CN102604299A - Thermoplastic resin blend with weather resistance, scratch resistance, high gloss and high heat resistance and preparation method of the resin blend - Google Patents
Thermoplastic resin blend with weather resistance, scratch resistance, high gloss and high heat resistance and preparation method of the resin blend Download PDFInfo
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- CN102604299A CN102604299A CN2012100374369A CN201210037436A CN102604299A CN 102604299 A CN102604299 A CN 102604299A CN 2012100374369 A CN2012100374369 A CN 2012100374369A CN 201210037436 A CN201210037436 A CN 201210037436A CN 102604299 A CN102604299 A CN 102604299A
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- styrene
- acrylonitrile
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
- B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
- B29C48/00—Extrusion moulding, i.e. expressing the moulding material through a die or nozzle which imparts the desired form; Apparatus therefor
- B29C48/25—Component parts, details or accessories; Auxiliary operations
- B29C48/92—Measuring, controlling or regulating
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
- B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
- B29C48/00—Extrusion moulding, i.e. expressing the moulding material through a die or nozzle which imparts the desired form; Apparatus therefor
- B29C48/25—Component parts, details or accessories; Auxiliary operations
- B29C48/36—Means for plasticising or homogenising the moulding material or forcing it through the nozzle or die
- B29C48/395—Means for plasticising or homogenising the moulding material or forcing it through the nozzle or die using screws surrounded by a cooperating barrel, e.g. single screw extruders
- B29C48/40—Means for plasticising or homogenising the moulding material or forcing it through the nozzle or die using screws surrounded by a cooperating barrel, e.g. single screw extruders using two or more parallel screws or at least two parallel non-intermeshing screws, e.g. twin screw extruders
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
- B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
- B29C48/00—Extrusion moulding, i.e. expressing the moulding material through a die or nozzle which imparts the desired form; Apparatus therefor
- B29C48/25—Component parts, details or accessories; Auxiliary operations
- B29C48/78—Thermal treatment of the extrusion moulding material or of preformed parts or layers, e.g. by heating or cooling
- B29C48/875—Thermal treatment of the extrusion moulding material or of preformed parts or layers, e.g. by heating or cooling for achieving a non-uniform temperature distribution, e.g. using barrels having both cooling and heating zones
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
- B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
- B29C2948/00—Indexing scheme relating to extrusion moulding
- B29C2948/92—Measuring, controlling or regulating
- B29C2948/92504—Controlled parameter
- B29C2948/92704—Temperature
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
- B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
- B29C2948/00—Indexing scheme relating to extrusion moulding
- B29C2948/92—Measuring, controlling or regulating
- B29C2948/92819—Location or phase of control
- B29C2948/92857—Extrusion unit
- B29C2948/92876—Feeding, melting, plasticising or pumping zones, e.g. the melt itself
- B29C2948/92895—Barrel or housing
Abstract
The invention discloses a thermoplastic resin blend with weather resistance, scratch resistance, high gloss and high heat resistance and a preparation method of the resin blend. The thermoplastic resin blend comprises the following components by weight: 33-80% of poly(methyl methacrylate) (PMMA); 10-30% of a flexibilizer, 0-50% of a binary copolymer of styrene-acrylonitrile/maleic anhydride, 0.5-1.5% of a lubricant, 0.3-0.8% of an antioxidant, and 0-2% of a light stabilizer. PMMA is added, so that the thermoplastic blend is improved in gloss and scratch resistance when compared with ordinary ABS (acrylonitrile-butadiene-styrene)/AAS (acrylic acrylonitrile styrene) /AES (acrylonitrile ethylene styrene) /ACS (acrylonitrile-chlorinated polyethylene-styrene) resin. Saturated rubber free from C=C double bonds is used as the flexibilizer, so that the thermoplastic blend is improved in weather resistance when compared with PMMA/ABS alloy. The binary copolymer of styrene-acrylonitrile/maleic anhydride is added so that the rigidity and high-temperature resistance of the thermoplastic blend are improved.
