Excerpt from the Proceedings of the COMSOL Users Conference 2006 Paris

Numerical Simulations of Thixotropic Fluids.

P. Dantan1*, M. Faye2 1 Universit Paris7 Denis Diderot, 2Universit Paris11
*Laboratoire MSC, Case 7056, 2 Place Jussieu, 75251 Paris cedex05, France email:philippe.dantan@paris7.jussieu.fr Abstract: Under attractive interactions between particles and hydrodynamic stress, complex suspensions have a changing internal structure. We introduce a kinetic equation coupled with Navier-Stokes equation in COMSOL Multiphysics in order to simulate internal structure changes of a flowing complex fluid. Two physical applications are considered, one in the biomedical field (starting blood flow in a stenosis) and an other which simulates a laboratory rheometric setup for experimental validation of the model. Results show a good agreement with experimental well-known hysteresis loops. Hence, biomedical applications in diagnosis of some blood pathologies are in view. Keywords: complex fluid, thixotropy, kinetic equation, aggregation-disaggregation processes. between individual particles compete with hydrodynamic stresses to modify the structural units (size, number fraction), both their arrangements and their internal structure (compactness). Some structural units are in formation with a characteristic time TA (aggregation); some others are rupturing with a characteristic time TD (disaggregation) leading to a viscosity which depends not only on shear rate but also on time. This rheological behavior is called thixotropy. Therefore, the simplest way for modelling thixotropy of complex fluids is based on: i) a scalar structural variable S characterizing the structure, ii) a kinetic equation which governs S describing the rupturing and restoring of the structure induced by the flow, iii) the dependence of kinetic parameters occurring in the kinetic equation with shear rate or shear stress, iiii) the relationship between the viscosity and the structural variable.

1. Introduction Thixotropy of Complex Fluids

Many complex fluids (slurries, foods, paints, blood, cosmetics) have a non-newtonian rheological behavior: their viscosity is not constant but depends on applied shear rate or shear stress. Such fluids can be described as concentrated suspensions of structural units such as individual particles, clusters, aggregates, clusters of aggregates, up to an eventual network filling all the fluid volume. These structural units have a size which depends on the applied shear due to hydrodynamic stress under which the fluid is flowing. In a quasi-steady flow, these structural units can be considered as uniform in size with a mean radius depending only on shear. Therefore, the complex fluid can be described with a viscosity which depends only on the shear rate. It is very easy to modell such a steady rheology in COMSOL Multiphysics by introducing one of the several phenomenological laws obtained by fitting rheometric measurements. But in most of complex fluids, shear-induced changes are observed in their internal structure, especially in unsteady flows. Interactions

2. Theoretical model of thixotropy

2.1 Structural variable Evolution of structural units has to be described by a structural scalar dimensionless variable S defined as the number fraction of aggregated particles contained in the structural units. S varies from the value 0 when the structure is completely destroyed under very high shear, up to 1 when the structure is complete after a long time at rest or under very low shear. 2.2 Kinetic equation for S We assumed that kinetic processes involved in formation and reduction of structural units are relaxation processes with mean relaxation times TA and TD respectively. Under these assumptions, the number fraction of aggregated particles S is governed by the kinetic equation (Cf. Quemada [1]):

Excerpt from the Proceedings of the COMSOL Users Conference 2006 Paris

1 1 dS = (1 S ) S dt TA TD
in which
dS dt

(1)

power law (2) and equation (3) (the viscosity is eta). time

means

substantial

derivative. 2.3 Kinetic parameters The equilibrium structure reached by the fluid under steady conditions depends on shear rate only. Moreover, the steady state solution of equation (1) depends obviously on TA , so we
TD
Fig.1 Shear rate and characteristic times expressions

can deduce that TA

TD

depends on shear rate,

3.2 The kinetic equation In the model navigator we add the equation (1) by using the PDE coefficient form of the PDE mode with the dependent variable S. The coefficients are defined in Subdomain Settings (Fig.2)

therefore for the simplest modelling it will be assumed that:

TA (TC . ) q TD

where TC is a characteristic time and shear rate. For instance, for blood:

the

TA = TA0 ; TD = TD 0 /(TC . ) q (2)

2.4 Relation viscosity-structural variable From equations generalizing the well-known Einstein relation between viscosity and number fraction in dilute media, it can be shown that the structural variable is related to viscosity by the equation:

= 1 (1 ).S (3) 0 Where , 0 are respectively the limiting

steady states viscosities at very high shear rate ( ) and very low shear rate ( 0 ).

Fig.2: kinetic equation coefficients

Boundary conditions are of homogeneous Neumann kind.

