Lubricated optical rheometer for the study of two-dimensional complex flows of polymer melts

We describe a novel optical cross-slot channel rheometer generating two-dimensional and isothermal complex flows of polymer melts. This is made possible by lubricating the channel front and back viewing windows. Flow-induced birefringence and particle tracking velocimetry are reviewed and used to investigate the cross-slot flow of a low density polyethylene melt involving mixed shear and planar extensional deformations. This new device solves the issue of end effects in flow birefringence experiments where no variations of the optical properties along the light path are expected. It greatly facilitates the interpretation of stress field data by providing reliable measurements of the polymer melt extinction angle χ$\chi$ and retardation δ$\delta$, with a spatial resolution of one tenth of a millimeter. At the same time, it offers an enhanced temperature control and an increased optical accuracy due to an improved laser beam shaping. The capabilities and performances of this unique type of lubricated rheometer are discussed in detail and compared with previous approaches.     

Lubricated cross-slot flow of a low density polyethylene melt

Flow-induced birefringence and particle tracking velocimetry are used to investigate the lubricated flow of a low density polyethylene melt in a cross-slot geometry. The numerical predictions of the extended Pom-Pom (XPP) model in its original and modified (mXPP) version as well as those of the Giesekus model are analyzed along selected streamlines in two-dimensional (2D) complex flows involving a mixture of shear and planar extensional deformations at two Weissenberg numbers of Wi=21 and 29. Oil film light reflections perturbing the particle tracking velocimetry data analysis together with multiple orders of retardation occurring within the laser beam close to the stagnation point prevent a conclusive discrimination between the mentioned models. Although the agreement with the experimental data is mostly qualitative, the Pom-Pom model does not overestimate the data along the cross-slot symmetry lines contrary to what was observed in other cross-slot experiments without lubrication. This is a clear indicator that end effects play a central role in unlubricated cross-slot geometries having a large aspect ratio.     

Study of two-phase flows in reduced gravity using ground based experiments

Experimental studies have been carried out to support the development of a framework of the two-fluid model along with an interfacial area transport equation applicable to reduced gravity two-phase flows. The experimental study simulates the reduced gravity condition in ground based facilities by using two immiscible liquids of similar density namely, water as the continuous phase and Therminol 59^® as the dispersed phase. We have acquired a total of eleven data sets in the bubbly flow and bubbly to slug flow transition regimes. These flow conditions have area-averaged void (volume) fractions ranging from 3 to 30% and channel Reynolds number for the continuous phase between 2,900 and 8,800. Flow visualization has been performed and a flow regime map developed which is compared with relevant bubbly to slug flow regime transition criteria. The comparison shows that the transition boundary is well predicted by the criterion based on critical void fraction. The value of the critical void fraction at transition was experimentally determined to be approximately 25%. In addition, important two-phase flow local parameters, including the void fraction, interfacial area concentration, droplet number frequency and droplet velocity, have been acquired at two axial locations using state-of-the-art multi-sensor conductivity probe. The radial profiles and axial development of the two-phase flow parameters show that the coalescence mechanism is enhanced by either increasing the continuous or dispersed phase Reynolds number. Evidence of turbulence induced particle interaction mechanism is highlighted. The data presented in this paper clearly show the marked differences in terms of bubble (droplet) size, phase distribution and phase interaction in two-phase flow between normal and reduced gravity conditions.     

A model long-discontinuous-fiber filled thermoplastic melt in extensional flow

The shear cell model works for dilute fiber filled systems in extensional flow. This research investigates the suitability of the idea for highly aligned fibers in a concentrated suspension. A model fiber-filled polymer system made from nylon fibers in low-density polyethylene provided a means of controlling the material parameters. Two systems, with fiber aspect ratios of 20 and 100, containing 50% 0.5 mm fibers by volume are investigated. The thickness of the polymer layer, i.e. with fibers this size, allows bulk viscosity data to be compared with the data from the filled fluid. A weaving process created the discontinuous fiber/polyethylene preforms with high alignment of the fibers and with control of the fiber to fiber overlap. Testing the polyethylene in simple shear and extending the nylon/polyethylene provided the data needed to check the micro mechanics. A cone and plate rheometer and a capillary instrument produced the viscosity/strain rate data that characterized the specific polyethylene used in the composite. A furnace inset placed in an Instron hydraulic test machine allowed extension of the filled system at strain rates from 0.002 to 0.4 s⁻¹. The shear experiments show that the low-density polyethylene is a simple shear-thinning melt that provides a good model fluid. The extension of the filled systems shows an increase of the apparent extensional viscosity from that of neat polyethylene. Apparent viscosity rises two to three orders of magnitude for the systems investigated. The micromechanics allowed the conversion of the extensional data from the two filled systems to the shear viscosity of the polymer surrounding the fibers. The calculated polyethylene viscosity compares well with the data from the standard rheometers. The shear cell approach may be applied to highly aligned, high fiber-volume-fraction suspensions when the viscosity of the polymer is known at the scale of the film surrounding each fiber.     

