C&mica/ Engineetin.g Science. Vol. 47. No. 13fL4. pp. 3501-3508, 1992. om9-2509/x ss.m+o.

oo
Printed in Great Britain. 0 1992 Pergunon Press LAd

DEVELOPMENT OF TRICKLE-BED HEAT TRANSFER CORRELAlTON

FOR FLOW MEASUREMENT PROBE

DAVID H. ANDERSON, FREDERICK J. KRAMBECK,

and AJIT V. SAPRE

Mobll Research and Development Corporation

Paulsboro Research Laboratory
Paulsboro. New Jersey 08066

ABSTRACT

The heat transfer coefficient from a heated pipe In a trickle-bed catalytic reactor was
correlated with combined gas and liquid flow rates along with fluid and packing physical
properties. The correlation ls readily applicable for flow rate measurements in commercial-
scale trickle-bed reactors. Data for the correlation were obtained using petroleum distillate
liquid fed to a laboratory reactor over a range of temperatures along with hydrogen and
nitrogen as gases. Our analysis showed that the heat transfer coefficient data are represented
based on the combined thermal mass flux of the fluids plus the effective conductlvtty of the
packed bed. The latter depends on gas, liquid. and solid thermal conductivitles, but not
significantly on flow rates or flow regime.

KEYWORDS

Trickle-bed; flow measurement; heat transfer coefficient; effective conductivity

INTRODUCTION

Trickle-bed reactors involve cocurrent flow of gas and liquid through a packed bed of catalyst
particles. These reactors are widely used in the petroleum industry in processes such as
hydrodesulfurizatlon. Reactor efficiency is greatly reduced under conditions of nonuniform
flow across the bed. It is of interest, therefore, to measure and control the extent of flow
nonuniformity in a commercial reactor. A heated thermocouple probe was developed In our
laboratory to measure flow distribution In a trickle-bed reactor based on the correlation of the
probe heat transfer coefficient with gas and liquid fluxes. This paper discusses development of
this correlation based on laboratory data.

me nature of this two-phase flow heat transfer in a packed bed is not well defined. Existing
resutts are generally correlations of data of air/water systems (e.g., Specchla et. (1979). or
Weekrnan and Myers (196511. We developed a correlation of data In the form of a theoretical
expression derived for heat transfer from an infinite cylinder to ideal fluid flaw perpendicular to
its axis. This correlation successfully accounts for data of hydroprocessing reactors with Hz/oil
and N,/oil two-phase flow and H, and N, single-phase flow with a single set of parameters. lt
was subsequently applied to commercial data with only extrapolation to the larger probe
diameter and higher range of vapor and liquid fluxes CSapre -.’ et al 1990).

EXPERIMENTAL

Experiments were conducted in a 0.10 m <ID) pilot unit. Figure 1 shows the test probe consisted
of a 0.05 m long (0.04 m heated length) cartridge heater (0.01 m ID) placed dlrectty In a bed
of 0.0016 m hydrotreating catalyst extrudates <deactivated). A thermocouple was soldered

3501
3502 DAVID H. ANDERSON et al. c3

into a groove at the midpoint of the heater and the probe was placed at the center of the
reactor normal to the fluid flow direction. The recessed thermocoupb is designed to measure
the heater surface temperature when heat is applied. Fluids used Included a petroteum
distillate feedstock for a hydroprocessing reactor along with either H, or N, gaseous feeds at
5.27 MPa pressure. Temperatures ranged from 300 K to 644 K to vary the gas to liquid ratio.

- Packed - Bad

Thermocouple

Fig. 1. Pilot plant experimental set-up

For a fixed-gas and liquid flow rate, an experiment consisted of making two temperature
measurements: one, with the heater off, gives the ambient reactor temperature; the second,
with the heater switched on and allowed to reach thermal equilibrium. gives an indication of
the skin temperature of the heater. The heat transfer coefficient is the heat transfer rate
divided by 1) the temperature rise measured upon heating the probe, and 2) the heat transfer
area determined by the probe diameter and heated length.

The heat transfer coefficient is dependent upon gas and liquid mass fluxes. along with physical
properties of fluids. Vapor and liquid fluxes and physical properties were determined after
accounting for any vaporization of the liquid feed. Figure 2 compares the pilot unit gas and
liquid fluxes with the range used commercially. We could not match the commercial range of
fluxes due to the pump and compressor limitations on the pilot unit.

