CN109651794A - Low sporadic, wear-resisting PC/ABS alloy material of one kind and preparation method thereof - Google Patents
Low sporadic, wear-resisting PC/ABS alloy material of one kind and preparation method thereof Download PDFInfo
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- CN109651794A CN109651794A CN201811624455.5A CN201811624455A CN109651794A CN 109651794 A CN109651794 A CN 109651794A CN 201811624455 A CN201811624455 A CN 201811624455A CN 109651794 A CN109651794 A CN 109651794A
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L69/00—Compositions of polycarbonates; Compositions of derivatives of polycarbonates
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K2201/00—Specific properties of additives
- C08K2201/011—Nanostructured additives
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K2201/00—Specific properties of additives
- C08K2201/014—Additives containing two or more different additives of the same subgroup in C08K
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L2205/00—Polymer mixtures characterised by other features
- C08L2205/03—Polymer mixtures characterised by other features containing three or more polymers in a blend
- C08L2205/035—Polymer mixtures characterised by other features containing three or more polymers in a blend containing four or more polymers in a blend
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L2205/00—Polymer mixtures characterised by other features
- C08L2205/06—Polymer mixtures characterised by other features having improved processability or containing aids for moulding methods
Abstract
The present invention relates to field of alloy material, more particularly to a kind of low sporadic, wear-resisting PC/ABS alloy material and preparation method thereof.Wherein, low sporadic, wear-resisting PC/ABS alloy material is made of the raw material that following parts by weight match: polycarbonate, ABS resin, nanometer mine crystalline substance, polytetrafluoroethylene (PTFE), 1-3 parts of silane coupling agent, MBS, antioxidant, polyethylene wax.The present invention passes through the synergistic effect of nanometer mine crystalline substance and polytetrafluoroethylene (PTFE), effectively improves the big problem of PC/ABS alloy material smell, and improve the scratch-resistant of PC/ABS alloy, wear-resisting property.The preparation method of low sporadic, the wear-resisting PC/ABS alloy material provided is invented, simple and easy, the PC/ABS alloy smell diversity prepared is small, wear-resisting and crazing amount is small.PC/ABS alloy material is set to meet automobile interior decoration plastics towards beautiful, environmental protection, the trend development of health.
Description
Technical field
The present invention relates to field of alloy material, in particular to a kind of low sporadic, wear-resisting PC/ABS alloy material and its system
Preparation Method.
Background technique
In recent years, automobile industry develops rapidly, and simultaneously with this, the consumption view of people is also being continuously improved, and vehicle body is in addition to wanting
Outside the requirement for meeting intensity and service life, should also meet the needs of performance, appearance, safety, price, environmental protection, energy conservation etc..
It is improved day by day with every safety and environment law, to the performance requirement of the inside and outside exterior material of automobile also more standardization and specific
Change.For interior material, main development trend is exactly: low-density, scratch-resistant, weatherability, low gloss, exempt from spraying with
And balance performance of rigidity/toughness etc..In addition, also being specially required to reduce injury of the interior harmfulness volatile matter to human body
Interior material must have low smell/low VOC characteristic.
Polycarbonate and acrylonitrile-butadiene-styrene copolymer and mixture (PC/ABS) are by polycarbonate (letter
Claim PC) and polyacrylonitrile (abbreviation ABS) alloy made of thermoplastic plastic rubber, combine the excellent characteristics of two kinds of materials, ABS material
The mouldability of material and the properties such as mechanicalness, impact strength and the heatproof of PC, uvioresistant (abbreviation UV).PC/ABS is improved compared with PC
Mobility, improves processing performance, reduces product to the sensibility of stress, heat-resisting and weatherability is improved compared with ABS,
And cost falls between.Thus it is widely used in the high intensity such as automobile interior decoration, exterior trim, car light, high heat resistance part.So
And PC/ABS material smell is larger, limits it in the application in automobile interior decoration field.
