Ind. Eng. Chem. Res.

199433, 647-656 647

SEPARATIONS

Effective Mass-Transfer Area in a Pilot Plant Column Equipped with

Structured Packings and with Ceramic Rings
M. Henriques de Brito,t U. von Stockar,’ A. Menendez Bangerterj P. Bomio,t and
M. Lasoil
Institute of Chemical Engineering, Swiss Federal Institute of Technology (EPFL),
CH 1015 Lausanne, Switzerland

The effective area for mass transfer of the Sulzer structured packing Mellapak 125.Y, 250.Y, and
500.Y was measured under industrial-scale operating conditions, with a broad range of gas and
liquid flows, in a pilot plant with a column having an internal diameter of 295 mm and a packing
height of 420 mm. The experimental procedures and apparatus employed in this work were checked
by making additional measurements of the effective area for 25-mm ceramic ring packing; these
values were compared with literature data. This contribution shows that the effective mass-transfer
area for packings 125.Y, 250.Y, and 500.Y can be considerably higher than the defined geometric
area of the packing. The ratio of the effective area to the geometric area is a function of the Reynolds
number defined with the liquid characteristic velocity and the wetted perimeter. The additional
mass-transfer area beyond the fully wetted packing is attributed to liquid flow instabilities, leading
to waves, film detachment, and droplet formation between the sheets. The effect is particularly
important in Mellapak with low specific geometric area.

1. Introduction however, to the necessity of a careful choice of a “suitable

Structured packings have been widely used in separation
columns since they offer an excellent mass-transfer ef-
ficiency while affording a lower pressure drop than
compared to irregular packings. These facts reduce both
fixed and operating costs. Despite the importance of
effective area values for the understanding and design of
absorption equipment, and despite the increased use of
structured packings in industrial separation columns, no
investigation reporting actual measurements with struc-
tured packings of any kind has been published to our
knowledge. Fair and Bravo (1987) suggest a procedure
for estimating effective areas of structured packings. This
will be discussed in section 3.
Therefore, the aim of the present work is to characterize
the effective area of the structured packing. Specific
effective areas for gas absorbers are measured by combining
absorption with a chemical reaction, such that the ab-
sorption rate is independent of the mass-transfer resistance
in the liquid phase. There are also works in which effective
areas were determined simultaneously with the k ~ using
a system to use”. The authors do point out that ”this system
the “Danckwert’s plot method” (Sharma and Danckwerts,
1970). Landau et al. (1977) state that chemical methods
are the only ones which “do not require verification by
another kind of measurement and which can yield from
a single measurement an overall value of the interfacial
area”. The review paper of Guillen et al. (1982) expresses
the same opinion. Landau et al. (1977) draw attention,
reaction” and to the extensive experimental time required.
Table 1 lists those chemical systems which have been
used for determining the mass-transfer area in packed
columns. The sulfite method, employing the oxidation of
NazSOs, has been frequently proposed for giving estimates
of various mass-transfer parameters, such as effectiveareas
and k ~ aaccording
, to the range of reaction rate. Linek et
al. (1981) recommend that “it is not justifiable to adopt
kinetic constants of the reaction reported in the literature;
the constants must be determined experimentally sepa-
rately for each production charge of sulfite”. Delaloye
(1986) carried out such experiments with a wetted wall
column to verify the kinetics of the reaction, but no
reproducible results were obtained. The reaction kinetics
may be very sensitive to trace impurities, so that repro-
ducibility is almost impossible. In view of the results,
further use of the method is not recommended.
The absorption of COz diluted with air into NaOH
solutions is frequently used. Sharma and Danckwerts
(1970) consider that the reaction is a “very convenient
cannot be easily used when effective areas are higher than
10 cm2/crn3because of the evolution of heat”. However,
packed columns present lower values of specific effective
areas. The applicability of this reaction for obtaining
effective area values is discussed in the Materials and
Methods section.

