3720 Ind. Eng. Chem. Res.

2008, 47, 3720-3751

REVIEWS

Structured Packings for Multiphase Catalytic Reactors

Kalyani Pangarkar,*,†,§ Tilman J. Schildhauer,‡ J. Ruud van Ommen,§ John Nijenhuis,§
Freek Kapteijn,*,† and Jacob A. Moulijn†
Catalysis Engineering, Delft UniVersity of Technology, Julianalaan 136, 2628 BL, Delft, The Netherlands,
Laboratory for Energy and Materials Cycles, Paul Scherrer Institut, 5232 Villigen PSI, Switzerland, and
Product and Process Engineering, Delft UniVersity of Technology, Julianalaan 136, 2628 BL, Delft, The
Netherlands

Reactor design for multiphase catalytic fixed bed reactors is always based on conflicting objectives. In the
past, catalyst discovery and development preceded and motivated the selection of an appropriate multiphase
reactor type. This type of sequential approach is increasingly been replaced by a parallel approach to catalyst
and reactor selection. In nearly all respects, structured catalysts and reactors have the ability to outperform
randomly packed reactors. Structured packings, apart from their advantages of high voidage and low-pressure
drop, have the benefit of ease of scale-up and accurate description of the fluid mechanics. In this review we
have evaluated the potential of using structured internals for multiphase catalytic reactions, which are currently
carried out in randomly packed fixed bed reactors. Characteristics of various structured internals such as
monoliths, corrugated sheet or gauze packings, knitted wire packings and foams are discussed in detail. Since
designing a structured device for gas-liquid-solid contacting requires a sound knowledge of hydrodynamics
and transport phenomena, a concise review of the above-mentioned structured packings and their characteristics
based on hydrodynamics and transport phenomena is presented. Existing models (empirical, phenomenological
and mechanistic) are outlined with respect to flow regime transition, pressure drop, liquid hold-up, gas-
liquid interfacial area, gas to liquid mass transfer, liquid to solid mass transfer, residence time distribution
(RTD), and heat transfer. The models are critically evaluated, and their limitations are discussed. An overview
is given about what information is available, what needs to be evaluated and what kind of existing methodology
can be applied in order to arrive at quantitative models for the physical parameters. Last, the structured
internals are compared with each other and with randomly packed bed reactors, allowing a rational selection
of the preferred packing for a given application.

1. Current Multiphase Reactors problems associated with catalyst separation. The major disad-
Multiphase reactors are found in diverse applications such vantage of the stirred tank and slurry bubble column reactors
as in manufacture of petroleum-based fuels and products, in is the required separation of product and catalyst, necessitating
production of commodity and specialty chemicals, pharmaceu- a filtration step of the fine catalyst particles from the liquid
ticals, herbicides and pesticides, in production of materials and product. Moreover, when applied in the continuous mode, back
in pollution abatement.1 A key motivation for implementing mixing lowers the conversion and usually the selectivity. A
multiphase reactor technology has largely been driven by the packed bed reactor, such as the trickle bed reactor, is much more
discovery and development of new or improved catalysts for convenient but large particles (>1 mm) have to be used to limit
either emerging or existing processes.2 Typical reaction types the pressure drop. A summary of the most important processes
that are encountered in multiphase processes of the chemical carried out in trickle-bed reactors is given in Al-Dahhan et al.3
industry are summarized in Dudukovic et al.2 A wealth of Trickle bed reactors are typically applied for processes involving
products are produced in multiphase catalytic reactions. Among slow reactions because of their advantage of high catalyst
the multiphase reaction systems, the stirred tank slurry reactor, loading and longer residence time and its narrower distribution.
slurry bubble column and the trickle bed reactor are being used Because of the low and tortuous porosity of the packed bed,
most extensively. The pros and cons of the various reactor types liquid flow rates are limited to low values in order to avoid the
are summarized in Table 1. development of pockets of stagnant liquid, which can lead to
It is evident from the information given in the table that an an undesired high-pressure drop and eventually flooding, when
optimum has still not been reached with respect to reliable in countercurrent operation. Flooding occurs at high gas and
reactor performance. Every type has its pros and cons. While high liquid flow rates and is characterized by accumulation of
bubble columns and stirred tank reactors have the advantage of liquid across the bed cross-section disabling further operation.
small catalyst particles, trickle bed reactors do not have any Therefore, due to the limitations imposed on the flow rates,
packed beds show incomplete catalyst wetting and poor mass
* To whom correspondnece should be addressed. Fax: transfer rates and are nearly always used in the co-current mode.
+31-15-2785006. E-mail addresses: [email protected],
In view of the rapid improvements in the area of catalysis,
[email protected].
†
Catalysis Engineering, Delft University of Technology. leading to highly active catalyst particles, severe intraparticle
‡
Laboratory for Energy and Materials Cycles, Paul Scherrer Institut. diffusion and heat transport limitations can be foreseen in these
§ reactors. Thus, difficulties with heat removal may lead to hot
Product and Process Engineering, Delft University of Technology.

10.1021/ie800067r CCC: $40.75 © 2008 American Chemical Society

Published on Web 05/01/2008
 Ind. Eng. Chem. Res., Vol. 47, No. 10, 2008 3721

Table 1. Qualitative Comparison of Existing Multiphase Catalytic Reactorsa

aspects considered
stirred tank slurry reactor slurry bubble column trickle bed reactor
reactor type mixed plug flow/ mixed dispersed plug flow
catalyst separation difficult difficult simple
replacement simple simple difficult
manufacture established established established
loading low-moderate low-moderate high-low
pure catalyst-egg shell catalyst
utilization high high low-moderate
mass transfer internal good good bad-good
liquid-solid good good fair
particles in suspension particles in suspension particles stationary
small particles small particles larger particles
gas-liquid moderate moderate fair
larger bubble size larger bubble size sufficient gas-liquid interaction
RTD gas and liquid backmixing backmixing axially dispersed plug flow
for both gas and liquid for liquid and small bubbles for both gas and liquid
heat transport to outside very good very good low-moderate
scale-up hydrodynamics difficult difficult medium
high pressure costly fair fair
a Data taken from ref 4.

spots resulting in catalyst deactivation. The heat removal of the structured internal, then the stability and resistance of
problem is also one of the main causes for lower selectivity the coating to adverse conditions such as high pressure and
toward the desired product in many processes. It is self-evident temperature need to be considered.
that these limitations are unfavorable from the point of view of Adequate knowledge of the hydrodynamics and transport
process economics. This motivates a systematic research for parameters is a key to designing an efficient structured catalytic
alternative reactor types that will overcome as much as possible reactor. For a good design, the hydrodynamics and transport
the limitations in the existing reactors. processes need to be described in satisfactory way.4 A catalytic
reactor can never perform better than the catalyst and, as a
2. Structured Internals for Multiphase Catalytic Reactors consequence, catalyst preparation methodology should be further
Process intensification draws a lot of attention and it has developed for various structured internals made of different
become clear that multifunctional and structured reactors will materials required for specific applications. Thus, research is
play a key role in the near future.5 A structured reactor contains needed to provide the enabling tools fully exploiting the high
a structured internal which can be made out of ceramics, metals potential of structured reactors.
or carbon, situated inside a reactor. It can be considered as an
intensified form of a randomly packed bed reactor. A monolith 3. Goal and Structure of the Review
is an example of a structured reactor; in fact, the borderline The goal of this review is to provide concise information on
between catalyst and reactor vanishes for this application.6 the hydrodynamics and transport phenomena based on existing
The advantage of a structured reactor is that it may be data in different structured packings applicable for multiphase
designed in full detail up to the local surroundings of the catalyst, catalytic reactors. This information is then used to bring out a
allowing ultimate precision.7 The exact shape and size of all table for a user-friendly rational selection of randomly packed
column internals is determined by design rather than chance.7 bed and structured multiphase catalytic reactors.
Moreover, these structured reactors show flexibility with respect The next two sections discuss the currently envisaged types
to different length scales, i.e., diffusion lengths, voidage etc. of structured packings with a focus upon the hydrodynamic and
They effectively allow the decoupling of intrinsic reaction transport parameters.
kinetics, transport phenomena and hydrodynamics.8 This de- The sections 6.1-6.5 focus in more detail on monoliths,
coupling is extremely valuable because it allows independent corrugated open crossflow packings, corrugated closed crossflow
optimization for all these three aspects, each of which has a packings, knitted packings, and foams. The correlations for
significant influence on the behavior of a catalytic reactor, giving hydrodynamic and transport parameters resulting from these
rise to a reliable and excellent reactor performance.8 The best studies are discussed critically.
example where decoupling between hydrodynamics and reaction The last two sections sum up what information is available,
rates is needed is the requirement of small particles for high what needs to be evaluated and what kind of existing methodol-
catalyst effectiveness whereas hydrodynamics is demanding a ogy can be applied in order to arrive at quantitative models for
low-pressure drop, and as a consequence, the particles should the physical parameters. A concise matrix of relevant process
be large. These two are the classical conflicting demands in a parameters with ranking for the individual packings is presented.
packed bed. In such cases structured internals can play a very
important role and allow solutions that were previously impos- 4. Structured Internals for Reaction and Separation
sible. Structured internals such as monoliths can be coated with Since the 1960s structured packings have been applied
catalysts, supports or their precursors.5 Due to the short diffusion successfully in industrial distillation and absorption columns.9
distances obtained by coating, the catalytically active material It is estimated that already 25% of all refinery towers worldwide
can be utilized more efficiently. are fitted with structured packings.10 The main type of structured
Usually structured internals do have disadvantages, the major packing used in the process industry is the corrugated plate type
ones being low catalyst loading, when the catalyst is present as packing. They are mainly used to create sufficient gas-liquid
a coating, and high costs. To achieve comparable catalyst contact area, which is essential for a good separation. A typical
loadings with that of a randomly packed bed, either a high example is the application of corrugated wire gauze packings
geometric area of the structured internal or an integral structured to purify oleochemicals such as glycerol, fatty acids, and fatty
catalyst is a prerequisite. If the catalyst is coated on the surface alcohols and wax esters in vacuum distillation.11 As these
3722 Ind. Eng. Chem. Res., Vol. 47, No. 10, 2008

Figure 1. Different types of structured packings (from left to right): (a) Katamax developed by Koch Engineering; (b) catalyst bales developed by CDTech;
and (c) Katapak for laboratory-scale tests.52

products are extremely heat sensitive, they have to be distilled

at low temperatures and therefore vacuum conditions are
preferred. The corrugated wire gauze packings are extremely
efficient for these applications, as they do not have to operate
under a high-pressure drop. The inherent capillary action of the
wire gauzes is sufficient to facilitate the liquid spreading on
the packing. On the one hand, for trickle bed reactors the use
of structured packings is yet hardly commercialized and is still
limited to lab scale research. On the other hand, structured
packings are in increasing demand for reactive distillation
applications where reaction and separation is carried out in one
single process.
A number of reactive distillation packing concepts have been
developed to fulfill the required criteria, few examples “catalyst
bales” developed by CDTech (Catalytic Distillation Technolo-
gies), Katapak-S developed by Sulzer ChemTech and Katamax
developed by Koch Engineering. Sketches of the packings are
presented in Figure 1.
A commercial process illustrating the use of corrugated
structured packings is the hydrolysis of methyl acetate using
Katapak-SP packing. Sulzer ChemTech has developed this
process together with Wacker-Chemie and the first plant is in
operation at Wacker’s site in Burghausen, Germany, since
2000.12 In this process, methyl acetate and excess water are fed
to a prereactor, where the hydrolysis reaction takes place almost
to chemical equilibrium. The reactor outlet product is fed to
the reactive distillation column, where reaction conversion is Figure 2. Flow sheet of the reactive distillation process for methyl acetate
hydrolysis.13
increased up to 97%. By continuously removing the products
from the reactive section, a shift of the chemical equilibrium
of the hydrolysis reaction can be achieved leading to an increase
in overall conversion. A simplified process flow scheme of this
process is presented in Figure 2.
Other structured catalysts frequently encountered are ceramic
monolithic catalysts.6 They have found many applications in
combustion and environmental uses, e.g., as afterburners of
engine exhausts and for removal of harmful compounds from
industrial off-gases. The first important commercial applications
of monolithic catalysts were for decolorization of nitric acid
tail gas and for car exhaust emission control. The main reasons
for focusing research on monoliths was their low-pressure drop,
low sensitivity to plugging and high mechanical strength.13 By
Figure 3. Number of publications with the word “monolith” or “honey-
1975, the first cars equipped with catalytic converters became comb” in the title. The patent category includes patent applications (data
available. Monoliths are available made from different materials, obtained from www.ISIKnowledge.com).
and an interesting application of metal monoliths is for
controlling heat removal in packed beds due to their superior Comprehensive reviews on catalytic combustion, including the
heat transfer characteristics compared to those of ceramic use of monoliths for automotive converters, have been published
monoliths.14 Thus, metal monoliths can be applied when a in the past few decades.15-17 Reviews on monoliths including
thorough control of the temperature in tubular reactors is needed. nonenvironmental and noncombustion applications of monoliths
 Ind. Eng. Chem. Res., Vol. 47, No. 10, 2008 3723

Figure 4. Cordierite monoliths: (a) square, rounded corners, hexagonal channels; (b) open crossflow structure; (c) closed crossflow structure; (d) knitted
wire packing; (e) aluminum foam.

have also been published.6,18 The increasing interest in mono- the packing to the outside of the reactor.25 They are not (yet)
lithic catalysts is reflected in the literature. The number of commercially manufactured.
publications on monoliths and/or honeycomb structures (see (3) Knitted wire packing is the next category, which consists
Figure 3) is rising almost exponentially. It is striking that the of knitted multiple fine metallic filaments that are then crimped
fraction of patents is over two thirds. Lately, cellular metallic and spirally wound. Typical characteristics are low-pressure
foams have seen increased application as an excellent thermal drop, high porosity, and high geometric surface areas. Radial
management material. An example of such applications is the mixing properties and heat transfer performance of these
use of metal foams as compact heat sinks for cooling of packings are unexplored as yet.26
microelectronic devices such as computer chips or power (4) Open-celled foams yield the final category, which are 3D
electronics.19 A unique graphitized foam developed at the Oak cellular materials made of interconnected solid struts (pores),
Ridge National Laboratory (ORNL) promises more efficient and forming a sponge type tortuous path network. Typical charac-
compact heat exchangers.20 The foam combines a high heat teristics are low- and high-pressure drop, high porosity, high
conductivity, porosity and geometric surface area due to which geometric surface areas, and good heat transfer characteris-
the overall heat transfer coefficients of foam-based heat tics.27,28
exchangers can be up to 2 orders of magnitude greater than Figure 4 gives typical examples.
conventional heat exchangers.20 As a whole, these packings provide additional degrees of
Apart from these there are number of structured packings that freedom with respect to pressure drop, porosity, catalyst hold-
have proven to be successful at laboratory scale from either up etc. An appropriate example is the variation of catalyst hold-
mass transfer or heat transfer point of view but yet have to be up without having an equivalent effect on the pressure drop.
commercialized. Details of these packings can be found in Wen Depending on the application, the catalyst hold-up in a structured
et al.21 and Kolodziej et al.22 packing can be simply varied over a broad range by manipulat-
ing the coating thickness. Filling the channels of the packing
In this review, we will discuss a number of commercially
with catalyst particles is an alternative solution for increasing
available structured packings as potential structures that can be
the catalyst hold-up.4,29 Thus, structured catalysts offer greater
applied for multiphase catalytic reactions. They can be classified
flexibility with respect to catalyst hold-up compared to a packed
in the following categories.
bed.
(1) Monoliths are the first category, which are structures of
parallel straight channels, with typical characteristics of low- 5. Transport Phenomena in Random and Structured
pressure drop, high porosity, high geometric surface areas.6 Fixed Bed Reactors: Hydrodynamics, Mass Transfer and
Monoliths can be ceramic (cordierite) or metal based (copper, Heat Transport.
aluminum, etc.). The heat transfer characteristics of ceramic
Extensive reviews of hydrodynamics and transport parameters
based monoliths are poor compared to metal based monoliths,
in trickle bed reactors have been published.1-3,30-32 The most
due to their low heat conductivity.
important parameters such as flow regime, pressure drop, liquid
(2) Corrugated sheet/gauze packings are the second category, hold-up, gas to liquid mass transfer coefficient and gas-liquid
which can be subdivided into the following two categories: interfacial area and heat transport from the packed bed to the
(2a) The open cross flow structure (OCFS), which consists heat transfer fluid are outlined in this section. It will be clear
of corrugated sheets stacked parallel to each other, and whose that not only catalyst development but also hydrodynamics and
corrugation orientation is alternately inclined to the axis. Typical mass and heat transfer studies are of prime importance for a
characteristics are low pressure drop, high porosity, high proper evaluation of the various reactor types and for creation
geometric surface areas, and efficient radial mixing.23 These of an optimal reactor performance.4
packings are manufactured as metal sheet or metal wire gauze 5.1. Flow Regimes. Under the conditions employed in
packings both available commercially. Examples of metal sheet industrial co-current trickle-bed reactors, two types of flow
packings are Katapak-MK or Mellapak and that of wire gauze regimes can be encountered: the low interaction and the high
packings is Sulzer BX, all manufactured by Sulzer.24 interaction regime.33 The low interaction regime consists of
(2b) The closed cross flow structure (CCFS) contains an trickle or film flow and the high interaction regime consists of
additional flat plate between the corrugated sheets, forming spray, pulse and bubble flow.34 The majority of the co-current
closed channels inclined to the axis. Typical characteristics are fixed bed operations are carried out in the trickle flow regime.
low-pressure drop, high porosity, high geometric surface areas In analogy to randomly packed bed reactors, two distinct flow
and mixing at the wall, thus allowing efficient heat transfer from regimes can be observed in structures with closed channels (e.g.,
3724 Ind. Eng. Chem. Res., Vol. 47, No. 10, 2008

