3140 Ind. Eng. Chem. Res.

1997, 36, 3140-3148

Operational and Structural Nonidealities in Modeling and Design of

Multitubular Catalytic Reactors
Andrzej Cybulski*
CHEMIPAN, R&D Laboratories, Polish Academy of Sciences, Kasprzaka 44/52, 01-224 Warszawa, Poland

Gerhart Eigenberger
Institut fur Chemische Verfahrenstechnik, Universitat Stuttgart, Boblinger Strasse 72,
70199 Stuttgart, Germany

Andrzej Stankiewicz
DSM Research, P.O. Box 18, 6160 MD Geleen, The Netherlands

Idealized mathematical models for multitubular packed-bed reactors, based upon simplifying
assumptions concerning symmetry, regularity, and homogeneity of the packing and the
intertubular space, are commonly used for analysis and design. In reality, substantial deviations
from these assumptions occur and give rise to maldistributions, both for the flow of reactants
through a packed tube and for the flow of a heat-transfer medium through the intertubular
space. These maldistributions and methods of how to deal with them in reactor design and
simulation are reviewed in this paper.The following areas are covered: (i) porosity and flow
patterns inside tubes, (ii) heat and mass transfer inside tubes, (iii) flow distribution over
individual tubes, and (iv) distribution of coolant flow over the intertubular space.

1. Introduction uniformities will be reviewed. The following problem

The catalytic fixed-bed reactor is the dominating
reactor type for large-scale, heterogeneously catalyzed
gas-phase reactions. In case of strongly exothermic or
endothermic reactions, the multitubular arrangement
with catalyst-filled tubes and a liquid heat-transfer
medium pumped around the tubes is the standard
design (Froment and Bischoff, 1979; Eigenberger, 1992,
1996). For analysis, scale-up and design of fixed-bed
reactors, mathematical modeling and simulation is one
of the most useful tools. The hitherto developed ideal
models describing phenomena occurring inside tubes in
multitubular reactors, as classified first by Froment
(1962, 1967, 1972, 1979), have been based upon simpli-
fying assumptions such as homogeneous and isotropic
packing of catalyst particles and plug flow of the
reaction mixture within all individual tubes of the whole
reactor. Moreover, uniform conditions of heat exchange
between the tubes and a coolant flowing through the
intertubular space are commonly assumed. In reality,
maldistributions of all kinds occur in multitubular
reactors. This gives rise to a number of problems when
the commonly accepted mathematical models are used
for design and analysis of industrial fixed-bed reactors.
A general observation is that idealized models cannot
represent the reactor behavior quantitatively, if inde-
pendently determined, intrinsic kinetics and transport
parameters are used (Hofmann, 1979a,b; Eigenberger
and Ruppel, 1986). There have been many attempts to
identify key problems and to refine and work out models
accounting for nonuniformities, while preserving Fro-
ments concept of modeling based upon intrinsic and
independently determined kinetics.
In this paper, the inference of maldistributions in
multitubular reactors and methods to deal with non-
* E-mail: acybul@ichf.edu.pl.
E-mail: eigenberger@cvtserv1.verfahrenstechnik.uni-stutt-
gart.de.
E-mail: a.i.stankiewicz@research.dsm.nl.
S0888-5885(96)00596-9 CCC: $14.00
areas are discussed: porosity and flow patterns inside
the tube, heat and mass transfer inside the tubes, flow
distribution over individual tubes, and distribution of
the coolants flow over the intertubular space.
2. Transport Phenomena inside the Tubes
The present models of catalyst-filled reactor tubes
assume a deterministic behavior based upon a regular
and axisymmetric structure of the catalyst packing. This
holds both for cell models which try to mimic the
sequence of pellets and voids and for one- or two-phase
continuous models where a continuous variation of
temperature and concentration is assumed. In reality,
a fixed bed is a random arrangement of nonuniform
pellets, and the nonuniformity is apparent on each level
of scale, from the active-site distribution in single pores
over the pore distribution in single pellets to the
arrangement of individual pellets in axial, radial, and
circumferential directions in a single tube. This has led
to the question whether deterministic models are able
at all to describe the behavior of such a system with a
sufficient degree of detail. The answer has been given
by industrial practice, which showed that a carefully
designed and operated multitubular fixed-bed reactor
of some 20 000 parallel tubes has indeed about the same
performance as a single test tube which was used for
its design. The obvious explanation is that nonunifor-
mities tend to level out even in single-catalyst tubes and
for sensitive reactions like high-conversion partial
oxidations if conversion and selectivity are considered
not pointwise but over a larger reactor volume. A
significant difference between the performance of a
single tube and that of a multitubular reactor appears
when the reaction mixture and/or the coolant are
distributed nonuniformly. The main reasons of flow
maldistributions in multitubular reactors and the means
to deal with maldistributions are discussed in sections
3.1 and 3.2 of this paper.
