CN1159379C - Toughened polystyrene and its preparing process - Google Patents
Toughened polystyrene and its preparing process Download PDFInfo
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Abstract
The present invention provides toughened polystyrene obtained through melt blending of polystyrene and a toughening component and a preparation method thereof. In the present invention, the toughening component is powdered rubber in a crosslinked structure, the average particle diameter of the powdered rubber is not larger than 0.5 mu m, or the toughening component is prepared by mixing the powdered rubber and at least one of the following substances: unvulcanized rubber and a thermoplastic elastomer. The form and the particle diameter distribution of a rubber phase contained in the toughened polystyrene can be controlled by changing the particle diameter of the mixed-in powdered rubber in the crosslinked structure or selecting the proper unvulcanized rubber or the proper thermoplastic elastomer. The toughened polystyrene has the advantages of high toughness, good processing performance, high strength maintenance and high rigidity maintenance.
Description
The present invention relates to toughened plastics, specifically, the present invention relates to enhancing touthness of polyphenylethylene by adding and preparation method thereof.
Polystyrene plastic has advantages such as high rigidity, easy dyeing and easy processing forming, and it more and more is subject to people's attention as a kind of widely used material.But because polystyrene belongs to brittle plastic, erosion-resisting characteristics is lower, has limited its application aspect the high-impact goods.In order to improve the toughness of polystyrene, often adopt polymerization or blending method in the prior art.Polymerization is to adopt the method that adds rubber in polystyrene polymeric process, as cis-1,4-polybutadiene rubber is dissolved in the styrene monomer, adopts the polymeric method to make at last and contains the toughness reinforcing high-impact polystyrene of rubber particles that contains structure.But this method processing condition are harsh.Sometimes the rubber that adds in polymerization process occurs excessively crosslinked easily, influences toughening effect.Blending method is the method that adopts rubber and polystyrene melt blending, and it is toughness reinforcing promptly to add unvulcanized thermoplastic elastic body p-poly-phenyl ethene, for example adopts styrene-butadiene rubber(SBR) to come enhancing touthness of polyphenylethylene by adding.Because the form of rubber particles in polystyrene substrate and distribution have a significant impact toughening effect, this method is difficult to the dispersion state of rubber in polystyrene substrate effectively controlled, so toughening effect is not really desirable, and in order to reach required toughness index, usually need add more rubber, thereby can make the performance loss such as intensity, rigidity of polystyrene bigger.
The inventor is on the basis of blending method enhancing touthness of polyphenylethylene by adding plastics, find by great deal of experimental, adopt the powdered rubber with crosslinking structure of small particle size or this powdered rubber to mix to make to be used for enhancing touthness of polyphenylethylene by adding, can reach good toughening effect with unvulcanized rubber, thermoplastic elastomer.
The purpose of this invention is to provide above-described this enhancing touthness of polyphenylethylene by adding, maintain higher intensity and rigidity when it has excellent toughness.
Another object of the present invention provides the preparation method of described enhancing touthness of polyphenylethylene by adding.
Enhancing touthness of polyphenylethylene by adding of the present invention is to comprise polystyrene and toughness reinforcing component melts blend and get.Wherein toughness reinforcing component is that median size is 0.02 μ m～0.5 μ m, the powdered rubber that is preferably 0.05 μ m～0.3 μ m, has crosslinking structure; Or toughness reinforcing component mixed with unvulcanized rubber and/or thermoplastic elastomer by this kind powdered rubber and forms, and wherein unvulcanized rubber and thermoplastic elastomer proportioning arbitrarily mix.The weight ratio of toughness reinforcing component and plastics is 5: 95～40: 60, is preferably 10: 90～30: 70.Wherein to account for the weight percentage of toughness reinforcing component be 30%～100% to powdered rubber, is preferably 50%～100%.
Polystyrene as enhancing touthness of polyphenylethylene by adding main body plastics of the present invention comprises various types of polystyrene, as general purpose polystyrene, high-impact polystyrene etc.
The powdered rubber that has crosslinking structure in the toughness reinforcing component of enhancing touthness of polyphenylethylene by adding of the present invention is preferably the rubber particles of equal phase structure, and its gel content is in 60% weight or higher, preferred 80% weight or higher.