Brownian dynamics simulations of star-branched polymers in dilute solutions in extensional flow

Using Brownian dynamics (BD) simulations of FENE bead-spring models, the dynamics of star-branched polymers in dilute solutions under extensional flow have been investigated. Studies on star polymers in transient extensional flow reveal that the initial transient stress response at low strains is governed by both the number of arms and the shortest arm. On the other hand, the steady-state behavior of star polymers in elongational flow is limited by the maximum effective “contour” length of the molecules. The distribution of arm extension and birefringence of the star-branched molecule are broader and the mean is shifted to lower values, when compared to equivalent linear systems. As a result, the degree of arm extension at steady-state decreases as the number of arms in the star increases. Both an analysis of individual ensembles in Brownian dynamics simulations and a study of a simple force balance indicate that the constraint imposed on the star arms by the central branch point and contributions from “asymmetric” arm arrangements give rise to overall less extended and oriented star-branched molecules with broader arm extension and birefringence distributions. The results obtained from stress-conformation hysteresis simulation indicate that less-stretched arms exhibit more retarded relaxation, as the number of arms increases in star-branched molecules. The effect of excluded volume (EV) interactions, incorporated through the Lennard–Jones potential, on the dynamics of star polymers in extensional flow appears unimportant.     

Modeling the evolution of droplet size distribution in two-phase flows

A theoretical model is developed in the present study to simulate droplet motion and the evolution of droplet size distribution (DSD) in two-phase air/dispersed water spray flows. The model takes into account several processes which influence DSD and droplet trajectory: droplet collision and coalescence, evaporation and cooling, gravitational settling, and turbulent dispersion of dispersed phase. The DSDs determined by the model at different locations in a two-phase flow are evaluated by comparing them to experimental observations obtained in an icing wind tunnel. The satisfactory coincidence between simulation and experimental results proves that the model is reliable when modeling two-phase flows under icing conditions. The model is applied for two particular examples in which the modification of DSD is calculated in two-phase flows under conditions describing in-cloud icing and freezing drizzle.     

Numerical simulation studies of the planar entry flow of polymer melts

This paper is concerned with the numerical simulation of planar entry flow using a penalty finite element method and the comparison of predictions with flow visualization and birefringence data for two polymer melts. The Phan-Thien Tanner (PTT) model was fit to the steady state shear and extensional viscosity data and the transient extensional viscosity data of both polystyrene and low-density polyethylene (LDPE) melts to obtain the parameters λ, ξ, and ϵ in this model. Agreement was found between the flow visualization and birefringence data and the predictions of streamlines and stress. With some modification of the constitutive equation, the vortex growth and intensity observed for LDPE could be predicted by the use of the PTT model and the material parameters fit to the rheological properties. Likewise, the flow behavior of polystyrene, in which only small vortices with no growth were observed, was also predicted. Furthermore, it was found that the size and intensity of the vortex could be affected by the parameter ϵ in the PTT model which controls the predictions of the extensional viscosity. Based on these results it seems that accurate simulation of entry flow behavior requires the use of a constitutive equation which is capable of giving realistic preciction's of a fluid's extentional flow properties.     

Determination of the elongational viscosity of polymer melts by melt spinning experiments. A comparison with different experimental techniques

In this work, melt spinning experiments were tentatively used for the determination of the elongational viscosity of polymer melts at different levels of tensile strain and strain rate. The materials examined were two high-density polyethylene grades for blow moulding with similar number-average molecular mass but different polydispersity index. The data from melt spinning tests were compared with transient extensional viscosity data obtained by uniform isothermal tensile tests, performed by means of an extensional rheometer, as well as with those produced by converging flow tests (Cogswell model). The results showed that for high strain and strain rate levels, the melt spinning experiments provide elongational viscosity data quite close to the transient extensional viscosity values obtained from the tensile tests.     