Uqtdd FIIJX.kWw.mJS

Fig. 2. Trickle bed reactor operating regime

c3 Development of trickle-bed heat transfer correlation 3503

HEAT TRANSFER CORRELATIONS

Literature correlations of Iwo-phase flow heat transfer in packed beds have been summarized
by Herskowttz and Smith (1983). These involve bed effective radial conductivtty and wall heat
transfer coefficients in terms of catalyst, gas, and liquid thermal conductivity values. and the
contributions of hydrodynamics. None of these correlations is directly applicable to the
present situation because of the different geometry of the probe in the path of the flow. Two
different possible models were considered. The first relates heat transfer coefficient as a
function of local gas and liquid mass fluxes with heat convected by the liquid film. The second
relates heat transfer CO8ffki8nt t0 total <gas and liquid) thermal flUX based on the 8ff8CtiV8
conductivity of the packed bed. The second approach was found to be more suitable, as
explained in the following sections.

Liquid Film Method

The first approach is a Nusselt number correlation form for heat transfer to the probe based on
the wall heat transfer correlation of Specchia et. (1979. 1980). Neglecting heat transfer at
zero fluid flow rate,

h - d
P b
i Nu = a. Re (1)
I.4
kL

where the particle diameter is taken as the characteristic length. Parameters a and b are
determined from the data. All fluid physical properties in the dimensionless groups are of liquid
which is considered to flow as a film over the probe surface and carry the heat transfened.
The characteristic liquid film velocity. uf. Is related to the superficial velocity, us, by

B is the liquid saturation of the bed voldage, l . 6 depends on liquid and gas fluxes; i.e.,
increasing with increasing liquid flux and decreasing with increasing gas flux. At constant liquld
flux <or uJ. decreasing 0 by increasing the gas flux would increase the heat transfer coefficient.
h. Larkins et. (1961) correlated liquid saturation based on the ratio of liquid to gas phase
friction losses computed using the single phase flow Ergun equation. Friction loss for phase i is
calculated by:

= (1.75 Gi + 150(1-•)L( /d )Gi(l-c)/c3d p g

% i P PiC

G, ls the mass flux of phase I. Defining

x I (6pg) l’*

the liquid saturation was fii to the following form

2
log 0 = --c + d log x -e (log x) ; O.O5<x<30 (5)

where c. d, and e were parameters in their fit. These were left as free parameters along with a
and b in equation Cl) in fitting our data.

The correlation was fit to the Hz-oil data with the parameters a = 1.3: b = 0.39; c = 1.33: d = 1 .Ol:
e = 0.21. A simulation by Chang , et. (1983) of heat transfer in single-phase flow past a
cylinder l8d to the following correlation which is similar to equation (1).
3504 DAVID H. ANDERSON et al. c3

Nu - 0.88 Ftmz,,* Paz’-= (6)

SP

The cylinder diameter was the characteristic length in this expression. as there was no packing.
Larkins et., found Cc. d. e> = (0.774.0.525.0.109) in their ftt of liquid saturation. and our set of
parameters (c, d, e) gives the same qualitative dependence on liquid and gas fluxes. The fit of
our data is shown in Fig. 3.

‘zoo0

1500

loo0

500
0

01
500 loo0 : DO
-wed Heat Transfer Coeflicient. bV.iiK

Fig. 3. Liquid film heat transfer correlation

Equation (1) has reasonable validity as tt represents observed trends in heat transfer
coefllclent, and corresponds with the single phase flow correlation (6) assuming B-al with onfv
liquid flowing. However, the correlation breaks down for single phase gas flow C&>o), which
would occur in regions with no liquid flux either by severe maldisttibution or complete
vaporization at high temperature: Also, Fig. 3 shows this correlation does not adequately
predict the effects of varying gas phase conductivity when substituting N, for H,.

Effective Conductivity Method

An altematfve heat transfer correlation which includes thermal propettles from all three phases
derives from the solution of pseudcrhomogeneous conduction and convection about a
cylinder in a stream flowing perpendicular to the axis. This method was illustrated by Drew
C1931). At steady state with constant fluid properties, the equation describing the bed
temperature, T, is

al afr a*tc a*T

(71
cp~(By K + ay -1
ay
= k_‘-
a=*
+ -)
au*

The bulk fluid flow is pamllel to the y-axis outside the region around the cylinder (probe). me x-
axis is perpendicular to the axis of the cylinder and the y-axis. The system supposes an infinite
cylinder length. F, and F are the combined gas and liquid mass fluxes in the x and y
directions. respectively: 8pt is the heat capacity of this combined stream. and k, is the three-
phase effective bed conductivity. Upstream from the probe, the solution should reduce to the
free-stream temperature; i.e., that measured by the probe without heat input, T,. The probe is
assumed Isothermal and the fluid in contact with the probe is at the probe temperature. TP.

