Extrudate swell of linear and branched polyethylenes: ALE simulations and comparison with experiments

Extrudate swell is a common phenomenon observed in the polymer extrusion industry. Accurate prediction of the dimensions of an extrudate is important for appropriate design of dies for profile extrusion applications. Prediction of extrudate swell has been challenging due to (i) difficulties associated with accurate representation of the constitutive behavior of polymer melts, and (ii) difficulties associated with the simulation of free surfaces, which requires special techniques in the traditionally used Eulerian framework. In a previous work we had argued that an Arbitrary Lagrangian Eulerian (ALE) based finite element formulation may have advantages in simulating free surface deformations such as in extrudate swell. In the present work we reinforce this argument by comparing our ALE simulations with experimental data on the extrudate swell of commercial grades of linear polyethylene (LLDPE) and branched polyethylene (LDPE). Rheological behavior of the polymers was characterized in shear and uniaxial extensional deformations, and the data was modeled using either the Phan–Thien Tanner (PTT) model or the eXtended Pom–Pom (XPP) model. Additionally, flow birefringence and pressure drop measurements were done using a 10:1 contraction–expansion (CE) slit geometry in a MultiPass Rheometer. Simulated pressure drop and contours of the principal stress difference were compared with experimental data and were found to match well. This provided an independent test for the accuracy of the ALE code and the constitutive equations for simulating a processing-like flow. The polymers were extruded from long (L/D = 30) and short (L/D = 10) capillaries dies at 190 °C. ALE simulations were performed for the same extrusion conditions and the simulated extrudate swell showed good agreement with the experimental data.     

Quantitative evaluation of extrudate swell from viscoelastic properties of polystyrene

A theory of extrudate swell for short, intermediate or long dies is presented. In our experiment, we consider that the swelling phenomenon is mainly due to the recoverable elongational strain induced by the converging flow at the die entrance, as well as by recoverable shear strain originating within the die. From these concepts, an equation has been derived for the quantitative prediction of extrudate swell from the elastic material properties such as the entrance pressure drop, the relaxation modulus and the recoverable shear strain. Excellent agreement is found between predicted and measured values of extrudate swell obtained on commercial polystyrene melt, using capillaries of length-to-diameter ratios ranging from 1 to 20 and in a wide range of shear rates.     

Distortions of polymer melt extrudates and their elimination using slippery surfaces

An overview is given of extrudate distortions, flow fields and flow curves observed for flexible polymer melts, when they are extruded using axisymmetric or two-dimensional dies.Die walls with high surface energy and low-energy slippery surfaces are considered, as well as the influence of wall roughness.     

Morphology development of a PS/PMMA polymer blend during flow in dies

The morphology development in dilute and semi-concentrated blends (2 and 15 wt% disperse phase) of viscoelastic polymers is studied during flow in dies. In the entrance region the droplets deform into fibrils. In the die itself some of the fibrils can break up depending on their shear history and hence on their radial position. The morphology at the exit of the die is investigated by quenching the extrudate and visualizing the structure via scanning electron microscopy (SEM). For fibrils moving along the die axis, the theory of Tomotika for break-up of a fibril in a quiescent matrix describes the observations satisfactorily. Fibrils flowing off center undergo a shearing flow in the die, which could have an effect on the growth of the Rayleigh disturbances that cause break-up. It is observed that during flow break-up still occurs via Rayleigh instabilities. As a first approximation the theory of Tomotika also predicts the break-up of fibrils flowing off center, if the viscosity at the relevant shear rate is used.     

A simple model to predict extrudate swell of polystyrene and linear polyethylenes

In a previous paper (Guillet and Seriai, 1991) we derived a simple analytical expression which allows the prediction of extrudate swell of polystyrene in a wide range of residence time. This was done using the rubber-like elasticity theory and calculation of the elongational strain recovery of a Lodge fluid. The theoretical extrudate swell ratio mainly depends on the relaxation modulus, the extension ratio and the recoverable shear strain. The main advantage of this model is to provide good accuracy with short dies in a wide range of shear rate. In this paper, we examine the validity of the proposed equation with different contraction ratios at the die entrance (ECR) and its ability to predict extrudate swell of other commodity polymers such as polyethylenes.     

