WO2019242556A1 - Modificateur d'asphalte à base de caoutchouc-composite de graphène, son procédé de préparation et son utilisation - Google Patents

Modificateur d'asphalte à base de caoutchouc-composite de graphène, son procédé de préparation et son utilisation Download PDF

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Publication number
WO2019242556A1
WO2019242556A1 PCT/CN2019/091060 CN2019091060W WO2019242556A1 WO 2019242556 A1 WO2019242556 A1 WO 2019242556A1 CN 2019091060 W CN2019091060 W CN 2019091060W WO 2019242556 A1 WO2019242556 A1 WO 2019242556A1
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WIPO (PCT)
Prior art keywords
graphene
powder
asphalt modifier
rubber
composite rubber
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Ceased
Application number
PCT/CN2019/091060
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English (en)
Chinese (zh)
Inventor
田植群
沈培康
翁晓娜
归立发
梁立喆
李卫庆
尹诗斌
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Guangxi Zhengtong Engineering And Technology Co Ltd
Guangxi University
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Guangxi Zhengtong Engineering And Technology Co Ltd
Guangxi University
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Application filed by Guangxi Zhengtong Engineering And Technology Co Ltd, Guangxi University filed Critical Guangxi Zhengtong Engineering And Technology Co Ltd
Publication of WO2019242556A1 publication Critical patent/WO2019242556A1/fr
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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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
    • C08L95/00—Compositions of bituminous materials, e.g. asphalt, tar, pitch
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L2201/00—Properties
    • C08L2201/08—Stabilised against heat, light or radiation or oxydation
    • 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
    • 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