monoliths and closed crossflow packings): film flow and slug of the liquid film over the whole geometric area of the packing
or Taylor flow. Film flow is characterized by films covering is a key factor in improving the gas-liquid interfacial area for
the channel walls with only low interaction between gas and mass transfer. Although turbulence is not relevant in Taylor flow
liquid.35 Taylor flow consists of gas bubbles and liquid slugs operated monoliths, at increasing flow rates the gas to liquid
flowing consecutively through the small monolith channels. The mass transfer rate increases. This is because, though Taylor flow
gas bubbles occupy the whole cross section of the channel and occurs under laminar flow conditions, the recirculation patterns
are elongated. Only a thin liquid film separates the gas bubble in the liquid slugs enhances transfer of gas from the caps of the
from the catalyst.36 Such a flow pattern is associated with high bubbles to the liquid slug.
gas to liquid mass transfer rates as will be evident in the Very high values of gas-liquid mass transfer rates are
subsequent sections. A gas to liquid ratio between one and three achieved in Taylor flow operated monoliths.
typically leads to stable Taylor flow with liquid superficial 5.4. Liquid)Solid Mass Transfer. The rate of mass transfer
velocities ranging from 0.05 to 0.15 m/s and channel diameters of the reactants and products from liquid to catalyst particle
of less than 2 mm.37 surface is very important and needs to be accounted for in
Since a coated structure will have a much lower catalyst evaluating trickle bed reactor performance.39 Liquid hold-up and
loading (∼20%) compared to a randomly packed bed (∼60%), pressure drop affect the interstitial gas and liquid velocities
it is extremely important to aim for high geometric surface areas which have a direct influence on the mass transfer coefficients
for the coated structures. For this, the channel dimensions of and catalyst wetting efficiency.39 External catalyst wetting
the structure should be in the order of mm. This is sufficient to efficiency is an important design and scale-up parameter in
facilitate the Taylor flow pattern provided the gas and liquid determining the degree of catalyst utilization in trickle bed
velocities are in the right ranges. Because of the high mass reactors.3 Generally speaking, pressure and gas velocity have a
transfer rates associated with Taylor flow, it is the most preferred positive effect on the catalyst wetting efficiency. This is because
regime of operation for fast reactions that are mass transfer the liquid film thickness at a fixed liquid mass velocity decreases
limited. Since Taylor flow requires high liquid velocities, with pressure and gas velocity. This results in an improved
structured packings having low-pressure drop can be easily spreading of the liquid film over the external packing area.3
operated in this flow regime. The same cannot be said for monoliths operated in the Taylor
Thus, the flow regimes most likely to occur in monolith and flow regime. In Taylor flow, which is a surface tension
closed channel packings are film flow (at low liquid velocities dominated flow regime, high gas velocity leads to increased
and intermediate gas velocities) and Taylor flow (at high liquid film thickness and as a consequence decreases the liquid-solid
velocities and intermediate gas velocities). For corrugated mass transfer.
packings, foams and multifilament wire mesh packing, trickle 5.5. Residence Time Distribution (RTD). In real flow
flow (at low liquid velocities and intermediate gas velocities) systems the flow pattern is intermediate to the two extremes of
and pulse flow regimes (at high liquid velocities and high gas plug flow and back mixed (CSTR) behavior.40 This deviation
velocities) can be found. from ideal flow conditions can be attributed to channelling and
5.2. Pressure Drop and Liquid Holdup. The estimation of dead zones. Therefore, the usual assumption of plug flow in
liquid hold-up is of great interest as it has a strong influence packed columns may not be correct in all instances.41 In Taylor
on pressure drop, catalyst wetting, and heat transfer. Pressure flow, the dispersion is low because the gas bubbles seal the
drop is important in determining the energy losses, sizing of liquid slugs. The only dispersion mechanism is the exchange
the compression equipment etc. At a given gas density, the two- with the stationary film. However, on the scale of the reactor
phase pressure drop increases with gas and liquid mass fluxes, the differences in residence time distributions between the
liquid hold-up and liquid viscosity. Liquid hold-up increases channels have to be taken into account. Very important is the
with liquid superficial velocity and liquid viscosity and decreases inlet design.
with increasing gas density and gas superficial velocity. Back mixing commonly termed as “axial mixing” is detri-
Two basic approaches to describe the hydrodynamics of a mental to the performance of multiphase reactors in the case of
packed bed reactor are the channel model and the particle positive order reactions, especially at high conversions, or for
model.38 In the channel model, the gas is assumed to flow inside consecutive reaction schemes where selectivity is the main
numerous small channels having a characteristic dimension; as issue.42 This is because axial mixing reduces the driving force
liquid flows down the “walls” of the same channels it reduces for mass transfer, heat transfer and reaction and usually
the available cross-sectional area for gas flow, thus causing additional height needs to be allowed for to achieve a given
increased pressure drop. In the particle model the gas is assumed transfer rate in physical processes, e.g., distillation or conversion
to flow around a packing particle having a characteristic in chemical processes.41 It is well-known that the liquid-phase
dimension and the liquid acts to increase this dimension by its flow pattern in a packed column does not deviate significantly
adherence to the particle surface. The presence of the liquid from plug flow, and therefore the dispersed plug flow model
also reduces the void fraction of the bed. has been widely used to describe it.40
5.3. Gas)Liquid Mass Transfer and Interfacial Area. RTD is a powerful tool to analyze the axial mixing and
Gas-liquid mass transfer resistance can have a detrimental hydrodynamic behavior of the fluids in the reactor.43,44 The
effect on the reactor performance. Therefore, accurate estimation variance of RTD of the reactor indicates the deviation from ideal
of the mass transfer parameters is important for achieving plug flow.43 It is a strong function of the flow patterns prevalent
successful reactor design and scale-up. In principle, for a given in a certain reactor type.
pressure, temperature and gas-liquid system, the mass transfer Generally a narrow residence time distribution is desired.
coefficient kL is generally a function of the diffusivity of the 5.6. Heat Transport. Reactions, which are characterized by
gas in the liquid and renewal rates of the liquid phase. As a a large heat evolution and selectivity problems, are often carried
consequence, it is largely dependent on the level of turbulence out in wall-cooled packed bed reactors. The heat of reaction is
occurring in the reactor and hence the type of reactor. For a removed from the reactor by a cooling agent, e.g., evaporating
given gas density, the gas-liquid interfacial area increases with steam. The complex heat transfer phenomena in packed beds
liquid mass flux and velocity. In film flow, improved spreading with co-current gas-liquid flow have been extensively analyzed
 Ind. Eng. Chem. Res., Vol. 47, No. 10, 2008 3725

Figure 5. (A) Internally finned monoliths (a and b, Corning, Inc., New York; c, ECN, Petten). (B) Copper-based monolith with square channels.14

Table 2. Typical Geometric Properties and Hydrodynamic Regime of Monoliths

cell density (cpsi) 25 50 100 25 200 400 600
GL flow type film film film film Taylor Taylor Taylor
channel shape square square square square finned square square square
void fraction (%) 67 68 69 73 74 75 79
surface-to-volume ratio (m2/m3) 654 939 1312 1040 1900 2800 3500
hydraulic diameter (mm) 4.12 2.91 2.1 2.8 1.56 1.08 0.9

in the literature and several models have been developed in order patterns in both cases are similar for, e.g., liquid flowing down
to describe heat transfer in the bed. the wall as a film and gas flowing through the central core of
The most widely used model is the 2-D pseudo homogeneous the channel. Moreover, a major application of structured
plug flow model in which two main assumptions are made: catalysts is in catalytic distillation, where counter-current flow
(1) At any location of the reactor, all three phases (gas, liquid, is dominant.
solid) are at the same temperature. Furthermore, heat transfer and pressure drop correlations for
(2) Plug flow conditions exist for the gas and liquid phases. gas phase only are also included for foams, static mixers and
The model contains two parameters: the effective bed radial metal monoliths where two-phase data are not available. The
conductivity, λe,r which determines the amount of heat that can single-phase models can be used as starting point for modeling
be transferred from the bed to the vicinity of the tube wall and pressure drop and heat transfer rates for multiphase applications.
the wall heat transfer coefficient, Rw, which allows taking into
account a poorer heat transfer close to the wall. On the one 6. Structured Internals
hand λe,r for structured packings is typically larger than that for
randomly packed beds. This is due to the significant contribution 6.1. Monoliths: Ceramic and Metal. Monoliths are ceramic
of the radial convection component in addition to the improved or metallic blocks containing parallel, straight channels. The
static conductivity which depends mainly on the geometry of open structure without bends hardly obstructs flow, yielding a
the matrix and the conductive properties of the material, e.g., low-pressure drop. The size of the channels is usually small,
copper monolith, aluminum foam, etc. On the other hand, Rw and is characterized by the cell density in cells per square inch
is expected to be smaller in the case of structured packings, (cpsi).6 On the walls of the channel a thin layer of catalytically
due to a defined gap present between the skin of the packing active material can be deposited. In this way, a high external
and the tube wall. The gap constitutes the main thermal contact surface area and a short diffusional distance are obtained.4 The
resistance for the heat transfer from the packing to the coolant. material of construction includes various ceramics as well as
Various approaches used in literature to describe the flow metals. Ceramic monoliths have been used extensively in gas-
patterns, pressure drop, liquid hold-up and transport rates in solid applications such as the automotive exhaust converter and
the structures mentioned above are critically discussed in the deNOx reactors.6 Monoliths are being increasingly considered
subsequent sections. as an interesting alternative for gas-liquid-solid applications.4
Though multiphase reactors are usually operated in the gas- The only current large scale gas-liquid-solid commercial
liquid down-flow mode, data obtained for the structured application of monoliths is the hydrogenation of anthraquinone
packings in counter-current mode is included in this review. in hydrogen peroxide production.45 Reviews on hydrodynamics
Counter-current operation is relevant in order to bring out and transport phenomena in multiphase monolith reactors have
similarities between co-current and counter-current flow modes been published.46,47
in the low-interaction regime. A good example to demonstrate Ceramic monoliths are commercially available in different
this are the phenomenological correlations developed for channel shapes and sizes, the most common being square,
structured packings tested in a counter-current flow mode which hexagonal, and triangular (see Figure 5A). Extruded metal
can be applied to co-current flow mode provided the flow monoliths made out of copper are developed by Corning
3726 Ind. Eng. Chem. Res., Vol. 47, No. 10, 2008

