CN112442216B - Oriented high-thermal-conductivity rubber composite material and preparation method thereof - Google Patents
Oriented high-thermal-conductivity rubber composite material and preparation method thereof Download PDFInfo
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Abstract
The invention discloses an oriented high-thermal-conductivity rubber composite material and a preparation method thereof. The composite material is prepared from the following raw materials: 100 parts by weight of rubber latex; 0.1-20 parts by weight of graphene oxide aqueous dispersion; 10-400 parts by weight of anisotropic filler; 0.2-40 parts by weight of a reducing agent; 0.1-20 parts by weight of an emulsifier; 0.2-4 parts by weight of a vulcanizing agent. According to the invention, the three-dimensional network is formed by the anisotropic filler and the rubber latex particles guided by graphene oxide gelation, and then the network is subjected to hot-pressing orientation to prepare the oriented high-thermal-conductivity rubber composite material, so that the composite material has excellent thermal conductivity and the preparation method is simple.
Description
Technical Field
The invention relates to the technical field of rubber, in particular to an oriented high-thermal-conductivity rubber composite material and a preparation method thereof; the thermal-pressing oriented high-thermal-conductivity rubber composite material is guided by graphene oxide hydrogel.
Background
With the development of miniaturization and high power consumption of electronic devices, the energy density of the electronic devices is higher and higher, which causes a large amount of heat to be generated in the use process, and if the heat cannot be led out in time, local overheating, device seizure and even circuit damage can be caused. The contact between the heat generating end and the heat dissipating end of the electronic device usually creates voids, which greatly hinder the transfer of heat. In order to solve the problem, people are dedicated to develop a rubber thermal interface material with high flexibility and high thermal conductivity to fill the gaps and improve the heat dissipation efficiency.
Anisotropic heat conductive fillers, such as graphene, boron nitride, carbon nanotubes, carbon fibers, and the like, have been the materials for which the research on the heat and the fire has been conducted for nearly 10 years. Such materials have extremely high thermal conductivity in a certain direction. Thus, when these fillers are oriented in the polymer matrix, the composite material will have extremely high thermal conductivity in the direction of orientation. In recent years, researchers have developed various high thermal conductivity polymer composite materials prepared by orientation methods such as an ice template method, a double-roller shear orientation method, a vacuum filtration method and the like. However, many orientation methods or processes have various limitations, such as complicated process, inability to expand production, single applicable system, etc.
The rubber material is a material with intrinsic high flexibility and high elasticity, and is an excellent substrate used as a thermal interface material. At present, thermal interface materials using liquid silicone rubber as a matrix have been widely used. However, various general-purpose rubbers, such as natural rubber, styrene butadiene rubber, etc., are limited by processing methods and have low thermal conductivity, and no suitable high thermal conductivity product is available.
Disclosure of Invention
In order to solve the problems in the prior art, the invention provides an oriented high-thermal-conductivity rubber composite material and a preparation method thereof.
The invention aims to provide an oriented high-thermal-conductivity rubber composite material.
The composite material is prepared from the following raw materials:
the components are calculated according to the parts by weight,
the latex in the invention can be selected from all latexes in the prior art, and is preferably one or a combination of natural latex, styrene-butadiene latex, butyronitrile latex, chloroprene latex, butadiene latex, epoxidized natural rubber latex, butadiene pyrene latex, carboxylic butadiene-acrylonitrile latex, acrylic latex, silica gel latex, polyurethane latex and the like.
The graphene oxide referred to in the present invention generally refers to graphene oxide prepared by various conventional methods (such as modified hummers method), wherein the graphene oxide concentration in the preferred graphene oxide aqueous dispersion is 2mg/ml-20 mg/ml; the graphene oxide dispersion is alkaline, and the preferable pH range is 8-12.
The anisotropic filler is one or a combination of hexagonal boron nitride sheets, graphene nanosheets, carbon fibers, metal silver nanosheets and nanowires, metal copper nanosheets and nanowires, and silicon carbide nanosheets and nanowires.
The anisotropic filler of the present invention is a one-dimensional filler or a two-dimensional filler. The preferred sizes of the one-dimensional fillers are: the diameter is 100nm-5 μm, and the length is 500nm-50 μm; preferred dimensions for the two-dimensional filler are: the thickness is 5nm-25 μm, and the sheet diameter is 500nm-50 μm.
