Sannomiya, A., K. Ichimura, M. Yano and Y. Harano: 17) Uemura, Y., Y. Hatate andA. Ikari: /. Japan Petrol. Inst.

ndA. Ikari: /. Japan Petrol. Inst., 29,

143 (1986).
Kagaku Kogaku Ronbunshu, 10, 158 (1984).
Sannomiya, A., M. Yano and Y. Harano: Kagaku Kogaku 18) Uemura, Y., Y. Hatate and A. Ikari: /. Chem. Eng. Japan, 19,
560 (1986).
Ronbunshu, ll, 381 (1985).
Satterfield, C. N.: "Heterogeneous Catalysis in Practice," p. 19) Uemura, Y., Y. Hatate and A. Ikari: /. Japan Petrol. Inst., 30,
137, McGraw-Hill (1980). 53 (1987).

Summers, J. C. and S. A. Ausen: /. CataL, 52, 445 (1978). 20) Uemura, Y., Y. Hatate and A. Ikari: /. Chem. Eng. Japan, 20,
Turlier, P., H. Praliaud, P. Moral, G. A. Martin and J. A. 117 (1987).
Dalmon: Appl. CataL, 19, 287 (1985). 21) Vincent, R. C. and R. P. Merrill: /. Catal, 35, 206 (1974).

HEAT TRANSFER COEFFICIENT IN THREE-PHASE VERTICAL

UPFLOWS OF GAS-LIQUID-FINE SOLID
PARTICLES SYSTEM

Yasuo HATATE, Shuichi TAJIRI, Takanori FUJITA,

Takashi FUKUMOTO,Atsushi IKARI
AND TADASHI HANO
Dept. of Chemical Engineering, Kagoshima Univ., Kagoshima 892

Key Words: Heat Transfer Coefficient, Three Phase Flow, Slurry Flow, Vertical Up flow, Solid Particle
Heat transfer characteristics between the inner tube wall and fluid of air-water-fine glass spheres three-phase
vertical up flow were investigated using three kinds of glass spheres and two tubes under the following operating
conditions:
gas velocity (£/G)=80- 900cm/s, slurry velocity (£/L) = 30- 160cm/s, and solid particles concentration in
slurry (Cs)=5-54wt% for DT=15-mm tube; and UG=15-305cm/s, UL=8-62cm/s, and Cs=0.2-57wt%
for Dr=21-mmtube.
The following results were obtained.
1) The heat transfer coefficients of three-phase vertical upflow exhibit larger values than those of gas-liquid two-
phase vertical up flow in the range of 0-40 wt % solid concentration.
2) Monotonous small increases of the heat transfer coefficient with increase of both gas and slurry velocities were
observed over the whole range of experimental conditions.
3)
30%.
A new empirical correlation of heat transfer coefficient was proposed to fit all data obtained in this work within

