The relevance of entry flow measurements for the estimation of extensional viscosity of polymer melts

The extensional viscosity of some flexible chain polymers and a thermotropic liquid crystalline polymer was measured in uniaxial extensional flow at constant extension rate. Power law functions were found for the dependence of the extensional viscosity at constant accumulated strain on strain rate. The stress growth curves were compared with measurements in axisymmetric entry flow, where both elongation and shear occur. The comparison showed that the values of the extensional viscosity calculated from the measurements in the entry flow correspond to the ones calculated from the viscosity growth measured in uniaxial elongation and averaged over extensional strain equal to what is accumulated on the fluid as it flows from the barrel into the capillary.     

Numerical breakdown at high Weissenberg number in non-Newtonian contraction flows

 Planar contraction flows of non-Newtonian fluids with integral constitutive models are studied to investigate the problem of numerical breakdown at high Weissenberg or Debrorah numbers. Spurious shear stress extrema are found on the wall downstream of the re-entrant corner for both sharp and rounded corners. Moreover, a non-monotonic relation between shear stress and strain rate is found when the Deborah number limit is approached, which correlates with these shear extrema. This strongly suggests that non-monotonicity between shear stress and strain rate may be responsible for the Deborah number limit problem in contraction flow simulations. This non-monotonicity is caused by the inaccuracy of the quadrature, using constitutive equations that do not have shear stress maxima when exactly evaluated. This conclusion agrees with recent analytical findings by others that inaccuracy of the integration along the streamlines – either by numerical integration or asymptotic approximation – makes the problem ill-conditioned, with spurious growth occurring on the wall downstream of the re-entrant corner. Received: 5 March 1999/Accepted: 1 September 1999     

Numerical simulation of entry flow of the IUPAC-LDPE melt

Numerical simulations have been undertaken for the creeping entry flow of a well-characterized polymer melt (IUPAC-LDPE) in a 4:1 axisymmetric and a 14:1 planar contraction. The fluid has been modeled using an integral constitutive equation of the K-BKZ type with a spectrum of relaxation times (Papanastasiou–Scriven–Macosko or PSM model). Numerical values for the constants appearing in the equation have been obtained from fitting shear viscosity and normal stress data as measured in shear and elongational data from uniaxial elongation experiments. The numerical solutions show that in the axisymmetric contraction the vortex in the reservoir first increases with increasing flow rate (or apparent shear rate), goes through a maximum and then decreases following the behavior of the uniaxial elongational viscosity. For the planar contraction, the vortex diminishes monotonically with increasing flow rate following the planar extensional viscosity. This kinematic behavior is not in agreement with recent experiments. The PSM strain-memory function of the model is then modified to account for strain-hardening in planar extension. Then the vortex pattern shows an increase in both axisymmetric and planar flows. The results for planar flow are compared with recent experiments showing the correct trend.     

Instabilities in multi-hole converging flow of viscoelastic fluids

Studies of the onset of instabilities were conducted on single hole and multi-hole contractions using laser speckle visualization. A well characterized elastic fluid was used with constant viscosity of 13.1 Pa · s and elasticity characterized by a longest relaxation time constant of 2.233 s. The onset of instabilities was characterized in terms of the Deborah number and the contraction ratio. Three types of instabilities were observed: pulsing vortices, azimuthally rotating vortices, and swirling vortices. For the single hole contractions the critical Deborah number for instability increased from 4.4 to 5.07 to 5.25 as the contraction ratio increased from 4: 1 to 8: 1 to 12: 1. The magnitude of the instabilities was much greater for the 4: 1 contraction than for the other two contraction ratios. For the multi-hole contraction a square array of nine holes was used and the ratio of the hole diameter to hole spacing was varied. The height of the vortices is very similar for the single hole and multi-hole contractions at low Deborah numbers. At high Deborah numbers the effect of adjacent holes is to reduce the height of the vortices by a factor of three. For the 4: 1 spacing no secondary vortex was observed below a Deborah number of De = 3.7. Secondary vortices occurred for the 8:1 and 10:1 spacing at all Deborah numbers. Unstable pulsing vortices appeared for all spacings at a critical Deborah number around 5.5. Adjacent holes decreased the strength of the unsteady vortex motions. The centerline velocities were measured for the multi-hole contraction at shear rates of 5, 30, and 300 s^–1. The elongational strain rates are similar at a low shear rate of 5 s^–1. As shear rate is increased the onset of stretching occurs closer to the plane of the contraction for the smaller contraction ratios.     