* To whom all correspondence should be addressed. 2. Materials and Methods

+ Present address: Rua Paulisthia 575/71,5440-001 Vila 2.1. Packings. The structured metal sheet packing
Madalena, SBo Paulo, Brasil. Mellapak was supplied by Sulzer Brothers Limited (Win-
* Present address: Woodward-Clyde International, CH 1006 terthur, Switzerland). Performance characteristics of
Lausanne, Switzerland.
Present address: Sulzer Brothers Limited, CH 8401 Win- Mellapak are described by Spiegel and Meier (1987).
terthur, Switzerland. The structured packing Mellapak (see Figure 1)consists
11 Present address: Institut fur Polymere, Swiss Federal In- of cylindrical elements of height h (see Figure 2a-c) made
stitute of Technology (ETHZ), CH 8092 Zurich, Switzerland. of corrugated metal, ceramic, or plastic sheets. In this
0888-5885/94/2633-0647$04.50/0 0 1994 American Chemical Society
648 Ind. Eng. Chem. Res., Vol. 33, No. 3, 1994
Table 1. Measurements of Mass-Transfer Area Using Chemical Methods
reference chemical system used
Bennett and Goodridge (1970) absorption of trace quantities of radioactive C"O2 in NaOH solutions
Bornhiitter and Meramann (1991) absorption of COz into a solution of NaOH
Danckwerta and Guillbam (1966) absorption of pure CO2 into different solutions (NadO,; buffer solutions of KzCOs with KHCOs
and KCIO,NaOH solutions with NaS."Od
Danckwerta and Rizvi (1971) absorption of 0 2 from air into NalsOs with Cos04 88 catalpt
Dharwadkar and Sawant (1985) absorption of C02 in air into solutions of NaOH with NazCOa
Cianetto and Sicardi (1972) absorption of COz in air into NaOH solutions
Jhaveri and Sharma (1968) absorption of @ into different solutions (cuprouschloride and sodium dithionite); absorption of
isobutene in aqueous HISO,
Joosten and Danckwerta (1973) absorption of pure COz into carbonate buffer solutions
Kolev (1973) absorption of Cot in air into solutions of NaOH
KrBbch and K W n (1979) absorption of 0 2 from air into NazSOa solutions with CcSO, 88 catalyst
Lee and Kim (1982) ahsorption of COSin air into buffer solutions (KzCOs. KHCOa, KCI. and NaOCI)
Lineket al. (1984) ahsorption of COSin air into solutions of NaOH
Lineket al. (1974) absorption of pure 0 2 into NazSOs solutions with COS04 88 catalyst
Merchuk (1980) absorption of COz in air into NaOH solutions
Mohunta et al. (1969) absorption of COZin air into a solution of NaOH
Neelakantanet al. (1982) absorption of pure 0 2 in aqueous solutions of ammonium sulfite
Richards et al. (1964) absorption of pure COZinto carbonate buffer solutions with arsenious oxide ions
Riuuti and Brucato (1989) absorption of pure CO2 into a buffer solution K&Os and KHCOs with arsenious oxide ions
Sahay and Sharma (1973) absorption from 0 2 from air in dithionite solutions and absorption of lean CO, in NaOH and
diethanolaminesolutions
Sedelieset al. (1987) absorption of 0 2 into NalSOs solutions
Vidwans and Sharma (1967) absorption of pure COZinto aqueous solutions of NaOH and MEA
Ycshida and Miura (1963) absorption of COSin air into solutions of NaOH and KOH

work, stainless steel Mellapak was used. Besides the

corrugations, the metal sheets are embossed and grooved
horizontally to promote turbulence and improve spreading
of the liquid. The additional area provided by the surface
structure is not taken into account in the nominal packing
area. The corrugations of the metal sheets are inclined by
an angle 8 with respect t o a vertical axis. For the
Mellapak-Y type this angle 8 is 45O (see Figure 2c). The
sheets are arranged vertically and parallel to each other
(Figure Za), so that the corrugations of contiguous sheeta
are inclined alternately by +8 and -8 and, therefore, in the
case of Mellapak-Y type, they run perpendicular to each
other. These corrugations define straight, inclined chan-
nels of triangular cross section through which the gas flows
(a top view of these channels is given in Figure 2b). The
liquid flows down the corrugated sheeta approximately in
countercurrent fashion to the gas.
TheMellapaktypesueedin thisstudywere 125.Y.250.Y.
and 500.Y, corresponding to a nominal specific surface ap
of 125,250, and 500 m2/m3, respectively. Measurements
were also carried out with 25-mm ceramic Raschig ring
packings using the same experimental procedure. These
Figure 1. The Sulzer structured packing Mellapsk.
rings have a geometric area of 195-210 m2/m3,the exact
figure depending on the packing procedure used. In this 1
work, a value of 200 m2/m3was found. Ha < sEi
2.2. The System COrNaOH for Measuring Mass-
Transfer Area. The absorption of COz into NaOH where the Hatta number and the enhancement factor for
solutions occurs with the following chemical reaction: instantaneous reaction are defined for a second-order

CO, + 2 NaOH - Na&O, + H,O (1)

reaction as

(3)
In highly alkalinesolutions, this reaction becomes pseudo-
first order. In mathematical terms, the conditions for
pseudo-firstorder kinetics aregiven as (Danckwerts, 1970) and, respectively,
 Ind. Eng. Chem. Res., Vol. 33, No. 3, 1994 649
corrugated metal sheets
(4) /

It is well-known that reaction 1 is sufficiently fast as

compared to mass transfer that, given the right conditions,
the carbon dioxide cannot be transported far away from
the interface before it reacts. The criterion to be fulfilled
is
Ha>3 (5)
If both criteria 2 and 5 are satisfied, the absorption rate
becomes independent of mass-transfer parameters and is
given by
-
- Liquidflow
Gasflow

