拉伸形变主导作用的TPU增韧复合材料制备及其结构性能研究
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摘要
拉伸形变主导作用的聚合物塑化输运机理是由拉伸形变支配的聚合物动态塑化加工新方法，实现了聚合物加工成型原理和方法由基于剪切流变到基于拉伸流变的变革，开辟了聚合物加工成型技术及理论研究的新领域。拉伸形变主导作用的聚合物动态塑化加工成型设备与传统螺杆挤出机相比，具有塑化输运过程能耗低、对物料的适应性广以及设备体积小等优点。在研究叶片塑化输运机理的基础上深入探讨聚氨酯增韧复合材料的制备，对基于拉伸流变的高分子材料塑化输运方法及设备的推广应用无疑具有重要意义。
通过体积拉伸形变主导作用的叶片塑化输运技术制备聚氨酯/聚丙烯增韧复合材料，并与双螺杆挤出机的剪切流场塑化加工进行对比，揭示拉伸形变主导作用的叶片塑化加工对复合材料结构与性能的影响规律。研究表明，热塑性聚氨酯分散相在叶片单元内获得原位成纤，复合材料有着更完善的晶体构型、更好的热稳定性和两相相容性，最终在宏观上表现出更优越的力学性能。体积拉伸形变加工方法具有分散混合效果好、机械热历程短、原位成纤作用明显以及对物料的低剪切、低损伤等独特的加工特性。
利用拉伸形变支配的叶片塑化挤出机制备高性能聚氨酯/聚乳酸复合材料，并建立了分散相含量与材料宏观性能之间的关系。结果表明，热塑性聚氨酯能明显提高聚乳酸韧性，在高含量时独特的纤维状结构使得材料拉伸强度反而比低含量下有所提高，聚氨酯在拉伸流场作用下呈现出对聚乳酸独特的增韧作用。
在叶片塑化挤出机上制备生物可降解的聚氨酯/聚乳酸/蒙脱土纳米复合材料，并对材料在拉伸流场作用下的纳米颗粒网络结构与基体的协同作用进行深入研究。结果表明，蒙脱土在经过叶片挤出机塑化加工后在基体中呈现出插层与剥离共存的分散结构，剥离程度随着蒙脱土含量的增加而增加，而且复合材料的模量均高于聚乳酸。熔融曲线呈现独特的“双熔融峰”及其明显左移、熔融温度降低，表明复合材料在叶片挤出机的熔融挤出过程中所受热历程较短、破坏较小，分子链在拉伸流场作用下排列规整、有序取向。聚氨酯/聚乳酸/蒙脱土纳米复合材料在保持高强度的同时，模量和韧性都有着明显的提高，复合材料在强度和韧性之间取得良好的平衡。剥离的蒙脱土片层在叶片挤出机的拉伸流场作用下呈现出一种楔形收敛结构，它有利于减小了聚合物插层时所受的阻力，更有效的使蒙脱土片层发生剥离并均匀分散在聚合物基体中，并以此提出纳米蒙脱土在拉伸流场作用下分散和剥离的“双层剥离”机理。
拉伸形变主导作用的聚合物叶片塑化输运方法及设备是一种全新的聚合物加工理论和设备，本文的研究在聚氨酯增韧复合材料制备、加工成型的理论方面取得了创新性研究成果，形成了全新的高分子复合材料制备加工技术，解决了传统成型加工方法不能胜任的许多关键技术问题，为进一步研究聚合物叶片塑化挤出过程与机理打下了良好的基础，也为聚合物叶片塑化输运设备的推广应用提供了重要的理论依据。
Polymer plasticizing conveying mechanism based on elongational deformation is a novelnon-screw dynamic plasticizing processing method dominated by elongational deformation. Itis a great change of polymer processing theory from shear flow to elongational flow, breakingnew ground on polymer processing technology. Polymer dynamic plasticizing processingequipment based on elongational flow has advantages over screw equipment in low energyconsμmption, extensive adaptive for materials and small volμme. Therefore, the deeplyresearch on the dispersed mixing process of incompatible plastic is of great significance to thepopularization and application of polymer plasticizing conveying method and equipmentbased on elongational flow.
