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Chemical Enclineerim d Science, Vol. 53, No. 3, pp. 495 5(13, 1998
1998 Published by Elsevier Science Ltd. All rights reserved
Printed in Great Britain
0oo9 250998 $19.00 ~-o.l~)

PII: b01109-2509197)00320-5

Mass transfer in wetted-wall columns:

Correlations at high Reynolds numbers
Christian H. E. Nielsen, Soren Kill, Henrik W. Thomsen and Kim
Department of Chemical Engineering, Technical University of Denmark, DK-2800 Lyngby,
(Received 11 April 1997; accepted 14 August 1997)
Abstract--The rate of gas- and liquid-phase mass transport in a pilot-scale wetted-wall column
with an inner diameter of 3.26 cm and a length of 5 m was investigated. Empirical correlations
for the physical liquid-phase mass transfer coefficient (k) and the gas-phase mass transfer
coefficient (kG) were determined. In dimensionless form, the correlations are given by
ShL = 0.01613 Re 664 Re 426 Sc~)5
Sh~ = 0.00031Re~ 5 t~et,n0.207 ~c~;"o.
and are valid at gas-phase Reynolds numbers from 7500 to 18,300 and liquid-phase Reynolds
numbers from 4000 to 12,000, conditions of industrial relevance. To our knowledge, no
correlations for ShG have been reported in the literature which are valid at such high Reynolds
numbers. The wetted-wall column was equipped with six intermediate measuring positions for
gas and two for liquid samples, giving rise to a high accuracy of the obtained correlations. Our
data showed that ShL and Sh~ both depend on Rea and ReL due to changes in the interfacial
area at the high Reynolds numbers employed. The presence of inert particles in the liquid-phase
may influence the rate of mass transport, and experimental work was initiated to study the effect
on k~. A decrease in ka of up to 15% was seen at solid concentrations ranging from 0 to 30 wt%,
though the observed effect could not be correlated. ,,~' 1997 Published by Elsevier Science Ltd
Keywords: Wetted-wall column; mass transport: correlation; inert particles; transport area.


The falling film principle (i.e. wetted-wall column) is

used in many different industrial applications for mass
transfer between fluids, e.g. sulphonation of organic
products and cleaning of flue gasses (Elvers et al.,
1992). The rate of mass transfer in wetted-wall columns has been extensively investigated because this
type of equipment is simple in design and the falling
liquid film is assumed to have a fixed and known
interfacial area. The latter is the case for most laboratory-scale columns using a laminar liquid film without
waves or ripples, but in studies employing pilot- or
full-scale columns with turbulent and wavy liquid
films, the interfacial area is unknown and the subsequent data analysis becomes more complex.
Transport area
A number of investigators, e.g. Stirba and Hurt
(1955), Brauer (1956), Tailby and Portalski (1960),

* Corresponding author. Tel.: 4545 25 28 45;

fax: 45 4588 22 58; e-mail:

Jepsen et al, (1966) and Portalski and Clegg (1971),

have studied the increase of the interfacial area due to
waves on the liquid film. The extent to which the
interfacial area increases is in dispute. Brauer (1956),
for instance, observed a 0.5 to 3% increase, whereas
Tailby and Portalski (1960) found an increase of up to
50% for water films (Re L ~ 200-2000 and no gas flow).
Attempts to describe the formation of waves and
incorporate the effect on the rate of mass transport
have been conducted by Barrdahl (1988), Wasden and
Dukler (1989, 1990) and Yoshimura et al. (1996). High
gas flow rates may also influence the wave formataon
on the liquid film, as will be shown in this work.
Gas-phase mass transfer coefficient, k~
The rate of gas-phase mass transport in wetted-wall
columns has been examined by a large number of
investigators, of which the best-known study is perhaps that of Gilliland and Sherwood (1934). A comprehensive review is given by Spedding and Jones
(1988), who summarized 31 mass transport studies in
wetted-wall columns published prior to 1978. Table 1
shows some of the more important studies on
gas-phase mass transport available in the literature.


