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Ind. Eng. Chem. Res.

1997, 36, 227-237

227

Mass Transfer in Beds of Modern, High-Efficiency Random Packings


Ingo Wagner, Johann Stichlmair, and James R. Fair*
Chemical Engineering Department, The University of Texas at Austin, Austin, Texas 78712

A new model has been developed for the prediction and correlation of mass-transfer rates in
distillation columns containing random packings. Emphasis is placed on the characteristics of
the newer high-efficiency random packings: IMTP, CMR, Fleximax, and Nutter. These
packings are of the high void fraction, through-flow type and have become quite popular for
new designs as well as for retrofits. In building the model use has been made of a large bank
of experimental data from the laboratories of Fractionation Research, Inc., and the Separations
Research Program (SRP) at The University of Texas at Austin. The model is based on an earlier
SRP study of liquid holdup and gas pressure drop in beds of random or structured packing
(Stichlmair et al. Gas Sep. Purif. 1989, 3, 19]. The only packing parameter needed is a packing
characteristic which has a value of about 0.030 for a 2-in. Pall and Raschig rings and about
0.050 for the 2-in. nominal size of the high-efficiency packings listed above. The model was
found to fit 95% of 326 experimental values of height equivalent to a theoretical plate (HETP)
to within (25% and all values within (30%.
Prediction of the mass-transfer efficiency of distillation columns containing random packings has long been
considered a risky endeavor, primarily because of a lack
of understanding of the complex two-phase flow that
prevails in such packings. While reasonable masstransfer models have evolved for the older, bluff-body
packings, such as Raschig rings and Berl saddles, the
advent of newer, through-flow type metal random
packings has left the existing models wanting. For one
thing, there has been an insufficient amount of commercial-scale efficiency data published for these newer
packings, certainly not enough data for preparing
generalized models. For another, there is the problem
of a different kind of surface generation in the newer
packings, certainly a departure from the traditionally
assumed liquid film flow and vapor channel flow approaches. Examples of the through-flow packings are
IMTP (Norton Co.), Nutter rings (Nutter Engineering
Co.), CMR (Glitsch, Inc.), and Fleximax (Koch Engineering Co.) and have registered trade names. The
traditional metal Pall ring also can be classified as
through-flow.
The work described here has resulted from further
investigations of the character of flow through the newer
packings, particularly the work reported by Stichlmair
et al. in 1989. In addition, a large amount of commercially important experimental data have become
available in recent years, especially those from the
Separations Research Program at The University of
Texas at Austin (SRP) and from Fractionation Research,
Inc. (FRI). With these sources coupled with pertinent
previously published information, a data bank of 326
experimental efficiency points has been assembled.
This bank comprises the basis for evaluating the model
to be described below. The objective of the work was to
develop a semiempirical model taking into account the
effect of irrigated pressure drop and liquid holdup on
mass transfer.
* To whom correspondence should be addressed. E-mail:
fair@che.utexas.edu.
Present address:
Technische Universitat Munchen,
Munchen, Germany.
S0888-5885(96)00019-X CCC: $14.00

Previous Work
Generalized methods for predicting the mass-transfer
performance of larger-scale packed distillation columns
have been reviewed by Kister (1992). For random
packings, only four methods have been thought to be
general enough and reliable enough to merit serious
consideration for commercial design. The method of
Cornell et al. (1960) utilizes the two-film model and
empirical parameters specific to each packing type and
size. Its development was based on a rather limited
data set and did not include the more modern, throughflow packings. Onda et al. (1968a,b) developed a
random packing model based on a modest-sized data set,
using the two-film model and covering traditional
random packings such as ceramic rings and saddles.
Bolles and Fair (1982) expanded the Cornell et al. data
base and adapted the model to new experimental results
taken at larger scales of operation. They included
distillation results for a through-flow random packing,
the Pall ring, in their analysis. Bravo and Fair (1982)
used the Onda model plus the Bolles-Fair data base to
provide a correlation for effective interfacial area in
randomly-packed columns. These four approaches to
predicting mass transfer purported to cover absorption/
stripping as well as distillation applications.
A knowledge of fluid dynamic behavior is fundamental not only for column design but also for the prediction
of mass transfer. It is well-known that there is a strong
dependence on hydraulics of the effective interfacial
area in a packed bed. Thus, in the present work it was
necessary to consider pressure drop and liquid holdup
effects in arriving at a suitable model for mass transfer.
The pressure drop studies of Stichlmair et al. (1989)
compared the behavior of packed columns with the
experimental findings for a fluidized bed, with the result
of a slight modification of the Ergun model for fixed beds
of packing:

pd 3 1 -  V2
) f0 4.65 FV
Z
4 
dp
f0 )

C1
C2
+
+ C3
ReV Re 0.5
V

1997 American Chemical Society

(1)

(2)

228 Ind. Eng. Chem. Res., Vol. 36, No. 1, 1997

Figure 1. Dry and wet bed pressure drop for 25 mm Bialecki


rings (Billet, 1995). Reprinted with permission from VCH Publishers. Copyright 1997 American Chemical Society.

