Chemical Engineering Science 66 (2011) 31803184

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Chemical Engineering Science

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Layer inversion and mixing of binary solids in two- and three-phase uidized beds
Byung-Soon Chun a, Dong Hyun Lee a,n, Norman Epstein b, John R. Grace b, Ah-Hyung Alissa Park c, Sang Done Kim d, Jea Keun Lee e
Department of Chemical Engineering, Sungkyunkwan University, 440-746, Suwon Republic of Korea Department of Chemical and Biological Engineering, University of British Columbia, Vancouver, Canada V6T 1Z3 c Department of Earth and Environment Engineering and Lenfest Center for Sustainable Energy, Columbia University, New York, NY, USA d Department of Chemical and Biomolecular Engineering and Energy and Environment Research Center, Korea Advanced Institute of Science and Technology, Daejeon 305-701, Republic of Korea e Department of Environmental Engineering, PuKyong National University, Busan, Republic of Korea
b a

a r t i c l e i n f o
Article history: Received 12 September 2010 Received in revised form 18 February 2011 Accepted 19 February 2011 Available online 9 March 2011 Keywords: Liquid uidization Three-phase uidization Mixing Binary solids Layer inversion Mixing index

a b s t r a c t
Water uidization in a 210 mm diameter semi-cylindrical acrylic column of a binary solids mixture of 3.2 mm polymer beads (rs 1280 kg/m3) and 0.385 mm glass beads (rs 2500 kg/m3) at supercial liquid velocities from 18.1 to 43.1 mm/s is shown to generate layer inversion at a supercial liquid velocity, UL, of 33.1 mm/s. Introduction of air with a supercial velocity, Ug, of 1.92 mm/s yielded a layer inversion velocity at UL 30.4 mm/s. The latter is explainable if it is assumed that the determinant of layer inversion is the interstitial liquid velocity and that therefore the main function of the gas in this respect is to occupy space. Mixing of the binary solids, as quantied by a mixing index applied to measured particle compositions at different levels of the uidized bed, is shown to be greatest at the layer inversion velocity for liquid uidization and, in general, to increase as co-current gas ow increases at a xed value of UL. & 2011 Elsevier Ltd. All rights reserved.

1. Introduction Solids layer inversion occurs in a liquid uidized bed when binary solids with a density ratio opposite in relative magnitude to their size ratio undergo reversal of their relative vertical positions in the bed as the liquid velocity is increased. Though it was rst reported by Hancock (1936), this phenomenon did not receive much study until the nal two decades of the past century. Most of that work was reviewed critically by Escudie et al. (2006). Consider a binary solids system of spheres containing component 1 of diameter d1 and density rs1 with component 2 of diameter d2 and density rs2, such that d1/d2 414 rs1/rs2. If conditions are such as to give rise to layer inversion when a mixture of the two components is uidized by a liquid, then at very low liquid velocity the two components may be completely segregated by density and at very high velocity by size, i.e. with pure component 1 at the top and bottom of the bed, respectively, and pure component 2 correspondingly at the bottom and top. At intermediate velocities, however, the bottom layer contains a mixture of the two

Corresponding author. Tel.: 82 31 290 7340; fax: 82 31 299 4709. E-mail address: dhlee@skku.edu (D.H. Lee).

components, with only the top layer continuing to have only one solid component, namely component 1 at velocities below and component 2 at velocities above the layer inversion velocity (Di Felice, 1995). Only at the inversion velocity is there uniformity of composition throughout the entire bed. Whether or not a given binary solids mixture of d1/d2 414 rs1/rs2 will undergo layer inversion when uidized by a liquid can be determined from plots of bulk density, rb rs(1 e) rLe, vs. liquid supercial velocity, UL, for the individual components. Only if the two curves intersect at a velocity between Umf of component 1 and vt of component 2 can one expect a layer inversion for the mixture (Epstein, 2005). But, contrary to Epstein and LeClair (1985), the point of intersection is not necessarily the inversion point itself, since, as rst determined experimentally by Moritomi et al. (1982) and subsequently conrmed by others (see Escudie et al., 2006), the inversion velocity depends not only on the size, shape, and density of the two solid components, but also on their overall relative proportions. It should be noted that, for a mixed-size, mixed-density binary that undergoes layer inversion, the smaller denser particles experience minimum uidization at a liquid velocity below that of their opposite number, but when the latter are eventually uidized as well on further increasing the liquid velocity, they immediately