C. H. E. Nielsen et al.











Gilliland and Sherwood (1934) found that the gasphase mass transfer coefficient is pressure-independent in the investigated range from 0,145 to 3.06 atm,
but dependent on R % . The liquid flow was kept
constant (Re L ~ 1000) and so the dependency of Sh e
on Ret~ was not investigated. Using the Reynolds
number calculated relative to the column wall, R % ,
rather than the Reynolds number relative to the liquid
film surface, Rear, they found it feasible to correlate
both countercurrent and cocurrent mass transfer data
with just one correlation. Kafesjian et al. (1961), on
the basis of their own measurements and data from
the literature, including those of Gilliland and Sherwood (1934), determined a dimensionless correlation
for Sh G with a dependency on both Re a and Re L. The
dependency on S % was not investigated and no experimental temperature was provided in the paper,
preventing recalculation of the correlation with Sc 5
G '
which is the correct dependency on S % as reported
recently by Dudukovi6 et al. (1996). They showed that
the relative errors of the Gilliland and Sherwood
(1934) and Barnet and Kobe (1941) data are reduced
when the theoretical Schmidt number exponent of 0.5
for gas/liquid mass transport is used rather than the
theoretical exponent of 0.33 for gas/solid mass transport or an experimental value for the exponent of 0.44
found by Gilliland and Sherwood (1934). Braun and
Hiby (1970) studied the effect of humidity, H, on Sh G.
They found Sh e to be independent of H for H > 80%,
but dependent on the column height, L, and R% and
Re L. However, the correlation is only valid for
L i d i < 35, making it unsuitable for use on pilot- and
industrial-scale columns. Thus, published correlations
for She are valid at low liquid-phase Reynolds numbers only. There seems to be no correlations available
for the design of columns employing liquid-phase
Reynolds numbers of 5000 or higher. It is one of the
aims of this work to determine an empirical correlation for She, valid at industrially relevant flow conditions (i.e. high Reynolds numbers).

d~ X
Physical liquid-phase mass transfer coefficient, k











The rate of liquid-phase mass transport has also

been investigated by a large number of researchers,
some of whom are listed in Table 2. The pressure
dependency of k was studied by Yoshida and
Arakawa (1968) in a stirred autoclave. They absorbed
O 2 into distilled water and found that k is pressureindependent up to 4 atm. Lamourelle and Sandall
(1972) studied absorption in wetted-wall columns
with heights from 91 to 188 cm. Their data showed
that Sh L depends on Rec and S % raised to the power
1.506 and 0.5, respectively. No dependency on Re;
was found because no gas flow was applied. Henstock
and Hanratty (1979) investigated absorption in
a cocurrent wetted-wall column and found that Sh L
depends on both R % and Re L. They correlated their
data by assuming that the absorption is controlled by
eddies in the liquid film. Yih and Chen (1982) studied
absorption of 0 2 and CO 2 in a wetted-wall column
and showed that Sh~ depends on Re L and Sc L raised

Mass transfer at high Reynolds numbers

~X ~






"~ +




C. H. E. Nielsen et al.


to the powers of 0.6804 and 0.5, respectively. Palen

et al. (1994) derived a semi-empirical model for the
interactive heat and mass transfer phenomena in
a wetted-wall column and found Sh L to be a function
of Re L and Sc 5. Thus, though most investigators
agree on the Sc number exponent, inconsistencies
among the reported exponents for Re L and R % are
now clear. In this work, we demonstrate a new empirical correlation for Shi, based on three measuring positions in the column.
Inert particles
The effect of inert particles in the liquid phase on
the rate of mass transport may be important in the
design and modelling of industrial processes employing three-phase slurry reactors (Ramachandran and
Chaudhari, 1983; Beenacker and Van Swaaij, 1993).
Beenackers and Van Swaaij (1993) published a comprehensive review on the subject and it appears that
more work has been conducted to determine the effect
on kL than on k~. For bubble columns and stirred
tanks, it has been shown that the effect of inert particles on the rate of mass transport depends on the
size, concentration and type of particles. The observed
effect is, in most cases, a reduction in the rate of mass
transport, but enhancement has also been measured
at low solid concentrations, typically less than
10 Vol%. To our knowledge, no similar investigations
have been conducted in wetted-wall columns despite
the relevance to industry. Part of this work involves
some initial investigations in the field.
The first objective of this work was to determine
empirical correlations at high Reynolds numbers for
the dimensionless mass transfer coefficients, Sho and
Sh L, in a pilot-scale wetted-wall column. The correlations can be used in design of industrial falling film
columns due to the validation at high Reynolds numbers. The second objective was to examine the effect of
inert particles present in the liquid phase on the gasphase mass transfer coefficient, k~.