1997 American Chemical Society

Figure 1. Packing of particles in the core of the bed (a) and at
the wall (b).
Figure 2. Void fraction distribution for spherical particles.
Conversely, it has to be stated that point measure-
ments in catalyst-filled tubes will always show a large
degree of scattering and that only values which are
averaged over a certain volume of the tube can be
reasonably compared with the simulation results from
deterministic models. With the above restrictions in
mind, we will concentrate in the following on homoge-
neous one- or two-phase models since they seem to offer
the best compromise between computational simplicity
and the ability to incorporate additional modeling
details (see sections 2.1 and 2.2 of this paper).
2.1. Flow Maldistribution and Exothermic Re-
action. Considering the random flow-through catalyst-
filled tubes, there is one structural feature which is
apparent from all measurements. It stems from the
ordering influence of the tube wall. This is well seen
in Figure 1 where the black areas correspond to void
spaces between the particles; the volume fraction of
those spaces is obviously larger at the tube wall. This
difference is structural in character. It is superimposed
by random nonuniformities which originate from the
fact that the geometry and/or the filling procedure do
not allow for a regular arrangement of pellets so that
pellet clusters and larger voids are formed randomly.
Averaging over a certain distance, however, gives a
surprising regular and reproducible radial void distribu-
tion. The void fraction oscillates, decreasing from unity
at the wall to a damped porosity of ca. 0.4 at a distance
of 4 particles from the wall as shown in Figure 2 where
the well-known experimental data of Benenati and
Brosilov (1962) and of Schuster and Vortmeyer (1980)
are given. The broken line is an approximation of the
void fraction profile calculated from an equation derived
by Chandrasekhara and Vortmeyer (1979). The mini-
Ind. Eng. Chem. Res., Vol. 36, No. 8, 1997 3141
mum voidage (ca. 0.2-0.25) is located at a distance of
half a particle diameter from the wall. A voidage profile
with a pronounced decrease of the voidage toward the
tube center is characteristic for packings with more than
4-5 particles per tube diameter. The decrease is most
pronounced for spheres and least for Raschig rings. For
less than 3 particles per diameter, a voidage maximum
in the tube center may develop due to a kind-of spiral
arrangement of the pellets along the tube wall (Vort-
meyer, 1996).
A voidage profile with a maximum at the wall must
give rise to a maximum of the axial flow profile close to
the wall. Presumably, Schwartz and Smith (1953) were
the first who found that the radial flow pattern in
narrow tubes of catalytic reactors is nonuniform. The
velocity profile is affected by the particle shape. Figure
3 shows measurements below the packed bed for spheres
and Raschig rings for a sequence of bed repackings (Bey
and Eigenberger, 1996). For each radial position, point
measurements have been carefully averaged along the
circumference. The differences after repacking result
from the aforementioned unavoidable degree of scatter;
the solid lines give an averaged profile. It is important
to note that the maximum close to the wall which
dominates the radial nonuniformity of the flow can be
measured with the least degree of scattering. This is a
direct consequence of averaging a large number of
circumferential point measurements close to the wall.
Measurements below or above packed beds like Figure
4 give only a qualitative indication of the nonuniform
flow inside the packing since they are falsified by the
rapid reorientation of the gas flow after the bed exit.
So far, no reliable gas-flow measurements inside packed
beds could be performed. The only possibilities are
liquid-flow measurements with LDA in transparent
column packings with a carefully adjusted refractory
index of liquid and packing material (McGreavy et al.,
1986; Vortmeyer, 1996). Since these measurements are
delicate and time-consuming, published results are not
yet available to a sufficient extent. Research has
therefore been focused on a simulation of flow inside
the packing based upon the independently measured
voidage profiles and a consideration of flow reorientation
behind the packing. The pioneering work has been
performed by Vortmeyer and co-workers (Vortmeyer and
Schuster, 1983; Haidegger et al., 1989), who introduced
and used the extended Brinkmann equation (Brinkman,
1947). The Brinkmann equation consists of a momen-
tum balance based upon the two-dimensional Navier-
Stokes equation where the fluid-particle interactions
are described in a semiempirical way through an Ergun-
type pressure drop relation. Vortmeyers approach has
been adopted and somewhat modified by Daszkowski
(1991), Daszkowski and Eigenberger (1992), and Bey
and Eigenberger (1996). Figure 4 from the last men-
tioned publication shows simulated flow profiles inside
a packing of spheres (solid lines) and below the packing
(dashed lines). It can be seen that the velocity maxi-
mum of the predicted flow profile inside the packing
exceeds the mean velocity by more than a factor 2.