Incorporated to promote radial heat transfer mainly by conduc- The pressure drop model for film flow monoliths proposed
tion (see Figure 5B). Internally finned monoliths, invented at by Lebens et al.54 is based on a phenomenological approach,
TUDelft, with larger channel diameters have been designed originally used for randomly packed beds (see Table 3). The
mainly for countercurrent operations.48 The internal fins create approach is based on the pressure loss in a dry bed of particles
separate paths for the gas and the liquid and also contribute to and how it is affected by the presence of the liquid. An important
the catalyst hold-up. Typical geometric properties of the various feature of this work is that it takes into account the effect of
monoliths are given in Table 2. liquid hold-up on pressure drop and vice versa. The model
Different techniques of applying catalyst support material and predicted the data within (20%, thus proving that such models
active catalyst on a monolith body are discussed in literature.49-51 based on physical phenomena can describe the irrigated pressure
Table 3 lists the experimental details of the studies on drop in monoliths rather well. Figure 8 is a plot for the irrigated
hydrodynamics; mass transfer and heat transfer in monoliths pressure drop in which the experimentally obtained wet pressure
along with the respective correlations reported. drop is compared with the phenomenological model for a square
For the monolith reactor a good liquid distribution at the finned channel. The constants in the correlation depend on the
entrance is crucial because in the reactor radial transport is not channel geometries.
possible due to the absence of flow exchange between the Kreutzer et al.55 developed a semiempirical model for pressure
channels. Once a good distribution is ensured all the monolith drop of Taylor flow in monoliths based on quantifiable features
channels can be utilized for mass transfer and reaction. of the flow pattern, so that experimental pressure drop data can
Therefore, the selection and design of the appropriate distributor be used to characterize the flow pattern (see Table 3). The model
and its positioning is a major challenge. Correctly positioned was verified by determining the slug length experimentally and
spray nozzles have been proven to provide distributions far better comparing it with the value obtained from the pressure drop
than the conventional distributors used for trickle beds.35 model at a given liquid hold-up (see Figure 9). The agreement
Stacking of monoliths can improve mass transfer performance of the slug length obtained from pressure drop and the slug
in processes which are limited by intraparticle diffusion or when
length obtained from conductivity measurements is very good.
viscous or foaming liquids are present due to the radial remixing
As seen in Figure 10, for long slugs (L f 1) the value of fRe
of the laminar layers.52
approaches the limit value for infinitely long slugs (16 for square
Flow regime transition measurements were done in a monolith geometry and 14.2 for circular geometry) and the method loses
with 1.5 mm square channels using a conductivity probe its sensitivity.56
measurement method.53 Figure 6 shows a flow map, which
represents the flow transition from film flow to slug flow. The kLae values measured by various authors in monoliths are
correlation developed from these flow transitions is given in given in Table 4.
Table 3. Since the flow transitions have been determined for a Lebens et al.57 and Heibel et al.58 carried out measurements
specific system, i.e., a monolith with 1.5 mm square channels, in the film flow regime to determine the effect of monolith
aqueous liquid, it is uncertain whether this correlation can be length on kLae. The results of Lebens et al.57 show that the mass
extended to other systems For example, a monolith with circular transfer is significantly higher in the first part (0-0.25 m) of
channels will show flow transition at other gas and liquid the monolith than in the other two sections. The development
velocities than square channels due to lower cross-sectional area of both velocity and concentration profile leads to a strong
and due to the fact that in square channels the gas-liquid enhancement of the mass transfer at the inlet. The end effects
interaction is lower as liquid retracts in the corners of the need to be deduced for the determination of kLae of the
channel. Similarly, the flow transition will take place at lower considered monolith section as they are not measured in the
gas and liquid velocities when fluids of higher viscosity are developed flow regime. Thus, the kLae values of the section
used. 0.25-0.5 m should be considered for further analysis and
Liquid hold-up measurements are reported for monoliths comparison. Heibel et al.58 performed measurements in the film
operating in the film flow regime. An empirical correlation flow regime in both co-current and countercurrent mode and
derived from the classical Nusselt theory for smooth laminar showed that the mode of operation, i.e., co- or countercurrent
falling films along a vertical surface was proposed by Heibel film flow, has no influence on the mass transfer rates. This
et al.35 for the dynamic liquid hold-up in film flow monolith corroborates the conclusion that the film reactor operates in a
(see Table 3). This correlation is in good agreement with the low-interaction regime.
previously reported correlation of Lebens et al.48 (see Table 3)
Heiszwolf et al.36 measured kLae in slug flow regime and
for internally finned film flow monoliths. The correlation
compared the data with the kLae values obtained from the
predicts a strong dependence of βL on the hydraulic diameter
correlation of Bercic and Pintar59 using different values of the
of the monolith channels. Thus, the higher the geometric surface
area, the higher would be the liquid hold-up. This is logical, as slug length. The data were well correlated at high liquid
higher surface areas would lead to higher coverage of the velocities (uL > 0.1 m/s, see Figure 11). The observation that
channel wall, and eventually lead to higher hold-up. It is the correlation was not satisfactory at low flow rates can be
worthwhile to note the applicability of this correlation to low due to the fact that at a too low liquid velocity no slug flow
surface tension liquids and liquids with higher viscosities.35 can be established in the channels because of hydrodynamic
Figure 7 shows a plot of the liquid hold-up as a function of instabilities.60 So, it is understandable that the model, derived
Reynolds and Froude number for two different channel diam- for the slug flow regime, fails to describe the mass transfer
eters and two different systems. The effect of gas flow rate on process at low liquid velocities. The model of Bercic and Pintar59
the liquid hold-up is limited. Therefore, the correlation takes may be applied to obtain kLae in the slug flow regime provided
into account the effects of the liquid phase and gas-phase effects that the liquid slug length is known. It is striking that kLae values
can be neglected. In general, the correlation can be applied to obtained are in the range 0.4-1 s-1, remarkably high if
predict liquid hold-up in any monolith geometry for any kind compared to the values obtained in trickle bed reactors (∼0.1
of liquid. s-1).
Table 3. Correlations for Hydrodynamic and Transport Parameters for Monoliths
reference correlations method geometric properties operating conditions comments
Heibel and Lebens53 flow transition: slug flow to film flow measuring the conductivity using 150 mm long co-current down flow
1.5-mm square channels µL ) 0.5-6 m/s validated using aqueous
platinum
uG,trans ) -3.5 + 5.0(uL,trans × 100)0.3 systems, can be extended
microprobes,
to other systems
aqueous NaCl, and air 42-mm-diameter cordierite µG ) 0.5-6 m/s
Lebens et al.57 gas-liquid interfacial area in film flow modeling 1 m long valid for µL up to 2-D Poisson-type PDEs
ae ) 2673 xβL ∨ βL < 0.147 4.62-mm square channels with fins 0.055 m/s for water which define the
43-mm-diameter cordierite velocity profile
ae ) 1112 - 704 βL ∨ 0.147 < βL < 0.25
ae is based on the volume of the void space
al.35

( )
Heibel et liquid holdup in film flow magnetic resonance imaging, 0.5 m long co-current down flow effect of surface tension
FrL2 0.46 water, 10% and 25% 2.91- and 4.11-mm square channels µL ) 0.01-0.04 m/s and viscosity studied
βL ) 6.6 aqueous sucrose solution 42-mm-diameter cordierite µG ) 2.7 m/s βL ∝ 1/dh2
ReL

Lebens et al.48 liquid holdup in film flow weighing technique: static and 1 m long µL ) 0.005-0.06 m/s,
ReL
( ) dynamic hold-up, water, 4.62-mm square channels with fins no gas flow
0.46
βL ) 6.95 ∨ βL < 0.25 n-decane, and 20% 43-mm-diameter cordierite
GaL
aqueous sucrose solution
Lebens54 pressure drop in film flow differential pressure transmitter, 1 m long countercurrent
water and air 4.62 mm square channels with fins µL ) 0.005-0.06 m/s
dp
φ (1 - βL) ) 1 -
2 n
B2xReL 2
φ )
-
dz irrigated ( ) 43-mm-diameter cordierite µG ) 0.2-2 m/s

FrG dp
-
dz dry ( )
B2 ) 0.081, n ) 2 for circular tube
B2 ) 0.045, n ) 0.87 for circular finned tube
B2 ) 0.049, n ) 1.5 for square finned tube
Kreutzer et al.55 pressure drop in Taylor flow 300 mm long co-current down flow
µL ) 0.02-0.2 m/s

[ ]
1.5-mm square channels
(∆p/L - FLgL)d 2
0.17d Re 1/3
µG ) 0.02-0.3 m/s
fRe ) ) 16 1 + ( ) 100-mm-diameter cordierite

Ind. Eng. Chem. Res., Vol. 47, No. 10, 2008 3727
2µL(uL + uG)L Lslug Ca measuring the conductivity using
platinum microprobes,
(for circular channels) aqueous NaCl, and air

[ 0.17d Re
]
1/3
) 14.2 1 + ( )
Lslug Ca
(for square channels)

Lebens et al.57 gas-liquid mass transfer in film flow desorption of oxygen from 1 m long countercurrent semitheoretical correlation
δ2uL saturated water into nitrogen 4.62-mm square channels with fins µL ) 0.005-0.03 m/s
Shave ) 1.04 + 0.35(1/Gz)-0.63Gz ) 43-mm-diameter cordierite monolith µG ) 0.2-1 m/s
ZDL
Bercic and Pintar59 gas-liquid mass transfer in Taylor flow physical absorption of methane 1.12 m long glass capillary with 1.5, co-current down flow empirical correlation,
in water 2.5, and 3.1 mm i.d. 0.6 m long µL ) 0.01-0.4 m/s no dependence found
0.133µTP1.2
kLae ) glass capillary µG ) 0.01-0.4 m/s on channel dimensions
Lslug0.57

Irandoust et al.61 gas-liquid mass transfer in Taylor flow absorption of oxygen from air with 1.5 and 2.2 mm i.d. co-current up flow theoretical correlation,
kLae ) 4[δ(dc - δ)uave,filmym + DLShLdb]/[dc2(Lslug + Lbubble)] into water, ethanol, µL ) 0.092-0.56 m/s validated with
and ethylene glycol µG ) 0.01-0.4 m/s experimental results
kLdb
ShL )
DL
 3728
Ind. Eng. Chem. Res., Vol. 47, No. 10, 2008
Table 3. (Continued)
reference correlations method geometric properties operating conditions comments

Bercic and Pintar59 liquid-solid mass transfer in Taylor flow dissolution of benzoic acid into 25-35 cm long coated tubes µL ) 0.01-0.4 m/s L-S mass transfer increases

( ) ( )
0.44 Lslug -0.09 water, measuring dissolved with 2.5 mm i.d. with liquid velocity, Lslug
ReSc
ShLS ) 3.51 benzoic acid using refractory important parameter for
l/dcap dcap index detector determining L-S mass
transfer
Kreutzer et al.62 liquid-solid mass transfer in Taylor flow liquid to solid heat transfer - model validated with data
modeled with CFD from Bercic and Pintar59
1
kLS ) simulations performed
1 1 for a 1-mm-diameter cylinder

( )
-0.7
+
ψL Di/δ with a moving wall,
DL/dh20(1 + 0.003) for mass transfer with Sh
ReLSc
uTPµL
δ ) dh0.18(1 - e-3.08Ca0.54), Ca ) , aLS ) 4/dc
σL

Heibel et al.63 residence time distribution of the liquid in film flow dynamic response absorbance 0.5 m long co-current down flow effect of maldistribution
measuring technique, 25 cpsi square channels studied
no correlation developed air/water system, Ecoline 43 mm diam cordierite monolith µL ) 0.023 m/s
blue ink as tracer

Yawalkar et al.42 residence time distribution of the liquid in same as above 0.5 m long, co-current down flow effect of channel and
Taylor flow 200-, 400-, and 600-cpsi square channels µL ) 0.05-0.1 m/s inter-monolith redistribution
43-mm-diameter cordierite monolith µG ) 0.07-0.13 m/s studied, axial mixing lower
Pef ) 3.268 × 10-3Re0.31βG,Taylor -0.95 ψL -0.23 in down flow than in up
flow mode

( )
Groppi and Tronconi64 effective radial thermal conductivity based on theoretical analysis - - theoretical correlation
in gas-solid systems

x + ξ - x
(1 - x + ξ) +
λw
1 -x + ξ + x + ξ
λs
λe,r ) λs
x
+
λw λw
(1 - x + ξ) + (x + ξ - x) + x
λs λs
 Ind. Eng. Chem. Res., Vol. 47, No. 10, 2008 3729

Figure 9. Slug length versus liquid holdup for the coarse shower-head
distributors used on a 200-cpsi square-channel monolith (0.1 m diameter)
Figure 6. Flow map of film flow to slug flow (water/air) for a monolith determined (b) directly by conductivity and (O) indirectly from the pressure
(1.5 mm square channels, length of 150 mm), based on the conductivity drop.55
test method.53 The line represents the equation in Table 3.

Figure 10. Pressure drop correlation (fReL as a function of the dimension-

less group, ΨL(Ca/ReL) for Taylor flow, ΨL ) dimensionless slug length
Figure 7. Liquid holdup for a 25-cpsi monolith under film flow conditions, (for gas liquid flow in a round capillary with channel diameter dc ) 2.3
as a function of the dimensionless number for the liquid, NLS ) FrL2/ReL: mm): (b) air/water; (O) air/decane; (0) air/tetradecane; and (- - -) the single-
(0) water; (2) 10% sucrose in water; ([) 25% sucrose in water; (O) 50 phase limit.56
cpsi monolith for water; (line) correlation described in Table 3.35

of the mean residence time occurred to lower values (see Figure

12). Not only this but broadening of the residence time
distribution was also observed, which is of course not desirable
from reactor performance standpoint. Therefore, as stressed
earlier, a well-designed liquid distributor is important not only
to distribute the liquid evenly over the channels but also to
reduce axial dispersion.
Similarly Kreutzer et al.65 have remarked that although the
extent of back-mixing under Taylor flow conditions in a single
channel is in general minimal, the same does not necessarily
hold for a monolith column. If the distribution of gas and liquid
inside the monolith channels is not perfect, the velocity of the
slugs and bubbles can vary from channel to channel. Monoliths
are a special case because there is no flow from channel to
Figure 8. Irrigated pressure drop (i.e., pressure drop in the presence of
liquid) under film flow conditions for a square finned channel compared to
channel so unlike randomly packed bed reactors or other
the phenomenological model.54 The line represents the phenomenological structured packings, redistribution inside the packing is impos-
correlation derived based on the “channel model”. fi and fd represent the sible. As redistribution inside the packing cannot flatten out a
friction factors for the irrigated and dry system respectively, φ2 ) feed maldistribution, it is no surprise that previous studies,59,66
dimensionless pressure gradient ratio and βG ) the fraction of the void have shown more severe backmixing in monolith reactors in
space filled with gas. NGL ) FrG/ReL0.5.
comparison to trickle-bed reactors. Yawalkar et al.42 found Dax,L
values between 0.004 and 0.014 m2/s for the 200, 400, and 600
Heibel et al.63 reported RTD curves for monolith operated in cpsi monoliths operated in co-current down flow with Taylor
co-current down flow with film flow for conditions with and flow conditions. They concluded that degree of axial mixing
without maldistribution inside the channels. A Dax,L value of decreased with decrease in channel size. Inter-monolith redis-
around 0.01 m2/s was obtained from the curves. They found tribution, i.e., stacking of monolith elements, was found to
that due to the channel scale maldistribution effects a slight shift decrease not only the maldistribution effects but also axial
3730 Ind. Eng. Chem. Res., Vol. 47, No. 10, 2008

Table 4. kLae Values Obtained in Film Flow and Slug Flow Regime in Monoliths
kLae (s-1) (for different monolith
flow regime monolith geometry lengths, based on the reactor volume (in m3))
Lebens et al.57 film 4.6 mm, square channels with fins 0.02-0.08 (0.25 m)
0.01-0.03 (0.25-0.5 m)
0.005-0.01 (0.5-1 m)
Heibel et al.58 film 4.1 mm square channels 0.005-0.015 (0.08-0.5 m)
Heiszwolf et al.36 slug 1.5 mm, square channels 0.4-1 (1 m)

mixing. The corner flow of the liquid in the square channels on a theoretical analysis of heat conduction in the unit cell of
leads to tailing of the RTD curves (see Figure 13) thereby the monolith catalyst. Figure 14 shows the effect of material
leading to significant axial dispersion. This effect can be reduced properties and monolith void fraction on the estimated effective
by using rounded or circular channel monoliths where the radial thermal conductivity. Thus, values of λe,r greater by 1
amount of corner flow is significantly low. order of magnitude than those for packed beds (2-5 W/(m K))
A comparison between the Dax,L values in the two flow modes can be obtained. Metal monoliths have excellent radial heat
tells us that axial dispersion in film flow is higher than in Taylor transfer properties, and as a consequence, they have a high
flow, the reason being the larger channel sizes giving rise to a potential as reactor base for strongly exothermic reactions.
different flow pattern and the much lower liquid flow rates Tronconi et al.14 performed experiments with different monolith
employed to achieve film flow. materials to explore the differences in radial thermal conductiv-
The issue with monoliths is that by maldistribution and ity. The influence of the material properties is evident in parts
laminar flow profiles the RTD gradually shifts from a stochastic a and b of Figure 15, representing the axial temperature profile
to a deterministic determined phenomenon, meaning that the at different radial positions inside a cordierite and copper
dimensionless RTD does not sharpen up with reactor length as monolith respectively. Clearly, the much higher thermal con-
is the case with a stochastic process. Therefore, special care ductivity of the copper monolith compared to the cordierite has
must be taken to avoid maldistribution in structured systems a large impact on the radial transport of heat. It is not surprising
that are sensitive to this aspect.65 that a large resistance to heat transfer lies between the skin of
Determination of heat transport from the packing to the heat the packing and the inner reactor wall. Therefore, the difference
transfer fluid is extremely relevant for exothermal multiphase between the copper and cordierite monolith in terms of the
reactions. Work has been done comparing ceramic monoliths overall heat transfer coefficient is reduced because of the gap
and highly conducting monoliths, e.g., copper monoliths. between the skin of the packing and the inner reactor wall, as
Unfortunately, until now only gas-phase studies have been is clear from Figure 15b.
employed for studying heat transfer rates in monoliths. For Certain advanced packing methods were adapted for gas flow
ceramic (cordierite) monoliths severe radial temperature gra- reactive experiments in order to reduce the heat transfer
dients were observed, obviously due to the strong resistance to resistance in the gap.14 A significant reduction of the temperature
heat transport of the ceramic material to the heat transfer gradient was observed (Figure 16). Boger and Heibel68 exploited
fluid.14 Typically, radial convection is absent in monoliths and the differences in thermal expansion between the aluminum
conduction of ceramic monoliths is not sufficiently high to monolith and the stainless steel tube in order to achieve a tight
facilitate considerable radial heat transport. In contrast, contact between the monolith and the tube wall. As a result,
metal monoliths due to their good heat conduction properties very high heat transfer coefficients (>1000 W/(m2 K)) were
can provide considerable radial and axial heat transport.67 If achieved. In two-phase studies, the presence of a liquid film in
suitable materials and geometries are adopted, then the heat the gap can alleviate the resistance to heat transfer at the wall
conduction through the monolith matrix can become quite due to the good thermal conductivity of the liquid as compared
significant.67 to the gas.
Groppi and Tronconi64 have derived a predictive equation Two completely different concepts suggest themselves in-
for the effective radial thermal conductivity (see Table 3) based corporating the properties of both the metallic and cordierite
monoliths: metal monoliths with film flow or slug flow for

Figure 11. Mass transfer coefficient kLae for methane/water system as a

function of the unit cell velocity uTP (m/s) for a 1-m-long 200-cpsi monolith
under Taylor flow conditions. The lines were calculated with the results of
equation of Bercic and Pintar59 in Table 2 using different values of the unit Figure 12. Exit age distribution as a function of residence time for a 25-
cell length Ψuc ) ΨL + ΨG from 1 mm to 30 mm. The symbols refer to cpsi, 500-mm-long monolith at 20 °C and 1 bar under film flow conditions,
oxygen experiments of physical absorption of oxygen to water using 200- uL ) 0.023 m/s. Solid line curve represents maldistributed flow; dashed
cpsi monoliths.36 line curve represent uniformly distributed flow.63
 Ind. Eng. Chem. Res., Vol. 47, No. 10, 2008 3731

Figure 13. E curves for the three cordierite monoliths with square channels:42 ([) 200 cpsi, QL ) 300 L/h, QG ) 381 L/h; (2) 400 cpsi, QL ) 600 L/h,
QG ) 800 L/h; (9) 600 cpsi, QL ) 600 L/h, QG ) 720 L/h.

