Interface adhesion performance and adhesion mechanism between graphene/rubber composite modified asphalt and aggregate

doi:10.16085/j.issn.1000-6613.2024-0224

Abstract

Abstract:

To investigate the interfacial adhesion performance and adhesion mechanism between graphene/rubber composite modified asphalt and aggregate, photoelectric colorimetry and contact angle method were used to study the interfacial adhesion performance between graphene/rubber composite modified asphalt and aggregates. The interfacial model of asphalt and aggregate was constructed by using the molecular dynamics software MS, and the interfacial adhesion properties of asphalt and aggregate were quantified in terms of the work of adhesion, while the effects of temperature and water on the interfacial adhesion properties of asphalt and aggregate were considered. The adhesion mechanism and temperature and humidity sensitivity between asphalt and aggregates were analyzed and studied at the atomic scale. The results showed that the adhesion effect between graphene/rubber composite modified asphalt and granite was the best. Therefore, it was recommended to use graphene/rubber composite modified asphalt as asphalt binder in areas lacking alkaline aggregates. Graphene/rubber composite modified asphalt can significantly improve the adhesion performance between asphalt and aggregates. As the alkalinity of aggregate oxides increased, the polar molecules in asphalt changed from “inclined distribution” to “parallel distribution” on the surface of aggregates, thereby enhancing the adhesion performance between asphalt and aggregates. In this study, the interfacial adhesion mechanism of graphene/rubber composite modified asphalt and aggregate was analyzed at the atomic level, which would provide guidance for the design of graphene/rubber composite modified asphalt pavement.

Key words: graphene, rubber, molecular dynamics, interface adhesion, interfacial adhesion mechanism

摘要：

为探究石墨烯/橡胶复合改性沥青与集料的界面黏附性能及黏附机理，采用光电比色法和接触角法对石墨烯/橡胶复合改性沥青与集料的界面黏附性能进行了研究。利用分子动力学软件MS构建了沥青与集料的界面模型，以黏附功对沥青与集料的界面黏附性能进行了量化。从原子尺度对沥青与集料间的黏附机理以及温湿敏感性进行了分析研究。结果表明：集料种类对于黏附性能的影响要明显大于沥青种类对于黏附性能的影响；在碱性集料缺乏的地区，石墨烯/橡胶复合改性沥青与花岗岩的黏附性效果最优，因此此类地区推荐使用石墨烯/橡胶复合改性沥青作为沥青胶结料；石墨烯/橡胶复合改性沥青可以明显改善沥青与集料的黏附性能，随着集料氧化物碱性增强，沥青中的极性分子在集料表面从“倾斜分布”转为“平行分布”，从而增强沥青与集料间的黏附性能。本研究在微细观层面揭示了石墨烯/橡胶复合改性沥青与集料的界面黏附机理，旨在为石墨烯/橡胶复合改性沥青路面的设计提供指导。

关键词: 石墨烯, 橡胶, 分子动力学, 界面黏附性, 界面黏附机理

CLC Number:

U414

LIN Mei, LEI Yu, LI Ping, ZHANG Qiang. Interface adhesion performance and adhesion mechanism between graphene/rubber composite modified asphalt and aggregate[J]. Chemical Industry and Engineering Progress, 2025, 44(2): 991-1002.

林梅, 雷雨, 李萍, 张强. 石墨烯/橡胶复合改性沥青-集料界面黏附性能及机理[J]. 化工进展, 2025, 44(2): 991-1002.

Figures/Tables 22

检测指标	实验结果	技术要求	实验方法
针入度（25℃）/×0.1mm	81	80~100	T0604
针入度指数	-1.46	-1.5~+1.0	T0604
软化点/℃	45	≥44	T0606
延度（5℃）/cm	78.6	—	T0605
旋转薄膜加热后
质量变化/%	-0.02	-0.4~+0.4	T0609
残留针入度比（25℃）/%	65	≥57	T0604
残留延度（10℃）/cm	9	≥8	T0605

检测指标	实验结果	技术要求	实验方法
体积密度/kg·m^-3	1.16	1.10~1.30	GB/T19208
金属质量分数/%	0.01	<0.05	GB/T19208
纤维质量分数/%	0.065	<1.0	GB/T19208
灰分/%	6.50	≤9	GB4498
丙酮抽出物/%	8	≤22	GB/T3516
碳黑质量分数/%	33	≥24	GB/T14837
橡胶烃质量分数/%	55	≥42	GB/T14837

检测指标	实验结果	技术要求
堆积密度/g·mL^-1	0.0135	0.01~0.02
碳质量分数/%	65	—
比表面积/m²·g^-1	1100	1000-1217
含水率/%	0.18	<2
pH	6.5	—