Similar results have been obtained for other packing
materials. A procedure has been given of how to
calculate the radially varying velocity profiles inside the
packing from voidage profiles for random packing of
spheres, cylinders, and rings.
The problems of geometry and flow in packed beds
have also been treated and reviewed by Ziokowska and
Ziokowski (1988). Readers interested in more details
are also referred to the book by Stanek (1994).
3142 Ind. Eng. Chem. Res., Vol. 36, No. 8, 1997
Figure 3. Velocity profiles measured 5 mm below a packing after repeated repackings (symbols) for an mean empty tube velocity of v0
) 0.5 m/s. The solid lines represent the model predictions (from Bey and Eigenberger (1996)).
Figure 4. Simulated flow profiles inside (solid lines) and below
the packing (circles) for spheres, dp ) 7.5 mm, at v0 ) 0.5 m/s
(from Bey and Eigenberger (1996)).
The radial variation of flow velocity has originally
been considered to be of minor importance for pure heat-
transfer applications. It was obvious early, however,
that it should have a great influence on fixed-bed
reactors with strongly exothermic reactions, cooled
through the wall. If the gas flows preferentially along
the wall, the residence time will be short where the
cooling is best, resulting in low conversion close to the
wall. Conversely, a long residence time in the poorly
cooled tube center gives rise to high conversion with
much more pronounced hot spots as compared to plug
flow. This general behavior has been found by
Choudhary et al. (1976), who introduced the concept of
a two-region model, dividing the bed into a central core
with the annular space between the core and the wall
with porosities and, hence, velocities differing in both
sections. A two-region model was also used by Borkink
and Westerterp (1992).
Lerou and Froment (1977) accounted for the distribu-
tion of the superficial velocity in calculations of a reactor
for the partial oxidation of o-xylene. It was heuristically
assumed that the velocity is inversely proportional to
voidage and the effective heat conductivity consists of
a static contribution depending upon voidage and a
dynamic contribution depending upon velocity. The
porosity profiles of Benenati and Brosilov (1962) were
used in the calculations. The wall heat-transfer coef-
ficient appeared to be higher than that for plug flow,
while the radial thermal conductivities were lower.
Peak temperatures in the cases of the radial velocity
profiles were higher than those in plug flow, and the
reactor model was more sensitive to the operating
conditions. A similar influence was predicted by Eigen-
berger and Ruppel (1986).
Delmas and Froment (1988) extended the model of
Lerou and Froment to the dependence of the effective
diffusivity on radial position. They found considerably
different reactor performances for a number of realistic
models. The differences were particularly pronounced
for small Dt/dp ratios. A comparison of the model results
based upon the Brinkmann equation with detailed
measurements was presented by Kalkhoff and Vort-
meyer (1980), Daszkowski and Eigenberger (1992), and
Vormeyer and Winter (1984). They proved the above-
mentioned differences between plug flow and radially
varying flow models and showed that the latter lead to
a considerably better agreement between experiment
and simulation. However, most of the existing correla-
tions between heat-transfer coefficients and flow condi-
tions have been derived based upon plug flow. As such,
these correlations should not be used for models ac-
counting for nonuniform radial flow. New correlations
for such models are needed.
2.2. Mass and Heat Transfer in the Bed. There
are three levels where heat and mass transfer cause
temperature and concentration gradients: the intra-
particle level, where differences in temperatures and
concentrations inside the particle exist; the interphase
level, where differences in temperatures and concentra-
tions between the bulk of the fluid and the catalyst
surface exist; and the intrareactor level, where differ-
ences in temperatures and concentrations appear be-
tween different radial and axial positions in the bulk of
the fluid or the catalyst particles.
At all three levels, inhomogeneities in mass and heat
transfer exist which are due to the inhomogeneity of
particle sizes, shapes, pore structure, and packing as
well as flow maldistribution around particles and over
the entire bed. In this paper, nonidealities at the third
level will be discussed. Generally, axial heat and mass
dispersion can be neglected if the axial aspect ratio, L/dt,
is greater than, say, 50, and this is usually the case for
industrial reactors. Radial mass transport is usually
considered to be fast enough to justify the plug-flow
assumption. Therefore, the scope of this paper is limited
only to inhomogeneities influencing heat transport over
the cross section of tubes.
Radial transport of mass and heat in catalyst-filled
tubes is primarily due to convection since fluid flow
splits before and recombines behind each pellet. For
heat transport, heat conduction through the solid pellets
and the narrow pellet interstices is added. It is gener-
ally agreed that radiation needs not be considered
separately at temperatures below 400-500 C. Obvi-
ously its contribution can be significant also at lower
temperatures if the temperature gradients are steep.