Description
Technical field
The present invention relates to a kind of thermoplastic resin composition.
Background technology
PMMA (polymethyl methacrylate), promptly polymethylmethacrylate has another name called " synthetic glass ", " acrylic "; Have splendid transparency and scratch resistance, high, the good weatherability of while intensity, still; PMMA poor toughness, processibility are not good, have limited its application.
Have many can well when keeping its advantage, remedy its shortcoming through the method for preparing the PMMA polyblend as far as possible, like the PMMA/ABS alloy.This alloy passes through PMMA and ABS blend; Make it both keep the advantage of PMMA damage resistant, high gloss; Introduced again the ABS material good toughness, be easy to the characteristics of machine-shaping, so replace the technology of spraying paint in recent years in fields such as household electrical appliance, electronic product casings, use very extensive.But, from essence, the same divinyl rubber toughened system that all belongs to of PMMA/ABS alloy with the ABS material since the C=C key existence, be prone to be heated, influence such as light and variable color, weathering resistance is bad.
From structure, improve the ABS weathering resistance and need remove the divinyl rubber that contains the two keys of C=C, with the high functional rubber replacement of other special construction.Common in the market said material has; Acrylonitrile-acrylate-styrene (AAS), acrylonitrile-styrene-terpolymer EP rubber (AES) and acrylonitrile-styrene-chlorinatedpolyethylene (ACS) etc. are respectively as toughner with esters of acrylic acid rubber, terpolymer EP rubber and chlorinatedpolyethylene.The same with ABS, AAS, AES and ACS are to be external phase with SAN, and toughness reinforcing rubber grain is the sea-island structure of disperse phase.Compare with ABS, their its mechanical property and processibility are fine equally; Simultaneously, weathering resistance improves a lot.
Therefore; With resin alloys such as PMMA and AAS/AES; Simultaneously; If added some rigidity, resistant to elevated temperatures material (like styrene-acrylonitrile/maleic anhydride copolymer) again possibly obtain to have that weathering resistance is good, mechanical property is balanced, scrape resistant, high gloss, have the high and processing characteristics excellent material of heat resisting temperature simultaneously concurrently.
Summary of the invention
The purpose of this invention is to provide a kind of have excellent weathering resistance, scratch resistance, high gloss, can have the thermoplastic resin composition of high heat-resistant quality simultaneously.The household appliances that this thermoplastic resin can be applicable to weathering resistance, surface hardness and glossiness are had higher requirements, material of construction etc.
Another object of the present invention provides the preparation method of said thermoplastic resin composition.
Above-mentioned purpose of the present invention is achieved through following technical scheme:
A kind of thermoplastic resin composition, form by the component of following weight percentage:
Polymethylmethacrylate 33-80%;
Toughner 10-30%;
Styrene-acrylonitrile/maleic anhydride copolymer 0-50%;
Lubricant 0.5-1.5%;
Oxidation inhibitor 0.3-0.8%;
Photostabilizer 0-2%.
As a kind of preferred version, said polymethylmethacrylate (PMMA) specific density is preferably 1.18-1.20g/cm
3, pencil hardness is preferably 2H/500g, and under 230 ℃/3.8kg condition, its melt-flow coefficient is preferably 1-30g/10min.
Said toughner is preferably acrylonitrile-acrylate-styrene (AAS) or acrylonitrile-styrene-terpolymer EP rubber (AES), any one or its mixture wherein, and rubber content is preferably 30-80 weight % in the said AAS/AES resin.
Said styrene-acrylonitrile/maleic anhydride copolymer is any one or a two or more mixture in styrene-acrylonitrile copolymer or the styrene-maleic anhydride copolymer.
Said lubricant is one or more the mixture in ethylene bis stearamide, Magnesium Stearate or the pentaerythritol stearate.
Said oxidation inhibitor is one or more the mixture in Hinered phenols antioxidant or the phosphite ester kind antioxidant.