Figure 2. Liquid holdup for 25 mm Bialecki rings with the airwater system (Billet, 1995). Reprinted with permission from VCH
Publishers. Copyright 1997 American Chemical Society.

where calculation of the dry bed pressure drop pd


requires the use of friction factor f0, itself a function of
vapor flow and packing device geometry. Values of the
constants C1, C2, and C3 for many packings are given
in the Stichlmair et al. paper. Correlations similar to
that of eqs 1 and 2 have been presented by Kast (1964)
and Billet et al. (1989).
Determination of the irrigated pressure drop takes
into account the rise in interstitial gas velocity with
diminished flow area due to the presence of the flowing
liquid. A representative set of irrigated pressure drop
data is shown in Figure 1, where it may be observed
that above the loading point the liquid flow lines curve
away from the dry pressure drop line. Several authors
have presented models for irrigated pressure drop (Billet
et al., 1989; Billet and Schultes, 1993; Kolev, 1976;
Mackowiak, 1991; Reichelt and Blass, 1971; Robbins,
1991). For the present work, the model of Stichlmair
et al. (1989) was used; it was considered by Kister (1992)
to be the most fundamental model available, and,
importantly, it includes the determination of liquid
holdup both below and above the loading point. The
model is as follows:

In the loading zone, however, holdup increases as vapor


velocity approaches the flooding point.
The holdup relationship of Stichlmair et al. (1989)
does not account for physical properties and has been
validated for air/water systems only, but it was shown
that the equation is applicable for liquid viscosities up
to 5 10-3 Pas. This can be explained by the moderate
influence of viscosity and surface tension on liquid
holdup (Strigle, 1987). The equation is similar to that
of Billet and Mackowiak (1988) but does not include a
constant that depends on the packing type:

pirr
1 -  + h (2+c)/3
 4.65
)
pd
1-
-h

(3)

with friction factor f0 taken from eq 2 and

c) -

C1
C2
f -1
ReV (2Re )0.5 0
V

(4)

The liquid holdup in a packed column is defined as


the volume of liquid held under operating conditions per
volume of packed bed. This holdup can be divided into
two components, the static and the dynamic (or operating) holdup. The static holdup consists of the liquid
kept in the voids or dead spaces of the packing, while
the dynamic portion flows down the column. The static
holdup is influenced by the physical properties of the
liquid and the packing surface but is independent of the
liquid load (Jesser and Elgin, 1943). The static holdup
is normally of no great significance in packed columns
(Strigle, 1987). The dynamic holdup is primarily a
function of the liquid velocity. Figure 2, from Billet
(1995), shows the typical behavior of the holdup as a
function of vapor velocity in a packed column, for
various liquid loads. It is clear that the holdup below
the loading point is independent of the vapor velocity.

( )

h0 ) 0.555

apuL2

1/3

(5)

g4.65

Above the loading point, the correlation for liquid


holdup of Stichlmair et al. is dependent on the irrigated
pressure drop:

( )]

h ) h0 1 + 20

pirr
ZFLg

(6)

A disadvantage of eq 6 is that the irrigated pressure


drop must be known in order to determine the holdup
in the loading region. Since the calculation of the
irrigated pressure drop by eq 3 requires a value of
holdup, an iteration is necessary.
The amount of the existing effective vapor-liquid
interfacial area in randomly-packed distillation or absorption columns is a basic factor that affects the mass
transfer. It has been found that the area is smaller than
the total vapor-liquid surface area (Davidson, 1959;
Hanley et al., 1994a; Weiland et al., 1993). This, among
other things, is caused by negligible liquid flow through
thin liquid films, making the wetted surface largely
ineffective for mass transfer. The effective interfacial
area is also reduced because of a shielding effect
(Hanley et al., 1994a,b). This means that a part of the
vapor flow cannot interact with the liquid because of
gas maldistribution caused by liquid-filled voids which
block the vapor flow. This phenomenon will have a
great influence on mass transfer as the flooding point
is approached because of the rapidly increasing holdup.
Several investigators have proposed that a large part
of the effective interfacial area results from liquid drops
generated in the packed column (Bornhutter, 1991a,b;
Fair and Bravo, 1987). Bornhutter found that the
amount of drop flow is about 5-45% of the total liquid
flow depending on packing type and liquid properties,
and thus the effect of drop flow on mass transfer cannot