In spite of the dominating convective nature, radial heat
and mass transport have been traditionally described
by a conduction (radial heat conductivity) and diffusion
mechanism (radial diffusivity). The radial diffusivity
can be safely calculated from a superposition of molec-
ular diffusion and convective flow splitting, given by
Schlunder and Tsotsas (1988).
There has been some discussion on whether a radially
varying radial effective conductivity or the traditional
model with constant r,eff and an additional wall heat-

transfer coefficient Rw is the better representation for
radial heat transport (see Cheng and Vortmeyer, 1988;
Delmas and Froment, 1988; Foumeny and Pahlevan-
zadeh, 1990). Based upon detailed analysis, Tsotsas
and Schlunder (1990) came to the conclusion that the
r,eff, Rw model is a reasonable approximation for large
mass-flow velocities prevailing in industrial fixed-bed
reactor operation.
Correlations for the calculation of r,eff and Rw have
been proposed by numerous authors. However, in spite
of advanced techniques used, there is a significant
scatter of experimental data on heat transfer even for
physically similar systems (see, e.g., the books by
Froment and Bischoff, 1979; and Wakao and Kaguei,
1982; or a review by Stankiewicz, 1989) with no clear
indication to which of the literature correlations to
choose for reactor modeling.
A significant portion of the literature correlations on
radial heat transfer are presented as
r,eff
) C1 + C2RePr (1)
f
Nup ) C3 + C4ReC5PrC6 (2)
where f is thermal conductivity of the fluid, Re is the
Reynolds number, Pr is the Prandtl number, Nup is
Nusselt number defined as Rwdp/f, and Ci are adjusting
coefficients: C1 and C3 express static contributions to
effective conductivity and the wall heat-transfer coef-
ficient. The values of coefficients in the above equations
can be found in the books by Froment and Bischoff
(1979) and by Wakao and Kaguei (1982) or in the review
by Stankiewicz (1989). All those correlations have been
derived for plug flow. This is justified only for larger
ratios of tube-to-particles diameters (Dt/dp) (see Zi-
okowska and Ziokowski, 1988). As shown by Dasz- were found (Kim et al., 1966; Emig et al., 1972; Cybulski
kowski and Eigenberger (1992), this leads to a 20-40%
difference compared with heat-transfer coefficients es-
timated for real velocity profiles. Real velocity profiles
were considered by Legawiec and Ziokowski (1995) in
their study on heat transfer in packed beds. The
differences between heat-transfer coefficients for plug
flow and for a two-region model were also found by
Borkink and Westerterp (1992).
Besides of the neglectance of radial flow variation, a
second source for the differences in published heat-
transfer data may stem from deficiencies in the measur-
ing procedure. It was pointed out that measurements
will always contain a large degree of random scattering.
Cybulski (1971) found that angular differences in tem-
perature at the same radial position were up to about
20 C when heating air from ca. 20 to 100 C (see Figure
5). This was confirmed by Cresswell (1986), who found
a 10 C spread between angular replicates at a total
gradient of 40 C. Reprocessing the data of Cybulski
and Gowacka-Lesniak (1974) on angular temperature
differences resulted in an apparent but significant
relationship between the estimates of heat-transfer
coefficients in the pseudohomogeneous deterministic
model and the angular position of thermocouples (see
Figure 6). Ziokowski and Legawiec (1987) repeated
temperature measurements repacking the bed and
estimated heat-transfer coefficients from those profiles.
They found differences between r,effs ranging from 50
to 75%. Wijngaarden and Westerterp (1992) applied the
same procedure and found a significant scatter of
temperatures at the same angular and radial positions
after the bed was repacked. Borman and Westerterp
Ind. Eng. Chem. Res., Vol. 36, No. 8, 1997 3143
Figure 5. Temperature vs angular position of thermocouples at
various radial positions; Dt ) 54 mm, L ) 95 mm, dp (lead spheres)
) 3.1 mm, G ) 2558 kg/(m2 h) (air flow) (from Cybulski (1971)).
Figure 6. Heat-transfer coefficients for radial temperature
profiles measured at different angular positions; for configuration
and operation conditions, see Figure 5.
(1992) attributed a large scatter of their temperature
profiles to angular temperature variations.