Simplified diagram of structured packing

N = nA, = A, = ( k 2 C w ~ D ~ 0 > 1 / 2 ( C i ~ ~ (6)
>
structured packing

The concentration of dissolved C02 at the interface is in

equilibriumwith the concentration of the gas phase at the
interface, as given by

where:

The physical consequence of eq 8 is that the absorption Cross section of pilot plant column
rate is independent of the mass-transfer coefficients but
column
remains directly proportional to the effective interfacial axis
area. Measuring absorption rates therefore enables de-
termination of A, independently from either ki or ko (for
reviews, see: Charpentier, 1981; or Shah, 1979).
In most literature references reporting effective inter-
facial area measurements using this technique, the dif- line of
fusivities and the rate constant needed in eq 9 were
estimated based on the literature. Criteria 2 and 5 are descent
usually checked, but again often using literature values.
However, as shown in Table 2 there is quite a disagreement
on the chemical rate constant in the literature, and errors
in this constant will affect directly the result of the
measurement. For this study, it was thus decided to
determine t#J experimentally, using the same experimental
conditions, the same concentrations, and the same chem-
icals as in the semi-industrial packed column.
Absorption rates were measured in a falling film column e = 45' h = 210 m m
of diameter 27 mm. Two film heights, 80 and 52 mm, a = 60' h,,, = 11.5 b = 32.5 m m
were used. In order to prevent depletion of hydroxyl ions Packing geometry for Mellapak 250.Y
at the interface, NaOH solutions of between 1.6 and 2 M
were used. Lack of OH- ions at the surface, Le., depletion, Figure 2. (a, top) Simplified diagram of structured packing, (b,
violates the pseudo-first-ordercondition and thus criterion middle) crass section of structured packing, and (c,bottom) packing
2 (Danckwertsand Kennedy, 1958). The liquid flow rate geometry for Mellapak 250.Y.
was varied within the relatively narrow bounds that
permitted obtainment of a ripple-free film, and the C02 the conditions for a fast, pseudo-first-order reaction were
mole fraction was varied between 1 and 0.3, the smallest met. The same conclusions were reached from checking
value enabling precise absorption rate measurements.Full criteria 2 and 5. Using a diffusivity ratio for OH-/C02 of
details were given by Henriques de Brito (1992). 1.7 (Danckwerta, 1970) Ei values ranged between 80 and
Figure 3 shows the observed absorption rates as a 280. Based upon simple falling film theory, the upper
function of yica and of the film height. From the slopes limit for k~ could roughly be estimated at 1.3 X m/s
of the two regression lines, the same value of4 was found. which makes the Hatta number 2.8. Realistic k~ values
It is reported in Table 2 in comparison with literature are expected to be lower.
data. The fact that 4 depended neither on yich nor on As the same experimental conditions were also used in
the film height or the flow rate testifies to the fact that the pilot plant column, it is expected that the fast pseudo-
650 Ind. Eng. Chem. Res., Vol. 33,No. 3, 1994

Table 2. Chemical Rate Constants for the Reaction of COz f 3 ) "C by a heat exchanger before the column inlet. The
in NaOH Solutions at 295 K feed solution was supplied by a stirred tank reactor having
CWH, k2,m3 4, a volume of 2.5 m3. Liquid samples were taken above and
reference kmol m4 kmol-l s-l mol m-2 s-l below the packing by means of small purpose designed
Pinsent et al. (1956) 2 6630 collector cups connected to peristaltic pumps. The
Nijsing et al. (1959) 2.07 8550 8.3 X carbonate content was determined by automatic titration
Nijsing et al. (1959) 1.05 5770 7.6 X with 0.1 M HC1. Further details have been given by
Astarita, cited in 2 9580 Henriques de Brito (1992).
Tseng et al. (1988) 2.4. Evaluation of the Results. Equation 8 neces-
Pohorecki and 2 14470 12 X le2 sitates the measurement of the concentration of C02 at
Moniuk (1988)
present work 1.6-2.0 b (7.3 f 0.5) X the gas-liquid interface, where only bulk concentrations
can be measured. If in the pilot column, the gas-phase
a These values have been recalculated from original data for
comparison. b Not determined as such. mass-transfer resistance is negligible, then the gas con-
centration at the interface is approximately the same as
the concentration in the bulk. Spiegel and Meier (1987)
propose a model for predicting the gas side Sherwood
number in structured packings. However, the empirical
n coefficient contained therein was not published. Fair and
t Bravo (1990) suggested that with their publication "from
0 a data plot one can infer values in the range 0.018-0.040".
r Using the value of 0.0338 proposed by Fair and Bravo
4l
(1990):
cn
\
I

0
E
Y

0 . . 1 . 1 ' ' . ' .