On approximating the fluid flow as krotational. the system can be tmnsformed to flat plate
geometry with the direction of fluid flow paralleE to the heat transfer surface. Conduction is
c3 Development of trickle-bed heat transfer correlation 3505

neglected In the main flow direction. The solution under these conditions comes from
Boussinesq < 1903). and when transformed back to cylindrical probe geometry Is:

= 1.016 (k-/C
l/2 (8)
WC PT-r - p - DP)
PT

This expression was used to determine the effective bed conductivity which produces the
measured heat transfer coefficient at the given combined thermal mass flux, CPTF,

= G-C + L-C (9)

=pT* PQ PL

The effective bed conductivity has been found to be a sum of static and dynamic
contributions by Specchia et. (1979).

ke = (Q, + (k-ID
I
Q + (kJD
I
L (10)

The first term is basically a volume average of the conductivities of the solid, liquid, and
gaseous phases. We assume the catalyst pores are liquid-filled in the two-phase flow runs and
neglect the interparticle liquid holdup contribution to bed conductivity. Complete liquid
saturation is assumed in cases of single-phase liquid flow, however. Convective mixing of the
fluids in the direction normal to the bulk flow is included in the dynamic terms.

Static conductivity, (k& The static conductivity was correlated by Specchia et. (1979) in
the following form where’ k, is the interparticle (gas phase) conductivity.

(kJ,, = kg cc + (l-c)/49 + 7
k
P

Q,was a function of voidage, which wos constant for our runs. 7=2/3 was expected based on
geometry and was observed in their data.

The effective particle conductivity, kP, is a function of solid and liquid phase values under our
assumption. Several proposed expressions for k, have been evaluated by Lin and Ford (1984).
with the recommended form being based on Maxwell’s derivation (1954) for particles with
internal porosity. 8.

k
P kL
- = (1 - (l-f -_) e) / (1 + (f-1) 8) (12)
k
1 kd

and
f = 3 kS/(2kS + kL) (13)

Dynamic conductivity, <k&_ Dynamic conductivity was correlated by Specchia m, (1979)

by linear variation with thermal mass flux of each phase, i.e.,

(ke), 9 = A - Cps - G - dp (14=)

,

(kelp L = B - CpL - L - dp (1-1

I
 3506 DAVID H. ANDERSON et al. 0
with constant coefficients A and B. d is the particle diameter. Gas phase dependence in this
form has been observed for air in botR single-phase and two-phase flows by 5pecchia mar.
Liquid phase dynamic conduction has also been observed to depend on gas velocity through
the impact on holdup, which would introduce some additional complexity as well as
correlating parameters. Since our experimental data shows the dynamic contribution is small,
the form in equations (14) was used.

Figure 4 is a log-log plot of the heat transfer coefficient vs. average thermal mass flux, Cpt F. in
the pilot unit test runs. C + was assumed to include heat effects of vaporization. and itwas
calculated for each run & y the slope of the total fluid specific enthalpy vs. temperature.

Fig. 4. Experimental data Fig. 5. Correlation without

dynamic terms

The least-squares ftt of the data is neariy h = QFI 112, which is itself a reasonable correlation
and follows equution (8) assuming constant k, for ail runs. k, values which are relatively
insensitive to variation in fluid conductivity by either temperature or composition changes is
accounted for by a large contribution of the solid-phase conductivity, &. Our data were
represented by a constant value of b as a correi~ion parameter.

Constant parameters to be determined were &, aiong with # in equation (11). and A. B in
equations (14). 8 was taken as 0.6 and c was fixed at 0.4. For the dynamic contributions in
equations (14). CPL was assumed to be 3.14 J/gm/K. With HS-oil systems, C,, was set to 6.28.
With N2-oil. it was taken as 3.14.

The best fit of the data was obtained with the following parameter values based on minimizing
the difference between k, by equation < 10) and k, which satisfies equation (8) based on the
measured heat transfer coefficient.

q, = 0.0138 A = 0.033

k, = 7.75 W/m/s/K B=O

The small values of A and B indicate that the data are basically represented by the static
conductivity only. Negligible dynamic contributions of (k&n were aiso found with pure NP or
H,. We then determined the M of the entire data without accounting for the dynamic terms.
The results are shown in Fig. 5. There 9 = 0.0094 and k, = 7.69 W/m/s/K. Aithough these
parameters are dtfferent now, indicating some dynamical contribution, no significant
deterioration in the precision of the correlation occurred.

