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Mass Transfer Models 2
Mass Transfer Models 2
1
State Key Laboratory of Organic-Inorganic Composites and 2Research Center of the
chugw@mail.buct.edu.cn
This article has been accepted for publication and undergone full peer review but has
not been through the copyediting, typesetting, pagination and proofreading process
which may lead to differences between this version and the Version of Record. Please
cite this article as doi: 10.1002/aic.16595
A rotating packed bed (RPB) is recognized for its merits in chemical process
intensification. In most studies of RPB mass transfer modeling, however, the effects
of the end and cavity zones have not been taken into consideration since it was very
difficult to distinguish the end and bulk zones by hydrodynamics and mass transfer
process. In this work, the radial thickness of the end zone was obtained by developing
a probability method and imaging experiments to separate the end and bulk zones. A
three-zone model, including end, bulk, and cavity zones, of the overall gas-side
dissolved MEA chemisorption of CO2 was carried out to validate the proposed
three-zone mass transfer model. The results of the MEA-CO2 absorption experiments
showed that the experimentally obtained values of CO2 absorption efficiency were in
Keywords: rotating packed bed, radial thickness of end zone, three-zone, mass
process intensification.1-2 When the liquid phase is introduced into the rotor of a RPB,
it is split into fine droplets, ligaments, and thin liquid films by the rotating porous
RPB are up to 1-3 orders of magnitude in comparison with a traditional packed bed.5-7
RPBs have been widely used for gas-liquid, liquid-liquid, and gas-liquid-solid
more universal, although being dependent upon the hydrodynamics, but beneficial for
the scale-up of the RPB. Guo et al.14 developed models of overall gas-side volumetric
mass transfer coefficient (KGa) and overall liquid-side volumetric mass transfer
coefficient (KLa) considering liquid droplets and films in the packing of the RPB
based on the surface renewal theory.15 Luo et al.12 evaluated the liquid-side volumetric
mass transfer coefficient (kLa) by the assumption of droplets and films flowing in a
the existence of liquid droplets and films in a RPB. Qian et al.17 proposed a mass
transfer model of kLa for the MDEA absorption of CO2 with assumption of liquid
films in the packing zone of a RPB. Zhang et al.18 took droplet flow into consideration
in the RPB and developed kLa expression for absorption of CO2 by an ionic liquid.
As shown in Figure 1, the RPB consists of a static casing, a rotating rotor loaded
with packing, a static liquid distributor, and static gas/liquid inlets and outlets. For
RPBs, it is expected that hydrodynamics was different from the packed columns due
to the packing rotation. The most significant zone of the packing in the rotor is the
so-called end zone (the inner packing zone). Because of a large relative velocity
between liquid and packing, this zone has the advantage of intense fluid mass transfer
and mixing enhancement. The rest part of the packing zone is called the bulk zone.
The cavity zone is the annular space between the outer rotor edge and the inner casing
boundary, where lots of small liquid droplets fly. In most studies of RPB mass transfer
modeling, the effects of the end and cavity zones on the mass transfer were not taken
into separated and combined consideration since it was very difficult to distinguish
the physically continuous packing zone to be the end and bulk zone by
hydrodynamics and mass transfer process. Ten years ago, Yi et al.19 developed a KGa
model of the RPB by considering different droplet sizes in the end and bulk zones,
the radial thickness of the end zone was not discussed, and the lack of appropriate
mass transfer model studies hampers the further structure optimization and industrial
applications of the RPB, especially applied for fast gas-liquid mass transfer process
The objective of the present work aimed at completing these shortcomings. The
radial thickness of the end zone was first obtained by a probability calculation method,
and then the end and bulk zones were distinguished. The overall gas-phase volumetric
mass transfer coefficient model was established based on the end, bulk, and cavity
and a mass transfer theory, the three-zone mass transfer model of the RPB was
developed to predict the MEA absorption of CO2. Effects of various parameters on the
radial thickness of the end zone, such as rotational speed and liquid initial velocity, as
Model Development
loaded in a RPB as an example, the liquid is introduced into the rotating packing by
the liquid distributor and the liquid flow in the end zone is complex. Part of the liquid
is intensely torn and sheared into droplets along the radial direction of the end zone.