The reducing agent of the invention can be selected from all graphene reducing agents in the prior art, preferably one or a combination of ascorbic acid, ethylenediamine and pyrrole;
the emulsifier of the invention can be selected from the existing emulsifiers in the prior art, and is preferably one or a combination of alkylphenol ethoxylate (OP, NP, TX) series emulsifiers, fatty alcohol polyoxyethylene ether (AEO) series emulsifiers, (peregal) series emulsifiers, sorbitan fatty acid ester polyoxyethylene ether (Tween series) emulsifiers, sorbitan fatty acid ester (span series) emulsifiers, coconut oil diethanolamide (6501) emulsifiers and the like.
The vulcanizing agent in the invention can be selected from the vulcanizing agents which are available in the prior art, and preferably, the vulcanizing agent is one or more of common rubber crosslinking agents such as sulfur, dicumyl peroxide, 2, 5-dimethyl-2, 5-di (tert-butylperoxy) hexane and the like.
The formulations of the invention may also comprise conventional auxiliaries, such as: the dosage of the activating agent, the accelerator, the anti-aging agent and the like is also conventional, and the technical personnel can adjust the dosage according to the actual situation.
The activating agent in the invention can be selected from the activating agents existing in the prior art, and preferably, the activating agent is one or more of common rubber activating agents such as zinc oxide, magnesium oxide, zinc carbonate, zinc hydroxide, organic zinc, stearic acid and the like.
The accelerator used in the present invention may be any one or more of conventional rubber accelerators such as accelerator DM (benzothiazole disulfide), accelerator CZ (N-cyclohexyl-2-benzothiazole sulfenamide), accelerator NS (N-tert-butyl-2-benzothiazole sulfenamide), accelerator TMTD (tetramethylthiuram disulfide), accelerator TMTM (tetramethylthiuram monosulfide), accelerator DTDM (4, 4 '-dithiodimorpholine), accelerator D (1, 3-diphenylguanidine), accelerator NOBS (N- (oxydiethylene) -2-benzothiazole sulfenamide) and accelerator DM (2, 2' -dithiodibenzothiazole).
The antioxidant in the invention can be selected from the existing antioxidants in the prior art, and preferably one or more of common rubber accelerators such as antioxidant 4010NA (N-isopropyl-N '-phenyl-p-phenylenediamine), antioxidant RD (2,2, 4-trimethyl-1, 2-dihydroquinoline polymer), antioxidant 4020(N- (1, 3-dimethyl) butyl-N' -phenyl-p-phenylenediamine), antioxidant AW (6-ethoxy-2, 2, 4-trimethyl-1, 2-dihydroquinoline), antioxidant D (N-phenyl-beta-naphthylamine), antioxidant TPPD (N-N-phenyl-p-phenylenediamine) and the like.
The preferred amounts in the present invention are (based on 100 parts by weight of the rubber latex):
0.5-8 parts by weight of an activator; more preferably 1 to 5 parts by weight;
0.2-4 parts by weight of an accelerator; more preferably 0.5 to 3 parts by weight;
0.5-8 parts of an anti-aging agent; more preferably 1 to 4 parts by weight.
The small materials such as the vulcanizing agent, the activating agent, the accelerator, the anti-aging agent and the like related by the invention are not limited by the adding method, can be directly added, and can also be prepared into a stable aqueous dispersion liquid commonly used in the latex product industry in advance for adding; the addition amount of the small materials is reasonably determined according to the parts of the added rubber, and normal vulcanization can be ensured.
The second purpose of the invention is to provide a preparation method of the oriented high-thermal-conductivity rubber composite material.
The method comprises the following steps:
uniformly mixing the graphene oxide aqueous dispersion and the nano filler, adding other components according to the using amount, and uniformly stirring; reducing to obtain hydrogel; and washing, drying and hot-pressing the hydrogel for vulcanization to obtain the oriented high-thermal-conductivity rubber composite material.
Among them, preferred are:
the reduction temperature is 70-98 ℃; the reduction time is 30min-12 h.
The addition method of each component other than the graphene oxide aqueous dispersion is not particularly limited, and the components may be added directly or in the form of a dispersion.