Ind. Eng. Chem. Res., Vol. 36, No. 1, 1997 229


Table 1. Equations for the Liquid-Side Mass-Transfer Coefficient

( )( )
( )( )( )
( ) ( ) ( )( )
( )
()
(
) ( )
DL
4

0.5

Billet (1993)

kL ) C

Onda (1968b)

kL ) 0.0051

Schultes (1990)

kL ) C

Shi and Mersmann (1964)

kL ) 0.91

FLg
L

FLg
L

Lg
FL

1/3

L1/3

1/3

uLFL
aeL

apDL
4

1/6

6DL
dn

0.5

0.5

kL ) 25.1

van Krevelen (1942)

kL ) 0.015

Zech (1987)

kL ) C

uL uL
ap ap

0.5

(apdn)0.4

1/3

uL0.19g0.220.2FL0.23
FL
0.23a 0.4
L

0.5

L
FLDL

2/3

(1 - 0.93 cos )1/3

FL2g

1/3

L
F L DL

L2

DLap

6(1 - )

( )( )( )
uLFL
aeL

0.05

0.45

6(1 - )uLFL
apL

Shulman et al. (1955)

DL F L
L

2/3

DL

( ) ( )( )
FLgdn2

-0.15

uLgdn
3

1/6

6DL
da

0.5

Table 2. Exponents Used in Correlations for the Liquid-Side Mass-Transfer Coefficient


author

uL

DL

FL

Billet (1993)
Schultes (1990)
Shi and Mersmann (1964)
Shulman et al. (1955)
Zech (1978)
new model

0.33
0.33
0.19
0.45
0.167
0.167

0.5
0.5
0.5
0.5
0.5
0.5

0.33
0.167
0.23
-0.05
-0.15

-0.33
-0.167
-0.23
0.05

g
0.33

0.05
0.15

0.22
-0.017
0.167

Table 3. Summary of Equations for the Vapor-Side Mass-Transfer Coefficienta

( )

DV uVFv
dn apv

0.8

ScV1/3

van Krevelen and Hoftijzer (1948)

kV ) 0.20

Shulman and de Gouff (1952)

kV ) 0.0137(uVFV)0.65

Onda et al. (1968b)

kV ) 5.23DVap

Zech and Mersmann (1979)

kV ) C

Billet (1993)

ap
DV
FVuV
kV ) C
(4)0.5 ( - h)0.5 apV

Cornell et al. (1960)

HV )

( )
1
ScV

( )
FVuV
apV

2/3

0.7

ScV1/3(apdn)-2

2
2
 + 0.012 (1 - )DV uV FV

Vdn

( )

1/3

0.75

ScV1/3

( )( )

uV
Dc
C
)
Sc 0.5
kVae (3600F u f f f )q V 3.66
L L 1 2 3

Z
3.05

1/3

ScV ) V/FVDV.

be neglected. It is also important to note that the


amount of effective interfacial area in a given system
is the same for vapor- and liquid-side mass transfer
(Bravo and Fair, 1982).
It is clear that the interfacial area in a packed column
is closely related to the hydrodynamics. The fluid
conditions are mainly described through irrigated pressure drop and holdup. Previous workers have concluded
that the amount of vapor-liquid surface area is directly
linked to the operating holdup (Bravo and Fair, 1982;
Martin et al., 1988; Puranik and Vogelpohl, 1974; Rocha
et al., 1993; Yilmaz, 1973). Relationships between
effective interfacial area and actual packing surface
have been developed by a number of researchers (Onda
et al., 1968a,b; Billet and Schultes, 1993; Kolev, 1976;
Bravo and Fair, 1982; Zech, 1978; Shi and Mersmann,
1984). The ratio of ae/ap was determined in various
ways, but not for any of the newer through-flow random
packings.

In distillation applications the liquid-side masstransfer resistance normally has a minor effect on masstransfer rate, unlike absorption and desorption applications which may be dominated by the liquid-side
mass-transfer resistance. However, the liquid-side
resistance in distillation is still significant enough to
merit attention by the present work. A summary of the
equations for the liquid-side mass-transfer coefficient
contributed by other authors is given in Table 1. A
summary of the exponential relationships for the various parameters is given in Table 2. The only consistency is the 0.5 exponent on the diffusion coefficient, as
predicted by the penetration model of Higbie (1935).
The vapor-side mass-transfer coefficient has been the
subject of much experimental and theoretical study. A
summary of the various published correlating equations
for the vapor side is given in Table 3, with the exponents
of the principal parameters given in Table 4. The
variations of the exponents for the vapor side are less

230 Ind. Eng. Chem. Res., Vol. 36, No. 1, 1997

The same process for the gas phase leads to

Table 4. Exponents Used in Correlations for the


Vapor-Side Mass-Transfer Coefficient
author

uV

DV

Billet (1993)
Mersmann and Deixler (1986)
Onda et al. (1968b)
Shulman et al. (1955)
van Krevelen (1948)
Zech and Mersmann (1979)
new model

0.75
0.66
0.7
0.65
0.8
0.66
0.5

0.66
0.66
0.66
0.66
0.66
0.66
0.5

FV

-0.416 0.416 - -0.33 0.33 - -0.367 0.367 - 0.65 - -0.467 0.467 - -0.33 0.33 - -

than those for the liquid side, but it is notable that the
variation of the diffusion coefficient is to the 0.66 power,
which is not predicted by the penetration model. However, that model was developed primarily for the liquid
phase.