Definitions

  • the invention relates to the field of asphalt modifiers, in particular to a graphene composite rubber asphalt modifier, and a preparation method and application thereof.
  • Asphalt pavement has the characteristics of comfortable driving, quiet driving and convenient maintenance. At present, more than 95% of the roads in the world are paved with asphalt pavement.
  • the important material composition of asphalt pavement ranges from the original residual oil, experienced ordinary asphalt, heavy traffic asphalt to current usage. With more than 50% of modified asphalt, with the rapid development of rapid economic development, the traffic load has increased rapidly.
  • Asphalt pavements constructed of ordinary asphalt or heavy traffic asphalt have various problems, such as cracks, ruts, and deformation due to insufficient high-temperature performance. Many problems such as cracking of the pavement caused by insufficient low temperature performance can no longer meet the requirements of practical use.
  • Rubber asphalt is an asphalt cementing material formed by processing rubber powder from waste tires and then fully blending with matrix asphalt in a certain proportion.
  • Graphene is a new type of functional material.
  • the carbon atoms in the structure are connected by a strong ⁇ bond, which makes the graphene sheet have excellent mechanical properties.
  • there are two methods for preparing two-dimensional graphene one is a top-down method, which is to obtain graphene from the decomposition of graphite or carbon nanotubes with a higher structure than graphene, such as mechanical peeling, insertion Layer stripping method, solvent liquid phase stripping method and redox method; the other is a bottom-up method, which uses a carbon source (small molecules such as methane, CO, alcohol, etc.) with a lower structure than graphene to pass CVD,
  • Graphene is prepared by arc discharge, solvothermal method, and the like. The performance of graphene in specific applications is closely related to the preparation method.
  • graphene asphalts use graphene oxide, with graphene oxide as an additive, and SBS as a modifier, mixed with matrix asphalt and sulfur-containing accelerators to obtain graphene-modified asphalt; or matrix asphalt and The modifier is mixed, and then the carboxyl-modified graphene oxide is added to obtain a polyethylene-modified asphalt based on the carboxyl-modified graphene oxide.
  • graphene oxide and ethanol are dispersed ultrasonically in a certain proportion to prepare graphene oxide The sol is uniformly mixed and stirred with the medium-temperature coal pitch until the solvent in the pitch is evaporated, and the final product is obtained.
  • the prior art shows that the addition of graphene can improve asphalt adhesion, mechanical properties, high and low temperature stability, and high temperature rut resistance.
  • graphene oxide is hydrophilic and has poor compatibility with asphalt, despite functionalizing it, graphene oxide is still a two-dimensional sheet structure. It is necessary to fully disperse graphene in asphalt directly, which is technically certain. Difficulty: In the prior art, nitrogen or sulfur-doped graphene is used to increase the degree of cross-linking of graphene and asphalt, but sulfur-containing substances are not environmentally friendly. If harmful substances are released during construction, health will be endangered.
  • graphene pitch is roughly as follows: graphene is functionalized, and graphene, asphalt, and modifiers are blended and blended. This blending and blending method makes the interface performance of the three poor. Poor capacitance results in poor dispersion of graphene in asphalt, and stability cannot be guaranteed.
  • the purpose of the present invention is to provide a graphene composite rubber asphalt modifier and a preparation method and application thereof.
  • the graphene composite rubber asphalt modifier can greatly improve the compatibility and stability of rubber powder in asphalt, and can improve the Adhesive performance of modified asphalt and sand and gravel, high and low temperature stability performance, at the same time reduce the temperature of the road surface and extend the service life of the road surface.
  • the present invention provides a graphene composite rubber asphalt modifier, which includes the following components by weight: graphene powder 0.00005-0.01 parts, dispersion medium 3-23 parts, rubber powder 78-92 parts And additives of 0.05-6 parts;
  • the graphene composite rubber asphalt modifier includes the following components by weight: graphene powder 0.0001-0.005 parts, dispersion medium 5-20 parts, rubber powder 80-90 0.1-5 parts of additives, and further preferably, the graphene composite rubber asphalt modifier includes the following components by weight: 0.003 parts of graphene powder, 13 parts of dispersion medium, 85 parts of rubber powder, and additives 2.5 servings.
  • the graphene powder is selected from at least one of graphene microchips, reduced graphene oxide, and three-dimensional structure graphene; preferably, the graphene powder is three-dimensional structure graphene ; Further preferably, the specific surface area of the graphene powder is greater than or equal to 300 m2 / g; wherein the graphene microplatelets (Graphene Nanoplatelets) refer to those having less than 10 carbon layers and a lateral dimension in the range of 100 nm to 1000 microns Ultra-thin layered graphene layered body; reduced graphene oxide is the first oxidation of graphite to graphite oxide, and then to graphene oxide by exfoliation, and finally through various reduction methods (to obtain excellent performance in electrochemical, photochemical and other properties Graphene; three-dimensional structure graphene is a powder material with a honeycomb-like structure composed of two-dimensional graphene sheets, and its basic structural characteristics meet the requirements of technical standards DB 45 / T 1421-2016 and
  • the dispersion medium is selected from at least one of paraffin rubber oil, aromatic rubber oil, naphthenic rubber oil, and polycyclic aromatic rubber oil; preferably, the dispersion medium is selected At least one of a self-paraffin rubber oil, an aromatic rubber oil and a naphthenic rubber oil; further preferably, the dispersion medium is a naphthenic rubber oil.
  • the powder size of the rubber powder is 20-200 mesh; preferably, the powder size of the rubber powder is 30-150 mesh; further preferably, the powder size of the rubber powder is 40 -80 mesh.
  • the additive is selected from the group consisting of acrylonitrile-butadiene-styrene copolymer, polyethylene, ethylene bisstearic acid amide, C9 petroleum resin, C12 petroleum resin, and silane coupling agent KH- 580, at least one of silane coupling agent KH550, silane coupling agent KH792, dodecyltrimethoxysilane, cetyltrimethoxysilane, dispersant KC163, dispersant BYK110, dispersant BYK164; preferably
