Gross melt fracture mitigation in converging dies: A singular behavior due to polymer wall slip

This work focuses on mitigating the gross melt fracture defect of polymer flowing through axisymmetrical and two‐dimensional dies. The die entrance angle is considered as well as the influence of the converging wall roughness. Singular results are obtained with a random styrene butadiene rubber (SBR) copolymer, as the gross melt fracture defect cannot be eliminated or mitigated by reducing the die entrance angle. Other experiments carried out with rough converging dies do not give better results. Indeed, the polymer essentially slips along the walls, as shown from capillary rheometer and birefringence experiments. Thus, these results point out the importance of elongational stresses and interfacial conditions in the die entrance region on flow instabilities and the gross melt fracture defect.     

Flow analysis of natural rubber in a capillary rheometer. 1: Rheological behavior and flow visualization in the barrel

Capillary rheometers have been widely used in the study of the rheological behavior of thermoplastics but their application to rubber has so far been limited. An investigation was therefore carried out to determine the effect of mastication and temperature on the rheological properties of natural rubber using a capillary rheometer. The flow of the rubber in the barrel of the capillary rheometer was observed at various test conditions such as die geometry, piston speed, and test temperature using layers of pigmented rubber compound, this involving the use of a split barrel system. It was found that the flow patterns in the barrel of the capillary rheometer used were very complex and were a function of piston displacement.     

A study of melt density of flowing linear polyethylene

Linear polyethylene was extruded from a capillary rheometer with the driving piston operated at fixed speed and at fixed pressure. Apparent viscosity and melt density were measured in both extrusion modes. Apparent density decreased at shear rates approaching the melt fracture region in fixed piston-speed operation. Flow of other polymer melts was essentially incompressible in fixed piston-speed operation, and all polymers exhibited incompressible flow in fixed-pressure extrusion. The oscillating portion of the flow curve of linear polyethylene reflects alternating periods in which the polymer exits faster and slower than the rate at which the advancing piston clears the rheometer reservoir. Linear polyethylene behaves differently from most other polymers in fixed piston-speed extrusion and during melt fracture because of the existence of a more extensive entanglement network in the melt. It is suggested that melt fracture in general results from a tensile failure of the entanglement network, which may occur at the die inlet and in the orifice.     

Investigation of the oscillating flow phenomenon in high density polyethylene

The nature and causes of the oscillating flow phenomenon in high density polyethylene are examined in this report. Empirical equations are developed describing the onset (both stress, SSOF, and rate, SROF) of oscillating flow in terms of molecular structure. The SSOF is not constant, but is found to vary slightly with the molecular weight distribution. The SROF is shown to be predictable in terms of molecular weight distribution. The physics of the oscillations is critically examined, and the simple model of Okubo and Hori describing these oscillations has been successfully tested. The model involves alternating compression of the polymer in the capillary rheometer barrel and decompression after a material breakdown in the die, in which flow from the capillary exceeds that expected from the rheometer output for an incompressible material. The point for initiation for oscillating flow is positively identified to be in the die, not, as some have suggested, in the die entrance region. Examination of the critical shear stress for random ethylene–propylene rubbers suggests that the reason why linear polyethylene appears unique is that the critical stress may be unattainable in other polymers and that the magnitude of the effect tends toward being vanishingly small. A critical shear strain criterion seems to describe the variations in critical stress with ethylene–propylene copolymer composition, but the critical strain criterion appears to be an oversimplification in general.     

A die rotating system for moderations of extrusion load and pressure drop profiles for molten PP and wood/polypropylene composites in extrusion processes

A die‐rotating system was proposed in this work for moderations of extrusion forces and entrance pressure drop for molten polypropylene (PP) and wood/polypropylene (WPP) composites in a capillary rheometer and a single screw extruder. The effects of processing conditions and wood loading in PP were of our interests. The extrusion force and entrance pressure drop with and without the die rotating system were monitored in real‐time. This was the first time that the die‐rotating system was used for processing of highly viscous wood/polymer composite materials. It was found that the flow properties of the molten PP and WPP composites obeyed pseudoplastic non‐Newtonian behavior. The behavior was more obvious at wood contents of above 6 wt % and in the capillary rheometer. The rotation of the die could moderate the extrusion load by 60% and entrance pressure drop by 20% in the capillary rheometer, and the entrance pressure drop by 30% in the single screw extruder, especially at the conditions where the viscosities of the WPP and the extrusion rate were high. Greater fluctuations in entrance pressure drop caused by die rotation were observed in the single screw extruder. © 2010 Wiley Periodicals, Inc. J Appl Polym Sci 120:1006–1016, 2011     