A dimensional analysis (Bird et al., 1960) was conducted on the setup to predict the dimensionless
groups in terms of which Sh a and Shl~ may be correlated. It was assumed in the analysis that the liquid
film is plane. The analysis showed that, theoretically,
S h L depends on Re~. and SCL, whereas Sh G depends on
R % and Sc~ for L/di>>l. The latter criterion was
found to be valid for all measurement positions in the
applied column. The dimensional analysis does not,
however, provide any information on the functional
relationship of the dimensionless groups. It will be
shown later that experimental data suggest that Sh~
also depends on Re L and Shr. on Rea. The reason for
this is probably the formation of waves or ripples on
the liquid film at high Reynolds numbers which alter
the interracial area and cause more turbulent fluid

flow. Upon correlating the mass transport data, it was

found that the well-known form, given by eq. (1),
describes the data well.
Sh = klRe k 2Rel)k Sc k4 .


As mentioned earlier, the correct value for constant k4

has been shown theoretically and experimentally to be
0.5 in correlations for both Sh L and Sh~. There exists,
to our knowledge, no theoretical basis for choosing
the functional form ofeq. (1) to correlate mass transfer
data. Thus, the functional relationship of dimensionless groups in eq. (1) is purely empirical.


The experimental setup is shown in Fig. 1. All pipes

and vessels are made of PVC, glass or stainless-steel
coated with Teflon. The main components are the
wetted-wall column, the holding tank, and the film
distributor (pictured in Fig. 2). The column is a vertical, transparent PVC tube, 5 m in length, and with an
inner diameter of 3.26 cm. The holding tank is made
of PVC and it holds a volume of 110 1. The tank is
equipped with four baffles, a stirrer, an air spiral with
nozzles, and a flow loop allowing measurements of
temperature, pH and the 0 2 concentration in the
liquid phase. The film distributor is made of glass and
has an inner diameter of 10 cm and a coated stainlesssteel bottom plate. The distributor ensures a uniform
liquid film on the inner surface of the column tube.
The L-pipe mounted in the bottom plate of the distributor yields a rotating liquid flow and a liquid cone
rises as illustrated in Fig. 2. The gas flow is supplied
by a compressor and the liquid is recycled by a hose
pump. The fluid temperatures are controlled by three
heat exchangers, A water nozzle is mounted at the top
of the gas heat exchanger to ensure humidification
(exceeding 80%) of the gas phase.
Gas and liquid samples can be withdrawn from the
column by two types of probes, both of which are
illustrated in Fig. 3. The gas probes are made of
stainless-steel (~6") and designed to cause minimal
disturbance of the liquid film. The cuvette (liquid
probe) for the insertion of the oxygen electrode is
made up of transparent PVC and fitted with a hole to
ensure a steady liquid flow through the cuvette. The
cuvette was removed from the column when not in use
to avoid disturbance of the liquid film. The gas
samples were analyzed successively on-line at six positions in the column tube (, 1, 2, 3, 4 and 5 m from the
column top) and at the gas inlet. The liquid samples
were analyzed successively on-line at two intermediate positions (2 and 4 m measured from the column
top) and at the liquid inlet.
Calculation methods
A differential mass balance over the gas phase for
the absorbed component produces the following

Mass transfer at high Reynolds numbers

" 'SO~_


' HzO

Film distributor
Atr m
Gas probe


Liquid probe\

Wetted-wall column

Gas analyzer
Hold tank

Flow loop for
measuring pH ect.



Fig. 1. Experimental setup of pilot-scale wetted-wall column.

Gas inlet

Gas probe

Liquid probe
Liquid out

Oxygen electrode
Volt signal to PC

Wetted-wall column

Corm, cting piece

for Pt 100

Absorber tube


Liquid inlet

Fig. 2. Schematic illustration of the liquid film distributor.

Gas to sample train

Fig. 3. Schematic illustration of the gas and liquid probes.