Said photostabilizer is one or more the mixture in benzotriazole category light absorber or the hindered amine light stabilizer.
Described compsn also can comprise other tinting material, filler etc.
The preparation method of above-mentioned thermoplastic resin composition comprises the steps:
(1) takes by weighing various raw materials;
(2) with polymethylmethacrylate, styrene-acrylonitrile/maleic anhydride copolymer in super mixer premix 2-5 minute, and then add toughner, lubricant, oxidation inhibitor and photostabilizer, remix 2-5 minute, obtain mixed raw materials;
(3) mixed raw materials is placed twin screw extruder, through melt extrude, tie rod, water-cooled, pelletizing.
In the step (3), said extrusion temperature is 80-220 ℃.
As a kind of preferred version, in the step (3), said extruding, each barrel temperature is preferably: 80 ℃ of district's temperature; 200 ℃ of two district's temperature, 210 ℃ of three district's temperature, 210 ℃ of four district's temperature, 210 ℃ of five district's temperature; 210 ℃ of six district's temperature, 210 ℃ of seven district's temperature, 210 ℃ of eight district's temperature; 210 ℃ of nine district's temperature, 210 ℃ of ten district's temperature, 220 ℃ of head temperatures.
Compared with prior art, the present invention has following beneficial effect:
(1) among the present invention, the adding of PMMA makes this thermoplastic blend with respect to common ABS/AAS/AES/ACS resin, is improving a lot aspect glossiness, the scrape resistant degree;
(2) among the present invention, do not contain C=C saturation of double bonds rubber and do toughner, make this thermoplastic blend, aspect weather-proof, be significantly increased with respect to common PMMA/ABS alloy owing to adopted;
(3) among the present invention, the adding of styrene-acrylonitrile/maleic anhydride copolymer can make the rigidity of this thermoplastic blend, high thermal resistance be improved.
Description of drawings
Fig. 1 is the performance test data of each embodiment sample.
Embodiment
Come further to explain the present invention below in conjunction with embodiment, but embodiment does not do any type of qualification to the present invention.
The experimental technique of unreceipted actual conditions in the following example, usually according to normal condition, or the condition of advising according to manufacturer.Ratio and per-cent are based on weight, unless stated otherwise.
Polymethylmethacrylate (PMMA) select for use melting index 15-20g/10min (230 ℃/3.8kg), density is at 1.19g/cm
3Marketable material, strange U.S.A provides by Taiwan; It is that 60-75%, acrylonitrile content are the AS resin of 25%-40% that styrene-acrylonitrile copolymer is selected styrene content for use, is provided by Korea S Jin Hu; It is 20-30% that styrene-maleic anhydride copolymer is selected maleic anhydride content for use, and weight-average molecular weight is 80-130kg/mol, is provided by Polyscope Polymer Company; It is that 50-58%, glue content are the ABS of 21%-26% that ABS resin is selected styrene content for use, and strange U.S.A provides by Taiwan; AES selects the import resin of glue content at 65-75% for use, is provided by UMG company; AAS selects the import resin of glue content at 55-65% for use, is provided by Polyone company; Lubricant is selected home-made ethylene bis stearic acid amide (EBS) for use, is provided by rich commerce and trade ltd of Beijing Star; Oxidation inhibitor selects for use antioxidant 1010 that Shanghai Ciba company produces and oxidation inhibitor 168 by weight the composite mixture that forms of 1:2; Photostabilizer selects for use benzotriazole category light absorber and hindered amine light stabilizer by weight the composite mixture that forms of 1:1.