On the Kinetics of Polymer Crystallization in Opposite-Nozzle Flow

The present work was encouraged by the successes obtained previously in this laboratory with short-term shearing experiments on slightly undercooled melts of i-PP: post-shearing lamellar growth on (inconspicuous) thread-like precursors. For the present purpose (evaluation of the influence of extensional flow) the pioneering work by Mackley and Keller is taken as the point of departure. Our own machine of the same type has been adapted for creep experiments (adjustment to steady flow in fractions of the time needed in the original machine). The range of extension rates, where a transition takes place from a mere multiplication of the number of nuclei to the induction of highly oriented structures, appears to be quite narrow in undercooled i-PP melts. In the range of high extension rates (≅50 s⁻¹ ) the critical time for the formation of an oriented structure could not be measured because of its shortness (less than 0.2 s). It turns out that the flow pattern in the opposite-nozzle machine is far from ideal. A proposal had to be made for a redesign. In spite of the preliminary nature of some of our results, several interesting insights should not be “bottled up”. First of all, there is the usefulness of creep flow (because of its fast transition into steady state, after an almost instantaneous compliance). Secondly, there is the quite unexpected ineffectiveness of lower stretching rates for the formation of oriented structures. Thirdly, there is the overwhelming influence of a change of the geometry: the provisional introduction of trumpet-shaped (nearly hyperbolic) entrance regions to the nozzles caused a remarkable broadening of the birefringent zone, which was previously observed as a very thin “string” connecting the nozzles. Finally, the almost certain usefulness of the revised machine for other (sometimes purely rheological) purposes, e.g., for steady-state flow birefringence measurements in extensional flow should be mentioned. Received: 22 June 1999 Accepted: 28 September 2000     

Structure and rheology of wormlike micelles

In a semi-dilute aqueous solution under certain conditions, surfactant molecules will self assemble to form wormlike micelles. The micelles are dynamic in structure since they can break and reform, providing an additional mode of relaxation. The viscoelastic properties of the wormlike micelles can be predicted using simple theological models. For many surfactant solutions the mechanical data can be related to the optical data by the stress-optical rule. From the viscoelastic data it is possible to estimate the breaking time of the micelle. The techniques of birefringence and small angle light scattering are used to study the microstructure of a surfactant solution under simple shear and extensional flow. The sample under investigation is a solution of cetyltrimethylammonium bromide and sodium salicylate in water, with a salt to surfactant ratio of 7.7. Below a critical shear rate, the birefringence increases linearly with shear rate and the stress-optical rule is valid. The SALS patterns reveal distinctive butterfly patterns indicating that scattering is a result of concentration fluctuations that moderately couple to the flow. However, above a critical shear rate the birefringence plateaus and the stress-optical rule is no longer valid. SALS patterns show both a bright streak and a butterfly pattern. The bright streak is caused by elongated structures aligned in the direction of the flow. The oriented structures occur when the characteristic time of flow is faster than the breaking time of the micelles.Dedicated to Prof. Dr. J. Meissner on the occasion of his retirement from the chair of Polymer Physics at the Eidgenössische Technische Hochschule (ETH) Zürich, Switzerland     

Birefringence and stress growth in uniaxial extension of polymer solutions

Simultaneous measurements of extensional stresses and birefringence are rare, especially for polymer solutions. This paper reports such measurements using the filament stretch rheometer and a phase modulated birefringence system. Both the extensional viscosity and the birefringence increase monotonically with strain and reach a plateau. Estimates of this saturation value for birefringence, using Peterlin’s formula for birefringence of a fully extended polymer chain are in agreement with the experimental results. However, estimates of the saturation value of the extensional viscosity using Batchelor’s formula for suspensions of elongated fibres are much higher than observed. Reasons for the inability of the flow field to fully unravel the polymer chain are examined using published Brownian dynamics simulations. It is tentatively concluded that the polymer chain forms a folded structure. Such folded chains can exhibit saturation in birefringence even though the stress is less than that expected for a fully extended molecule.Simultaneous measurements of stress and birefringence during relaxation indicate that the birefringence decays much more slowly than the stress. The stress-birefringence data show a pronounced hysteresis as predicted by bead-rod models. The failure of the stress optic coefficient in strong flows is noted.Experiments were also performed wherein the strain was increased linearly with time, then held constant for a short period before being increased again. The response of the stress and birefringence in such experiments is dramatically different and can be traced to the different configurations obtained during stretching and relaxation. The results cast doubt on the appropriateness of pre-averaging the non-linear terms in constitutive equations.     

Stretching polymer chains

This paper is based on a presentation given at the de Gennes discussion meeting held at Chamonix in February 2009. The paper gives a personal review of the way developments relating to the stretching of polymer chains has taken place over the last 40 years. de Gennes was very influential in relation to chain dynamics concepts at the University of Bristol, where many pioneering concepts relating to chain stretching were developed by the late Sir Charles Frank and Andrew Keller. The paper reviews basic concepts on extensional rheology, droplet deformation, chain extension from extensional flow and the achievement of high chain extension for high-modulus polyethylene. The paper also reviews recent developments concerning the influence of chain stretching on polymer melt processing.     