Effect of spatial discretization schemes on numerical solutions of viscoelastic fluid flows

This study examines the effect of discretization schemes for the convection term in the constitutive equation on numerical solutions of viscoelastic fluid flows. For this purpose, a temporally evolving mixing layer, a two-dimensional vortex pair interacting with a wall, and a fully developed turbulent channel flow are selected as test cases, and eight different discretization schemes are considered. Among them, the first-order upwind difference scheme (UD) and artificial diffusion scheme (AD), which are commonly used in the literature, show most stable and smooth solutions even for highly extensional flows. However, the stress fields are smeared too much by these schemes and the corresponding flow fields are quite different from those obtained by higher-order upwind difference schemes. Among higher-order upwind difference schemes investigated in this study, a third-order compact upwind difference scheme (CUD3) with locally added AD shows stable and most accurate solutions for highly extensional flows even at relatively high Weissenberg numbers.     

On the stability of plane parallel viscoelastic shear flows in the limit of infinite Weissenberg and Reynolds numbers

Elastic effects on the hydrodynamic instability of inviscid parallel shear flows are investigated through a linear stability analysis. We focus on the upper convected Maxwell model in the limit of infinite Weissenberg and Reynolds numbers. We study the effects of elasticity on the instability of a few classes of simple parallel flows, specifically plane Poiseuille and Couette flows, the hyperbolic-tangent shear layer and the Bickley jet.The equation for stability is derived and solved numerically using the spectral Chebyshev collocation method. This algorithm is computationally efficient and accurate in reproducing the eigenvalues. We consider flows bounded by walls as well as flows bounded by free surfaces. In the inviscid, nonelastic case all the flows we study are unstable for free surfaces. In the case of wall bounded flow, there are instabilities in the shear layer and Bickley jet flows. In all cases, the effect of elasticity is to reduce and ultimately suppress the inviscid instability.     

Measuring uniaxial extensional viscosity using a modified rotational rheometer

Knowledge of the extensional behaviour of polymer melts is extremely important due to the industrial relevance of extensional flows in common processing techniques and sequences such as blow moulding, film blowing, fibre spinning, melt flow through extrusion dies and injection mould filling. One of the main problems both researchers and industrialists come across is the fact that, unlike shear flows, steady-state extensional flows are not easy to generate and maintain experimentally. This fact limits the extent to which one can characterise the materials and, therefore, the degree of optimisation of the productive process. In this paper, a modification to a commercially available controlled rate rotational rheometer is proposed in order to produce a cheap, easy to set-up, flexible extensional rheometer. This is based on the well-known Meissner-type extensional rheometer and makes use of the accurate velocity control and torque measurement possibilities of the rotational apparatus. In this case, the adaptation was performed on a TA Instruments Weissenberg Rheogoniometer, but the idea is applicable to most other similar devices. The feasibility of the modification will be discussed and confirmed, results being presented for two materials at different temperatures. These include the calculation of transient uniaxial extensional viscosity and a study of rupture conditions.     

Evaluation by means of stress relaxation (after a step strain) experiments of the viscoelastic behavior of polymer melts in uniaxial extension

 As is widely acknowledged, morphology in most materials is far more sensitive to extensional than to shear deformations but, unfortunately, due to the experimental difficulties involved, there are no non-destructive, morphology probing techniques in such flows, i.e., the equivalent of stress relaxation and oscillatory experiments in shear flows. This paper tries to overcome some of those drawbacks by proposing an experimental technique that allows stress relaxation experiments after a step strain in uniaxial extension to be performed. The benefits of this technique are twofold: (a) while the deformation is small enough for the response to be in the linear viscoelastic regime it constitutes a probe of the microstructure of the material and (b) it allows the departure to the non-linear regime to be studied, useful, for example, for the definition of the damping function in uniaxial extensional flow or for the study of the response of materials to fast transient flows with a strong extensional component, such as contraction flows. In this work the proposed technique, which requires a correction to the apparent (theoretical) strain rate in order to allow the calculation of the true Hencky strains attained during the strain step, is tested and validated for two polyisobutylene melts. Received: 9 April 2001 Accepted: 26 July 2001     