The product blend preparation method:
At first each component of each Comparative Examples/embodiment is successively added by proportioning and carries out uniform mixing in the high-speed mixer, then with said mixture send into mixing in the twin screw extruder, extrude, tie rod, water-cooled, pelletizing; Wherein, the length-to-diameter ratio of twin screw extruder is 40:1; The barrel temperature is set at: 80 ℃ of district's temperature, 200 ℃ of two district's temperature, 210 ℃ of three district's temperature, 210 ℃ of four district's temperature; 210 ℃ of five district's temperature, 210 ℃ of six district's temperature, 210 ℃ of seven district's temperature, 210 ℃ of eight district's temperature; 210 ℃ of nine district's temperature, 210 ℃ of ten district's temperature, 220 ℃ of head temperatures; Screw speed is 450 rev/mins.
The product performance testing method:
Table 1 performance test methods
Embodiment 1-6 and Comparative Examples 1-2
With the proportioning described in the table 2 according to above-mentioned product blend preparation method extruding pelletization.
Each concrete proportioning (wt%) of forming among each embodiment of table 2
? | Comparative Examples 1 | Comparative Examples 2 | |
Embodiment 2 | Embodiment 3 | Embodiment 4 | Embodiment 5 | Embodiment 6 |
PMMA | ? | ? | 90 | 80 | 60 | 33 | 60 | 55 |
AS | 80 | 70 | ? | ? | ? | 50 | ? | 15 |
SMA | ? | ? | ? | ? | ? | ? | 20 | ? |
AES | 20 | ? | 10 | 20 | 20 | 17 | 20 | ? |
AAS | ? | 30 | ? | ? | 20 | ? | ? | 30 |
Lubricant EBS | 0.5 | 0.5 | 0.5 | 0.5 | 0.5 | 0.5 | 0.5 | 0.5 |
Antioxidant 1010+168 | 0.3 | 0.3 | 0.3 | 0.3 | 0.3 | 0.3 | 0.3 | 0.3 |
Above-mentioned each routine prepared blend is injection molded into the standard batten of testing usefulness by standard size earlier, carries out each performance test by the testing standard shown in the above-mentioned table 1 then; The performance test data of each routine sample is seen shown in the table 3.
The performance test data of each embodiment sample of table 3
Performance index | Comparative Examples 1 | Comparative Examples 2 | |
Embodiment 2 | Embodiment 3 | Embodiment 4 | Embodiment 5 | Embodiment 6 |
Tensile strength (mPa) | 49 | 47 | 62 | 51 | 41 | 53 | 47 | 52 |
Flexural strength (mPa) | 75 | 67 | 87 | 80 | 57 | 75 | 74 | 61 |
IZOD notched Izod impact strength (J/m) | 97 | 130 | 52 | 87 | 167 | 94 | 69 | 124 |
The surface pencil hardness | B | 2B | H | H | HB | F | H | F |
Surface gloss (GU) | 67.2 | 68.3 | 85.8 | 81.2 | 74.1 | 78.8 | 79.5 | 78.1 |
Vicat softening point (℃) | - | - | - | 80.1 | - | 88.3 | 90.8 | - |
Visible by table 2 and table 3, compare with general A ES/AAS resin, all be significantly improved by glossiness, the surface hardness of the corresponding blend of the present invention's preparation, simultaneously, the adding of AS/SMA can significantly improve the intensity/high thermal resistance of this blend.
Embodiment 7-9 and Comparative Examples 3:
With the proportioning described in the table 4 according to above-mentioned product blend preparation method extruding pelletization.
Each concrete proportioning (wt%) of forming among each embodiment of table 4
? | Comparative Examples 3 | Embodiment 7 | Embodiment 8 | Embodiment 9 |
PMMA | 50 | 60 | 60 | 60 |
AS | ? | 20 | 20 | ? |
SMA | ? | ? | ? | 20 |
AES | ? | ? | 20 | 20 |
AAS | ? | 20 | ? | ? |
ABS | 50 | ? | ? | ? |
Lubricant EBS | 0.5 | 0.5 | 0.5 | 0.5 |
Antioxidant 1010+168 | 0.3 | 0.3 | 0.3 | 0.3 |
|
1 | 1 | 1 | 1 |
Above-mentioned each routine prepared blend is injection molded into the colour table of testing usefulness earlier, then by the testing method measuring colour difference shown in the above-mentioned table 1; The performance test data of each routine sample is seen shown in Figure 1.Visible from Fig. 1, with conventional P MMA/ABS alloy phase ratio, the colour-change of thermoplastic resin composition of the present invention is little a lot, and the time is long more obvious more, and weather resistance is excellent.
