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t
a
q
q
q
_ _
a
q
q
q
~v
q
_ _
_ _
n
p1
_ m
pq
_ m
qp
(1)
where q is the volume-averaged density. The q
th
fluid volume
fraction in the cell is denoted as a
q
, _ m
qp
is the mass transfer
from phase q to phase p, and _ m
qp
is the mass transfer from
phase p to phase q.
2.2 Momentum Equation
t
q~v q~v~v p l ~v ~v
T
_ _ _
q~g
~
F (2)
where p is the static pressure, ~v is the component of the flow
velocity parallel to the gravitational vector, l is the viscosity, g
is the gravitational acceleration, and
~
F is the external body
force.
2.3 Energy Equation
t
qE ~vqE p k
eff
T (3)
in which k
eff
is the effective thermal conductivity. The VOF
model treats the energy, E, and the temperature, T, as mass-
averaged variables.
2.4 Closure Equations
The RNG k-e turbulence model is derived from the instanta-
neous Navier-Stokes equations, using a mathematical tech-
nique called the renormalization group (RNG) method. The
analytical derivation results in a model with constants different
from those in the standard k-e model, and additional terms
and functions in the transport equations for k and e.
t
qk
x
i
qku
i
x
j
a
k
l
eff
k
x
j
_ _
G
k
G
b
qe (4)
t
qe
x
i
qeu
i
x
j
al
eff
e
x
j
_ _
C
1e
e
k
G
k
C
3e
G
b
C
2e
q
e
2
k
Re
(5)
where R
e
is given by
R
e
C
l
qg
3
1 g=g
0
e
2
1 bg
3
e
2
k
(6)
In these equations, G
k
represents the genera-
tion of turbulence kinetic energy due to the
mean velocity gradients, and G
b
is the genera-
tion of turbulence kinetic energy due to buoy-
ancy. The quantities a
k
and a
e
are the inverse
effective Prandtl numbers for k and e, respec-
tively. g = Sk/e, g
0
= 4.38, and b = 0.012.
Chem. Eng. Technol. 2012, 35, No. 2, 334340 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim www.cet-journal.com
Table 1. Comparison of two types of corrugated gauze packing.
Packing types Peak height
[mm]
Wave length
[mm]
Hydraulic
diameter
[mm]
Porosity Area
[m
2
m
3
]
Common corrugated
packing
2.5 4 2.8 0.77 1100
Zigzag-pak 2.5 2.5 1.3 0.62 1900
Transfer intensification 335
3 Geometry and Boundary Conditions
Structured packing has a complicated geometric construction,
and, therefore, needs a lot of time and physical memory to
solve the above dynamic equations even for the calculation of
one packing element. In the current paper, the simulation
model is based on one triangular channel from a piece of the
packing element. The boundary conditions are as follows: the
inlet velocity of the gas is 0.743 ms
1
, the outlet pressure of the
gas is 60 kPa, the inlet velocity of the liquid is 0.0013 ms
1
, and
the outlet boundary of the liquid is the outflow. The tempera-
ture is 80 K, and the fluids are the two phases of CO.
Fig. 1 is a schematic of the common corrugation geometry
of the packing used in the
13
C distillation installation. The cor-
rugation height is 2.5 mm, the corrugation width is 4 mm, and
the side length is 3.2 mm.
Fig. 2 presents schematically the new corrugation geometry
Zigzag-pak, where the corrugation height is 2.5 mm and the
corrugation width is 2.5 mm. The main difference in geometry
between the Zigzag-pak and common packing is that the for-
mer has a right-angled triangle corrugation whereas the latter
has an isosceles triangle corrugation.
The schematic diagrams of the current CFD models
for the common packing and the new Zigzag-pak are
illustrated in Figs. 3 and 4, respectively. They both have
the same corrugation inclination angle of 45 and the
same length of flow channel with 50 mm. As shown in
Figs. 3 and 4, there is one inlet velocity for gas, one
inlet velocity for liquid, one outlet pressure for gas,
one outflow for liquid, two walls, and one symmetry
boundary for each 3D model.