The basic principle of the invention is to guide the heat-conducting filler and the rubber latex particles to form a three-dimensional network by utilizing the characteristic that graphene oxide sheets can be mutually overlapped to form hydrogel in a weak reduction state. The hydrogel is dried in an oven to obtain a regular gel block, and a large amount of pore structures are left in the internal network structure of the gel block after drying due to the large size of the used heat-conducting filler. And (3) hot-pressing the dried gel, wherein in the process, internal gaps are continuously removed, so that the heat-conducting filler is highly oriented. The oriented material can be directly vulcanized or vulcanized by converting the orientation direction into the vertical plane direction through curling.
The specific technical scheme of the invention is as follows:
the first step is as follows: uniformly stirring or ultrasonically mixing the graphene oxide aqueous dispersion and the anisotropic filler, sequentially adding a reducing agent, an emulsifying agent, rubber latex, a vulcanizing agent, an activating agent, an accelerating agent, an anti-aging agent and the like, and uniformly stirring. And (3) hermetically placing the slurry which is uniformly stirred into a constant temperature environment (an oven, a water bath or an oil bath kettle) of 70-98 ℃ for reduction for 30min-12h to obtain the hydrogel. The second step is that: and fully washing the obtained hydrogel with purified water, drying the hydrogel in an oven, and putting the dried gel in a flat vulcanizing machine for hot-pressing vulcanization to obtain the oriented high-thermal-conductivity rubber composite material.
The vulcanization conditions (vulcanization pressure, vulcanization temperature and vulcanization time) of the hot-pressing vulcanization are determined according to the dosage of different rubbers, different vulcanizing agents and different accelerators.
The hot-pressing vulcanization process of the invention is not limited in the form of the mold. For example, moulds with different thicknesses are adopted, or the mould is placed into other forms of moulds for vulcanization by means of curling and the like after mould pressing.
The invention has the advantages of
1. The invention utilizes the characteristic of graphene oxide gelation to guide the heat-conducting filler to form a three-dimensional structure, is beneficial to improving the heat-conducting property of the product, and has mild condition and easy large-scale production.
2. The hydrogel obtained by the method can be directly dried in a drying oven by hot air, freeze drying or vacuum drying is not involved, the operation is simple and convenient, and the energy consumption is lower.
3. The invention leads the filler to be oriented by removing the gap generated in the dried gel, and the thought is simple, convenient and efficient, and the obtained material has high orientation degree.
4. The invention creates a new idea of rubber latex blending, namely, latex is introduced into graphene hydrogel, the gelation process is a rubber flocculation process, the traditional demulsification and rubber flocculation process is omitted, and the rubber latex blending method has certain advantages in process.
Drawings
FIG. 1 is a schematic view of the brittle fracture surface of the composite material prepared in comparative example 2 under a scanning electron microscope.
FIG. 2 is a schematic view of the brittle fracture surface of the composite material prepared in example 1 under a scanning electron microscope.
FIG. 3 is a schematic scanning electron microscope of the brittle fracture surface of the composite material prepared in example 4.
FIG. 4 is a Scanning Electron Microscope (SEM) representation of the brittle failure surface of the xerogel before molding of the composite material prepared in example 4.
Detailed Description
While the present invention will be described in detail and with reference to the specific embodiments thereof, it should be understood that the following detailed description is only for illustrative purposes and is not intended to limit the scope of the present invention, as those skilled in the art will appreciate numerous insubstantial modifications and variations therefrom.
Comparative example 1
The components are calculated according to the parts by weight,
the specific operation process is as follows:
dispersing 10g of hexagonal boron nitride tablets in 200ml of deionized water, sequentially adding 0.2 g of Triton X-100 emulsifier, 16.67 g of natural rubber latex (with the gel content of 60 wt%), 0.5 g of sulfur aqueous dispersion (with the sulfur content of 20 wt%), 2 g of zinc oxide aqueous dispersion (with the zinc oxide content of 20 wt%), 0.5 g of accelerator D aqueous dispersion (with the accelerator D content of 20 wt%), 2 g of anti-aging agent AW aqueous dispersion (with the AW content of 20 wt%) and the like, and uniformly stirring. Adding anhydrous formic acid flocculation glue into the system drop by drop, repeatedly washing the flocculated rubber with purified water, and fully drying in a 60 ℃ blast oven. And finally, placing the mixture in a flat vulcanizing machine for hot-press vulcanization to obtain the oriented high-thermal-conductivity rubber composite material with the thickness of 1mm, wherein the vulcanization pressure is 15MPa, the vulcanization temperature is 150 ℃, and the vulcanization time is 20 min.