Model Development
Height Equivalent to a Theoretical Plate (HETP).
The HETP is used extensively for characterizing the
mass-transfer capability of a packed bed. It suffers,
however, from not being fundamentally-based with
respect to interphase transport. Rather, the height of
an overall transfer unit, Hov, is more appropriate in that
it includes individual phase mass-transfer coefficients
and concentration driving forces. Well-known theory
leads to the following representation of Hov:

Hov )

uV
FVMLkV
1+m
kVae
FLMVkL

(7)

The second term on the right represents the additional


transfer resistance of the liquid phase. As can be seen,
this relationship includes three unknowns: the liquidand vapor-side mass-transfer coefficients kL and kV and
the effective interfacial area ae.
Mass-Transfer Rate. The penetration theory of
Higbie (1935) was extended by Lockett and Placka
(1983), who introduced an enhancement factor to
account for turbulent diffusion and multiple surface
renewals. This leads to equations for the liquid- and
vapor-side mass-transfer coefficients:

kL )
kV )

( )
( )
4LDL
L

0.5

4VDV
V

0.5

kL )
kV )

4LDLuL
h

4VDVuV

0.5

(14)

0.5

(15)

( - h)

One should note that the exposure times for liquid,


L, and vapor, v, are different, which is in agreement
with the findings of Chen and Chuang (1994). Looking
at eqs 14 and 15, one can see that there are now three
instead of two unknown factors, the liquid and gas
phase enhancement factors L and V as well as the
characteristic length . At operating conditions the
enhancement factors can approximately be set equal to
unity, so that only the value of the characteristic length
must be determined in order to calculate the masstransfer coefficients.
It may be pointed out that use of the penetration
model for determining the gas-phase coefficient in
packed columns is not common. For sieve trays, on the
other hand, the penetration model is used to predict
both the liquid- and vapor-side mass-transfer coefficients, and there are investigators who have proposed
an exponent of 0.5 for the vapor diffusion coefficient in
packed columns, according to penetration theory (Cornell et al., 1960; Lynch and Wilke, 1955; Vidwans and
Sharma, 1967). It seemed reasonable in the present
study to utilize the penetration model as an approximate representation of the physical mechanisms involved in phase contacting in random packings.
Effective Interfacial Area. As mentioned earlier,
the effective interfacial area is closely related to the
hydrodynamics in the column. Considering the pressure drop model of Stichlmair et al. (1989), eqs 1 and 3,
the particle diameter dp can be replaced by its definition:

dp )

6(1 - )
ap

(16)

(9)

pd 3 ap
) f0 4.65FVuV2
Z
4 6

(10)

(17)

Thus, the dry pressure drop is proportional to the


packing surface area. The basic idea now is that the
irrigated pressure drop as well is directly dependent on
the total surface area in the wetted packing. The
Stichlmair equation for the irrigated pressure drop
becomes

pirr 3
atot
) f0
F u 2
Z
4 6( - h)4.65 V V

(18)

(11)
This can be transformed, using eq 17, into

so that time can be written as:

L ) h/uL

Dovetailing eqs 12 and 13 into eqs 8 and 9 results in:

which leads to the following expression for the dry


pressure drop:

The effective velocity can be determined by using the


liquid holdup:

uLeff ) uL/h

(13)

(8)

The time the liquid is in contact with the gas phase can
be expressed through the effective liquid velocity uLeff
and a characteristic length :

L ) /uLeff

V ) ( - h)/uV

(12)

pirr f0 atot  4.65


)
pd
f0 a p  - h

(19)

Ind. Eng. Chem. Res., Vol. 36, No. 1, 1997 231


Table 5. Physical Properties of the Test Systems
system

FL (kg/m3)

p (kPa)

cyclohexane/n-heptane

33.3
165.5
413.7
1160.0
13.3
6.7
100.0
100.0

i-butane/n-butane
ethylbenzene/styrene
ethanol/water
methanol/ethanol

656.7
608.7
560.6
493.6
829.7
842.5
760.9
752.8

FV (kg/m3)

L (Pas)

(N/m)

DL (m2/s)

DV (m2/s)

1.18
5.45
13.14
28.37
0.48
0.26
1.44
1.20

0.43
0.23 10-3
0.16 10-3
0.97 10-4
0.39 10-3
0.47 10-3
0.50 10-3
0.45 10-3

17
12 10-3
8 10-3
6.2 10-3
26 10-3
27 10-3
2 10-3
19 10-3

2.7
6.2 10-9
9.3 10-9
1.35 10-8
3.0 10-9
2.7 10-9
6.2 10-9
3.6 10-9

1.1 10-3
2.9 10-4
1.4 10-4
5.6 10-7
2.4 10-3
3.8 10-3
1.5 10-3
1.0 10-5

where, according to Stichlmair et al., the ratio of wet


and dry friction factors is

f0
1 -  + h c/3
)
f0
1-

(20)

