道路沥青的老化动力学研究
摘要
沥青老化是影响道路沥青使用性能的重要因素,它主要有四个方面:氧化老化、挥发物的衰减、自然硬化和渗流硬化。氧化引起的硬化一直被认为是沥青老化的主要原因,氧化主要依赖于温度、时间和沥青膜的厚度,并与沥青的组成与结构有关。道路沥青老化动力学研究,有助于了解老化机理,认识老化过程,评价和预测道路沥青的老化性能,为提高其抗老化性能提供理论基础。基于此,本文通过沥青老化过程中化学结构、官能团和性能的变化以研究沥青的老化动力学。
首先,通过核磁共振氢谱和红外光谱对比了不同老化试验下(薄膜老化试验、压力老化试验和室外光氧老化试验)老化时间和老化温度对沥青化学结构的影响。核磁共振氢谱测定表明,在老化过程中沥青的芳香度是逐渐增加的,即老化是沥青组分的芳构化过程,并建立以芳香度为参数的动力学方程;推导出老化后沥青的平均分子结构,以揭示沥青的老化实质:沥青中各组成化合物化学结构的变化,引起沥青中沥青质与软沥青质的溶度参数变化,导致沥青中沥青质与软沥青质溶度参数差值增大,因而相容性降低,最终表现为沥青路用性能的衰降。红外光谱分析结果表明,沥青经老化后分子中羰基和亚砜的官能团吸收峰显著增加,老化温度越高变化越明显,表明沥青分子中的活性基团在老化过程中与氧反应,生成了以含羰基官能团的极性分子。并根据试验结果建立了羰基吸收因子和亚砜基吸收因子为参数的老化动力学模型。
其次,研究了老化对沥青流变性能的影响,结果表明老化沥青复合模量降低,相位角提高,求得平移因子a(T)在不同老化方式下的活化能,活化能越高粘弹性材料温度依赖性越低。根据复合模量主曲线计算出零切粘度,并建立了其动力学模型。
最后,采用经验分析和灰色系统理论研究了沥青老化后化学结构与沥青性能的指标变化的关系。结果表明,老化沥青羰基吸收因子的增加是导致沥青粘度增加的直接原因,化学分子结构的变化是导致物理性能变化的的直接原因。
Asphalt ageing is one of the principal factors causing the deterioration of asphalt pavements. In asphalt ageing, four types of mechanisms are involved. The processes contributing to this type of ageing include oxidation, loss of volatile components, exudation (migration of oily components from the asphalt into the aggregate) and physical hardening. The mechanism of asphalt oxidation is very complex. The functionalities formed should introduce an increase in the overall polarity of the asphalt, which in turn will influence asphalt performance. The aging kinetic model could offer a simple and feasible way to study the aging process of road asphalt, so as to evaluate deferent performance of the asphalt and reveal the chemical aging mechanism of asphalt. In this paper, the author tried to set up a first order aging kinetic model based on chemical structures and physical properties to investigate the anti-aging performance of aging asphalt.
This paper studied the influence of on chemical structures and physical properties of asphalt through thin film oven test (TFOT), Pressure Aging Vessel test (PAV) and long-time ray-oxidizing field aging. The investigation of the structure of aging asphalt by Nuclear Magnetic Resonance (NMR) hydrogen spectra is recommended. Study showed that the content of aromaticity increased during the ageing process and a complete system is established for estimating concentrations of structural groups and structural parameters. The solubility parameter model was used to predict the ageing effect. The change of functional-group of asphalt was investigated by FT-IR spectra. The results showed that the content of carbonyl absorbing peak increasing in ageing. The change in the content of aromaticity and C=O for aging asphalt was described by a first-order Arrhenius equation, with a small activation energies that suggested a diffused-controlled process of the oxidation of the asphalt highly dependent of aging time, and the aging process of road asphalt could be expressed by said aging kinetic model.
Secondly, the effects of ageing on the rheological properties of asphalt were taken into consideration. The results indicate that the complex modulus is decreased increased while the phase angel is increased. The correlation between the shift factor and the apparent activation energy show that the lower activation energy is an index of a lower temperature deoendence of viscoelastic materals. The change of zero shear viscosity was described by a first-order aging kinetic model.
In this paper, grey system theory was used to study the relationship between the change of asphalt chemical structure and the change of its deferent performance during its aging. The associated degree analysis showed that the change of the absorbance of C=O is the most important reason why the zero shear viscosity turns increase and the change of molecule structr is the main reason why the deferent performance of the asphalt turns worse after aging. The result from mathematics analysis was in accordance with that from experiential analysis.