This kind powdered rubber preferably adopts the prepared fully vulcanized powder rubber of the Chinese patent application submitted on December 3rd, 1999 according to the applicant 99125530.5.Preferentially select the fully vulcanized powder rubber good with the polystyrene consistency in preparation process for use, it comprises at least a of following fully vulcanized powder rubber: form of finely divided powder, mehtod natural rubber, form of finely divided powder, mehtod styrene-butadiene rubber(SBR), form of finely divided powder, mehtod polybutadiene rubber or fully sulfurized silicon rubber powder etc.This kind fully vulcanized powder rubber is meant that gel content reaches 60% weight or higher, and more excellent is 75% weight or higher, and need not with separant after the drying is free flowable rubber micro mist.The particle diameter of this powdered rubber is 0.02 μ m～2 μ m, is preferably 0.03 μ m～1.5 μ m, and more excellent is 0.05 μ m～0.5 μ m.Each particulate in this fully vulcanized powder rubber all is a homogeneous, and promptly single particulate all is a homogeneous on forming, and does not find layering in the particulate under the observation of existing microtechnique, divides the phenomenon that equates uneven phase.This powdered rubber is by with corresponding rubber latex cross-linking radiation and with rubber particles particle diameter fixed.
Above-described powdered rubber can also adopt the prepared cross-linked powdered rubber of the Chinese patent application submitted on November 3rd, 2000 according to the applicant 00130386.4.Preferentially select the cross-linked powdered rubber good with the polystyrene consistency in preparation process for use, it comprises at least a of following cross-linked powdered rubber: cross-linked powdery styrene-butadiene rubber(SBR) or cross-linked powdery polybutadiene rubber etc.This kind cross-linked powdered rubber be a kind of be raw material with the cross-linking type synthetic rubber latex, the powdered rubber that drying obtains.This cross-linked powdered rubber need not add separant and get final product unrestricted flow.Its particle diameter is 0.05 μ m～0.3 μ m.Its gel content is consistent with gel content as the cross-linking type synthetic rubber latex of raw material, is 80% weight or higher, is preferably 85% weight or higher.Each particulate in this cross-linked powdered rubber all is a homogeneous, and promptly single particulate all is a homogeneous on forming, and does not find layering in the particulate under the observation of existing microtechnique, divides the phenomenon that equates uneven phase.
Preferentially select the rubber good with the polystyrene consistency for use as the unvulcanized rubber in the toughness reinforcing component of enhancing touthness of polyphenylethylene by adding disperse phase of the present invention, it comprises at least a in the following rubber: natural rubber, styrene-butadiene rubber(SBR), divinyl rubber, polyisoprene rubber, ethylene-propylene rubber(EPR), isoprene-isobutylene rubber, silicon rubber or viton; Described thermoplastic elastomer is also preferentially selected the rubber good with the polystyrene consistency for use, and it comprises that the following stated is elastomeric at least a: styrene-butadiene-styrene block copolymer (SBS), styrene isoprene styrene block copolymer (SIS) (SIS), Hydrogenated SBS (SEBS), hydrogenation SIS (SEPS) or ethylene copolymer thermoplastic elastomer.Above-described various unvulcanized rubber and various thermoplastic elastomer can be distinguished separately or combination in any way, as one of integral part in the toughness reinforcing component.
The preparation method of enhancing touthness of polyphenylethylene by adding of the present invention is:
Polystyrene and toughness reinforcing component are made described enhancing touthness of polyphenylethylene by adding by the rubber plastic blend method.Used toughness reinforcing component is that median size is 0.02 μ m～0.5 μ m, is preferably the powdered rubber with crosslinking structure of 0.05 μ m～0.3 μ m; Or toughness reinforcing component mixed with unvulcanized rubber and/or thermoplastic elastomer by this powdered rubber and forms, and wherein unvulcanized rubber and thermoplastic elastomer proportioning arbitrarily mix.The weight ratio of above-mentioned toughness reinforcing component and plastics is 5: 95～40: 60, is preferably 10: 90～30: 70.Wherein to account for the weight percentage of toughness reinforcing component be 30%～100% to powdered rubber, is preferably 50%～100%.
Used polystyrene comprises various types of polystyrene in present method, as general purpose polystyrene, high-impact polystyrene etc.
The used powdered rubber particle with crosslinking structure is preferably the rubber particles of equal phase structure in present method, and its gel content is in 60% weight or higher, preferred 80% weight or higher.