Elongational viscosity of polymer melts: A lubricated skin-core flow approach

Previous work by this research group has shown that the use of a lubricated skin/core flow of polymer melts and a hyperbolic converging die results in an essentially pure elongational flow at a constant elongational strain rate in the core. The previous work was carried out on a laboratory-scale coextrusion system in a planar slit die; tracer particles and an image analysis system were used to confirm the predicted behavior. In this work, the technique was implemented first on the coextruder assembly, as a planar elongational rheometer, and then on a commercial capillary rheometer, as a uniaxial elongational rheometer for polymer melts. The later is achieved by replacing the standard capillary die with a hyperbolic axisymmetric die. A two-laycred billet is prepared for placement in the rheometer barrel by completely encapsulating the core polymer (the polymer to be analyzed) with a low-viscosity polyethylene skin. Commercial grades of polypropylenes, syndiotactic polystyrene, and nylon-66 were analyzed using this technique. Elongational viscosity at high extensional rates can be determined with this method; values in excess of 500 s⁻¹ have already been achieved. © 1996 John Wiley & Sons, Inc.     

Rheological properties,flow visualization and extrudate swell of NR compound by rotating‐die rheometer

An experimental apparatus coupled with a rotating die system was especially designed and manufactured to study the rheological properties, flow patterns and swelling behavior of natural rubber (NR) compound for different shear rates and die rotating speeds at a test temperature of 110°C, the results being compared with those by the static capillary die. It was found that NR compound used exhibited psuedoplastic non‐Newtonian behavior. The rotation of the capillary die could reduce the extrusion load. The wall shear stress for any given shear rates increased with increasing die rotating speed. The fluctuation of the entrance pressure drop increased with increasing die rotating speed. The flow pattern development in the rotating‐die rheometer was different from that observed in the static die. The flow patterns in the rotating die were clearly unstable and contained two flow components which included axial flow along the barrel and circumferential flow at the die entrance. The size and shape of the axial and circumferential flows were more dependent on the piston displacement. It was found that the swelling ratio of the NR compound decreased with increasing die rotating speed. POLYM. ENG. SCI., 2008. © 2008 Society of Plastics Engineers.     

Experimental and theoretical investigation of extrudate swell of polymer melts from small (length)/(cross-section) ratio slit and capillary dies

An experimental and theoretical study is presented of extrudate swell from short capillary and slit dies. The polymer melts studied were polystyrene and polypropylene. The swell from slit dies is greater than the swell from capillaries. Decreasing die entry angle for capillary dies decreases swell. The argument is made that elongational How existing in the die entry region and for short dies determines extrudate swell. Dimensional analysis arguments are used to relate extrudate swell to a Weissenberg number based on elongational flow at the die entrance and the detailed die geometry. Correlations are developed. The theoretical study is based on unconstrained elastic recovery following elongational How through the die entrance region.     

Flow visualization and extrudate swell of natural rubber in a capillary rheometer: Effect of die/barrel system

An investigation was carried out to examine the effect of die/barrel system on the flow patterns and extrudate swell of natural rubber in the barrel of a capillary rheometer, using a colored tracer as the visualization technique. The capillary rheometer used in this work had two dies located along the barrel, which is novel in rheometer design. The flow of the rubber in the upper barrel was dependent on the piston/barrel action and changed with piston displacement, whereas the complexity of the flow in the lower barrel was dependent not only on the piston displacement, but also on the geometry of the upper die design. The flow patterns that developed in the whole barrel were independent of the die located at the bottom of the barrel. In addition, the change in extrudate swell was associated with the flow occurring in the barrel, residence time, elastic characteristic, and the temperature rise during the flow. It was concluded that the general style of the flow patterns of natural rubber was greatly dependent on the die geometry that the material had previously moved past. © 2001 John Wiley & Sons, Inc. J Appl Polym Sci 82: 2525–2533, 2001     