4. Physical applications a
Several numerical simulations of thixotropic flowing fluids have been performed with different geometries, flow conditions and rheological constants. We present here two physically relevant cases. The first one is a starting flow of blood in a converging-diverging vessel (a stenosis). The second case is a Couette flow (flow between two coaxial cylinders) of a food gelling agent for which experimental measurements are available in our laboratory.

3. Numerical implementation thixotropic model in COMSOL

3.1 Predefined mode Navier-Stokes

of

application

In Subdomain Expressions (Fig.1) we introduce the shear rate as the second invariant of the velocity gradient tensor (gamma), the

Excerpt from the Proceedings of the COMSOL Users Conference 2006 Paris

4.1 Starting blood flow in a stenosis 4.1.1 The model The 2D geometry of the channel (width: 1cm., length: 15cm.) reveals a 40% narrowing zone (Fig.4) which generates very high shear in the smaller width and very low shear downstream. The fluid is initially at rest from long time so it can be assumed to be almost complete (S=1). This can be obtained in in-vivo experiments by clamping the vessel. The input velocity on the axis is a quasi-square signal (1 cm/s from t=1s up to t=8s and 0 cm/s after) as shown on Fig.3

Fig.3: Input velocity signal on the centerline

Fig.4: Structural variable field, velocity vectors and streamlines at t=1s, 1.5s, 8s, 12s.

The kinetic constants are: TA0 =1s for aggregation and TD0 =2s for disaggregation. 4.1.2 The results On figure 4, the fluid domain is colored with the structural variable S (S=1=red; S=0=blue), velocity vectors and streamlines are also plotted at different times. At t=1s, the rupturing of structural units begins only in the boundary layer, especially in the narrower part of the channel due to very high shear stress. At t=1.5s, (t < TD0) a larger layer of unstructured fluid spreads along the wall, but the core of the flow in which shear rate is very low remains still highly structured. At t=8s, (t >> TD0) just before the flow stop, the internal fluid structure is broken almost everywhere and is at equilibrium. At t=12s, the fluid has recovered an almost complete internal structure induced by the null flow rate since a time longer than TA0.

The dynamics of the internal fluid structuration is visible by plotting the time evolution of the structural variable. On figures 5a and 5b, S is plotted as a function of time at y=3mm (red line) and y=6mm (blue line). On figure 5a the point plot is just near the stenosis (x=0.041m) whereas, on figure 5b, it is far downstream (x=0.1m).

Fig.5a: S(t) at y=3mm (red), y=6mm (blue); x=0.041m

Excerpt from the Proceedings of the COMSOL Users Conference 2006 Paris

Fig.5b: S(t) at y=3mm (red), y=6mm (blue); x=0.1m

By comparing blue and red lines, it can be observed that the fluid is more structured far from the wall at every time. Otherwise, due to the geometrical singularity of the stenosis, the fluid looses quickly and deeply its internal structured state (S#0.66 near the center, S#0.4 near the wall), whereas, far downstream in the quasi-Poiseuille flow, it remains strongly structured (S#0.93 near the center, S>0.7 near the wall). 4.1.3 Application: comparison of two kinetics A second fluid has been tested with other kinetic constants: TA0 =2s and TD0 =1s, all the other parameters being the same. The velocity profiles u(y) are shown on figures 6a (fluid 1) and 6b (fluid 2) during the deceleration of the flow rate (t=7.8s, 8s, 8.2s) at a site very close downstream the stenosis (x=0.041m)

Fig 6b: velocity profiles at t=7.8s, 8s, 8.2s near the stenosis; Fluid 2: Aggregation time TA0 =2s, breaking up time TD0 =1s.

These plots reveal so different patterns that it is possible to discriminate between distinct kinetics by analyzing velocity profiles near a geometrical singularity. Thus, velocity profiles of in-vivo blood flows in arteries can be obtained easily by a non invasive way with ultrasonic Doppler devices. By comparisons between in-vivo measurements and several numerical simulations as those described here, it might be possible to characterize the kinetic behavior of a given blood. It should be of a great interest because some blood pathologies like diabetes lead to abnormal kinetic constants. 4.2 Couette Flow of carrageenan 4.2.1 The kinetic parameters Iota carrageenan is a typical food gelling agent which exhibits a thixotropic inelastic behavior. From rheometric measurements, kinetic parameters have been found to follow power laws (Cf. Baravian, Quemada [2]) such as:

TA = TA

TA TA0

1 + (Tc . )

; TD =

TA

(Tc . )

(4)
p

4.2.2 The geometry and boundary conditions The coaxial cylinders of the rheometer used in [2] can be reduced to the 2D-space bounded by two circles with inner radius 13.83 mm and outer radius 15 mm (Fig.8). Only a sector is used to save some mesh nodes and computer memory. This leads to add periodic conditions at the

Fig 6a: velocity profiles at t=7.8s, 8s, 8.2s near the stenosis; Fluid 1: Aggregation time TA0 =1s, breaking up time TD0 =2s.