  • the additive is at least one selected from the group consisting of acrylonitrile-butadiene-styrene copolymer, polyethylene, and ethylene bisstearate; further preferably, the additive is acrylonitrile-butadiene- Copolymer of styrene. This additive is used to increase the interfacial interaction between graphene and rubber powder and to stabilize the dispersion of graphene.
  • the invention also provides a method for preparing a graphene composite rubber asphalt modifier, comprising the following steps: (1) mixing graphene powder and a dispersion medium, mechanically stirring, and then obtaining a graphene dispersion liquid through high-speed dispersion (2) The graphene dispersion liquid is densely mixed with rubber powder and additives to prepare the graphene composite rubber asphalt modifier.
  • the mass ratio of the graphene powder mixed with the dispersion medium is (0.00005-0.01): (3-23); preferably, the graphene powder The mass ratio for mixing with the dispersion medium is (0.0001-0.005): (5-20); further preferably, the mass ratio for mixing the graphene powder and the dispersion medium is 0.003: 13.
  • the high-speed dispersion is performed by dispersing the graphene powder and the liquid mixed with the dispersion medium at a temperature of 60-120 ° C for 10-60 minutes by using a high-speed shearing machine, and obtaining the solution after cooling.
  • Graphene dispersion liquid, the graphene sheet diameter distribution in the graphene dispersion liquid is 100-2000 nanometers; preferably, the high-speed shearing machine disperses the liquid after the graphene and the dispersion medium are mixed at 70 ° C.
  • the high-speed shearing machine disperses the graphene powder and the liquid mixed with the dispersion medium at 70 ° C for 35min; further preferably, the sheet diameter distribution of the graphene in the graphene dispersion liquid It is 500-1000 nm.
  • the graphene dispersion liquid, the rubber powder and the additive are added at a mass ratio of (3-23): (78-92): (0.05-6) to 200-260 ° C.
  • the mixture is kneaded for 10-60 minutes, and then cooled to prepare a graphene composite rubber asphalt modifier.
  • the graphene dispersion liquid, rubber powder and additives are (5-20): (80 -90): (0.1-5) mass mixing and kneading at 220-240 ° C for 20-50min; further preferably, in step (2), the graphene dispersion liquid, rubber powder and additives are added at 13:85: The mass ratio of 2.5 was kneaded and kneaded at 230 ° C for 35 minutes.
  • the invention also provides the application of the graphene composite rubber asphalt modifier or the preparation method thereof to the asphalt modifier.
  • the present invention has the following beneficial effects:
  • the graphene composite rubber asphalt modifier according to the present invention is selected from at least one of graphene microflakes, reduced graphene oxide, and three-dimensional structure graphene, and has better dispersibility than graphene oxide;
  • the preparation method of the graphene composite rubber asphalt modifier according to the present invention adopts a high-temperature compaction process to fully mix graphene and rubber powder, improve the modification effect of graphene, and avoid direct graphene and the matrix Insufficient dispersion caused by asphalt mixing;
  • the combination of the graphene powder and the high-temperature compaction process used in the present invention the use of less than 0.01% of the graphene powder in the asphalt can achieve better results, greatly reducing the cost of graphene-modified asphalt,
  • the graphene composite rubber asphalt modifier can greatly improve the compatibility and stability of rubber powder in asphalt, improve the bonding performance of modified asphalt and sand and gravel, high and low temperature stability, and reduce the temperature and extension of the road surface. Road life.
  • Example 1 Components and preparation method of graphene composite rubber asphalt modifier
  • the graphene composite rubber asphalt modifier components are shown below (by parts by weight)
  • the specific surface area of the three-dimensional graphene is 500 m2 / g, and the powder particle size of the rubber powder is 60 mesh.
  • the preparation method of the graphene composite rubber asphalt modifier is as follows:
  • Example 2 Components and preparation method of graphene composite rubber asphalt modifier
  • the graphene composite rubber asphalt modifier components are shown below (by parts by weight)
  • the specific surface area of the reduced graphene oxide is 400 m2 / g, and the powder particle size of the rubber powder is 40 mesh.
  • the preparation method of the graphene composite rubber asphalt modifier is as follows:
  • the graphene composite rubber asphalt modifier components are shown below (by parts by weight)
  • the specific surface area of the graphene microchip is 600 m2 / g, and the powder particle size of the rubber powder is 80 mesh.
  • the preparation method of the graphene composite rubber asphalt modifier is as follows:
  • the graphene microchips and the paraffinic rubber oil are mixed at a mass ratio of 0.005: 20, mechanically stirred, and dispersed at 120 ° C. for 50 minutes using a high-speed shearing machine, and cooled to obtain a graphene dispersion liquid.
  • Rubber powder 87 copies
  • the graphene composite rubber asphalt modifier in Example 1-3 and the non-graphene rubber asphalt modifier in Example 4 were used to modify the 70 # matrix asphalt, respectively.
  • the weight ratio of the graphene composite rubber asphalt modifier modifier to the matrix asphalt is 20:80
  • the weight ratio of the graphene-free rubber asphalt modifier to matrix asphalt according to Example 4 is 20:80.
  • the test uses relevant technology Standard specifications are carried out. Among them, the technical specifications of graphene rubber asphalt modifiers are shown in Table 1, and the specifications of graphene rubber asphalt mixtures (that is, after the modifier is added to the asphalt) are shown in Table 2.
  • the graphite thin composite rubber asphalt modifier in Examples 1-3 is higher than the graphene-free rubber asphalt modified in Example 4 in both the modified softening point and the 10 ° C ductility.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Civil Engineering (AREA)
  • Materials Engineering (AREA)
  • Structural Engineering (AREA)
  • Health & Medical Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Medicinal Chemistry (AREA)
  • Polymers & Plastics (AREA)
  • Organic Chemistry (AREA)
  • Compositions Of Macromolecular Compounds (AREA)