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assume their vertical position in the bed above the already-uidized smaller denser particles. This switch during transition from xed to uidized bed is a pseudo-inversion, not to be confused with layer inversion during uidization. What happens when gas is co-introduced with the liquid to uidize a solids binary that undergoes layer inversion in the absence of the gas is the subject of the present paper. Of the two prior studies of gasliquid uidization of binary solids, both by Fan et al. (1985, 1987), only the earlier paper tested binaries in which the two components differed in both size and density. In the 1987 study, the pairs differed only in size. In the 1985 study, of the ten binary mixtures investigated, only one had properties conducive to layer inversion, and for that binary, two separate layer inversion (complete intermixing) regions were reported in a plot of Ug vs. UL, one in the vicinity of UL E20 mm/s and the other at or near (depending on Ug) UL E200 mm/s. However, the former occurred immediately above the minimum uidization line and was clearly a manifestation of the pseudo-inversion mentioned above. Unlike the present study, no runs were reported for Ug 0 (liquid uidization).

1800 PB GB 1600 b, [kg/m3]

1400

1200

1000 0 10 20 30 40 50 60 70 UL, [mm/s]

Fig. 2. Bulk density of each type of solid particle vs. supercial liquid velocity. GB glass beads; PB polymer beads.

2. Experimental Fig. 1 shows a schematic diagram of the experimental setup. The semi-cylindrical acrylic column had an inner diameter of 210 mm and a test section height of 1.8 m. Gas and liquid distributors were installed at the bottom of the test section to provide uniformly distributed gas and liquid ows. The liquid and gas distributors had 35 holes of 3 mm diameter and 33 holes of 1 mm diameter, respectively. The binary solids mixtures consisted of spherical, closely sized 3.2 mm polymer beads (rs 1280 kg/m3,Umf 15.0 mm/s) and 0.385 mm glass beads (rs 2500 kg/m3,Umf 1.3 mm/s). This binary was chosen because, as shown in Fig. 2, the experimentally determined curves of bulk density vs. supercial liquid velocity fulll the above mentioned criterion of intersecting at UL between minimum uidization and minimum free settling. For the principal runs, 1.8 kg of polymer beads (PB) was mixed with 3.0 kg of glass beads (GB) so that the PB:GB volumetric ratiox1 : x2 0:54 : 0:46: Some subsidiary experiments were also performed with other PB:GB volumetric ratios. Water at 2072 1C and ambient air were the only liquid and gas used in the experiments. Pressure taps, axially spaced at 0.1 m intervals starting 0.06 m above the liquid distributor, were connected to pressure transducers.

Phase holdups were determined primarily from the axial pressure proles, aided in some cases by visual observation of expanded bed height and by particle sampling. Particle samples were withdrawn through ports at the wall of the column 0.1, 0.2, 0.3, 0.4, 0.5, 0.6, and 0.9 m above the liquid distributor.

3. Data processing For both the liquid uidization and the gasliquid uidization runs, the total solids holdup, es, was determined as solids volume/ bed volume, given by

es

M1 =rs1 M2 =rs2 AH

For the liquid uidization, the expanded bed height, H, could be determined both visually and from the sharp break in the pressure prole, whereas for gasliquid uidization, only the latter method was reliable due to the large bed level uctuations. At the liquid inversion point, es (and hence eL 1 es) could alternatively be determined from the uniform pressure gradient in the uniformly mixed bed, dp=dz es rs eL rL g es rs 1es rL g 2 where

rs x1 rs1 x2 rs2
For gasliquid uidization at the inversion point,   dp=dz es rs eL rL eg rg g with rs again given by Eq. (3) and

es eL eg 1

If es is known, the two unknowns eL and eg can be determined by simultaneous solution of Eqs. (4) and (5). To evaluate the extent of solids mixing at various values of UL, Ug and x1 : x2 from the particle sampling at various levels, the intermittency index, g, of Brereton and Grace (1993) was invoked. In the present context, g becomes a segregation index, dened as
Fig. 1. Schematic of experimental setup: (1) test section; (2) calming section; (3) computer; (4) differential pressure transducer; (5) data acquisition; (6) pump; (7) reservoir; (8) gas owmeter; (9) liquid owmeter; (10) pressure taps; (11) distributors; (12) sampling ports.

g s=sfs

where the standard deviation, s, of the local uid-free binary composition x2 ( 1 x1) from its average value, x2 , for N

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samplings is given by v u N u1 X st x x2 2 N i 1 2i and x2

N 1X x N i 1 2i

Thus, for perfect mixing, s 0, and therefore g 0, whereas for complete segregation, s sfs, and therefore g 1. Here, we simply reverse the scale by dening the mixing index, MI, as MI 1g 1s=sfs 10

4. Results and discussion 4.1. Layer inversion: visual Fig. 3 shows snapshots of the liquid uidized bed containing PB:GB at volume ratio of 0.54:0.46 and different liquid supercial

while the standard deviation corresponding to full segregation, sfs, can be shown to be given by p sfs x2 1x2 9

Fig. 3. Snapshots showing bed inversion in liquid uidized bed for PB:GB volume ratio 0.54:0.46 with increasing supercial liquid velocity: (a) 18.2 mm/s, (b) 28.1 mm/s, (c) slightly greater than 33.1 mm/s, (d) 38.2 mm/s, (e) 43.1 mm/s. Inversion was observed at UL 33.1 mm/s.