In a number of cases, the differences between heat-
transfer coefficients in reacting and nonreacting systems
et al., 1973; Hofmann, 1979a,b; Clement and Jrgensen,
1983). On the other hand, Daszkowski (1991) and
Daszkowski and Eigenberger (1992) could show in a
number of carefully conducted experiments that good
agreement between experiments and model simulations
based upon independently determined heat-transfer
parameters and kinetics could be obtained. In their
model, they used the detailed radial flow variation both
for the reactor simulation and for the determination of
their heat-transfer parameters from independent heat-
up experiments without reaction. Similar observations
have been made by Vortmeyer and Winter (1984). This
gives rise to the hope that a better quantitative predic-
tion of packed-bed reactor operation and scale-up will
be possible if more detailed information on radially
varying velocity profiles for different catalyst shapes and
heat-transfer parameter correlations based upon these
velocity profiles become available. However, heat-
transfer coefficients in packed beds can depend, among
others, on the location and intensity of the heat source.
Therefore, especially in view of the above literature
discrepancies, it might be useful to find whether differ-
ences between heat-transfer coefficient measured under
process and nonprocess conditions are caused by the
influence of reaction on heat-transfer coefficients by
variation in packing and flow distribution. Whether,
in addition, a mixed deterministic-stochastic model for
heat transfer is necessary to take the unavoidable
randomness of packings into account remains a question
of further research. Randomness of packing leads to
randomness in flow distribution, and this, in turn,
results in local differences of heat-transfer coefficients.
3144 Ind. Eng. Chem. Res., Vol. 36, No. 8, 1997
Figure 7. Cumulative Gaussian distribution for flow rates in
individual tubes of a multitubular reactor; points represent a
number of experimental data.
Hence, a mixed deterministic-stochastic model for heat
transfer in packed beds seems to be a reasonable
solution.
3. Transport Phenomena outside the Tubes
It has been found that the yield of the desired product
in processes of partial oxidations of hydrocarbons in
single-tube reactors can differ from that in multitubular
reactors and that it can also vary in time (Cybulski and
Gowacka-Lesniak, 1974; Eigenberger and Ruppel, 1986).
Several reasons for this have been proposed: (1) the
differences in activity of various batches of the catalyst,
(2) catalyst aging, (3) nonuniform distribution of the
reaction mixture over individual tubes, and (4) nonuni-
form heat exchange between the tubes and the coolant.
The last two points will be addressed in the following.
3.1. Flow Distribution over Individual Tubes.
In multitubular reactors with random packings, the
pressure drop in the tubes usually exceeds the pressure
drop in the inlet and exit hood by orders of magnitude.
If the tubes are packed carefully and the pressure drop
is adjusted to a common value in each individual tube,
an equal flow distribution to all tubes can be safely
assumed, irrespective of the specific hood construction.
Only if very short tubes and a low pressure drop packing
(thin walled rings or monoliths) are used must both
hoods be carefully designed to avoid an unequal flow
distribution (Eigenberger and Nieken, 1991).
It has been observed in industrial operation that an
initially uniform flow distribution tends to deteriorate
with time on stream. Cybulski and Gowacka-Lesniak
(1974) measured the flow rate distribution in an indus-
trial reactor with 8540 tubes of 1-in. diameter filled with
catalyst particles ca. 5 mm in diameter. The gas was
introduced tangentially into the hood. The pressure
drop in all tubes was thoroughly equalized at the same
flow rate to a standard value before the reactor was
started up. Flow-rate measurements were repeated in
some tubes after the reactor had been shut down. The
distribution turned out to be close to the Gaussian one
(see Figure 7) with considerable deviations at the low-
flow-rate range (the lowest flow rates were observed
near the reactor shell). The deviations can be caused
by either inadequacy of the normal distribution model
to fit experimental data and/or greater weight of ex-
perimental points at the higher flow-rate range where
each point represents more measurements than these
for the low-flow-rate region. Similarly, significant
deviations of the pressure drop which developed during
the reactor operation were reported by Eigenberger and
Ruppel (1986). The highest pressure drop was observed
near the reactor centerline, just opposite to the central
hood inlet pipe. An explanation which was substanti-
Figure 8. Relative yield of maleic anhydride vs normalized flow
rate; V-Mo catalyst KMD-32; benzene-to-air ratio of 1:66.5; (b)
coolant of 415 C; (O) coolant of 425 C (from Cybulski and
Gowacka-Lesniak (1974)).
Figure 9. Coolant cross-flow (A) and coolant parallel-flow design
(B) for multitubular fixed-bed reactors with molten salt cooling
(from Eigenberger (1992)).
ated by visual inspection was a nonuniform deposition
of dust particles on the top layer of the catalyst. Such
a deposition will be, of course, strongly dependent upon
the flow conditions in the inlet hood, where a tangential
inflow favors deposition at the peripheral and at central
inflow a deposition below the feed pipe. Hence, care
must be taken in industrial fixed-bed reactors to com-
pletely remove any dust particles or droplets from the
feed preparation stage before the gas enters the reactor.
