WO2023097549A1 - Agent de renforcement de caoutchouc noir de carbone blanc hydrophobe, son procédé de préparation et son application - Google Patents

Agent de renforcement de caoutchouc noir de carbone blanc hydrophobe, son procédé de préparation et son application Download PDF

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WO2023097549A1
WO2023097549A1 PCT/CN2021/134748 CN2021134748W WO2023097549A1 WO 2023097549 A1 WO2023097549 A1 WO 2023097549A1 CN 2021134748 W CN2021134748 W CN 2021134748W WO 2023097549 A1 WO2023097549 A1 WO 2023097549A1
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solution
preparation
silane coupling
coupling agent
concentration
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PCT/CN2021/134748
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English (en)
Chinese (zh)
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陈南飞
卢爱平
王明贺
陈辰
陈家树
史彤
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无锡恒诚硅业有限公司
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Priority to CN202180004233.7A priority Critical patent/CN114286800B/zh
Priority to PCT/CN2021/134748 priority patent/WO2023097549A1/fr
Publication of WO2023097549A1 publication Critical patent/WO2023097549A1/fr

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    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B33/00—Silicon; Compounds thereof
    • C01B33/113—Silicon oxides; Hydrates thereof
    • C01B33/12—Silica; Hydrates thereof, e.g. lepidoic silicic acid
    • C01B33/18—Preparation of finely divided silica neither in sol nor in gel form; After-treatment thereof
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B33/00—Silicon; Compounds thereof
    • C01B33/113—Silicon oxides; Hydrates thereof
    • C01B33/12—Silica; Hydrates thereof, e.g. lepidoic silicic acid
    • C01B33/18—Preparation of finely divided silica neither in sol nor in gel form; After-treatment thereof
    • C01B33/187—Preparation of finely divided silica neither in sol nor in gel form; After-treatment thereof by acidic treatment of silicates
    • C01B33/193—Preparation of finely divided silica neither in sol nor in gel form; After-treatment thereof by acidic treatment of silicates of aqueous solutions of silicates
    • 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
    • C08K7/00—Use of ingredients characterised by shape
    • C08K7/22—Expanded, porous or hollow particles
    • C08K7/24—Expanded, porous or hollow particles inorganic
    • C08K7/26—Silicon- containing compounds
    • 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
    • C08K9/00—Use of pretreated ingredients
    • C08K9/04—Ingredients treated with organic substances
    • 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
    • C08K9/00—Use of pretreated ingredients
    • C08K9/04—Ingredients treated with organic substances
    • C08K9/06—Ingredients treated with organic substances with silicon-containing compounds
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02T—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION
    • Y02T10/00—Road transport of goods or passengers
    • Y02T10/80—Technologies aiming to reduce greenhouse gasses emissions common to all road transportation technologies
    • Y02T10/86—Optimisation of rolling resistance, e.g. weight reduction 