Summary of the invention
To solve the problems, such as to mention in above-mentioned background technique, the present invention provides a kind of low sporadic, wear-resisting PC/ABS alloy
Material and preparation method thereof.Wherein, a kind of low sporadic, wear-resisting PC/ABS alloy material, the alloy material is by following weight
The raw material of number proportion is made:
Further, the alloy material is made of the raw material that following parts by weight match:
Further, the polycarbonate weight average molecular weight is 20000-30000g/mol.
Further, the ABS resin is acrylonitrile-butadiene rubber-styrene composition of the rubber content in 35-75%
Graft copolymer.
Further, the nanometer mine crystalline substance is prepared by sepiolite, attapulgite, diatomite, bentonite.
Further, the maximum operation (service) temperature of the polytetrafluoroethylene (PTFE) is 290-300 DEG C.
Further, the coupling agent is silane coupling agent.
Further, the toughener is MBS.
Further, the lubricant includes at least following at least one: calcium stearate, polyethylene wax.
The present invention passes through the synergistic effect of nanometer mine crystalline substance and polytetrafluoroethylene (PTFE), effectively improves PC/ABS alloy material smell
Big problem, and improve the scratch-resistant of PC/ABS alloy, wear-resisting property.
The present invention provides a kind of preparation method of low sporadic, wear-resisting PC/ABS alloy material, and the preparation method is specific
It is as follows:
S10, nanometer mine crystalline substance is placed in baking material 1-1.5h in 150-200 DEG C of baking oven；
S20, the nanometer mine crystalline substance and polytetrafluoroethylene (PTFE) of drying are matched to stir in investment mixing agitator in parts by weight and mixed
Close 5-8min；Then polycarbonate, ABS resin, silane coupling agent, MBS, antioxidant, polyethylene wax are matched in parts by weight
Continue to put into mixing agitator and be stirred 5-15min, forms mixing；
S30, then mixing is added in double screw extruder, the melting extrusion at 240-270 DEG C, using be granulated,
Cooling obtains low sporadic, the wear-resisting PC/ABS alloy material；The screw machine revolving speed is 200-500rpm, and extrusion process is adopted
With black soy sauce vacuum.
The preparation method of low sporadic, the wear-resisting PC/ABS alloy material provided, simple and easy, the PC/ prepared are provided
ABS alloy smell diversity is small, wear-resisting and crazing amount is small.Also make PC/ABS alloy material meet automobile interior decoration plastics towards
Beautiful, environmental protection, healthy trend development.
Specific embodiment
In order to make the object, technical scheme and advantages of the embodiment of the invention clearer, it is carried out below in conjunction with embodiment clear
Chu is fully described by, it is clear that described embodiments are some of the embodiments of the present invention, instead of all the embodiments.It is based on
Embodiment in the present invention, it is obtained by those of ordinary skill in the art without making creative efforts every other
Embodiment shall fall within the protection scope of the present invention.
In the description of the present invention, it should be noted that the similar word such as term " connection " or " connected " is simultaneously non-limiting
It but may include electrical connection, light connects etc. with the connection of physics or machinery, it is either direct or indirectly.