A model for droplet entrainment in heated annular flow

The ability to accurately predict droplet entrainment in annular two-phase flow is required to effectively calculate the interfacial mass, momentum, and energy transfer, which characterizes nuclear reactor safety, system design, analysis, and performance. Most annular flow entrainment models in the open literature are formulated in terms of dimensionless groups, which do not directly account for interfacial instabilities. However, many researchers agree that there is a clear presence of interfacial instability phenomena having a direct impact on droplet entrainment. The present study proposes a model for droplet entrainment, based on the underlying physics of droplet entrainment from upward co-current annular film flow that is characteristic to light water reactor safety analysis. The model is developed based on a force balance and stability analysis that can be implemented into a transient three-field (continuous liquid, droplet, and vapor) two-phase heat transfer and fluid flow systems analysis computer code.     

Simulation of incompressible multiphase flows with complex geometry using etching multiblock method

The incompressible two-phase flows are simulated using combination of an etching multiblock method and a diffuse interface (DI) model, particularly in the complex domain that can be decomposed into multiple rectangular subdomains. The etching multiblock method allows natural communications between the connected subdomains and the efficient parallel computation. The DI model can consider two-phase flows with a large density ratio, and simulate the flows with the moving contact line (MCL) when a geometric formulation of the MCL model is included. Therefore, combination of the etching method and the DI model has potential to deal with a variety of two-phase flows in industrial applications. The performance is examined through a series of numerical experiments. The convergence of the etching method is firstly tested by simulating single-phase flows past a square cylinder, and the method for the multiphase flow simulation is validated by investing drops dripping from a pore. The numerical results are compared with either those from other researchers or experimental data. Good agreement is achieved. The method is also used to investigate the impact of a droplet on a grooved substrate and droplet generation in flow focusing devices.     

Elongational flow and rheology of monodisperse polymers in solution

We describe the utilization of idealized stagnation point extensional flows, produced by opposed jets, for birefringence visualization of induced molecular strain and flow resistance measurements. We identify rheological changes associated with the coil---stretch transition which occurs beyond a critical strain-rate in elongational flow-fields. In dilute solutions of monodisperse atactic polystyrene, increases in extensional viscosity are observed as isolated molecules become stretched. The largest increases in extensional viscosity, however, are found only beyond a critical concentration and strain rate, and are associated with the stretching of transient networks of interacting molecules. These results parallel similar effects seen in porous media flow and capillary entrance experiments. We determine the molecular weight dependence of the critical concentration which scales as M^−0.55 in agreement with pairwise interaction of coils, but is much lower than conventional values of the critical polymer concentration, c^*. We believed that polydispersity may play an important role in the development of such transient networks, and in controlling the degradation behaviour during flow.     

Some features of spray breakup in effervescent atomizers

The near orifice spray breakup at low GLR (gas to liquid ratio by mass) values in an effervescent atomizer is studied experimentally using water as a simulant and air as atomizing gas. From the visualizations, the near orifice spray structures are classified into three modes: discrete bubble explosions, continuous bubble explosions and annular conical spray. The breakup of the spray is quantified in terms of the mean bubble bursting distance from the orifice. The parametric study indicates that the mean bubble bursting distance mainly depends on airflow rate, jet diameter and mixture velocity. It is also observed that the jet diameter has a dominant effect on the bubble bursting distance when compared to mixture velocity at a given airflow rate. The mean bubble bursting distance is shown to be governed by a nondimensional two-phase flow number consisting of all the aforementioned parameters. The location of bubble bursting is found to be highly unsteady spatially, which is influenced by flow dynamics inside the injector. It is proposed that this unsteadiness in jet breakup length is a consequence of varying degree of bubble expansion caused due to the intermittent occurrence of single phase and two-phase flow inside the orifice.     

A filtered mass density function approach for modeling separated two-phase flows for LES I: Mathematical formulation

The overall objective of this study is to develop a full velocity-scalar filtered mass density function (FMDF) formulation for large eddy simulation (LES) of a separated two-phase flow. Required in the development of the two-phase FMDF transport equation are the local instantaneous equations of motion for a two-phase flow previously derived by Kataoka. In Kataoka’s development, phase interaction terms are cast in terms of a Dirac delta distribution on the phase interface. For this reason, it is difficult to close these coupling terms in the instantaneous formulation and this difficulty is propagated into the phase-coupling terms in the FMDF transport equation. To address this point a new derivation of the local instantaneous equations for a separated two-phase flow is given. The equations are shown to be consistent with the formulation given by Kataoka, and in the development, a direct link between the conditionally surface-filtered coupling terms, arising in the FMDF formulation, and LES phase-coupling terms is established. Clarification of conditions under which conditionally filtered interphase conversion terms in the marginal FMDF transport equations may be disregarded in a separated continuum-dispersed phase flow is discussed. Modeling approaches and solutions procedures to solve the two-phase FMDF transport equation via Monte-Carlo methods are outlined.