A nonuniform flow rate through individual tubes of
a multitubular reactor can easily result in low yields
and an increased danger of temperature runaway if a
temperature-sensitive reaction is considered. Particu-
larly sensitive are tubes with a reduced throughput
because of their higher conversion and reduced heat
removal. This has been shown clearly by Westerterp
and Ptasinski (1984). On the other hand, if flow is too
high, conversion decreases because residence time is too
short. This is illustrated in Figure 8, where data on
the partial oxidation of benzene to maleic anhydride
(Cybulski and Gowacka-Lesniak, 1974) are presented.
An apparent plateu in Figure 8 is likely to be caused
by commensurability of experimental errors with rather
low yield sensitivity to flow rate near the maximum
yield area. Obviously for lower flow rates, yield de-
creases, but no replicated data from that region were
available. A 10% increase of the flow rate resulted in a
yield drop by 3-5%. Thus, both factors contribute to
lowering the yield of the desired product.
3.2. Distribution of Coolant Flow in the Inter-
tubular Space. Generally there are two main classes
of multitubular reactors as far as design of the inter-
tubular space is concerned: the parallel-flow and cross-
flow units (Figure 9). In the reactors of the first
category (Figure 9B), the coolant flows in parallel to

Figure 10. Distribution of shell-side heat-transfer coefficients in
a leakage-proof exchanger of rectangular cross section (11.7 6
in.), containing 144 tubes of 1/2-in. diameter on 3/4-in. triangular
pitch (form Stachiewicz and Short (1963)).
tubes in the region where the reaction occurs. Hence,
active catalyst is restricted to the space between the
upper distribution and the lower collection plate; the
rest of the tubes may be filled with inert material. The
coolant is pumped through the reactor by a strong
circulation pump which nowadays is usually placed
outside the reactor for better service. Part of the coolant
is led through a steam generator to remove the heat of
reaction, and the coolant temperature is adjusted via
this side stream. For properly designed distributing and
collecting plates, the flow is uniform over the cross
section of the reactor. Heat transfer due to the forced
convection at flow parallel to the tubes is rather poor
for typical heat exchangers. Accordingly, the parallel-
flow reactors are considered to be demanding for the
higher flow rates of the coolant to ensure a sufficiently
high rate of heat removal. In the cross-flow design
(Figure 9A), baffles are installed to force the coolant to
flow mainly perpendicularly to the tubes. This flow
pattern is expected to enhance heat exchange between
the tubes and the coolant. Baffled reactors contain
segmental baffles or disk-and-doughnut baffles, the
latter being the most commonly used in industrial
practice. Obviously, dead zones for the coolant can be
formed where the coolant motion changes from parallel
to perpendicular.
Dead zones are particularily pronounced in the center
and at the peripheral ifscontrary to Figure 9Asthe
central part and the peripheral part where the coolant
flow changes direction are also equipped with tubes. In
these local dead zones, the coolant heat transfer can
be much worse than in the parallel-flow reactors. We
(A.C. and A.S.) witnessed the occurrence of such zones
when an industrial reactor of the Rheinstahl-Von
Heyden-Deggendorfer type containing ca. 10 000 tubes
was dismantled for repair. The areas of the tubes near
the potential dead zones located at the region of
expected hot spots were reddish violet, indicating over-
heating of the tubes from inside. Sintering of the
catalyst particles in those tubes might result in an
increase of pressure drop and, consequently, a decrease
of flow rate. This can be a further explanation for the
development of nonuniform flow through individual
tubes of the bundle during time on stream. These
observations of the dismantled reactor tubes are in
agreement with results of Stachiewicz and Short (1963).
The distribution of local shell-side heat-transfer coef-
ficients in a cross-flow heat exchanger as found by
Stachiewicz and Short is shown in Figure 10. Measure-
ments were carried out with the aid of a specially
Ind. Eng. Chem. Res., Vol. 36, No. 8, 1997 3145
developed heat-transfer probe consisting of a closely
wound fine wire coil of the same diameter as that of
the heat-exchanger tubes. Local heat-transfer coef-
ficients were determined by accurately positioning the
short-length coil in the test section in place of a tube.
Care was taken that no leakage between the tubes and
the holes in the buffle plates occurred. Nevertheless,
considerable differences up to 400% have been observed.
To determine the distribution of the coolant flow, the
coefficients of hydraulic resistance in all elementary
geometrical configurations are needed. These configu-
rations include the tube bundle (for both parallel flow
and cross-flow), baffle windows, gaps between tube
bundle and the shell, and finally the baffle-shell and
tube-baffle clearances. These hydraulic resistances
have been reviewed by Stankiewicz (1989). A model
consisting of continuity and momentum balance equa-
tions containing these resistances gives the flow distri-
bution over the intertubular space. The model for flow
in the intertubular space was experimentally verified
(Adamska-Rutkowska et al., 1983a,b, 1984; Stankiewicz
et al., 1986; Cybulski et al., 1987) using an apparatus
consisting of two chambers with cross-flow and one
chamber with parallel flow, containing 28 rows of tubes.