0 20 40 60 80 100

Figure 3. Absorption rate versus C02 mole fraction from in a wetted

wall column. Film height: 80 mm (+), 52 mm ( 0 ) .Best fit of data:
80 mm (broken line), 52 mm (solid line).
first-order kinetics are preserved with the same value of
4. The C02 mole fraction in the gas, however, was lowered
to 1% in order to prevent substantial heat release and to
minimize cost. As is shown in Figure 3 , this should not
affect 4.
2.3. The Pilot Plant. The experiments were carried
out under industrial-scale operating conditions in a pilot
plant column with an internal diameter of 295 mm, a
packing height of 420 mm (2 packing elements), and with
a liquid distributor having a high drip point density of 527
points/m2, thus eliminating possible entrance effects. The
pilot plant and associated analytical equipment is de-
scribed elsewhere (Henriques de Brito (1992).
The inlet gas was saturated with water in another packed
column to prevent heat effects due to the evaporation of
the solvent in the column.
The COSwas supplied by a gas manifold (Carbagas AG,
Lausanne, Switzerland) connected to CO2 bottles with dip
tubes. Liquefied C02 drawn from the bottles was gasified
in an evaporator. To measure and guarantee a stable flow
of C02, two mass flow meters (Brooks, model 58513,
Rosemount AG, Baar, Switzerland) were installed in the
pilot plant. The C02 flow could be adjusted up to about
9.2 m3/h. The mixture of C02 with air was homogeneous
due to the installation of four static mixers Sulzer SMV
(Sulzer Brothers Ltd., in Winterthur, Switzerland) in the
pilot plant.
The concentration of COP in the inlet and outlet gas
stream was measured with an infrared gas analyzer (Binos
1, Leybold-Heraeus, Hanau, Germany). This equipment
was calibrated at the beginning of each experiment.
The liquid flow was fed into the liquid distributor at the
top of the column and had its temperature adjusted to (22
PG
sc = -
p&G
Actually, the original model suggests the interfacial area
and not the geometric area in eq lob. For a rough
estimation up was used.
The specific absorption rate is
where Ay accounts for the concentration gradient in the
gas phase. Thus:
Y
k -PG+ @
GMG
The resistance in the gas phase is small if the above ratio
is small. This ratio is almost independent of the C02
concentration in the gas flow. For 250.Y, with F-factors
of 0.85, 1.1, and 2.1 m0.33kgo.6s-l, the ratios given by eq
12 are respectively 16.4%, 14.196, and 8.6%. Some
dependence on packing density would be expected through
the factor kG in eq 12. The packing density governs the
hydraulic diameter and thereby kG (eq 10). Using eqs 10
and loa-c, it is seen that kG is proportional to the geometric
area of the packing raised to the power of 0.2. This means
that the Mellapak type should not significantly affect the
above values. For 500.Y, for a F-factor of 0.85, the ratio
of eq 12 is 14.6%. For 125.Y, for a F-factor of 2.1, the
lowest that will be used, the ratio of eq 12 is 9.8%.
The above values are very conservative. Dharwadkar
and Sawant (1985) estimated 10-15 % resistance to be on
the gas side with the C02-NaOH system for their
 Ind. Eng. Chem. Res., Vol. 33, No. 3, 1994 651
Table 3. Average of the Ratio m/aL (Mass Balance Ratio) Table 4. Estimate in Evaluating the Mass-Transfer Area
average a d a L error, %
for two 125.Y packing elements 1.00 a b remark
for two 250.Y packing elements 0.83
for two 500.Y packing elements 0.70 UL 26 15 for two 125.Y packing elementa
for three 125.Y packing elements 0.88 20 9 for two 250.Y packing elementa
for 25-mmceramic rings with h = 800 mm 1.19 17 8 for two 500.Y packing elementa
20 4 for three 125.Y packing elements
19 4 for 25-mmceramic rings with h = 800 mm
measurements of effective areas in columns packed with
irregular packings. The gas superficial velocity was aG 65 25 for two 125.Y packing elementa
between 0.09 and 0.17 m/s. Yoshida and Miura (1963) 48 21 for two 250.Y packing elementa
37 13 for two 500.Y packing elements Y
suggested that the gas-phase resistance accounted for less 65 27 for three 125.Y packing elements
than 5% of the overall resistance in their experiments 29 4 for 25-mmceramic rings with h = 800 mm
with COz and NaOH. The gas flows were not published.
a Estimate based on an error propagationstudy and on estimations
Both teams of authors did not consider the gas side of the errors in the individual measurements affecting a (Henriquea
resistance in their calculations. In the light of the de Brito, 1992). b Estimate based on the standard deviation in the
uncertainty of the kG estimation and based on the fact final a values (Henriques de Brito, 1992).
that errors due to a possible gas-phase mass-transfer
resistance are within measurement accuracy (see later), n

the effect was not further considered. As mentioned 500

0
8 1I a)
before, this practice is common. / A
A differential mass balance for the COz must be 375
established and integrated together with eq 8 through the
packing height. Assuming a straight operating line, the
integration yields:

