A parallel coextrusion technique for simultaneous measurements of radial die swell and velocity profiles of a polymer melt in a capillary rheometer

This article proposes a new experimental technique to simultaneously measure radial die swell and velocity profiles of polystyrene melt flowing in the capillary die of a constant shear rate rheometer. The proposed technique was based on parallel coextrusion of colored melt‐layers into uncolored melt‐stream from the barrel into and out of the capillary die. The size (thickness) ratio of the generated melt layers flowing in and out of the die was monitored to produce the extrudate swell ratio for any given radial position across the die diameter. The radial velocity profiles of the melt were measured by introducing relatively light and small particles into the melt layers, and the times taken for the particles to travel for a given distance were measured. The proposed experimental technique was found to be both very simple and useful for the simultaneous and accurate measurement of radial die swell and velocity profiles of highly viscous fluids in an extrusion process. The variations in radial die swell profiles were explained in terms of changes in melt velocity, shear rate, and residence time at radial positions across the die. The radial die swell and velocity profiles for PS melt determined experimentally in this work were accurate to 92.2% and 90.8%, respectively. The overall die swell ratio of the melt ranged from 1.25 to 1.38. The overall die swell ratio was found to increase with increasing piston speed (shear rate). The radial extrudate swell profiles could not be reasoned by the shear rate change, but were closely linked with the development of the velocity profiles of the melt in the die. The die swell ratio was high at the center (～1.9) and low (～0.9) near the die wall. The die swell ratio at the center of the die reduced slightly as the piston speed was increased. Polym. Eng. Sci. 44:1960–1969, 2004. © 2004 Society of Plastics Engineers.     

Effect of molecular structure on extrudate swell behavior for different thermoplastic melts in an electro‐magnetized die

The extrudate swell ratio of five different thermoplastic melts flowing in a constant shear rate rheometer having a capillary die with and without application of magnetic field was studied. The effects of the magnetic flux direction and density, die temperature, and wall shear rate on the extrudate swell and flow properties were investigated. The experimental results suggested that an increasing wall shear rate increased the swelling ratio for the polystyrene (PS), LLDPE, and PVC melts, but the opposite effect was observed for the ABS and PC melts. The extrudate swell ratio for the PS, ABS, PC, and LLDPE melts decreased with increasing die temperature, the effect being reversed for the PVC melt. Thermoplastic melts having high benzene content in the side‐chain and exhibiting anisotropic character were apparently affected by the magnetic field, the extrudate swell ratio increasing with magnetic flux density. The effect of the magnetic field on the extrudate swell ratio decreased in the order of PS → ABS → PC. The extrudate swell ratio for the co‐parallel magnetic field system was slightly higher than that for the counter‐parallel magnetic field system at a high magnetic flux density. POLYM. ENG. SCI., 47:270–280, 2007. © 2007 Society of Plastics Engineers.     

Extrudate swell and texture of PS,LDPE, ABS,PVC melts and their blends in extrusion capillary flow using a magnetic die

The extrudate swell behavior and extrudate texture of various thermoplastic melts, namely, polystyrene (PS), low‐density polyethylene (LDPE), acrylonitrile‐butadiene styrene (ABS) copolymer, poly(vinyl chloride) (PVC), and their blends, were examined weith a magnetic die system in a constant‐shear‐rate capillary rheometer at a shear rate range 5–28 s^?1 and a temperature range 170–230 °C. The extrudate swell results obtained from the magnetic die were then compared with those produced by a nonmagnetic die. The results showed that the extrudate swell increased with shear rate, but decreased with temperature. In a pure polymer system, up to 25% increase in the extrudate swell was observed with the application of the magnetic field to the PS melt, and the effect decreased in the order ABS > LDPE > PVC. The extrudate swell changes were associated with the changes in rheological properties of the melts. The extrudate textures of the ABS and PVC melts were improved by the magnetic field. In PS/LDPE or PS/ABS blend, it was found that the magnetic die resulted in higher values of the extrudate swell than the nonmagnetic die for all blends, the magnetic effect being less as the LDPE or ABS content was increased. For PS/LDPE system, the extrudate swell of the PS melt did not change much with addition of 20% LDPE, but slightly decreased at the LDPE loading of 40%. At higher LDPE loadings, the extrudate swell increased towards the value of the pure LDPE melt. For PS/ABS system, the extrudate swell ratio progressively decreased with increasing ABS content. © 2002 Wiley Periodicals, Inc. J Appl Polym Sci 86: 509–517, 2002     