This kind powdered rubber can adopt the prepared fully vulcanized powder rubber of the Chinese patent application submitted on December 3rd, 1999 according to the applicant 99125530.5.Preferentially select the fully vulcanized powder rubber good with the polystyrene consistency in preparation process for use, it comprises at least a of following fully vulcanized powder rubber: form of finely divided powder, mehtod natural rubber, form of finely divided powder, mehtod styrene-butadiene rubber(SBR), form of finely divided powder, mehtod polybutadiene rubber or fully sulfurized silicon rubber powder etc.This kind fully vulcanized powder rubber is meant that gel content reaches 60% weight or higher, and more excellent is 75% weight or higher, and need not with separant after the drying is free flowable rubber micro mist.The particle diameter of this powdered rubber is 0.02 μ m～2 μ m, is preferably 0.03 μ m～1.5 μ m, and more excellent is 0.05 μ m～0.5 μ m.Each particulate in this fully vulcanized powder rubber all is a homogeneous, and promptly single particulate all is a homogeneous on forming, and does not find layering in the particulate under the observation of existing microtechnique, divides the phenomenon that equates uneven phase.This powdered rubber is by with corresponding rubber latex cross-linking radiation and with rubber particles particle diameter fixed.In this preparation method, can add with the crosslinked powder morphology of exsiccant or with undried crosslinked emulsions form according to processing needs fully vulcanized powder rubber.
Above-described powdered rubber can also adopt the prepared cross-linked powdered rubber of the Chinese patent application submitted on November 3rd, 2000 according to the applicant 00130386.4.Preferentially select the cross-linked powdered rubber good with the polystyrene consistency in preparation process for use, it comprises at least a of following cross-linked powdered rubber: cross-linked powdery styrene-butadiene rubber(SBR) or cross-linked powdery polybutadiene rubber etc.This kind cross-linked powdered rubber be a kind of be raw material with the cross-linking type synthetic rubber latex, the powdered rubber that drying obtains.This cross-linked powdered rubber need not add separant and get final product unrestricted flow.Its particle diameter is 0.05 μ m～0.3 μ m.Its gel content is consistent with gel content as the cross-linking type synthetic rubber latex of raw material, is 80% weight or higher, is preferably 85% weight or higher.Each particulate in this cross-linked powdered rubber all is a homogeneous, and promptly single particulate all is a homogeneous on forming, and does not find layering in the particulate under the observation of existing microtechnique, divides the phenomenon that equates uneven phase.
Used unvulcanized rubber is preferentially selected the rubber good with the polystyrene consistency for use in present method, and it comprises at least a in the following rubber: natural rubber, styrene-butadiene rubber(SBR), divinyl rubber, polyisoprene rubber, ethylene-propylene rubber(EPR), isoprene-isobutylene rubber, silicon rubber or viton etc.; Used thermoplastic elastomer is preferentially selected the elastomerics good with the polystyrene consistency for use, and it comprises at least a of the following stated: styrene-butadiene-styrene block copolymer (SBS), styrene isoprene styrene block copolymer (SIS) (SIS), Hydrogenated SBS (SEBS), hydrogenation SIS (SEPS) or ethylene copolymer thermoplastic elastomer etc.Above-described various unvulcanized rubber and various thermoplastic elastomer can be distinguished separately or combination in any way, as one of integral part in the toughness reinforcing component.
Adopt the rubber plastic blend method to prepare in the enhancing touthness of polyphenylethylene by adding process of the present invention, the blending temperature of material is the general processing temperature of polystyrene, selects not only guaranteeing the complete fusion of matrix polystyrene but also can not make in the scope of its decomposition.In addition, according to the processing needs, can in the blend material, add the conventional auxiliary agent and the expanding material of plastic working in right amount.
The employed blending equipment of present method is the general blending equipment in the rubber and plastic processing industry, can be twin screw extruder, single screw extrusion machine, mill or Banbury mixer etc.
Enhancing touthness of polyphenylethylene by adding of the present invention, as the form of the toughness reinforcing component of disperse phase and size distribution can be by changing the powdered rubber with crosslinking structure of being sneaked into particle diameter or select suitable unvulcanized rubber or thermoplastic elastomer incompatible control that match with it, have good toughness and processing characteristics, and maintain higher intensity and rigidity.
The preparation method of enhancing touthness of polyphenylethylene by adding of the present invention, technology is simple, and the enhancing touthness of polyphenylethylene by adding of gained has good strong and unyielding balance.