Excerpt from the Proceedings of the COMSOL Users Conference 2006 Paris

straight ending edges. The inner cylinder being at rest, an homogeneous Dirichlet condition is applied on the inner circle. The outer cylinder is moving around its axis and controlled by a signal of velocity which is also the non-homogeneous Dirichlet condition applied on the outer circle. This signal is chosen in order to point out the memory effect of thixotropic fluids. It is made of a 10s ramp-up and ramp-down time with a maximum angular velocity 27 s-1 (Fig.7).

Fig.9: S(t) on inner (blue) and outer (red) circles

Fig.7: Ramp-up ramp-down signal of angular velocity applied on the outer cylinder of the rheometer.

Such a signal leads to an hysteresis loop in the diagram angular velocity versus stress. The study of such an hysteresis loop is a popular way of testing thixotropic materials. 4.2.3 Numerical results The evolution of the structural variable can be seen either by coloring the S-field in the fluid domain (Fig.8) or by plotting S as a function of time on each circle (Fig.9).

The fluid was initially weakly structured (S=0.5). Its formation time being relatively low, at low shear, up to 2s, aggregates are in formation (interactions between particles dominate hydrodynamic stress) and S increases quickly. Since 3s the shear becomes high enough inducing a breaking up of the previous structure. Therefore, S decreases and is minimal 1 or 2s after the time when the shear is maximal (11s). After 11s, the shear decrease induces a fluid restoring. When the signal reaches the 0 value at t=21s, the relaxation of hydrodynamical stress makes the fluid free to aggregate, up to be complete at t=30s (S=1). Moreover, it can be seen that S has higher values on the outer circle. In such a non newtonian fluid, shear rate is higher on the inner cylinder (in newtonian fluids, it is quasi-uniform in the gap) so the fluid is less structured there. 4.2.4 Hydrodynamic Stress Hysteresis loop During simulations the hydrodynamic shear stress can be computed on the inner cylinder in order to compare it to experimental data. In numerical calculations, the shear rate is calculated from its definition (Fig.1), the viscosity comes from equation (3) and the shear stress is then given by: (4) Its variation versus time (Fig.10) reveals the typical behavior of inelastic thixotropic materials in response to an applied shear rate step. Moreover, such a curve can be used to evaluate kinetic parameters of the complex fluid. During the first 2s, the formation process increases the

= .

Fig.8: S in the model of rheometer at t=6s, 10s, 19s, 20s, 22s, 24s.

Excerpt from the Proceedings of the COMSOL Users Conference 2006 Paris

Fig.10: Shear Stress on the inner cylinder

Fig. 12 Experimental hysteresis loop ([2])

viscosity; in the same time grows also, leading to a fast increasing of stress. From 3s up to 11s, the shear-induced breaking up takes place, the viscosity decreases but the shear is increasing faster leading to an increase of stress but with a lower slope. On the contrary, after 11s, the recovering process leads to an increase of the viscosity lower than the decrease of shear inducing a decreasing stress. The characteristic memory effect of this thixotropic fluid is revealed by the lack of symmetry of the curve; it is more visible on the hysteresis loop obtained (Fig.11) by plotting shear stress versus shear rate or angular velocity.

7. Conclusions
The methodology for modelling the thixotropy of inelastic fluids by a single structural scalar variable and a kinetic equation has been previously validated in the case of steady flow conditions (Cf.[2]). Our numerical approach based on the coupling of the kinetic equation with Navier-Stokes equation in the frame of COMSOL Multiphysics provides a farther validation in case of unsteady flows. Furthermore, such numerical simulations of thixotropic flowing fluids give rise to many applications in the field of biomedical diagnosis of blood pathologies.

8. References
1. Quemada, Towards a unified model of elastothixotropy of biofluids, Biorheology, volume 21, page 423-436 (1983) 2. Baravian, Quemada, Modelling thixotropy using a novel structural kinetics approach, Journal of Texture Studies, Volume 27,page 371390 (1996)

Fig. 12 Numerical hysteresis loop

These curve is in good agreement with that obtained by rheometric measurements (Cf. [2]) (Fig.12). The magnitudes of each variables are very close, there is a slight discrepancy between the slopes due to a non ideal fit of some constants of the model. Furthermore, the experimental determination of shear rate is based on approximations whereas its numerical calculation is quasi-exact. From this comparison, it can be concluded that the numerical approach used here is validated.