Experimental studies on extrudate swell behavior of PS and LLDPE melts in single and dual capillary dies

Extrudate swell behavior of polystyrene (PS) and linear low‐density polyethylene (LLDPE) melts was investigated using a constant shear rate capillary rheometer. Two capillary dies with different design configurations were used, one being a single flow channel and the other being a dual flow channel. A number of extrudate swell related parameters were examined, and used to explain the discrepancies in the extrudate swell results obtained from the single and dual flow channel dies, the parameters including output rate and output rate ratio, power law index, wall shear rate, wall shear stress, melt residence time, pressure drop induced temperature rise, flow channel position relative to the barrel centerline, and the flow patterns. It was found in this work that the power law index (n value) was the main parameter to determine the output rate ratio and the extrudate swell between the large and small holes for the dual flow channel die: the greater the n value the lower the output rate ratio and thus decreased extrudate swell ratio. The differences in the extrudate swell ratio and flow properties for PS and LLDPE melts resulted from the output rate ratio and the molecular chain structure, respectively. The extrudate swell was observed to increase with wall shear rate. The discrepancies in the extrudate swell results from single and dual dies for a given shear rate were caused by differences in the flow patterns in the barrel and die, and the change in the melt velocities flowing from the barrel and in the die to the die exit. © 2002 Wiley Periodicals, Inc. J Appl Polym Sci 87: 1713–1722, 2003     

LLDPE／LDPE共混物熔体挤出胀大行为的研究

应用毛细管流变仪，考察了实验条件下线性低密度聚乙烯与低密度聚乙烯共混物（ＬＬＤＰＥ／ＬＤＰＥ）熔体挤出胀大行为及其影响因素。结果表明，挤出胀大比Ｂ与剪切应力近似呈幂律关系，而随口型长径比的增加呈指数衰减，当共混比为５０／５０时，Ｂ产生局部极涉值现象。     

Effect of die temperature on the flow of polymer melts. Part II: Extrudate swell

The effect of die wall temperature on the extrudate swell of polymer melts flowing through dies with single and dual circular channels was studied. Extrudate swell was measured at constant flow rates using an Instron capillary rheometer with a modified die section. It was found that under isothermal conditions, extrudate swell plotted against the average wall shear stress gave rise to a temperature independent correlation for polystyrene. Under non-isothermal conditions, such a correlation did not exist, which might be due to the change of wall shear stress in the axial direction. The extrudate swell in the non-isothermal cases can be better correlated with the wall shear stress at die exit. For the two-hole die, changes of die wall temperature varied both the flow rate ratio and the extru date swell ratio. The latter is, however, much less sensitive to the die wall temperature than the former.     

The effct of asymmetries of die exit geometry on extrudate swell and melt fracture

Experimental investigations were performed to see how the die exit geometry and the extrusion velocity influence on extrudate swell and melt fracture for several polymer melts [low-density polyethylene, styrene-butadiene rubber (SBR) and SBR/HAF (carbon black) compound]. Four different types of die exit geometry were considered; 0° (symmetric. usual capillary die), and 30°, 45° and 60° (asymmetric dies) were chosen for the die exit angle. Extrudate diameters were measured without draw-down under isothermal condition. Polymer melts were extruded into an oil that has the same density and temperature as those of the extrudate. Extrudate swells from dies with different diameters were correlated with volumetric flow rates. It was observed that the extrudate swell increases with increasing volumetric flow rate and exhibits through a minimum value at about 45° die exit angle. As to the fracture phenomena, it was observed that the critical shear for the onset of melt fracture increases with the increasing die exit angle up to 45°. However, for 60° die exit angle, the onset of melt fracture is again similar to that of 0° exit angle.     