The agreement between the calculated overall pressure
drop values and the experimental ones was sufficient
for the design purposes. Heat-transfer coefficients are
evaluated by summing up contributions for both parallel
flow and cross-flow. The correlations for these heat-
transfer coeffficients have also been extensively dis-
cussed in the review paper by Stankiewicz (1989). The
required heat-transfer conditions hrequired can be ob-
tained from the model of a single tube. If hcalculated,min
< hrequired, the overall flow rate of the coolant must be
increased and/or the design of the intertubular space
must be modified.
As mentioned above, the prime objective of modeling
of the intertubular space is to properly arrange the
geometrical configuration of this space and to determine
the minimal coolant flow rates which will guarantee a
sufficiently high heat transfer. Literature data on heat-
transfer coefficients in bundles of tubes are commonly
used in such procedures. However, literature correla-
tions do not take the occurrence of a heat source of high
intensity (region near the temperature peak) into ac-
count. Under such conditions, turbulent natural con-
vection can contribute considerably to the overall heat-
transfer coefficient. This has been observed by Cybulski
et al. (1986, 1987). Coolant flow rates in a single-tube
reactor were measured by using radioactive tracers.
Heat removal in processes of partial oxidation of ben-
zene and o-xylene appeared to be high enough at coolant
velocities as low as ca. 2 cm/s, i.e., deep in laminar
regime. The yields of the desired products maleic and
phthalic anhydrides were as high as those for the higher
coolant flow rates, indicating that a heat-transfer mech-
anism other than forced convection was prevailing.
Further work on coolant heat transfer under high heat
flux conditions seems necessary to better understand
and predict turbulent natural convection in multitubu-
lar reactors.
The first models combining the tube- and the shell-
side phenomena in a multitubular reactor were devel-
oped for publication at the University of Leeds (Adder-
ley, 1973; Dunbobbin, 1976; McGreavy and Dunbobbin,
1976; Biscaia, 1980). In those early models, ideal
coolant cross-flow with constant velocity through the
tube bundle in a reactor of rectangular cross section had
been assumed. Thus, the shell-side effects in those
models were limited to the continuous increase in the
3146 Ind. Eng. Chem. Res., Vol. 36, No. 8, 1997
Figure 11. Two-dimensional cell model of the baffled shell side
in a multitubular reactor (from Stankiewicz (1989)).
Figure 12. Axial temperature profiles in catalytic tubes at several
locations in intertubular space.
coolant temperature during its flow through the inter-
tubular space. A detailed calculation of heat transfer
in the outer tubular space is contained in Eigenberger
and Ruppel (1986). It is restricted, however, to the heat
transfer from a hot flue gas to the tube bundle for an
endothermic dehydrogenation reaction.
Figure 13. Response of the reactor with disk-and-doughnut baffles (a) and of the parallel flow reactor (b) to a step increase in reactant
concentration. Temperature profiles in the tubes positioned at the reactor axis.
The first attemps to include the coolant maldistribu-
tion phenomena into the multitubular reactor model,
originating also from Leeds, were made by Stankiewicz
(1985, 1989) and consisted in dividing the intertubular
space into a number of two-dimensional cells, in which
both cross and parallel components of the local coolant
flow were considered, as it is shown in Figure 11.
Knowing the relations for hydraulic resistances in all
individual elements of the intertubular space (tube
bundle, tube-to-baffle clearances, baffle windows, etc.),
it was possible to estimate the local parallel- and cross-
flow components of the coolant velocity in each shell-
side cell. Combination of the coolant heat balance in
each cell with the balances on the tube side allowed for
determination of the tube-side profiles as a function of
the tube position in the bundle. Stankiewicz found that
the parallel leakage flows of the coolant through the
tube-to-baffle clearances may lead to substantial dif-
ferences in the temperature profiles in individual tubes.
An example of such differences is presented in Figure
12, in which j indices are the column numbers in the
two-dimensional cell matrix, as shown in Figure 11,
with j ) 1 and j ) 4 denoting the column adjacent to
the coolant inlet and the column next to the reactor axis,
respectively. The results shown in Figure 12 concern
a multitubular unit for benzene oxidation to maleic
anhydride, 4.652 m in diameter containing 12 144 tubes
and fitted with five disk-and-doughnut baffles. In the
same paper, Stankiewicz proposed five characteristic
factors for multitubular fixed-bed reactors. The factors
describe the uniformity of the tube bundle operation,
thermal uniformity of tube and shell sides, and power
consumption necessary for pumping the coolant through
the intertubular space.