A comparison of eq 3 with eqs 19 and 20 shows that


the total interfacial area in a wetted packing can be
determined by

atot
1 -  + h 2/3
)
ap
1-

10-9

substituted into eq 7. Further, it was assumed that for


all test systems the average slope of the equilibrium line
was approximately unity. Under this assumption, and
operating with total reflux (L/V ) 1), the HETP is equal
to the height of an overall vapor transfer unit Hov. This
leads to:

HETP )

)[ (

( - h)uV
4DV

0.5

1+

hDVMLFV

)]

( - h)DLMVFL

0.5

0.5
ae
(23)

(21)

The total surface area in the irrigated column is


expected to be greater than the effective area for mass
transfer; thus

ae
1-+h
)
-R
ap
1-

10-3

10-3

(22)

The term R takes into account the dry or ineffective


part of the total surface area in the wetted packing and
can be deduced from experimental data.
Adjusting the Model Parameters. To adjust the
missing parameters for the new model developed earlier,
experimental data taken from the Separations Research
Program (SRP) and Fractionation Research, Inc. (FRI;
1986), as well as from the investigations of Billet (1979)
and Kirschbaum (1969) were used. These data include
several types of metal random packings tested with
aqueous and nonaqueous systems under various conditions. Table 5 shows physical properties for the test
systems. The FRI information for Pall rings is included
in a paper by Shariat and Kunesh (1995); the SRP data
are new, and the research facility and experimental
methods have been described by Fair and Bravo (1990)
and by Rocha et al. (1993).
The different experimental conditions and the column
geometries for all packings tested are listed in Table 6.
For the experiments of the SRP a perforated pipe type
distributor with feed reservoir and 430 pour points/m2
of bed cross section was used. The distributor of FRI
was a tubed drip pan device with 5 mm tubes and 120
pour points/m2. Billet used a drip-tube/riser distributor
with 246 nozzles of 3 mm diameter in a column of 0.8
m diameter and in other work in a 0.5 m column, a
special orifice-riser type distributor with liquid under
pressure, with the 108 orifices being extended 2 mm
nozzles. Kirschbaum used a rotating perforated pipe
distributor in his experiments. All of these distributors
provided a very good initial liquid distribution. It can
be seen from Table 6 that the experiments cover a wide
range of physical properties, packing geometries, and
operating pressures.
To determine the two missing parameters in the
newly developed mass-transfer model, the characteristic
length, , and the ineffective part of the total surface
area, R, in the wetted packing, eqs 14 and 15 for the
liquid- and vapor-phase mass-transfer coefficients were

Equation 23 can be rearranged to

ae
)
0.5
( - h)uV
4DV

)[ (
0.5

1+

hDVMLFV

)]

V
( - h)DLMVFL L

0.5

1
(24)
HETP

The value of holdup was calculated by means of the


correlation of Stichlmair et al. (1989), i.e., eqs 5 and 6.
The relationships do not take into account physical
properties, since the interfacial area was based on the
Stichlmair et al. holdup correlation.
The experimental results for HETP now can be
inserted into eq 24. In Figures 3 and 4 the values of
ae/0.5 are plotted against holdup for IMTP No. 40,
Fleximax 300, CMR No. 2, and 50 mm Pall rings. It is
clear that all the curves begin at the origin. Further,
it can be concluded that physical properties have little
or no effect on the term ae/0.5, while the packing height
seems to have a significant influence on the mass
transfer (Figure 4).
Those data points that are out of line are based on
conditions close to flooding, where HETP rises rapidly
with increasing loading. By eq 24, high values of HETP
imply low values for the effective interfacial area. This
means that the effective interfacial area decreases as
the flooding point is approached. Since operation in this
region is of no commercial interest, these data points
were excluded from further work.
Characteristic Length. The observation that the
packing height has a significant influence on mass
transfer leads to the assumption that the characteristic
length can be expressed by

) Cpk2Z

(25)

where Cpk is a dimensionsless packing characteristic


and Z is the bed height. Figure 5 shows the results of
the Z0.5 assumption for 50 mm Pall rings. The results
for the different packing heights are in good agreement,
especially since three different systems in a pressure
range from 13.3-413.7 kPa are compared in the plot.
This seems to prove the hypothesis that increasing bed
height causes a decrease in the overall mass transfer.
This fact was observed earlier by other investigators,
and the exponent of 0.5 used for the packing height is
close to the value 0.4 proposed by Bravo and Fair (1982).

