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WO2024225686A1 - Composition de résine thermoplastique et article moulé fabriqué à partir de celle-ci - Google Patents

Composition de résine thermoplastique et article moulé fabriqué à partir de celle-ci Download PDF

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Publication number
WO2024225686A1
WO2024225686A1 PCT/KR2024/005128 KR2024005128W WO2024225686A1 WO 2024225686 A1 WO2024225686 A1 WO 2024225686A1 KR 2024005128 W KR2024005128 W KR 2024005128W WO 2024225686 A1 WO2024225686 A1 WO 2024225686A1
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WIPO (PCT)
Prior art keywords
weight
resin composition
thermoplastic resin
polyolefin
ethylene
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PCT/KR2024/005128
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English (en)
Korean (ko)
Inventor
김명훈
박정은
추동휘
Original Assignee
롯데케미칼 주식회사
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Priority claimed from KR1020230056574A external-priority patent/KR20240159365A/ko
Application filed by 롯데케미칼 주식회사 filed Critical 롯데케미칼 주식회사
Publication of WO2024225686A1 publication Critical patent/WO2024225686A1/fr

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  • the present invention relates to a thermoplastic resin composition and a molded article manufactured therefrom.
  • Polycarbonate resin is one of the engineering plastics and is a widely used material in the plastics industry.
  • Polycarbonate resin has a glass transition temperature (Tg) of approximately 150°C due to its bulky molecular structure, such as bisphenol-A, and thus exhibits high heat resistance.
  • Tg glass transition temperature
  • the carbonyl group of the carbonate group has high rotational mobility, which provides flexibility and rigidity to the polycarbonate resin.
  • amorphous polymer it has excellent transparency, impact resistance, and compatibility with other resins.
  • polycarbonate resin has a disadvantage of low fluidity, so it is also widely used in the form of alloys with various resins to improve workability and post-processing.
  • polycarbonate/polyethylene terephthalate alloy resin has excellent durability, formability, heat resistance, and impact resistance, and is applied to a wide range of fields such as electrical/electronic, automobile, construction, and other living materials, and is particularly attracting attention as a material that can replace metal parts when used as an automobile exterior material.
  • polycarbonate/polyethylene terephthalate alloy resins have a problem in that they lack dimensional stability, making it difficult to completely replace metal parts used in automobiles. Accordingly, a method of supplementing dimensional stability by reinforcing mineral fillers in polycarbonate/polyethylene terephthalate alloy resins has been attempted, but this method has a problem in that impact resistance decreases due to reinforcement of mineral fillers.
  • thermoplastic resin composition having excellent impact resistance and dimensional stability.
  • the present invention provides a thermoplastic resin composition having excellent impact resistance and dimensional stability, and a molded product using the same.
  • a thermoplastic resin composition comprising: 100 parts by weight of a base resin including: (A) 50 to 70 parts by weight of a polycarbonate resin; and (B) 30 to 50 parts by weight of a polyethylene terephthalate resin; (C) 10 to 30 parts by weight of a mineral filler; (D) 0.5 to 3 parts by weight of a polyolefin-maleic anhydride graft copolymer; and (E) 1 to 5 parts by weight of an ethylene-methyl acrylate copolymer, wherein a weight ratio of the (D) polyolefin-maleic anhydride graft copolymer to the (E) ethylene-methyl acrylate copolymer is 1:1 to 1:2.
  • the above (A) polycarbonate resin may have a melt flow index of 5 to 30 g/10 min as measured under conditions of 300°C and 1.2 kg weight according to ASTM D1238.
  • the above (B) polyethylene terephthalate resin may have an intrinsic viscosity of 0.7 to 1.5 dl/g as measured according to ASTM D4603.
  • the above (C) mineral filler may be in the form of fine particles or flakes.
  • the above (C) mineral filler may be any one of talc, mica, or a combination thereof.
  • the average particle diameter (D50) of the above (C) mineral filler may be 1 ⁇ m or more and 10 ⁇ m or less.
  • the above (D) polyolefin-maleic anhydride graft copolymer may include 95 to 99 wt% of a substituted or unsubstituted polyolefin-derived component and 1 to 5 wt% of a maleic anhydride-derived component based on the total weight of the (D) polyolefin-maleic anhydride graft copolymer.
  • the above (E) ethylene-methyl acrylate copolymer may contain 50 to 80 wt% of an ethylene-derived component and 20 to 50 wt% of a methyl acrylate-derived component based on the total weight of the (E) ethylene-methyl acrylate copolymer.