C. H. E. Nielsen et


Table 3. Experimental parameters and dimensions

equation for calculation of k G

k a = z(di _





where R A is the ratio of the interfacial area in the

presence of waves to the plane interfacial area. The
liquid film is not plane at high Reynolds numbers
yielding R A > 1, and a correction factor, a C, is introduced and defined as

( di - 26L~R A.
ac = \
di ]

Q G l n ( C~'in ~ = kGacL.


In this way, all uncertainties concerning the interfacial

area are lumped into the final data, expressed as kza~.
The modified gas-phase mass transfer coefficient,
kza ~, is calculated as the slope of a straight-line fitted
to the seven successive on-line measurements and the
column height. All slopes are determined by the
method of least squares with a confidence level ~>0.95.
An equation for k is obtained in a similar way

The calculation of ka~ is based on three successive

on-line measurements. The concentration at the interphase, CL, u in eq. (5) is calculated using Henry's law

Cl~,i - HO.

1 atm
5, 110, 180 #m
5, 10, 20, 30 wt%
5.0 m
3.26 cm

Table 4. Physical parameters at 50'C


QLln(CL,i = CL,o,.,t) = kOa~L.

rcdi \ CL.i -- CLAn//

Liquid flow, QL
Gas flow, Qc,, at 50C and 1 atm
Temperature, T
Pressure, P
Particle mean diameter, dp
Solid concentrations, 4,,
Height of column, L
Inner diameter of column, d~


Equation (2) is rewritten by the use of eq. (3) and the

following expression is obtained:




The partial pressure of the absorbed gas, p, is obtained

from the gas-phase measurements and the Henry constant, H , is calculated by the semi-empirical correlation presented by Harvey (1996). H is assumed
independent of the humidity level of the gas phase. All
the experiments were conducted at 50C and the pressure in the column tube was maintained at 2 to 5 cm
of H 2 0 above ambient pressure to prevent a leakage.
Experimental parameters and dimensions are listed in
Table 3 and the physical parameters in Table 4.
The most accurate way to determine k~ in
gas/liquid systems is to eliminate the liquid-phase
mass transfer resistance while measuring k~ and vice
versa for k . This can be done by choosing a suitable
chemical system as shown below.

The S 0 2 / N a O H system
To obtain data for k~, a system in which lean SO 2
( ~ 1000 ppmv) was absorbed into a strong N a O H
solution (pH > 11.9) was used. In this system, the
liquid-phase mass transfer resistance can be con-

988.04 kg/m a
1.0928 kg/m 3
546.8 x l0 -6 kg/ms
19.6x10 6kg/ms .
1.22 x 10- s mZ/s

Water density, p*
Dry air density, p*
Water viscosity, p~
Air viscosity,/~
Diffusion coefficient for
SO2 in air, Ds*o2
Diffusion coefficient for
02 in water, D~o:
Henry constant for 02, H *

3.93 x 10 9 m2/s
32.94 x 10- 3 atm l/mg

*Dean (1992) and Weast (1986).

*Andrussow et al. (1969).
*Harvey (1996).

sidered negligible as verified theoretically for

pH > 11.3 by the criterion for an instantaneous irreversible reaction (Levenspiel, 1993)

k~Pso 2 <<,kLCNaOH


where k and k~ were calculated from the correlations

presented in this paper and at experimentally fixed
conditions with pH values ranging from 11.6 to 13.2.

The 02/H20 system

Data for k was obtained by absorbing 0 2 from air
into distilled water with a low concentration of 0 2.
The O 2 in the feed water was removed by blowing N 2
through the air spiral in the bottom of the holding
tank. The gas-phase mass transfer resistance was assumed to be negligible because O z has a low solubility
in water and the 0 2 concentration in atmospheric air
is as high as 20 Vol%. According to Astarita et al.
(1983), the gas-phase mass transfer resistance is negligible if




A worst-case calculation, using the correlations of this

work, showed that the criterion was met in all the
cases considered.

Entrance and exit effects

During the experiments, no exit effect was observed
in the column and the effect of the liquid cone in the

Mass transfer at high Reynolds numbers

film distributor was accounted for as an additional
height added to the physical column height.