Melt elasticity behavior and extrudate characteristics of rigid poly(vinyl chloride)/epoxidized natural rubber miscible blends

A study on the melt elasticity behavior and extrudate characteristics of melts of rigid poly(vinyl chloride), PVC, and rigid poly(vinyl chloride)/epoxidized natural rubber (ENR) miscible blends were conducted. Extrusion studies were carried out in a capillary rheometer and examinations of the surface characteristics of the extrudate were made by taking photomicrographs in a scanning electron microscope. The anomalous behavior in the die swell ratio of rigid PVC arising from the particle agglomerates continued in its blends up to 50 wt% composition of ENR. Temperature independence for high ENR blends was noted for the principal normal stress difference and elastic shear modulus, when shear stress was held constant. Recoverable shear strain and die swell ratio behaved identically in terms of blend composition and processing temperature. Factors which control the extrudate distortion and melt fracture of the melts of rigid PVC/ENR systems were fusion of particle agglomerates and strength of melts. Diamond cavitations were typical of the extrudate surface of PVC melts as those of the fracture surface of the tensile failure of PVC. Conditions to obtain a smooth extrudate surface of rigid PVC melts in blends with ENR have been found to be the low ENR content, low shear rate, or stress and high processing temperature.     

Die design for rigid PVC—the effect of die land length on extrudate swell

PVC profile extrusion compounds have a unique morphology. While other polymers gradually decrease in extrusion die swell with increasing length/thickness (L/D) ratio, PVC profile extrusion compounds have a low die swell, quite independent of the die's L/D ratio in the range of 5 to 20. The fact that the die land length can be changed without changing the extrudate swell is an important consideration, which makes die design and balancing dies simpler and easier for PVC profile extrusion compounds. While other polymers substantially increase extrudate swell with increased shear rate, the swell of the PVC profile compounds is not much affected by shear or extrusion rate. This unique behavior allows wider processing latitude in profile extrusion and faster extrusion rates than with other polymers. Another unique factor in the rheology of PVC profile extrusion compounds is that extrusion die swell increases with increasing melt temperature, while other polymers have decreasing die swell with increasing melt temperature. The unusual rheology of PVC profile extrusion compounds is attributed to its unique melt morphology, where the melt flow units are 1 um bundles and molecules that have low surface to surface interaction and entanglement at low processing temperatures but increased melting and increased entanglement at higher processing temperatures. Other polymers, unlike PVC, have melt flow at the molecular level.     

Rheological behavior of highly filled ethylene propylene diene rubber compounds

The rheological behavior of highly filled ethylene propylene diene rubber (EPDM) compounds was studied with respect to the effect of curative system, grafted rubber, shear rate, temperature and die swell using a Monsanto Processability Tester (MPT) to gain an understanding of the molecular parameters that control the surface finish. All systems show pseudoplastic behavior. At a particular shear rate, shear viscosity increases with blend ratio. The dependence of flow behavior on extrusion velocity indicates a surface effect. The extrudate die swell and maximum recoverable deformation are related by a linear relationship, which is independent of sulfur/accelerator ratio, extrusion temperature and shear rates and blend ratio. The principal normal stress difference increases nonlinearly with shear stress. Activation energy decreases with shear rate in most cases. The faster relaxing system produces extrudate of better surface quality.     

Die swell of liquid crystal-forming solutions of hydroxypropyl cellulose through a long capillary die

The die swell and shear viscosity of lyotropic liquid crystal-forming hydroxypropyl cellulose solutions in N,N-dimethylacetamide were determined over a relatively wide range of shear stress or polymer concentration at 30°C by using a long capillary die with an aspect ratio of 114. The dependence of die swell on the concentration was similar to that of shear viscosity: a maximum at a critical concentration C_a and a minimum at another critical concentration C_b (C_a < C_b). The dependence of the swell on shear stress is greatly affected by the solution phase: in an isotropic range (below C_a), the die swell increased monotonously with shear; in the vicinity of C_a, the die swell exhibited a maximum; in a biphasic range (between C_a and C_b), the die swell decreased monotonously; in a single-phase anisotropic range (above C_b), the die swell exhibited a minimum. Above C_b, extrudate distortion was observed and disappeared around the shear where the die swell exhibited a minimum.     