Comparative example 2
The components are calculated according to the parts by weight,
the specific operation process is as follows:
200ml of graphene oxide aqueous dispersion with the concentration of 5mg/ml (the PH value of the graphene oxide aqueous dispersion is adjusted to 10.5) and 10g of hexagonal boron nitride sheet are stirred or ultrasonically mixed uniformly, and 2 g of ascorbic acid, 0.2 g of Triton X-100 emulsifier, 16.67 g of natural rubber latex (with the rubber content of 60 wt%), 0.5 g of sulfur aqueous dispersion (with the sulfur content of 20 wt%), 2 g of zinc oxide aqueous dispersion (with the zinc oxide content of 20 wt%), 0.5 g of accelerator D aqueous dispersion (with the accelerator D content of 20 wt%), 2 g of antioxidant AW aqueous dispersion (with the AW content of 20 wt%) and the like are added in sequence and stirred uniformly. And dropwise adding anhydrous formic acid flocculation glue into the system, and then putting the system into a 90 ℃ forced air drying oven for reduction for 2 hours. The second step is that: and fully washing the obtained product rubber with purified water, drying in a 60 ℃ blast oven, putting the dried gel in a flat vulcanizing machine, and carrying out hot-press vulcanization on the gel to obtain the oriented high-thermal-conductivity rubber composite material with the thickness of 0.2mm, wherein the vulcanization pressure is 15MPa, the vulcanization temperature is 150 ℃, and the vulcanization time is 20 min.
Example 1
The components are calculated according to the parts by weight,
the specific operation process is as follows:
200ml of graphene oxide aqueous dispersion with the concentration of 5mg/ml (the PH value of the graphene oxide aqueous dispersion is adjusted to 10.5) and 5g of hexagonal boron nitride sheet (the thickness is 5nm, the diameter is 500nm) are stirred or ultrasonically mixed uniformly, and 2 g of ascorbic acid, 0.2 g of Triton X-100 emulsifier, 16.67 g of natural rubber latex (the rubber content is 60 wt%), 0.5 g of sulfur aqueous dispersion (the sulfur content is 20 wt%), 2 g of zinc oxide aqueous dispersion (the zinc oxide content is 20 wt%), 0.5 g of accelerator D aqueous dispersion (the accelerator D content is 20 wt%), 2 g of antioxidant AW aqueous dispersion (the AW content is 20 wt%) and the like are added in sequence and stirred uniformly. And sealing the slurry which is uniformly stirred, and putting the slurry into a blowing drying oven at the temperature of 90 ℃ for reduction for 2 hours to obtain the hydrogel. The second step is that: and fully washing the obtained hydrogel with purified water, drying the hydrogel in a 60 ℃ blast oven, putting the dried gel in a flat vulcanizing machine, and carrying out hot-pressing vulcanization on the gel to obtain the oriented high-thermal-conductivity rubber composite material with the thickness of 1mm, wherein the vulcanization pressure is 15MPa, the vulcanization temperature is 150 ℃, and the vulcanization time is 20 min.
Example 2
The components are calculated according to the parts by weight,
the specific operation process is as follows:
50ml of graphene oxide aqueous dispersion with the concentration of 2mg/ml (the PH value of the graphene oxide aqueous dispersion is adjusted to 10.5) and 10g of graphite nanoplatelets (the thickness is 5 mu m, the diameter of the graphite nanoplatelets is 50 mu m) are stirred or ultrasonically mixed uniformly, and 0.2 g of ascorbic acid, 0.02 g of sorbitan fatty acid ester polyoxyethylene ether emulsifier, 16.67 g of nitrile rubber latex (the rubber content is 60 wt%), 0.5 g of sulfur aqueous dispersion (the sulfur content is 20 wt%), 2 g of zinc oxide aqueous dispersion (the zinc oxide content is 20 wt%), 0.5 g of accelerator D aqueous dispersion (the accelerator D content is 20 wt%), 2 g of antioxidant AW aqueous dispersion (the AW content is 20 wt%) and the like are added in sequence and stirred uniformly. And sealing the slurry which is uniformly stirred, and putting the slurry into a forced air drying oven at the temperature of 80 ℃ for reduction for 6 hours to obtain the hydrogel. The second step is that: and fully washing the obtained hydrogel with purified water, drying the hydrogel in a 60 ℃ blast oven, putting the dried gel in a flat vulcanizing machine, and carrying out hot-pressing vulcanization on the gel to obtain the oriented high-thermal-conductivity rubber composite material with the thickness of 0.2mm, wherein the vulcanization pressure is 15MPa, the vulcanization temperature is 150 ℃, and the vulcanization time is 20 min.