(14)

where the logarithmic mean for the gas concentration is

defined as 1254 I
Q
._
Y
5

Ya
In -
Yw
There are then two possibilities for evaluating the effective
specific mass-transfer area, either by measuring the
concentrations in the liquid phase (eq 13) or by measuring
the concentrations in the gas phase (eq 14). The indexes
1250 01 1 2 3 4

L and G were used to distinguish the two equations.
Both quantities have been measured in this work. The
error in the mass balance is given by the ratio of eqs 13
and 14. The average ratios of all measurements for each
packing type are given in Table 3. The mass balance
indicates that the error may be of the order of 20%.
Nevertheless, it should be borne in mind that the uncer-
tainties associated with QG are higher than those associated
with aL (Table 4). Thus, the mass balance check mainly
reflects the uncertainties in measuring aG. The results
given in this work therefore are based exclusively on aL.
All the measurement errors affecting eq 13 have been
estimated individually (Henriques de Brito, 1992). For
example, the F-factor and the specific load are believed
to be known with a precision of *lo% and *l%,
respectively. An error propagation study taking into
account all of these estimations yielded column a of Table
4. Column b is an estimate of the errors based on the
reproducibility of the measurements. The precision of QL
is principally influenced by the evaluation of the parameter
C#J and the carbonate content.
With large F-factors, during the experiments with 125.Y,
there was liquid in the outlet gas samples. Droplet
formation is impeded less by 125.Y than by denser
packings, and some droplet carryover in the gas stream at
F-Factor [m/s dkglm31
Figure 4. Mass-transferarea versus F-factorfor a l l Mellapak types:
(a) Mellapak 500.Y, (b) Mellapak 250.Y, (c) Mellapak 125.Y. The
liquid flow rates used in these experiments were, in ms m-2 h-l, 12.3
(A), 19.8 (W), 40.1 ( O ) , 48.9 ( O ) , 57.7 ( O ) , 71.5 (A).
the top of the column was observed with this packing. The
sampling position had to be changed at a certain stage
and was installed over the distributor, reducing the
likelihood of contact with the liquid drops. After this
change, there was a slight decrease of the concentration
measured at the gas outlet by the gas analyzer.
3. Results and Discussions
3.1. Effective Mass-Transfer Area for Mellapak.
Figure 4 presents all specific mass-transfer area measure-
ments as a function of the F-factor. The error bars are
omitted for clarity.
The values for the specificmass-transfer area for packing
500.Y for a given specificliquid load and F-factor are higher
than those for 250.Y, which in turn are higher than those
for 125.Y. This is in accordance with the expectation that
the effective area increases with the geometric area.
The effective mass-transfer area depends primarily on
the packing and on the specific liquid load. The influence
652 Ind. Eng. Chem. Res., Vol. 33, No. 3, 1994
0 50 100 150
Re,
Figure 5. The ratio ada, as function of the Reynolds number. The
line is the best fit given by eq 17.
of the F-factor is apparently linked to the packing. For
500.Y (Figure 4a), the effective area appears to increase
with the F-factors, whereas a, clearly remains unaffected
in packings with less internal surface. This would be
expected since a given value of the F-factor lies much closer
to the flooding conditions in the 500.Y than in the other
packings.
The horizontal lines of the mass-transfer area with the
F-factor for a given liquid load are in line with the
contention that the gas side resistance is unimportant. A
systematic variation of the apparent a, values with F could
have been interpreted as reflecting the variation of a gas-
phase mass-transfer resistance with F. Given the absence
of such variations, a gas-phase mass-transfer resistance,
if it really exists, would have to be independent of F.
The results for all three packings can be correlated as
a function of only a Reynolds number. The correct
characteristic length to be used in this Reynolds number
is the wetted perimeter, i.e., the total length of all the lines
in Figure 2b. Since in Mellapak, as opposed to random
packings, this length is proportional to the specific
geometric area of the packing, the liquid Reynolds number
may be defined as follows:
Re, = -
PLWL
(16)
FLU,
The resulting correlation for all measurements is shown
in Figure 5. Its mathematical form is as follows:
(17)
It must be stressed that the correlation appearing in
Figure 5 has not been checked with fluids of different
densities and viscosities, since these two variables were