three-phase flow with high fluid velocities in analyzing

Intr oduction and designing the preheater section, in which slug
Reaction systems of gas-liquid-solid three-phase flow is predominant.^ In that section, temperature
type have become of interest in recent years, since rises to about 450°C and the coal fed is almost
they have a wide variety of applications such as coal dissolved to preasphaltenes. To develop an analysis of
liquefaction, petroleum desulfurization and waste- the preheater section, the flow characteristics in the
water treatment. In the coal liquefaction process, vertical and horizontal tubes have been described in
pulverized coal is mixed with a solvent and hydrogen previous works2'3) using air, water and fine glass
under high pressures of 100-200 atm in the preheater spheres in place of hydrogen, solvent oil and coal
section and is then fed to the dissolver section to be particles, respectively. However,most studies of heat
liquefied.1} It is especially important to understand the transfer in three-phase flow have been carried out
flow, heat transfer and mass transfer characteristics of under relatively mild conditions such as those in
slurry bubble columns and three-phase fluidized beds.
Received December 25, 1986. Correspondence concerning this article should be
addressed to Y. Hatate. T. Fujita is now at Daikin Co., Ltd., Osaka. T. Hano is at
Little information is available for systems with the
Dept. of Environmental Chemistry and Engineering, Oita Univ., Oita. high fluid velocities that are predominant in some
568 JOURNAL OF CHEMICAL ENGINEERING OF JAPAN
practical reactors and transport lines.4'6) Therefore,
the parameters required for design are presently esti-
mated from those of gas-liquid two-phase flow. To
improve this situation, heat transfer data from three-
phase flow should be used for design instead of those
from two-phase flow. In this work, as a cold model
study to obtain effective heat transfer data for analyz-
ing and designing the preheater section of coal
liquefaction equipment, experimental work concern-
ing the heat transfer of gas-liquid-solid three-phase
flow in vertical up flow tubes was carried out under
various conditions to clarify the effects of the solid
phase on thermal behavior. The heat transfer coef-
ficient between three-phase flow and inner tube wall in
the slug flow regime was studied to derive a useful
correlation.
1. Experimental
Fig. 1. Experimental apparatus.
1.1 Equipment
A schematic diagram of the experimental apparatus Table 1. Experimental conditions
is shown in Fig. 1. The up flow vertical column
consisted of a test section for measuring heat transfer rj, u
Tube
^ u
Tube
Test
.
. Slurry
Air flow ,,
Solid
J
rate, a calming section below the test section, and a ,. x ,
diameter length , section
t . rT
rate UG now rate
TT cone,
A in
length G UL slurry Cs
transport section above the test section. Twotubes, A
and B, were used. The outer and inner diameters of [mm] [mm] [mm] [cm/s] [cm/s] [wt %]
27.0 6000 1000 0- 300 7.5-60 0-60
each copper test section were respectively, 27 mmand
35mmforTubeA, and 15mmand 25mmforTube B. 15.0 6000 1000 0- 1000 16-200 0-60
The copper tube was heated by a Teflon-coated wire-
heater wound uniformly and closely on the outer
surface, and was insulated with 10cm-thick glass- Table 2. Properties of glass spheres
wool to prevent heat loss to the surrounding air. The Glass spheres Density Average size frim]
calming and transport sections, having the same inner
diameter as the test section, were composed of acrylic [g/cm3] dp32 dp50
resin and their lengths were 4m and 1 m, respectively.
The temperatures were measured by copper- A 2.52 29 28
constantan thermocouples. B 2.52 63 63
The heat flux through the tube wall was determined
from the product of the voltage and amperageread- C 2.52 98 94
ings loaded to the heating coil.4) No control device
was prepared to hold a constant temperature through-
out the heating coil section. The heat fluxes obtained tie test section were measured at the same locations
were confirmed to be the same values as estimated s those of the holes on the wall. The temperatures at
from the temperature differences between the calming l measuring points were taken after reaching the
section at 50cmbelow the inlet of the test section and teady state. The experimental conditions are listed in
the mixing box at 30cmabove the outlet of the test able1.
section. The longitudinal temperature distributions of .2 Procedure
both the tube wall and fluid in the test section were Air, tap water and fine glass beads were used as the
determined by measuring their temperatures at five as, liquid and solid. Three kinds of glass beads were
points located at equal intervals. The wall tempera- sed. The density and average diameter of the beads
ture was measured as follows. Copper-constantan re listed in Table 2. Air supplied from the compres-
thermocouples were inserted into holes bored in the dy was introduced through an air filter and air-oil
outer surface of the tube. The diameter of the holes sparator to the vertical tube after adjusting the flow
was 1.5mm, and the depth was 3.5mm for Tube A ate by orifice. Water and glass beads were mixed
and 4.5mm for Tube B. They were closely packed loroughly in a tank and pumped into the column.
with a fine copper powder after setting the ther- iir and slurry were mixed in the T-tube mixer just
mocouples (see Appendix). The fluid temperatures in efore the calming section. Air and slurry from the
VOL 20 NO. 6 1987 569
transport section were separated in a gas-liquid sepa-
rator, and slurry was recycled to the mixing tank. The
solid concentration in the slurry was determined by
weighing the dried glass beads of slurry samples from
the gas-liquid separator.
1.3 Calculation of heat transfer coefficient
The heat transfer coefficient between the tube inner
and bulk flow was calculated from the following
equation.
h=Q/(AAtJ (1)

The value of Q was given by the product of the

voltage and amperage readings loaded to the heating
coil. The average temperature difference A tm between
the fluid and wall was calculated from the following Fig. 2. Comparison of single-phase flow with Sieder-Tate
equation. equation.