Three-dimensional streamlined finite elements: Design of extrusion dies

A method to determine three-dimensional die shapes from extrudate swell and vice versa is presented using a three-dimensional Galerkin finite element method based on a streamlined formulation with the fluid velocities and pressures represented by triquadratic and trilinear basis functions respectively. The three-dimensional streamlined method, an extension of the two-dimensional formulation, uses successive streamsurfaces to form a boundary-conforming co-ordinate system. This produces a fixd, computational domain leaving the spatial location of the elements as unknowns to be determined with the standard primary variables (u, v, w, p). The extrudate produced by a die of a given shape is considered for moderate Reynolds numbers. Finally, the method is extended to address the problem of die design, where a die profile is sought to produce a target extrudate shape.     

Prediction of extrudate swell in polymer melt extrusion using an Arbitrary Lagrangian Eulerian (ALE) based finite element method

Accurate prediction of extrudate (die) swell in polymer melt extrusion is important as this helps in appropriate die design for profile extrusion applications. Extrudate swell prediction has shown significant difficulties due to two key reasons. The first is the appropriate representation of the constitutive behavior of the polymer melt. The second is regarding the simulation of the free surface, which requires special techniques in the traditionally used Eulerian framework. In this paper we propose a method for simulation of extrudate swell using an Arbitrary Lagrangian Eulerian (ALE) technique based finite element formulation. The ALE technique provides advantages of both Lagrangian and Eulerian frameworks by allowing the computational mesh to move in an arbitrary manner, independent of the material motion. In the present method, a fractional-step ALE technique is employed in which the Lagrangian phase of material motion and convection arising out of mesh motion are decoupled. In the first step, the relevant flow and constitutive equations are solved in Lagrangian framework. The simpler representation of polymer constitutive equations in a Lagrangian framework avoids the difficulties associated with convective terms thereby resulting in a robust numerical formulation besides allowing for natural evolution of the free surface with the flow. In the second step, mesh is moved in ALE mode and the associated convection of the variables due to relative motion of the mesh is performed using a Godunov type scheme. While the mesh is fixed in space in the die region, the nodal points of the mesh on the extrudate free surface are allowed to move normal to flow direction with special rules to facilitate the simulation of swell. A differential exponential Phan Thien Tanner (PTT) model is used to represent the constitutive behavior of the melt. Using this method we simulate extrudate swell in planar and axisymmetric extrusion with abrupt contraction ahead of the die exit. This geometry allows the extrudate to have significant memory for shorter die lengths and acts as a good test for swell predictions. We demonstrate that our predictions of extrudate swell match well with reported experimental and numerical simulations.     

Extrudate swell of Newtonian fluids from converging and diverging annular dies

Finite element results are presented for the extrudate swell of Newtonian fluids from converging and diverging annular dies. Numerical calculations for a variety of diameter ratios and taper angles show the dependance of diameter and thickness swell on the angle. For diverging dies a thickness contraction occurs for angles greater than 30 degrees, while the diameter swell increases rapidly. For converging dies the design is limited to angles that do not allow contact of the inner free surfaces. The present results show that the diameter swell is highest for the diverging, followed by the straight and then the converging dies.     

Free (open) boundary condition: some experiences with viscous flow simulations

The free (or open) boundary condition (FBC, OBC) was proposed by Papanastasiou et al. (A new outflow boundary condition, International Journal for Numerical Methods in Fluids, 1992; 14:587–608) to handle truncated domains with synthetic boundaries where the outflow conditions are unknown. In the present work, implementation of the FBC has been tested in several benchmark problems of viscous flow in fluid mechanics. The FEM is used to provide numerical results for both cases of planar and axisymmetric domains under laminar, isothermal or non‐isothermal, steady‐state conditions, for Newtonian fluids. The effects of inertia, gravity, compressibility, pressure dependence of the viscosity, slip at the wall, and surface tension are all considered individually in the extrudate‐swell benchmark problem for a wide range of the relevant parameters. The present results extend previous ones regarding the applicability of the FBC and show cases where the FBC is inappropriate, namely in the extrudate‐swell problem with gravity or surface‐tension effects. Particular emphasis has been given to the pressure at the outflow, which is the most sensitive quantity of the computations. In all cases where FBC is appropriate, excellent agreement has been found in comparisons with results from very long domains. The formulation for Picard‐type iterations is given in some detail, and the differences with the Newton–Raphson formulation are highlighted regarding some computational aspects. Copyright © 2011 John Wiley & Sons, Ltd.     