constant at 1077 kg m-3 and 1.177 mPa s (Vazquez et al.,
1989) during this study.
An important consequence of eq 17 is that the ratio of
the effective area to the geometric area increases with
decreasing packing surface at constant specific liquid load.
The specific effective area is dependent on the specific
geometric area to the power of 0.7.
The experimental evidence clearly indicates that the
effective area can considerably exceed the geometric area.
The magnitude of this effect is significantly larger than
the experimental uncertainty. In view of the pivotal
importance of such results, a calibration of the C02-NaOH
system using dumped packings (section 3.3) as well as a
painstaking experimental check of possible additional
factors affecting a, was performed (section 3.2).
Considering the geometry of Mellapak, it would seem
natural to assume that the maximum possible effective
area would correspond to a totally wetted packing (un-
fortunately, it is not possible to visualize the flow inside
the packing, since it is opaque). The evidence, however,
clearly suggests that additional mass-transfer area exists
beyond the geometric nominal value. Although the nature
of this additional area can only be elucidated by further
research, it is conceivable that instabilities in the liquid
flow (like ripples or waves, detachment, and subsequent
fragmentation of the film into copious liquid showers, etc.)
lead to an increased effective area. Such liquid flow
instabilities develop more extensively with the larger film
running lengths and therefore should be more noticeable
with the spacing between corrugations is larger, Le., the
coarser the packing. This is indeed the trend that is
experimentally observed: the fractional additional area
is largest for the coarsest packing 125.Y (Figure 4c).
The possibility of a,/a, ratios in excess of unity is not
mentioned explicitly in the literature, although Bravo and
Fair (1982) note that in dumped packings “the value of
the effective area is composed not only by the wetted area
over the packing but also by the area provided by
suspended and falling droplets, gas bubbles within liquid
puddles, ripples on the liquid film surface, and any
contribution from film falling on the walls of the column”.
In a more recent work, the same authors (Fair and Bravo,
1987) attempt to estimate the effective interfacial area of
structured packings and come up with ada, ratios as high
as 1.2 for Mellapak 250.Y. It should perhaps be noted
that ae/apratios above unity are common in gas/liquid
contactors of completely different kinds, such as spray
towers, where this ratio is actually infinite.
3.2. The Influence of the Drip Point Density and
Packing Height. The liquid distributor in the present
work originally had a drip point density of 527 points/m2.
This was in an effort to minimize entrance effects. The
value corresponds to the upper limit of density used for
research liquid distributors, which should be higher than
300 points/m2 according to Perry et al. (1990).
Some experiments with 3 packing elements of 125.Y
were carried out with 28 of the 36 available drip points
blocked. The resulting drip point density was 117 points/
m2, which is still higher than the value recommended for
industrial operations, quoted at 100 points/m2 by Nutter
Engineering (Perry’s Chemical Engineering Handbook,
1990) and at 130 points/m2 by Fair and Bravo (1990).
With the new drip point density of 117 points/m2 and
using 3 elements of 125.Y,thevalue of the specificeffective
area, a L , for a specific liquid load of 19.8 m3/(m.*h) and
F-factor of 2.65 was 156 f 4 m2/m3. With the original drip
point density, the value of the specific effective area was
160 f 7 m2/m3. This shows that the number of drip points
had a negligible effect on the effective area in the range
of drip point densities used.
For packing 125.Y, the ratio of the specific effective
area to geometric area was the highest of all the Mellapak
types. This packing was therefore chosen to studywhether
a higher packing height would reduce the specific effective
area values by a constant factor, which would reveal that
“dead area” is measured, thus yielding artificially high a,
values.
Table 5 compares data from three packing elements
with two packings for an F-factor of 2.65. This represents
a height increase of 50 % (from 420 to 630 mm). The values
of all other experimental variables were maintained as
before.
Clearly, there is a reduction of the effective area values
of packing 125.Y with packing height. But the fact that
the fractional reduction also markedly depends on the