Definitions

  • the application belongs to the technical field of green tires and relates to a rubber reinforcing agent, in particular to a hydrophobic white carbon black rubber reinforcing agent and its preparation method and application.
  • the main component of precipitated silica is hydrated silica.
  • silica There are many groups on the surface of silica, including hydroxyl, siloxane, etc., so it has strong hydrophilicity and is easy to form agglomerates or secondary aggregation.
  • the main use of silica is in the rubber industry, which can be used to produce high-quality rubber products, such as increasing wear resistance and wet skid resistance, effectively reducing rolling resistance and rubber heat generation. Therefore, silica is used in green tires field plays an important role.
  • due to the presence of a large number of hydroxyl groups on the surface of silica, which is highly hydrophilic it is not easy to combine with the rubber matrix, thus affecting the performance of rubber products.
  • the methods of industrial production of white carbon black include liquid phase precipitation method and gas phase method.
  • the precipitation method uses water glass and inorganic acid as raw materials, and the white carbon black product is obtained through precipitation reaction, aging, washing, drying and granulation.
  • the production process Simple, cheap and easy-to-obtain raw materials, less equipment investment, and low energy consumption.
  • the silica prepared by the conventional precipitation method has insufficient dispersibility, and it is difficult to meet the use requirements of tire rubber or high-grade silicone rubber, and there are problems such as serious structure, poor reinforcing effect, and easy yellowing.
  • the gas phase method uses silicon tetrachloride as a raw material and reacts at high temperature to form silicon dioxide.
  • the resulting product has small particle size, high yield and superior performance.
  • this method has high energy consumption, low production efficiency, and relatively expensive products.
  • CN110746794A discloses a kind of preparation method of superhydrophobic white carbon black, comprises the following steps: (1) silane coupling agent, organic solvent and water are mixed by volume ratio 1:(1-8):(1-2) , to obtain a silane coupling agent modification solution; (2) add a silane coupling agent modification solution to the silica suspension, and stir at 50-90°C for 0.5-24h; then add a nonionic surfactant and Fluoropolymer, stirred at 40-95°C for 0.5-20h to obtain a composite modified silica suspension; (3) filter, dry and pulverize the composite modified silica suspension to obtain superhydrophobic silica black.
  • silane coupling agent organic solvent and water are mixed by volume ratio 1:(1-8):(1-2) , to obtain a silane coupling agent modification solution
  • CN109942003A discloses a method for dry grinding modified precipitated white carbon black, the specific steps are as follows: different types and different amounts of surfactants are added to a certain amount of absolute ethanol solution to obtain ethanol solutions of active agents with different concentrations . Add different concentrations of ethanol solutions of active agents into the white carbon black at a certain rate, and grind with a grinder. It utilizes the chemical mechanical force generated in the grinding process to make the surface modifier chemically react with the hydroxyl groups on the surface of the white carbon black, thereby improving the dispersibility and hydrophobicity of the white carbon black.
  • the grinding machine is easy to destroy the structure and morphology of silica, and the grinding and mixing time is long, otherwise it is difficult to obtain a good modification effect.
  • CN113150389A discloses a preparation method of hydrophobic white carbon black, comprising the following steps: weighing each component according to parts by weight: 2-8 parts of emulsifier, 10-25 parts of modifier, 2 parts of nonionic surfactant -5 parts, 3-6 parts of fluorine-containing high molecular polymer, 6-100 parts of white carbon black; pour the emulsifier and modifier into the mixing tank, and mix evenly at high speed; In the barrel, stir and mix for 0.5-1h under the environment of 50-90°C. It uses a modifier composed of silane coupling agent, dichloromethane and dilute sulfuric acid to modify the white carbon black. The silane coupling agent performs surface grafting treatment on the white carbon black, and dilute sulfuric acid is used to improve the modification effect. But it also has the problem of directly modifying white carbon black, and the modification effect is poor.
  • the application provides a hydrophobic silica rubber reinforcing agent and its preparation method and application.
  • the preparation method is simple to operate, and the dispersion effect of silica is improved through process regulation, and the hydrophobicity of the final silica is improved. .
  • the application provides a kind of preparation method of hydrophobic silica rubber reinforcing agent, described preparation method comprises the steps:
  • step (2) Add acid solution dropwise to the mixed solution obtained in step (1), adjust the pH value to 3.5-4.5, carry out precipitation reaction, and then carry out solid-liquid separation to obtain the hydrophobic silica rubber reinforcing agent;
  • the modified organic solvent described in step (1) includes a silane coupling agent, a surfactant and an organic solvent;
  • the surfactant includes lauroyl diethanolamine and/or cetyltrimethylammonium bromide.
  • sodium silicate is obtained by reacting sodium silicate in modified organic solution, which improves the modification effect of silane coupling agent and surfactant on white carbon black, and reduces the amount of white carbon black.
  • the surface energy of black improves the hydrophobicity of silica, so that it can show good compatibility and dispersion in the application of tires.
  • the concentration of the silane coupling agent in the modified organic solution described in step (1) is 3-5wt%, such as 3wt%, 3.5wt%, 4wt%, 4.5wt% or 5wt%, but not limited to Listed values, other unlisted values within the range of values also apply.
  • the concentration of the surfactant in the modified organic solution described in step (1) is 0.3-0.8wt%, such as 0.3wt%, 0.4wt%, 0.5wt%, 0.6wt%, 0.7wt% or 0.8wt%. wt%, but not limited to the listed values, other unlisted values within the range of values are also applicable.
  • the organic solvent in the modified organic solution in step (1) includes absolute ethanol.