Enhanced melt strength and stretching of linear low-density polyethylene extruded under strong slip conditions

The influence of extrusion under strong slip conditions on the extensional properties of linear low-density polyethylene was studied in this work. The material was extruded at two different temperatures under strong slip and no slip conditions, and was subsequently subjected to uniaxial elongational flow by means of a Rheotens device. Strong slip was evident through the elimination of sharkskin distortions and the stick-slip instability, as well as by the electrification of the extrudates. The extrudate swell was smaller in the presence of slip when comparing with no slip conditions at constant apparent shear rate, but it was found to be a unique function of the shear stress if comparison was performed at constant stress. The draw ratio and melt strength of the filaments obtained under slip conditions were larger compared to those without slip. In addition, draw resonance was postponed to higher draw ratios during the extrusion with strong slip at constant apparent shear rate. It is suggested that slip of the polymer at the die wall decreases the shear stress in the bulk, and therefore, restricts the disentanglement and orientation of macromolecules during flow, which subsequently produces the increase in draw ratio and melt strength during stretching.     

Two-dimensional planar flow of a viscoelastic plastic medium

The present study is concerned with finite element simulation of the planar entry flow of a viscoelastic plastic medium exhibiting yield stress. The numerical scheme is based on the Galerkin formulation. Flow experiments are carried out on a carbon black filled rubber compound. Steady-state pressure drops are measured on two sets of contraction or expansion dies having different lengths and a constant contraction or expansion ratio of 4:1 with entrance angles of 90, 45 and 15 degrees. The predicted and measured pressure drops are compared. The predicted results indicate that expansion flow has always a higher pressure drop than contraction flow. This prediction is in agreement with experimental data only at low flow rates, but not at high flow rates. The latter disagreement is possibly an indication that the assumption of fully-developed flow in the upstream and downstream regions is not realistic at high flow rates, even for the large length-to-thickness ratio channels employed. The evolution of the velocity, shear stress, and normal stress fields in the contraction or expansion flow and the location of pseudo-yield surfaces are also calculated.     

Instabilities in viscoelastic flows

Viscoelastic instabilities are of practical importance, and are the subject of growing interest. Reviewed here are the fresh developments as well as earlier work in this area, organized into the following categories: instabilities in Taylor-Couette flows, instabilities in cone-and-plate and plate-and-plate flows, instabilities in parallel shear flows, extrudate distortions and fracture, instabilities in shear flows with interfaces, instabilities in extensional flows, instabilities in multidimensional flows, and thermohydrodynamic instabilities. Emphasized in the review are comparisons between theory and experiment and suggested directions for future work.     

A numerical stabilization framework for viscoelastic fluid flow using the finite volume method on general unstructured meshes

A robust finite volume method for viscoelastic flow analysis on general unstructured meshes is developed. It is built upon a general‐purpose stabilization framework for high Weissenberg number flows. The numerical framework provides full combinatorial flexibility between different kinds of rheological models on the one hand, and effective stabilization methods on the other hand. A special emphasis is put on the velocity‐stress‐coupling on colocated computational grids. Using special face interpolation techniques, a semi‐implicit stress interpolation correction is proposed to correct the cell‐face interpolation of the stress in the divergence operator of the momentum balance. Investigating the entry‐flow problem of the 4:1 contraction benchmark, we demonstrate that the numerical methods are robust over a wide range of Weissenberg numbers and significantly alleviate the high Weissenberg number problem. The accuracy of the results is evaluated in a detailed mesh convergence study.     