The data were taken only over a low range of gas fluxes relative to commercial trickle-bed
reactor conditions. Retaining the gas phase dynamic term would result in significant
extrapolation of dependence on gas fiux for a commercial application. in our use. we
neglected the dynamic contribution. and do not need to know the gas to liquid ratio to
c3 Development of trickle-bed heat transfer correlation 3507

determine thermal ftux from the measured heat transfer Co8ffici8nt. As shown in the next
section, this form of correlation was validated in high flux testing.

APPLICATION

Thiseffective conductivtty correlation was used along with equation (8) in a commercial
trickle-bed reactor application (Sapre et.. 1990). Much higher fluid fluxes were involved. so
there was some concern about the impact of the dynamic terms to effective conductivity.
And flow regime transition on increasing fluxes (i.e., trickling to pulsing flow) was found to
increase radial heat transfer rotes by Weekman and Myers (19651. But we neglected these
effects initially, and applied equation (81 to the commercial data in a high temperature Hroil
system. Probe diameter was about 0.025 m. Neglect of the dynamic terms to effective
conductivity allows calculation of combined thermal mass flux, CP+F, without needing to know
the gas/liquid ratio. Figure 6 shows the comparison between thermal mass flux mR values
determined with this probe correlation and the average values calculated from total gas and
liquid flow rates in the reactor. The correspondence is good. with no indication of significant
bias attributable to dynamic effective conductivity or change in flow regime.

0
_.-...“‘O
r
f”” -
0 Commerdal Probe Data
Ptbt Unit Com3latton 8 .. . .”
0
,_/ ._- .. 0

,,,.
e 2omo- 0 __....~~$I.-.
0 0 _...’ 0

,./
0

Fig. 6. Commercial reactor/pilot plant comparison

CONCLUSIONS

Heat transfer data from a heater probe in the laboratory pilot experiments are
correlated based on three-phase static bed conductivity. The correlation represents
packed bed heat transfer to flowing H, and N,. and flowing two-phase mixtures of these
gases with petroleum distillates at reaction temperatures.

Based on this heat transfer correlation. the calculated thermal mass fluxes from a heater
probe agreed well with observations in a commercial reactor at significantly higher gas
and liquid fluxes than in the laboratory experiments.

Our data suggestthat the contribution of dynamic terms for the gas and liquid phase is
negligible to the effective bed conductivity even at high gas and liquid fluxes in Mckle-
bed reactors.

Flow regime transition has no apporent impact on the heat transfer rate.

ACKNOWLEDGEMEM

We are grateful for the support and assistance of Mobil Research and Development
Corporation and the Paulsboro Research Laboratory in this work.
3508 DAVID H. ANDEIUON et al. c3

SYMBOLS

A.B,a.b,c.d,e constant parameters in heat transfer conelations

c,&a&, specific heat capacities: gas,Iiquid.mixture
dP particle diameter
DP probe diameter
f group defined by equation 13
F.F,.Fy mass flux of mbcture and its components in x and y directions
gravity conversion factor
ZG, gas mass flux, mass flux of phase i
h heat transfer coefficient, q/rD&t
k,.k,.k, gas, liquid, and solid phase conductivities
kp particle conductivity
k&k&+k& effective bed conductivity, static and dynamic contributions
I probe heated length
L liquid mass flux
Nu Nusseit number, hd,/k,
PrL Prandtl number, CpLYL/kL
heat transfer rate per probe length
Z8 Reynolds’ number, Ldp/pLcB
ReL Reynolds’ number for single phase flow. Ldp/pL
T,Tr bed temperature
TP probe temperature
AT Tp-To
WJS liquid interstitial and superficial velocities

pressure gradients: gas, liquid. two-phase flow

bed interparticle voidage
term defined by equation 4
terms in equation 11
intraparticie porosity
density of phase I
viscosity of phase i

REFERENCES

Boussinesq (1903). Theorie Anaiytique de la Chaieur, II, Gauthier-Villars, Paris.

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Methodologies in Heat Transfer, Ed. by T. M. Shlh, Hemisphere Pub. Corp., Washington, 349.
Drew, T. B. (193 1). ‘Mathematical Attacks on Forced Convection Problems: A Review: AiChE
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Herskowifz, M., and J. M. Smith (1983). “Trickle Bed Reactors: A R8Vi8W’. AlChE J.. 29.1.
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Flow Maidistribution in Large Scale Trickle Bed Reactors,” Chem. Ena. Sci.. 3.2263.
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Gas-Liquid Flow in Packed Beds,’ AlChE J., 11, 13.
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Alcoa R. E. Searies Labs, E. St. Louis, iii., 17.