^m=K \L{tjl)-th{l)}dl (2)

The longitudinal temperature profiles, tb(l) and
tw (l), were obtained from the fluid and wall tempera-
tures
section.
respectively at five measuring points in the test
2. Results and Discussion
2.1 Heat transfer coefficients in single-phase flow of
water
To check the reliability of the experimental meth-
ods, heat transfer coefficients observed for water
flow were compared with those calculated by the
correlation of Sieder and Tate.10) The results are
shown in Fig. 2. It is apparent that the data obtained
in this study satisfy well the correlation of Sieder and
Tate.10)
Fig. 3. Relation between h and UG at various UL for

2.2 Heat transfer coefficients in two-phase and three-

phase flows
1) Effects of gas and slurry flow rates Heat trans-
fer coefficients h observed in the 27-mmtube for two-
phase flow without particles and three-phase flow
containing 30 wt% solid particles of Bead B are shown
in Fig. 3. Similar results with the 15-mm tube are
shown in Fig. 4. From these figures, the heat transfer
coefficients are found to increase significantly when a
small amount of gas is introduced into the vertical
tube. It is also shown that the heat transfer coef-
ficients gradually increase with flow rates of gas and
liquid. The presence of solid particles resulted in slight
increases in the heat transfer coefficients.
Salamore et al.9) obtained data for a 3.18-cm
horizontal tube using water suspension systems of
particular solid powders such as copper, carbon, Fig. 4. Relation between h and UG at various UL for
chalk and silica that behave as pseudoplastic non- DT= 1.5-cm tube.
Newtonian fluids, so that their apparant viscosity
decreases with increasing rate of flow. Although they particles concentration on heat transfer coefficient but
proposed a new correlation based on a wide experi- exhibits a comparatively large effect of solid diameter
mental range which predicts almost no effect of solid on heat transfer, it is so much different from the
570 JOURNAL OF CHEMICAL ENGINEERING OF JAPAN
Fig. 5. Relation between h and Cs for DT=2.1- and 1.5-cm Fig. 6. Data correlation with Sieder-Tate equation for Dr=2.7cm.
tubes.

ordinary Newtonian-type heat transfer correlatior

that a comparison of our result with Salamore'j
correlation does not seem worthwhile.
Konnoet al.1] carried out detailed experiments witl
water-suspended spherical glass beads (0.15-1.0 mn
in diameter) and water-ion exchange resin (0.5 mmir
diameter) systems using 1.28- and 1.90-cm vertica
up flow tubes to study the heat transfer characteristics
They concluded that temperature profiles of liquid
solid two-phase flows at the test section outlet wen
almost the same as those of water at large Re, bu
were entirely different from those of water at smal
Re. The difference between their results and ours a
small Re comes from the fact that their particles an
extremely larger than ours. Their paper7) also predict!
that the same heat transfer characteristics as those o
water would be obtained under the conditions o:
Cs/Csf=l. This may support our result because
Cs/CSj= l is always satisfied in our experimenta
conditions. Fig. 7. Data correlation with Sieder-Tate equation for
2) Effects of particle diameter and concentratior D -1.5-cm tube.
The effects of particle diameter and concentratior
are shown in Fig. 5. The particle diameter did no
affect the rate of heat transfer in the range of 3( single-phase and liquid-solid flows due to the mixing
to 100jum. The solid concentrations, however, gav< effect of gas flow. The solid lines in the figures are the
slight changes in h which were maximum at 2( calculated results from the Sieder-Tate correlation10)
to 30wt%. written by the following equations.
Nu - Prl^ifiJfiJ-^^ lMRe^iL/D^-^
2.3 Data correlations with previously reported
equations lfc?2 < 2100
In a manner similar to the Sieder-Tate correlatior
Nu à"Prl1/3(fib/fiwy0-14=0.027Re°2 8
for single-phase flow in tubes, an approximate cor-
relation was carried out for our data in Figs. 6 and 1 Re2 > 10,000 (3)
for 27- and 15-mmtubes, respectively, using Nusseli
number, Prandtl number, Reynolds number and vis- Katsuhara and Kazama's correlation5} for gas-
cosity ratio of the bulk flow to tube interior. It h liquid flow seems to be the best of manycorrelations
evident from these figures that heat transfer coef- so far. It is represented as follows.
ficients of gas-liquid and gas-liquid-solids flows an Nu* - Pr*-°A=8.7(1 -8G)°-125ite*0-25 (4)
similar and that they are much larger than those oj
VOL 20 NO. 6 1987 571
Fig. 8. Data correlation with Katsuhara-Kazama equation
for DT= 1.5cm tube.
Fig. 9. Effect of ReG on Nuà"PrL1/3à"(/i6/juw)

Katsuhara and Kazama's correlation5} is applied to

our data in Fig. 8 for DT= 15mm. In the figure, data
points form a block around the solid line, which fits
them within UL60%.
concerning
However, systematic
are apparently
deviations
found in the figures.
Here, eG-values were estimated from the following
equation.8)
UG/UT
^G= , (5)
1.20 + 0.35/7^
2.4 Derivation of a new correlation
To obtain better correlations that can describe the
effects of tube diameter and slurry velocity on heat
transfer coefficients, the dependence of the left-hand
side of Eq. (3) was examined for gas and slurry
Reynolds numbers separately for all the experimen- Fig. 10. Effect of ReL on Nu-PrI;1/3-(fib/fiJ-0A4/Re 0.055

tal data. Figure 9 shows the dependence of Nu à"

