EVA/POE/EPDM/OMMT纳米复合发泡材料的制备与性能研究
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摘要
乙烯-醋酸乙烯酯共聚物（EVA）发泡材料具有比重轻、柔软、减震、无毒、耐化学药品等优点，广泛用于运动鞋底、箱包内衬、保温材料、隔音材料等的制造。作为轻质材料的使用，EVA发泡材料依然存在易变形，抗撕裂性低，回弹性能不够高等缺陷，从而限制了它的使用。开发密度低，柔软抗震，同时具有高回弹性能和优异的压缩永久变形性能的新型EVA基复合发泡材料，具有重要意义。本文将纳米改性技术与聚合物共混改性技术结合起来，制备了综合性能优异的EVA基纳米复合发泡材料，主要包括以下三方面内容：
（1）蒙脱土（MMT）的有机化改性及其对EVA发泡材料的影响研究。考察了未改性蒙脱土（MMT）在EVA基体中的分散性，研究了EVA/MMT复合发泡材料的泡孔结构及性能。采用不同阳离子季铵盐表面活性剂改性MMT，考察改性剂的碳链长度、碳链数目对MMT插层行为的影响，系统研究不同有机改性蒙脱土（OMMT）对EVA基发泡材料微观结构和综合性能的影响规律。通过有机化改性后，OMMT在EVA基体中的分散性和界面相容性得到提高，在发泡过程中起到异相成核的作用；阳离子季铵盐表面活性剂的碳链长度及碳链数目对EVA/OMMT纳米复合发泡材料的微观结构具有显著的影响，进而影响其物理性能。通过考察双十八烷基二甲基氯化铵改性的蒙脱土的官能团结构、分散状况对EVA/OMMT复合发泡材料的影响，分析了OMMT片层对于EVA发泡材料增强增韧的机理。结合EVA/OMMT纳米复合发泡材料的微观形貌和宏观性能，探索了EVA异相成核发泡过程中OMMT粒径的临界值。
（2）乙烯-辛烯共聚物弹性体（POE）对EVA基发泡材料增强改性的研究。考察了POE与EVA之间的相容性及复合材料的储能模量。对POE/EVA体系进行发泡，考察了不同POE含量对复合发泡材料微观形貌的影响以及物理性能的影响。研究发现，POE的引入使复合发泡材料的回弹性能显著提高。对EVA/POE/OMMT三元发泡体系进行研究，考察复合发泡材料的泡孔形貌及综合性能，分析POE对EVA/OMMT两相体系的影响，并对POE改善复合发泡材料的回弹性能进行了理论分析。
（3）三元乙丙橡胶（EPDM）对EVA发泡材料增强改性的研究。考察了EPDM与EVA基体之间的相容性。通过将EPDM加入EVA基体中进行共混发泡，分别考察了EPDM占基体不同比例对EVA/EPDM及EVA/POE/EPDM/OMMT复合发泡材料的微观结构及物理性能的影响。加入EPDM后，无论是EVA/EPDM发泡材料体系还是EVA/POE/EPDM/OMMT复合发泡体系，复合发泡材料的泡孔孔径均变小，泡孔壁厚增加，复合发泡材料的压缩永久变形性能得到明显改善。对比加入EPDM和未加EPDM的复合发泡材料的压缩实验，观察特定时间点两种发泡材料泡孔形貌的差异，研究EPDM对复合发泡材料的形变恢复能力的影响，并对其改善压缩永久变形性能的机理进行了分析。
Ethylene vinyl acetate copolymer (EVA) foams, because of their lightweight, softness, good shock absorption, non-toxicity and resistance to chemicals,have been widely used in the manufacture of soles of athletic shoes, luggagelining, thermo-insulating materials, and sound-proof materials. Nonetheless, aslightweight material, EVA foams are fraught with weaknesses such as pronenessto deform, low tear resistance, and low rebound resilience, which consequentlylimit its application. Thus, it is of great significance to develop new compositefoams based on EVA with properties such as low density, softness, high reboundresilience and excellent compression set. This paper discussed the preparation ofEVA-based nanocomposites with outstanding comprehensive properties, byintegrating nano modification and polymer blending modification. The followingthree aspects were highlighted:
(1) Organic modification of montmorillonite (MMT) and its effect on theproperties of EVA foams. The dispersion of pre-modified MMT in the EVAmatrix was examined. The cell structure of EVA/MMT composite foams andtheir physical properties were discussed. MMT was modified by differentcationic quaternary ammonium surfactants. The effect of length and quantity ofcarbon chain in the surfactants on MMT intercalation was examined. The effectof different organic montmorillonite (OMMT) on the microstructure andcomprehensive properties of the EVA-based foams was investigated. After beingorganically modified, the dispersion of OMMT in the EVA matrix and theinterfacial compatibility between them was improved. OMMT played the role ofheterogeneous nucleation in the EVA foaming process. The length and quantityof carbon chain of cationic quaternary ammonium surfactant affected themicrostructure and further, affected the physical properties of the EVA/OMMTnanocomposite foams. Through the analysis of the effect of the functional groupstructure and the dispersion of the MMT modified by dioctadecyl dimethyl ammonium chloride on EVA/OMMT composite foams, the enhancing andtoughening mechanism of OMMT layers to EVA foams was analyzed. Byinvestigating the physical properties and microstructure properties of theEVA/OMMT nanocomposite foams, the threshold of OMMT particle size inEVA heterogeneous nuclearation foaming process was explored.
