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.     

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.     

Extrudate swell for a round jet with large surface tension

The problem of extrudate swell of a viscoelastic fluid from a round pipe is studied by the method of domain perturbations. The perturbation problems are solved by a finite-element method through second-order in the flow rate parameter ∈ for small flow rates. The analysis extends the work of Sturges on swelling in two-dimensional channels to round capillary tubes. In perturbation studies for small ∈, the rheology of the fluid may be expressed by three parameters, the viscosity and the two constants α₁ and α₂ appearing at order two in the expansion of the extra stress around zero shear. Surface tension has an important influence on the shape of the jet at low speeds. The shape of the surface on a round jet depends on α₁ and α₂, in the plane jet only on α₁. The analysis predicts that no matter what the constitutive equation may be, the jet will first contract if the radius of the pipe is sufficiently small. The contraction takes place in a length less than $\text{1}\text{10}$ the diameter of the jet and is followed by a swell. The contraction is usually small and may be hard to observe. There are five different contributions to the jet shape at second-order but only the viscoelastic ones persist as the pipe radius goes to zero.     

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.     

The effect of slip in the flow of a branched PP melt: experiments and simulations

In this paper visualisation and direct velocity profile measurement experiments for a branched polypropylene melt in a 10:1 axisymmetric contraction demonstrate the onset of wall slip. Video processing of the flow shows the formation of vortices and their diminution with increasing flow rate. Numerical simulations using a multimode K-BKZ viscoelastic and a purely viscous (Cross) model—both of them incorporating a nonlinear slip law—were used to predict the flow kinematics and dynamics as well as to deduce the slip velocity function by performing fitting to the velocity profiles. It was found that the numerical predictions agree well with the experimental results for the velocity profiles, and vortex formation, growth and reduction. It is suggested that such experiments (visualisation of entrance flow and direct velocity profile measurement) can be useful in evaluating the validity of constitutive equations and slip laws in the flow of polymer melts through processing equipment.     

Numerical prediction of extrudate swell of branched polymer melts

This paper is concerned with the numerical prediction of the extrudate swell behaviour of branched polymer melts in a planar configuration. The multi-mode extended pom-pom (XPP) model is used to describe the polymer dynamics. A second-order operator-integration-factor splitting scheme is used for the temporal discretisation of the problem, whilst a spectral element scheme is used in space. The free surface is evolved in a Lagrangian manner using the third-order conditionally stable Adams–Bashforth method. A thorough mesh convergence study is performed with respect to the temporal and spatial discretisation parameters. The influence of the nature of the discrete relaxation spectrum on the swelling ratio and as an indicator of polydispersity is investigated. The predictions of numerical simulations are also compared with a selection of experimental results from the literature. The parameters in the XPP model are determined from rheological data. Good agreement is obtained for branched low-density polyethylenes. The ability to model a melt with a high molecular weight tail using a discrete relaxation spectrum for which the largest relaxation time is isolated from the others is also investigated.     

Exponential shear flow of branched polyethylenes in rotational parallel-plate geometry

Exponential shear flow, as a strong flow with the potential to generate a high degree of molecular stretching, has attracted considerable interest in recent years. So far, exponential shear flow has been realized by either sliding-plate or cone-and-plate (CP) geometry. Both geometries guarantee homogeneous shear flow. Here, we present experimental data on exponential shear flow of several long-chain branched polyethylene melts with different degrees of strain hardening obtained by using parallel-plate (PP) geometry in a rotational rheometer. This type of geometry, which is standard in linear-viscoelastic characterization of polymer materials, produces inhomogeneous shear flow. A comparison of exponential shear flow data obtained by PP and CP geometry is made. Additionally, the experimental data are compared to predictions of the rubber-like liquid (RLL) and the molecular stress function (MSF) theories. For this purpose, the relaxation spectra of the polymer melts considered were obtained by standard linear-viscoelastic characterization. In addition, two irrotational parameters and one rotational parameter are required by the MSF theory. While the irrotational parameters were obtained from fitting to elongational viscosity data, the value of the rotational parameter was used as given in the literature. It can be concluded that viable experimental data in exponential shear flow can be obtained by PP geometry. For finite linear-viscoelasticity (RLL theory), predictions of reduced shear stress for CP and PP geometry coincide, but nonlinear material behavior (as modeled by the MSF theory) leads to small differences between both geometries. Furthermore, it is shown that the MSF predictions are in excellent agreement with the experimental data in exponential shear flow and that this type of flow leads to much less chain stretching than elongational flow.Dedicated to the memory of Prof. Arthur S. Lodge (1922–2005).     