Comparison of squeeze flow and vane rheometry for yield stress and viscous fluids

Two principal squeeze flow modes are investigated for yield stress and Newtonian materials squeezed by a constant force, F, between plates of equal or unequal diameters. In mode A, the material fills the space between the plates and is extruded at their periphery as their separation decreases. Experiments are described to measure the contribution to F from the extrudate. In mode B, all the material remains in contact with the planes of the plates as their separation decreases; there is no extrudate. The results of mode B experiments agree closely with the predictions of theory and give rheological parameters in fair agreement with those measured by the rotational vane method. The material properties and extrusion behaviour which complicate mode A experiments are discussed.     

A study of viscoelasticity and extrudate distortions of wood polymer composites

Natural fiber composites exhibit a characteristic surface tearing and extrudate distortions upon exiting from extrusion dies. This type of defect is characterized by highly rough, cracked, and distorted extrudate surface. In this study, the extrudate distortions and viscoelastic nature of metallocene-catalyzed polyethylene (mPE)/wood flour composites have been investigated. As the wood flour loading increases the region of linear viscoelasticity shortens. The first normal stress difference decreases, while the storage modulus increases. It was observed that increasing the wood flour loading up to 50 wt% aggravated the surface tearing; however, 60 wt% wood flour in mPE completely eliminated the surface defect. It was also found that increasing the shear rate improved the surface appearance of the filled compounds. This is due to the increased wall slip velocity of the composites at high shear rates and wood filler loadings. Increasing the diameter of the die at the same aspect ratio generally provides more severe surface tearing. This paper was presented at the 3rd Annual Rheology Conference, AERC 2006, April 27–29, 2006, Crete, Greece.     

The compressible Newtonian extrudate swell problem

We solve the compressible Newtonian extrudate swell problem in order to investigate the effect of compressiblity on the shape of the extrudate. We employ a first-order equation of state relating the density to the pressure and use finite elements for the numerical solution of the problem. Our results show that the shape of the extrudate and the final extrudate swell ratio are not significanlty affected even at high compressibility values.     

Extrudate swell of Boger fluids

Boger fluids are dilute polymer solutions exhibiting high elasticity at low apparent shear rates, which leads to high extrudate swell. Numerical simulations have been undertaken for the flow of three Boger fluids (including benchmark Fluid M1), obeying an integral constitutive equation of the K-BKZ type, capable of describing the behavior of dilute polymer solutions. Their rheology is well captured by the integral model. The flow simulations are performed for planar and axisymmetric geometries without or with gravity. The results provide the extrudate swell and the excess pressure losses (exit correction), as well as the shape and extent of the free surface. All these quantities increase rapidly and monotonically with increasing elasticity level measured by the stress ratio, S_R. It was found that the main reason for the high extrudate swelling is high normal stresses exhibited in shear flow (namely, the first normal-stress difference, N₁). Surprisingly, the elongational parameter of the model or a second normal-stress difference N₂ do not affect the results appreciably. Gravity serves to lower the swelling considerably, and makes the simulations easier and in overall agreement with previous experiments.     

Extrudate swell through an orifice die

The extrudate swell of a viscoelastic fluid through an orifice die is investigated by using a mixed finite element and a streamline integration method (FESIM), using a version of the K-BKZ model. The free surface calculation is based on a local mass conservation scheme and an approximate numerical treatment for the contact point movement of the free surface. The numerical results show a vortex growth and an increasing swelling ratio with the Weissenberg number. Convergence with mesh refinement is demonstrated, even at a high Weissenberg number of O(587), where the swelling ratio reaches a value of about 360%. In addition, it is found that the effective flow channel at the entrance region next to the orifice die is reduced due to the enhanced vortex growth, which may be a source of flow instability.     

A low‐dimensional spectral approach for transient axisymmetric free‐surface flow inside thin cavities of arbitrary shape

A low‐dimensional spectral method is used to solve the transient axisymmetric free surface flow inside thin cavities of arbitrary shape. The flow field is obtained on the basis of the lubrication equations, which are expanded in terms of orthonormal functions over the cavity gap. The formulation accounts for nonlinearities stemming from inertia and front location. The work is of close relevance to the filling stage during die casting, and injection molding, or the flow inside annular (extrusion) dies. Both flows under an imposed flow rate, and an imposed pressure at the cavity entrance are examined. The influence of inertia, aspect ratio, gravity, and wall geometry on the evolution of the front, flow rate, and pressure is assessed particularly in the early stage of flow, when a temporal behavior of the ‘boundary‐layer’ type develops. The multiple‐scale method is applied to obtain an approximate solution at small Reynolds number, Re. Comparison with the exact (numerical) solution indicates a wide range of validity for the multiple‐scale approach, including the moderately small Re range. Copyright © 2002 John Wiley & Sons, Ltd.     