Effects of Extrusion Rate,Temperature, and Die Diameter on Melt Flow Properties During Capillary Flow of Low-Density-Polyethylene

The melt flow properties of a low-density polyethylene were measured at test temperatures varying from 140 to 170°C and in a wide range of extrusion rates by means of a capillary rheometer, to identify the influence of extrusion conditions (such as temperature, shear rate, and die diameter) on the melt flow behavior in the present paper. The results showed that the entry pressure drop increased nonlinearly with an increase of the piston speeds, and it decreased with an addition of the die diameter. The melt shear flow obeyed roughly the power law and the melt shear viscosity decreased approximately linearly with an increase of the true shear rates in a bi-logarithmic coordinate system. The dependence of the melt shear viscosity on temperature accorded approximately the Arrhenius expression. Under these experimental conditions, the entrance pressure drop increases as an exponential function with an addition of the channel contraction ratio.     

Flow analysis of natural rubber in a capillary rheometer. 2: Flow patterns and entrance velocity profiles in the die

An investigation was carried out to determine the effect of variations in test conditions, such as die geometry, for example die entry angles, on the flow patterns observed in the die of a Davenport Extrusion Rheometer. In addition, the velocity profile near the die entrance was determined for different piston displacements. The results indicate that the velocity profile generated in the capillary near the die entrance was parabolic in form. However, there appeared to be a non-zero velocity at the capillary wall. Melt fracture was observed, this being linked with the appearance of a disturbance in the flow along the capillary, the disturbance being of a converging helical form.     

Converging flow analysis,entrance pressure drops,and vortex sizes: Measurements and calculated values

The use of converging flows for the determination of the elongational behavior of polymer melts is interesting provided that the solving of the inverse problem is fast. For this purpose, this paper shows that the entrance pressure drops that occur during the axisymmetric flow of a polymer melt from the reservoir of a capillary rheometer into a cylindrical die with flat entry can be rapidly calcylated using a Wagner constitutive equation and Protean coordinates. This calculation technique performs particle tracking, which is absolutely necessary when using integral constitutive equations. In turn, the method also enables the determination of the particle path in the entrance zone and gives the boundary of the vertex. The appropriate solution is obtained through the minimization of the power consumption in the entrance zone. Calculation results are compared with experimental pressure drops and vortex pictures using two well‐characterized polyethylenes and show good agreement.     

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.     

Correlation between polyethylene topology and melt flow instabilities by determining in-situ pressure fluctuations and applying advanced data analysis

Using three high sensitive pressure transducers located inside a slit-die of a capillary rheometer and applying a set of advanced mathematical tools to process the acquired time dependent pressure signals, we are able to detect in-situ pressure fluctuations associated with sharkskin instabilities. Other distortions, as spurt and gross melt fracture, can also be in-situ detected. This originates from a factor of 10³ and 10² improvement in terms of time and pressure resolution achieved using the new set-up and data analysis that it will be described in detail in this article. Our approach quantifies the effect of polymer topology and shear rate on the characteristic frequency and amplitude of these pressure fluctuations inside the die. Depending on the polymer structure and the shear rate, different instabilities with large deviation in their main properties at melt-state, can be determined. Based on our results, a polymer-independent power law relationship between the characteristic frequency of the instability and the apparent shear stress has been found. Combining this new technique with the advanced mathematical analysis used, clear evidences concerning the origin and location of these instabilities, could be established. According to our analysis, the spurt instability starts in the entrance of the die and it propagates downstream while increasing its velocity along the die. This was confirmed by non-zero-time-lags in the cross-correlation function between the transducers located inside the slit-die. In case of sharkskin instability, pressure fluctuations inside the die indicate that its origin could also be already inside the die instead of being exclusively located at the die-exit region, as stated in earlier investigations.     

Rheological properties of a liquid crystalline copolyester

Rheological studies of an experimental liquid crystalline (LC) copolyester were carried out using a capillary rheometer and a cone and plate rheometer. Rheological characteristics of the polymer in the nematic state were observed. The nematic melt was found to be pseudoplastic and the degree of pseudoplasticity varied with shear rate. Melt viscosity was found to decrease with shear rate. Negative die swelling was observed at the exit of the capillary rheometer at temperatures marginally above the solid-nematic transition temperature of the polymer and was also found to be a function of shear rate. The dynamic mechanical properties of the polymer were studied as a function of temperature. The activation energies of flow and of dynamic mechanical deformation were calculated.     

