PSM/PP共混体系结构与性能研究
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摘要
通过控制聚合物形态结构达到提高材料力学性能的目标是人们关注的焦点，本文从加工过程中流变性能与结构形态对产品力学性能的影响入手，以实验测量、理论分析与数值模拟三个方面全面地分析了PSM/PP (生物基低碳材料/聚丙烯)共混物的结构与性能。
对于PSM/PP结构与形态研究，本文分析了温度序列、组分序列、剪切序列对PSM/PP共混物结构与形态、界面层厚度等的影响。1. PSM/PP(90/10)共混物中分散相为PSM颗粒，随着温度升高分散相平均粒径都有先变大后变小的规律，其粒径分布逐渐变宽，界面层厚度先变大后变小。但是共混温度对共混物力学性能的影响较小；2.随着PSM含量增加，分散相间距有明显减小的趋势，拉伸强度、弯曲强度、冲击强度均呈减小的趋势；3.140~170℃，0~103S-1剪切速率越大越有利于PSM在PP基体中的分散均匀细化，然而PSM作为分散相的粒径大小、分布宽度与冲击性能大小并没有绝对的决定性关系，验证了分散相平均粒径并不是越小其冲击性能越高的结论。实验数据显示而言，当转速为40rpm分散相颗粒粒径大小为8.36μm其冲击强度最高，其界面层厚度为0.9μm。
本文通过DMA研究表明，随着PSM含量的减少，PSM/PP共混体系的力学内耗tanδ次级转变峰越来越尖锐，验证了材料冲击性能与力学内耗tanδ成正比；-80～120℃时PSM/PP(90/10)储能模量Kerner理论值与实验值已基本吻合。
应用毛细管流变仪研究PSM/PP体系的流变学性质，1.讨论了挤出成型温度、剪切速率、LPP含量和PP支链结构对PSM流动性能的影响：140~170℃，0~103S-1下PSM/PP共混体系流动曲线具假塑性流体特点；表观粘度随温度、剪切速率增加而降低，黏度随剪切速率下降逐渐减少；170℃后曲线有向牛顿型流体变化的趋势；PSM/SCBPP比PSM/LPP的表观粘度低，PSM/LCBPP比PSM/LPP的表观粘度高；PSM对剪切速率的敏感性低于PP。2.探讨了PSM/PP共混体系粘弹性：随着口模温度的升高或口模长径比的增大挤出胀大比B相对有所减小；随着压力载荷或剪切速率增大挤出胀大比随之增大。
对于PSM/PP共混体系流变性能本构方程基础参数研究，本文利用关于B与第一法相应力差5个不同的方程式模拟PSM/PP共混体系的第一法相应力差的结果相近，这说明可选用方程之一模拟PSM/PP(90/10)共混体系的第一法向切应力作为本构方程的参数。
It is the focus of attention to improve material mechanical properties bycontrolling blend rheology and morphology. This paper studies the blend from theprocessing rheological property and morphology of the product mechanical propertyto the experimental measurements, theoretical analysis and numerical simulation toanalyse the properties of the PSM/PP (Plastic Starch bio-based Material/polypropylene) blends.
To study structure and morphology of PSM/PP (90/10) blends, this papermeasures disperse phase and interface thickness through the sequence of temperature,components and shear rate structure and morphology.1. With increasing temperature,the interface layer average particle size of PSM/PP (90/10) has become smaller, andthe size distribution is wider, and trend of the interfacial layer thickness is smaller.But the blending temperature has little effect on the mechanical properties.2. WithPSM content increased, the the surface of the dispersed phase layer, the mechanicsproperties including tensile strength, flexural strength, impact strength showesdecreasing trend.3. It is useful for improving shear rate to refine the dispersed phase.But there is not directly relationship between particle disperse phase size, distributionwidth and the impact properties. This result verifies the conclusion that the impactproperty is not higher when the average particle size of dispersed phase is smaller.