The present invention provides following examples, as shown in table 1:
Table 1
| Embodiment 1 | Embodiment 2 | Embodiment 3 | Embodiment 4 | Comparative example 1 | Comparative example 2 | |
| Polycarbonate | 75 parts | 65 parts | 65 parts | 55 parts | 65 parts | 65 parts |
| ABS resin | 19.5 parts | 16.3 parts | 16.1 parts | 24.5 parts | 29.6 | 29.6 |
| Nanometer mine is brilliant | 10 parts | 13 parts | 13 parts | 14 parts | - | 14.5 parts |
| Polytetrafluoroethylene (PTFE) | 0.1 part | 0.3 part | 0.5 part | 0.1 part | - | - |
| Silane coupling agent | 3 parts | 2 parts | 1 part | 2 parts | 2 parts | 3 parts |
| MBS | 2 parts | 1 part | 1 part | 2 parts | 1 part | 1 part |
| Antioxidant | 0.4 part | 0.4 part | 0.4 part | 0.4 part | 0.4 part | 0.4 part |
| Polyethylene wax | 1 part | 0.2 part | 0.5 part | 1 part | 1 part | 1 part |
Embodiment 1
S10,10 nanometers of mine crystalline substances are placed in baking material 1h in 150 DEG C of baking ovens；
S20,5min will be stirred in the nanometer mine crystalline substance of drying and 0.1 part of polytetrafluoroethylene (PTFE) investment mixing agitator；So
75 parts of polycarbonate, 19.5 parts of ABS resins, 3 parts of silane coupling agents, 2 parts of MBS, 1 part of antioxidant, 1 part of polyethylene wax are continued afterwards
It is stirred 8min in investment mixing agitator, forms mixing；
S30, then mixing is added in double screw extruder, the melting extrusion at 270 DEG C, using granulation, cooling
Obtain low sporadic, the wear-resisting PC/ABS alloy material；The screw machine revolving speed is 200rpm, and extrusion process is true using black soy sauce
It is empty.In the step, 240-270 DEG C is the suitable processing technology of PC/ABS, is lower than 240 DEG C of bad processing, is higher than 270 DEG C and is easy drop
Solution
Embodiment 2
S10,13 parts of nanometer mine crystalline substances are placed in baking material 1h in 180 DEG C of baking ovens；
S20,5min will be stirred in the nanometer mine crystalline substance of drying and 0.3 part of polytetrafluoroethylene (PTFE) investment mixing agitator；So
Afterwards by 65 parts of polycarbonate, 16.3 parts of ABS resins, 2 parts of silane coupling agents, 1 part of MBS, 0.4 part of antioxidant, 0.2 part of polyethylene wax
Continue to put into mixing agitator and be stirred 8min, forms mixing；
S30, then mixing is added in double screw extruder, the melting extrusion at 240 DEG C, using granulation, cooling
Obtain low sporadic, the wear-resisting PC/ABS alloy material；The screw machine revolving speed is 500rpm, and extrusion process is true using black soy sauce
It is empty.
Embodiment 3
S10,13 parts of nanometer mine crystalline substances are placed in baking material 1.5h in 100 DEG C of baking ovens；
S20,7min will be stirred in the nanometer mine crystalline substance of drying and 0.5 part of polytetrafluoroethylene (PTFE) investment mixing agitator；So
Afterwards by 65 parts of polycarbonate, 16.1 parts of ABS resins, part silane coupling agent, 1 part of MBS, 0.4 part of antioxidant, 0.5 part of polyethylene wax
Continue to put into mixing agitator and be stirred 15min, forms mixing；
S30, then mixing is added in double screw extruder, the melting extrusion at 260 DEG C, using granulation, cooling
Obtain low sporadic, the wear-resisting PC/ABS alloy material；The screw machine revolving speed is 300rpm, and extrusion process is true using black soy sauce
It is empty.
Embodiment 4
S10,14 parts of nanometer mine crystalline substances are placed in baking material 1.5h in 100 DEG C of baking ovens；
S20, the nanometer mine crystalline substance of drying is matched in parts by weight with 0.1 part of polytetrafluoroethylene (PTFE) and is stirred in investment mixing agitator
Mix mixing 5min；Then by 55 parts of polycarbonate, 24.5 parts of ABS resins, 2 parts of silane coupling agents, 2 parts of MBS, 0.4 part of antioxidant,
1 part of polyethylene wax, which continues to put into mixing agitator, is stirred 10min, forms mixing；
S30, then mixing is added in double screw extruder, the melting extrusion at 270 DEG C, using granulation, cooling
Obtain low sporadic, the wear-resisting PC/ABS alloy material；The screw machine revolving speed is 350rpm, and extrusion process is true using black soy sauce
It is empty.
Comparative example 1
S10, by 65 parts of polycarbonate, 29.6 parts of ABS resins, 2 parts of silane coupling agents, 1 part of MBS, 0.4 part of antioxidant, 0.2
It is stirred 15min in part polyethylene wax and the nanometer mine crystalline substance of drying investment mixing agitator, forms mixing；
S20, then mixing is added in double screw extruder, the melting extrusion at 240 DEG C, using granulation, cooling
Obtain low sporadic, the wear-resisting PC/ABS alloy material；The screw machine revolving speed is 500rpm, and extrusion process is true using black soy sauce
It is empty.