Compressible rubber materials: experiments and simulations

Porous rubber materials are often used in automotive industries. In this paper, a carbon black-filled one is investigated, which is used, for example, as sealing. Such materials are distinguished by viscoelastic behaviour and by a structural compressibility induced by the porous structure. To identify the material behaviour, uniaxial tension tests and hydrostatic compression tests are performed. Therein the main focus of attention lies on the basic elasticity and on the viscoelasticity in the whole loading range. An important observation of these tests is the viscoelastic behaviour under hydrostatic compression, which has to be included in the material model. Because of the two-phase character of cellular rubber, the theory of porous media is taken into account. To model the structural compressibility, a volumetric–isochore split of the deformation gradient is used. Therein the volumetric part includes the aspect of the point of compaction. Finally, the concept of finite viscoelasticity is applied introducing an intermediate configuration. Because of the viscoelastic behaviour under hydrostatic compression, the volumetric–isochore split is taken into account for the nonequilibrium parts, too. Nonlinear relaxation functions are used to model the process-dependent relaxation times and the highly nonlinear behaviour with respect to the deformation and feedrate. The material parameters of the model are estimated using a stochastic identification algorithm.     

Die swell measurements of second‐order fluids: numerical experiments

An analysis of the flow of a second‐order fluid is presented. Reference values for some variables are defined, and with these a non‐dimensional formulation of the governing equations. From this formulation, three dimensionless numbers appear; one is the Reynolds number, and two numbers that are called the first‐ and second‐dimensionless normal stress (NSD) coefficients. The equations of motion are solved by a finite element method using a commercially available program (Fidap), and the steady state converged solution was used to measure the die swell. The factors that influence die swell and that are studied in this work include: the die geometry for circular cross sectional dies, including tubular, converging, diverging, half‐converging/half‐tubular shapes; fluid characteristics such as Reynolds number and first‐ and second‐DNS coefficients (both positive and negative values); and flow rates, as determined by the maximum velocity in a parabolic velocity profile at the entrance to the die. The results suggest that shear and deformation histories of the fluid directly influence not only swell characteristics, but also convergence characteristics of the numerical simulation. © 1999 John Wiley & Sons, Ltd.     

Creep recovery behavior of metallocene linear low-density polyethylenes

The rheological behavior of two metallocene linear low-density polyethylenes (mLLDPE) is investigated in shear creep recovery measurements using a magnetic bearing torsional creep apparatus of high accuracy. The two mLLDPE used are homogeneous with respect to the comonomer distribution. The most interesting feature of the two mLLDPE is that their molecular mass distributions are alike. Therefore, as one of the mLLDPE contains long-chain branches, the influence of long-chain branching on the elastic properties of polyethylene melts could be investigated. It was found that long-chain branches increase the elasticity of the melt characterized by the steady-state recoverable compliance. The long-chain branched mLLDPE has a flow activation energy of 45 kJ/mol which is distinctly higher than that of the other mLLDPE. The shear thinning behavior is much more pronounced for the long-chain branched mLLDPE. A discrepancy between the weight average molecular mass M _w calculated from size exclusion chromatography measurements by the universal calibration method and the zero shear viscosities of the two mLLDPE was observed. These observations are discussed with reference to the molecular architecture of the long-chain branched mLLDPE. The rheological properties of the long-chain branched mLLDPE are compared with those of a classical long-chain branched LDPE. It is surprisingly found that the rheological behavior is very much the same for these two products although their molecular mass distributions and presumedly the branching structures differ largely. Received: 15 February 1999 Accepted: 10 June 1999     