Example 3
The components are calculated according to the parts by weight,
the specific operation process is as follows:
200ml of graphene oxide aqueous dispersion with the concentration of 5mg/ml (the PH value of the graphene oxide aqueous dispersion is adjusted to 8.5) and 15g of copper nanowire (the diameter is 100nm, the length is 500nm) are stirred or ultrasonically mixed uniformly, 2 g of ascorbic acid, 0.5 g of Triton X-100 emulsifier, 16.67 g of styrene-butadiene rubber latex (the gel content is 60 wt%), 0.5 g of sulfur aqueous dispersion (the sulfur content is 20 wt%), 2 g of zinc oxide aqueous dispersion (the zinc oxide content is 20 wt%), 0.5 g of accelerator D aqueous dispersion (the accelerator D content is 20 wt%), 2 g of antioxidant AW aqueous dispersion (the AW content is 20 wt%) and the like are added in sequence and stirred uniformly. And sealing the slurry which is uniformly stirred, and putting the slurry into a 95 ℃ forced air drying oven to be reduced for 30min to obtain the hydrogel. The second step is that: and fully washing the obtained hydrogel with purified water, drying the hydrogel in a 60 ℃ blast oven, putting the dried gel in a flat vulcanizing machine, and carrying out hot-pressing vulcanization on the gel to obtain the oriented high-thermal-conductivity rubber composite material with the thickness of 2mm, wherein the vulcanization pressure is 15MPa, the vulcanization temperature is 150 ℃, and the vulcanization time is 20 min.
Example 4
The components are calculated according to the parts by weight,
the specific operation process is as follows:
200ml of graphene oxide aqueous dispersion with the concentration of 5mg/ml (the PH value of the graphene oxide aqueous dispersion is adjusted to 11.5) and 30g of carbon fibers (the diameter is 5 mu m, the length is 50 mu m) are stirred or ultrasonically mixed uniformly, and 2 g of ethylenediamine, 0.2 g of sorbitan fatty acid ester emulsifier, 16.67 g of epoxidized natural rubber latex (the rubber content is 60 wt%), 0.5 g of sulfur aqueous dispersion (the sulfur content is 20 wt%), 2 g of zinc oxide aqueous dispersion (the zinc oxide content is 20 wt%), 0.5 g of accelerator D aqueous dispersion (the accelerator D content is 20 wt%), 2 g of antioxidant AW aqueous dispersion (the AW content is 20 wt%) and the like are added in sequence and stirred uniformly. And sealing the slurry which is uniformly stirred, and putting the slurry into a 70 ℃ forced air drying oven to be reduced for 12 hours to obtain the hydrogel. The second step is that: and fully washing the obtained hydrogel with purified water, drying the hydrogel in a 60 ℃ blast oven, putting the dried gel in a flat vulcanizing machine, and carrying out hot-pressing vulcanization on the gel to obtain the oriented high-thermal-conductivity rubber composite material with the thickness of 0.3mm, wherein the vulcanization pressure is 15MPa, the vulcanization temperature is 150 ℃, and the vulcanization time is 20 min.
Description of the test results
It can be seen from fig. 1 that the boron nitride flakes inside the rubber composite material obtained by the conventional rubber flocculating process through hot-press vulcanization tend to be randomly distributed, and it is apparent from fig. 2 and 3 that the boron nitride flakes in the embodiment are obviously oriented along a certain direction. As can be seen in FIG. 4, the xerogel which is not molded has a distinct three-dimensional filler network structure inside, which contains a large number of voids. It can be seen that the randomly distributed boron nitride flakes are highly oriented during the molding process due to the continuous evacuation of these voids.
The comparative examples and examples were tested for thermal conductivity (test standard ASTM E1461) and the results are shown in table 1.
TABLE 1
As can be seen from the table, the thermal conductivity of comparative examples 1 and 2 is significantly lower than that of examples 1 to 4, which is apparently due to the fact that the fillers in the examples are highly oriented to cause a large increase in thermal conductivity in the orientation direction. Comparative example 2 is slightly higher than comparative example 1 because of the addition of graphene network in comparative example 2; examples 1-4 the thermal conductivity was gradually increased due to the increasing boron nitride content.
