Atmospheric Pollution Research 5 (2014) 464 470

Atm spheric Pollution Research

www.atmospolres.com

Modeling and experimental analysis of packed column for SO2 emission

control process
Chenniappan Maheswari, Kasilingam Krishnamurthy, Rathinasamy Parameshwaran

Department of Mechatronics Engineering, School of Building and Mechanical Sciences, Kongu Engineering College, Perundurai, Tamil Nadu, India

ABSTRACT
Sulfur dioxide (SO2) emissions from chemical process plants are increasing at an alarming rate. It is necessary to
implement the best methodology to reduce the SO2 emissions. This paper presents physical modeling, computational
fluid dynamics (CFD) analysis, and experimental analysis of a packed column used for flue gas desulfurization (FGD)
process to reduce SO2 emission at a greater extent. The packed column parameters such as liquid/gas (L/G) ratio,
diameter, packed height and total height were determined using physical modeling with twofilm gasliquid
absorption theory. Simulation model of the packed column is developed by GAMBIT 2.2.30 and analysis is carried out
by FLUENT 6.2.16. In CFD analysis, hydrogen peroxide (H2O2) (with different concentrations) was used as an absorbent.
CFD simulation result ensures that when H2O2 is used as a reactant, better removal efficiency is obtained. Based on
the physical modeling and CFD analysis, a lab scale packed column was developed. Experimental result showed that Corresponding Author:
95% SO2 removal efficiency is achieved for 0.1 M H2O2 as a reactant. Experimental results agreed excellently with the
developed CFD model and can be used for designing industrial packed columns.
Chenniappan Maheswari
: +91 9865210838
Keywords: Packed column, CFD analysis, SO2 emission control process, hydrogen peroxide (H2O2) : maheswarikec@gmail.com

Article History:
Received: 05 January 2014
Revised: 15 March 2014
Accepted: 15 March 2014

doi: 10.5094/APR.2014.054

1. Introduction by Maheswari et al. (2013) ensures that when H2O2 is used as an

This section reviews background information on the various
approaches, methods and materials that are currently being used
to control SO2 emissions. In Industry, coal and oil emits SO2 as a
flue gas during combustion process. The increasing usage of fossil
fuel has resulted in an increase of world total SO2 emission rate
during recent years. It poses a number of environmental and
human health effects such as wheezing, chest tightness, shortness
of breath, etc.. Control techniques are incorporated in the recent
years, which reduces the SO2 emissions and it is investigated by
Lonsdale et al. (2012). Flue gas desulfurization (FGD) is the
effective and reliable SO2 removal methodology and it is classified
as dry, semidry, and wet FGD. Among these techniques, wet FGD
is the cost effective method (Cofala et al., 2004) and produces 60
95% removal efficiency (Liu et al., 2008). In wet FGD process, the
desulfurization takes place due to mass transfer and chemical
reactions of liquid and gas phases. Different absorbents are used in
FGD such as lime (Liu et al., 2008), water with NH3 (Ipek et al.,
2008), and NaOH (Schultes, 1998). Ruitang et al. (2008) investi
gated lime based FGD process, in which lime reacts with SO2 and
produces CO2 as a secondary pollutant to the atmosphere. Hence
an alternative solution is given by Colle et al. (2003), and they
investigated the FGD process with H2O2 added with H2SO4 as an
absorbent. H2SO4 produces adverse effect on SO2 absorption with
H2O2. FGD process with H2O2 as a reactant has already patented by
Copenhafer and Pfeffer (2011). When H2O2 is used as a reactant, it
produces highly concentrated H2SO4 as a byproduct after contin
uous recirculation. Hence, FGD process with H2O2 as a reactant is
considered as an absorbent for this present work. The study given
absorbent enhances the SO2 removal efficiency.
There are several types of scrubbers proposed by researchers
for FGD process such as bubbling jet reactor (Zheng et al., 2003),
combined packed and spray tower absorber (Gomez et al., 2007),
cable bundle wet scrubber, and packed column (Colle et al., 2004).
Packed column is taken for analysis because of its increased
absorption rate by providing a good contact with liquid and gas.
FGD processes with different absorbents are simulated using
computational fluid dynamics (CFD) by several researchers
(Ebrahimi et al., 2003; Marocco, 2010). CFD modeling and opti
mization of scrubber parameters is revealed by Ruitang et al.
(2008). The study by Gomez et al. (2007) have reported that 90%
SO2 removal efficiency was achieved in a real plant developed
based on CFD modeling. Bravo et al. (2002) developed CFD model
for SO2 absorption and they investigated that the concentration of
SO2 across gasliquid interface did not vary with the operating
temperature. Literature rarely focused on the simulation studies of
FGD process with H2O2 as a reactant. Thus, in this work, CFD
analysis was used to find transport behavior between gas and
liquid in the packed column for maximum SO2 removal efficiency
when H2O2 is used as a reactant. Absorption of SO2 in H2O2 is a
complex process which involves both chemical and mass transfer
analysis. Mass transfer is an important phenomenon that should
be described properly for packed column design. Hence the
present study focused on the following:
(1) Determination of L/G ratio, packed height, diameter and height
of the packed column based on physical modeling,