Comparative example 2
S10, by 65 parts of polycarbonate, 29.6 parts of ABS resins, 14.5 parts of nanometer mine crystalline substances, 2 parts of silane coupling agents, 1 part of MBS,
It is stirred 15min in the nanometer mine crystalline substance investment mixing agitator of 0.4 part of antioxidant, 0.2 part of polyethylene wax and drying, is formed mixed
Material；
S20, then mixing is added in double screw extruder, the melting extrusion at 240 DEG C, using granulation, cooling
Obtain low sporadic, the wear-resisting PC/ABS alloy material；The screw machine revolving speed is 500rpm, and extrusion process is true using black soy sauce
It is empty.
Comparative example 3
S10, by 65 parts of polycarbonate, 16.1 parts of ABS resins, 13 parts of nanometer mine crystalline substances, 0.5 part of polytetrafluoroethylene (PTFE), 1 part of silane
Stirring is mixed in coupling agent, 1 part of MBS, 0.4 part of antioxidant, 0.5 part of polyethylene wax and the nanometer mine crystalline substance of drying investment mixing agitator
10min is closed, mixing is formed；
S20, then mixing is added in double screw extruder, the melting extrusion at 260 DEG C, using granulation, cooling
Obtain low sporadic, the wear-resisting PC/ABS alloy material；The screw machine revolving speed is 300rpm.
Wherein, polycarbonate is selected from the L-1250Y of Japanese Supreme Being people；ABS resin is selected from the 0215A of Jilin Petrochemical, and rubber contains
Amount is in 35-75%；Nanometer mine is brilliant, commercially available；Polytetrafluoroethylene PTFE, it is commercially available；Coupling agent is silane coupling agent, commercially available；Toughener
For core-shell structure MBS anti-impact modifier, the EXL-2690 selected from ROHM AND HAAS；Antioxidant is the antioxidant 1076 of Ciba company
And irgasfos 168, weight ratio 1:1；Lubricant is pentaerythritol stearate (PETS), commercially available.
To examine the application of low sporadic, wear-resisting PC/ABS alloy material provided by the invention in practice, by alloy material
Material carries out scratch-resistant (color difference DE), wear-resisting, VOC, oder levels test, and testing standard is followed successively by GMW14688 standard, ASTM
D4060-01 standard, VDA277 standard and VDA270 standard；Crazing amount can be observed by naked eyes detection, and there are a large amount of crazings
Grade be 3 grades, be 2 grades there are the grade of a small amount of crazing, being visually difficult to observe crazing, then grade is 1 grade.Test result is such as
Shown in table 2:
Table 2
From embodiment 1-4 and comparative example 1,2 as can be seen that the TVOC of embodiment 1-4, oder levels are significantly lower than comparative example
1-3, it can be seen that, PC/ABS alloy material provided by the invention effectively improves the larger problem of smell.
The present invention passes through the synergistic effect of nanometer mine crystalline substance and polytetrafluoroethylene (PTFE), effectively improves PC/ABS alloy material smell
Big problem, and prepare PC/ABS alloy material color difference, abrasion vector, all decrease；It can be seen that the present invention mentions
The high scratch-resistant of PC/ABS alloy, wear-resisting property.
The nanometer mine crystalline substance is prepared by sepiolite, attapulgite, diatomite, bentonite.Wherein sepiolite clay and bumps
The nanometer lattice of stick can adsorb the poisonous and hazardous nanoscale small molecule polar substances such as formaldehyde, benzene, ammonia in air, and diatom
Earth removal can adsorb micron-sized macromolecular air plankton, also for nanometer mine crystalline substance provide sorption channel, and it is brilliant to improve nanometer mine
Adsorption effect.The rigidity and intensity of product can be remarkably reinforced in diatomite, settling volume up to 95%, and can be improved product it is heat-resisting,
The performances such as wear-resisting, anti-aging, diatomite is from a wealth of sources and cheap, has the characteristics that large specific surface area and porous structure, no
The effect for only opening packing material enhancing, also as porous structure, which has adsorbed small molecule present in resin, can also reduce resin
Dosage reduces cost.