  • the silane coupling agent in the organic solution of the silane coupling agent includes ⁇ -(methacryloyloxy)propyltrimethoxysilane (KH-570) and/or ⁇ -aminopropyltriethoxy Silane (KH-550).
  • KH-570 ⁇ -(methacryloyloxy)propyltrimethoxysilane
  • KH-550 ⁇ -aminopropyltriethoxy Silane
  • the concentration of the sodium silicate aqueous solution in step (1) is 0.5-2mol/L, such as 0.5mol/L, 0.8mol/L, 1mol/L, 1.2mol/L, 1.5mol/L, 1.8 mol/L or 2mol/L, but not limited to the listed values, other unlisted values within the range of values are also applicable.
  • the concentration of the silane coupling agent is 0.5-1wt%, such as 0.5wt%, 0.6wt%, 0.7wt%, 0.8wt%, 0.9wt% or 1wt% , but not limited to the listed values, other unlisted values within the range of values are also applicable.
  • the pH value adjusted in step (1) is adjusted by bubbling CO 2 .
  • the temperature of the precipitation reaction in step (2) is 85-90° C., and the time is 30-60 min.
  • the temperature of the precipitation reaction described in this application is 85-90°C, for example, it can be 85°C, 86°C, 87°C, 88°C, 89°C or 90°C, but it is not limited to the listed values, other unlisted values within the range Numerical values also apply.
  • the precipitation reaction time described in this application is 30-60min, for example, it can be 30min, 35min, 40min, 45min, 50min, 55min or 60min, but it is not limited to the listed values, and other unlisted values within the numerical range are also applicable.
  • the process of the precipitation reaction in step (2) is accompanied by stirring, and the stirring speed is 300-600r/min, such as 300r/min, 350r/min, 400r/min, 450r/min, 500r/min , 550r/min or 600r/min, but not limited to the listed values, other unlisted values within the range of values are also applicable.
  • the stirring speed is 300-600r/min, such as 300r/min, 350r/min, 400r/min, 450r/min, 500r/min , 550r/min or 600r/min, but not limited to the listed values, other unlisted values within the range of values are also applicable.
  • the solid-liquid separation method in step (2) includes spray drying.
  • the acid solution described in step (2) comprises citric acid and/or sulfuric acid, preferably a mixed acid of citric acid and sulfuric acid.
  • the mass ratio of citric acid to sulfuric acid is 1:(3-5), such as 1:3, 1:3.5, 1:4, 1:4.5 or 1:5, but not limited to the listed Numerical values, other unrecited numerical values within the numerical range also apply.
  • the temperature of the dropwise addition of the acid solution in step (2) is 85-90°C, and the time is 50-60min.
  • the temperature for adding the acid solution is 85-90°C, for example, it can be 85°C, 86°C, 87°C, 88°C, 89°C or 90°C, but it is not limited to the listed values, the range of values Other unlisted values also apply.
  • the time for adding the acid solution in step (2) of the present application is 50-60min, such as 50min, 51min, 52min, 53min, 54min, 55min, 56min, 57min, 58min, 59min or 60min, but not limited to the listed values , other unlisted values within the value range are also applicable.
  • the process of adding the acid solution in step (2) is accompanied by stirring, and the stirring speed is 300-600r/min, such as 300r/min, 350r/min, 400r/min, 450r/min, 500r /min, 550r/min or 600r/min, but not limited to the listed values, other unlisted values within the range of values are also applicable.
  • the stirring speed is 300-600r/min, such as 300r/min, 350r/min, 400r/min, 450r/min, 500r /min, 550r/min or 600r/min, but not limited to the listed values, other unlisted values within the range of values are also applicable.
  • the mixed solution in step (1) further includes a modifier.
  • the modifier includes any one or a combination of at least two of alkylphenol polyoxyethylene ethers, fatty alcohol polyoxyethylene ethers, or polyol fatty acid esters.
  • Typical but non-limiting combinations include alkylphenol polyoxyethylene ethers.
  • the concentration of the modifier in the mixed solution in step (1) is 0.1-0.5wt%, such as 0.1wt%, 0.2wt%, 0.3wt%, 0.4wt% or 0.5wt%, but not limited to For the numerical values listed, other unlisted numerical values within the numerical range are also applicable.
  • the preparation method includes the following steps:
  • step (2) Under the condition of 85-90°C, add acid solution dropwise to the mixed solution obtained in step (1) for 50-60min, adjust the pH value to 3.5-4.5, the process of adding acid solution is accompanied by stirring, and the stirring speed 300-600r/min; 85-90°C precipitation reaction for 30-60min, the process of precipitation reaction is accompanied by stirring, the stirring speed is 300-600r/min; then spray drying to obtain the hydrophobic silica rubber strong agent;
  • the mixed solution in step (1) also includes a modifying agent with a concentration of 0.1-0.5 wt %;
  • the modified organic solvent in step (1) includes a silane coupling agent, a surfactant and absolute ethanol; the surfactant includes lauroyl diethanolamine and/or cetyltrimethylammonium bromide.
  • the present application provides a hydrophobic silica rubber reinforcing agent, which is obtained by the preparation method described in the first aspect.
  • the present application provides an application of the hydrophobic silica rubber reinforcing agent described in the second aspect for green tires.
  • sodium silicate is obtained by reacting sodium silicate in modified organic solution, which improves the modification effect of silane coupling agent and surfactant on white carbon black, and reduces the amount of white carbon black.
  • the surface energy of black improves the hydrophobicity of silica, so that it can show good compatibility and dispersion in the application of tires.
  • the present embodiment provides a kind of preparation method of hydrophobic silica rubber reinforcing agent, and described preparation method comprises the following steps:
  • the modified organic solvent of step (1) includes silane coupling agent, surfactant and dehydrated alcohol;
  • the silane coupling agent is ⁇ -(methacryloyloxy)propyltrimethoxysilane (KH-570 );
  • the surfactant includes lauroyldiethanolamine and cetyltrimethylammonium bromide in a mass ratio of 1:1; the concentration of the silane coupling agent in the modified organic solution is 4wt%; in the modified organic solution The concentration of surfactant was 0.5 wt%.
  • the present embodiment provides a kind of preparation method of hydrophobic silica rubber reinforcing agent, and described preparation method comprises the following steps:
  • the concentration of silane coupling agent is 0.5wt% in the mixed liquor;
  • the sodium silicate aqueous solution The concentration is 0.5mol/L;
  • the modified organic solvent described in step (1) includes a silane coupling agent, a surfactant and dehydrated alcohol; the silane coupling agent is ⁇ -aminopropyltriethoxysilane (KH-550); the surface
  • the active agent includes lauroyl diethanolamine and cetyltrimethylammonium bromide in a mass ratio of 1:3; the concentration of the silane coupling agent in the modified organic solution is 3wt%; the concentration of the surfactant in the modified organic solution is 0.3wt%.
  • the present embodiment provides a kind of preparation method of hydrophobic silica rubber reinforcing agent, and described preparation method comprises the following steps:
  • the modified organic solvent described in step (1) includes a silane coupling agent, a surfactant and dehydrated alcohol; the silane coupling agent is ⁇ -aminopropyltriethoxysilane (KH-550); the surface
  • the active agent comprises lauroyl diethanolamine and cetyltrimethylammonium bromide in a mass ratio of 3:1; the concentration of the silane coupling agent in the modified organic solution is 5wt%; the concentration of the surfactant in the modified organic solution is 0.8wt%.
  • the present embodiment provides a kind of preparation method of hydrophobic silica rubber reinforcing agent, and described preparation method comprises the following steps:
  • the modified organic solvent of step (1) includes silane coupling agent, surfactant and dehydrated alcohol;
  • the silane coupling agent is ⁇ -(methacryloyloxy)propyltrimethoxysilane (KH-570 );
  • the surfactant includes lauroyldiethanolamine and cetyltrimethylammonium bromide in a mass ratio of 1:1; the concentration of the silane coupling agent in the modified organic solution is 4wt%; in the modified organic solution The concentration of surfactant was 0.5 wt%.
  • the present embodiment provides a kind of preparation method of hydrophobic silica rubber reinforcing agent, and described preparation method comprises the following steps:
  • the modified organic solvent of step (1) includes silane coupling agent, surfactant and dehydrated alcohol;
  • the silane coupling agent is ⁇ -(methacryloyloxy)propyltrimethoxysilane (KH-570 );
  • the surfactant includes lauroyldiethanolamine and cetyltrimethylammonium bromide in a mass ratio of 1:1; the concentration of the silane coupling agent in the modified organic solution is 4wt%; in the modified organic solution The concentration of surfactant was 0.5 wt%.
  • the present embodiment provides a kind of preparation method of hydrophobic silica rubber reinforcing agent, and described preparation method comprises the following steps:
  • the modified organic solvent of step (1) includes silane coupling agent, surfactant and dehydrated alcohol;
  • the silane coupling agent is ⁇ -(methacryloyloxy)propyltrimethoxysilane (KH-570 );
  • the surfactant includes lauroyldiethanolamine and cetyltrimethylammonium bromide in a mass ratio of 1:1; the concentration of the silane coupling agent in the modified organic solution is 4wt%; in the modified organic solution The concentration of surfactant was 0.5 wt%.
  • This example provides a method for preparing a hydrophobic silica rubber reinforcing agent, except that the surfactant is only lauroyl diethanolamine, the rest are the same as in Example 1.
  • This example provides a method for preparing a hydrophobic silica rubber reinforcing agent, except that the surfactant is only cetyltrimethylammonium bromide, the rest are the same as in Example 1.
  • This example provides a method for preparing a hydrophobic silica rubber reinforcing agent, which is the same as Example 1 except that the concentration of the surfactant in the modified organic solution is 1.2 wt%.
  • This embodiment provides a kind of preparation method of hydrophobic silica rubber reinforcing agent, except that the acid solution in step (2) is the citric acid whose pH value is identical with mixed acid, all the other are the same as embodiment 1.
  • This example provides a method for preparing a hydrophobic silica rubber reinforcing agent, except that the acid solution in step (2) is sulfuric acid with the same pH value as the mixed acid, and the others are the same as in Example 1.
  • This comparative example provides a preparation method of a white carbon black rubber reinforcing agent, except that the pH value is adjusted to 7.5 in step (1), the rest are the same as in Example 1.
  • This comparative example provides a preparation method of a white carbon black rubber reinforcing agent, except that the pH value is adjusted to 9.5 in step (1), the rest are the same as in Example 1.
  • This comparative example provides a preparation method of a white carbon black rubber reinforcing agent, except that the pH value is adjusted to 3 in step (2), the rest are the same as in Example 1.
  • This comparative example provides a preparation method of a white carbon black rubber reinforcing agent, except that the pH value is adjusted to 5 in step (2), the rest are the same as in Example 1.
  • Performance tests were performed on the hydrophobic silica rubber reinforcing agent provided in Examples 1-11 and the silica rubber reinforcing agent provided in Comparative Examples 1-4. Determine the specific surface area according to GB/T10722-2014 "Determination of Total Surface Area and External Area of Carbon Black by Nitrogen Adsorption Method”; determine the oil absorption value according to HGT 3072-2019 "Determination of Oil Absorption Value of Precipitated Hydrated Silica as Rubber Compounding Agent”; determine the oil absorption value according to GB/T10722-2014 T 32698-2016 "Determination of Particle Size Distribution of Precipitated Hydrated Silica in Rubber Compounding Agent by Laser Diffraction Method” to determine the apparent particle size; according to GB/T 6030-2006 "Evaluation of Carbon Black and Carbon Black Silica Dispersion in Rubber Quickly Comparative method” to measure the degree of dispersion.
  • this application directly mixes sodium silicate aqueous solution and modified organic solution, and reacts sodium silicate in modified organic solution, which improves the modification effect of silane coupling agent and surfactant on white carbon black , reduces the surface energy of silica, improves the hydrophobicity of silica, so that it can show good compatibility and dispersion in the application of tires.