The other part of the liquid adheres to the packing surface under the influence of the
By these actions, we assumed that 99% of liquid has been ever captured by the
rotating packing layers at the tail (outer edge) of the end zone.20 The probability of
liquid captured by every packing layer is pi . When 99% of liquid has been completely
∏ (1 − p )Q ≤ (1 − 0.99)Q
i =1
i (1)
As shown in Figure 2, the radial thickness of each packing layer is d w and the
gap between two adjacent packing layers is bw . There is almost no gap between the
first packing layer and the packing support. When eth packing layer is at the tail of the
end zone, the radial thickness of the end zone is given by Eq. 2.
Re = ed w + (e − 1)bw (2)
Due to the complexity of the packing structure within the RPB, it is necessary to
multi-layer of wire meshes in the shape of concentric annuli, and the structure of the
packing layer of the wire mesh consists of horizontal and vertical fibers. The diameter
of the fiber is named as d w (equaling to radial thickness of one packing layer) and
the length of the square opening is named as cw . It can be considered that pi of one
square unit is the same as each layer of the wire mesh packing.
Figure 4 shows the calculation processes of pi for one square unit. The packing
characteristic pi of one square unit equals the captured area of horizontal and
vertical fibers ( Sv , S w ) divided by the total area of one square unit ( St ), which can be
obtained by
Sv + S w
pi = (3)
St
Figure 4(a) shows that the total area of one square unit can be obtained by
=
S t ( cw + d w ) 2 (4)
The shadowed area of Figure 4a shows the total captured area of both horizontal
and vertical fibers. It can be seen from the shadowed area of Figure 4b that the
captured area of the vertical fiber ( Sv ) equals to the moving circumferential length ( l )
Sv = cwl (5)
mesh fiber ( v ) multiplied by the residence time of liquid flowing through one square
l = vt (6)
v = ω ri.out (7)
dw
t= (8)
u0
cw d ww ri ,out
Sv = (9)
u0
The fixed captured area of the horizontal and vertical fibers ( S w ), shown by the
=S w d w (2cw + d w ) (10)
cw d ww ri ,out
d w (d w + 2cw ) +
u0
pi = (11)
(cw + d w ) 2
dw u0
≤ (13)
cw exp w ri ,out min
The opening of the corrugated wire mesh actually used in the followed
experiments is irregular as shown in Figure 5a and the width of the opening is not
easy to be measured directly. The width of the square opening was calculated by
simplifying the structure of the corrugated wire mesh opening as shown in Figure
rhomboid was assumed to be equal to the area of two square openings, thus cw
=
S r 2=
S s 2cw2 (14)
transfer performance. Taking CO2 absorption into MEA solution as an example, the
absorption rate of CO2 under a steady operating condition, according to the two-film
= (∗
N CO2 a K G aP yco2 − yco2
) (15)
y CO
N CO2 ⋅ a ⋅ 2π rhdr =GI d ( 2
) (16)
1 − y CO
2
yco2
K G aP( yco2 − yco∗ 2 )2π rhdr =
GI d ( ) (17)
1 − yco2
Because of the fast reaction rate between CO2 and MEA solution, the absorbed
CO2 in the solution is consumed immediately during the absorption process. 22 The
∗
yCO2
can thus be assumed to zero and K G a can be derived from Eq. 17 as
where rin and rout are the inner and outer radii of packing, respectively. If K G a
yco2 ,out
η= 1 − (19)
yco2 ,in
Next step, we give the calculation model of K G a in the whole RPB based on
average of the total gas-side volumetric mass transfer coefficient of the three zones,
( K G a )t can be written as
( K G a )e Ve + ( K G a )b Vb + ( K G a )c Vc
( K G a )t = (20)
Ve + Vb + Vc
As shown in Figure 6, K G a of each mass transfer zone can be determined by the gas
1 1 1
= + (21)
K G a kG a Hk L a
Before establishing the three-zone mass transfer model for the absorption, the
1. The pore flow, liquid film flow, and droplet flow were observed in the end and
bulk zones,23 but the proportion of the different liquid flow patterns is still unclear.