首先,通过核磁共振氢谱和红外光谱对比了不同老化试验下(薄膜老化试验、压力老化试验和室外光氧老化试验)老化时间和老化温度对沥青化学结构的影响。核磁共振氢谱测定表明,在老化过程中沥青的芳香度是逐渐增加的,即老化是沥青组分的芳构化过程,并建立以芳香度为参数的动力学方程;推导出老化后沥青的平均分子结构,以揭示沥青的老化实质:沥青中各组成化合物化学结构的变化,引起沥青中沥青质与软沥青质的溶度参数变化,导致沥青中沥青质与软沥青质溶度参数差值增大,因而相容性降低,最终表现为沥青路用性能的衰降。红外光谱分析结果表明,沥青经老化后分子中羰基和亚砜的官能团吸收峰显著增加,老化温度越高变化越明显,表明沥青分子中的活性基团在老化过程中与氧反应,生成了以含羰基官能团的极性分子。并根据试验结果建立了羰基吸收因子和亚砜基吸收因子为参数的老化动力学模型。
其次,研究了老化对沥青流变性能的影响,结果表明老化沥青复合模量降低,相位角提高,求得平移因子a(T)在不同老化方式下的活化能,活化能越高粘弹性材料温度依赖性越低。根据复合模量主曲线计算出零切粘度,并建立了其动力学模型。
最后,采用经验分析和灰色系统理论研究了沥青老化后化学结构与沥青性能的指标变化的关系。结果表明,老化沥青羰基吸收因子的增加是导致沥青粘度增加的直接原因,化学分子结构的变化是导致物理性能变化的的直接原因。
Asphalt ageing is one of the principal factors causing the deterioration of asphalt pavements. In asphalt ageing, four types of mechanisms are involved. The processes contributing to this type of ageing include oxidation, loss of volatile components, exudation (migration of oily components from the asphalt into the aggregate) and physical hardening. The mechanism of asphalt oxidation is very complex. The functionalities formed should introduce an increase in the overall polarity of the asphalt, which in turn will influence asphalt performance. The aging kinetic model could offer a simple and feasible way to study the aging process of road asphalt, so as to evaluate deferent performance of the asphalt and reveal the chemical aging mechanism of asphalt. In this paper, the author tried to set up a first order aging kinetic model based on chemical structures and physical properties to investigate the anti-aging performance of aging asphalt.
This paper studied the influence of on chemical structures and physical properties of asphalt through thin film oven test (TFOT), Pressure Aging Vessel test (PAV) and long-time ray-oxidizing field aging. The investigation of the structure of aging asphalt by Nuclear Magnetic Resonance (NMR) hydrogen spectra is recommended. Study showed that the content of aromaticity increased during the ageing process and a complete system is established for estimating concentrations of structural groups and structural parameters. The solubility parameter model was used to predict the ageing effect. The change of functional-group of asphalt was investigated by FT-IR spectra. The results showed that the content of carbonyl absorbing peak increasing in ageing. The change in the content of aromaticity and C=O for aging asphalt was described by a first-order Arrhenius equation, with a small activation energies that suggested a diffused-controlled process of the oxidation of the asphalt highly dependent of aging time, and the aging process of road asphalt could be expressed by said aging kinetic model.
Secondly, the effects of ageing on the rheological properties of asphalt were taken into consideration. The results indicate that the complex modulus is decreased increased while the phase angel is increased. The correlation between the shift factor and the apparent activation energy show that the lower activation energy is an index of a lower temperature deoendence of viscoelastic materals. The change of zero shear viscosity was described by a first-order aging kinetic model.
In this paper, grey system theory was used to study the relationship between the change of asphalt chemical structure and the change of its deferent performance during its aging. The associated degree analysis showed that the change of the absorbance of C=O is the most important reason why the zero shear viscosity turns increase and the change of molecule structr is the main reason why the deferent performance of the asphalt turns worse after aging. The result from mathematics analysis was in accordance with that from experiential analysis.