Thermoplastic polyurethane/polypropylene composite was prepared by Vane plasticizingconveying technology based on elongational deformation. The results were compared to thatprocessed by conventional shear flow, revealing the effect of plasticizing conveyingtechnology dominated by elongational flow on the structure and performance of composite.The results reveal that dispersed phase become in-situ fibrillation under the combined actionof axial flow and circμmferential flow in vane unit. The composite has smaller and narrowerparticle distribution, better crystal texture, thermal stability and compatibility, ultimatelydemonstrating better mechanical performance.
High-performance thermoplastic polyurethane/polylactic acid composite was preparedby vane plasticizing conveying technology dominated by elongational force, and therelationship between dispersed phase content and mechanical performance was established.The results show that thermoplastic polyurethane toughens polylactic acid evidently. Theunique fiberlike texture makes the tensile strength with high content larger than that with lowcontent.
Biodegradable polylactic acid/nanoclay composite and thermoplasticpolyurethane/polylactic acid/montmorillonite nanocomposites were prepared by VaneExtruder based on elongational flow. Montmorillonite presents intercalation and exfoliationstructure. Exfoliation increases with the content of montmorillonite. All of the modulus ofcomposites are higher than polylactic acid, with unique “bimodal melting peak” and reducedmelt temperature on melting curves. It states that the composites experience short heat historyand small damage during the extrusion in vane extruder, and molecular chains line array andordered orientation.The synergy of nano particle network configuration and elastomer underelongational flow was also investigated. The results show that the stiffness and toughness of composite increase evidently with the tensile strength remaining high level. The compositefinds a proper equilibriμm between strength and toughness.Besides, in the effect of VaneExtruder elongational flow exfoliated montmorillonite platelets present a convergent structuredecreasing the resistance during polymer intercalation, which makes the montmorilloniteplatelets exfoliate more effectively and homodisperse in polymer matrix. According to that,“double platelets exfoliation” mechanism of montmorillonite is put forward in the effect ofelongational flow.
Polymer plasticizing conveying method and equipment based on elongational flow arebrand new polymer processing theory and equipment. Creative progress has been made in theresearch about polymer preparation and processing theory. Brand new preparation processingtechnology of polymer composite reaches a certain scale and many key technical problemsleft by conventional processing method have been solved. It lays the first stone of furtherresearch about extrusion process and principle of vane plasticizing and provides the basis ofthe popularization and application of vane plasticizing conveying equipment.
通过体积拉伸形变主导作用的叶片塑化输运技术制备聚氨酯/聚丙烯增韧复合材料，并与双螺杆挤出机的剪切流场塑化加工进行对比，揭示拉伸形变主导作用的叶片塑化加工对复合材料结构与性能的影响规律。研究表明，热塑性聚氨酯分散相在叶片单元内获得原位成纤，复合材料有着更完善的晶体构型、更好的热稳定性和两相相容性，最终在宏观上表现出更优越的力学性能。体积拉伸形变加工方法具有分散混合效果好、机械热历程短、原位成纤作用明显以及对物料的低剪切、低损伤等独特的加工特性。
利用拉伸形变支配的叶片塑化挤出机制备高性能聚氨酯/聚乳酸复合材料，并建立了分散相含量与材料宏观性能之间的关系。结果表明，热塑性聚氨酯能明显提高聚乳酸韧性，在高含量时独特的纤维状结构使得材料拉伸强度反而比低含量下有所提高，聚氨酯在拉伸流场作用下呈现出对聚乳酸独特的增韧作用。
在叶片塑化挤出机上制备生物可降解的聚氨酯/聚乳酸/蒙脱土纳米复合材料，并对材料在拉伸流场作用下的纳米颗粒网络结构与基体的协同作用进行深入研究。结果表明，蒙脱土在经过叶片挤出机塑化加工后在基体中呈现出插层与剥离共存的分散结构，剥离程度随着蒙脱土含量的增加而增加，而且复合材料的模量均高于聚乳酸。熔融曲线呈现独特的“双熔融峰”及其明显左移、熔融温度降低，表明复合材料在叶片挤出机的熔融挤出过程中所受热历程较短、破坏较小，分子链在拉伸流场作用下排列规整、有序取向。聚氨酯/聚乳酸/蒙脱土纳米复合材料在保持高强度的同时，模量和韧性都有着明显的提高，复合材料在强度和韧性之间取得良好的平衡。剥离的蒙脱土片层在叶片挤出机的拉伸流场作用下呈现出一种楔形收敛结构，它有利于减小了聚合物插层时所受的阻力，更有效的使蒙脱土片层发生剥离并均匀分散在聚合物基体中，并以此提出纳米蒙脱土在拉伸流场作用下分散和剥离的“双层剥离”机理。
拉伸形变主导作用的聚合物叶片塑化输运方法及设备是一种全新的聚合物加工理论和设备，本文的研究在聚氨酯增韧复合材料制备、加工成型的理论方面取得了创新性研究成果，形成了全新的高分子复合材料制备加工技术，解决了传统成型加工方法不能胜任的许多关键技术问题，为进一步研究聚合物叶片塑化挤出过程与机理打下了良好的基础，也为聚合物叶片塑化输运设备的推广应用提供了重要的理论依据。