Effects of plasticizer on shear modification of polystyrene

The elastic and viscous properties of polymer melts may be affected by the shear history of the polymer. The extrudate swell of a polymer melt is primarily a manifestation of the elasticity of the polymer melt. In this study, a single screw extruder was used to impose different shear histories on a polystyrene polymer which was processed with and without added plasticizer. The extrudate swell and apparent viscosity of these melts were measured with a capillary rheometer. These characteristics of unplasticized polystyrene are almost not affected by the various preshearing processes. However, the extrudate swell and viscosity of polystyrene containing plasticizer are affected by plasticizer level, shear history and thermal history. After most of the plasticizer in the presheared plasticized polystyrene was extracted, the extrudate swell was still lower than that of the parent sheared polystyrene with the same shear history and the same plasticizer content. These results were obtained without significant changes in molecular weight. Shear modification by conventional process equipment may become impractical if the shear field intensity or dwell time of the material in the apparatus is limited. In such cases, shear refinability by standard process equipment may be observed if the coupling density in the polymer is reduced by some additional means, such as blending with a plasticizer.     

管壁厚度对微挤出成型的影响分析

基于Bird-Carreau黏度模型,运用有限元方法对三维等温微管挤出成型流动模型进行了数值分析,主要研究了管壁厚度对微管挤出成型过程中挤出胀大、速度分布、剪切速率和口模压降等重要指标的影响。结果表明,当熔体入口体积流率相等时,随着管壁厚度的增大,挤出物挤出胀大率和横截面尺寸变化量增大;口模出口端面上熔体的二次流动增强,但挤出速度和剪切速率减小;熔体在口模内的压力降明显下降;适当增加管壁厚度,有利于提高微管挤出质量。     

Melt extrudate swell behavior of multi‐walled carbon nanotubes filled‐polypropylene composites

The extrudate swell behavior of polypropylene (PP) composite melts filled with multi‐walled carbon nanotubes (MWCNTs) was studied using a capillary rheometer in a temperature range from 190 to 230°C and at various apparent shear rates varying from 50 to 800 s⁻¹. It was found that the values of the extrudate swell ratio of the composites increased nonlinearly with increasing apparent shear rates, while the values of the extrudate swell ratio decreased almost linearly with increasing temperature. The values of the melt extrudate swell ratio increased approximately linearly with increasing shear stress, while decreased approximately nonlinearly with an increase of the MWCNT weight fraction. In addition, the extrudate swell mechanisms were discussed with observation of the fracture surface of the extrudate using a scanning electronic microscopy. This study provides a basis for further development of MWCNTs reinforced polymer composites with desirable mechanical and thermal properties. POLYM. COMPOS., 38:2433–2439, 2017. © 2015 Society of Plastics Engineers     

Melt fracture,melt viscosities,and die swell of polypropylene resin in capillary flow

The melt fracture, shear viscosity, extensional viscosity, and die swell of a polypropylene resin were studied using a capillary rheometer and dies with a 0.05‐cm diameter and length/radius ratios of 10, 40, and 60. A temperature of 190°C and shear rates between 1 and 5000 s^?1 were used. A modified Bagley plot was used with consideration of pressure effects on both the melt viscosity and end effect. The shear viscosity was calculated from the true wall shear stress. When the true wall shear stress increased, the end effect increased and showed critical stresses at around 0.1 and 0.17 MPa. The extensional viscosity was calculated from the end effect and it showed a decreasing trend when the strain rate increased. Both the shear and extensional viscosities correlated well with another polypropylene reported previously. The die swell was higher for shorter dies and increased when shear stress increased. When the shear rates increased, the extrudate changed from smooth to gross melt fracture with regular patterns (spurt) and then turned into an irregular shape. In the regular stage the wavelength of the extrudates increased when the shear rate increased. The frequency of melt fracture was almost independent of the shear rate, but it decreased slightly when the die length increased. © 2002 Wiley Periodicals, Inc. J Appl Polym Sci 87: 1587–1594, 2003     

Observation of melt fracture of polypropylene resins in capillary flow

Melt fracture, shear viscosity, extensional viscosity, and die swell of two polypropylene resins were studied using a capillary rheometer. A modified Bagley plot with consideration of pressure effects on melt viscosity and end effect was used. From the true wall shear stress the shear viscosity was calculated. Extensional viscosity was calculated from the end effect. Both shear and extensional viscosities of different molecular weights and temperatures correlated well under the time-temperature Williams-Landel-Ferry (WLF) superposition. Die swell increased when shear stress increased, and was higher for shorter dies at a given shear rate. When shear rates increased the extrudate staged from smooth to gross melt fracture with regular patterns (spurt), and then turned into irregular shapes. In the regular stage the wavelength of extrudates was measured, and corresponding frequency was calculated. The frequency increased when molecular weight decreased and when melt temperature increased. The shift factor based on shear viscosity also brought frequency data of different molecular weights and temperatures into master curves. The frequency decreased slightly when die lengths increased from L/R=10 to 60. A small maximum was observed when shear rates increased.     