Further describe the present invention below in conjunction with embodiment, scope of the present invention is not subjected to the restriction of these embodiment.Scope of the present invention proposes in claims.
Embodiment 1-2:
To vulcanize the butylbenzene powdered rubber entirely (in butylbenzene-50 emulsion of Lanhua Latex Research and Development Centre, after pressing 3% adding crosslinking coagent Viscoat 295 of the dried glue weight of styrene-butadiene emulsion, carry out radiation vulcanization, irradiation dose is 2.5Mrad, obtain after spray-dried, median size is 0.1 μ m, and gel content is 90.4% weight) and transparent polystyrene pellet (Yanshan Petrochemical production, trade mark 666D) and antioxidant 1010 (Switzerland vapour Ba Jiaji production) uniform mixing.Adopt the ZSK-25 twin screw extruder blend granulation of German WP company, each section of forcing machine temperature is respectively: 170 ℃, 180 ℃, 180 ℃, 180 ℃, 180 ℃ and 180 ℃ (head temperature).Concrete prescription sees Table 1, and wherein the component concentration of form of finely divided powder, mehtod styrene-butadiene rubber(SBR) and transparent polystyrene is all in parts by weight, and oxidation inhibitor is to account for the weight percentage of each component summation.Pellet is made the standard batten through injection moulding, carries out every Mechanics Performance Testing, and testing standard and result are as shown in table 1.
Embodiment 3
With transparent polystyrene pellet (with embodiment 1-2), cross-linking type butylbenzene powdered rubber (self-control) and antioxidant 1010 (with embodiment 1-2) mix, specifically consist of: the weight ratio of polystyrene, cross-linking type butylbenzene powdered rubber is 85: 15, is that 100 parts of oxidation inhibitor consumptions are 0.5 part in rubber and plastics gross weight.Adopt the ZSK-25 twin screw extruder blend granulation of German WP company, each section of forcing machine temperature is respectively: 170 ℃, 180 ℃, 180 ℃, 180 ℃, 180 ℃ and 180 ℃ (head temperature).Pellet is made the standard batten through injection moulding, carries out every Mechanics Performance Testing, and its result is as shown in table 1.
At this cross-linking type butylbenzene powdered rubber is preparation like this:
(this kind is crosslinked to be brought owing to certain cross takes place between the rubber molecule in the synthetic process rubber latex with styrene-butadiene emulsion itself that have certain crosslinking degree, thereby make rubber latex have certain crosslinking degree), by the spray-dryer spraying drying, the inlet temperature of spray-dryer is 140 ℃-160 ℃, temperature out is 40 ℃-60 ℃, in cyclonic separator, collect dried butylbenzene powdered rubber, promptly obtain cross-linking type butylbenzene powdered rubber, its particle diameter is about 0.1 μ m, and gel content is 88.9% weight.The trade mark that adopts Lanhua Latex Research and Development Centre to produce at this styrene-butadiene emulsion is the styrene-butadiene emulsion that butylbenzene-50, gel content are about the cross-linking type of 88% weight.
Comparative example 1:
Polystyrene pellet among the embodiment 1-2 is directly made the standard batten through injection moulding, carry out every Mechanics Performance Testing, the results are shown in table 1.
Embodiment 4
With transparent polystyrene pellet (with embodiment 1-2), cross-linking type butylbenzene powdered rubber (with embodiment 3), (the Yanshan Petrochemical production of SBS thermoplastic elastomer, the trade mark 1401) and antioxidant 1010 (with embodiment 1-2) mix, specifically consist of: the weight ratio of polystyrene, cross-linking type butylbenzene powdered rubber and SBS thermoplastic elastomer is 85: 13.5: 1.5, is that 100 parts of oxidation inhibitor consumptions are 0.5 part in rubber and plastics gross weight.Adopt the ZSK-25 twin screw extruder blend granulation of German WP company, each section of forcing machine temperature is respectively: 170 ℃, 180 ℃, 180 ℃, 180 ℃, 180 ℃ and 180 ℃ (head temperature).Pellet is made the standard batten through injection moulding, carries out every Mechanics Performance Testing, and its result is as shown in table 2.
Embodiment 5
Change the polystyrene among the embodiment 4, cross-linking type butylbenzene powdered rubber and SBS thermoplastic elastomer three weight ratio into 85: 12: 3, all the other conditions are identical with embodiment 4, and Mechanical test results is listed in table 2.