The effects of chain conformation in the microfluidic entry flow of polymer–surfactant systems

An associative polymer–surfactant system has been used to observe the effects of chain conformation in the entry flow through a microfabricated planar 16:1:16 contraction–expansion geometry. The well-studied system of the flexible polymer poly(ethylene oxide) (PEO) and anionic surfactant sodium dodecyl sulfate (SDS) was used. Dilute polymer solutions with increasing SDS concentration were characterized in steady and dynamic shear, as well as capillary breakup extensional rheology. Based on this characterization, the primary quantitative difference is an increase in zero-shear viscosity as a result of the PEO chain expansion brought on by association of SDS surfactant micelles. However, these quantitatively similar solutions were observed to exhibit much more qualitatively different flow patterns via fluorescent streak imaging in the entry flow. In contrast to previous work on PEO solutions, the PEO–SDS systems were observed to transition to a steady viscoelastic flow regime characterized by stable lip vortices at much lower elasticity and Weissenberg numbers. The resulting insight gained regarding the utility of microfluidic flows in elucidating effects of subtle conformational changes further illustrates the potential for using microfabricated devices as rheometric tools for measuring the properties of dilute and weakly viscoelastic fluids.     

The stability of two-dimensional linear flows of an Oldroyd-type fluid

A linear stability analysis is made for an Oldroyd-type fluid undergoing steady two-dimensional flows in which the velocity field is a linear function of position throughout an unbounded region. This class of basic flows is characterized by a parameter λ which ranges from λ = 0 for simple shear flow to λ = 1 for pure extensional flow. The time derivatives in the constitutive equation can be varied continuously from co-rotational to co-deformational as a parameter β varies from 0 to 1. The linearized disturbance equations are analyzed to determine the asymptotic behavior as time t → ∞ of a spatially periodic initial disturbance. It is found that unbounded flows in the range 0 < λ ? 1 are unconditionally unstable with respect to periodic initial disturbances which have lines of constant phase parallel to the inlet streamline in the plane of the basic flow. When the Weissenberg number is sufficiently small, only disturbances with sufficiently small wavenumber α₃ in the direction normal to the basic flow plane are unstable. However, for certain values of β, critical Weissenberg numbers are found above which flows are unstable for all values of the wavenumber α₃.     

Wall slip of mayonnaises in viscometers

The shear flow of mayonnaise is generally characterized by an apparent yield stress, shear thinning in steady flow, stress overshoots upon inception of flow and other time-dependent effects. These observations are usually understood to be the result of structural rearrangement within the material. Additionally and separately, the possibility that emulsions may exhibit apparent wall slip on a microscopic scale at a solid-liquid boundary has been reported by some researchers. Thus, observed rheological behavior is likely to be the result of the interplay between these two phenomena. In the present work, it is demonstrated that when measurements are sought to be made on mayonnaise using rotational viscometers visible wall slip occurs, rendering such instruments ineffective for the purpose of making viscosity measurements even at shear rates as low as 10^–3s^–1. The factors that influence the onset and extent of slip are investigated with the help of parallel plate viscometers, and it is concluded that the observed “yielding” of mayonnaise is actually an artifact of the onset of macroscopic slip. Slip effects are also found in capillary flow but are ameliorated with increasing shear rate. To circumvent these problems, it is proposed that extensional viscometry be employed for determining the flow behavior of mayonnaises. Received: 18 August 1997 Accepted: 1 April 1998     

An approximate analysis for contraction and converging flows

An approximate analysis is presented for the flow of fluids through planar and axisymmetric contractions. Energy principles are employed to relate the entry pressure drop to flow rate and fundamental rheometric properties. One of the aims of the analysis is to investigate the influence of extensional viscosity on such flows, particularly with regard to the occurrence and enhancement of vortex motion in the entry corners.For the sake of mathematical simplicity, independent power-law models are used to represent the shear and extensional viscosity functions. The analysis indicates that, once significant vortex motion is present, enhancement occurs whenever the Trouton ratio is an increasing function of shearrate (or stretch-rate). It is readily seen how the occurrence of vortices serves as a stress relief mechanism. Indeed, for highly stretch-thickening materials, the entry pressure drop is seen to be dominated by shear properties.The power-law parameters of the extensional viscosity function may be obtained in a straight-forward way from entry pressure drop versus flow rate data.Finally, the extension and application of the analysis to other similar flows, such as through converging nozzles, is briefly discussed.     