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  • Organic Chemistry (AREA)
  • Health & Medical Sciences (AREA)
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Abstract

L'invention concerne un agent de renforcement de caoutchouc noir de carbone blanc hydrophobe, son procédé de préparation, et son application. Le procédé de préparation comprend les étapes suivantes consistant à : (1) mélanger une solution aqueuse de silicate de sodium et une solution organique modifiée, et ajuster la valeur de pH entre 8 et 9 dans le processus de mélange pour obtenir une solution mixte ; et (2) ajouter goutte à goutte une solution acide à la solution mixte obtenue à l'étape (1) jusqu'à ce que la valeur de pH soit ajustée entre 3,5 et 4,5, effectuer une réaction de précipitation, puis effectuer une séparation solide-liquide pour obtenir l'agent de renforcement de caoutchouc noir de carbone blanc hydrophobe. Le solvant organique modifié dans l'étape (1) comprend un agent de couplage au silane, un tensioactif et un solvant organique, et le tensioactif comprend du diéthanolamide de lauryle et/ou du bromure de cétyltriméthylammonium. La solution aqueuse de silicate de sodium et la solution organique d'agent de couplage au silane sont directement mélangées de telle sorte que le silicate de sodium est obtenu par réaction dans un solvant contenant l'agent de couplage au silane, ce qui permet d'améliorer l'effet de dispersion de l'agent de couplage au silane sur le noir de carbone blanc et d'améliorer les performances hydrophobes du produit final de noir de carbone blanc.
PCT/CN2021/134748 2021-12-01 2021-12-01 Agent de renforcement de caoutchouc noir de carbone blanc hydrophobe, son procédé de préparation et son application WO2023097549A1 (fr)