4 Experiments
A commonly used corrugated gauze packing,
PACK-
13
C, with a specific surface area of 1135 m
2
m
3
was installed in the CO cryogenic distillation column
[13]. The PACK-
13
C was fabricated by compressing a
double-layer silk screen, made of stainless steel, into
the corrugated shape. Pieces of the screens were then
assembled with an inclination angle of 45, corruga-
tion height of 2.5 mm, porosity of 0.77, and silk diameter of
0.085 mm. The packing bed was 18 m high, and the diameter
of the packing was 45 mm. When the F-factor varied from 0.18
to 0.90 ms
1
(kg m
3
)
1/2
, the numbers of theoretical stages per
meter ranged between 20 and 30. In that case, the pressure
drop was less than 25 Pa for one theoretical plate, the dynamic
liquid holdup was between 11 % and 21 %, and the pilot-scale
plant produced 2.1 g of 15 %
13
C per day. The experimental
measurements demonstrated that the PACK-
13
C exhibited a
higher mass transfer efficiency than traditional random pack-
ing when used for
13
C distillation.
As demonstrated in the flow sheet of Fig. 5, the purified CO
gas flowed into the cryogenic distillation column at the feeding
point, the extracted gas was removed at the top of the column
by a vacuum pump, and the concentrated
13
C product was taken
out at the bottom of the column. The
13
CO was enriched by
numerous liquid-vapor exchanges on the surface of the packing.
The column was well insulated using multilayer insulation, and
the total heat leakage of the column was less than 30 W. Raw
materials were high-purity CO gas and commercial liquid nitro-
gen. The CO vapor and liquid nitrogen exchanged heat in the
condenser located on the top of the column, and the vaporized
nitrogen gas was drawn out by a pump. The installation real-
ized automatic operation and ran smoothly for over six
months.
5 Simulation Results and Discussion
The CFD simulations were carried out using the Fluent 6.3
software platform. In this solver, a first-order upwind scheme
and pressure-velocity coupling algorithms were applied for the
discretization of differential equations. The two-phase fluids of
liquid CO and vapor CO flow as countercurrents in the com-
mon corrugated packing installed in the cryogenic column.
The operation conditions were the same as those in the experi-
ments. The distribution of liquid phase in the common corru-
gated gauze packing is displayed in Fig. 6.
www.cet-journal.com 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim Chem. Eng. Technol. 2012, 35, No. 2, 334340
Figure 1. Geometry of the common corrugated packing.
Figure 2. Geometry of the newly developed packing Zigzag-pak.
Figure 3. 3D model for the common corrugated packing.
336 H.-L. Li et al.
Liquid CO streams down on one side of the chan-
nel even though it spreads out as a thin film on the
inlet surface. Most of the packing surfaces are not
moistened. This does not agree with the common
opinion which assumes that liquids cover uniformly
all of the packing surfaces. Therefore, the CFD simu-
lation proves that large areas are not wetted and the
liquid is not well distributed in a distillation column
filled with common corrugated packing. It is clear
that this structural limitation can lead to liquid mis-
distribution. Previously, liquid misdistribution has
often been considered as the result of too high pack-
ing beds. It is concluded that it is not appropriate to
simplify the packing element as a large plane, as pre-
vious reports have done, although these have vali-
dated the flow behavior on the plates by experimental
measurements. The reason is that liquids are more
sensitive to the structure of the flowing channels than
gases. In short, fluid flow in the channels of the cor-
Chem. Eng. Technol. 2012, 35, No. 2, 334340 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim www.cet-journal.com
Figure 4. 3D model for the new Zigzag-pak.
vacuum
pump
vacuum
pump
purification
column
waste
gas
rotameter
high vacuum
pump
product
coolant
CO cylinder
cryogenic-
destillation
column
liquid
nitrogen
tank
nitrogen
gas
structured
packing
P
P
P
P
P
H
H
Figure 5. Flow sheet of the
13
C cryogenic installation.
Transfer intensification 337
rugated packing cannot be studied by simplifying it as a large
plane plate.
In comparison, the CFD simulation for CO countercurrent
flow in the Zigzag-pak packing is given in Fig. 7. The wavy liq-
uid film flows downward and spreads to both sides of the
downside wall. The surfaces are evenly covered by liquid,
which is more consistent with the assumption of the mass
transfer calculations. As a result, the moistened surfaces of this
packing are much larger than those of common packing, and,
therefore, the mass transfer is intensified.