232 Ind. Eng. Chem. Res., Vol. 36, No. 1, 1997


Table 6. Test Systems, Packing Types, and Bed Geometries
source
SRP

system

packing type

cyclohexane/n-heptane

1.0 in Pall rings


1.5 in. Pall rings
2.0 in. Pall rings
IMTP No. 40
CMR No. 2
Fleximax 30

FRI

5/ in. Pall rings


8
1.0 in. Pall rings

cyclohexane/n-heptane

2.0 in. Pall rings


CMR No. 3
Fleximax 300
FRI

5/ in. Pall rings


8
1.0 in. Pall rings

cyclohexane/n-heptane

2.0 in. Pall rings


3.5 in. Pall rings
Nutter rings No. 2
Billet

methanol/ethanol

15 mm Pall rings
25 mm Pall rings
35 mm Pall rings
50 mm Pall rings
50 mm Raschig rings
15 mm Pall rings
25 mm Pall rings
35 mm Pall rings
50 mm Pall rings
15 mm Raschig rings
25 mm Raschig rings
35 mm Raschig rings
50 mm Raschig rings

ethylbenzene/styrene

Kirschbaum

ethanol/water

25 mm Pall rings

Ineffective Part of the Total Surface. As mentioned before all the curves in Figures 3-5 appear to
begin at the origin. Accordingly, for a value of holdup
equal to zero, the effective interfacial area must be zero.
This leads to a value of R ) 1 in eq 22, so that the
effective interfacial area can finally be expressed by:

ae )

[(1 -1 - + 0) - R]a

(26)

Keeping the value of R constant for all liquid loads


means that the amount of the dry surface area is
ineffective during operation under countercurrent liquid/
vapor flow conditions. An explanation can be found in
a poorly wetted metal surface leading to drop flow and
low liquid velocities in the thin film on the packing
surface. A part of the packing is wetted but is ineffective or only very slightly effective for mass transfer,
because of the small mass flow and long exposure time.
Figure 6 shows comparisons between the measured
and calculated effective interfacial areas for some of the
packings, assuming arbitrarily a packing characteristic
of 0.061.

pressure (kPa)

column diameter (m)

bed height (m)

33.3
165.5
413.7
33.3
165.5
413.7
33.3
165.5
413.7
33.3
165.5
413.7
33.3
165.5
413.7
33.3
165.5
413.7
34.0
34.0
165.0
34.0

0.425
0.425
0.425
0.425
0.425
0.425
0.425
0.425
0.425
0.425
0.425
0.425
0.425
0.425
0.425
0.425
0.425
0.425
1.22
1.22
1.22
1.22
1.22
0.425
0.425
0.425
0.425
0.425
0.425
1.22
1.22
1.22
1.22
1.22
1.22
1.22
0.5
0.8
0.5
0.5
0.5
0.5
0.5
0.5
0.5
0.5
0.5
0.5
0.5
0.5
0.5
0.3

3.12
3.12
3.12
3.16
3.16
3.16
3.16
3.16
3.16
3.09
3.09
3.09
3.16
3.16
3.16
3.07
3.07
3.07
3.66
3.66
3.66
3.66
3.66
3.16
3.16
3.16
3.07
3.07
3.07
3.66
3.66
3.66
3.66
3.66
4.30
4.30
1.50
2.00
2.00
2.00
2.00
2.00
1.50
2.00
2.00
1.33
1.50
2.00
2.00
2.00
2.00
2.00

33.3
165.5
413.7
33.3
165.5
413.7
34.0
34.0
165.0
34.0
34.0
34.0
165.0
100.0
100.0
100.0
100.0
100.0
100.0
13.3
13.3
13.3
13.3
13.3
13.3
13.3
13.3
6.7
100.0

Packing Characteristic. The last unknown factor


resulting from the substitution for the characteristic
length using eq 25 is Cpk, which must be determined
from experimental results. It was found that Cpk can
be expressed as a constant for each packing.
Final Model. For distillation columns filled with
random packing and on the basis of the development
outlined above, the design correlation becomes

)
) ][(

0.5

Z0.5 ( - h)uV

HETP ) Cpk
ap
4DV
hDVMLFV V 0.5 1 -  + h
1+
1-
( - h)DLMVFL L

[ (

) ]
2/3

-1

-1

(27)

Results and Discussion


The model has been applied to the experiments listed
in Table 6. The values predicted by the new model were
compared with 326 experimental data points. The
packing characteristic Cpk was evaluated for each packing type (Figure 7). Table 7 includes values for Cpk as

Ind. Eng. Chem. Res., Vol. 36, No. 1, 1997 233

Figure 4. Plot of the ae/0.5 function against liquid holdup at


several bed heights. Packing ) 50 mm Pall rings. Systems:
cyclohexane/n-heptane, methanol/ethanol, ethylbenzene/styrene,
all at total reflux. Pressure range; 13.3-413.7 kPa.

c
Figure 5. Plot of the function ae/Cpk vs liquid holdup, with
packing heights normalized by Z0.5. Pall rings, 50 mm; height
range ) 1.33-3.66 m.