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CN202180004233.7A CN114286800B (zh) 2021-12-01 2021-12-01 一种疏水白炭黑橡胶补强剂及其制备方法与应用
PCT/CN2021/134748 WO2023097549A1 (fr) 2021-12-01 2021-12-01 Agent de renforcement de caoutchouc noir de carbone blanc hydrophobe, son procédé de préparation et son application

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CN108467609A (zh) * 2018-03-30 2018-08-31 江苏新亿源环保科技有限公司 一种改性疏水分散型白炭黑的制备方法
WO2020244182A1 (fr) * 2019-06-05 2020-12-10 确成硅化学股份有限公司 Procédé de préparation de silice à dispersion élevée par précipitation en gradient de ph

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CN116715985A (zh) * 2023-07-04 2023-09-08 连城县佳辉科技有限公司 一种防锈颜料和涂料及其制备方法
CN116715985B (zh) * 2023-07-04 2023-12-15 连城县佳辉科技有限公司 一种防锈颜料和涂料及其制备方法
CN117326564A (zh) * 2023-11-30 2024-01-02 万达集团股份有限公司 一种增强轮胎耐磨性材料的生产工艺
CN117326564B (zh) * 2023-11-30 2024-02-13 万达集团股份有限公司 一种增强轮胎耐磨性材料的生产工艺

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