Technical notes

Experiments in Fluids 22 (1997) 261264

Springer-Verlag 1997

Refractive index matching and marking methods for highly concentrated solidliquid flows
M. M. Cui, R. J. Adrian

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Abstract Two index-matched systems of solid particles in liquid have been developed to enable the study of velocity and concentration distributions in the highly concentrated solidliquid ows. The mixtures have excellent optical transparency up to depths exceeding 80 mm at concentrations up to 50% solids by volume. Highly visible marker particles with nearly the same mechanical properties as the index-matched particles are formed by metal plating or substitution. Good quality images of marker particles are obtained in both stationary and moving two-phase mixtures, and permit accurate tracking of the individual markers. and when the concentration approaches close packing, they cannot be penetrated more than a few particle diameters. Magnetic resonance imaging and acoustical scattering techniques are useful methods for measuring some aspects of the ows, but it is desirable to be able also to bring the powerful optical techniques of laser Doppler velocimetry and particle image velocimetry (cf. Adrian 1991) to bear on the experimental study of these ows. A well known method of achieving optical transparency in model systems of solidliquid mixtures is to match the refractive indices of the solids and the liquid by careful choice of both. While this approach should, in principle, render the mixture perfectly transparent, in practice the depth to which one can image into the mixture is limited by imperfections in the solid particles such as ne bubbles, by variations of the refractive index within the solids, and by variations of the refractive index of the liquid caused by temperature sensitivity and/or changing properties of the liquid mixture. For example, Zisselmar and Molerus (1978) report penetration of 50 mm into a 5.6% mixture of 55 m glass beads, and Nouri et al. (1986) report penetration of 25.4 mm into a 14% mixture of 116212 m Diakon particles in a mixture of tetraline and turpentine. By using silica gel particles Abbas and Crowe (1987) were able to increase the concentration to 30% with 17.5 mm penetration using 96 210 m particles, and Chen and Kadambi (1990) achieved 25.4 mm penetration through 50% concentrations of 40 m silica in a sodium iodide solution. Park et al. (1989) used 12 m silica gel particles in a 51 mm pipe at 14% volume concentration, but reported that some of the other brands of silica gel particles that they tried gave limited penetration at high concentrations due to refractive index variations within the particles. This Note describes two new refractive index-matched systems of solid particles in liquids. These suspensions extend the repertoire of model systems available for experimental study by providing penetration depths and maximum concentrations that are signicantly greater than those reported heretofore. The high transparencies achieved make possible experimental investigations in relatively large scale apparatus, of order 100 mm in thickness. The liquids used in these systems have also been selected to have viscosity and density near that of water, making them suitable as models of coalwater slurries. A new aspect of the technique described here is the introduction of special marker particles into the transparent mixture to make the motion and concentration of the solids visible. Instead of relying on uncontrolled impurities in the primary population of solids to scatter light, the marking

1 Introduction
Concentrated solidliquid ow occurs when the mean volume concentration of suspended solids exceeds 510%. It is characterized by momentum and energy transfer due to the translation of particles from one layer to another and collisions among the particles. Continuum descriptions require constitutive equations that relate the concentration of solids, the rate-of-strain, and the stress, energy and dissipation of the mixture to micro-mechanical aspects of particle motion and material properties of the particles. In addition to the macroscopic velocity and concentration of the mixture, the granular temperature, dened as the mean square of the random particle velocity, is a fundamental and often difcult to predict dependent variable that should be measured (Savage 1984; Campbell 1990). Important physical properties that should be controlled experimentally are the ratio of solid and uid densities, the shape and mechanical properties of the solid particles, and the viscosity of the uid. Experimental studies of concentrated two-phase ows such as slurries and rapid granular ows are hindered by the high opacity of the real solid-in-uid mixtures. Even at solids fractions of 0.1, the mixtures are difcult to penetrate optically,

Received: 4 March 1996/Accepted: 14 June 1996 M. M. Cui, R. J. Adrian Department of Theoretical and Applied Mechanics University of Illinois Urbana, IL 61801 USA Correspondence to: R. J. Adrian The research was supported by the Department of Energy through Argonne National Laboratory.

is controlled making possible improved accuracy of velocity measurements and the measurement concentration.