Embodiment 6
Change the polystyrene among the embodiment 4, cross-linking type butylbenzene powdered rubber and SBS thermoplastic elastomer three weight ratio into 85: 8: 7, all the other conditions are identical with embodiment 4, and Mechanical test results is listed in table 2.
Comparative example 2
Except not adding cross-linking type butylbenzene powdered rubber, the weight ratio of polystyrene and SBS thermoplastic elastomer is outside 85: 15.All the other conditions are identical with embodiment 4, and Mechanical test results is listed in table 2.
Embodiment 7
With transparent polystyrene pellet (with embodiment 1-2), (road-Exxon produces to vulcanize butylbenzene powdered rubber (with embodiment 1-2), SIS thermoplastic elastomer entirely, trade mark kraton D1017) and antioxidant 1010 (Switzerland vapour Ba Jiaji production) mix, specifically consist of: transparent polystyrene resin, the weight ratio of vulcanizing butylbenzene powdered rubber and SIS thermoplastic elastomer entirely are 90: 8: 2, are that 100 parts of antioxidant 1010 consumptions are 0.5 part in rubber and plastics gross weight.Adopt the ZSK-25 twin screw extruder blend granulation of German WP company, each section of forcing machine temperature is respectively: 170 ℃, 180 ℃, 180 ℃, 180 ℃, 180 ℃ and 180 ℃ (head temperature).Pellet is made the standard batten through injection moulding, carries out every Mechanics Performance Testing, and its result is as shown in table 3.
Embodiment 8
The weight ratio of vulcanizing butylbenzene powdered rubber and SIS thermoplastic elastomer three changes 80: 16: 4 into the transparent polystyrene pellet among the embodiment 7, entirely, and all the other conditions are identical with embodiment 7, and Mechanical test results is listed in table 3.
Comparative example 3
Except not adding full sulfuration butylbenzene powdered rubber, the weight ratio of transparent polystyrene pellet and SIS thermoplastic elastomer is 90: 10.All the other conditions are identical with embodiment 7, and Mechanical test results is listed in table 3.
Comparative example 4
Except not adding full sulfuration butylbenzene powdered rubber, the weight ratio of transparent polystyrene pellet and SIS thermoplastic elastomer is 80: 20.All the other conditions are identical with embodiment 7, and Mechanical test results is listed in table 3.
Table 1
| Transparent polystyrene | Form of finely divided powder, mehtod styrene-butadiene rubber(SBR) | Cross-linking type butylbenzene powdered rubber | Oxidation inhibitor | Tensile strength | Tension fracture elongation rate | The socle girder notched Izod impact strength | Flexural strength | Modulus in flexure | |
| Unit | ---- | ---- | ---- | ％ | MPa | ％ | J/m | MPa | GPa |
| Embodiment 1 | 85 | 15 | ---- | 0.5 | 39.3 | 12 | 39.1 | 58.0 | 2.46 |
| Embodiment 2 | 80 | 20 | ---- | 0.5 | 33.8 | 23 | 69.8 | 44.2 | 1.95 |
| Embodiment 3 | 85 | ---- | 15 | 0.5 | 35.2 | 32 | 99.5 | 50.9 | 2.36 |
| Comparative example 1 | 100 | 0 | ---- | 0.5 | 50.1 | 5 | 32.7 | 83.8 | 3.22 |
| Testing standard | ---- | ---- | ---- | ---- | GB 1040 | GB 1040 | GB 1843 | GB 9341 | GB 9341 |
Table 2
| Tensile strength | Tension fracture elongation rate | The Izod notched Izod impact strength | Flexural strength | Modulus in flexure | |
| Unit | MPa | ％ | J/m | MPa | GPa |
| Embodiment 4 | 35.0 | 36 | 137 | 51.1 | 2.40 |
| Embodiment 5 | 32.9 | 38 | 127 | 50.9 | 2.43 |
| Embodiment 6 | 32.8 | 42 | 112 | 50.7 | 2.55 |
| Comparative example 2 | 38.3 | 36 | 47.4 | 53.8 | 2.66 |
| Testing standard | GB1040 | GB1040 | GB1843 | GB9341 | GB9341 |
Table 3
| Tensile strength | Tension fracture elongation rate | The Izod notched Izod impact strength | Flexural strength | Modulus in flexure | |
| Unit | MPa | ％ | J/m | MPa | GPa |
| Embodiment 7 | 39.5 | 15 | 73.8 | 51.9 | 2.74 |
| Embodiment 8 | 30.7 | 37 | 173 | 40.7 | 2.06 |
| Comparative example 3 | 39.8 | 15 | 39.7 | 46.9 | 2.79 |
| Comparative example 4 | 20.2 | 34 | 105 | 26.1 | 1.81 |
| Testing standard | GB1040 | GB1040 | GB1843 | GB9341 | GB9341 |
Claims (12)
1. enhancing touthness of polyphenylethylene by adding, be to comprise polystyrene and toughness reinforcing component blend and get, wherein toughness reinforcing component is that median size is 0.02 μ m～0.5 μ m, powdered rubber with crosslinking structure, or toughness reinforcing component mixed with unvulcanized rubber and/or thermoplastic elastomer by this kind powdered rubber and forms, and described powdered rubber with crosslinking structure comprises: natural rubber, styrene-butadiene rubber(SBR), polybutadiene rubber or silicon rubber.