Predicting the rheology of linear with branched polyethylene blends

A series of melt blended commercial linear and branched polyethylenes are used to explore the generality of blending laws. The measured relaxation modulus G(t), and zero shear viscosity ₀ for each blend and blend fraction, have been compared with prediction for miscible blends, particularly using equations derived by Tsenoglou (1987). Plus or minus deviation between theory and measurement is dependent on the relative molecular weights of the blend components. We have found empirically that a generalised form of the blending law for G(t) and for ₀, with a floating index C, provides an improved prediction of the blend fraction data. In particular the function defining C is non-symmetrical, from which we infer the significance of branching as well as molecular weight. The optimum value of the index differs for each of our blends, in the range 1.25 to 4, the variability being accounted for by the different degrees to which branched and linear polymers relax co-operatively in the melt. Blends of two near linear polymers do not fit the floating index prediction and conform more closely, though not precisely, to the original Tsenoglou rule.     

Aerodynamics of ski jumping: experiments and CFD simulations

The aerodynamic behaviour of a model ski jumper is investigated experimentally at full-scale Reynolds numbers and computationally applying a standard RANS code. In particular we focus on the influence of different postures on aerodynamic forces in a wide range of angles of attack. The experimental results proved to be in good agreement with full-scale measurements with athletes in much larger wind tunnels, and form a reliable basis for further predictions of the effects of position changes on the performance. The comparison of CFD results with the experiments shows poor agreement, but enables a clear outline of simulation potentials and limits when accurate predictions of effects from small variations are required.     

Rheological properties of branched polystyrenes: linear viscoelastic behavior

Oscillatory shear measurements on a series of branched graft polystyrenes (PS) synthesized by the macromonomer technique are presented. The graft PS have similar molar masses (M _w between 1.3×10⁵ g/mol and 2.4×10⁵ g/mol) and a polydispersity M _w /M _n around 2. The molar masses of the grafted side chains M _w,br range from 6.8×10³ g/mol to 5.8×10⁴ g/mol, which are well below and above the critical entanglement molar mass M _c of linear polystyrene. The average number of side chains per molecule ranges from 0.6 to 6.7. The oscillatory measurements follow the time–temperature superposition principle. The shift factors do not depend on the number of branches. The zero-shear viscosities of all graft PS are lower than those of linear PS with the same molar mass, which can be attributed to the smaller coil size of the branched molecules. It is shown that the influence of branching on the frequency dependence of the dynamic moduli is weak for all graft PS that were investigated, which can be explained by the low entanglement density.Electronic Supplementary Material Supplementary material is available for this article at This article has already been published online first (DOI: ). Due to an oversight at the publisher's, this version contained several mistakes. The article is herewith republished in its entirety as a "publisher's erratum".     

An ALE method for simulations of axisymmetric elastic surfaces in flow

The dynamics of membranes, shells, and capsules in fluid flow has become an active research area in computational physics and computational biology. The small thickness of these elastic materials enables their efficient approximation as a hypersurface, which exhibits an elastic response to in-plane stretching and out-of-plane bending, possibly accompanied by a surface tension force. In this work, we present a novel arbitrary Lagrangian-Eulerian (ALE) method to simulate such elastic surfaces immersed in Navier-Stokes fluids. The method combines high accuracy with computational efficiency, since the grid is matched to the elastic surface and can, therefore, be resolved with relatively few grid points. The focus of this work is on axisymmetric shapes and flow conditions, which are present in a wide range of biophysical problems. We formulate axisymmetric elastic surface forces and propose a discretization with surface finite-differences coupled to evolving finite elements. We further develop an implicit coupling strategy to reduce time step restrictions. We show in several numerical test cases that accurate results can be achieved at computational times on the order of minutes on a single core CPU. We demonstrate two state-of-the-art applications which to our knowledge cannot be simulated with any other numerical method so far: we present first simulations of the observed shape oscillations of novel microswimming shells and the uniaxial compression of the cortex of a biological cell during an AFM experiment.     