检测指标	实验结果			技术要求	方法实验
检测指标	花岗岩	石灰岩	玄武岩	技术要求	方法实验
压碎值/%	19.1	13.1	10.8	≤26	T0316
洛杉矶磨耗值/%	15.1	12.5	10	≤28	T0323
表观密度/g·cm^-3	2.808	2.832	2.865	≥2.6	T0304
吸水率/%	0.2	0.5	0.3	≤2	T0307
SiO₂质量分数/%	74.81	13.64	55.79	—	—
针片状颗粒质量分数/%	8.3	3	7.12	≤15	T0312

测试液	化学式	总表面能γ_l	色散分量 ${γ_{l}}^{d}$	极性分量 ${γ_{l}}^{p}$
蒸馏水	H₂O	72.80	22.20	51.00
丙三醇	C₃H₈O₃	63.40	33.40	30.00
甲酰胺	CH₃NO	57.90	38.90	19.00

测试液	化学式	总表面能γ_l	色散分量 ${γ_{l}}^{d}$	极性分量 ${γ_{l}}^{p}$
蒸馏水	H₂O	72.80	22.20	51.00
丙三醇	C₃H₈O₃	63.40	33.40	30.00
甲酰胺	CH₃NO	57.90	38.90	19.00

组分	化学式	物质的量/g·mol^-1	质量分数/%	实验结果^[29]/%
沥青质	C₅₃H₅₅NOS	754.089	7.2	7.25
胶质	C₁₈H₁₀S₂	290.398	20.9	20.74
饱和分	C₂₂H₄₆	310.610	22.6	22.54
芳香分	C₁₂H₁₂	156.228	49.3	49.47
橡胶	C₆₉H₉₈	819.444	18.0	18.24
石墨烯	C₄₈H₁₈	594.672	0.4	0.3

矿物类型	化学式	晶格常数						超晶胞参数
		长度/Å			角度/（°）			常见暴露面	U、V	超晶胞尺寸/Å
		a	b	c	α	β	γ	常见暴露面	U、V	超晶胞尺寸/Å
石英	SiO₂	4.913	4.913	5.4052	90	90	120	（001）	U=9、V=9	44.217×44.217×20.976
方解石	CaCO₃	4.990	4.990	17.061	90	90	120	（104）	U=6、V=10	48.575×49.900×22.809
钠长石	NaAlSi₃O₈	8.115	12.762	7.157	94.218	116.803	87.707	（100）	U=4、V=7	51.048×50.103×36.163

沥青种类	集料种类	酚藏花红溶液起始浓度C₀/mg·mL^-1	集料吸附后溶液浓度C₁/mg·mL^-1	酚藏花红溶液体积V/mL	集料质量/g	混合料吸附后溶液浓度/ mg·mL^-1	集料吸附量q/mg·g^-1	混合料剥落试验后吸附量q'/ mg·g^-1	剥落度S_t(q)/%	黏附性 A_d/%
SK-90	花岗岩	0.01	0.00133	200	100	0.00532	0.01734	0.00936	53.98	46.02
	玄武岩	0.01	0.00786	200	100	0.00938	0.00428	0.00124	28.97	71.03
	石灰岩	0.01	0.00626	200	100	0.00944	0.00748	0.00112	14.97	85.03
橡胶改性沥青	花岗岩	0.01	0.00133	200	100	0.00780	0.01734	0.0044	25.37	74.63
	玄武岩	0.01	0.00786	200	100	0.00953	0.00428	0.00094	21.96	78.04
	石灰岩	0.01	0.00626	200	100	0.00966	0.00748	0.00068	9.09	90.91
石墨烯/橡胶复合改性沥青	花岗岩	0.01	0.00133	200	100	0.00792	0.01734	0.00416	23.99	76.01
	玄武岩	0.01	0.00786	200	100	0.00959	0.00428	0.00082	19.16	80.84
	石灰岩	0.01	0.00626	200	100	0.00979	0.00748	0.00042	5.61	94.39

沥青种类	接触角/（°）
沥青种类	蒸馏水	丙三醇	甲酰胺
基质沥青	90.223	81.469	85.927
橡胶改性沥青	81.753	67.049	58.790
石墨烯/橡胶改性沥青	81.152	64.698	57.880

集料种类	接触角/（°）
集料种类	蒸馏水	丙三醇	甲酰胺
花岗岩	76.001	97.652	56.220
玄武岩	61.664	77.753	41.084
石灰岩	50.020	66.761	32.680

沥青种类	花岗岩（SiO₂）			玄武岩（CaCO₃）			石灰岩（NaAlSi₃O₈）
沥青种类	光电比色法	接触角法	分子动力学模拟	光电比色法	接触角法	分子动力学模拟	光电比色法	接触角法	分子动力学模拟
基质沥青	46.02	43.436	67.17	71.03	52.653	119.39	85.03	57.176	11480.82
橡胶改性沥青	74.63	51.304	84.89	78.04	62.008	132.29	90.91	66.039	12842.63
石墨烯/橡胶复合改性沥青	76.01	53.009	89.39	80.84	64.064	137.18	94.39	68.198	12950.86

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