The average molecular weight selects the polycarbonate weight of 20000-30000g/mol, this average molecular weight is excessively high not to be suitable for
Injection molding, molecular weight is too low to be only applicable to thin pieces.
The ABS resin is acrylonitrile-butadiene rubber-styrene composition of the rubber content in 35-75%.If rubber
Content is too low to be not easy to toughening, is not easy to disperse if rubber content is too high.The maximum operation (service) temperature of the polytetrafluoroethylene (PTFE) is
290-300 DEG C, with extremely low coefficient of friction, good wearability and chemical stability, main in the present invention outer
Lubricating action.The setting of temperature is the problem of causing polytetrafluoroethylene (PTFE) to be degraded in order to avoid temperature is excessively high.
The coupling agent is silane coupling agent, and silane coupling agent can be erected between inorganic substances and the interface of organic substance
" molecular bridge ", the performance for improving composite material that the material of two kinds of property great disparities is linked together and the work for increasing adhesive strength
With.
MBS plays the role of interfacial agent on PC and ABS phase interface, and obtain PC and ABS has preferable compatibility,
The interfacial tension between two components is reduced, and the rubber phase in MBS can cause crazing when material is by stress, improves material
Impact strength, improve toughness of material.MBS only when by larger stress can just generate crazing, production prepare
In the process, which can't generate gas line silver line below.
Polyethylene wax reduces torque, reduces equipment friction, punch die appearance for improving plastic processing mobility and release property
Easily, product fraction defective is reduced, plastic melt rupture is eliminated, reduces die head accumulation, significantly improve the impact strength of plastics.
Comparative example 1-3 and comparative example 3, the PC/ABS alloy material being prepared using preparation method provided by the invention
Material, while reducing diversity, the crazing amount of generation is also few；Although and also using provided by the invention match in comparative example 3
Fang Zufen, but do not prepared using method provided by the invention, therefore there are a large amount of silver in its PC/ABS alloy material produced
Line.Due in PC/ABS alloy material preparation process, being also easy to produce crazing, especially nanometer mine porous polycrystalline material, in gap
The bulk gas of carrying can aggravate crazing phenomenon when prepared by PC/ABS alloy, and the appearance of alloy material is caused defect occur.For
Solve the problems, such as this, one aspect of the present invention, by the high temperature drying in step S10, after making a nanometer mine crystalline substance discharge gas at high temperature
Again with other components hybrid reaction, so that nanometer mine crystal zone be avoided to carry out excessive gas, and the problem of lead to a large amount of crazings.Another party
Face can balance smell and silver in 10-14 parts of nanometer mines crystalline substance and the ratio range of 0.1-0.5 parts of polytetrafluoroethylene (PTFE)
Line problem avoids the generation of a large amount of crazings while realizing low emission.
In addition, due to the more difficult melt-processed of polytetrafluoroethylene (PTFE), and it has the characteristics that easy heat build-up, in order to avoid more
Polytetrafluoroethylene (PTFE) aggregation caused by heat build-up problem, the present invention is mixed with polytetrafluoroethylene (PTFE) first by the nanometer mine crystalline substance after dry
It closes, porous nanometer mine crystalline substance can adsorb polytetrafluoroethylene (PTFE), and in subsequent mixing, nanometer mine crystalline substance is able to drive polytetrafluoro
Ethylene dispersion, so that the dispersibility of polytetrafluoroethylene (PTFE) is improved, it is dispersed by improving, so that polytetrafluoroethylene (PTFE) is uniformly dispersed, from
And there is local heat build-up problem in alloy material caused by avoiding the dispersion of polytetrafluoroethylene (PTFE) uneven.