Viscoelastic simulations of stick‐slip and die‐swell flows

Numerical solutions of viscoelastic flows are demonstrated for a time marching, semi‐implicit Taylor–Galerkin/pressure‐correction algorithm. Steady solutions are sought for free boundary problems involving combinations of die‐swell and stick‐slip conditions. Flows with and without drag flow are investigated comparatively, so that the influence of the additional component of the drag flow may be analysed effectively. The influence of die‐swell is considered that has application to various industrial processes, such as wire coating. Solutions for two‐dimensional axisymmetric flows with an Oldroyd‐B model are presented that compare favourably with the literature. The study advances our prior fixed domain formulation with this algorithm, into the realm of free‐surface viscoelastic flows. The work involves streamline‐upwind/Petrov–Galerkin weighting and velocity gradient recovery techniques that are applied upon the constitutive equation. Free surface solution reprojection and a new pressure‐drop/mass balance scheme are proposed. Copyright © 2001 John Wiley & Sons, Ltd.     

Predicting the linear viscoelastic properties of monodisperse and polydisperse polystyrenes and polyethylenes

 For linear homopolymers the linear viscoelastic predictions of the double reptation model are compared to those of a recent, more detailed model, the “dual constraint model” and to experimental data for monodisperse, bidisperse, and polydisperse polystyrene melts from several laboratories. A mapping procedure is developed that links the empirical parameter K of the double reptation model to the molecular parameter τ_e of the dual constraint model, thereby allowing the parameter K to be related to molecular characteristics such as the monomeric friction coefficient ζ. Once K (or τ_e) are determined from data for monodisperse polymers, the double reptation model predicts that for fixed weight-average molecular weight M_w, the zero-shear viscosity η₀ increases slightly with increasing polydispersity M_w/M_n for log normal distributions, while for the dual constraint model η₀ is almost independent of M_w/M_n. Experimental data for polystyrenes show no increase (or even a slight decrease) in η₀ with increasing M_w/M_n at fixed M_w, indicating a deficiency in the double reptation model. The dual constraint theory is also applied to hydrogenated polybutadienes and commercial high-density polyethylenes, where we believe it can be used to indicate the presence of long side branches, which are difficult to detect by other analytic methods. Received: 11 October 2000 Accepted: 17 May 2001     

Rheological and foaming behavior of linear and branched polylactides

In this work, a chain extender (CE) was added to polylactide (PLA) to improve its foamability. The steady and transient rheological properties of neat PLA and CE-treated PLA revealed that the introduction of the CE profoundly affected the melt viscosity and elasticity. The linear viscoelastic properties of CE-enriched PLA suggested that a long-chain branching (LCB) structure was formed from the reaction with the CE. LCB-PLA exhibited an increased viscosity, more shear sensitivity, and longer relaxation time in comparison with the linear PLA. The LCB structure was also found to affect the transient shear stress growth and elongational flow behavior. LCB-PLA exhibited a pronounced strain hardening, whereas no strain hardening was observed for the linear PLA. Batch foaming of the linear and LCB-PLAs was also examined at foaming temperatures of 130, 140, and 155 °C. The LCB structure significantly increased the integrity of the cells, cell density, and void fraction.     

Classification of thermorheological complexity for linear and branched polyolefins

Thermorheological complexity in polyolefins has been reported many times but so far it has not been systematically investigated. Here, a classification of the different types of thermorheologically complex behavior is proposed, which categorize the available data in five different types and describe key characteristics. These definitions are based on polyethylene, but other polymers show similar patterns for materials with comparable branching structure. Linear materials are thermorheologically simple as long as many very long short-chain branches do not introduce phase separation. Sparsely branched materials show the most significant thermorheological complexity, with significant shape changes of rheological functions with temperature, while higher amounts of branching (such as trees or combs) reduce thermorheological complexity and increase E_a at the same time. Low-density polyethylene shows a significant modulus shift at different temperatures probably due to excessive low molecular components.