  • the thermoplastic resin composition may further include at least one additive selected from a flame retardant, a nucleating agent, a coupling agent, glass fiber, a plasticizer, a lubricant, an antibacterial agent, a release agent, a heat stabilizer, an antioxidant, an ultraviolet stabilizer, an antistatic agent, a pigment, and a dye.
  • at least one additive selected from a flame retardant, a nucleating agent, a coupling agent, glass fiber, a plasticizer, a lubricant, an antibacterial agent, a release agent, a heat stabilizer, an antioxidant, an ultraviolet stabilizer, an antistatic agent, a pigment, and a dye.
  • thermoplastic resin composition a molded product using a thermoplastic resin composition according to one embodiment can be provided.
  • the above molded article may have a notched Izod impact strength of greater than or equal to 8 kgf ⁇ cm/cm at 1/8 inch thickness as measured in accordance with ASTM D256.
  • the above molded product can have a total energy of 48 J or more in a drop impact strength evaluation measured by dropping a 5 kg weight from a height of 1 m onto a 3.2 mm thick flat specimen according to ASTM D1709.
  • thermoplastic resin composition according to one embodiment and the molded article using the same have excellent impact resistance and dimensional stability, and thus can be widely applied to various purposes, and in particular, can be usefully applied to purposes such as automobile exterior materials.
  • Figure 1 shows specific criteria for judging the degree of impact resistance according to the fracture shape of a specimen in the evaluation of falling ball impact strength.
  • a thermoplastic resin composition comprising: 100 parts by weight of a base resin including (A) 50 to 70 parts by weight of a polycarbonate resin; and (B) 30 to 50 parts by weight of a polyethylene terephthalate resin; (C) 10 to 30 parts by weight of a mineral filler; (D) 0.5 to 3 parts by weight of a polyolefin-maleic anhydride graft copolymer; and (E) 1 to 5 parts by weight of an ethylene-methyl acrylate copolymer, wherein a weight ratio of the (D) polyolefin-maleic anhydride graft copolymer to the (E) ethylene-methyl acrylate copolymer is 1:1 to 1:2.
  • the above (A) polycarbonate resin is a polyester having a carbonate bond, and its type is not particularly limited, and any polycarbonate resin available in the field of resin compositions can be used.
  • it can be produced by reacting a compound selected from the group consisting of diphenols represented by the following chemical formula 1 and phosgene, halogen acid esters, carbonic esters, and combinations thereof.
  • Two or more diphenols represented by the above chemical formula 1 may be combined to form a repeating unit of a polycarbonate resin.
  • diphenols include hydroquinone, resorcinol, 4,4'-dihydroxydiphenyl, 2,2-bis(4-hydroxyphenyl)propane (also called 'bisphenol-A'), 2,4-bis(4-hydroxyphenyl)-2-methylbutane, bis(4-hydroxyphenyl)methane, 1,1-bis(4-hydroxyphenyl)cyclohexane, 2,2-bis(3-chloro-4-hydroxyphenyl)propane, 2,2-bis(3-methyl-4-hydroxyphenyl)propane, 2,2-bis(3,5-dimethyl-4-hydroxyphenyl)propane, 2,2-bis(3,5-dichloro-4-hydroxyphenyl)propane, 2,2-bis(3,5-dibromo-4-hydroxyphenyl)propane, Bis(4-hydroxyphenyl)sulfoxide, bis(4-hydroxyphenyl)ketone, bis(4-hydroxyphenyl)ether, etc.
  • 2,2-bis(4-hydroxyphenyl)propane 2,2-bis(3-methyl-4-hydroxyphenyl)propane, 2,2-bis(3,5-dimethyl-4-hydroxyphenyl)propane, 2,2-bis(3,5-dichloro-4-hydroxyphenyl)propane, or 1,1-bis(4-hydroxyphenyl)cyclohexane can be preferably used.
  • 2,2-bis(4-hydroxyphenyl)propane can be more preferably used.
  • the above (A) polycarbonate resin may be a mixture of copolymers prepared from two or more diphenols.
  • the polycarbonate resin may be a linear polycarbonate resin, a branched polycarbonate resin, a polyester carbonate copolymer resin, or the like.
  • a specific example of the linear polycarbonate resin is a bisphenol-A polycarbonate resin.
  • a specific example of the branched polycarbonate resin is a resin produced by reacting a polyfunctional aromatic compound, such as trimellitic anhydride or trimellitic acid, with diphenols and carbonates.
  • the polyester carbonate copolymer resin can be produced by reacting a difunctional carboxylic acid with diphenols and carbonates, and the carbonate used here can be a diaryl carbonate, such as diphenyl carbonate, or ethylene carbonate.
  • the above (A) polycarbonate resin may have a weight average molecular weight of 10,000 to 200,000 g/mol, for example, 14,000 to 50,000 g/mol. When the weight average molecular weight of the above (A) polycarbonate resin is within the above range, excellent impact resistance and fluidity can be obtained.
  • the above (A) polycarbonate resin can be included in an amount of 50 to 70 wt% based on 100 wt% of the base resin including (A) polycarbonate resin and (B) polyethylene terephthalate resin, for example, 50 to 60 wt%, for example, 60 to 70 wt%.
  • the thermoplastic resin composition can exhibit excellent appearance properties and mechanical strength.
