공중합체를 사용하더라도 동일한 효과를 얻을 수 있다.As the impact modifier in the thermoplastic resin composition according to the present invention, styrene-ethylene-butylene-styrene block copolymer is used. Since it is a rubber component, the impact strength can be improved and the styrene block can easily penetrate between the layers of the organic agent. The type of styrene content is 20 to 40 parts by weight in the block copolymer and is not particularly limited. If excessive use of styrene-ethylene-butylene-styrene block copolymer is used as a reinforcing agent, the physical properties of the basic resin may be rather deteriorated. Therefore, it is preferable to use 5 to 10 parts by weight with respect to 100 parts by weight of polypropylene resin. In the present invention, the same effect can be obtained even if styrene-butadiene-styrene block copolymer is used in addition to the styrene-ethylene-butylene-styrene block copolymer.
본 발명에서 사용된 유기화된 몬모릴로나이트는, 그 종류가 특별히 한정되지 않으며, 예를 들면, 도데실트리메틸암모니윰이나 옥타데실암모니윰등으로 처리된 몬모릴로나이트가 있으며, 그 제조는 통상의 방법에 따른다.The type of organicated montmorillonite used in the present invention is not particularly limited, and examples thereof include montmorillonite treated with dodecyltrimethylammonium, octadecyl ammonium, and the like according to a conventional method.
구체적으로는 Na-몬모릴로나이트 20g을 80℃의 증류수 4L에 분산시킨다. 여기에 도데실트리메틸암모니윰염 7g을 80℃ 증류수 500㎖에 녹인 후 혼합한다. 30분간 교반 후 24시간 방치를 하면 흰색 침전물이 발생한다. 흰색 침전물을 증류수로 2∼3회 세척 후 100℃에서 24시간 건조하면 유기화된 몬모릴로나이트를 얻을 수 있다.Specifically, 20 g of Na-montmorillonite is dispersed in 4 L of distilled water at 80 ° C. Here, 7 g of dodecyl trimethyl ammonium salt is dissolved in 500 ml of distilled water at 80 ° C. and mixed. If left for 24 hours after stirring for 30 minutes, white precipitates are formed. The white precipitate was washed 2-3 times with distilled water and then dried at 100 ° C. for 24 hours to obtain organicated montmorillonite.
이같은 유기화된 몬모릴로나이트는 먼저 스티렌-에틸렌-부틸렌-스티렌 블록공중합체와 1차 혼합한 후 폴리프로필렌 수지와 2차 혼합하는데 1차 혼합시스티렌-에틸렌-부틸렌-스틸렌 블록공중합체에 대한 유기화된 몬모릴로나이트의가 50를 넘으면 가공하기가 힘들어 폴리프로필렌 100 중량부에 대하여 2∼5중량부인 것이 바람직하다.This organicized montmorillonite is first mixed with styrene-ethylene-butylene-styrene block copolymer and then secondly mixed with polypropylene resin to organically mixed with the first mixed cystyrene-ethylene-butylene-styrene block copolymer. When montmorillonite exceeds 50, it is difficult to process and it is preferable that it is 2-5 weight part with respect to 100 weight part of polypropylene.
이하, 각종 실시예를 통하여 본 발명을 보다 구체적으로 설명하면 다음과 같은 바, 본 발명이 실시예에 의해 한정되는 것은 아니다.Hereinafter, the present invention will be described in more detail with reference to various examples as follows. However, the present invention is not limited to the examples.
하기의 실시예 및 비교예에서 채택한 각종 물성 평가 방법은 다음 시험법에 의해 행하였다.Various physical property evaluation methods adopted in the following Examples and Comparative Examples were carried out by the following test method.
(1) 용융흐름지수는 ASTM D-1925법으로, 230℃에서 2.6kg의 추를 사용하여 1분간 흘러나오는 무게를 측정한 후, 10분간 흘러나오는 양으로 환산하여 측정하였다.(1) Melt flow index was measured by ASTM D-1925 method using a weight of 2.6 kg at 230 ° C. for 1 minute and then converted to 10 minutes.
(2) 충격강도는 ASTM D-256법으로, 아이조드 충격시험기를 사용하여 측정하였다.(2) The impact strength was measured by ASTM D-256 method using an Izod impact tester.
(3) 인장물성은 ASTM D-638법으로, 50mm/min의 속도로 측정하였다.(3) Tensile properties were measured at a rate of 50 mm / min by ASTM D-638.
(4) 굴곡물성은 ASTM D-790법으로, 6mm/min의 속도로 측정하였다.(4) Flexural properties were measured at a rate of 6 mm / min by ASTM D-790.
이와같이 얻어진 유기화된 몬모릴로나이트를 다음 실시예 및 비교예에서 사용하였다.The organicized montmorillonite thus obtained was used in the following examples and comparative examples.