2 Model system for suspensions of spherical, neutrally buoyant particles

Theoretical analyses and numerical simulations of solidliquid suspensions commonly treat simplied conditions in which the particles are monodisperse, spherical and neutrally buoyant, the latter condition permitting the neglect of gravitational force. Since the primary concern is with characteristics that arise predominantly from transport by the particulates, it is also desirable for the uid viscosity to be small. (To model dry granular ow it is also necessary for the uid density to be small compared to the particle density, but this is not compatible with achieving refractive index matching.) By using a combination of three liquids it is possible to adjust both the liquid refractive index and the liquid density independently, so as to achieve good refractive index matching and neutrally buoyant particles. The system reported here consists of a liquid mixture of tetraline, 1-methanaphthalene and 1-chloronaphthalene and styrene/divinylbenzene particles (Bangs Laboratories, Inc.). As shown in Fig. 1a, the shape of styrene/divinylbenzene particles is perfectly spherical, and they are available in a range of sizes. Table 1 summarizes the properties of tetraline, 1-methanaphthalene, 1-chloronaphthalene and styrene/divinylbenzene particles. The neutrally buoyant solid/liquid mixture is a combination of 41% tetraline, 28% 1-methanaphthalene and 31% 1-chloronaphthalene by volume. In this combination the refractive index is 1.5903, and the density is 1050 kg m\3, matching the values listed for the particles in Table 1. The dynamic viscosity is 2.547;10\3 kg m\1 s\1, and the kinematic viscosity is 2.426;10\6 m2 s\1, about two and one-half times that of water. The transparency of each refractive index-matched mixture and the visibility of marker particles have been studied in both stationary and moving suspensions. Figure 1b demonstrates the transparency of a 15 mm deep layer of a 50% by volume suspension styrene/divinylbenzene particles in a laboratory dish resting on a ruled pattern. The visibility of the pattern seen looking through the suspension is excellent. By controlling the percentage of different chemicals one can also obtain index-matched liquid mixtures with different densities which can be used to study the inuence of solid/ liquid density ratio on the behavior of the two-phase ow.

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2.1 Spherical, neutral buoyancy marker particles

Unlike previous LDV techniques which used air bubbles in the solid particles (Nouri et al. 1986) or index mismatch of solid and uid (Abbas and Crowe 1987), the present idea is to match the indices of solid and liquids as well as possible, and then to seed the suspension with a selected number of marker particles that are made visible by special treatment. The number of marker particles is chosen to permit measurements with acceptable data rate while maintaining satisfactory transparency. The independent selection of index-matched particles and marker particles provides valuable freedom which can be used to maximize the penetration depth at a given conFig. 1. a Photograph of styrene/divinylbenzene particles (250 m mean diameter); b optical transparency of a 50% suspension of styrene/divinyl benzene particles in index-matched liquids. The depth of the layer of suspended particles is 15 mm; c nickel plated styrene/ divinylbenzene particles (250 m mean diameter)

centration of solid particles in which the measurements can be done. Ideally, the marker particles should have the same mechanical properties as the unmarked particles, and their scattering

Table 1. Basic properties of 1-methanaphthalene, 1chloronathalene, tetraline and styrene/divinylbenzene particles

Property

1-Methanaphthalene 1001 1.615 240243 3;10\3

1-Chloronaphthalene 1194 1.632 111113 3.5;10\3

Tetraline

Styrene-divinylbenzene particle 1050 1.5903

Density (kg m\3) Refractive index (20C) Boiling point (0C) Viscosity at (20C (kg m\1 s\1)

967970 1.546 207.2 2.2;10\3

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characteristics should produce enough light to give clear images. An ideal method of meeting these criteria is to plate a mechanically thin but optically thick layer of metal onto the same particles as those used in the suspension. For the styrene/divinylbenzene particles nickel plating by precipitation proved successful in creating very bright particles that produced excellent images, Fig. 1c. The marker particles retain the sphericity of the original particles, and because of the thinness of the plating they have the same mechanical properties as the unplated particles, including essentially the same density.
Table 2. Properties of alcohols and silica gel particles Property Density (kg m\3) Refractive index (20C) Boiling point (C) Viscosity at 20C (kg m\1 s\1) Benzyl alcohol 1045 1.540 205 2.0;10\3 Ethyl alcohol 800888 1.3601.362 7879 1.2;10\3 Silica gel 2100 1.452

3 Model system for suspensions of irregular, heavy particles

The rheology of dense suspensions of heavy, irregularly shaped particles is of interest because of the technological importance of coal slurries and slurries from mining operations. Silica gel particles have irregular shape which is qualitatively similar to coal particles. In the present system refractive index matching is achieved using a mixture of 45% benzyl alcohol and 55% ethyl alcohol by volume. The properties of the alcohols and silica gel particles are listed in Table 2. The data varies slightly depending upon the manufacturer and the purity. The refractive index of liquid is measured by a refractometer (ATAGO R5000). The liquid temperature was controlled within 0.1C. The refractive index of the alcohol mixture is not sensitive to change of temperature, making the mixture easy to use. There is no special requirement to control the temperature of the test section as long as the room temperature is stable to within <2C. Naturally, the tolerance for temperature variation decreases with increasing depth of penetration. The viscosity of the mixture of benzyl and ethyl alcohols has been measured as a function of temperature with a standard viscometer (Brookeld synchro-lectric viscometer model LVT) and temperature-dependent data can be found in Cui (1994). At 20C the density is 974.4 kg m\3, the dynamic viscosity is 2.0;10\3 kg m\1 s\1, and the kinematic viscosity is 2.05 m2 s\1, close to that of water. Because of the irregular particle shape and the distribution of sizes over the range 75580 m, close packing of the silica gel particles (after immersion in the alcohol mixture) occurs at a concentration of 83.3% by volume, rather higher than for spherical particles. The silica gel can be sieved to obtain different size distributions, and the volume concentration at which close packing occurs would vary with the size distribution. The most useful property of this suspension is its extreme clarity. Figure 2b shows a 1 mm rectangular grid viewed