  • the above (A) polycarbonate resin may have a melt flow index of 5 to 30 g/10 min, for example, 5 to 25 g/10 min, for example, 5 to 20 g/10 min, as measured under conditions of 300° C. and 1.2 kg weight according to ASTM D1238.
  • the melt flow index of the above (A) polycarbonate resin is within the above range, it may exhibit excellent formability and excellent impact resistance.
  • the polycarbonate resin (A) may be used by mixing two or more polycarbonate resins having different weight average molecular weights or melt flow indices. By mixing and using polycarbonate resins having different weight average molecular weights or melt flow indices, it is easy to control the thermoplastic resin composition to have the desired fluidity.
  • the above (B) polyethylene terephthalate resin can provide excellent chemical resistance, fluidity, and moldability to a thermoplastic resin composition.
  • the above (B) polyethylene terephthalate resin may use a resin obtained by a polycondensation reaction from terephthalic acid or a derivative thereof and ethylene glycol or a derivative thereof, and may include polyethylene terephthalate (PET), glycol-modified polyethylene terephthalate (PETG), polytetramethylene glycol (PTMG), polypropylene glycol (PPG), a copolymer of an aliphatic polyester or an aliphatic polyamide and polyethylene terephthalate (PET), and combinations thereof.
  • PET polyethylene terephthalate
  • PETG glycol-modified polyethylene terephthalate
  • PTMG polytetramethylene glycol
  • PPG polypropylene glycol
  • PET polyethylene terephthalate
  • the (B) polyethylene terephthalate resin may be a regenerated polyethylene terephthalate resin regenerated from waste polyethylene terephthalate resin.
  • the waste polyethylene terephthalate resin refers to a polyethylene terephthalate resin that has been used, such as waste PET bottles, and may be a waste polyethylene terephthalate resin that has been used one or more times.
  • the above (B) polyethylene terephthalate resin may have an intrinsic viscosity of 0.7 to 1.5 dl/g as measured according to ASTM D4603 in order to sufficiently secure impact resistance of a molded product using the thermoplastic resin composition.
  • the (B) polyethylene terephthalate resin may be included in an amount of 30 to 50 wt% based on 100 wt% of the base resin, for example, 30 to 40 wt%.
  • the thermoplastic resin composition has excellent chemical resistance, fluidity, and moldability.
  • (C) the mineral filler can improve the dimensional stability of the thermoplastic resin composition.
  • the above (C) mineral filler may be, for example, in the form of fine particles or flakes.
  • (C) mineral filler mica, quartz powder, titanium dioxide, silicate, aluminosilicate, chalk, wollastonite, mica, layered clay, montmorillonite (especially ion-exchange modified organo-philic form of montmorillonite), talc, kaolin, zeolite, vermiculite, aluminum oxide, silica, magnesium hydroxide, aluminum hydroxide, glass flakes, etc. can be used, and mixtures of different mineral fillers can also be used.
  • the (C) mineral filler may be any one of talc, mica, and combinations thereof, preferably talc.
  • the average particle size of the above (C) mineral filler may be 1 ⁇ m or more, for example, 2 ⁇ m or more, for example, 3 ⁇ m or more, for example, 5 ⁇ m or more, for example, 7 ⁇ m or more, as measured by a particle size analysis device using laser diffraction (for example, a particle size analysis device from Malvern Panalytical) in accordance with ISO 13320-1, as a median value (D50), and may be 10 ⁇ m or less, for example, 8 ⁇ m or less, for example, 5 ⁇ m or less, for example, 4 ⁇ m or less, and may be, for example, 1 to 6 ⁇ m, for example, 2 to 5 ⁇ m.
  • the mechanical strength and appearance of a molded product using the thermoplastic resin composition may be excellent.
  • the above (C) mineral filler may be included in an amount of 10 to 30 parts by weight, for example, 10 to 20 parts by weight, based on 100 parts by weight of the base resin.
  • the thermoplastic resin composition including the (C) mineral filler and the molded product using the same may have excellent dimensional stability, heat resistance, mechanical strength, and appearance.
  • the (D) polyolefin-maleic anhydride graft copolymer is used together with the (E) ethylene-methyl acrylate copolymer described below to impart excellent impact resistance and appearance properties to the thermoplastic resin composition.
  • the (D) polyolefin-maleic anhydride graft copolymer may be one in which maleic anhydride is grafted onto a substituted or unsubstituted polyolefin backbone.
  • olefin constituting the substituted or unsubstituted polyolefin for example, ethylene, propylene, 1-butene, isobutylene, 2-butene, cyclobutene, 1-pentene, 1-hexene, 4-methyl-1-pentene, 1-octene, 3-methyl-1-butene, 4-methyl-1-butene, cyclopentene, 1-hexene, cyclohexene, 1-octene, 1-decene and 1-dodecene, or combinations thereof may be mentioned.
