摘要
聚合物的共混改性是实现高分子材料高性能化的一条重要的途径。在研究与开发高性能聚合物新材料的同时,兼顾资源、环境、能源等三大问题,使高分子产业实现可持续发展。开发新型的绿色来源、高性能、可生物降解的聚合物新材料高分子材料利用技术是一个重要的发展趋势。其中一个值得关注的方法是在生物可降解高分子共混物加工成型过程中,利用外场变化以及物理、化学手段,使分散相原位取向变形,实现共混材料的原位增强,从而简便、高效、环保地实现聚合物材料的高性能化。
本论文选取了PLA和PBS为研究对象,利用体积拉伸形变支配的叶片塑化输运设备,通过调整加工过程中的工艺参数与组分参数,成功制备了PLA/PBS全生物可降解原位增强塑料,避免了传统石油基原位增强材料对环境和资源造成破坏的缺点。而且,本文还系统研究了共混物的原位增强,通过SEM观察PLA/PBS增强塑料加工后的微结构变化,利用DSC、TGA、WAXD与DMA等手段多角度对共混塑料的结晶行为与热性能进行测试,并且,还通过力学试验全方位表征了拉伸性能、弯曲性能和冲击性能。研究结果表明,共混物的拉伸模量和弯曲强度较纯PBS最大提升30.3%和40.6%,并使分散相PLA以长条状和椭圆状均匀分散于基体PBS中,成功实现了加工过程中共混物的原位增强。
另外,研究发现,通过先高温-后低温的两次叶片挤出机加工后,共混物的分散相以长条状和椭圆状均匀分布在基体中,并且其显示出最优良的拉伸和冲击性能。而且,研究还发现热压过程并不会对共混物的微观形貌造成太大的影响。通过改变加工流场发现,螺杆挤出机制备的共混物分散相在基体中以圆形呈现,而叶片挤出机加工的则呈现长条状或椭圆状,其共混物的拉伸性能与冲击性能均优于单螺杆挤出机制备的,冲击强度同比增长最大幅度为69.31%。
分析测试表明,挤出模头和挤出速率的变化,对共混物的微观形貌、结晶行为和力学性能都有显著的影响。当模头长径比为15或挤出速率为60rpm时,所对应的共混物的分散相形貌呈现长条状和椭圆状,对共混物起到很好的增韧增强效果。
在加工工艺参数恒定后,改变共混物组分配比后发现,取向变形后的PLA并未影响PBS在共混物中的晶型。增加PLA的含量,共混物的弯曲性能和拉伸模量均得到提高,弯曲模量最大增加了24.4%。另外,交联后,分散相与基体之间的界面粘结得到提高,PBS分子链的结晶性能受到影响,共混物的耐热性能、拉伸强度、断裂伸长率和冲击强度均高于未交联的共混物,拉伸强度同比最大增幅达16.87%。同时,研究还得知,PLA和PBS的熔体流动速率分别为7.72g/10min和4.5g/10min时,PLA在PBS中以长条状和椭圆状呈现。
Blending modification is a major route to enhance performance of polymer materials.With the research and development of high performance polymer materials, the problems ofresources, environment and energy must be considered, in order to realize sustainabledevelopment of polymer industry. Therefore, it is a development trend to exploit a novel highperformance biodegradable polymer from renewable resource. One of the promising methodsof worth attention is employed to generate some deformed dispersed phase in situ duringbiodegradable polymer blending processing with physical and chemical means or externalfield change. This method puts forward a simple, effective and clean process to enhanceperformance of polymer materials.
In this paper, PLA and PBS are applied. The PLA/PBS truly biodegradable in-situreinforced plastic are prepared by Vane Extruder and changes disadvantages of traditionalpetroleum in-situ reinforcement materials, which destroying ecology environment andresources. Furthermore, the mechanism of in-situ reinforcement is systematic investigated.Morphologies of prepared blends are characterized by scanning electron microscope (SEM).Differential scanning calorimetry (DSC), thermogravimetric analysis (TGA), wide angleX-ray diffraction (WAXD) and dynamic mechanical analysis (DMA) are used to multiangularcharacterize the thermal behavior and crystalline structure of the blends. The mechanicalproperties of tensile, flexural and impact properties are examined. The results show that theincrease amplitudes of tensile modulus and flexural strength of blends are respectively30.3%and40.6%, and the PLA phase dispersed uniformly in PBS matrix displays oval shape andlong strip structure, implying that the in-situ reinforcement of blends was realized duringprocess.
In addition, the blend prepared by Vane Extruder under initial higher temperaturefollowing by lower temperature process exhibit optimum tensile and impact properties, andthe PLA phase dispersed uniformly in PBS matrix displays oval shape and long strip structure.Moreover, the effect of hot press on morphology of blends is not detected. In addition, thedispersed phase of blends prepared by single screw extruder shows round shape in matrix, andthe tensile and impact properties are inferior to the blends of Vane Extruder, which impactstrength maximum increases by approximately69.31%.
The analysis and testing show that the change of extrusion die head and extrusion ratehas great influence on the mechanical properties, crystallization behavior and morphology ofthe PLA/PBS blends. The blends associated with die head aspect ratio of15or extrusion rate of60rpm display ideal toughening and reinforcing effect. And the dispersed phase disperseduniformly in matrix displays oval shape and long strip structure.
At a fixed technological process, with the increase of PLA contents, PLA phase in PBSmatrix was shown as fibrillar structure, and the flexural properties and Young’s modulus ofblends increased as well, which increase amplitudes of flexural strength is24.4%. However,the crystalline of PBS is not change after adding PLA. Furthermore, the DCP can improve theinterfacial adhesion between PLA and PBS phase and effect crystallization capacity of PBScomponent, resulting in the higher heat resisting properties, tensile strength, elongation atbreak and notched impact strength for cosslinked PLA/PBS blends, and the tensile strengthincreases maximum by16.87%. In addition, melt flow rate proportion of disperse phase andcontinuous phase exert an important role in morphology of disperse phase. Moreover, theresults indicate that the PLA displays oval shape and long strip structure in PBS when meltflow rate proportions of disperse phase and continuous phase are respectively7.72g/10minand4.5g/10min.
引文
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