Table 5. Influence of the Packing Height for Packing
125.Y.
effective mass-transfer area
with an F factor = 2.65, m2/m3
B, 3 packings 2 packings reduction,
m3/(m2h) h = 630 mm h = 420 mm
19.8 160 f 7 207 f 18
40.1 *
185 6 222 f 42
57.7 *
220 11 235 f 13
71.5 250 f 6 265 f 45
a The errors shown come directly from the calculations of the
standard deviation of a set.
300 1
F-Factor [mlsdkglm3]
Figure 6. Mass-transfer area versus F-factor for 25-mm ceramic
rings, The liquid flow rates were, in m3 m-2 h-l, 12.3 ( O ) , 19.8 (m),
40.1 (O), 57.7 (a).The F-factors at flooding conditions for these
liquid flow rates are, respectively (ms-' kp0.5 m-1.6): 1.76,1.50,1.07,
and 0.8 (Eckert, 1970).
specific liquid load suggests that it cannot be attributed
simply to a constant additional area acting as an "entrance
effect". Rather, it is reasonable to suppose that increasing
the specific liquid loads decreases the influence of chan-
neling effects, thus reducing the difference. The same
conclusion was reached by Henriques de Brito (1992) who
compared the measured results with a prediction based
on a numerical model of possible entrance effects.
Bravo and Fair (1982) predicted in their correlation for
irregular packings that the effective area would be
proportional to the packing height to the power of -0.4.
An increase of 50%of the packing height would thus reduce
the effectivearea by about 155%. Consideringthat irregular
packings can be denser than 125.Y and that denser
packings may be less sensitive to an increase of the packing
height, the reduction of effective area values presented by
structured packing is thus not high. The results in Table
5 show that the reduction was less than 17%, except for
the smallest liquid load.
3.3. Effective Mass-Transfer Area for 25-mmCe-
ramic Rings. In order to verify the validity of the results
with structured packings, the effective mass-transfer area
was also measured for 25-mm ceramic rings for which
similar results can be found in the literature for compar-
ison. Figure 6 plots the specificmass transfer, aL,evaluated
from measured data according to eq 13as a function of the
F-factor.
A first important observation is that all values for
effective areas were below the packing's geometric area of
200 m2/m3.
There is a clear dependence of the specific mass-transfer
area on the F-factor even for F-factors far from full capacity
conditions as shown in Figure 6. Such a dependence is
not mentioned in the literature, in which the gas flows
used are rarely cited.
A possible influence of the gas-phase mass-transfer
coefficient &a is difficult to evaluate. The literature does
Ind. Eng. Chem. Res., Vol. 33, No. 3, 1994 653
a 250
T
%
23
17
6
6
.-
,,I
v
%
L
E - 0
0 20 40 60 80
B [m3 m-' h-' ]
- Kolev (1973)
.\\\\.
Yoshida and Miura (1963)
-
Tnis work F-Factor = 0.32
Figure 7. Mass-transfer area versus specific liquid load for 25-mm
rings. Points: this study, with F-factors (in ms m-2 h-l) of 0.32 (m)
and0.47 (0).Lines: measurementapublished by Sahay and Sharma
(1973) (solid black), Kolev (1973) (gray), and Yoshida and Miura
(1963) (hashed).
not consider this mass-transfer resistance. According to
section 2.4, the influence of this resistance should be within
experimental uncertainty.
When trying to compare these results with published
data, it is important to use only literature references
reporting measurements of effective mass-transfer areas
done in actual columns packed with 25-mm ceramic rings.
Work on wetted area and on indirect determinations of
wetted or interfacial area probably do not constitute a
reliable basis for quantitative comparison. A careful
analysis of the literature compiled in Table 1 revealed
that the only reports on chemically determined mass-
transfer area in columns pertaining to 25-mm ceramic rings
are those by Sahay and Sharma (19731, Kolev (19731, and
Yoshida and Miura (1963). The curves were reproduced
in Figure 7 after extrapolating for liquid loadings higher
than 30 m3/(m2h), or in the case of Kolev (1973),the data
was recalculated for the experimental conditions used in
the present study. The widely used correlation of Onda
et al. (1967, 1968), which is based on a large number of
experimental data including 25-mm ceramic Raschig rings,
was also examined and compared with the above data.
The predictions of this correlation for the system used in
the present work agrees to better than 10%with the values
obtained by Sahayand Sharma (1973)and by Kolev (1973)
(Figure 7) in the whole range of liquid loads.
The measurements of this work are somewhat higher
than those reported in the literature (Figure 7). For a gas
velocity of 0.3 m/s, the curves reflecting the literature
values obtained by the chemical method are between 5 %
and 20% lower than the present results. The difference
is within the experimental uncertainty, but it appears to
be systematic.
In order to understand the differences between the
chemical absorption measurements, it is important to
examine the experimental conditions used by the various
authors. Table 6 presents the column characteristics and
the range of flow rates applied by the four works used for
comparison.
The lower results obtained by Yoshida and Miura (1963)
may be due to the unreasonably low ratio of column
654 Ind. Eng. Chem. Res., Vol. 33, No. 3, 1994
Table 6. Experimental Conditione from t h e Literature
column characteristics ratio
ref no.a height, mm diameter, mm d/d, h/d
1 870 200 8 4.8
2 1900 190 7.6 10.0
3 762 121 4.8 6.3
this work 800 295 11.8 2.7
a Ref no.: 1, Sahay and Sharma (1973); 2, Kolev (1973); 3, Yoshida and Miura (1963).
diameter to packing size they used. Low column diameters