聚合物熔体三维挤出胀大的数值模拟

采用有限元方法分析K-BKZ本构方程描述的聚合物熔体的三维挤出胀大.对于本构方程中偏应力张量的计算,首先给出质点的运动轨迹,分段求出局部的变形梯度张量,再求出整体的变形梯度、Cauchy-Green应变张量和 Finger应变张量,沿轨迹采用分段高斯积分计算应力.把应力作为方程的右端项,给出迭代方法,求解非线性方程组.并根据自由面处的边界条件,迭代得出出口处自由面的最终位置.对轴对称流道和矩形流道进行分析计算,并把结果与二维分析和实验结果进行了比较,显示方法是可行的.     

Numerical study of the combined effects of inertia,slip, and compressibility in extrusion of yield stress fluids

The axisymmetric extrudate swell flow of a compressible Herschel–Bulkley fluid with wall slip is solved numerically. The Papanastasiou-regularized version of the constitutive equation is employed, together with a linear equation of state relating the density of the fluid to the pressure. Wall slip is assumed to obey Navier’s slip law. The combined effects of yield stress, inertia, slip, and compressibility on the extrudate shape and the extrudate swell ratio are analyzed for representative values of the power-law exponent. When the Reynolds number is zero or low, swelling is reduced with the yield stress and eventually the extrudate contracts so that the extrudate swell ratio reaches a minimum beyond which it starts increasing asymptotically to unity. Slip suppresses both swelling and contraction in this regime. For moderate Reynolds numbers, the extrudate may exhibit necking and the extrudate swell ratio initially increases with yield stress reaching a maximum; then, it decreases till a minimum corresponding to contraction, and finally, it converges asymptotically to unity. In this regime, slip tends to eliminate necking and may initially cause further swelling of the extrudate, which is suppressed if slip becomes stronger. Compressibility was found to slightly increase swelling, this effect being more pronounced for moderate yield stress values and wall slip.     

Extrusion of a compressible Newtonian fluid with periodic inflow and slip at the wall

We explore a mechanism of extrusion instability, based on the combination of nonlinear slip and compressibility. We consider the time-dependent compressible Newtonian extrudate swell problem with slip at the wall. Steady-state solutions are unstable in regimes where the shear stress is a decreasing function of the velocity at the wall. Compressibility provides the means for the alternate storage and release of elastic energy, and, consequently, gives rise to periodic solutions. The added novelty in the present work is the assumption of periodic volumetric flow rate at the inlet of the die. This leads to more involved periodic responses and to free surface oscillations similar to those observed experimentally with the stick-slip instability. To numerically simulate the flow, we use finite elements in space and a fully-implicit scheme in time.Dedicated to the memory of Prof. Tasos Papanastasiou     

Rheostructural studies of a discotic mesophase pitch at processing flow conditions

The flow-induced microstructure of a mesophase pitch was studied within custom-made dies for changing wall shear rates from 20 to 1,100 s^− 1, a flow scenario that is typically encountered during fiber spinning. The apparent viscosity values, measured at the nominal wall shear rates ranging from 500 to 2,500 s^− 1 using these dies, remain fairly constant. The microstructure was studied in two orthogonal sections: r–θ (cross section) and r–z (longitudinal mid plane). In these dies, the size of the microstructure gradually decreases toward the wall (to as low as a few micrometers), where shear rate is highest. Furthermore, as observed in the r–θ plane of the capillary, for a significant fraction of the cross section, discotic mesophase has a radial orientation. Thus, the directors of disc-like molecules were aligned in the vorticity (θ) direction. As confirmed from the microstructure in the r–z plane, most of the discotic molecules remain nominally in the flow plane. Orientation of the pitch molecules in the shear flow conditions is consistent with that observed in controlled low-shear rheometric experiments reported earlier. Microstructral investigation suggests that the radial orientation of carbon fibers obtained from a mesophase pitch originates during flow of pitch through the die.