Pr£1/3(fib/jnwy0A4 on ReG at Q=30wt% of Particle
B and at constant ReL. The slope of0.055 was obtain-
ed by the least square method. In Fig. 10, the
values of Nu à" PrL 1/3(fib/iawy0A4/Re0G055 are plotted
against ReL for three kinds of glass beads. Irrespec-
tive of tube diameter difference, a slope of 0.2 was
obtained. Consequently, the left-hand side of the
Sieder-Tate correlation10) was found to be propor-
tional to ReG055 and Re°L2. The effects of solids
concentration are shown in Fig. ll. From these ex-
aminations, a correlation for heat transfer coeffi-
cients
lows.
in up flow vertical tubes, was written as fol-
Fig. ll. Effect of Cs on
Nu à"/VZ1/3WMw)"°-14/^055M'2 Nu- Pr^1/3 ' (fib/fiwy0-1A/Re0G055 à" Re°L2.

= 10.5exp{-3.18 x l0~4(Cs-22)2} (6)

Figure 12 shows a comparison between the calcu-
lated and observed heat transfer coefficients. It can
be seen that the present correlation predicts the heat
transfer coefficients within the deviation
Furthermore, the calculated values from Eq. (6) were
572
compared with recent data of a gas-liquid-fine solid
particles system using Z)r=5.08cm by Kitahara et
al.6) in the figure, in which all their experimental data
in the slug and churn flow regimes are plotted,
of 30%. showing fairly good agreement with the calculated
values. The solid lines drawn in Figs. 3 to 5 are the
JOURNAL OF CHEMICAL ENGINEERING OF JAPAN
 Fig. 12. Comparison of observed heat transfer coefficients with calculated values from Eq. (6).

calculated results based on the present correlation.

Satisfactory agreement with the experimental data
was found except in Fig. 4, in which experimental
data seem ambiguous because of too high UL-
dependency of the three-phase flow at Q= 30wt%.
Conclusion
Heat transfer coefficients of gas-liquid-fine solid
particles three-phase up flow in vertical tubes were
measured at various operating conditions to obtain
Fig. A-l. Details of thermocouple installation for Tube A.
the following results.
1) The heat transfer coefficients of gas-liquid-fine
solid particles three-phase flow exhibit larger values heat capacity of slurry [J'kg 1 K x]
than those of gas-liquid two-phase flow in the range weight inpercent
slurry
of solid particles [wt%]
of 0-40wt% solid concentrations. The heat transfer Cs at feed [wt%]
coefficients of three-phase flow decrease above a solid volume fraction of solid particles in
concentration of 25wt% to exhibit the maximum s lu rry [-]
value of heat transfer coefficient, and becomelower Sauter average size [/mi]
than that of gas-liquid two-phase flow at the high 50% particle size [/mi]
solid concentrations. No effect of solid particle size on tube diameter [cm]
U2T/(g - DT), Froude number based on
heat transfer coefficient was detectable in the range of total fluid velocity [-]
experimental conditions. gravitational acceleration [cm/s2]
2) Monotonous and small increases of the heat heat transfer coefficient [W à" m~2 à" K~1]
tube length [m]
transfer coefficient with both gas and slurry velocities
were observed over the whole range of experimental h à" DT/XL, Nusselt number [-]
conditions. h à" DT/A*, modified Nusselt number [-]
CPGftG/)iG, Prandtl number of gas [-]
3) A new empirical
coefficient
correlationsolid of particles
for gas-liquid-fine
heat transfer
three-
CPL/iL/2L, Prandtl number of liquid or
slurry [-]
phase flow was proposed. This correlation fits all data {eGpG' PrG+Q -eG)pL- PrL}lp*,
obtained in this work within 30%. modified Prandtl number [-]
heat flux supplied to the test section [W]
Appendix DTUGpG/pG, Reynolds number based on
gas flow [-]
DTULpL/fiL, Reynolds number based on
Acknowledgment liquid or slurry flow [-]
This work was supported in part by a Grant-in-Aid by the Japan ReG + ReL [-]
Securities Scholarship Foundation. DTU*lfi*, modified Reynolds number [-]
Nomenclature
bulk fluid temperature at tube length / [K]
wall temperature at tube length / [K]
A = heat transfer area |m2] average temperature difference between bulk
PG flow and tube wall [K]
CPG = heatcapacity of gas [J-kg X K *]
VOL. 20 NO. 6 1987 573
 superficial gas velocity [cm/s] Literature Cited
superficial liquid or slurry velocity [cm/s]
UT UG+ UL, total fluid velocity [cm/s] 1) Hatate, Y., C. J. Louch and C. Y. Wen: AIChE Symp. Ser.,
U*T
No. 202, Vol. 77, ll (1981).
(UGpG + ULpL)/p*, modified total fluid
velocity [cm/s] 2) Hatate, Y., H. Nomura, T. Fujita, S. Tajiri, N. Hidaka andA.
Ikari: /. Chem. Eng. Japan, 19, 56 (1986).
UJ(l -sG), apparent linear velocity of
slurry [cm/s] 3) Hatate, Y., H. Nomura, T. Fujita, S. Tajiri and A. Ikari: /.
Chem. Eng. Japan, 19, 330 (1986).