Polymer plasticizing conveying mechanism based on elongational deformation is a novelnon-screw dynamic plasticizing processing method dominated by elongational deformation. Itis a great change of polymer processing theory from shear flow to elongational flow, breakingnew ground on polymer processing technology. Polymer dynamic plasticizing processingequipment based on elongational flow has advantages over screw equipment in low energyconsμmption, extensive adaptive for materials and small volμme. Therefore, the deeplyresearch on the dispersed mixing process of incompatible plastic is of great significance to thepopularization and application of polymer plasticizing conveying method and equipmentbased on elongational flow.
Thermoplastic polyurethane/polypropylene composite was prepared by Vane plasticizingconveying technology based on elongational deformation. The results were compared to thatprocessed by conventional shear flow, revealing the effect of plasticizing conveyingtechnology dominated by elongational flow on the structure and performance of composite.The results reveal that dispersed phase become in-situ fibrillation under the combined actionof axial flow and circμmferential flow in vane unit. The composite has smaller and narrowerparticle distribution, better crystal texture, thermal stability and compatibility, ultimatelydemonstrating better mechanical performance.
High-performance thermoplastic polyurethane/polylactic acid composite was preparedby vane plasticizing conveying technology dominated by elongational force, and therelationship between dispersed phase content and mechanical performance was established.The results show that thermoplastic polyurethane toughens polylactic acid evidently. Theunique fiberlike texture makes the tensile strength with high content larger than that with lowcontent.
Biodegradable polylactic acid/nanoclay composite and thermoplasticpolyurethane/polylactic acid/montmorillonite nanocomposites were prepared by VaneExtruder based on elongational flow. Montmorillonite presents intercalation and exfoliationstructure. Exfoliation increases with the content of montmorillonite. All of the modulus ofcomposites are higher than polylactic acid, with unique “bimodal melting peak” and reducedmelt temperature on melting curves. It states that the composites experience short heat historyand small damage during the extrusion in vane extruder, and molecular chains line array andordered orientation.The synergy of nano particle network configuration and elastomer underelongational flow was also investigated. The results show that the stiffness and toughness of composite increase evidently with the tensile strength remaining high level. The compositefinds a proper equilibriμm between strength and toughness.Besides, in the effect of VaneExtruder elongational flow exfoliated montmorillonite platelets present a convergent structuredecreasing the resistance during polymer intercalation, which makes the montmorilloniteplatelets exfoliate more effectively and homodisperse in polymer matrix. According to that,“double platelets exfoliation” mechanism of montmorillonite is put forward in the effect ofelongational flow.
Polymer plasticizing conveying method and equipment based on elongational flow arebrand new polymer processing theory and equipment. Creative progress has been made in theresearch about polymer preparation and processing theory. Brand new preparation processingtechnology of polymer composite reaches a certain scale and many key technical problemsleft by conventional processing method have been solved. It lays the first stone of furtherresearch about extrusion process and principle of vane plasticizing and provides the basis ofthe popularization and application of vane plasticizing conveying equipment.
引文
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