Author(s) 2014. This work is distributed under the Creative Commons Attribution 3.0 License.
Maheswari et al. Atmospheric Pollution Research (APR)
(2) Development of CFD model for a packed column based on
physical modeling and analysis for maximum SO2 removal
efficiency,
(3) Comparative study with CFD simulation results and experi
mental results.
2. Physical Modeling
The performance of the column depends on the maintenance of
good liquid and gas distribution throughout the surface area of the
column. The oxidation reaction that occurs inside the packed column
is expressed in Equation (1). The reaction produces sulfuric acid as the
end product.
(1)
The packed column was selected for SO2 removal, since packed
area in the column is used to develop larger interfacial area between
gas and liquid which increases the absorption rate. Random packing
was used in this packed column since high randomness in packing
gives high removal efficiency (Coulson and Richardson, 1991).
2.1. Determination of minimum L/G ratio
During the mass transfer between SO2 and H2O2 in the packed
column, H2O2 becomes aqueous sulfuric acid solution. Though H2O2
is used as a reactant initially, once it is circulated through the
packed column, it becomes an aqueous sulfuric acid. Hence,
aqueous sulfuric acid is taken as the liquid for physical modeling.
The experiment by Hayduk et al. (1988), detailed the absorption of
SO2 in to aqueous sulfuric acid, and the solubility data taken from
this study is shown in Table 1.
Mole fraction of SO2 in liquid phase X (in aqueous sulfuric acid)
is calculated as:
(2)
The mole fraction of SO2 in gas phase (Y) is computed by
dividing the partial pressure of SO2 (PSO2) by the total pressure
(PTOT=101 KPa) of the packed column. Equation (3) is used to
express the equilibrium solubility of gasliquid systems:
(3)
From the tabulated values (Table 1), equilibrium diagram is
plotted between X and Y. The slope between X and Y in the
equilibrium line gives solubility constant H. The equilibrium line is
straight; hence the value obtained from the slope of the equilibrium
line is used to predict the solubility of SO2 in to aqueous sulfuric acid
solutions (Manyele, 2008). For different values of X and Y, calculated
H values are shown in Table 1. Also, the slope of the equilibrium line
is used to calculate minimum L/G ratio by taking mass transfer
characteristics across liquid and gas in the packed column. Twofilm
theory proposed by Whitman (1923) is the simplest theory designed
for mass transfer analysis and it is expressed in Equation (4):
Table 1. Solubility data for SO2 absorption in aqueous sulfuric acid
Solubility g of SO2/100 g Mole Fraction of the
Partial Pressure PSO2
of Aqueous H2SO4 Solute (SO2) in the Liquid
(KPa)
Solution Phase (X)
102.6 2.95
152.2 4.69
185.2 6.03
203.0 6.86
247.8 8.48
(Source: Hayduk et al., 1988)
465
(4)
where, Gm is the inlet gas flow rate, Lm is the inlet liquid flow rate, X1
is the mole fraction of aqueous H2SO4 leaving the column, X2 is the
mole fraction of aqueous H2SO4 entering the column, Y2 is the mole
fraction of SO2 in gas stream leaving the column, and Y1 is the mole
fraction of SO2 in the gas stream entering the column. The
minimum liquid flow rate to the packed column was determined as
152.5 Lph, based on the Equations (3) and (4) by considering Y1=0.05
mole fraction of SO2 (5% SO2 by volume), Y2=0.005 mole fraction of
3
SO2, Gm=40 m /hr, Henrys constant=1.21 (selected from the
Table 1), to obtain maximum of 99% (based on the assumption) SO2
removal efficiency.
2.2. Determination of the column diameter
Determination of column diameter plays a key role to ensure
good liquid and gas interaction, to make the packed column, to
withstand for high pressure drop across the walls and the packed area
and to determine the capacity of the column. Pressure drop in the
packed column must not exceed a certain level that is described as
flooding. Column diameter should be determined so as to operate the
column below 75% of the flooding velocity (Coulson and Richardson,
1991). Based on the generalized pressure drop correlations between
flooding factor (K4) and pressure drop (or) abscissa (FLV), the column
diameter is determined. Equation (5) is used to compute the pressure
drop of the column:
(5)
where, G and L are the densities of SO2 gas and aqueous H2SO4
respectively. Based on the Equation (5), FLV=0.149 was calculated and
corresponding flooding factor (K4) is calculated as 0.7. The percentage
of flooding is 70% and it is satisfactory for further analysis.
Computation of column cross sectional area based on of gas
mass flow rate (VW) is given by the Equation (6) (Coulson and
Richardson, 1991):
(6)
where, V is the SO2 gas density at 20 C, L is the liquid density, L is
the liquid viscosity, and FP is the packing factor for 25 mm
polypropylene pall ring. Polypropylene pall ring was selected as the
packing material with 25 mm diameter and its packing factor is
determined as 170 (Coulson and Richarson, 1991).
(7)
Cross sectional area of the packed column was determined using
Equation (7) and the required diameter of the column was computed
as 152.5 mm.
Mole Fraction of SO2 H=(Y/X) Henrys
in the Gas Phase (Y) Law Constant
0.0295 0.0384 1.32