Claims (10)
1. thermoplastic resin composition is characterized in that being made up of the component of following weight percentage:
Polymethylmethacrylate 33-80%;
Toughner 10-30%;
Styrene-acrylonitrile/maleic anhydride copolymer 0-50%;
Lubricant 0.5-1.5%;
Oxidation inhibitor 0.3-0.8%;
Photostabilizer 0-2%.
2. thermoplastic resin composition as claimed in claim 1 is characterized in that, the specific density of said polymethylmethacrylate is 1.18-1.20g/cm
3, pencil hardness is 2H/500g, under 230 ℃/3.8kg condition, its melt-flow coefficient is 1-30g/10min.
3. thermoplastic resin composition as claimed in claim 1 is characterized in that, said toughner is a kind of or its mixture in acrylonitrile-acrylate-styrene or the acrylonitrile-styrene-terpolymer EP rubber; Rubber content is 30-80 weight % in said acrylonitrile-acrylate-styrene or the acrylonitrile-styrene-terpolymer EP rubber.
4. thermoplastic resin composition as claimed in claim 1 is characterized in that, said styrene-acrylonitrile/maleic anhydride copolymer is a kind of or its mixture in styrene-acrylonitrile copolymer or the styrene-maleic anhydride copolymer.
5. thermoplastic resin composition as claimed in claim 1 is characterized in that, said lubricant is one or more the mixture in ethylene bis stearamide, Magnesium Stearate or the pentaerythritol stearate.
6. thermoplastic resin composition as claimed in claim 1 is characterized in that, said oxidation inhibitor is one or more the mixture in Hinered phenols antioxidant or the phosphite ester kind antioxidant.
7. thermoplastic resin composition as claimed in claim 1 is characterized in that, said photostabilizer is one or more the mixture in benzotriazole category light absorber or the hindered amine light stabilizer.
8. the preparation method of the described thermoplastic resin composition of claim 1 is characterized in that comprising the steps:
(1) takes by weighing various raw materials;
(2) with polymethylmethacrylate, styrene-acrylonitrile/maleic anhydride copolymer in super mixer premix 2-5 minute, and then add toughner, lubricant, oxidation inhibitor and photostabilizer, remix 2-5 minute, obtain mixed raw materials;
(3) mixed raw materials is placed twin screw extruder, through melt extrude, tie rod, water-cooled, pelletizing.
9. preparation method as claimed in claim 8 is characterized in that, the said extrusion temperature of step (3) is 80-220 ℃.
10. preparation method as claimed in claim 9 is characterized in that, said each the barrel temperature extruded of step (3) is: 80 ℃ of district's temperature, 200 ℃ of two district's temperature; 210 ℃ of three district's temperature, 210 ℃ of four district's temperature, 210 ℃ of five district's temperature; 210 ℃ of six district's temperature, 210 ℃ of seven district's temperature, 210 ℃ of eight district's temperature; 210 ℃ of nine district's temperature, 210 ℃ of ten district's temperature, 220 ℃ of head temperatures.