The majority of liquid inside the packing zone under the high-gravity environment
existed as dispersed droplets by the strong shear and impingement of packing fibers
based upon previous imaging studies of liquid flow in a RPB.24 Because droplets from
the outer edge of the packing move into the cavity zone and impact upon the inner
wall of the casing, lots of mother liquid droplets flows in the cavity zone, and liquid
films would form on the inner wall of the casing and daughter droplets were generated
in the cavity zone.25 The surface areas of droplets in the three zones and surface area
2. The gas behavior, such as the gas flow, gas temperature, gas viscosity, and gas
composition almost has no effect on the shape and flow path of liquid flow pattern.
reaction. 21, 22 The mass transfer process of the simultaneous absorption of CO2 can be
droplets at radial direction was assumed as plug flow in a RPB.7 The mass equation of
∂c D ∂ ∂c
= 2L (r 2 ) − k1c (22)
∂t r ∂r ∂r
The concentration gradient of CO2 tends to zero at the center of the droplet,
whereas the initial concentration of CO2 is c0 at the surface of the droplet. Therefore,
∂c
=0 (23-a)
∂t
d
c = c0 (r = ) (23-c)
2
d k k d
c = c0 sinh( 1 r ) / sinh( 1 ) (24)
2r DL DL 2
∂c
=J AL D= k Ld c0 (25)
∂r r = d
L
2
The mass transfer coefficient of CO2 in the droplet can hence be expressed as
k1 k d 2
=k Ld DL ( / tanh( 1 )− ) (26)
DL DL 2 d
∂c ∂c
= DL − k1c (27)
∂t ∂y
The initial concentration of CO2 on the surface of the film is c0 . The boundary
∂c
=0 (28-a)
∂t
∂c
=0 ( y = 0) (28-b)
∂y
c = c0 ( y =δ ) (28-c)
k1 k
c = c0 sech( δ ) cosh( 1 y ) (29)
DL DL
∂c
=J AL D= k Lf c0 (30)
∂y y =δ
L
The mass transfer coefficient of CO2 in the liquid film can therefore be expressed
as
k1 k k
k Lf = sech( 1 δ ) sinh( 1 δ ) (31)
DL DL DL
Previous studies reported that gas-side mass transfer coefficient ( kGp ) was not
significantly influenced by the centrifugal force in the RPB.26 The gas flow in RPB is
akin to that in a packed column and the values of kGp of a RPB lie in a range similar
to that in the packed column.16, 19 Hence, kGp in the end and bulk zones can be
estimated by 27
A larger number of dispersed droplets flying were observed in the cavity zone
based on a visual study. The interaction of gas and liquid flows in the cavity zone was
akin to that in a spray tower and the values of the gas-side mass transfer coefficient in
DG
=
kGc (2 + 0.552 Re0.5 Sc1/3 ) (33)
d
In previous studies, the droplet diameter of the end zone was very small due to
the intense impingement between the liquid and rotational packing.23 Because of the
smaller flow area in the end zone, droplets had more possibility to coalesce than those
in the bulk zone. The droplet diameter of the end zone grew moderately when liquid
flowed from the inner edge to the tail of the end zone. The expression of droplet
The gas-liquid effective interfacial area of the end zone can be calculated as
6e e
ae = (35)
de
e e = 47.45Le 0.772 (ω 2 re )
−0.545
(36)
In the bulk zone, the cross-sectional flow area increases as liquid flows outward,
so the possibility of coalescence between liquid droplets is relatively small. Thus, the
droplet diameter decreases with increasing the outer packing radius and is regressed
σ
db = 12.84( )0.630 L0.201 (37)
ω rb r
2 b
The gas-liquid effective interfacial area of the bulk zone can be calculated as
6ε b
ab = (38)
db
ε b = 47.45Lb 0.772 (ω 2 rb )
−0.545
(39)
The mass transfer surface area of the cavity zone ( Ac ) had been determined 25 and
Ac
ac = (40)
Vc
Experimental Section
flow in the cavity zone of the RPB was conducted by a high-speed camera. Figure 7a
shows a setup of the experimental system, including an image acquisition system and
a RPB system. The experimental procedure for the imaging processes was described
as follows. At a constant temperature of about 15 °C, water was fed into the rotor
through two stationary distributors and moved radically outwards through the rotor
consists of two pipes configured in parallel with the shaft, and each pipe has a single
nozzle of 3 mm diameter. The water was subsequently collected at the bottom of the
casing and discharged through the liquid outlet. A high-speed camera (FASTCAM
SA4, Photron Limited, Japan) with lens (AF 200 mm f/4D, Nikon Co., Japan) placed
right above the various outer packing radii was utilized to capture the images of
droplet motion in the cavity zone. The illumination was placed around the shooting
area and was on when the high speed camera was imaging. The specifications of RPB,
liquid flow rate of 60-140 L/h. The packing was added two layers by two layers
closely starting from the inner packing support to avoid the deformation of one layer
of the wire mesh. The total changing number of packing layers was 26.
parameter to judge the radial thickness of the end zone because the variation of
droplet tangential angle is remarkable in the end zone and almost unchanged in the
bulk zone in the rotor of the RPB.29 We assumed that if the ratio of the tangential
th
tangential angle at i packing layer is less than 0.05, as shown in Eq. 41, the radius
end zone.