Figure 14. Effect of material properties and monolith void fraction on

estimated radial effective thermal conductivity, λe,r of honeycomb monoliths
with square channels:67 (0) Cu, (2) Al, (4) AlN, (9) SiC, and ([) AISI304.

efficient radial heat removal through the reactor wall, or

cordierite monoliths for heat removal through convection and
an external heat exchanger in an adiabatic operation. The second
concept is the “monolith loop reactor” developed by Heiszwolf
et al.69 This reactor type can be applied at low conversions and
high liquid flow rates, which support Taylor flow. Thus, both
high mass and high heat transfer rates can be achieved.
Additionally, the heat removal is decoupled from the reactor
design itself, allowing independent scaling of both the reactor
and the heat exchanger. De Deugd et al.70 have presented a
reactor model for the monolith loop reactor, which demonstrates
a high productivity and acceptable pressure drop while ensuring
Figure 15. (a) Axial temperature profiles over a corderite monolith, Toven
a high selectivity and low-temperature rise in the reactor. ) 250 °C, air flow rate ) 10 dm3/min (STP):14 (s) oven temperature; (4)
6.2. Corrugated Packings: Open Cross Flow Structure. wall temperature; (9) peripheral temperature (close to the wall); (])
The early corrugated packings were BX gauze packings24 and centerline temperature. (b) Axial temperature profiles over a copper
they were used for the separation of heat-sensitive products. In monolith, Toven ) 150 °C, air flow rate ) 40 dm3/min (STP).14 (s) oven
the 1970s Mellapak structured packings10 opened up a large temperature; (4) wall temperature; (9) peripheral temperature (close to the
wall); (0) intermediate temperature; and (]) centerline temperature.
field of applications in chemistry, petroleum chemistry, refinery,
and absorption processes. Figure 17 summarizes the develop-
ment history of corrugated structures since 1955. Because of the excellent radial mixing properties of the
Table 5 summarizes the typical geometric properties of the corrugated packings, liquid distribution is not a critical issue.
different types of corrugated packings discussed in this section. Even with a poorly designed distributor, the packing redistributes
Information on applying a catalyst support and active catalyst the flow and hence a fully developed flow profile is achieved
material on the corrugated structure is available.11 There are within a relatively short distance.
numerous contributions on hydraulic and mass transfer models Earlier single-phase flow visualization experiments with
for corrugated packings applied in the countercurrent mode. The corrugated structures similar to Katapak-M revealed three main
most important and widely applied correlations applicable for fluid paths within such structures.71 The first follows the
the low-interaction mode are included in this work. orientation of the “valleys” in the corrugated sheets, which
Table 6 lists the experimental details of the studies on alternately transfer the fluid from one reactor wall through the
hydrodynamics, mass and heat transfer in corrugated structures structure to the opposite reactor wall in one layer, where the
along with the respective (semi-)empirical correlations. heat transfer occurs, and from left to the right in the neighboring
3732 Ind. Eng. Chem. Res., Vol. 47, No. 10, 2008

of perforations. These perforations add to the geometric area,

which is not taken into account by the manufacturer. Second,
the perforations most probably led to the formation of liquid
ripples or waves adding to the effective interfacial area. Thus,
the interfacial area ends up being larger than the geometric area.
It is concluded that the application of the correlation for effective
interfacial area developed by de Brito et al.23 to other packings
is not recommended.
Murrieta et al.74 obtained ae/ap from the relationship of Shi
and Mersmann75 (see Table 6) for Sulzer-BX packing. These
values can be compared with the values obtained from experi-
mental results of Weiland et al.76 on Montz A2 packing which
is exactly the same as a Sulzer BX packing. The difference
Figure 16. CO oxidation runs over copper monoliths: effect of packing between prediction and experiment is striking (see Figure 22,
of the monolith in the reactor tube on the temperature difference between parts a and b). Application of the correlation of Shi and
monolith axis and tube wall. Flow rate ) 7 dm3/min (STP), COfeed ) 5
v/v%, (9) Toven) 215 °C (sample with packaging), and (0) Toven ) 200 °C
Mersmann75 for the prediction of the effective interfacial area
(sample without packaging).14 in corrugated packings can be doubted. The correlation of
Weiland et al.76 is one of the few which predicts a dependence
of interfacial area on gas velocity and not on liquid velocity.
layers (see case a) Figure 18). The second main fluid path always This indicates that the packing is wetted completely at all liquid
stays inside the packing, winding itself around the cross-points velocities. Since the Montz A2 packing they considered is
of the sheet’s corrugations and ensuring the good mixing constructed of very fine stainless steel wires, it is likely that
behavior and the heat and mass transfer between fluid flow and the spreading of the liquid occurs very easily and, as a
structure surface (see case c) Figure 18). The third fluid path consequence, the assumption of full wetting is reasonable.
(see case b) Figure 18) is the bypassing flow in the gap between Furthermore, they show that the hold-up is almost independent
the structure and reactor wall. of gas velocity until flooding occurs while the interfacial area
Battista et al.72 were among the first to study two phase flow decreases with gas velocity. This implies that liquid film
patterns in corrugated structures operated in co-current mode. thickness increases pointing to a certain degree of segregation.
They trace three different flow regimes: annular flow at low Szulczewska et al.77 performed experiments on Mellapak
liquid velocities, stratified wavy flow at higher liquid velocities 250Y and observed that toluene covered the wetted surface much
and bubble flow at larger liquid velocities. They distinguish the better than water. This effect can be attributed to the surface
flow regimes by measuring instantaneous current intensities as tension properties of the two liquids and their ability to wet
a function of time (see Figure 19). At low liquid velocities, the metal surfaces. They observed that although toluene has better
current intensity signal is homogeneous, at intermediate liquid wetting properties than water, only above 0.004 m/s the total
velocities, irregular fluctuations in the signal are detected and surface is covered with toluene.
at high liquid velocities, the signal becomes more homogeneous Recently, liquid hold-up data was reported for corrugated
indicating that the gas-liquid flow has become more regular. open crossflow structured packings with gas-liquid flowing in
The flow map of liquid velocity versus gas velocity for different co-current mode. Sidi-Boumedine and Raynal78 demonstrated
liquid viscosities is given in Figure 20. The liquid velocity that the 1-D model of Bravo et al.79 does not predict properly
strongly affects the transition, while the gas flow has only a the experimental liquid hold-up because the 1-D model is based
slight negative influence for all the liquid viscosities, i.e., as on the assumption that the packing is completely wetted which
the gas velocity increases the transition occurs at a slightly lower in reality is never true. The correlation (see Table 6) takes the
liquid velocity. effect of viscosity on liquid hold-up into account, but not the
For gas-liquid mass transfer, it is very important to know effect of surface tension though it is known that there is a strong
the surface area of the gas-liquid interface (gas-liquid effect of surface tension and contact angle on the wetting
interfacial area). Important results are from Brito et al.23 who characteristics of the packing; see the study of Szulczewska et
showed that the interfacial area can be significantly larger than al.77 Thus, the liquid hold-up correlation should be improved
the geometric surface area. They attribute the additional area further by taking the effect of surface tension into account.
to instabilities in the liquid flow like ripples or waves, There is practically no information on pressure drop correla-
detachment, and subsequent fragmentation of the film into liquid tions for two-phase film flow in the co-current down flow mode
showers. Similar work was carried out by Frank et al.11 in corrugated packings, although the concept of two-phase
(Katapak-MK) and Raynal et al.73 (P-X packing) (see Table pressure drop is well described for counter-current mode in
6) with corrugated structures without any perforations. They structured packings by Stichlmair et al.38 The method applied
observed that the ratio of interfacial area to geometric surface by them is fundamental in nature and can be used for any
area increased with increasing liquid flow-rates but the ratio packing with gas and liquid flowing in trickle mode. The
never went above one at comparable or even higher liquid flow- approach is based on the particle model in which the gas is
rates. The ratio of gas-liquid interfacial area to the geometric assumed to flow around a packing particle having a characteristic
surface area obtained by Brito et al.23 as a function of liquid dimension and the liquid increases this dimension by its
Reynolds number is provided in Figure 21a and that obtained adherence to the particle surface, thereby reducing the void
by Frank et al.11 and Raynal et al.73 as a function of liquid fraction of the bed. The model was validated for a variety of
velocity is provided in Figure 21b. Clearly, the results are very random packings and a structured packing by comparing the
different for the two types of packing. The high values Brito et predicted values of the irrigated pressure drop (see Table 6) to
al.23 report should be restricted to Mellapak or similar packings the measurements performed by different authors on different
with the corrugated plates having a rough texture in the form structured and random packings.
 Ind. Eng. Chem. Res., Vol. 47, No. 10, 2008 3733

Figure 17. History of developments in structured packings. The time between major developments seems to decrease from an average of 15 years until the
1980s down to 6 years since the 1990s.9

Table 5. Typical Geometric Properties of Some Open Crossflow Structured Packings

surface to void corrugation
vol ratio fraction corrugation side/height
no. packing type (m2/m3) (%) angle (deg) (mm) structure
1 corrugated Ni-based - 820 0.88 30 5.7 layered, smooth nickel
packing sheet packing
2 Sulzer Mellapak layered, sheet metal
embossed and grooved
125 Y 125 0.98 45 23
250 Y 250 0.96 45 11.5
500 Y 500 0.91 45 5.75
3 Sulzer Katapak-MK 650 0.85 45 4.0 layered, sheet packing
4 Montz A2 492 0.83 60 n/a layered, woven fabric
5 P-X similar to Mellapak 446 0.93 60 8.5/6.3 layered, smooth stainless
500-X and 500-Y steel sheet packing
P-Y 445 0.93 45 9.82/6.3
6 Gempak 2B 492 0.83 n/a 11.0 layered, slit, and perforated sheet
7 Flexipac 2 233 0.95 45 18.0 layered, fluted surface and large holes
8 Sulzer BX-packing 492 0.90 60 8.9/6.4 layered, perforated gauze
9 Flexeramic 28 282 0.70 45 9.0 layered, ceramic packing
10 Katapak-S 270 270 0.46 45 dh ) 6.9 wire gauze corrugated sheets forming
440 440 0.6 45 dh ) 5.4 channels filled with solid catalyst
11 Montz Multipak I 355 0.56 60 dh ) 6.3
corrugated sheets and flat envelopes
II 325 0.575 60 dh ) 7.0
of wire gauze containing the catalyst

All models for predicting the mass-transfer rates of corrugated mixing effects in corrugated inclined plates in terms of the
packings are based on experimental results for distillation Kapitsa number (see Table 6). In contrast with the other authors
systems. Although such systems involve transfer resistances on they took into account the effect of column height on the mass
both vapor and liquid sides, it has usually been assumed that transfer performance of a corrugated packing. They claim from
the vapor side dominates and thus models for the liquid side their experimental data that there is a critical packing height
do not need high precision.74 Bravo et al.79 proposed the first below which the liquid side mass transfer is a function of
general model for predicting the mass transfer performance of packing height. They compared their model with the model
wire gauze structured packings. The liquid-side mass transfer proposed by Bravo et al.83 and found that their model success-
coefficient was estimated from the penetration theory (see Table fully fitted the experimental data of Mellapak 250-Y and Sulzer-
6). The model was validated by various authors.74,80,81 Raynal BX (see Figure 23). They used a mechanistic model of Brunazzi
et al.73 used the penetration theory to validate their experimental et al.84 to estimate the interfacial area for mass transfer (see
data but found that the model resulted in an important Table 6). Note that the correlation of Brunazzi and Paglianti82
underestimation of the liquid side mass transfer coefficient, kL. is of a general type and can be used to predict the performances
They assumed that the characteristic dimension of the packing, of columns equipped with completely different kinds of
S (channel side of the packing), is appropriate for the gas flow structured packing. Mellapak type has an embossed and grooved
since it occupies most of the volume, but this is not the case surface whereas BX type is made of perforated gauze. As seen
for the liquid flow which is of trickling type. By choosing 4δ in Table 6, only the constants in the correlation would take a
as the characteristic length, they found excellent agreement different value if used for different structured packing.
between their experimental values and the model. Two studies on determination of kLae and ae for corrugated
Brunazzi and Paglianti82 developed a Sherwood correlation packings in a co-current downflow operation have been reported.
as a function of packing height in terms of Graetz number and The results are presented in Table 7. They can be directly
Table 6. Correlations for Hydrodynamic and Transport Parameters for Open Crossflow Structured Packings

3734
reference correlations method geometric properties operating conditions comments
Battista et al.72

Ind. Eng. Chem. Res., Vol. 47, No. 10, 2008

flow transition-film flow to pulse flow current intensity, using a polarized corrugated smooth nickel sheets, co-current down flow effect of viscosity studied
no correlation available electrode, effect of viscosity: 40 mm × 40 mm × 350 mm1 µL ) 0.001-0.073 m/s
0.6-1.1% cmc µG ) 0-0.35 m/s
de Brito et al.23 gas-liquid interfacial area in film flow lean CO2 absorption with reaction Mellapak 125-Y, 250-Y, 500-Y, co-current down flow ae ∝ uL0.3
(ae/ap) ) 0.465ReL0.3 in aqueous NaOH 295 mm i.d. × 420 mm long2 uL ) 0.005-0.02 m/s
uG ) 0.4-2.8 m/s
Frank et al.11 gas-liquid interfacial area in film flow lean CO2 absorption with reaction Sulzer Katapak-MK FeCr-alloy co-current down flow ae ∝ uL0.4
ae ) 95L0.4 in aqueous diethanolamine 38 mm i.d. × 100-500 mm long4 uL ) 0.002-0.01 m/s
uG ) 0.01-0.1 m/s
Raynal et al.73 gas-liquid interfacial area in film flow lean CO2 absorption with P-X 54 mm i.d. × 2 m long5 co-current down flow ae ∝ uL up to uL ) 0.04 m/s
no correlation available reaction in NaOH/NaHCO3 uL ) 0.01-0.1 m/s and then independent
uG ) 1.4 m/s indicating all all geometric
surface area is wetted
Weiland et al.76 gas-liquid interfacial area in film flow lean CO2 absorption with chemical MontzA2 co-current down flow dependence on gas velocity
ae ) 265(µGFG1/2)-0.4 reaction in aqueous NaOH 1.06 m long, 0.15 m i.d.3 uL ) 0.0028-0.011 m/s found
uG ) 0.46-1.0 m/s
Sidi-Boumedine liquid hold-up in film flow mapping the liquid holdup across P-X and P-Y co-current down flow effect of viscosity studied
βL ∝ (mL/µw)1/3