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Cited By (17)
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CN103289289A (en) * | 2013-02-28 | 2013-09-11 | 章磊 | Novel ABS-PMMA composite material |
CN103740018A (en) * | 2013-12-17 | 2014-04-23 | 宁波韦邦展示道具有限公司 | Cigarette display stand and preparation method thereof |
CN103804898A (en) * | 2014-02-28 | 2014-05-21 | 长城汽车股份有限公司 | Composite material for peripheral interior trim part of automobile instrument panel and preparation method |
CN104072923A (en) * | 2014-06-18 | 2014-10-01 | 金发科技股份有限公司 | High-heat-resistant transparent reinforcing material as well as preparation method and application thereof |
CN104497461A (en) * | 2014-12-15 | 2015-04-08 | 上海锦湖日丽塑料有限公司 | Heat-resistant scratch-resistant high-transmittance PMMA alloy resin composition and preparation method thereof |
CN105504626A (en) * | 2016-01-06 | 2016-04-20 | 金发科技股份有限公司 | PMMA/PVC alloy material and preparing method thereof |
CN107254131A (en) * | 2017-07-01 | 2017-10-17 | 合肥会通新材料有限公司 | A kind of solvent resistance bloom exempts from spraying PMMA alloy material and preparation method thereof |
CN107418082A (en) * | 2017-06-21 | 2017-12-01 | 安徽江淮汽车集团股份有限公司 | A kind of wear-resisting heat conduction ACS composites and preparation method thereof |
CN107936436A (en) * | 2017-12-22 | 2018-04-20 | 鄢海军 | A kind of PMMA materials of scratch-resistant and preparation method thereof |
CN108559184A (en) * | 2018-01-11 | 2018-09-21 | 湖南盛亚体育实业有限公司 | Environment-friendly type ethylene propylene diene rubber particle and preparation method thereof |
CN108976687A (en) * | 2018-06-20 | 2018-12-11 | 安徽江淮汽车集团股份有限公司 | A kind of AES-PMMA composite material and preparation method |
CN109790296A (en) * | 2016-08-10 | 2019-05-21 | Sabic环球技术有限责任公司 | Polymer composition comprising (methyl) acrylic acid series polymeric compounds |
CN109810441A (en) * | 2019-01-22 | 2019-05-28 | 重庆鑫翎创福光电科技股份有限公司 | Outdoor light conducting plate made from a kind of anti-aging polymethylmethacrylacomposition composition, preparation method and combinations thereof |
CN112745620A (en) * | 2020-12-29 | 2021-05-04 | 江阴市羽项汽车饰件有限公司 | Environment-friendly paint-spraying-free highlight AES/PMMA alloy grid and preparation method thereof |
CN112745616A (en) * | 2020-12-28 | 2021-05-04 | 中化学科学技术研究有限公司 | Modified acrylic ester polymer composition |
CN115304880A (en) * | 2022-08-31 | 2022-11-08 | 宁波恒拓高分子材料有限公司 | Transparent automobile logo material capable of resisting temperature of above 110 ℃ and preparation method thereof |
CN115772325A (en) * | 2022-11-29 | 2023-03-10 | 上海金发科技发展有限公司 | Good electrostatic spraying PC/ABS composition and preparation method and application thereof |
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CN103289289A (en) * | 2013-02-28 | 2013-09-11 | 章磊 | Novel ABS-PMMA composite material |
CN103740018A (en) * | 2013-12-17 | 2014-04-23 | 宁波韦邦展示道具有限公司 | Cigarette display stand and preparation method thereof |
CN103804898A (en) * | 2014-02-28 | 2014-05-21 | 长城汽车股份有限公司 | Composite material for peripheral interior trim part of automobile instrument panel and preparation method |
CN104072923A (en) * | 2014-06-18 | 2014-10-01 | 金发科技股份有限公司 | High-heat-resistant transparent reinforcing material as well as preparation method and application thereof |
CN104497461A (en) * | 2014-12-15 | 2015-04-08 | 上海锦湖日丽塑料有限公司 | Heat-resistant scratch-resistant high-transmittance PMMA alloy resin composition and preparation method thereof |
CN105504626A (en) * | 2016-01-06 | 2016-04-20 | 金发科技股份有限公司 | PMMA/PVC alloy material and preparing method thereof |
CN109790296A (en) * | 2016-08-10 | 2019-05-21 | Sabic环球技术有限责任公司 | Polymer composition comprising (methyl) acrylic acid series polymeric compounds |
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