Fig. 4. Photographs of three-phase uidized bed as a function of liquid velocity. PB:GB volume ratio 0.54:0.46; Ug 1.92 mm/s. UL: (a) 18.1 mm/s; (b) 23.1 mm/s; (c) 28.1 mm/s; (d) 30.4 mm/s; (e) 38.1 mm/s; (f) 43.1 mm/s. Inversion was observed at UL 30.4 mm/s.

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MI, [ - ]

velocities. The black and white particles are polymer and glass beads, respectively. The inversion velocity, (UL)inv, at which the two solid components appeared to be perfectly uniformly blended throughout the bed, was observed to be 33.1 mm/s, just slightly below the velocity in Fig. 3(c). Fig. 4 shows similar photographs of the gasliquid uidized bed, again with a PB:GB volume ratio of 0.54:0.46, and with Ug 1.92 mm/s. The layer inversion point in this case occurred visually at (UL)inv 30.4 mm/s, Fig. 4(d). 4.2. Layer inversion: quantitative

1.0 PB: GB = 0.32:0.68 PB: GB = 0.54:0.46 PB: GB = 0.67:0.33

0.8

0.6

0.4

0.2

Table 1 records bed holdups at the above two layer inversion velocities calculated from Eqs. (1)(5). To relate liquid inversion velocity of the same solids in the absence of a gas, we will test a hypothesis that has worked well in predicting the onset of minimum liquid uidization in the presence of a gas (Zhang et al., 1995). We assume that the main relevant function of the gas for our purpose is simply to occupy space, thereby reducing the crosssectional area available to the liquid and solids. We then assume that the intermixing of the solids is governed by the interstitial liquid velocity, ULi, which would therefore have similar values at the respective layer inversion points. Thus, for the gasliquid uidization described above, (ULi)inv 30.4/0.699543.5 mm/s, while, for the corresponding liquid uidization in the absence of a gas, (ULi)inv 33.1/0.742 44.6 mm/s. The match between the two values is even closer if, in the latter calculation, instead of using the average value of eL 0:742, which is based in part on visual observation of the bed expansion and Eq. (1), one uses eL 0.754 obtained from the pressure gradient (Eq. (2)), as we did for gasliquid uidization (Eq. (4)). Then (ULi)inv for the gas-free uidization inversion becomes 33.1/0.75443.9 mm/s. The qualitative implication of the above hypothesis is that, in a plot of (UL)inv vs. Ug for gasliquid (three-phase) uidization of binary solids, (UL)inv should gradually decrease as the supercial gas velocity increases. That is precisely what is shown by the previously mentioned layer inversion region of Fan et al. (1985) for a mixture of 2.27 mm alumina beads (rs 3690 kg/m3) and 6.11 mm glass beads (rs 2200 kg/m3) uidized by water and air. The region of complete intermixing is a band of narrowing thickness with increasing Ug that, within the limited precision of the published plot, shows (UL)inv E210720 mm/s at Ug 20 mm/s and (UL)inv E160710 mm/s at Ug 60 mm/s. Empirical equations (22) for the overall voidage, e, and (23) for eg of Fan et al. (1985) can be used to estimate eL e eg for these two well-intermixed cases. These estimates are only approximate since these equations are explicitly designated only for regions of partial intermixing. Assuming a water temperature of 23 1C (see Escudie et al., 2006, Table 1), the two equations yield eL E0.737 (0.018, 0.019) at Ug 20 mm/s and eL E0.679 (0.011, 0.012) at Ug 60 mm/s. The corresponding values of (ULi)inv [(UL)inv/eL] are

0.0 15 20 25 30 35 40 45 50 UL, [mm/s]

Fig. 5. Effect of liquid velocity on solids mixing index for liquidsolid uidized beds.

Fig. 6. Effect of gas velocity on solids mixing index for three-phase uidized beds.