() ()
et al.78 the packing with γ-ray 400 mm i.d. × 2 m long5 uL ) 0.006-0.057 m/s
µL 1/3
Τ µL 1/3
tomographic measurements uG ) 0.1 m/s
βL ) βw0 +Κ ,
µw FL µw
Bh
T ) FLQL
4S
Stichlmair et al.38 pressure drop in film flow phenomenological model based on Mellapak 250-Y plastic,2 data countercurrent βL ∝ uL1/3
the fluidized bed analogy, validated from Sulzer used for uL ) 0-0.041 m/s
(-dpdz)
[ ]
packings in countercurrent flow validation uG ) 0.5-4 m/s
1 - (1 - βL/) (2+c)/3
) [1 - (1 - βL/)]-4.65 below the load point
irrigated
,
1-
(-dpdz) dry

βL ) 0.55FrL1/3
Fr ) uL2 aP/g4.65
Bravo et al.85 pressure drop in film flow based on the channel model, validated Gempak6 and Flexipac7 countercurrent βL ∝ uL0.36
uL ) 0-0.05 m/s

( )
for structured packings in counter- pressure drop data from Koch validated for aqueous and
3 (1 - ) FG‚uG
2
dp c1 c2 current flow below the load point, used for validation uG ) 0-0.15 m/s organic systems
- ) f 4.65 ,f) + + c3 i.e., film flow regime
dz 4  dh Reg Re 1/2

[ ]
dry g

1 c1 1 c2
c) +
f Reg 2 Re 1/2
g

Rocha et al.86 pressure drop in film flow based on the channel model, validated Flexipac,7 Gempak,6 Sulzer BX,8 countercurrent takes into account the effect
for structured packings in counter- column i.d. 430 mm and uL ) 0-0.035 m/s of gas and liquid flow rates
2
fFGuG,eff c2 uG current flow below the load point height 3 m uG ) 0-0.5 m/s on liquid holdup, hold-up
(-dpdz) dry
)
dh
, f ) c1 +
Reg
, uG,eff )
(1 - βL) sin θ and pressure drop model
validated for air-water
AFG βFG system, pressure drop
(-dpdz) dry
) u 2+ 2
dh(1 - βL) sin θ G dh (1 - βL) sin θ
uG model also validated at
high pressure and low
surface tension liquids
packing-geometry-dependent constants
Table 6. (Continued)
reference correlations method geometric properties operating conditions comments
Uresti-Melendez pressure drop in film flow based on the channel model, pressure drop measurements countercurrent takes into account the
et al.87 uL ) 0-0.035 m/s
(-dpdz) irrigated
)
1
, C ) 0.626 + 32.669s,
validated for structured packings
in countercurrent flow below
from databank for
Flexeramic9 packings using uG ) 0.5-4.5 m/s
effect of gas and
liquid flow rates
the load point, i.e., film flow regime air-water system on liquid holdup
(1 - CβL)5
(-dpdz) dry

CβL ) 2.5113FrL0.36

βL ) 4 ( ) Ft
S
2/3 3µLuL
FL(sin θ)geff

ae 29.12(We × Fr)L0.15S0.359
Ft ) )
aP Re 0.6(1 - 0.93 cos γ)(sin θ)0.3
0.2
L

efficiency of Shi and Mersmann75

θ ) angle with respect to horizontal axis
uG,effSFG
CβL ) 0.381FrL0376ReG,eff0.257, ReG,eff )
µG
Frank et al.11 gas-liquid mass transfer in film flow lean CO2 absorption with reaction Sulzer Katapak-MK FeCr-alloy co-current down flow kL ∝ uL0.6
kLae ) 0.0025uLFL in aqueous triethanolamine 38 mm i.d. × 100-500 mm long4 uL ) 0.002-0.01 m/s
desorption of oxygen from saturated uG ) 0.01-0.1 m/s
water into nitrogen co-current down flow
desorption of CO2 from water into uL ) 0.005-0.02 m/s
air and absorption of chlorinated uG ) 0.4-2.8 m/s
solvents
Laso et al.10 gas-liquid mass transfer in film flow
Mellapak 125-Y, 250-Y, 500-Y,
kLae ) 0.574uL0.62 Mellapak 250-Y
295 mm i.d. × 420 mm long2
kLae ) 0.713uL0.71 Mellapak 500-Y
Brunazzi et al.82 gas-liquid mass transfer in film flow Mellapak 250-Y, 100 mm validated the model by

Ind. Eng. Chem. Res., Vol. 47, No. 10, 2008 3735
i.d. × 0.4-2 m long2 using distillation data
Gz B
k 4δ σL FL
L 3
using Sulzer-BX packing
ShL ) A , ShL ) , Ka ) 4 , also validated for
Ka C D L µL g liquids of different
δ surface tension and
Gz ) ReLScL
H viscosities
3 µL
( uL
)
0.5
Z
H) ,δ)
sin a FLg sin a βL sin a

ae
(
dh sin θ
) ( )
FLg 0.5
) βL1.5
ap 4 3µLuL
A ) 16.43, B ) 0.915, C ) 0.09
for Mellapak 250-Y (metal/plastic)
A ) 63.1, B ) 0.676, C ) 0.09
for Sulzer BX (plastic)
ae
(
dh sin θ
) ( )
FLg 0.5
) βL1.5
ap 4 3µLuL
Table 6. (Continued)

3736
reference correlations method geometric properties operating conditions comments
Brunazzi et al.84

Ind. Eng. Chem. Res., Vol. 47, No. 10, 2008

gas-liquid mass transfer in film flow countercurrent

( )( )
uL ) 0-0.008 m/s
3Γ FL2 1/3
uL,eff ) (falling film relationship) or
2FL 3µLΓ

(x ) (x )
uG ) 0.4-1.4 m/s
DL DLuL,eff
kL ) 2 or kL ) 2
πt πs
uL
uL,eff )
βL sin θ
Bravo et al.79 gas-liquid interfacial area modeling work using
calculated using the following penetration theory
correlation from Shi and Mersmann75

ae 29.12(We × Fr)L0.15s0.359
) ,
ap Re 0.20.6 (1 - 0.93 cos γ)(sin θ)0.3
L
γ ) contact angle for surface material wettability
Battista and Bohm88 wetted area for liquid-solid mass transfer adding red ink to the circulating corrugated packing made of smooth co-current down flow measured values compared
liquid and measuring the nickel sheets, 40 mm × 40 mm to those predicted by the
colored area × 500 mm long1 correlations of Billet
(aLS/ap) ) 0.58ReL0.5FrL0.1 ReL < 5 uL ) 0.01-0.065 m/s
(aLS/ap) ) 0.85CReL0.25FrL0.1 ReL g5 uG ) 0.0-0.3 m/s
Battista and Bohm88 liquid-solid mass transfer coeff electrochemical technique corrugated packing made of smooth verified for different
nickel sheets, 40 mm × 40 mm × liquid viscosities
500 mm long1
Sh(aLS/ap) ) 0.33Sc1/3ReL0.63 ae/ap ∝ 1/µL
1256 < Sc < 17045,
0.15 < ReL < 84
Macias-Salinas residence time distribution for gas phase dynamic response conductivity column of 4.3 mm i.d. and 2.1 m long counter-current evaluated effect of axial
et al.89 PeG ) 4.2468 × 108Reg-0.896 × measurement technique, packed with Flexipac-27 and uL ) 0.03-0.09 m/s mixing on mass transfer
10-0.00208Rel(deap) -7.792 air/water system, Sulzer-BX8 processes
residence time distribution for liquid phase helium as tracer for gas phase uG ) 0.75-2.5 m/s Sulzer BX with lower axial
PeL ) 8.154Fi0.7082(3/sin 2φ)1.159(deap)6.337 and NaCl as tracer for liquid phase mixing in both phases
than Flexipac-2
381 < Reg < 3516, 25 < Rel < 122,
45° < φ < 60°, Fi ) µu/deq2Fg,
1.5 × 10-6 < Fi < 1.59 × 10-5,
3.16 < deap < 3.53
Kolodziej et al.90 residence time distribution for liquid phase dynamic response technique Katapak-S-270;10 440 Multipak I and II11 counter-current validated for a lower surface
tension liquid, Multipak
Multipak-II Dax,L ) 0.0663uL,eff nitrogen/ n-heptane system 55 mm diameter × 1.9 m long uL ) 0.001-0.008 m/s shows higher axial
Katapak-S-440 Dax,L ) 0.0332uL,eff with o-xylene as tracer uG ) 0.0-1.6 m/s dispersion than Katapak-S
von Scala et al.71 effective radial thermal conductivity,
wall heat transfer coefficient
no correlation developed
heat transfer parameters λe,r and aw heating of cool air and measuring the Katapak-M packing, uG ) 0.5-1.5 m/s good agreement between
evaluated based on a two-dimensional radial temp profile at the exit 48-mm-diameter packed in 50 mm CFD simulations and
pseudohomogeneous steady-state of the tube filled with the packing i.d. × 400 mm long experimental results
plug flow model
 Ind. Eng. Chem. Res., Vol. 47, No. 10, 2008 3737

Figure 18. Main fluid paths in open crossflow structures: (a) flow
following the valleys, which is reflected at the side wall and returns through
a valley of the opposite plate; (b) bypassing flow in the gap between the
structure and reactor wall; (c) fluid following the main flow direction and Figure 20. Flow map of film flow to stratified wavy flow in OCFS packing
crossing the valleys. Adapted from ref 71. made of smooth Nickel sheets at different liquid viscosities: ([) µL )
0.97 mPa s; (]) µL ) 1.17 mPa s; (2) µL ) 4.4 mPa s; (4) µL ) 7.4 mPa
s; (0) µL ) 10.0 mPa s; (9) µL ) 12.6 mPa s.72

of channeling at low liquid flow rates and incomplete wetting

over the complete range of liquid velocity studied persist. Not
surprisingly, viscosity shows a negative effect on the fractional
surface wetting.
Macias-Salinas et al.89 evaluated the impact of axial mixing
on mass transfer efficiency based on mass transfer data reported
for the cases of gas absorption, stripping, water cooling and
distillation using Flexipac-2 and Sulzer-BX packing. They
concluded that neglecting axial mixing can lead to an overes-
timation of the mass-transfer driving forces, thus leading to an
underestimation of the mass transfer coefficients. Results of
oxygen desorption from water into air showed that deviation
from plug flow diminished as liquid flow increased. This case
clearly demonstrated the importance of properly assessing the
impact of axial mixing effects in order to be able to establish
the range of operating conditions over which these effects can
be safely neglected.
Only one paper reports gas phase heat transfer measurements
in Katapak-M packing.71 The heat transfer parameters λe,r and
Rw increase with increasing flow rate due to (a) improved mixing
inside the structure and (b) reduced thickness of the boundary
layers. The influence of the gap (1-2 mm) between the structure
and the wall on the heat transfer rate was also studied. With
Figure 19. Flow regime transitions in OCFS packing made of smooth nickel
increasing gap, the bypass flow becomes more important and
sheets are identified from the time series of instantaneous current intensities mixing is less efficient, decreasing the overall heat transfer
for the nitrogen/potassium ferrocyanide and ferricyanide aqueous solutions coefficient. Effective radial thermal conductivities, λe,r, were
at the following gas and liquid velocities: uG ) 0.24 m/s and (a) uL ) found to be between 1 and 2 W/(m K) and the wall heat transfer
0.01 m/s; (b) uL ) 0.014 m/s; (c) uL ) 0.024 m/s; (d) uL ) 0.035 m/s; (e) coefficients, Rw, were between 60 and 80 W/(m2 K). These
uL ) 0.053 m/s; (f) uL ) 0.065 m/s. The film flow regime corresponds to
low or no current intensity fluctuations, stratified wavy flow to significant values are very low compared to what are actually required in
current intensity fluctuations.72 multiphase exothermic reactions. In two-phase flow, the liquid
hold-up in addition to the mass flow-rate and the heat capacity
plays a prominent role in the heat transport mechanism.
compared as the corrugated packings used by both authors have Additionally, the turbulence generated by the interaction between
almost the same geometric dimensions, including the column the gas and liquid intensifies radial mixing giving rise to
diameter. Raynal et al.73 found kLae and ae values which are relatively high λe,r. The intense radial mixing directed from the
higher than those obtained by Frank et al.11 The measurements packing to the wall also might lead to convective transport of
were carried out at different velocities and, as a consequence, heat at the wall and thus a relatively high Rw. This hypothesis
the flow regime might have been different in both cases. We should be further investigated.
expect that the measurements of Frank et al.11 were carried out 6.3. Corrugated Packings: Closed Cross Flow Structures.
in trickling flow regime (low interaction) and that of Raynal et The closed crossflow structure is also made of thin corrugated
al.73 were carried out either in Taylor or churned flow (high metal sheets arranged side by side with opposing channel
interaction). orientations but in addition a flat sheet is inserted between the
The fractional surface wetting measured by Battista and corrugated sheets (Figure 25). The open channel packing
Bohm88 is plotted at different liquid viscosities against the liquid geometry is then transformed into a monolith-like structure
velocity in Figure 24. From the values it is clear that problem with a multiplicity of closed inclined triangular channels. This
3738 Ind. Eng. Chem. Res., Vol. 47, No. 10, 2008

Figure 21. Ratio of gas-liquid interfacial area to geometric surface area, ae/ap, in open crossflow structures as a function of the Reynolds number: (a) left
graph, Mellapak packing;23 (b) right graph, ([) Katapak-M packing11 and (0) P-X packing73 (similar to Mellapak 500-X without perforations).

Figure 22. Comparison between (a) left graph, experimental results of effective interfacial area, ae (m2/m3) of Montz A2 packing,76 and (b) right graph,
values obtained for the effective interfacial area from the correlation of Shi and Mersmann75 for a Sulzer BX packing at Fs ) 1.18 (m/s)(kg/m3)0.5.