θi + 2 − θi
≤ 0.05 (i=2, 4, 6...24) (41)
θi
Figure 7b shows the top view of the packing and cavity zones of the RPB. From
Figure 7b, the droplet tangential angle can be calculated as shown in Eq. 42.
180 u
θ= arcsin( r ) (42)
π u
The droplet radial (Eq. 43) and resultant velocity (Eq. 44) are expressed as
( x3 − x1 ) 2 + ( y3 − y1 ) 2 − ( x2 − x1 ) 2 + ( y2 − y1 ) 2
ur = λ (43)
∆t
( x3 − x2 ) 2 + ( y3 − y2 ) 2
u=λ (44)
∆t
where O1(x1, y1), O2(x2, y2), and O3(x3, y3) are the centroid coordinate of the rotor, the
target droplet in the first image, the target droplet in the second image, respectively.
∆t is the time interval between two consecutive images in pixels. For the sake of
reducing errors, the value of the average droplet velocity under each experimental
condition was obtained by measuring 30 liquid droplets from the images recorded at
different frames.
Figure 8 presents the effect of rotational speed on the average droplet tangential
angle. The average droplet tangential angle decreased when increasing the number of
the packing layer at various rotational speeds. The increase of the number of the
packing layer meant an increase of outer packing radius and resulted in a larger linear
velocity of packing. Thus more droplets were captured and flew along the tangential
direction, leading to the decrease of the average droplet tangential angle with the
increase of the number of the packing layer. It also can be seen from Figure 8 that the
speed, probably by an increase in the liquid captured probability of the vertical fibers,
as the rotational speed increases. The packing layer number at the tail of the end zone
could be calculated by Eq. 41 and then the radial thickness of end zone was calculated
Figure 9 displays the effect of the liquid initial velocity on the average droplet
tangential angle, showing that the average droplet tangential angle decreased with an
increasing layer number of packing at various liquid initial velocities. It also can be
seen from Figure 9 that the variation of droplet tangential angle is slower to stabilize
with an increasing liquid initial velocity, since more liquids were introduced into the
packing at a constant rotational speed. The packing layer number at the tail of the end
zone could be calculated by Eq. 41 and then the radial thickness of end zone was
of the end zone at different rotational speeds or liquid initial velocities. The
experimental results agree well with the probability calculation method. The average
calculation error in the experiments is less than 19%. Two suggestions to further
reduce the difference between the experiments and predicted values are: (1) try to add
the packing layer one by one in the imaging experiments; (2) consider the influence of
The chemisorption CO2 into MEA solution was employed to validate the
three-zone mass transfer model for the prediction of CO2 absorption efficiency. The
experimental results of CO2 absorption was obtained from Li’s report of our group.30
The RPB was packed with stainless steel wire mesh packing, whose fiber diameter
and porosity were 0.22 mm and 0.95, respectively. The packing parameter of the
above literature is similar to that of the above imaging work, thus packing parameter
used for the model calculation of CO2 absorption efficiency are based on the imaging
Figure 11 is the diagonal plot of the experimental and predicted values of CO2
absorption efficiency. It can be found that the three-zone mass transfer model offers
Calculated KGa in the three zones of the RPB with various operating conditions
Figure 12 shows the values of the model-calculated KGa in the three zones of the
RPB under different rotational speeds. It can be seen that KGa of the end zone is about
3 times that of bulk and cavity zones. The values of KGa of cavity zone are a little
higher than that of the bulk zone. Figure 12 also displays the dependence of the
increasing rotational speed. With an increase in rotational speed, the droplet diameter
decreased, which led to a increment of the gas-liquid contact area (a) and liquid side
volumetric mass transfer coefficient (kLa) to obtain a larger KGa of end zone. The
values of KGa of bulk zone seem to be no obvious change with the increase of the
rotational speed. For the cavity zone, the values of KGa increased with an increasing
rotational speed from 400 to 1000 r/min firstly, and then slightly decreased with an
increasing rotational speed from 1000 to 1200 r/min. The higher rotational speed
significantly increased the gas-liquid contact area and hence intensified the mass
time in the cavity zone and thus weaken the absorption of CO2. The latter factor was
more predominant at rotational speed beyond 1000 r/min, and resulted in the slow
reduction in KGa.