Attention has also been given to the stability of
multitubular reactor operation. Modeling studies (Dun-
bobbin, 1976; Stankiewicz, 1985; Stankiewicz and Leszcz-
ynski, 1986) indicated that the cocurrent coolant-flow
configuration presents a safer option than the counter-
current one, which, under certain conditions (e.g.,
coolant pump failure), is likely to move the reaction into
the multiple steady-state region with accompanying
thermal runaway in the catalyst beds. This phenom-
enon is due to the heat feed-back loop in countercurrent
systems and can also occur locally in a part of the tube
bundle being caused by maldistribution of the coolant
flow (existence of stagnant zones).

A group from the Industrial Chemistry Research
Institute, Warsaw, used subsequently the above-de-
scribed two-dimensional cell approach to investigate the
operational characteristics of the so-called mixed-flow
co/countercurrent reactors (Stankiewicz et al., 1986) and
the regions of steady-state multiplicity in large-scale
industrial reactors for maleic anhydride production
(Adamska-Rutkowska et al., 1988, 1990). Modeling
strategies similar to that proposed by Stankiewicz have
also been used by other authors, either to study the
general characteristics of multitubular units (Baptista
and Castro, 1993) or to investigate the influence of the
configuration on the reactor controller design (Maciel
Filho and McGreavy, 1993).
Another, this time dynamic, model of a multitubular
catalytic reactor was proposed by Stankiewicz and
Eigenberger (1991). The main assumption and a novel
feature of this model was a porous body approach,
which implied that the entire intertubular space was
regarded as a pseudohomogeneous continuum. The
steady-state momentum and the unsteady-state heat
and mass balances were written both for the tube and
the shell sides in form of a system of mixed partial
differential and algebraic equations and then discretized
and solved using a semiimplicit Eulers method. Stank-
iewicz and Eigenberger used the model to simulate the
dynamic behavior of a reactor with parallel coolant flow
as compared to a cross-flow unit with disk-and-dough-
nut baffles. The latter design appeared to be far less
sensitive to diverse disturbances, both on the reactants
as well as on the coolant side. Differences were most
pronounced in the tubes positioned near the reactor
axis. A typical example of the observed differences is
presented in Figure 13, in which the response of the
tube-side temperature profiles to a step increase in the
reactant concentration is shown for both designs con-
sidered.
4. Concluding Remarks and Recommendations
In modeling of multitubular reactors for fast and
highly exothermic reactions, the first steps should be
the selection of the most appropriate ideal model as
classified by Froment (1979). Parametric sensitivity of
this model should then be studied. If the model appears
to be sensitive to flow rate, mass and heat-transfer
coefficients maldistributions in these areas should be
specifically included in the model.
Considering the radial flow distribution in packed
tubes, there is still a lack of reliable models and model
parameters for different packings and operating condi-
tions. Since radial heat evolution and wall heat transfer
are strongly affected by the radial flow profile, radial
heat transfer in packed-bed reactors can only be put on
a sound basis if the heat-transfer parameters are
determined in connection with the respective flow
conditions.
A second source of maldistribution in packed tubes
originates from the essentially random character of a
catalyst packing. Point measurements in packed beds
will therefore always exhibit a large scatter and a weak
reproducability. Larger differences therefore have to be
accepted if such point measurements are compared with
simulation results from conventional models. These
models assume an averaging (e.g., around the priphery
of a tube radius or a cross section of a reactor). A better
agreement can therefore only be expected if the model
results are compared with measurements which are also
averaged in a similar way. It is so far not clear whether,
Ind. Eng. Chem. Res., Vol. 36, No. 8, 1997 3147
in addition, the development of stochastic reactor mod-
els is necessary to cope with the unavoidable random-
ness.
For the design and operation of multitubular fixed-
bed reactors of industrial dimensions, special care must
be taken to ensure sufficient and equal coolant condi-
tions on the shell side and equal throughput through
all individual tubes. This task, which presented sub-
stantial problems in the past, has been alleviated to
some extent, on the one hand, through the availability
of a great number of reliable heat-transfer data for the
design of the shell side in shell-and-tube heat exchang-
ers (here, the data of, e.g., VDI, ASME, or HTRI can be
recommended for engineering calculations) and, on the
other hand, through the development of sufficiently
flexible and powerful computational fluid dynamics
programs in recent years.
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Received for review September 30, 1996
Revised manuscript received February 23, 1997
Accepted March 8, 1997X
IE960596S
X Abstract published in Advance ACS Abstracts, June 15,
1997.