What makes this structure so special is that it is open at the

wall and as the flow is directed from left to right and vice versa
in the adjacent layers it directly hits the reactor tube wall causing
disturbances of the stagnant layers at the wall.25 If the channel
size is sufficiently small, Taylor flow will be induced, provided
the ratio gas to liquid flow rate is in the right range. In
combination with improved heat transfer at comparatively lower
pressure drop, Taylor flow might result in high mass transfer
rates.
Closed channel packings with larger channels (dh ) 11.3 mm)
were studied by Behrens et al.91 for counter-current applications.
They concluded that because of the inclination of closed
channels, the liquid tends to flow in rivulet form along the base
of channel formed between corrugations and the flat plate, which
Figure 23. Parity plot of kLae, comparison between experimental and implies a significant loss of effective surface area, and hence
predicted values obtained by using the model of Brunazzi et al.82 and the an increased bypassing. This phenomenon might not occur in
model proposed by Bravo et al.83 for Sulzer BX plastic (0, Bravo et al.; 9,
smaller diameter channels as due to significant surface tension
Brunazzi et al.) and BX metal packing (O, Bravo et al.; 2, Brunazzi et al.).
Experimental kLae values obtained with air/CO2/water system. forces and capillary action wetting will be high.
The pressure drop in closed channel packing is lower than
the standard packing even though the closed channel has a
way the specific surface area can be increased considerably.91 higher geometric surface area.91 By inserting a flat sheet between
Wash coating of closed crossflow structured packings can be two corrugated sheets the energy consuming gas-gas interaction
carried out in the same manner as open crossflow structured is replaced with less energy consuming gas-liquid friction.
packings. Although pressure drop correlations are not found in literature
Initial flow distribution in closed channel packings is as for closed channel packings, the two-phase pressure drop can
important as it is for monoliths, since there is no exchange of be modeled as a function of dry pressure drop and liquid hold-
liquid between adjacent channels. up, similar to the corrugated packing.
Flow patterns in the closed channels are similar to those in The closed channel packings being open at the wall, very
a monolith as the channels are closed with no interconnection efficiently help in disturbing the laminar film present in the gap
with adjacent channels. Thus, radial mixing will be very limited. between the skin of the packing and the wall when the flow is
 Ind. Eng. Chem. Res., Vol. 47, No. 10, 2008 3739

Table 7. kLae and ae Values Obtained in Open Crossflow Structures

author range of gas and liquid velocities flow regime kLae (s-1) ae (m-1)
Frank et al.11 µL ) 0.002-0.01 m/s low interaction 0.005-0.025 150-250
µG ) 0.01-0.1 m/s
Raynal et al.73 µL ) 0.01-0.1 m/s high interaction 0.15-0.25 200-500
µG ) 1.4 m/s

Table 8. Typical Geometric Properties of Commercially Available Knitted Wire Packing

surface-to-volume void fraction wire diameter crimp pitch
packing supplier ratio (m2/m3) (%) (µm) (mm)
Goodloe Koch-Glitsch 1920 0.95 114 8.0
HYFlux Evergreen Tech. Pvt. Ltd. 1932 0.95 ∼100 ∼8.0

directed from the structure to the wall. This creates turbulence Table 8 gives typical geometric properties of these packings
thus improving the heat transfer from the packing to the wall. Table 9 lists the experimental details of the studies on
Unlike the monolith, the closed channel packing shows a lower hydrodynamics and mass transfer in knitted structured packing
sensitivity to gap sizes between the skin of the packing and the along with the respective empirical correlations.
wall.25 Flow visualization experiments carried out by Schildhau- Unlike the corrugated packings, this packing has almost no
er25 have confirmed that the flat plate between the corrugated self-distribution property.26 Similar to monoliths, the liquid
sheets directs the fluid more efficiently toward the inside reactor distributor design plays a crucial role in the performance of
wall to improve overall heat transfer coefficients. reactors packed with such packings.
Single phase heat transfer measurements with closed channel Figure 26 presents a flow map for the knitted wire packing,
packings show improved wall heat transfer coefficient at lower showing the transition from trickle flow to pulse flow, pulse
pressure drop compared to open crossflow structured packing flow to slug or Taylor flow and slug flow to spray flow. The
or a bed of spherical particles.25 fitted correlation (see Table 9) (for original data see Patil and
6.4. Knitted Wire Structured Packing. Knitted wire is a Sharma94) is obtained by regressing the experimental data. The
family of structured tower packings, which are particularly correlations have not been tested for other systems apart from
useful in distillation applications when a moderate to large air and water, making their applicability limited. Note that the
number of theoretical stages have to be accommodated in a transition from one to another regime is quite sharp. Since the
limited height of the tower. This packing is originally named data was obtained by ocular inspection it is likely that a
as Goodloe packing with the essential feature devised by A. transition region could not be detected.
M. Goodloe of the Metal Textile Corp.92 Patil and Sharma,94 Weiland et al.,76 and Niranjan et al.93
This packing is characterized by bundles of knitted strands measured gas-liquid interfacial areas in the low interaction
of stainless steel wires. The knitted strands are flattened, regime for this packing. The results are presented in Table 10.
crimped, and rolled to give the desired diameter of the Parts a-c of Figure 27 show the gas-liquid interfacial area
cylindrical packing.93 It gives a combination of low-pressure as a function of gas and liquid velocities measured by the three
drop and excellent wetting characteristics with a low surface authors. The interfacial areas are in the same range but the
tension liquid. dependences on the gas and liquid velocities vary significantly.
Since the interfacial areas measured are significantly smaller
The inherent capillary action of the fine wires causes the
than the geometric area of the packing and the dependence on
liquid to spread into thin films that continuously combine and
the gas velocity is weak, the differences observed might be due
divide for optimum mixing and contact with the gas throughout
to experimental errors and hence the correlations can be
the entire packing volume. The net result is a packing with high
questioned. The high ae values observed by Niranjan et al.93 at
mass transfer efficiency and low-pressure drop. Both co-current
relatively low liquid and gas velocities are remarkable. Since
and counter-current (pre-flooding) data are available in the
the measurements carried out by them are in counter-current
literature. Unfortunately, there is no data or information on the gas-liquid mode, it is concluded that the mode of operation
heat transfer properties and catalytic coating methods for this has a significant effect on the hydrodynamics and eventually
packing as it is primarily used in distillation processes. the interfacial area. Patil and Sharma94 also investigated the
effect of surface tension on the effective interfacial area by
adding 5 vol % 2-propanol in aqueous sodium dithionite. As
expected, the interfacial area was higher than for the aqueous
system. The increase in ae was observed to be different in
different flow regimes and it was approximately 15%-20%,
30%-45%, and 80%-125% for trickle, pulse and slug flow
regime, respectively. In the case of slug flow, they observed
foaming with values of ae as high as 2470 m2/m3, which is
higher than the geometric surface area of the packing. This result
is not surprising as the high values of ae in the slug flow might
arise due to the formation and breaking of foaming slugs,
analogously to the results obtained by de Brito et al.,23 which
was already elaborated upon in section 6.2. Thus, Patil and
Sharma94 successfully demonstrated that the surface tension has
Figure 24. Fractional surface wetting for OCFS packing made of smooth
a significant effect on the effective interfacial area.
nickel sheets, ae/ap, as a function of µL for different liquid viscosities: ([) Summarizing, the wetting characteristics of this packing is
µL ) 1.0 mPa s, (0) µL ) 3.0 mPa s, and (2) µL ) 5.0 mPa s.88 are remarkably good for low surface tension liquids. Though
3740 Ind. Eng. Chem. Res., Vol. 47, No. 10, 2008

Figure 25. (a) Right photo: top view of CCFS. (b) Left photo: side view of two CCFS elements rotated by 90° to each other.

these packings have high geometric surface areas, there is yet mass transfer, pressure drop, liquid hold-up and RTD were
no know-how on how to coat these packings with catalytic reported by Stemmet et al.101 for co-current up flow operations.
material in order to achieve considerable mechanical strength Washcoating of the Fecralloy foam with a stable layer of Pd/γ
and activity. It should be realized that these packings are formed Al2O3 is reported in the literature.99
out of thin woven fibers, and it can be speculated that coating Table 11 lists the experimental details of the studies on
the packing would destroy the geometric surface area created hydrodynamics and mass transfer in foams along with the
by the woven fibers. This would mean that after coating the respective empirical correlations.
area available for mass transfer and reaction might be consider- The two-phase pressure drop in foams can be modeled in a
ably lower than stated by the manufacturer. similar way, i.e., as a function of the dry pressure drop and
The pressure drop model developed by Patil and Sharma94 is liquid hold-up. The dry pressure drop concept in foams is well-
not based on any mechanistic model (Table 9) as it is only fitted defined95,102 and was modeled based on the Forchheimer
against experimental data. The two-phase pressure drop is not equation.103 This relationship is synonymous with the Ergun
a simple addendum to the single-phase pressure drop but it is model,104 in which the pressure drop is the sum of viscous and
higher due to the formation of a liquid film on the filaments inertial terms.
thus lowering the effective diameter of the channels for the gas Stemmet et al.100 measured pressure drop in the liquid phase
flow. The channel model developed by Bravo et al.85 and Rocha in countercurrent mode for a 2-D open-celled solid aluminum
et al.86 for countercurrent flow in corrugated packings is also foam in the range of 5-40 PPI with voidages of 92%-94%.
recommended for these packings in the trickle flow regime. Figure 28 presents the dry and wet pressure drop versus gas
The kLae values measured by Niranjan et al.93 and Weiland load for different PPI and liquid velocities. Pressure drop
et al.76 are compared in Table 10. Again the dependence on increases not only with increasing gas loads but also with
gas and liquid velocities are different in both cases. The counter- increasing PPI and liquid velocity. This plot can give an
current mode of operation applied by Niranjan et al.93 has a indication of the pressure drop in a co-current operation with a
significant effect on hydrodynamics and eventually the volu- fair assumption that the low interaction regime in counter-current
metric gas to liquid mass transfer coefficient which includes mode will render similar pressure drops as in co-current low
the interfacial area. interaction regime.
6.5. Foams: Metals-, Ceramic-, and Graphite-Based. Solid As given in Table 11, Stemmet et al.105 used the relative
foam packings represent a generation of materials combining permeability model to predict the total liquid hold-up in the
high specific surface area with low-pressure drop. This is largely foam. This model assumes that the drag force per unit volume
due to the open-celled structure with high voidages (up to 97%) for each fluid is a function of the relative permeability, fR, of
of small dimensions. Solid foams are produced in a variety of each phase. Stemmet et al.105 correlated the static hold-up as a
materials (metal, ceramics, carbon, SiC, polymers, etc.). Metallic function of the Eötvös number, for foams in the range 5 to 40
foams have in recent years seen increased application for flow PPI, see Figure 29. They fitted their data with the model
control and heat transfer enhancement.95 The excellent perfor- developed by Saez and Carbonell.106 The total liquid hold-up
mance of metallic foams in these applications is attributed to data and fitted model results for 5 PPI foam are presented in
their intricate interfacial geometries, creating a highly tortuous Figure 30. The liquid holdup is not predicted well in the low
flow path with a continuous disruption of established hydro- liquid hold-up region, probably because it is highly dependent
dynamic and thermal boundary layers. In the case of aluminum on the static hold-up. Stemmet et al.100 also showed that the
foam, good thermal contact achieved with the foam brazed onto liquid holdup increases with increasing PPI, because the foam
an aluminum substrate material is combined with the good with a higher PPI has a higher specific surface area that gives
thermal conductivity of aluminum.95 The review by Banhart et a higher restriction to the flowing liquid.
al.19 outlines the methods and procedures for producing these A graph of mass transfer coefficient per liquid volume for
and many other types of foam. 10 and 40 PPI solid foam for different liquid velocities in the
The applications considered for these foam materials in the co-current upflow configuration is given in Figure 31. Measure-
chemical industry have been minimal. Only single phase studies ments were carried out by Stemmet et al.101 in the pulsing regime
have been reported, in ceramic foams on mass and heat transfer where the interaction between gas and liquid is strong.
rates by Richardson et al.,96 pressure drop in aluminum foams Therefore, high rates of mass transfer are expected per liquid
by Fourie and Du Plessis,95 axial dispersion in nickel foams by volume (0.1-1.2 s-1). These high rates correspond to the fact
Montillet et al.,97 heat transfer characterization by Gianni et al.,98 that equilibrium conditions are achieved, i.e., oxygen is almost
and mass transfer characterization by Gianni et al.99 in Fecralloy completely desorbed from the liquid. This can lead to a large
and copper foams. Recently characterization of foams with error in the calculation of mass transfer coefficient, and therefore
respect to pressure drop and liquid hold-up for countercurrent one has to be careful while scrutinizing mass transfer data
operation was reported by Stemmet et al.100 and gas to liquid obtained using a physical technique.
Table 9. Correlations for Hydrodynamic and Transport Parameters for Knitted Wire Packings
reference correlations method geometric properties operating conditions comments
Patil and Sharma94 flow transition-trickle flow to pulse flow visual inspection, 150 mm long, co-current downflow limited to air/water systems
LtransΨ/ ) 33.592(Gtrans/λ)2 - 162.37(Gtrans/λ) + 200.65 air-water system 25 mm diameter, uL ) 0.002-0.045 m/s
valid for 0.005 e uL e 0.045 m/s and 0.99 e uG e 1.76 m/s bulk density ) 440 kg/m3 uG ) 0.5-8 m/s
flow transition-pulse flow to slug flow
LtransΨ/ ) -0.6838|(Gtrans/λ)2 -28.813(Gtrans/λ) + 122.79
valid for 0.005 e uL e 0.045 m/s and 1.9 e uG e 2.9 m/s
Ψ ) (σw/σL)[(µL/µw)(Fw/FL)2]0.33
λ ) [(FG/Fair)(FL/Fw)]0.5
Patil and Sharma94 gas-liquid interfacial area air oxidation of alkaline 150 mm long, 25 mm diam, co-current downflow also tested for low surface tension
ae ) auβG1uβL2 aqueous sodium bulk density ) 440 kg/m3, uL ) 0.001-0.03 m/s liquids, correlation developed
R ) 5970 β1 ) 0.156 β2 ) 0.514 for trickle flow dithionite solution 1.02 m long, 0.15 m i.d. uG ) 0.5-2.5 m/s for all regimes
R ) 1772 β1 ) 0.267 β2 ) 0.316 for pulse flow ae∝ uG0.15 uL0.5
R ) 141660 β1 ) 0.526 β2 ) 1.33 for slug flow
Weiland et al.76 gas-liquid interfacial area in film flow lean CO2 absorption with countercurrent valid only for aqueous systems,
ae ) 356(uGFG1/2)-0.2 chemical reaction in uL ) 0.0028-0.011 m/s dependence on gas velocity
aqueous NaOH uG ) 0.46-1.0 m/s
Niranjan et al.93 gas-liquid interfacial area in film flow lean CO2 absorption with 1.05 m long, 0.1 and counter-current valid only for aqueous systems,
gas-liquid interfacial area remained constant chemical reaction in 0.2 m column diameter uL ) 0.0005-0.0044 m/s no dependence on gas and liquid velocity
over the entire range of gas and liquid velocities aqueous NaOH uG ) 0.4-1.14 m/s ae ∼ constant
Niranjan et al.93 liquid hold-up in film flow weighing technique, 1.05 m long, counter-current valid only for aqueous systems,
βL ) 0.784uL0.28 dynamic hold-up, 0.2 m column diameter uL ) 0.001-0.0075 m/s βL should depend on liquid film
air and water system ug ) 0-0.3 m/s thickness, as ae is constant
Patil and Sharma94 pressure drop manometer reading 150 mm long, co-current downflow valid only for aqueous systems
25 mm diameter, uL ) 0.002-0.045 m/s

(dpdz) irrigated
) 1 + β3ReG + β4ReL
(dpdz) dry

β3 ) 70.2 × 105 bulk density ) 440 kg/m3 uL ) 0.5-8 m/s

β4 ) 67 × 103 for trickle flow
β3 ) -27.6 × 105
β4 ) 72.3 × 103 for pulse flow
β3 ) 13.2 × 105
β4 ) 34 × 103 for slug flow
Weiland et al.76 gas-liquid mass transfer in film flow lean CO2 absorption with 1.02 m long, 0.15 m id co-current valid only for aqueous systems,
chemical reaction in uL ) 0.0028-0.011 m/s negative dependence on liquid velocity
ShL ) 3.4ReL - 0.08ScL1/2 aqueous Na2CO3 + NaHCO3 uG ) 0.46-1.0 m/s kL ∝ uL-0.08
Niranjan et al.93 gas-liquid mass transfer in film flow lean CO2 absorption with 1.05 m long, 0.2 m counter-current valid only for aqueous systems
no correlation developed chemical reaction in column diameter uL ) 0.001-0.0075 m/s kL ∝ uL0.2
aqueous Na2CO3 + NaHCO3 uG ) 0-0.3 m/s
Ind. Eng. Chem. Res., Vol. 47, No. 10, 2008 3741
3742 Ind. Eng. Chem. Res., Vol. 47, No. 10, 2008

surface areas 100 times greater than conventional heat exchang-

ers. The bulk thermal conductivity of the 25% dense graphite
foam is 180 W/(m K) as compared to 15 W/(m K) of aluminum
and 40 W/(m K) of copper foam. Applications for the ORNL
graphite foam that are currently being explored are as follows:
Power electronics cooling with 10 times larger cooling potential
than traditional heat sinks and in radiators. Experiments have
demonstrated that the overall heat transfer coefficient is very
high compared to that of a standard automobile radiator (2500
W/(m2 K) vs 30 W/(m2 K)).
From the above it appears that the radial thermal conductivity
through the foam structure can be high compared to randomly
packed beds. It should be noted that nothing is reported on the
wall heat transfer coefficient, as it can be the limiting factor
Figure 26. Flow map for knitted wire packing (air-water system).94 Ψ ) for heat transfer for highly exothermic reactions carried out in
σwater/σL [µL/µwater(Fwater/FL)2]0.33; λ ) [FG/Fair(FL/Fwater)]0.5. small diameter tubes.