引文
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[22]戴跃玲,刘道胜,杨鹏,闫锋,魏毅,高枝荣 廖克俭.道路沥青老化后组成与使用性能关系的研究.公路,2002,22(2):9-13
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[2]沈金安主编.沥青与沥青混合料路用性能.北京:人民交通出版社,2001
[3]李立寒,张南鹭.道路建筑材料.上海:同济大学出版社,1999:24-39
[4]沈金安.高速公路沥青路面早期损坏分析与防治对策.北京:人民交通出版社,1998:35-65
[5]Petersen J C,Comparison of oxidation of SHRP asphalt by two different methods.Fuel Sci.Technol.Int'I,1993,11(1):89-121
[6]L.W.Corbett.Dumbbell mix for better asphalt.Hydrocabon Process,1997,26(4):173-177
[7]沙庆林.高速公路沥青路面早期破坏现象及预防.北京:人民交通出版社,200I:99-123
[8]金鸣林,杨俊和,史美仁.道路沥青老化机理分析.上海应用技术学院报,2001,1(1):14-18
[9]郎比、J.F.拉贝克著(瑞典),崔孟元等译.聚合物的光降解、光氧化和光稳定.北京:科学出版社,1986
[10]张倩,赵洁,史梦琪等.自然因素作用下沥青老化化学机理分析.西安建筑科技大学学报,2004,36(4):457-450
[11]交通部公路科学研究所.JTJ 052-2000,公路工程沥青及沥青混合料试脸规程.北京:人民交通出版社,2000:124-154
[12]Whiteoak O.Handbook of shell asphalts.London:Shell Bitumen,UK,1991:48-74
[13]Wright J R.Determination of oxidation rates of air-blown asphalts by infrare-red spectroscopy.Appl Chem,1962,12(1):256-266
[14]Wright J R.Determination of oxidation rates of air-blown asphalts by infrare-red spectroscopy.Appl Chem,1962,12(1):256-266
[15]Petersen J C,Comparison of oxidation of SHRP asphalt by two different methods.Fuel Sci.Technol.Int'I,1993,11(1):89-121
[16]Petersen J C.Factors affecting the kinetics and mechanisms of asphalt oxidation and the relative effects of oxidation products on age hardening.Prepr.Pap.-Am.Chem.Soc,Div.Fuel Chem,1996,44(4):1322-1344
[17]Petersen J C.Factors affecting the kinetics and mechanisms of asphalt oxidation and the relative effects of oxidation products on age hardening.Prepr.Pap.-Am.Chem.Soc,Div.Fuel Chem,1996,44(4):1322-1344
[18]亓玉柱,梁文杰等.石油沥青老化性能研究.石油沥青,1987,2(3):17-36
[19]亓玉柱,王明刚,陈斌.石油沥青在连续热和空气老化中化学族组成的变化及动力学研究.石油沥青,1993,26(4):17-22
[20]王明刚,廖克俭,丛玉风,杨彦海.沥青化学组成与其使用性能间的灰熵分析.石油沥青,2003,12(4):25-29
[21]周安娜,朱静.道路沥青老化过程中沥青组成与分子量分布的变化.安徽工业大学学报,2001,18(4):347-351
[22]戴跃玲,刘道胜,杨鹏,闫锋,魏毅,高枝荣 廖克俭.道路沥青老化后组成与使用性能关系的研究.公路,2002,22(2):9-13
[23]闫锋,魏毅,戴跃玲,杨鹏,刘道胜,廖克俭.沥青抗老化性能的研究.抚顺石油学院学报,2002,22(2):5-8
[24]水恒福.1H-NMR和IR对道路沥青老化过程的影响.华东理工大学学报,1998,24(4):405-409.
[25]丛玉凤,廖克俭,翟玉春.道路沥青老化动力学的研究—以软化点为参数建立沥青老化动力学模型.石油炼制与化工,2005,36(5):23-26
[26]Bamford C H,et al.Comprehensive Chemical Kinetics Volumen 22 Reactions in the Solid State.Ameterdam-Oxfod-New York:Elsecier Scientific Publishing Company,1980
[27]Brown M E,Maciejewski M,et al.Thermochimica Acta,2000,355:125.
[28]A.Yu.Kopylov,Study of structural parameters on some petroleum aromatic fractions by ~1H n.m.r.-i.r,and ~(13)C,~1H n.m.r,spectroscopy,fuel,1984,Vol 63,February 273.
[29]V.G.Kozin,The Use of Pulse Nuclear Magnetic Resonance for Studying the Mechanism of Solvation Separation of Natural Bitumen,Russian Journal of Applied Chemistry,Vol.74,No.5,2001,pp.870 3876.
[30]Laurent Michon,Estimation of average structural parameters of bitumens by ~(13)C nuclear magnetic resonance spectroscopy.Fuel Vol.76,No.1,pp.9-15,1997
[31]Laurent C.Michon,A ~(13)C NMR and DSC Study of the Amorphous and Crystalline Phases in Asphalts.Energy & Fuels 1999,13,602-610
[32]M.N.Siddiqui,M.F.Ali.Investigation of chemical transformations by NMR and GPC during the laboratory aging of Arabian asphalt.Fuel 78(1999)1407-1416
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