Figure 3. Plot of the ae/0.5 function against liquid holdup for


distillation tests at 33, 165, and 413 kPa: (a) IMTP No. 40, (b)
Fleximax 300, (c) CMR No. 2. Source: SRP data for the cyclohexane/n-heptane system at total reflux.

well as the main packing specifications, void fraction ,


and surface area ap.
Figure 8 comprises parity plots for calculated vs
measured HETP, for all sizes of Pall rings, Raschig
rings, and the high-efficiency packings, IMTP No. 40
(Norton Co.), Fleximax 300 (Koch Engineering Co.),
CMR No. 2 (Glitsch, Inc.), and Nutter rings No. 2
(Nutter Engineering Co.). The best agreement was
found for the high efficiency packings, but only one
organic test system and a constant bed height were
used. For these packings, 90% of the analyzed data
show a deviation of less that 10%. By way of contrast
the data for metal Raschig rings and Pall rings cover a
wide range of physical properties, packing height, and
pressure, with aqueous and nonaqueous systems. The
agreement between model predictions and experimental
data is quite reasonable. Most of the calculated values
are in a range of (25%. Over half of the calculated
values (56%) for Pall rings vary less than 10% from the

Figure 6. Representative plot of the effective interfacial area as


a function of liquid holdup. Packing, IMTP No. 40; packing
characteristic Cpk, 0.061.

experimental values. For metal Raschig rings the


maximum error was 28.5% for the 50 mm size, primarily
at very low mass flow rates.
Figure 9 presents all calculated vs measured HETP
values; 94.8% of the data points are in a (25% range,
and no deviations over 33% were observed. Using the
new model, 218 (66.9%) of the 326 experimental data
points could be predicted with less than 10% error, with
only 1.8% (6 data points) showing a deviation of more
than (30%. It must be mentioned that the model tends
to predict lower values for the HETP compared to the
experimental results, at low pressure and with the
ethylbenzene/styrene system.
Comparison of this method with generalized approaches discussed earlier is not straightforward be-

234 Ind. Eng. Chem. Res., Vol. 36, No. 1, 1997


Table 7. Summary of Packing Specifications
packing type

void fraction (m3/m3)

surface area (m2/m3)

particle diameter (mm)

packing characteristic

in. Pall rings


1.0 in. Pall rings
1.5 in. Pall rings
2.0 in. Pall rings
3.5 in. Pall rings
15 mm Pall rings
25 mm Pall rings
35 mm Pall rings
50 mm Pall rings
15 mm Raschig rings
25 mm Raschig rings
35 mm Raschig rings
50 mm Raschig rings
Nutter rings No. 2
IMTP No. 40
CMR No. 2
Fleximax 300

0.93
0.94
0.95
0.96
0.97
0.93
0.94
0.95
0.96
0.92
0.93
0.94
0.95
0.98
0.97
0.97
0.97

341
207
128
102
66
360
207
145
102
350
220
150
110
96
170
144
144

1.23
1.74
2.34
2.35
2.73
1.17
1.74
2.07
2.35
1.37
1.91
2.40
2.73
1.25
1.06
1.25
1.25

0.060
0.034
0.030
0.032
0.034
0.057
0.036
0.030
0.031
0.067
0.037
0.028
0.030
0.047
0.061
0.052
0.050

5/

Figure 7. Representative plot of packing characteristic Cpk as a


function of liquid holdup, based on experimental conditions.
Packing ) IMTP No. 40.

cause of the makeup of the data base. Only the Bolles/


Fair and Bravo/Fair methods included a modern,
through-flow packing, the Pall ring. For both methods,
85% of the data were within the (35% parity range.
Both used the same data set, which included ceramic
rings and saddles. As discussed by Bolles and Fair
(1982), deviations from a composite data base are
expected to be significant because of experimental
variations in such factors as bed uniformity, liquid
distribution, and sampling technique. The present
method appears to be an improvement in data fit for
the more traditional packings, and no comparison is
possible with the newer packings.
Besides the accuracy of the new model, an important
concern is how the model tracks the trend of HETP with
loading. Figure 10 shows comparisons between experimental and calculated values at a range of superficial
vapor velocities. The agreement is excellent. As pointed
out earlier, no attempt has been made to model HETP
values in the vicinity of the flood point. For predictions
above the loading point, it is necessary to determine
liquid holdup using eq 6. For operation below the
loading point the simpler form, eq 5, can be used. If
used above the loading point, eq 5 leads to conservative
values.
It must be pointed out that according to the new
model the only system property influencing mass transfer is the diffusion coefficient. This fact seems to be
unusual, but it has been shown that in the range of
properties tested, and for metal packings, surface tension and density have little or no effect on mass-transfer

Figure 8. Parity plots for several packing types, measured vs


predicted values of HETP: (a) Pall rings, all sizes; (b) Raschig
rings, all sizes; (c) IMTP No. 40, CMR No. 2, Fleximax 300, Nutter
rings.

rate. The effect of liquid viscosity is found in its


influence on the liquid diffusion coefficient. A broader

Ind. Eng. Chem. Res., Vol. 36, No. 1, 1997 235

Figure 9. Parity plots for all packings tested.