The axial dispersion coefficient values obtained by Stemmet 7. Discussion

et al.101 were at least two orders of magnitude larger than those
obtained by Montillet et al.,97 who found that Dax,L increases From previous sections, it can be concluded that structured
with liquid superficial velocity (see Table 11 and Figure 32). multiphase reactors has inspired many groups both form
This is not surprising since Stemmet et al.101 performed RTD academia and industry to focus (part of) their research effort
experiments with three time’s higher liquid velocity. Stemmet on this developing field. In many aspects, a wealth of results
et al.,101 used the co-current up-flow mode which results in large can be found in scientific and patent literature, but not
axial mixing while Montillet et al.97 worked in the down-flow surprisingly, still large gaps are clearly there. With respect to
mode. Stemmet et al.101 concluded that axial dispersion (Bo g hydrodynamics, pressure drop, and mass transfer rates, sufficient
10 at uL ) 0.02-0.1 m/s and uG ) 0.1-1.0 m/s) had negligible phenomena related information and correlations have been
effect on the calculated mass transfer coefficients. published with respect to monoliths and corrugated open
Richardson et al.96 measured gas phase overall wall heat crossflow structures, but only limited knowledge is available
transfer coefficient, U in 30 PPI ceramic foams. They compared for multifilament wire mesh, foams, and corrugated closed
the results obtained for the ceramic foam with conventional 0.5 crossflow structures. Regarding liquid solid mass transfer for
mm glass spheres with equivalent diameter, i.e., the same surface monoliths and OCFS packings some basic experimental work
to volume ratio. Figure 33 shows a comparison between the has been done. Axial mixing in monoliths, OCFS and foams
Nusselt numbers at 800 °C for 30 PPI foam, measured and the RTD due to maldistribution are the underlying phe-
experimentally, and for 0.5 mm glass spheres calculated from nomena causing “axial dispersion”, which is clearly documented.
an analogous expression for spheres. The foam shows a higher Despite the fact that the there are still many unknown areas,
Nusselt number by about a factor of 4, except for low Reynolds it is possible to get for most applications a sufficiently complete
numbers. It is evident that the convective heat transport in foams picture from an evaluation of existing information on the
is far superior to that in packed beds of spheres with only gas structured packings based on a critical assessment of three
flowing through the foam. aspects that the authors think are relevant, namely the following
The aluminum foam from ERGAerospace is used as a ones: (1) type of experiments conducted; (2) measurement
compact heat exchanger.27 The ligament structure of Duocel techniques used; and (3) hydrodynamic models applied.
aluminum foam promotes complete mixing and efficient scrub- 7.1. Types of Experiments. In general, there has been done
bing of the heat exchange surfaces. All aluminum brazed joints a vast amount of work on aqueous systems as the measurement
provide continuous, highly conductive heat paths and superior techniques are well-known for such systems and moreover
overall thermal conductivity, all at less than 10% the weight of aqueous systems are easy to handle. Except for some of the
solid aluminum. pressure drop and liquid hold-up studies, experiments have been
A novel technique for fabricating high-thermal-conductivity carried out primarily with aqueous solutions. This limits the
pitch-based carbon foams has been developed and patented at use of the correlations for other fluid systems, for, e.g., organic
the Oak Ridge National Laboratory.107 They produce graphite systems, which are mostly applied in industrial applications.
foams with a thermal conductivity equivalent to aluminum alloys Flow transitions shift to lower superficial gas and liquid
at one-fifth of their weight. It has an open porous structure with velocities when a low surface tension liquid is used.108 This

Table 10. kLae and ae Values for Knitted Wire Packing from Different Authors
range of gas and dependence of kLae dependence of ae
authors iquid velocities kLae (s-1) on gas and liquid velocity ae (m2/m3) on gas and liquid velocity
Patil and Sharma94 co-current downflow - - 150-400 ae ∝ uG0.15uL0.5
uL ) 0.002-0.045 m/s
uG ) 0.5-8 m/s
Weiland et al.76 co-current downflow 0.015-0.02 kL ∝ uL-0.08 350-450 ae ∝ uG-0.2
uL ) 0.0028-0.011 m/s
uG ) 0.46-1.0
Niranjan et al.93 counter-current 0.02-0.05 kL ∝ µL0.2 450-500 -
uL ) 0.001-0.0075 m/s
uG ) 0-0.3 m/s
 Ind. Eng. Chem. Res., Vol. 47, No. 10, 2008 3743

Figure 27. Comparison of the effective interfacial area, ae (m2/m3) measured by three different authors: (a) Weiland et al.76 on Goodloe packings, (b) Patil
and Sharma94 on HYFlux packings at (b) uG ) 1 m/s and (O) uG ) 2 m/s, and (c) Niranjan et al.93 on HYFlux between uG ) 0.4 and 1.14 m/s.

can be explained from a decrease in surface tension causing an to show this is the phenomenological model for pressure drop
increase of liquid dynamic hold-up and thus, an increase of the in film flow monoliths based on a channel model developed by
probability for the flow channels to be blocked; see Figure 34. Lebens et al.54 that can be applied to any packing. Similarly,
Further work is needed in this respect so that generalized the pressure drop model developed by Stichlmair et al.38 based
correlations can be obtained to predict hydrodynamic parameters on a particle model can also be used for a packed bed reactor.
also for liquids with different surface tensions and viscosities. Since these models are based on physical phenomena occurring
Only limited experimental data has been reported on the heat in the channels, the principles on which the model is based can
transport characteristics from the packing to the heat transfer be applied both to co-current and counter-current mode, provided
fluid for structured packings. This is quite understandable, since the hydrodynamic picture is similar. It is remarkable that RTD
most of the discussed packings were used in distillation measurements show large differences, even for monolithic
processes, and, as a consequence, there was no urge to determine reactors, that are relatively well-defined. In many, if not all,
the heat transfer capacity of these packings. In distillation cases where broad RTDs are reported this is due to maldistri-
processes, the main operation taking place is separation of fluids, butions occurring easily in structured reactors because of the
in which there is no evolution or absorption of large amounts inherent low friction.65
of heat unlike reactive processes. So, heat transfer is no issue. Unfortunately, models based on a full-fledged validation of
The first heat transfer studies carried out on these packings, experimental data are rarely found. A rare example of such
e.g., metal monoliths and corrugated open crossflow structure validation is the work of Lebens et al.48 with respect to liquid
were for gas-phase reactions. The results obtained show a lot hold-up in film flow monoliths. He developed a correlation for
of promise, e.g., very good heat transfer performance of metal liquid hold-up with experimental data validated for liquids of
monoliths. Therefore, it is indeed a right moment to put effort different viscosities, surface tensions and geometries. It is
on the research of heat transfer characteristics of structured important to appreciate the flexibility of such a correlation as
packings for multiphase applications. compared to the one, which is not validated over various relevant
7.2. Measurement Techniques. In order to get a good variables.
appreciation of the correlations presented in literature, it is
crucial to discuss the techniques used to measure gas to liquid 8. Industrial Applications of Structured Packings
mass transfer rates in the packing. Several authors have reported
kLae values, which were determined using physical methods and We expect that the research on the application of structured
represent the gas-liquid mass transfer rates without chemical packings for reactions with strong diffusional limitations,
reaction. In the case of a physical method, which involves the pressure drop constraints and heat transfer limitations will be
transfer of a sparingly soluble gas into liquid, care has to be intensified in the next years due to their obvious benefits over
taken that the saturation value of the gas in the liquid is not random beds. To sum up, we outline a few applications how
approached, leading to inaccuracies in the determination of kLae. the geometry of the structured packing giving rise to useful
This poses a serious limitation for the structured packings where hydrodynamic properties can be exploited to the maximum. A
mass transfer rates are often very high. The high geometric main industrial application of structured packings will be for a
surface areas of many structured packings makes it even more multitubular fixed bed reactor in which the tubes are packed
difficult to carry out reliable experiments as the saturation value with structured catalysts instead of the conventional catalyst
is reached after a relatively short length. Therefore, short lengths particles. Another unique application of structures such as
are used and end effects cannot be neglected. So, it is obvious ceramic monoliths is an adiabatic loop reactor where the heat
that compared to classical packings measurements with struc- is removed in an external heat exchanger. Such a configuration
tured packings deserve more care because of their often high is an easy way to replace a slurry reactor.
mass transfer rates. 8.1. Structured Multitubular Fixed Bed Reactor. This
7.3. Hydrodynamic Models. There is ample information concept can be an ideal retrofit for processes operated in
available regarding hydrodynamic models applicable to mono- multiples of small diameter tubes packed with catalyst. An
liths and open crossflow structures. Many authors summarized excellent example for this application would be the Fischer-
their data in the form of correlations. However, they are usually Tropsch (F-T) synthesis, which is an exothermic reaction
valid only within a certain regime of operation and at the same carried out in multitube reactors.70 This application suffers
time they often have not been validated for low surface tension mainly from pressure drop limitations, the difficulty to remove
and high viscosity liquids. We strongly recommend the use of the heat of reaction, and ineffective catalyst utilization. Since
physical phenomena or mechanism related models as compared the rate of reaction is the highest near the entrance, the
to (semi-)empirical correlations as they are much more realistic possibility of developing a hot-spot near the entrance that might
and can be applied in general to any packing. A good example lead to a decrease in selectivity or even a runaway is high. A
 3744

Table 11. Correlations for Hydrodynamic and Transport Parameters for Foams
reference correlations method geometric properties operating conditions comments
Richardson et al.102 dry pressure drop dry pressure drop measured 10-65 PPI of R-alumina foams uG ) 1-7 m/s experimental dry pressure,
dp/dz ) a0uG + a1uG2 a0 ) Aag2µ(1 - )2/3, with differential pressure drop data follow the
a1 ) BagF(1 - )/3 transducer Forchheimer equation,
A ) 9.73 × 102dp0.743(1 - ) - 0.0982 parameters A and B depend
B ) 3.68 × 102dp-0.7523(1 - )0.07158 on the media properties
Stemmet et al.105 static liquid holdup measuring the liquid holdup, 5-40 PPI Al foam, counter-current relative permeability model
by a weighing technique 30 cm × 1 cm × 80 cm height, uL ) 0-0.03 m/s adequately describes
Ind. Eng. Chem. Res., Vol. 47, No. 10, 2008

S0L ) 0L/ ) [(9 + 0.025Eo*)]-1

total liquid holdup (relative permeability model  ) 0.92 - 0.94 uG ) 0-0.8 m/s the liquid holdup in
of Saez and Carbonell106) the high liquid hold-up
FR/R ) 1/fR(SR)(AReR/GaR + BReR2/GaR)FRg R ) G,L regime in foams
SR ) R/, fG ) SnG1, fL ) (SL - S0L/1- S0L)n2
5 PPI: A ) 8.31 × 105, B ) 25.09, n1 ) 5.17, n2 ) 2.33
20 PPI: A ) 42.1 × 105, B ) 14.03, n1 ) 3.88, n2 ) 1.55
40 PPI: A ) 0.088 × 105, B ) 5.04, n1 ) 4.25, n2 ) 1.73
Stemmet et al.101 gas-liquid mass transfer physical desorption of oxygen 10 and 40 PPI Al foam, co-current upflow prediction of kLae values
no correlation available from water with nitrogen 30 cm × 1 cm × 30/60/90 cm height, uL ) 0-0.1 m/s per liquid vol between
 ) 0.92 - 0.94 uG ) 0-0.8 m/s 0.05-0.6 s-1
Montillet et al.97 residence time distribution of liquid dynamic tracer technique using 45 and 60 PPI Ni foam liquid phase only aqueous system used,
Dax ) 1.26 × 10-3uL for 45 PPI foam polarographic method uL ) 1.1 × 10-3 no effect of gas flow studied,
Dax ) 1.01 × 10-3uL for 60 PPI foam -8.9 × 10-3 m/s axial dispersion found to
be limited
Stemmet et al.101 residence time distribution of liquid dynamic tracer technique by 10 PPI aluminum foam, co-current up flow Dax,L ∝ 1/uG
BoL ) uLZ/(Dax,LL) ) 19 measuring conductivity 30 cm × 1 cm × 30/60/90 cm height, uL ) 0.02-0.1 m/s
at uL ) 0.02 m/s and uG ) 0.1 m/s nitrogen/water system,  ) 0.92 - 0.94 uG ) 0.1-1.0 m/s
BoL ) uLZ/(Dax,LL) ) 50 with KCI as tracer
at uL ) 0.02 m/s and uG ) 1.0 m/s
Richardson et al.96 overall heat transfer coefficient measuring outlet temperature 30 PPI ceramic foams,  ) 0.82, inlet T ) 650-850 °C, radiation effects included
Udt/λf ) 2.49 × 10 -8T3 + 12.6Res for different air flow rates ag ) 26200 m2/m3, air flow rates up to in the correlation
aP ) 4720 m2/m3 50 m3/min
 Ind. Eng. Chem. Res., Vol. 47, No. 10, 2008 3745

Figure 28. Pressure drop per unit length for 5 PPI and 40 PPI aluminum Figure 31. Mass transfer coefficient per reactor volume for 10 and 40
foam in the trickle flow regime.100 5 PPI: (2) only gas; (9) L ) 10.3 (PPI) aluminum foam packings for different liquid velocities in the co-
kg/(m2 s); (b) L ) 17.2 kg/(m2 s). 40 ppi: (4) only gas; (0) L ) 10.3 current upflow configuration: (b) 10 PPI, uL ) 0.02 m/s; (O) 40 PPI, uL
kg/(m2 s); (O) L ) 17.2 kg/(m2 s). ) 0.02 m/s; (2) uL ) 0.04 m/s; and (9) 10 PPI, uL ) 0.1 m/s.101

Figure 29. Static liquid holdup, L0 for aluminum foam packings in the Figure 32. Axial dispersion coefficient versus superficial liquid velocity
range 5 to 40 PPI, plotted against the Eötvös number, Eo*: (--) model of for (b) 45 PPI nickel foam and (4) 60 PPI nickel foam.101
Saez and Carbonell;106 and ([) model of Stemmet et al.105

Figure 33. Nu as a function of Res for (9) 30 PPI ceramic foam and (0)
0.5 mm glass spheres at 800 °C.96

Figure 30. Data and modeling results of the liquid holdup versus ReG using transport can be improved mainly in two ways. One option
model of Saez and Carbonell106 for a 5 PPI aluminum foam.105 Low liquid
hold-up (trickle flow): bottom increasing trend, high liquid hold-up (bubble would be to intensify the conduction to improve the effective
and pulsing flow): top decreasing trend, (0) ReL ) 295; (/) ReL ) 593; radial thermal conductivity and the other option would be to
(+) ReL ) 889; (O) ReL ) 1185; (‚‚‚) model. introduce radial convection, which is not based on mixing flow
patterns. The concept of good radial conduction can be fulfilled
profiled catalytic activity along the reactor bed in which the by a combination of good heat conduction of the packing and
catalyst loading is varied can effectively help in reducing the maximizing the heat transfer at the wall. The former can be
hot spots at the entrance. If a catalyst coating is applied on a realized by applying a metal monolith with thicker walls, e.g.,
structured backbone, the loading can be varied within limits by aluminum, copper, SiC etc. The latter benefits from a conducting
changing the coating thickness. The coating thickness would contact with the wall (see section 6.1). Alternatively, radial
have no effect on the hydrodynamics, as the hydrodynamics convection at the wall can be introduced by applying a
will be determined entirely by the geometry of the structure. corrugated open or closed crossflow packing (see sections 6.2
Another interesting alternative to the option of decreasing and 6.3).
productivity at the entrance is to improve the radial heat transport A third option can be to scale down the radial heat transport
without a proportional increase in pressure drop. The radial heat properties of the structured packing to enable low-pressure drop
3746 Ind. Eng. Chem. Res., Vol. 47, No. 10, 2008

Figure 34. Flow pattern diagram, three-lobed extrudates: (b) air-water,

(O) air-water + cmc; (4) air-water + C12H25SO3Na.108 λ and ψ have the
same meaning as given in Figure 26.