(2) The reinforcing modification of ethylene octene copolymer (POE) onEVA foams was studied. The compatibility between POE and EVA and thestorage modulus of the composite were examined. POE/EVA foam was producedusing mixture and blending method. The impact of different POE content on themorphology and physical properties of the composite foams was investigated. Itwas found that the rebound resilience of the composite foams significantlyincreased with the addition of POE. The EVA/POE/OMMT foaming system wasthen studied. The cell morphology and comprehensive properties of thecomposite foams were investigated. The effect of POE on the EVA/OMMTfoaming system was analyzed. In addition, a theoretical analysis on the POEimproving the rebound resilience of the composite foams had been discussed.
(3) The reinforcing modification of ethylene propylene diene monomer(EPDM) on EVA foam material was discussed. Firstly, EPDM was added to theEVA matrix and the compatibility between EPDM and EVA matrix wasexamined. The impact of different ratios of EPDM to the EVA matrix on themicrostructure and physical properties of foams were investigated. With theaddition of EPDM, the cell diameter of the composite foams became smaller andthe thickness of cell wall increased. The compression set of both EVA/EPDMfoams and EVA/POE/EPDM/OMMT composite foams was significantlyimproved. Then, composite foams with and without EPDM were compressed toobserve the difference of cell morphology at a specific time point. The effect ofEPDM on deformation reversal of the composite foams was investigated and themechanism of EPDM improving compression set was analyzed.
（1）蒙脱土（MMT）的有机化改性及其对EVA发泡材料的影响研究。考察了未改性蒙脱土（MMT）在EVA基体中的分散性，研究了EVA/MMT复合发泡材料的泡孔结构及性能。采用不同阳离子季铵盐表面活性剂改性MMT，考察改性剂的碳链长度、碳链数目对MMT插层行为的影响，系统研究不同有机改性蒙脱土（OMMT）对EVA基发泡材料微观结构和综合性能的影响规律。通过有机化改性后，OMMT在EVA基体中的分散性和界面相容性得到提高，在发泡过程中起到异相成核的作用；阳离子季铵盐表面活性剂的碳链长度及碳链数目对EVA/OMMT纳米复合发泡材料的微观结构具有显著的影响，进而影响其物理性能。通过考察双十八烷基二甲基氯化铵改性的蒙脱土的官能团结构、分散状况对EVA/OMMT复合发泡材料的影响，分析了OMMT片层对于EVA发泡材料增强增韧的机理。结合EVA/OMMT纳米复合发泡材料的微观形貌和宏观性能，探索了EVA异相成核发泡过程中OMMT粒径的临界值。
（2）乙烯-辛烯共聚物弹性体（POE）对EVA基发泡材料增强改性的研究。考察了POE与EVA之间的相容性及复合材料的储能模量。对POE/EVA体系进行发泡，考察了不同POE含量对复合发泡材料微观形貌的影响以及物理性能的影响。研究发现，POE的引入使复合发泡材料的回弹性能显著提高。对EVA/POE/OMMT三元发泡体系进行研究，考察复合发泡材料的泡孔形貌及综合性能，分析POE对EVA/OMMT两相体系的影响，并对POE改善复合发泡材料的回弹性能进行了理论分析。
（3）三元乙丙橡胶（EPDM）对EVA发泡材料增强改性的研究。考察了EPDM与EVA基体之间的相容性。通过将EPDM加入EVA基体中进行共混发泡，分别考察了EPDM占基体不同比例对EVA/EPDM及EVA/POE/EPDM/OMMT复合发泡材料的微观结构及物理性能的影响。加入EPDM后，无论是EVA/EPDM发泡材料体系还是EVA/POE/EPDM/OMMT复合发泡体系，复合发泡材料的泡孔孔径均变小，泡孔壁厚增加，复合发泡材料的压缩永久变形性能得到明显改善。对比加入EPDM和未加EPDM的复合发泡材料的压缩实验，观察特定时间点两种发泡材料泡孔形貌的差异，研究EPDM对复合发泡材料的形变恢复能力的影响，并对其改善压缩永久变形性能的机理进行了分析。
Ethylene vinyl acetate copolymer (EVA) foams, because of their lightweight, softness, good shock absorption, non-toxicity and resistance to chemicals,have been widely used in the manufacture of soles of athletic shoes, luggagelining, thermo-insulating materials, and sound-proof materials. Nonetheless, aslightweight material, EVA foams are fraught with weaknesses such as pronenessto deform, low tear resistance, and low rebound resilience, which consequentlylimit its application. Thus, it is of great significance to develop new compositefoams based on EVA with properties such as low density, softness, high reboundresilience and excellent compression set. This paper discussed the preparation ofEVA-based nanocomposites with outstanding comprehensive properties, byintegrating nano modification and polymer blending modification. The followingthree aspects were highlighted:
(1) Organic modification of montmorillonite (MMT) and its effect on theproperties of EVA foams. The dispersion of pre-modified MMT in the EVAmatrix was examined. The cell structure of EVA/MMT composite foams andtheir physical properties were discussed. MMT was modified by differentcationic quaternary ammonium surfactants. The effect of length and quantity ofcarbon chain in the surfactants on MMT intercalation was examined. The effectof different organic montmorillonite (OMMT) on the microstructure andcomprehensive properties of the EVA-based foams was investigated. After beingorganically modified, the dispersion of OMMT in the EVA matrix and theinterfacial compatibility between them was improved. OMMT played the role ofheterogeneous nucleation in the EVA foaming process. The length and quantityof carbon chain of cationic quaternary ammonium surfactant affected themicrostructure and further, affected the physical properties of the EVA/OMMTnanocomposite foams. Through the analysis of the effect of the functional groupstructure and the dispersion of the MMT modified by dioctadecyl dimethyl ammonium chloride on EVA/OMMT composite foams, the enhancing andtoughening mechanism of OMMT layers to EVA foams was analyzed. Byinvestigating the physical properties and microstructure properties of theEVA/OMMT nanocomposite foams, the threshold of OMMT particle size inEVA heterogeneous nuclearation foaming process was explored.
(2) The reinforcing modification of ethylene octene copolymer (POE) onEVA foams was studied. The compatibility between POE and EVA and thestorage modulus of the composite were examined. POE/EVA foam was producedusing mixture and blending method. The impact of different POE content on themorphology and physical properties of the composite foams was investigated. Itwas found that the rebound resilience of the composite foams significantlyincreased with the addition of POE. The EVA/POE/OMMT foaming system wasthen studied. The cell morphology and comprehensive properties of thecomposite foams were investigated. The effect of POE on the EVA/OMMTfoaming system was analyzed. In addition, a theoretical analysis on the POEimproving the rebound resilience of the composite foams had been discussed.
(3) The reinforcing modification of ethylene propylene diene monomer(EPDM) on EVA foam material was discussed. Firstly, EPDM was added to theEVA matrix and the compatibility between EPDM and EVA matrix wasexamined. The impact of different ratios of EPDM to the EVA matrix on themicrostructure and physical properties of foams were investigated. With theaddition of EPDM, the cell diameter of the composite foams became smaller andthe thickness of cell wall increased. The compression set of both EVA/EPDMfoams and EVA/POE/EPDM/OMMT composite foams was significantlyimproved. Then, composite foams with and without EPDM were compressed toobserve the difference of cell morphology at a specific time point. The effect ofEPDM on deformation reversal of the composite foams was investigated and themechanism of EPDM improving compression set was analyzed.
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