The pressure drop along the y-direction on the symmetry
surface of the Zigzag-pak is plotted in Fig. 8. The result is simi-
lar to the experimental result using common corrugated pack-
ing.
Unlike common corrugated packing, the liquid distribution,
plotted in Fig. 9, indicates that much of the liquid film is
located in the outlet of the right-angled triangle channel of the
Zigzag-pak. Because the liquid distribution is optimized in the
Zigzag-pak, there are larger vapor-liquid interfaces for mass
exchange for the same gross packing volume than for common
packing. Thus, the mass transfer is certainly intensified in the
Zigzag-pak channels.
Fig. 10 displays the particle path lines of the vapor and liq-
uid in the Zigzag-pak for
13
CO cryogenic distillation.
From the above CFD simulations, the details of the vapor-
liquid flow in the structured packing are clearly indicated, i.e.,
liquid misdistribution in the packed towers probably results
from the structural limitation of the packing, and the liquid
misdistribution is independent of the height of the packing
beds. Although the common corrugated packing used for
13
C
separation in tests proved to be superior to traditional random
packing, it has a serious geometrical limitation. The newly
developed Zigzag-pak with a corrugation geometry consisting
of a right-angled triangle has a better liquid distribution char-
acter and could be applied in distillation towers to replace the
common corrugated packing to provide higher mass transfer
efficiency.
6 Conclusions
A simplified 3D physical model representing the corrugated
packing element is established and solved by computer. These
CFD simulations illustrate that the common corrugated pack-
ing is not well wetted in precision distillation because of its
structural limitation. It has been proved that the mass transfer
equations, based on the Nusselt theory, are not suitable for dis-
tillation calculation in such a corrugated packing system. Liq-
uid misdistribution in the packed towers results from the
structure of the packing rather than from the height of the
packing beds. The new type of corrugated packing, the Zigzag-
pak, with right-angled triangle corrugation has a better liquid
distribution character and larger vapor-liquid interfaces than
those of the common corrugated packing. Considering its
prominent advantages in vapor-liquid intensification and high
www.cet-journal.com 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim Chem. Eng. Technol. 2012, 35, No. 2, 334340
Figure 6. Distribution of liquid CO in the common corrugated
packing.
Figure 7. Distribution of liquid CO in the Zigzag-pak.
Figure 8. Pressure drop along the y-direction on the symmetry
surface of Zigzag-pak.
338 H.-L. Li et al.
efficiency in mass transfer, the Zigzag-pak could replace com-
mon corrugated packing in chemical engineering.
Acknowledgment
This research has been financially supported by the Shanghai
Science and Technology Talent Project in China (No.
10QB1401700). The experiments were carried out in the labo-
ratory of the Shanghai Engineering Research Center for Stable
Isotopes.
The authors have declared no conflict of interest.
Symbols used
_ m [kg s
1
] mass flow rate
p [Pa] static pressure
E [J] total energy
T [K] temperature
k
eff
[Wm
1
K
1
] effective thermal conductivity
~
F [N] force vector
g [ms
2
] gravitational acceleration
G
k
[] generation of turbulence kinetic energy
due to the mean velocity gradients
G
b
[] generation of turbulence kinetic energy
due to buoyancy
S [J K
1
] total entropy
t [s] time
k [J kg
1
] kinetic energy per unit mass
u [ms
1
] velocity magnitude
~v [ms
1
] overall velocity vector
C
1e
[] constant, 1.42
C
2e
[] constant, 1.68
C
3e
[] constant, 0.0845
Greek symbols
q [kg m
3
] density
g [] effectiveness factor
l [Pa s] dynamic viscous
a
p
[] p
th
fluid volume fraction
a
q
[] q
th
fluid volume fraction
a
k
[] inverse effective Prandtl numbers for k
a [] inverse effective Prandtl numbers for e
l
eff
[Pa s] effective viscosity
e [m
2
s
3
] turbulent dissipation rate
Subscripts
q q
th
phase
p p
th
phase
Chem. Eng. Technol. 2012, 35, No. 2, 334340 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim www.cet-journal.com
Figure 9. Contours of liquid volume
fraction on the surface of the liquid out-
let for Zigzag-pak.
Figure 10. Particle path lines for the vapor and liquid in Zigzag-
pak.
Transfer intensification 339
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