While the invention has been described in detail with reference to the foregoing examples, it is not intended to be limited to the details shown, since various equivalent modifications, such as changes in the formulation of ingredients with different activators, curatives, etc., and in the order of addition/processing/article-forming processing, can be made by those skilled in the art. Such equivalent modifications and substitutions are intended to be included within the scope of the present application.
Claims (6)
1. An oriented high-thermal-conductivity rubber composite material is characterized in that the composite material is prepared from the following raw materials:
the components are calculated according to the parts by weight,
100 parts by weight of rubber latex;
0.1-20 parts by weight of graphene oxide aqueous dispersion;
10-400 parts by weight of anisotropic filler;
0.2-40 parts by weight of a reducing agent;
0.1-20 parts by weight of an emulsifier;
0.2-4 parts by weight of a vulcanizing agent;
the anisotropic filler is one or a combination of hexagonal boron nitride sheets, graphene nanosheets, carbon fibers, metal silver nanosheets and nanowires, metal copper nanosheets and nanowires, and silicon carbide nanosheets and nanowires;
the reducing agent is one or a combination of ascorbic acid, ethylenediamine and pyrrole;
the emulsifier is one or a combination of alkylphenol ethoxylates, fatty alcohol-polyoxyethylene ether, sorbitan fatty acid ester, peregal series emulsifier and coconut oil diethanolamide;
the oriented high-thermal-conductivity rubber composite material is prepared by the method comprising the following steps of:
uniformly mixing the graphene oxide aqueous dispersion and the anisotropic filler, adding other components according to the dosage, and uniformly stirring; reducing to obtain hydrogel; washing, drying and hot-pressing the hydrogel to obtain the oriented high-thermal-conductivity rubber composite material;
the concentration of the graphene oxide in the graphene oxide aqueous dispersion liquid is 2mg/ml-20mg/ml, and the value of p H is adjusted to be 8-12 by adding alkali.
2. The oriented high thermal conductivity rubber composite of claim 1, wherein:
the components are calculated according to the parts by weight,
100 parts by weight of rubber latex;
1-10 parts by weight of graphene oxide aqueous dispersion;
50-350 parts by weight of anisotropic filler;
2-20 parts by weight of a reducing agent;
0.2-10 parts by weight of an emulsifier;
0.5-3 parts by weight of a vulcanizing agent.
3. The oriented high thermal conductivity rubber composite of claim 1, wherein:
the rubber latex is one or a combination of natural latex, styrene-butadiene latex, butyronitrile latex, neoprene latex, cis-butadiene latex, epoxidized natural rubber latex, butadiene-pyrene latex, carboxyl butyronitrile latex, acrylic latex, silica gel latex, polyurethane latex and the like.
4. The oriented high thermal conductivity rubber composite of claim 1, wherein:
the anisotropic filler is a one-dimensional filler or a two-dimensional filler;
the size of the one-dimensional filler is: the diameter is 100nm-5 μm, and the length is 500nm-50 μm;
the dimensions of the two-dimensional filler are: the thickness is 5nm-5 μm, and the sheet diameter is 500nm-50 μm.
5. A method for preparing the oriented high thermal conductive rubber composite material as claimed in any one of claims 1 to 4, wherein the method comprises the following steps:
uniformly mixing the graphene oxide aqueous dispersion and the nano filler, adding other components according to the using amount, and uniformly stirring; reducing to obtain hydrogel; and washing, drying and hot-pressing the hydrogel for vulcanization to obtain the oriented high-thermal-conductivity rubber composite material.
6. The method for preparing the oriented high thermal conductive rubber composite material according to claim 5, wherein:
the reduction temperature is 70-98 ℃; the reduction time is 30min-12 h.
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| CN113072755B (en) * | 2021-04-25 | 2023-02-03 | 海南热作高科技研究院有限公司 | Natural latex pillow and preparation process thereof |
| CN113150408A (en) * | 2021-05-13 | 2021-07-23 | 慕思健康睡眠股份有限公司 | Temperature-reducing and heat-insulating graphene latex as well as preparation method and application thereof |
| CN113817242B (en) * | 2021-09-24 | 2023-06-13 | 五邑大学 | Conductive flexible material and preparation method and application thereof |
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