Correlation for kGa~


The modified gas-phase mass transfer coefficient,

k~a~, was investigated at different gas and liquid flow
rates and calculated by eq. (4). Experimental data and
the fitted correlation, given by eq. (9), are compared in
Fig. 4, in which Sh~/Sc 5 is plotted against Re~ for
four different values of ReL. The correlation is based
on 97 data points and predicts the experimental data
with a mean deviation of 2.7%:

Sh~; = O.O0031Re~SRe2TSc 5.

Correlation Jor kac

The modified physical liquid mass transfer coefficient, k~)ja,.,was measured for four gas and five liquid
flow rates. The 115 data points are compared with
eq. (10) in Fig. 5.

Sh L = O.Ol613Re664Re"*Z6Sc s.


Equation (10) predicts the experimental data with

a mean deviation of 12.1% and is valid for
Retr[4,000; 12,000] and R e ~ [ 7 , 5 0 0 ; 18,300] at
50 C. Fig. 5 shows the effect of Re~ and ReL on
ShL::ScI~'2. Here, the experimental data are more scattered than those obtained for k~ (Fig. 4). The reason
for this is that ShL/Sc 1:2 is based on liquid-phase
concentrations which (due to small variations in the
liquid flow) cannot be obtained with as high an accuracy as the gas-phase measurements. The increase in
the rate of mass transport with increasing liquid flow
can be explained by increased liquid film turbulence
and interfacial area. It has not been possible to separate the two effects. The exponent of ReL (0.426) in eq.
(10) is smaller than those reported previously in the
literature, e.g. 1.506 (Lamourelle and Sandall, 1972)
and 0.6804 (Yin and Chen, 1982). The exponents
found by Lamourelle and Sandall (1972) and Yin and
Chen (1982) should be the same because their type of

x ReL=12000
a ReL= 9500
ReL= 7000
o ReL= 4700



The correlation is valid for Re~ ~ [-7,500; 13,500] and

Ret~ [4,700; 12,000] at 50='C. It can be seen that ShG is
a function of both ReG and ReL. The dependency on
ReL is probably due to changes in the interfacial area
and increased turbulence of the fluid phases. The data
were also correlated by using Reynolds n u m b e r calculated relative to the liquid film, Re~,. In this way,
the influence of the liquid flow is built into the gasphase Reynolds n u m b e r and the Ret term can be
omitted in eq. (1). However, in agreement with the
work of Kafesjian et al. (1961), this correlation
method gave no satisfactory results, and eq. (9) is
recommended. It was not possible to find any suitable
correlations in the literature for comparison with
eq. (9) is recommended. It was not possible to find any
suitable correlations in the literature for comparison
with eq. (9) because earlier investigations were conducted at lower Reynolds numbers than those used in
this work.








Fig. 4. Experimental gas-phase mass transfer coefficient

data (symbols) compared with fitted correlation eq. (9) (solid


* R%= 18300
600 ~_ Re~-=12200.
o R%= 9900
Re~= 7600


- - Y~," /





7 0 0 0 9000

11000 13000

Fig. 5. Experimental physical liquid-phase mass transfer

coefficient data (symbols) compared with fitted correlation
eq. (10) (solid line).

experiment and setups are almost identical. No explanation for this inconsistency could be found. Figs 4
and 5 both show that the effect of increasing Re~ is to
enhance the rate of mass transfer. This is probably due
to more gas-phase turbulence and/or an increased
interfacial area. It is apparent that k~ac has a stronger
dependency on Ret. at high values of Re~ than at low
values. In Fig. 6, eq. (10) is compared with the correlation given by Henstock and Hanratty (1979). It can be
seen that the correlation of Henstock and Hanratty
(1979) predicts a physical liquid-phase mass transfer
coefficient significantly higher than eq. (10) at all
values of Ret. and has a stronger dependency on Rea.
The Henstock and Hanratty correlation suffers from
the disadvantage of having a strong dependency on
the falling liquid film thickness. An increase in the
liquid film thickness of as little as 0.2 m m reduces the

C. H. E. Nielsen et al.




Present work


Henstock and
Hanratty (1979)

Rec,= 18000




/ ~, ~"



R%= 7500




R%= 7500




9 0 0 0 11000 13000

Re L
Fig. 6. Comparison of fitted correlation eq. (10), with the
dimensionless correlation of Henstock and Hanratty (1979).