Simultaneous determination of shear and extensional viscosities and wall slip by on-line rheometry with parameter fitting: an application to EPDM rubber

Shear and extensional viscosities and wall slip are determined simultaneously under extrusion processing conditions using an on-line rheometer. Because it is not possible to independently control flow rate and temperature, classical methods for interpretation of capillary data cannot be used with on-line rheometry. This limitation is overcome using computational optimization to fit parameters in a flow model. This consists of three parts, representing shear viscosity, extensional viscosity, and wall slip. Three-parameter, power law forms, based on local instantaneous deformation rates and including temperature dependence, are used for each, and analytic solutions applied for entry flow and flow in the capillary. For entry flow, the Cogswell–Binding approach is used, and for developed flow in the capillary a solution incorporating wall slip is derived. The rheometer, with interchangeable capillaries, is mounted in place of the die on a rubber profile extrusion line. Pressure drops and temperatures for extrusion of an EPDM rubber through 2 mm diameter capillaries of length 0, 2, 3, 4, and 5 mm are logged and flow rates determined for a range of extruder speeds (5 to 20 rpm). Pressures ranged from 60 to 75 bar and temperatures from 86 to 116 °C. Mean flow velocity in the capillaries was between 5 × 10⁻³ and 5 × 10⁻¹ m s⁻¹. The nine material parameters are optimized for best fit of the analytic pressure drops to experimental data, using about 100 data points, with the Levenberg–Marquardt method. It is concluded that flow is dominated by extension and wall slip. Shear flow appears to play little part. The slip model indicates that slip velocity increases much more rapidly than the wall shear stress (in the range 0.5–1 MPa) and decreases with temperature for a given stress level. Results for the (uniaxial) extensional viscosity represent an engineering approximation to this complex phenomenon at the high strains (approximately 200) and high extension rates (up to 800 s⁻¹) applying in the extrusion. Results indicate a slight extension hardening and a decrease with temperature. Results are put into the context of the available studies in the literature, which, particularly with regard to wall-slip and extensional flow, consider conditions far removed from those applying in industrial extrusion. The present methods provide a powerful means for flow characterization under processing conditions, providing data suitable for use in computer simulations of extrusion and optimization of die design.     

Surface tension driven jet break up of strain-hardening polymer solutions

Experimental studies attempting to ascertain the influence of viscoelasticity on the atomization of polymer solution are often hindered by the inability to decouple the effect of shear thinning from the effect of extensional hardening. Here, the influence of viscoelasticity on the jet break up of a series of non-shear-thinning viscoelastic fluids is quantified. Previous characterization using an opposed-nozzle rheometer identified the critical extensional rates for strain hardening of these model fluids. The strain hardening fluids exhibit a beads-on-string structure with reduction or elimination of satellite drops. Capillary instabilities grow on the filaments connecting the spheres and eventually break the filaments up into a string of very small drops about one order of magnitude smaller than the satellite drops formed by a Newtonian fluid with the same shear viscosity, surface tension, and density. These results confirm that strain hardening is the key rheological property in jet break up and that the critical extensional rate of a fluid is pertinent in determining the final characteristics of break up. Results suggest that the opposed-nozzle rheometer does probe extensional behavior in the range of extensional rates that are relevant to jet break up, providing a tool to roughly predict jet break up.     

Flow of wormlike micelle solutions through a periodic array of cylinders

Solutions of self-assembled wormlike micelles are used with ever increasing frequency in a multitude of consumer products ranging from cosmetic to industrial applications. Owing to the wide range of applications, flows of interest are often complex in nature; exhibiting both extensional and shear regions that can make modeling and prediction both challenging and valuable. Adding to the complexity, the micellar dynamics are continually changing, resulting in a number of interesting phenomena, such as shear banding and extensional flow instabilities. In this paper, we present the results of our investigation into the flow fields generated by a controllable and idealized porous media: a periodic array of cylinders. Our test channel geometry consists of six equally spaced cylinders, arranged perpendicular to the flow. By systematically varying the Deborah number, the flow kinematics, stability and pressure drop were measured. A combination of particle image velocimetry in conjunction with flush mount pressure transducers were used to characterize the flow, while flow induced birefringence measurements were used to determine micelle deformation and alignment. The pressure drop was found to decrease initially due to the shear thinning of the test fluid, and then exhibit a dramatic upturn as other elastic effects begin to dominate. We present evidence of the onset of an elastic instability in one of the test fluids above a critical Deborah number manifest in fluctuating transient pressure drop measurements and asymmetric streamlines. We argue that this disparity in the two test fluids can be attributed to the measurable differences in their extensional rheology.