Melt Rheology and Morphology of Nitrile Rubber and Ethylene-Vinyl Acetate Copolymer Blends

The melt Theological behavior of nitrile rubber (NBR)/ethylene-vinyl acetate (EVA) copolymer blends was studied with special reference to the effect of the blend ratio, cross-linking systems, and shear rate using a capillary rheometer. At a given shear stress at 90°C, the viscosities of the blends vary slightly with composition. The effect of cross-linking systems [viz., sulfur (S), peroxide (DCP) and mixed (S+DCP) systems] on the viscosity of NBR/EVA blends is negligible. The melt viscosity of the blends decreases with increasing shear rate, showing pseudoplastic behavior. The flow behavior index values also support the pseudoplastic nature of these blends. Various theoretical models were used to predict the melt viscosity of the blends. Parameters such as die swell, principal normal stress difference, recoverable shear strain, and shear modulus were calculated to characterize the melt elasticity of these blends. The melt elasticity of the system was increased by the addition of NBR to EVA. The extrudate deformation at different shear rates was also studied. It was observed that as the shear rate increases, the extrudate surface exhibits a higher degree of deformation. The morphology of the extrudates of the blends at different shear rates has been examined by a scanning electron microscope. The morphology was found to be dependent on the blend ratio and shear rate.     

Swell and distortions of high-density polyethylene extruded through capillary dies

The effect of varying the die entrance angle and the die length on extrudate swell and on the onset of extrudate distortion in capillary extrusion has been studied. Using theory from the literature, we have analyzed the contribution to the total pressure drop from the elongational and shear deformation in the entrance region, and from the capillary pressure drop in the land region of the die. From the contribution of the elongational deformation, we obtained an estimate for the elongational viscosity of the polymer. The same analysis was used to study the influence of the die geometry on the stick-slip instability. It is found that the elongational component at the inlet region mainly influences the extrudate distortions. The onset of the stick-slip instability occurs within 10% at a wall stress τ_w of 0.3MPa, where τ_w is calculated from expressions assuming fully developed flow. The variation around this average value is systematic with changes in die geometry, and the observed variations are probably due to the non-homogeneous pressure field in the die. We also propose a model for predicting extrudate swell. Input to the model are material parameters obtainable from oscillatoric measurements of the loss and storage modulus and residence times calculated from the geometry of the die. The swell model includes a fitting parameter that sets the overall scale of the swell.     

高填充性聚丙烯基纳米复合材料挤出胀大行为研究

使用毛细管流变仪考察了3种高填充聚丙烯（PP）纳米复合材料的挤出胀大行为,研究了口模温度、剪切速率、熔体压力、纳米粒子填充比例和纳米粒子形貌对PP纳米复合材料熔体挤出胀大比的影响。结果表明,3种PP纳米复合体系熔体的挤出胀大比均随口模温度的增加而减小,且大致呈线性关系;随着剪切速率的增大而增加,且随着填料填充比例的增加有减小的趋势;随着熔体压力的增大而增加,并且随着熔体压力的增加,其挤出胀大比随填料填充比例的增加而减小的幅度下降;3种颗粒形貌纳米粒子填充体系中,在相同的体积分数和温度下,片状结晶纳米氢氧化镁［Mg（OH）2］填充体系熔体挤出胀大比最小,球状纳米碳酸钙（CaCO3）填充体系熔体挤出胀大比最大,棒状粒子埃洛石纳米管（HNTs）填充体系熔体挤出胀大比介于两者之间。     

Swell of extrudate from an annular die

Diameter and thickness swells have been measured as functions of time and wall shear rate for three high density polyethylenes at 170°C and one polypropylene at 190°C. By extruding into an oil having the same temperature and density as the extrudate, it was possible to measure isothermal swell in the absence of drawdown. Seventy to 80 percent of the swell occurs in the first one or two seconds, while several minutes are required to reach an equilibrium state. Relationships between various swell parameters, including parison weight swell and capillary extrudate swell, are examined. Important differences between the behavior of the polyethylenes and that of the polypropylene are noted.