Abstract

L'invention concerne un modificateur d'asphalte à base de caoutchouc-composite de graphène, son procédé de préparation et son utilisation, le modificateur d'asphalte à base de caoutchouc-composite de graphène comprenant les composants suivants en parties en poids : de 0,00005 à 0,01 partie d'une poudre de graphène, de 3 à 23 parties d'un milieu de dispersion, de 78 à 92 parties d'une poudre de caoutchouc et de 0,05 à 6 parties d'un additif. Le procédé de préparation comprend les étapes suivantes : (1) le mélange de la poudre de graphène et du milieu de dispersion et l'agitation mécanique, puis la dispersion du mélange à une vitesse élevée de façon à obtenir une solution de dispersion de graphène ; et (2) l'enfouissement de la solution de dispersion de graphène avec la poudre de caoutchouc et l'additif, pour préparer le modificateur d'asphalte à base de caoutchouc-composite de graphène.
PCT/CN2019/091060 2018-06-20 2019-06-13 Modificateur d'asphalte à base de caoutchouc-composite de graphène, son procédé de préparation et son utilisation Ceased WO2019242556A1 (fr)

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CN201810637994.6A CN108690360B (zh) 2018-06-20 2018-06-20 石墨烯复合橡胶沥青改性剂及其制备方法和应用
CN201810637994.6 2018-06-20

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Cited By (2)

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EP4559979A4 (fr) * 2022-07-18 2025-10-29 Central Fortune Creation Tech Group Co Ltd Asphalte modifié par du graphène et son procédé de préparation
CN121495371A (zh) * 2026-01-09 2026-02-10 上海晶顿科技有限公司 一种复合防水材料及其制备方法与一体化制备装置

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CN108690360B (zh) * 2018-06-20 2021-01-05 广西大学 石墨烯复合橡胶沥青改性剂及其制备方法和应用
CN109575618A (zh) * 2018-12-10 2019-04-05 青岛明象新材料技术有限公司 一种石墨烯复合岩沥青抗车辙改性剂及其制备方法
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CN112973626B (zh) * 2021-02-08 2023-09-26 常州大学 一种负载氧化石墨烯的沥青基活性炭复合材料的制备方法
CN112898789A (zh) * 2021-02-08 2021-06-04 青岛德通纳米技术有限公司 一种石墨烯改性抗剥落剂及高散热石墨烯复合改性沥青
CN113213461A (zh) * 2021-05-24 2021-08-06 崔云 一种晶形石墨烯及其制备方法和应用
CN113800820A (zh) * 2021-09-22 2021-12-17 南京宁通智能交通技术研究院有限公司 一种石墨烯复合材料橡胶沥青混合料及其制备方法
CN114213853A (zh) * 2021-12-14 2022-03-22 甘肃路桥建设集团养护科技有限责任公司 用于大温差气候条件下氧化石墨烯橡胶复合改性沥青及其制备方法
CN115304925A (zh) * 2022-01-27 2022-11-08 山东建筑大学 一种低融点速溶高黏沥青改性剂及其制备方法
CN114752350A (zh) * 2022-05-20 2022-07-15 广西北投交通养护科技集团有限公司 一种道路养护填缝胶及其制备方法
CN117757155A (zh) * 2022-09-16 2024-03-26 中国石油天然气股份有限公司 白炭黑复合橡胶沥青改性剂及其制备方法和应用
CN117004242A (zh) * 2023-08-22 2023-11-07 长沙万荣粉体设备科技有限公司 一种石墨烯复合橡胶改性沥青及其制备方法
CN117466563B (zh) * 2023-12-28 2024-03-19 水润天府新材料有限公司 一种添加废旧橡胶的可循环利用沥青混合料生产工艺

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CN121495371A (zh) * 2026-01-09 2026-02-10 上海晶顿科技有限公司 一种复合防水材料及其制备方法与一体化制备装置

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