Effects of convergent flow on in situ fibrillation of TLCP in PEN

A polymer melt entering a capillary die from a cylinder undergoes a convergent flow in which there is a complex combination of extensional and shear flows. The convergent flow plays an important role in controlling the in situ fibrillation of thermotropic liquid crystalline polymer (TLCP) in a thermoplastic matrix melt. This study examines effects of the convergent flow on development of TLCP fibrils in a TLCP/poly(ethylene naphthalate) (PEN) blend. A capillary rheometer was used and the extent of the convergent flow was varied by changing capillary dimension and shear rate. With a given capillary die, the TLCP fibrillation was found to increase with increasing shear rate because of the increased deformation of TLCP droplets. The establishment of a fully developed shear velocity profile by using a relatively long die is considered to be necessary to retain the TLCP fibrils initiated in the convergent flow region. At a given high shear rate, TLCP fibrillation improves with increasing capillary diameter (≤2 mm) because of the increased difference in velocity between the capillary and the cylinder. © 2003 Wiley Periodicals, Inc. J Appl Polym Sci 91: 1505–1513, 2004     

Development of freeze flow apparatus to study filled polymer melts

A novel method to study the distribution of filler particles and polymer orientation of a polymer melt within a capillary die has been developed. Material within the die is quench‐cooled and then removed to provide information about the flow regime at the instant it was frozen. The equipment has been used to examine calcium carbonate‐filled high density polyethylene under high shear. The samples were examined using Energy Dispersive X‐ray Spectrometry (EDS) as well as being studied using X‐ray Diffraction (XRD). The distribution of filler particles across the radius of the capillary has been studied at high and low wall shear rates using EDS. A constant particle distribution across the radius of the die was observed for both flow regimes. The arrangement of crystalline structures within the specimens was examined by XRD. An increase in crystalline order was noticed with increasing wall shear rate. POLYM. ENG. SCI., 47:1937–1942, 2007. © 2007 Society of Plastics Engineers     

Elastic fracture of polystyrene solutions

Based on the assumption of a constant critical shear strain, an expression for the critical stress at the onset of entrance fracture as a function of polymer concentration has been developed. Experimental results with 10-25 percent narrow distribution, high molecular weight polystyrene-benzene solutions show the critical stress to be much lower than that for the polymer melt and in agreement with predicted values. This result is all the more impressive when the contrast in flow behavior at the capillary entrance for melts and solutions is observed. Instead of the rotating toroidal vortices surrounding a 90-deg material entrance cone observed with polystyrene melt, cine movies of the solution flow birefringence patterns in the capillary entrance region reveal only a stagnant zone surrounding a narrow cone less than 20 deg. At fracture, the cone axis moves in a rotary path circulating about the capillary axis without undergoing the flow discontinuities typical of melt behavior.     

Development of an in-line rheometer suitable for reactive extrusion processes

This paper presents the development of a novel in-line extrusion rheometer based on the flow of polymer through a wedge (vertically tapered slit). This rheometer is suitable for measuring changes in rheological properties on-line during reactive extrusion, because it can be used to estimate the viscosity for a range of shear rates without the need to change the polymer flow rate (i.e., extruder throughput). Equations have been developed to estimate the parameters of the power-law equation, used to describe the viscosity-shear rate relationship, from measurements of pressure drops along the wedge. An experimental in-line wedge rheometer has been built and used to measure the viscosity for a series of polypropylenes prepared via reactive extrusion. Viscosity measurements from the experimental in-line wedge rheometer are compared with measurements from a capillary rheometer. Good agreement is found between the capillary and wedge rheometer measurements.     

LDPE熔体在挤出口模流动时入口区流型的观测

应用毛细管流变仪测量了在接近实际挤出工艺条件下低密度聚乙烯熔体的流变性质，应用流动可视化技术，观测了试样熔体流经突然收缩的轴对称口模时的入口收敛流型，发现，在口模入口前区的两侧存在明显的环流区，环流区长度随着挤出速率和流道收缩比的增加而增大，而随着温度的升高而减小，采用环流区长度的公式估算了实验条件下试样的环流区长度值，结果表明，预测值与实测值之间有较好的一致性。