Figure 13 presents the dependence of KGa on the liquid initial velocity in the
three zones of the RPB. As expected, the values of KGa increased with increasing the
liquid initial velocity in all the three zones. The increase of the liquid initial velocity
could result in the increase of the liquid holdup and gas-liquid contact area in the three
zones, which is the main reason for the increase of KGa. Besides, mass transfer
contribution of cavity zone is much more with different liquid initial velocities,
Figure 14 illustrates how KGa depends on the gas volumetric flow rate in the
three zones of the RPB. KGa of all three zones increases with gas volumetric flow rate,
due to an increased turbulence between gas and liquid phases and an decrease of
Figure 15 depicts KGa values with the MEA concentration in the three zones of
the RPB, with a steady increase with an increasing MEA concentration as the result of
an increasing reaction rate between MEA solution and CO2 with associated increase in
the total mass transfer of the whole RPB. According to the calculation, the end, bulk,
and cavity zones contribute cumulatively to the total gas-side volumetric mass transfer
15-26%, respectively, thus it could be found that dominant mass transfer contribution
to the total mass transfer in the whole RPB is the end zone.
Conclusions
This work calculates the radial thickness of the end zone by using a probability
method. The number of the packing layers in the end zone was about 6-16 with the
dividing the packing zone to be end and bulk zones. A three-zone model of overall
gas-side volumetric mass transfer coefficient (KGa)t has been established based on the
physical zones of end, bulk, and cavity. The system of MEA solution chemisorption
of CO2 was used to verify the mass transfer model. Experimental results of absorption
efficiency were in agreement within ±20% with the predicted data by the model. It
could be found that the end zone contributes more than 50% to the total mass transfer
Acknowledgments
This work was supported by the National Natural Science Foundation of China
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Figure 1. Schematic diagram of the RPB. (1) Gas outlet; (2) seal; (3) casing; (4) gas
inlet; (5) rotor with packing inside; (6) packing support; (7) shaft; (8) liquid
Figure 4. Schematic diagram of liquid captured area. (a) Total captured area; (b)
captured area by vertical fiber; (c) fixed captured area by vertical and horizontal
fibers.
Figure 5. (a) Photograph of one layer of corrugated wire mesh packing; (b) schematic
Figure 7. Schematic diagram of (a) experimental setup for visual study and (b)
droplet tangential angle calculation (top view) (1) spot lights; (2) high-speed camera;
(3) computer; (4) RPB; (5) liquid flowmeter; (6) storage tank; (7) valve; (8) pump.
Figure 10. Comparison of experimental and predicted radial thickness of the end zone
(1) Gas outlet; (2) seal; (3) casing; (4) gas inlet; (5) rotor with packing inside;
(6) packing support; (7) shaft; (8) liquid distributor; (9) liquid outlet; (10) liquid
inlet.
(b) (c)
(a) Total captured area; (b) captured area by vertical fiber; (c) fixed captured area by
wire mesh.
Figure 7. Schematic diagram of (a) experimental setup for visual study and (b)
(1) Spot lights; (2) high-speed camera; (3) computer; (4) RPB; (5) liquid flowmeter;
48
42
36
0 2 4 6 8 10 12 14 16 18 20 22 24 26
i
42
36
0 2 4 6 8 10 12 14 16 18 20 22 24 26
i
Re (mm)
Re (mm)
6 6
4 4
2 2
300 500 700 900 1100 1.0 1.5 2.0 2.5 3.0
N (r/min) u0 (m/s)
(a) (b)
Figure 10. Comparison of experimental and predicted radial thickness of the end
zone with different (a) rotational speed and (b) liquid initial velocity.
60
-20%
40
20
20 40 60 80 100
Experimental absorption efficiency η (%)
KGa (molPa-1m-3s-1)
0.0030
0.0015
0.0000
400 600 800 1000 1200
N (r/min)
0.0030
0.0015
0.0000
0.7 1.4 2.1 2.8 3.5
u0 (m/s)
0.010
0.005
0.000
0.5 1.0 1.5 2.0 2.5
3
G (m /h)
0.012
0.006
0.000
1.0 1.5 2.0 2.5 3.0 3.5
CMEA (mol/L)
Velocities
Items Values
Parameters of RPB
Specification of packing
Porosity 0.97
500 14 5.32
900 8 3.04
1100 6 2.28
Velocities
1.572 12 4.56
2.358 14 5.32
2.751 16 6.08