  • the (D) polyolefin-maleic anhydride graft copolymer may comprise 95 to 99 wt% of a substituted or unsubstituted polyolefin-derived component and 1 to 5 wt% of a maleic anhydride-derived component, based on the total weight of the (D) polyolefin-maleic anhydride graft copolymer.
  • the above (D) polyolefin-maleic anhydride graft copolymer may be included in an amount of 0.5 to 3 parts by weight, for example, 1 to 3 parts by weight, for example, 1 to 2 parts by weight, for example, 2 to 3 parts by weight, based on 100 parts by weight of the base resin.
  • the thermoplastic resin composition and the molded article manufactured therefrom may exhibit excellent impact resistance and compatibility.
  • the (E) ethylene-methyl acrylate copolymer is used together with the (D) polyolefin-maleic anhydride graft copolymer to impart excellent impact resistance and appearance properties to the thermoplastic resin composition.
  • the above (E) ethylene-methyl acrylate copolymer may contain 50 to 80 wt% of an ethylene-derived component and 20 to 50 wt% of a methyl acrylate-derived component based on the total weight of the (E) ethylene-methyl acrylate copolymer.
  • the (E) ethylene-methyl acrylate copolymer may be included in an amount of 1 to 5 parts by weight, for example, 2 to 3 parts by weight, based on 100 parts by weight of the base resin. In the above weight range, the impact resistance of the thermoplastic resin composition may be further improved.
  • the weight ratio of the (D) polyolefin-maleic anhydride graft copolymer to the (E) ethylene-methyl acrylate copolymer may be from 1:1 to 1:2.
  • the impact resistance of the thermoplastic resin composition and the molded article manufactured therefrom may be further improved.
  • thermoplastic resin composition may further include, in addition to the components (A) to (E), one or more additives necessary to achieve a balance between properties under conditions of maintaining excellent impact resistance, dimensional stability, etc., or depending on the final use of the thermoplastic resin composition.
  • the additives that can be used include flame retardants, nucleating agents, coupling agents, glass fibers, plasticizers, lubricants, antibacterial agents, release agents, heat stabilizers, antioxidants, ultraviolet stabilizers, antistatic agents, pigments, dyes, etc., and these can be used alone or in combination of two or more.
  • thermoplastic resin composition may be appropriately included within a range that does not impair the properties of the thermoplastic resin composition, and may be included in an amount of 20 parts by weight or less relative to 100 parts by weight of the base resin, but are not limited thereto.
  • thermoplastic resin composition according to the present invention can be produced by a known method for producing a thermoplastic resin composition.
  • thermoplastic resin composition according to the present invention can be manufactured in the form of pellets by mixing the components of the present invention and other additives and then melting/mixing them using an extruder.
  • a molded article according to one embodiment of the present invention can be manufactured from the thermoplastic resin composition described above.
  • the above molded article may have a notched Izod impact strength of greater than or equal to 8 kgf ⁇ cm/cm at 1/8 inch thickness as measured in accordance with ASTM D256.
  • the above molded product can have a total energy of 48 J or more in a drop impact strength evaluation measured by dropping a 5 kg weight from a height of 1 m onto a 3.2 mm thick flat specimen according to ASTM D1709.
  • thermoplastic resin compositions of Examples 1 to 4 and Comparative Examples 1 to 4 were prepared according to the component content ratios described in Table 1 below.
  • (A) and (B) represent the weight % of each component among 100 weight % of the base resin, and (C) to (E) represent the weight parts based on 100 weight parts of the base resin ((A) + (B)).
  • Example 1 Example 2 Example 3
  • Example 4 Comparative Example 1 Comparative Example 2 Comparative Example 3 Comparative Example 4
  • Bisphenol-A polycarbonate resin (Lotte Chemical Co., Ltd.) with a melt flow index of approximately 18 g/10 min measured under conditions of 300°C and 1.2 kg weight according to ASTM D1238
  • Polyethylene terephthalate resin (Lotte Chemical Co., Ltd.) with an intrinsic viscosity of approximately 1.2 dl/g as measured according to ASTM D4603
  • Ethylene-methyl acrylate copolymer containing about 24 wt% methyl acrylate (DOW, AC 12024)
  • Impact strength (unit: kgf ⁇ cm/cm): The notched Izod impact strength was measured at room temperature (approximately 23°C) on a 1/8 inch thick specimen according to ASTM D256.
  • thermoplastic resin composition having excellent impact resistance and dimensional stability and a molded product using the same can be realized.
  • the present example shows a ductile fracture in which the specimen is not broken but only deformed, whereas Comparative Examples 1, 3, and 4 show a brittle fracture in which the specimen is broken or fragmented.