Figure 36. Schematic diagram of a monolith loop reactor with external

heat exchanger.

transfer zones. The mass transfer takes place in the structured

packing and the heat transfer takes place in the external heat
exchanger where the heat of reaction is removed. The conversion
per pass is kept limited to avoid unacceptable temperature rise
in the reactor. An excellent example of a structured packing
which can be used in such an application is a cordierite monolith.
Because of its low thermal conductivity, it works as an adiabatic
reactor. The combination of Taylor flow resulting in high mass
transfer rates coupled with low-pressure drop at high liquid
recirculation rates would result in a reactor configuration ideal
for low conversions. In processes where higher conversion per
pass is desired, an option would be to introduce staged energy
removal. In this option, near-isothermal conditions can be
achieved by removing the heat of reaction stage wise via liquid
Figure 35. Schematic diagram of a multitubular fixed bed reactor with a
circulation through an external heat exchanger.
crossflow structure in the first section of each tube followed by a monolith
structure in the second section of each tube.
9. Comparison between Various Packings
in regions where not much heat needs to be removed, i.e., in
regions of low reactant concentration. An example for this option A comparison between the various structured packings and
would be to choose for a corrugated closed crossflow structure a randomly packed bed is carried out in Table 12. The most
or a metal monolith with a conducting contact with the wall important criteria, which are used to compare the various
for the first part of the reactor tube which demands substantial packings are as follows:
heat transfer rates followed by a monolith for the bottom part 9.1. Catalyst Holdup. Structured packings typically have a
of the reactor tube, thus gaining on pressure-drop (Figure 35). catalyst holdup between 10 and 30%. At first sight this seems
To summarize, the discussed structured packings can be to be a major limitation for processes requiring high catalyst
considered for various applications having heat removal and/or hold-up. On the other hand, new techniques are being developed
pressure drop limitations. However, they should be optimized in which with a good design the structured reactor can sustain
with respect to geometric and total surface area (which will be high catalyst loads. A modeling study was carried out by Desmet
proportional to the catalyst hold-up), G-L/L-S mass transfer and et al.109 to determine the optimal layer thickness in order to
pressure drop. maximize productivity. It is even possible to produce structured
8.2. Adiabatic Loop Reactor. This concept can be applied reactors from catalyst material enabling essentially unlimited
when low conversion per pass is acceptable (Figure 36). This catalyst loading. Of course, this requires a large catalyst
reactor concept very effectively decouples the heat and mass development program.
 Ind. Eng. Chem. Res., Vol. 47, No. 10, 2008 3747

Table 12. Qualitative Comparison of Different Catalytic Packings in Multiphase Flowa

packed bed metal/ceramic knitted wire metal
(base case) monolith OCFS CCFS packing foam
catalyst holdup ++ + + + -b +
short diffusion lengths -- ++ ++ ++ ++ ++
catalyst coating N/A (++) ++ ++ + ? +
radial mixing for mass ( -- ++ +c + +
kLae/∆P - ++ ++ ++ ++ +
axial dispersion + (d ++ ++ ? +e
liquid to solid mass transfer + + ( ( ? ?
heat transport by convection ( -- ++ ++ + +
heat transport by conduction -- +( + + ( ++
pressure drop -- ++ + + + (
convenience for loading into the reactor tubes ( ( ( ( ++f (
a Key: (++) high/very positive; (+) sufficient/positive; (() moderate; (-) negative; (?) not available; (N/A) not applicable. These ratings should be

regarded as a qualitative guideline to select the optimal packing. b The surface area provided by the multifilaments may be reduced after coating. c Because
of the closed channels, the radial mixing can be lower than, e.g., OCFS. d Taylor flow in each channel is close to plug flow but the maldistribution effects
over the complete monolith results into a significant axial dispersion. e Since foam can be considered as an inverted form of a random packed bed with a
high porosity the axial dispersion effects can be similar. f Knitted wire packing is flexible and hence can be pushed along the reactor length easily. But it
is not known if the coating will be sufficiently strong and stable to withstand the friction against the wall during the loading procedure.

9.2. Short Diffusion Lengths. In the case of fast reactions, order reactions because since both phases usually take part in
pore diffusion limitation will occur already with particles of the reaction, axial dispersion can decrease the effective con-
less than 1 mm. This is a realistic argument as due to the rapid centrations along the length which would in turn affect the
development in the area of catalysis, highly active catalysts have reaction rates. Thus, to minimize the adverse effects of axial
been employed for several industrially relevant processes. In mixing, better packing designs should be considered. For
fact it is to be expected that “to be developed” novel generations example, a high porosity packing with regular flow channels
of catalysts will be more active than the present ones. Thus, a such as monolith or OCFS packing may reduce mixing in the
catalyst coated structured reactor with the coating providing gas phase. Similarly packings having good wetting character-
short diffusion lengths is the best alternative to a pore diffusion istics may promote low levels of axial mixing in the liquid
limited fixed bed reactor. phase.89 To support this, in processes where the packing material
9.3. Catalyst Coating. It is important that the support matrix does not wet the process liquid, surface roughening or texturing
of the structure is able to retain the active catalytic material can improve wetting properties of the material.110 For monoliths
under severe conditions such as high flow rates, pressures, and Taylor flow in each channel is close to plug flow, but due to
temperatures. For most, but not all, packings, proven technolo- maldistribution over the channels, this may manifest itself as
gies for coating them with active material are available. axial dispersion.65
Nevertheless, in developing a new process catalyst optimization 9.7. Liquid to Solid Mass Transfer. L-S mass transfer
might be a barrier also for “simple” structured packings. mainly depends on the wetted area and the degree of turbulence
9.4. Radial Mixing. Radial mixing is a strong function of in the liquid phase. Stagnant liquid around the catalyst is not
geometric properties of the packing. If the geometry of the desired because it decreases the intrinsic liquid-solid mass
packing is such that it can create convection in the radial transfer coefficient, kLS. As said earlier, packings with good
direction of the flow or turbulence, then the radial mixing wetting characteristics will help increasing the wetted area.
properties of the packing are generally good. Efficient radial Moreover surfaces which promote turbulence in the liquid-phase,
mixing leads to flat concentration and temperature profiles in resulting in not only liquid films but also drops, jets, and sprays,
the radial direction. The radial mixing characteristics are relevant help to increase the interaction between the liquid and the solid
in heat transport when radial convection plays an important role surface. Monoliths operated in Taylor flow are not as efficient
in determining the radial heat transport properties of a packing. in transferring the liquid to the solid surface as they are in
9.5. Gas to Liquid Mass Transfer. In multiphase reactor transferring the gas to the liquid phase. This is due to the
systems, where gas and liquid compounds react in the presence presence of a liquid film on the channel walls which limits the
of a solid catalyst, or when the reactants are gases which have mass transfer process as the mass is transferred through this
to dissolve in the liquid in order to reach the catalytic sites, the film only by diffusion. It is important to maximize the geometric
mass transfer rate between gas and liquid is important for surface area and to reduce the thickness of the liquid film, by
efficient design of the reactor. Since gas to liquid mass transfer selecting the optimal conditions.
mainly depends upon the fluid properties and flow rates, it is Heat transport in the radial direction is a result of two
possible to increase this rate but most of the times at the expense effects: conduction of the packing and fluids and convection.
of pressure drop. The mass transfer rates obtained in random Depending on the packing geometry and packing material, either
packings are comparable to those obtained in structured packings of the two effects is relevant for a particular case.
provided that the regime of operation is the same (low 9.8. Heat Transport by Convection. Convective heat
interaction) but at a much higher pressure drop. Moreover when transport from the packing to the wall of the reactor tube is the
it is possible to achieve Taylor flow conditions in the structured primary mechanism in packings where convection of mass is
packings, then the mass transfer rates achieved are very high predominant. Good heat transport in the radial direction is a
(see Figure 11) as compared to the random packings. Therefore, result of efficient radial mixing properties of the packing.
overall this makes the random packings highly inefficient in 9.9. Heat Transport by Conduction. In certain packings
terms of the ratio of the mass transfer rate to the pressure drop: such as the monoliths, convective heat transport is completely
kLae/∆P. absent. Nevertheless, the thermally connected nature of such
9.6. Axial Dispersion. In multiphase reactions, axial mixing packings provides in principle for an alternative mechanism of
of both gas and liquid phase is relevant in the case of positive radial heat transport namely conductive heat transport. If suitable
3748 Ind. Eng. Chem. Res., Vol. 47, No. 10, 2008

materials, such as copper, aluminum, etc., and geometries are heat as well. There are several correlations available on
adopted then the thermal conduction through the solid phase phenomena based pressure drop models, which theoretically can
can become significant. be applied to any packing provided the prevalent hydrodynamics
Apart from these most important criteria, there are other support the underlying phenomena. Moreover existing correla-
factors that are also relevant for the comparison, i.e., pressure tions, though mostly developed for aqueous (water-air) systems,
drop and easiness of loading. All the structured packings are already give us sufficient information to look for when we want
characterized by a relatively low-pressure drop. Loading of the to extend them to other systems. Of course, ultimately the
structured packings can be as cumbersome as particles. Because validation of these models with experimental data is necessary
of the defined gap between the structure and the reactor wall, to substantiate their application in co-current two-phase flow
packing methods can be used for, e.g., monoliths, which will applications. Particularly experimental studies with lower surface
improve the heat transfer near the wall but at the same time tension liquids deserve attention as surface tension has a strong
will put their practical feasibility and ease of loading into effect on the contact angle and wetting characteristics affecting
question. Table 12 summarizes the most important properties mainly interfacial area and liquid holdup.
of structured packings and rates them in comparison to a Last, but not least, residence time distributions in structured
randomly packed bed reactor. The rating is largely based on a reactors must be well considered, maldistributions in the gas-
combination of results obtained for single-phase flow and liquid flow may turn their advantage into a disadvantage,
ongoing research in our group on determination of heat and although for monoliths the influence on the conversion is
mass transfer rates in the mentioned structured packings. limited.66
10. Outlook Nomenclature
Changing from a random packing to a structured packing ae ) gas-liquid interfacial area (m2/mreactor/liquid3)
would mean aiming for process-intensification as the new ag ) geometric surface area per unit volume of solid (m2/msolid3)
reactor-type will result in a higher productivity per cubic meter aLS ) liquid-solid interfacial area (m2/msolid3)
of reactor volume and higher selectivity compared to the ap ) geometric surface area (m2/mreactor3)
traditional randomly packed bed reactor. Structures with high B ) channel base (mm)
radial conductivity will enable going to larger tube diameters BoL ) liquid Bodenstein number; BoL ) uLZ/(Dax,LL)
in fixed bed operation. This will not only reduce the material Ca ) Carberry number, ηu/σ
costs but also ease out the loading and unloading procedures CPSI ) no. of cells per square inch (cells/in.2)
as fewer tubes will be required. db ) bubble diameter (m)
Substantial amount of research still needs to be done on dc ) channel diameter (m)
determining and possible improving of the heat transfer rates dcap ) capillary diameter (m)
in the structured packings. If future work confirms the forecasted de ) equivalent diameter (m)
advantages of the structured packings over random packings, it dh ) hydraulic diameter (m)
will be a big boost for commercial processes in which the dm ) average strand diameter (mm)
reactors suffer from heat transfer removal problems. dp ) pore diameter (mm)
dt ) tube diameter (m)
11. Conclusions
Dax,L ) liquid phase axial diffusion coefficient (m2/s)
Structured packings are a promising alternative to the existing DL ) liquid diffusivity (m2/s)
packed bed and slurry reactors. They show flexibility with Eo* ) modified Eötvos number; Eo* ) FLgde2/[σ(1 - )2]
respect to catalyst holdup, hydrodynamic regimes attainable, F ) interfacial force (kg/(m/s))
pressure drop, flow rates, and heat transfer properties, which is f ) relative permeability
not often seen in packed bed reactors. They are important for
Fr ) Froude number; Fr ) u/xgdh
Process Intensification. It is striking that unprecedented high
G ) gas mass velocity (kg/(m2 s))
mass transfer rates can be achieved on the one hand by intense
Gtrans ) gas mass velocity at transition (kg/(m2 s))
turbulence and on the other hand under laminar conditions.
Compared with slurry reactors they are much more convenient Ga ) Galileo number; Ga ) gdh3F2/µ2
and compact. With the fast progress in the area of catalysis, it Gz ) Graetz number; Gz ) ReLScLδ/H
is not too far from now that structured packings will overcome h ) crimp height of packing (mm)
the disadvantage of lower catalyst holdups and higher costs over H ) flow distance (m)
their obvious advantages of higher reaction rates and selectivi- Ka ) Kapitsa number; Ka ) σL3FL/(µL4g)
ties, lower pressure drop, and better heat removal when kL ) liquid side intrinsic mass transfer coefficient (m/s)
compared to packed bed reactors. Unlike packed bed reactors, kLS ) liquid-solid intrinsic mass transfer coefficient (m/s)
structured packings allow the decoupling of intrinsic kinetics, kLae ) gas to liquid mass transfer coefficient (s-1)
transport phenomena, and hydrodynamics making them far more kw ) thermal conductivity of washcoat (W/(m K))
flexible in all respects. ks ) thermal conductivity of support
Still, more work needs to be carried out to quantify the heat K ) parameter, which is a function of packing (W/(m K))
transfer rates in two-phase flow. Since the heat transfer rates in l ) capillary length (m)
single phase flow operation show a lot of promise, it is L ) liquid mass velocity (kg/(m2 s))
worthwhile to spend effort on investigating the heat transport Lbubble ) bubble length (m)
phenomena in two-phase flow systems. After analyzing the gas Lslug ) slug length (m)
phase heat transport studies, we believe that heat transfer Ltrans ) liquid mass velocity at transition (kg/(m2 s))
characteristics of the packings will have an edge over that of N ) no. of pores per inch (PPI) of the foam (in.-1)
randomly packed beds in two-phase flow due to the much Nu ) Nusselt number; Nu ) Udt/λf
effective radial transport of mass generated from the turbulence PPI ) pores per inch foam pore density
created by gas-liquid flow which leads to a better transport of Pef ) Peclet number based on channel size; Pef ) uLdc/(Dax,L)
 Ind. Eng. Chem. Res., Vol. 47, No. 10, 2008 3749

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