With the reduction in the content of PSM, PSM/PP blends mechanical internalfriction of the secondary transition peak became more acute through DMA studying,and it verifies mechanical internal friction is proportional to material impact property.During the entire experimental temperature range, PSM/PP (90/10) Kerner theoreticalstorage modulus and experimental values has been consistent. It is the explainationthat the Kerner theoretical storage modulus can be used as one of the constitutiveequation parameters.
The rheological behavior of PSM/PP composite was studied by die rheometer.1.The influences of temperature, shear rate, mass fraction of PP and chain branching PPon the rheological curves of PSM were investigated, used for extrusion forming. Theresults show that the rheological curves obey power law and descend along with theincrease of temperature and shear rate during140~170℃，0~103S-1, and the decliningrate is more and more small. Additionally, the curves transform from non-Newtonsection to Newton section increase when the temperature over170℃. The viscosity ofPSM/SCBPP blend is lower than PSM/LPP, and the viscosity of PSM/LCBPP blend ishigher than PSM/LPP. Finally, shear rate sensitivity of PSM is lower than PP.2.Viscoelastic: Extrudate swell B relative reduces, as the die temperature or die aspectratio increasing. And Extrudate swell B relative increases, as the pressure load orshear rate increasing.
About basic parameters of the constitutive equation for the rheological propertiesof the PSM/PP blends, in this paper, the first corresponding power differential results is similar to simulation of five different Extrudate swell B formulas. This shows thatwe can choose one of the formulas as constitutive equation parameter, throughsimulating the first corresponding power differential of the PSM/PP (90/10) blendsaccording to shear stress.
对于PSM/PP结构与形态研究，本文分析了温度序列、组分序列、剪切序列对PSM/PP共混物结构与形态、界面层厚度等的影响。1. PSM/PP(90/10)共混物中分散相为PSM颗粒，随着温度升高分散相平均粒径都有先变大后变小的规律，其粒径分布逐渐变宽，界面层厚度先变大后变小。但是共混温度对共混物力学性能的影响较小；2.随着PSM含量增加，分散相间距有明显减小的趋势，拉伸强度、弯曲强度、冲击强度均呈减小的趋势；3.140~170℃，0~103S-1剪切速率越大越有利于PSM在PP基体中的分散均匀细化，然而PSM作为分散相的粒径大小、分布宽度与冲击性能大小并没有绝对的决定性关系，验证了分散相平均粒径并不是越小其冲击性能越高的结论。实验数据显示而言，当转速为40rpm分散相颗粒粒径大小为8.36μm其冲击强度最高，其界面层厚度为0.9μm。
本文通过DMA研究表明，随着PSM含量的减少，PSM/PP共混体系的力学内耗tanδ次级转变峰越来越尖锐，验证了材料冲击性能与力学内耗tanδ成正比；-80～120℃时PSM/PP(90/10)储能模量Kerner理论值与实验值已基本吻合。
应用毛细管流变仪研究PSM/PP体系的流变学性质，1.讨论了挤出成型温度、剪切速率、LPP含量和PP支链结构对PSM流动性能的影响：140~170℃，0~103S-1下PSM/PP共混体系流动曲线具假塑性流体特点；表观粘度随温度、剪切速率增加而降低，黏度随剪切速率下降逐渐减少；170℃后曲线有向牛顿型流体变化的趋势；PSM/SCBPP比PSM/LPP的表观粘度低，PSM/LCBPP比PSM/LPP的表观粘度高；PSM对剪切速率的敏感性低于PP。2.探讨了PSM/PP共混体系粘弹性：随着口模温度的升高或口模长径比的增大挤出胀大比B相对有所减小；随着压力载荷或剪切速率增大挤出胀大比随之增大。
对于PSM/PP共混体系流变性能本构方程基础参数研究，本文利用关于B与第一法相应力差5个不同的方程式模拟PSM/PP共混体系的第一法相应力差的结果相近，这说明可选用方程之一模拟PSM/PP(90/10)共混体系的第一法向切应力作为本构方程的参数。
It is the focus of attention to improve material mechanical properties bycontrolling blend rheology and morphology. This paper studies the blend from theprocessing rheological property and morphology of the product mechanical propertyto the experimental measurements, theoretical analysis and numerical simulation toanalyse the properties of the PSM/PP (Plastic Starch bio-based Material/polypropylene) blends.