285720 and 236710 mm/s, respectively. Given the approximations involved in arriving at these values, their reasonable agreement is consistent with the idea that the interstitial liquid velocity is the prime determinant of the layer inversion point for a given binary mixture, its value being inuenced by the presence of the gas mainly by virtue of the space that it occupies. 4.3. Particle mixing Fig. 5 shows the effect of the liquid supercial velocity on the mixing index, MI, dened by Eq. (10), for liquid uidization of the present binary (PB, GB) system, with three different uid-free solids compositions. MI appears to achieve a maximum at about the same value of UL (33.1 mm/s) in all three cases. The implication of this result is that, at least for this particular binary system, the solids composition effect on the layer inversion velocity is small or even negligible. Solids mixing appears to be maximized in the vicinity of the liquid inversion velocity, a nding that could be useful in cases where blending of two particle species is sought. Fig. 6 shows the inuence of Ug on MI at three different liquid supercial velocities and three solids compositions. In most cases,

Table 1 Calculated bed holdups at layer inversion points.

es
Liquidsolid uidization Eq. (1), visual Eq. (1), pressure prole Eq. (2) Average 0.261 0.267 0.246 0.258

eL
0.739 0.733 0.754 0.742

eg

Gasliquidsolid (three-phase) uidization Eq. (1), pressure prole 0.2721 Eqs. (4) and (5)

0.6995

0.0284

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MI increased appreciably on rst introducing air into the wateruidized bed.

5. Conclusions For a binary solids mixture that undergoes layer inversion when uidized by a liquid, introduction of a gas co-currently with the liquid causes the liquid supercial velocity at the inversion point to decrease as the gas supercial velocity increases. This result is qualitatively, and even quantitatively, explainable if it is assumed that the interstitial liquid velocity is the principal determinant of the layer inversion, and therefore that the main effect of the gas ow is due to its occupation of space. Mixing of the binary solids, characterized by applying a mixing index to particle compositions at vertical increments of the uidized bed, is shown to maximize at the layer inversion velocity of a liquid-uidized bed and, in general, to increase as gas is rst introduced co-currently at any xed supercial liquid velocity.

rb rg rL rs s sfs

bulk density (kg/m3) gas density (kg/m3) liquid density (kg/m3) solid density (kg/m3) standard deviation given by Eq. (7) () value of s corresponding to full segregation () Subscripts

1 2 i inv

larger less-dense component smaller denser component ith particle sample layer inversion point Superscript

average over the entire bed

Acknowledgement Nomenclature A d g H M MI N p Ug UL ULi Umf vt x z cross-sectional area of column (m2) particle diameter (mm) acceleration of gravity (m/s2) expanded bed height (m) mass of solid particles (kg) mixing index () number of particle samples withdrawn () pressure (Pa) supercial gas velocity (mm/s) supercial liquid velocity (mm/s) liquid interstitial velocity (mm/s) minimum uidization velocity (mm/s) particle terminal settling velocity (mm/s) uid-free volume fraction of a solids component () height coordinate (m) This study was partly supported by the GRRC program of Gyeonggi Province, South Korea, through a research program and instrumental support. The Canadian co-authors are also indebted to the Natural Sciences and Engineering Research Council of Canada for continuing nancial support. References
Brereton, C.M.H., Grace, J.R., 1993. Microstructural aspects of the behaviour of circulating uidized beds. Chemical Engineering Science 48, 25652572. Di Felice, R., 1995. Hydrodynamics of liquid uidization. Chemical Engineering Science 50, 12131245. Epstein, N., 2005. Teetering. Powder Technology 151, 214. Epstein, N., LeClair, B.P., 1985. Liquid uidization of binary particle mixturesII. Bed inversion. Chemical Engineering Science 40, 15171526. Escudie, R., Epstein, N., Grace, J.R., Bi, H.T., 2006. Layer inversion phenomenon in binary-solid liquid-uidized beds: prediction of the inversion velocity. Chemical Engineering Science 61, 66676690. Fan, L.S., Matsuura, A., Chern, S.-H., 1985. Hydrodynamic characteristics of a gas liquidsolid uidized bed containing a binary mixture of particles. A.I.Ch.E. Journal 31, 18011810. Fan, L.S., Yamashita, Y., Jean, R.-H., 1987. Solid mixing and segregation in a gas liquidsolid uidized bed. Chemical Engineering Science 42, 1725. Hancock, R.T., 1936. The teeter condition. Mining Magazine 50, 9094. Moritomi, H., Iwase, T., Chiba, T., 1982. A comprehensive interpretation of solid layer inversion in liquid uidized beds. Chemical Engineering Science. 37, 17511757. Zhang, J.-P., Epstein, N., Grace, J.R., Zhu, J., 1995. Minimum liquid uidization of gasliquid uidized beds. Transactions of the Institution of Chemical Engineers 73 (Part A), 347353.

Greek Symbols

g e eg eL es

segregation index () overall bed void fraction () gas holdup () liquid holdup () solids holdup ()