gas holdup [-] 4) Kago, T., T. Saruwatari, M. Kashima, S. Morooka and Y.

Kato: /. Chem. Eng. Japan, 19, 125 (1986).
X
thermal conductivity [Wà" m"1 à" K"*] 5) Katsuhara, T. and T. Kazama: Nihon Kikai Gakkai
A* {sGpG^G + (l - £G)pL2L}/p*, modified thermal Ronbunshu, 24, 552 (1958).
conductivity [-]
6) Kitahara, H. and K. Yoshida, Proc. of World Congress III of
li viscosity [Pa à"s]
Chem. Eng., Vol. 2, 368 (1986).
Mb viscosity of fluid at average fluid 7) Konno, H., E. Harada, M. Toda, M. Kuriyama and S.
temperature [Pa à"s]
viscosity of fluid at the average wall
Saruta: Kagaku Kogaku Ronbunshu, 6, 308 (1980).
temperature [Pa à"s]
8) Nicklin, D. J., J. O. Wilkes and J. F. Davidson: Trans. Instn.
Chem. Engrs., 40, 61 (1962).
fi* {gG)uG+(l -eG)^L}/p*, modified viscosity [Pa-s]
9) Salamone, J. J. and M. Newman: Ind. Eng. Chem., 47, 283
P density [kg - m~3] (1955).
sgPg+(1 -£g)Pl, modified density [kgà" m~3] 10) Sieder,E. N. andG. E. Tate: Ind. Eng. Chem., 28, 1429 (1936).

THE REACTION CHARACTERISTICS OF PARALLEL

CONSECUTIVE REACTIONS IN A FLUIDIZED BED
KUNIO KATO, YUJI OKUBO AND TAKAYUKI TAKARADA
Dept. of Chem. Eng., Gunma Univ. Tenjin-cho, Kiryu 376

Key Words: Fluidized Bed Modeling, Scale Up, Fluidized Catalytic Reactor, Reactor Design, Process
Simulation

The reaction characteristics (the reactant conversion and the yield of the intermediate product) of a parallel
consecutive reaction in a fluidized bed were analyzed on the basis of the "Bubble Assemblage Model." The effects
of rate constants, particle size and bed diameter upon the reaction characteristics were investigated theoretically.
Whenthe rate constants and the size of particles were small, the reaction characteristics for a fluidized-bed reactor
closely approached those for a plug-flow reactor and scale-up of the fluidized bed reactor became easy.

Introduction reaction rate constants upon the reaction characteris-

tics have not yet been systematically investigated.
To develop an industrial fluidized-bed reactor, it is In this paper the reaction characteristics of a
very important to estimate correctly the reactant parallel consecutive reaction in a gas-solid catalytic
conversion and the yield of intermediate product from fluidized bed reactor are analyzed on the basis of the
"Bubble Assemblage Model" (B.A. model).2) The
operating conditions. To analyze the reaction per-
formance of the fluidized-bed catalytic reactor, many effects of individual reaction rate constants, size of
models4~8) have been published. The reaction per- fluidized particles, superficial gas velocity and bed
formance of small-scale fluidized bed reactors were diameter upon reactant conversion and yield of the
analyzed by these models. However, the effects of intermediate product were investigated theoretically.
fluidized particle size, gas velocity, reactor size and
1. Computational Method
Received December 26, 1986. Correspondence concerning this article should be The B.A. model has no adjustable parameter.
addressed to K. Kato. Y. Okubo is now with Shinetsu Chem. Co. Ltd, Annaka, Gunma
379-01.
Therefore, the effects of the above-mentioned factors
574 JOURNAL OF CHEMICAL ENGINEERING OF JAPAN