(실시예 1)(Example 1)
다음 표 1에 명시된 바와 같이 스티렌-에틸렌-부틸렌-스티렌 블록공중합체(SEBS)와 유기화된 몬모릴로나이트를 200℃에서 소형 이축압출기로 1차 압출한 후, 폴리프로필렌 수지와 혼합하여 이축압출기 내에서 210℃로 2차 용융혼합하여 다이를 통해 스파게티로 토출하였다. 그 다음, 냉각하여 커터로 절단하고 컴파운딩한 칩을 사용하여 220톤 사출성형기에서 수지 온도 210℃로 사출성형하였다.As shown in Table 1, styrene-ethylene-butylene-styrene block copolymer (SEBS) and organicized montmorillonite were first extruded at 200 ° C. with a small twin screw extruder, and then mixed with a polypropylene resin in a twin screw extruder. The secondary melt-mixing was carried out to a spaghetti through the die at ℃. Then, the molds were cooled, cut with a cutter, and then molded using a 220-ton injection molding machine at a resin temperature of 210 deg.
성형된 수지의 용융흐름지수, 충격강도, 인장강도 및 인장신율을 상기 물성측정방법으로 측정하고, 그 결과를 다음 표 1에 나타내었다.Melt flow index, impact strength, tensile strength and tensile elongation of the molded resin were measured by the property measurement method, and the results are shown in Table 1 below.
(실시예 2)(Example 2)
보강제로 스티렌-에틸렌-부틸렌-스티렌 블록공중합체 9중량부와 유기화된 몬모릴로나이트를 5중량부 사용하는 것을 제외하고는 상기 실시예 1과 동일한 방법으로 수지를 성형한 후, 물성측정방법에 따라 물성을 측정하고, 그 결과를 다음 표 1에 나타내었다.After molding the resin in the same manner as in Example 1, except that 9 parts by weight of styrene-ethylene-butylene-styrene block copolymer and 5 parts by weight of organicized montmorillonite were used as a reinforcing agent, Was measured, and the results are shown in Table 1 below.
(실시예 3)(Example 3)
보강제로 유기화된 몬모릴로나이트를 3중량부 사용하고, 스티렌-에틸렌-부틸렌-스티렌 블록공중합체(SEBS)을 5중량부 사용하는 것을 제외하고는 상기 실시예 1과 동일한 방법으로 수지를 성형한 후, 물성측정방법에 따라 물성을 측정하고, 그 결과를 다음 표 1에 나타내었다.After molding the resin in the same manner as in Example 1, except that 3 parts by weight of montmorillonite organicated as a reinforcing agent and 5 parts by weight of styrene-ethylene-butylene-styrene block copolymer (SEBS) were used. The physical properties were measured according to the physical property measurement method, and the results are shown in Table 1 below.
(실시예 4)(Example 4)
보강제로 유기화된 몬모릴로나이트를 3중량부 사용하고, 스티렌-부타디엔-스티렌 블록공중합체(SBS)을 5중량부 사용하는 것을 제외하고는 상기 실시예 1과 동일한 방법으로 수지를 성형한 후, 물성측정방법에 따라 물성을 측정하고, 그 결과를 다음 표 1에 나타내었다.After molding the resin in the same manner as in Example 1, except that 3 parts by weight of the organic montmorillonite as a reinforcing agent, and 5 parts by weight of styrene-butadiene-styrene block copolymer (SBS), The physical properties were measured according to the results, and the results are shown in Table 1 below.
(비교예 1)(Comparative Example 1)
다음 표 1에 명시된 성분 및 함량의 조성물을 헨셀믹서로 혼합한 후, 이축압출기내에서 210℃로 용융혼합하여 다이를 통해 스파게티로 토출하였다. 그 다음, 냉각하여 커터로 절단하고 컴파운딩한 칩을 사용하여 220톤 사출성형기에서 수지 온도 210℃로 사출성형하였다.The compositions of the ingredients and contents specified in the following Table 1 were mixed with a Henschel mixer, melt mixed at 210 ° C. in a twin screw extruder, and discharged through a die to spaghetti. Then, the molds were cooled, cut with a cutter, and then molded using a 220-ton injection molding machine at a resin temperature of 210 deg.
성형된 수지의 용융흐름지수, 충격강도, 인장강도 및 인장신율을 상기 물성측정방법으로 측정하고, 그 결과를 다음 표 1에 나타내었다Melt flow index, impact strength, tensile strength and tensile elongation of the molded resin were measured by the above-described physical property measurement method, and the results are shown in Table 1 below.