with respect to packing size is known to distort the
performance through wall effects. Vidwans and Sharma
(1967) have shown that the effective interfacial area of
3/s-in.ceramic rings increases by 15-20% when the column
diameter is increased from 43.7 to 100 mm and recom-
mended a minimum value of 8 for the ratio did,. On this
account, the solid line on Figure 7 is clearly the more
reliable reference for comparison.
The high aspect ratio (hid) employed in all literature
studies might also have influenced the data. A large packed
height as compared to column diameter enhances mal-
distribution of liquid and thus reduces the effective in-
terfacial area. This has been proven explicitly by Yoshida
and Koyanagi (1958)who assessed the effective interfacial
area of 25-mm ceramic rings using an indirect physical
method. Increasing the packed height of a 120 mm di-
ameter column from 203 to 406 mm resulted in an average
decrease of a, of about 22 % . Since the aspect ratios of the
packed beds used in the literature studies reported in Table
6 were larger than for the present study by a factor ranging
from 1.8 to 3.7, this effect may well be the major reason
for the observed differences. The data of Kolev (1973)
and of Yoshida and Miura (1963) might also be low
compared with the present work due to the possibility
that they might have used lower gas flow rates than the
0.3 m/s used for comparison. The same remark holds for
the general correlation of Onda et al. (1967, 19681, which
does not contain a term reflecting the influence of the
F-factor.
In summary, the effective interfacial areas of 25-mm
ceramic Raschig rings measured in this study agree to
within experimental uncertainty with comparable liter-
ature sources, and the slight but consistent deviation to
higher values can be explained by several factors, most
notably by the higher aspect ratios of the packed beds
used in the literature studies. The high ae/up ratios
obtained for the structured packings (section 3.1) must
therefore be accepted as real. Even if one assumed that
the discrepancy between the literature and this study
resulted from a systmatic measuring error and if hence
the a, results on the structured packing were corrected by
lowering them between 5 and 20% the ue/apratios would
still exceed unity by so much that the evidence could not
be explained away as an artifact.
3.4. Comparison of Effective Areas between Struc-
tures and Irregular Packings. A comparison of ef-
fective areas predicted by correlation 17 for structured
packings of up = 200 m-1 with our measured values for
random packings of the same up appears in Figure 8.
Clearly, the former offer higher effective areas than the
latter. In other words, the ratios of effective to geometric
area tend to be higher in structured packings, to the point
of even exceeding unity.
Ratios of ada, in excess of unity have even been reported
for irregular packings. Bornhutter and Mersmann (1991)
have measured ratios for modern irregular packings of
large size up to 1.5. According to Linek et al. (1984),
hydrophilized plastic Pall rings of 25, 35, and 50 mm do
B, m3/(m2h) range WG,m/s method used
40 0.3 chemical absorption
not given not given chemical absorption
30 not given chemical absorption
12-71 0.3-1.1 chemical absorption
400 1 i
0 20 40 60 80 100
B [m3m-2h" ]
Figure 8. Comparison of effective mass-transfer area for Mellapak
line and 25-mm ceramic rings (a, = 200 m2/m3and F-factor = 0.4).
present ratios of the effective area to the geometric area
of up to 1.2, and Sahay and Sharma (1973) have measured
effective areas of 25-mm stainless steel Pall rings 1.16times
higher than the specific geometric area of the packing.
Several other studies also indicate the possibility of a,la,
ratios in excess of unity on theoretical or semitheoretical
grounds (Schulthes (1990),Kolev (19731,Ondaet al. (19671,
Shi and Mersman (1985)).
This discussion suggests that the effective interfacial
area in randomly packed columns can be augmented by
such effects as liquid flow instabilities, waves, film
detachment, and droplets, but to a much lesser extent
than in structured packings.
4. Conclusions
The effective interfacial area of several types of struc-
tured packings and of 25-mm ceramic Raschig rings has
been measured under conditions pertinent for industrial
operations.
All three types of Mellapak studied can provide an
effective mass-transfer area higher than the geometric area
defined by the packing surface up to a factor of 2,
depending on the liquid and gas flowsand on the geometric
area of the packing. Although the mechanism responsible
for it remains to be studied in detail, it is suggested that
it is due to liquid flow instabilities between the sheets,
such as waves, film detachment, and droplets. This
phenomenon is especially prevalent in the packings of
relatively low geometric area often used in large-scalemass-
transfer equipment and is less pronounced in packings
with high up.
In measurements carried out with 25-mm ceramic rings,
no values of a, were found to exceed up. The measured
values agreed to within experimental uncertainty with
those literature references reporting comparable column
configurations. The fact that the experiments of this study
consistently yielded slightly higher values can be explained
by several factors that might have lowered the results
reported in the literature with respect to the measuring
conditions employed here. At any rate, these differences
 Ind. Eng. Chem. Res., Vol. 33, No. 3, 1994 655
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Receiued for reuiew November 11, 1993
Accepted December 1, 1993.
* Abstract published in Advance ACS Abstracts, February 1,
1994.