2. enhancing touthness of polyphenylethylene by adding according to claim 1, the powdered rubber that it is characterized in that having crosslinking structure is equal phase structure.
3. enhancing touthness of polyphenylethylene by adding according to claim 2, the weight ratio that it is characterized in that described toughness reinforcing component and polystyrene is 5: 95～40: 60, the weight percentage that described powdered rubber with crosslinking structure accounts for toughness reinforcing component is 30%～100%.
4. enhancing touthness of polyphenylethylene by adding according to claim 3, the powdered rubber gel content that it is characterized in that having crosslinking structure is 60% weight or higher.
5. enhancing touthness of polyphenylethylene by adding according to claim 4, the powdered rubber gel content that it is characterized in that having crosslinking structure is 80% weight or higher.
6. enhancing touthness of polyphenylethylene by adding according to claim 4, the weight ratio that it is characterized in that described toughness reinforcing component and polystyrene is 10: 90～30: 70.
7. enhancing touthness of polyphenylethylene by adding according to claim 4 is characterized in that the weight percentage that described powdered rubber with crosslinking structure accounts for toughness reinforcing component is 50%～100%.
8. according to each described enhancing touthness of polyphenylethylene by adding of claim 4～7, the powdered rubber that it is characterized in that having crosslinking structure is fully vulcanized powder rubber or cross-linked powdered rubber.
9. enhancing touthness of polyphenylethylene by adding according to claim 8 is characterized in that described fully vulcanized powder rubber comprises at least a of following material: form of finely divided powder, mehtod natural rubber, form of finely divided powder, mehtod styrene-butadiene rubber(SBR), form of finely divided powder, mehtod polybutadiene rubber or fully sulfurized silicon rubber powder.
10. enhancing touthness of polyphenylethylene by adding according to claim 8, the median size that it is characterized in that having the powdered rubber of crosslinking structure is 0.05 μ m～0.3 μ m.
11. enhancing touthness of polyphenylethylene by adding according to claim 10 is characterized in that described cross-linked powdered rubber comprises cross-linked powdery styrene-butadiene rubber(SBR) or cross-linked powdery polybutadiene rubber.
12., it is characterized in that polystyrene and toughness reinforcing component melts blend and make described enhancing touthness of polyphenylethylene by adding according to the preparation method of each described enhancing touthness of polyphenylethylene by adding of claim 1～11.
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| CN101293985B (en) * | 2007-04-28 | 2010-07-07 | 中国石油化工股份有限公司 | Polystyrene composition capable of marking with laser and preparation thereof |
| CN101418091B (en) * | 2007-10-26 | 2011-07-06 | 中国石油化工股份有限公司 | Laser marked plastic and preparation method thereof |
| CN106046585A (en) * | 2016-07-25 | 2016-10-26 | 金田集团（桐城）塑业有限公司 | Impact-resistant modified polystyrene material |
| CN110326845B (en) * | 2019-08-14 | 2022-08-02 | 安踏（中国）有限公司 | Elastomer material for sole, sneaker sole and sneaker |
| CN112430369B (en) * | 2020-12-05 | 2022-12-02 | 勇气模具塑胶(苏州)有限公司 | Refrigerator drawer material and preparation method thereof |
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