To study structure and morphology of PSM/PP (90/10) blends, this papermeasures disperse phase and interface thickness through the sequence of temperature,components and shear rate structure and morphology.1. With increasing temperature,the interface layer average particle size of PSM/PP (90/10) has become smaller, andthe size distribution is wider, and trend of the interfacial layer thickness is smaller.But the blending temperature has little effect on the mechanical properties.2. WithPSM content increased, the the surface of the dispersed phase layer, the mechanicsproperties including tensile strength, flexural strength, impact strength showesdecreasing trend.3. It is useful for improving shear rate to refine the dispersed phase.But there is not directly relationship between particle disperse phase size, distributionwidth and the impact properties. This result verifies the conclusion that the impactproperty is not higher when the average particle size of dispersed phase is smaller.
With the reduction in the content of PSM, PSM/PP blends mechanical internalfriction of the secondary transition peak became more acute through DMA studying,and it verifies mechanical internal friction is proportional to material impact property.During the entire experimental temperature range, PSM/PP (90/10) Kerner theoreticalstorage modulus and experimental values has been consistent. It is the explainationthat the Kerner theoretical storage modulus can be used as one of the constitutiveequation parameters.
The rheological behavior of PSM/PP composite was studied by die rheometer.1.The influences of temperature, shear rate, mass fraction of PP and chain branching PPon the rheological curves of PSM were investigated, used for extrusion forming. Theresults show that the rheological curves obey power law and descend along with theincrease of temperature and shear rate during140~170℃，0~103S-1, and the decliningrate is more and more small. Additionally, the curves transform from non-Newtonsection to Newton section increase when the temperature over170℃. The viscosity ofPSM/SCBPP blend is lower than PSM/LPP, and the viscosity of PSM/LCBPP blend ishigher than PSM/LPP. Finally, shear rate sensitivity of PSM is lower than PP.2.Viscoelastic: Extrudate swell B relative reduces, as the die temperature or die aspectratio increasing. And Extrudate swell B relative increases, as the pressure load orshear rate increasing.
About basic parameters of the constitutive equation for the rheological propertiesof the PSM/PP blends, in this paper, the first corresponding power differential results is similar to simulation of five different Extrudate swell B formulas. This shows thatwe can choose one of the formulas as constitutive equation parameter, throughsimulating the first corresponding power differential of the PSM/PP (90/10) blendsaccording to shear stress.
引文
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[2] Nara S, Komiya T. Studies on the relationship between water saturated state andcrystallinity by the diffraction method for moistened potato starch[J].Starch/Strike,1983,35:407-410.
[3] Wang L F, Wang Y J. Structure and physicochemical properties of acid-thinnedcorn, potato and rice starch[J]. Starch/Strike,2001,53:570-576.
[4] Paris M, Bizot H, Emery J. Crystallinity and structuring role of water in native andrecrystallized starches by13C CP-MAS NMR spectroscopy: Spectraldecomposition[J]. Carbohydrate Polymers,1999,39:327-339.
[5] Otey F H, Westhoff R P. Biodegradable film compositions prepared from starchand copolymers of ethylene andacrylic acid[J]. Industrial Engineering ChemistryProduction Research and Development,1977,16:305-308.
[6]梁兴荣.国外降解塑料发展动向[J].广东化工,1993,21:1-8.
[7]何光波.淀粉基生物降解聚合物[J].高分子学报,1996,2:116-119.
[8]彭少贤,池彩云.可生物降解淀粉基共混物的研究[J].塑料工业,2006,34:121-123.
[9] Funkea U, Bergthallera W, Lindhauera M G. Processing and characterization ofbiodegradable products based on starch[J], Polymer Degradation and Stability,1998,59:293-296.
[10]于昊.完全生物降解材料聚丙撑碳酸酯（PPC）/玉米淀粉共混物的研究[J].沈阳化工大学学报,2005,21:35-36.
[11]于九皋.淀粉细化及其与聚乙烯增容性的研究[J].化工进展,1997,3:25-29.
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