through an 80 mm deep layer of 50% by volume suspension of the 75580 m silica particles. The present silica system possess exceptional transparency and penetration depth, making it suitable for large-scale simulation. In comparison, a suspension of the same solid particles with 5% concentration by volume in water is totally opaque. The improved transparency is due, in part, to the use of high purity silica (Chromatographic Silica Media, Davis Chemical). Attempts to plate nickel onto the silica gel were not as successful as for the styrene/divinylbenzene particles. Application of the plating was irregular, even after etching the silica surfaces with acid, and the resulting images of the markers were weak. As an alternative, magnesium/aluminum 50/50 alloy particles (Reade Mfgr. Co.) of equal sieve size have been used to mark the silica gel/alcohol mixture. These particles possess irregular shapes not dissimilar from the silica gel, cf. Fig. 2c. The images of the magnesium/aluminum particles are very clear, even in close packed silica gel particles, as shown in Fig. 3. Images of marker particles moving within the suspension have also been obtained by using a video camera. The multiple exposed particle images shown in Fig. 4 illustrate the images obtained after thresh holding. Since the intensity of the light scattered by the marker particles is signicantly stronger than the background noise, threshold values that accurately isolate the marked particles from the background are easily chosen. These bilevel images can be used to calculate the locations of the centroids, sizes and distribution of the marker particles.

4 Concluding Remarks
Refractive index matching of two systems of solid particles and liquids has been achieved. The transparency of the mixtures is excellent at large depth-of-eld and close-packing of particles. The best result is obtained by developing the index matched two-phase mixtures and proper marker particles separately.

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Fig. 3. Magnesium/aluminum powder in a 20 mm thick close-packed layer of silica gel particles with refractive index matching alcohols

Fig. 4. Multiple exposed particle images in a refractive index matched layer of silica gel/alcohol mixture with 60% concentration. The layer thickness is 25 mm.

Fig. 2. a The shape of silica gel particles (250 425 m); b optical transparency of a 50% suspension of silica gel particles in a refractive index matching liquid. The particles are 75585 m in size and the thickness of the suspension is 80 mm. The scale of the grid is 1 mm/division; c the shape of magnesium/aluminium particles with 300 m mean diameter.

References
Abbas MA; Crowe CT (1987) Experimental study of the ow properties of the a homogeneous slurry near transitional Reynolds numbers. Int J Multiphase Flow 13: 357364

Adrian RJ (1991) Particle-imaging techniques for experimental uid mechanics. Annu Rev Fluid Mech 23: 261304 Bangs Laboratories, Inc. 979 Keystone Way, Carmel, In 46032 USA Campbell CS (1990) Rapid granular ows. Annu Rev Fluid Mech 22: 57 92 Chen RC; Kadambi JR (1990) LDV measurements of solidliquid slurry ow using refractive index matching technique. Particulate Sci Tech 8: 97109 Cui MM (1994) Experimental study of highly concentrated two-phase ows. Ph.D. thesis, University of Illinois, Urbana Davis Chemical, Baltimore, MD 21203 USA Nouri JM; Whitelaw JH; Yianneskis M (1986) A refractive-index matching technique for solid/liquid ows. Proc 3rd Int Symp on Application of LDA to Fluid Mechanics, Lisbon, Ladoan Park JT; Mannheimer RJ; Grimley TA; Morrow TB (1989) Velocity measurements of transparent non-Newtonian pipeline slurries with laser Doppler velocimetry. In: Applications of laser anemometry to uid mechanics, eds. R.J. Adrian et al., pp 292312. Heidelberg: Springer Reade Mfgr. Co., Lakehurst, NJ 08732 USA Savage SB (1984) The mechanics of rapid granular ows. Adv Appl Mech 24: 289366 Zisselmar R; Molerus O (1978) Investigation of solidliquid pipe ow with regard to turbulence modication. Int. Symp. on Momentum, Heat and Mass Transfer in Two-Phase Energy and Chemical Systems, Dubrovnik, Yugoslavia, pp. 4 9