The preparation method of low sporadic, the wear-resisting PC/ABS alloy material provided, simple and easy, the PC/ prepared are provided
ABS alloy smell diversity is small, wear-resisting and crazing amount is small.Also make PC/ABS alloy material meet automobile interior decoration plastics towards
Beautiful, environmental protection, healthy trend development.
Although more herein used such as polycarbonate, ABS resin, nanometer mine crystalline substance, polytetrafluoroethylene (PTFE), coupling
The terms such as agent, toughener, antioxidant, lubricant, but it does not exclude the possibility of using other terms.Only using these terms
It is to be more convenient to describe and explain essence of the invention；Being construed as any additional limitation is all and this hair
What bright spirit was disagreed.
Finally, it should be noted that the above embodiments are only used to illustrate the technical solution of the present invention., rather than its limitations；To the greatest extent
Pipe present invention has been described in detail with reference to the aforementioned embodiments, those skilled in the art should understand that: its according to
So be possible to modify the technical solutions described in the foregoing embodiments, or to some or all of the technical features into
Row equivalent replacement；And these are modified or replaceed, various embodiments of the present invention technology that it does not separate the essence of the corresponding technical solution
The range of scheme.
Claims (7)
1. a kind of low sporadic, wear-resisting PC/ABS alloy material, it is characterised in that: the alloy material is matched by following parts by weight
The raw material of ratio is made:
2. low sporadic, wear-resisting PC/ABS alloy material according to claim 1, it is characterised in that: the alloy material
It is made of the raw material that following parts by weight match:
3. low sporadic, wear-resisting PC/ABS alloy material according to claim 1, it is characterised in that: the polycarbonate
Weight average molecular weight is 20000-30000g/mol.
4. low sporadic, wear-resisting PC/ABS alloy material according to claim 1, it is characterised in that: the ABS resin is
Acrylonitrile-butadiene rubber-styrene composition graft copolymer of the rubber content in 35-75%.
5. low sporadic, wear-resisting PC/ABS alloy material according to claim 1, it is characterised in that: the nanometer mine is brilliant
It is prepared by sepiolite, attapulgite, diatomite, bentonite.
6. low sporadic, wear-resisting PC/ABS alloy material according to claim 1, it is characterised in that: the polytetrafluoroethyl-ne
The maximum operation (service) temperature of alkene is 290-300 DEG C.
7. a kind of preparation method of low sporadic, wear-resisting PC/ABS alloy material, it is characterised in that: the preparation method is specifically such as
Under:
S10, nanometer mine crystalline substance is placed in baking material 1-1.5h in 150-200 DEG C of baking oven；
S20, by the nanometer mine crystalline substance and polytetrafluoroethylene (PTFE) of drying in parts by weight match investment mixing agitator in be stirred 5-
8min；Then polycarbonate, ABS resin, silane coupling agent, MBS, antioxidant, polyethylene wax are matched into continuation in parts by weight
It is stirred 5-15min in investment mixing agitator, forms mixing；
S30, then mixing is added in double screw extruder, the melting extrusion at 240-270 DEG C, using granulation, cooling
Obtain low sporadic, the wear-resisting PC/ABS alloy material；The screw machine revolving speed is 200-500rpm, and extrusion process is using double
It vacuumizes.
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| CN113121974A (en) * | 2019-12-30 | 2021-07-16 | 苏州荣昌复合材料有限公司 | PC/ABS alloy material with high wear resistance and preparation method thereof |
| WO2021243652A1 (en) * | 2020-06-03 | 2021-12-09 | 湖南省普瑞达内装材料有限公司 | Environmentally-friendly thermally conductive polyurethane foam, preparation method therefor, and adhesive tape |
| CN115260726A (en) * | 2021-04-29 | 2022-11-01 | 广州视源电子科技股份有限公司 | High-gloss low-odor wear-resistant PC/ABS/PMMA alloy material and preparation method thereof |
| CN115260726B (en) * | 2021-04-29 | 2024-03-19 | 广州视源电子科技股份有限公司 | High-gloss low-odor wear-resistant PC/ABS/PMMA alloy material and preparation method thereof |
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Application publication date: 20190419 |