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Abstract

La présente invention concerne une composition de résine thermoplastique et un article moulé l'utilisant, la composition de résine thermoplastique comprenant, par rapport à 100 parties en poids d'une résine de base comprenant (A) entre 50 et 70 % en poids d'une résine de polycarbonate et (B) entre 30 à 50 % en poids d'une résine de poly(téréphtalate d'éthylène) ; (C) entre 10 et 30 parties en poids d'une charge minérale ; (D) entre 0,5 et 3 parties en poids d'un copolymère greffé de polyoléfine-anhydride maléique ; et (E) entre 1 et 5 parties en poids d'un copolymère d'éthylène-acrylate de méthyle, le rapport en poids entre (D) un copolymère greffé de polyoléfine-anhydride maléique et (E) un copolymère d'éthylène-acrylate de méthyle étant de 1 : 1 à 1 : 2.
PCT/KR2024/005128 2023-04-28 2024-04-17 Composition de résine thermoplastique et article moulé fabriqué à partir de celle-ci WO2024225686A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
KR10-2023-0056574 2023-04-28
KR1020230056574A KR20240159365A (ko) 2023-04-28 열가소성 수지 조성물 및 이로부터 제조되는 성형품

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WO2024225686A1 true WO2024225686A1 (fr) 2024-10-31

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Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US7119152B1 (en) * 1999-11-26 2006-10-10 Atofina Thermoplastic polyester compositions having improved impact properties
WO2016108539A1 (fr) * 2014-12-31 2016-07-07 삼성에스디아이 주식회사 Composition de résine de polycarbonate et article moulé comprenant cette composition
KR20170054382A (ko) * 2014-07-14 2017-05-17 버텔러스 홀딩스 엘엘씨 올레핀-말레산 무수물 공중합체들을 이용한 엔지니어링 플라스틱들의 변성
US20180155543A1 (en) * 2015-06-04 2018-06-07 Kaneka Corporation Polycarbonate resin composition having excellent thermal decomposition resistance
US20220033650A1 (en) * 2019-03-28 2022-02-03 Lotte Chemical Corporation Thermoplastic Resin Composition and Molded Article Formed Therefrom

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US7119152B1 (en) * 1999-11-26 2006-10-10 Atofina Thermoplastic polyester compositions having improved impact properties
KR20170054382A (ko) * 2014-07-14 2017-05-17 버텔러스 홀딩스 엘엘씨 올레핀-말레산 무수물 공중합체들을 이용한 엔지니어링 플라스틱들의 변성
WO2016108539A1 (fr) * 2014-12-31 2016-07-07 삼성에스디아이 주식회사 Composition de résine de polycarbonate et article moulé comprenant cette composition
US20180155543A1 (en) * 2015-06-04 2018-06-07 Kaneka Corporation Polycarbonate resin composition having excellent thermal decomposition resistance
US20220033650A1 (en) * 2019-03-28 2022-02-03 Lotte Chemical Corporation Thermoplastic Resin Composition and Molded Article Formed Therefrom

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