predicted values of k by the Henstock and Hanratty

correlation to almost the same level as predicted by
our correlation. Also, the dependency on ReG turns
out to be the same as for our correlation. A comparison of correlations, reported in the literature, for
prediction of falling liquid film thicknesses reveals
deviations of up to 0.4 mm in the range of liquidphase Reynolds numbers applied in this work. As
a consequence, the applicability of the Henstock and
Hanratty correlation seems questionable. In fact, this
is the case for all empirical mass transfer correlations
having a dependency on the liquid-film thickness at
high liquid-phase Reynolds numbers.

The gas- and liquid-phase mass transfer coefficients, koa,. and ka~, were measured for a broad
range of gas- and liquid-phase Reynolds numbers in
a pilot-scale wetted-wall column at atmospheric pressure and 50~C. Two empirical dimensionless correlations which describe the experimental data with mean
deviations of 2.7 and 12.1% were found. The correlations are valid at high Reynolds numbers, conditions
of industrial relevance. It was shown that the increased interracial area and turbulence, due to waves
on the liquid film, are of significant importance. The
effect of inert (sand) particles present in the liquidphase on kGac was investigated at solid concentrations
ranging from 0 to 30 wt%. At high solid concentrations, the effect was seen as a reduction in koa,. of up to
15%. The data obtained at low solid concentrations,
however, were too scattered for the results to be
correlated. More work needs to be done to clarify and
correlate the effect of inert particles on the mass transfer coefficients in wetted-wall columns.
This work was carried out as a part of the CHEC (Combustion and Harmful Emission Control) research programme.



correction factor for the interfacial area,

concentration, kg/m 3, ppmv

inner diameter of the column tube, m
mean particle diameter, m
diffusion coefficient, mZ/s
modified Martinelli parameter, m/Re 9,

RA(di - 2;)L)/di

Inert particles
The effect of inert particles present in the liquid
phase on the rate of gas-phase mass transport was
investigated. The particle type used was sand with
three different mean diameters, 5, 110 and 180pm.
The applied solid concentrations were 0, 5, 10, 20 and
30wt%; the initial liquid volume in the system
was kept constant at 30 1. Also, the gas and slurry
flows were kept constant at Rea = 11,000 and
QL = 7.9 l/rain. The results showed a reduction of
about 15% in koa,. at the high solid concentrations. At
low solid concentrations, however, both reduction
and enhancement of koa,. was observed, preventing
correlation of the data. No explanation could be
found for the scatter of the data, and the above conclusions are strictly qualitative. A number of investigators (e.g. Joosten et al., 1977; Oztiirk and Schumpe,
1987) have examined the effect in bubble-column
slurry reactors. Their results are somewhat similar to
ours, with enhancements of ka at low solid concentrations and reductions at high. It is thought that the
change in k~ a~ is due to a dilution and/or stabilization
of the liquid film by the solid particles. However, more
work needs to be done in this important field before
the data can be correlated.




(~L/~G)(P~/PL) s
gravity, 9.82 m/s 2
Henry's constant, atm m3/mol
gas-phase mass transfer coefficient, m/s
physical liquid-phase mass transfer coefficient, m/s
dimensionless empirical constants
height of column tube, m
dimensionless liquid film thickness,
(0.4203Re~/2s + 2.796Re~'2s) 4
partial pressure, atm
volumetric flow, m~/h
ratio of the interfacial area in the presence of
waves to the plane interfacial area
gas-phase Reynolds number, 4Q~p6/gdi#G
relative gas-phase Reynolds number,


liquid-phase Reynolds number, 4QLPL/~diPL

gas-phase Schmidt number, t~G/D~P~
liquid-phase Schmidt number, #L/DLPL
gas-phase Sherwood number, k6acdi/D G
liquid-phase Sherwood number, kacdi/DL
temperature, K
dimensionless height, L/d~

Mass transfer at high Reynolds numbers

Greek letters

mean liquid film thickness, m

solid concentration, wt%
viscosity, kg/m s
relative absorption rate, 1 -- (1 -- H)";
a =



density, kg/m 3


gas phase
liquid phase
relative to the liquid surface

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