Figure 11. Comparison between measured and predicted HETP


values for 50 mm metal Pall rings. Isobutane/n-butane system at
1160 kPa and total reflux, 1.22 m diameter column. The top curve
is based on data by Billet (1967) and the bottom curve on data by
Shariat and Kunesh (1995).

Conclusions

This paper presents a new model for predicting mass


transfer in randomly packed distillation columns. The
model was developed theoretically using pressure drop
and holdup to calculate the effective interfacial area.
The model was then tested using 326 experimental data
points taken with four different systems under various
conditions. The data cover a pressure range from high
vacuum (6.7 kPa) up to 413.7 kPa, a liquid viscosity
range from 0.16 to 0.5 mPas, a vapor density range
from 0.48 to 13.13 kg/m3, and a surface tension range
from 8 to 27.3 dyn/cm ()27.3 10-3 N/m). Although
the model only takes into account the diffusion coefficient as a physical property, 95% of the predicted
values showed a deviation of less than 25% from the
experimental results. It must be pointed out that the
physical properties do have an effect on mass transfer,
but the influence seems to be small. An improvement
of the model might be possible by using a modified
holdup correlation that considers additional physical
properties. This could make the model applicable to a
wider range of systems and pressures without any
fundamental changes. Further, it must be mentioned
that the equation for determining the effective interfacial area is derived from the pressure drop model of
Stichlmair et al. (1989) and therefore has the same
limitations.
Acknowledgment
The senior author is grateful for receiving a travel
and research grant from the Ernest-Solvay Foundation,
Essen, Germany. All authors acknowledge the financial
support of the Separations Research Program at The
University of Texas at Austin.
Addendum

Figure 10. Representative comparisons between measured and


predicted HETP values, for varying superficial vapor velocities.
(a) IMTP No. 40, (b) Fleximax 300, (c) CMR No. 2.

range of properties should be studied in order to validate


the completely general nature of the new model.

Since the completion of the paper, additional data


have become available for the distillation of isobutane/
n-butane at 1160 kPa, using 50 mm Pall rings in a 1.2
m column. This work was carried out in the facilities
of Fractionation Research, Inc., and was recently published (Shariat and Kunesh, 1995). Properties of the
test mixture are included in Table 5.

236 Ind. Eng. Chem. Res., Vol. 36, No. 1, 1997

The fit of the model with the new data is shown in


Figure 11. Also shown in the figure are the earlier data
of Billet (1967), for identical operating conditions except
for the use of an inferior liquid distributor. The reasonable fit of the new model to this higher pressure
operating data is encouraging.
Nomenclature
ae ) specific effective interfacial area (m2/m3)
ap ) specific packing surface area (m2/m3)
atot ) specific total surface area (m2/m3)
C ) constant
c ) exponent in eq 9
Cpk ) packing characteristic
DL ) liquid diffusion coefficient (m2/s)
dp ) particle diameter dp ) 6(1 - )ap-1 (m)
DV ) vapor diffusion coefficient (m2/s)
f ) Fanning friction factor in eq 10
f0 ) friction factor for flow past a single particle
f0 ) friction factor for flow past a single wetted particle
g ) gravitational constant (m/s2)
h ) operating holdup (m3/m3)
h0 ) operating holdup under loading point (m3/m3)
Hov ) height of a transfer unit based on overall vapor
resistance (m)
kL ) liquid-side mass-transfer coefficient (kmol/sm2)
kV ) vapor-side mass-transfer coefficient (kmol/sm2)
L ) molar liquid flow (kmol/s)
m ) slope of equilibrium line
ML ) molecular weight of liquid (kg/kmol)
MV ) molecular weight of vapor (kg/kmol)
n ) exponent
pd ) dry pressure drop (N/m2)
pirr ) irrigated pressure drop (N/m2)
ReV ) vapor Reynolds number
uL ) liquid velocity (m/s)
uV ) vapor velocity (m/s)
V ) molar vapor flow (kmol/s)
x ) characteristic length (m)
Z ) packed-bed height (m)
Greek Letters
R ) ineffective part of the total surface area in a wetted
packing
 ) void fraction (m3/m3)
L ) liquid viscosity (Pas)
V ) vapor viscosity (Pas)
FL ) liquid density (kg/m3)
FV ) vapor density (kg/m3)
L ) exposure time of liquid element to vapor phase (s)
V ) exposure time of vapor element to liquid phase (s)
L ) liquid phase enhancement factor for turbulent diffusion
V ) vapor enhancement factor for turbulent diffusion
) characteristic length (m)

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Received for review January 19, 1996


Revised manuscript received September 10, 1996
Accepted September 18, 1996X
IE9600194

X
Abstract published in Advance ACS Abstracts, December
1, 1996.

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