(비교예 2)(Comparative Example 2)
보강제로 스티렌-에틸렌-부틸렌-스티렌 블록공중합체 9중량부를 사용하고, 유기화된 몬모릴로나이트를 배합하지 않는다는 것을 제외하고는 상기 비교예 1과 동일한 방법으로 수지를 성형한 후, 물성측정방법에 따라 물성을 측정하고, 그 결과를 다음 표 1에 나타내었다.9 parts by weight of styrene-ethylene-butylene-styrene block copolymer is used as a reinforcing agent, and the resin is molded in the same manner as in Comparative Example 1 except that the organicized montmorillonite is not blended. Was measured, and the results are shown in Table 1 below.
(비교예 3)(Comparative Example 3)
보강제로 유기화된 몬모릴로나이트를 3중량부 사용하고, 스티렌-에틸렌-부틸렌-스티렌 블록공중합체(SEBS)를 배합하지 않는다는 것을 제외하고는 상기 비교예 1과 동일한 방법으로 수지를 성형한 후, 물성측정방법에 따라 물성을 측정하고, 그 결과를 다음 표 1에 나타내었다.Except that 3 parts by weight of montmorillonite organicated as a reinforcing agent was used and styrene-ethylene-butylene-styrene block copolymer (SEBS) was not blended, the resin was measured in the same manner as in Comparative Example 1, and then the physical properties were measured. The physical properties were measured according to the method, and the results are shown in Table 1 below.
(비교예 4)(Comparative Example 4)
보강제로 탈크를 3중량부 사용하고 스티렌-에틸렌-부틸렌-스티렌 블록공중합체(SEBS)를 배합하지 않는다는 것을 제외하고는 상기 비교예 1과 동일한 방법으로 수지를 성형한 후, 물성측정방법에 따라 물성을 측정하고, 그 결과를 다음 표 1에 나타내었다.Except that 3 parts by weight of talc is used as a reinforcing agent and styrene-ethylene-butylene-styrene block copolymer (SEBS) is not blended, the resin was molded in the same manner as in Comparative Example 1, and then the physical properties were measured. Physical properties were measured, and the results are shown in Table 1 below.
(비교예 5)(Comparative Example 5)
보강제로 탈크 3중량부와 스티렌-에틸렌-부틸렌-스티렌 블록공중합체(SEBS) 9중량부를 사용한다는 것을 제외하고는 상기 비교예 1과 동일한 방법으로 수지를 성형한 후, 물성측정방법에 따라 물성을 측정하고, 그 결과를 다음 표 1에 나타내었다.Except for using 3 parts by weight of talc and 9 parts by weight of styrene-ethylene-butylene-styrene block copolymer (SEBS) as a reinforcing agent, after molding the resin in the same manner as in Comparative Example 1, Was measured, and the results are shown in Table 1 below.
(비교예 6)(Comparative Example 6)
보강제를 사용하지 않는다는 것을 제외하고는 상기 비교예 1과 동일한 방법으로 수지를 성형한 후, 물성측정방법에 따라 물성을 측정하고, 그 결과를 다음 표 1에 나타내었다.Except not using a reinforcing agent, after molding the resin in the same manner as in Comparative Example 1, the physical properties were measured according to the physical property measurement method, the results are shown in Table 1 below.
이상에서 설명한 바와 같이, 폴리프로필렌계 수지를 기본 수지로 하는 열가소성 수지에 보강제로 유기화된 몬모릴로나이트와 스티렌계 블록공중합체를 배합한 경우, 충격강도와 기계적인 강도를 동시에 향상시킬 수 있는 효과를 얻을 수 있다.As described above, when montmorillonite and styrene-based block copolymers organicized as a reinforcing agent are mixed with a thermoplastic resin based on a polypropylene resin as a base resin, an effect of simultaneously improving impact strength and mechanical strength can be obtained. have.
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| KR100411863B1 (en) * | 2000-12-21 | 2003-12-18 | 금호석유화학 주식회사 | Method to prepare styrene type block copolymer nanocomposites |
| KR20190057719A (en) * | 2017-11-20 | 2019-05-29 | (주)태영필트레이션시스템 | Membrane filter plate for filter press with improved durability and mechanical property |
| US10844207B2 (en) | 2014-06-26 | 2020-11-24 | Lotte Chemical Corporation | Thermoplastic elastomer composition having advanced vibration isolation and thermal resistance, and molded article manufactured therefrom |
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| US10844207B2 (en) | 2014-06-26 | 2020-11-24 | Lotte Chemical Corporation | Thermoplastic elastomer composition having advanced vibration isolation and thermal resistance, and molded article manufactured therefrom |
| KR20190057719A (en) * | 2017-11-20 | 2019-05-29 | (주)태영필트레이션시스템 | Membrane filter plate for filter press with improved durability and mechanical property |
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