0.0469 0.0596 0.81
0.0603 0.0753 0.988
0.0686 0.0848 1.09
0.0848 0.103 1.21
Maheswari et al. Atmospheric Pollution Research (APR)
2.3. Determination of packing height
Total height and packing height of the column are interrelated
and both the parameters are used to determine the total liquid
hold up time. The higher the liquid hold up time, better the
removal efficiency is. Equation (8) is used to compute the packed
height of the column (Coulson and Richardson, 1991):
(8)
where, Z represents the packing height, NOG represents the number of
transfer units and HOG represents the height of a transfer unit. Packed
height at different flow rates was estimated by the procedure
proposed by Chilton and Colburn (1935). The calculated packed
height is 1 000 mm and total column height is 2 500 mm for the
selected specifications.
The following are the packed column specifications obtained
from the above sections:
Diameter of the column: 152 mm
Total height of the column: 2 500 mm
Packed Height: 1 000 mm
Inlet liquid flow rate: 150 Lph
Inlet gas flow rate: 40 m3/hr
3. CFD Model Development
Before fabricating the packed column for mass transfer
analysis, the parameters were selected based on physical modeling
and analyzed using CFD. CFD modeling and analysis part is carried
out in this section. The following assumptions were made during
CFD design and analysis:
(1) A synthetic SO2 gas was used in place of flue gas and the flow
was assumed as incompressible.
(2) Temperature was considered as constant throughout the
column. Based on the assumptions given by (Bravo et al., 2002;
Ebrahimi et al., 2003), flue gas was cooled by water before
entering the column. The liquid considered for the analysis is
H2O2, which is subjected to change in temperature when it
reacts with SO2. The temperature of the inlet liquid loop was
maintained at constant rate by placing a heat exchanger on the
liquid loop (detailed in Section 4) (Marocco, 2010). Therefore
the temperature of liquid and gas was assumed to be equal
during the analysis.
(3) Reaction taking place between gas and liquid is rather in the
packed area compared to the other areas of the column. The
reaction kinetics was developed only for the packed area of the
column and hence the packed area was considered for reaction
analysis while reaction over the wall of packed column was not
considered.
3.1. Modeled equipment
Various steps pertaining to the CFD modeling and analysis are
discussed in this section. Based on the parameters selected from
the physical modeling detailed in Section 2, modeling and simula
tion analysis of the packed column was developed using GAMBIT
2.2.30 and FLUENT 6.2.16, respectively. In GAMBIT 2.2.30, the
entire column was considered as solid volume and meshed with
tetrahedral element. The fluid path was considered as faces and
meshed with tri element. Meshing of the packed area is problem
atic due to its random arrangement and more number of packing
elements with small size of each element (25 mm). Also due to
more number of faces (387 970) defined for 1 000 mm packed
height, HYPERMESH software was used for meshing and defining
the fluid path accurately. Polypropylene pall rings were selected as
the packing material and its solid model for the structure of
individual pall ring was defined with a boundary layer (BL). The
466
packed area was considered as solid volume and has N number of
fluid faces. Volume division process was done by finite volume
method (FVM). For each control volume (each packing material)
the CFD solver software FLUENT solves the equation in the domain
discretized cells or mesh. To integrate each volume, the differential
forms of the governing equations are used. The resulting equation
is a discretization equation, expresses the conservation principle
for the packed material inside the column. Also, liquid flow in the
packed column was considered as turbulent, isothermal, steady
flow and time invariant, governing equations of fluid dynamics
include a nonlinear convection term and a nonlinear pressure
gradient term. These nonlinear equations must be solved numeri
cally with the help of suitable boundary and initial conditions. The
conserved quantities such as mass, momentum, energy, to
describe the motion of gas and liquid in the packed area are
governed by momentum equations also called as Reynolds
Averaged NavierStokes (RANS) equations. These equations are
used for turbulence modeling with steady state flow (Crowe et al.,
1998).
(9)
(10)
(11)
The Equations (9)(11) (Marocco, 2010) were solved using CFD
solver software FLUENT which solves the equation in the domain
as a discretized cells or mesh.
Smass, Smomentum and SA represent interchange of mass,
momentum, and chemical species between the gas and liquid
phase respectively. These values were calculated cell by cell using
the property of the droplets as they enter and leave the cell
(Montanes et al., 2009). The solver model is described as species
transportation model which is used to investigate the transporta
tion of mass and momentum of chemical species. The volumetric
reaction method was used to forecast the local mass transfer of
each species in the packed column through the solution of a
convectiondiffusion equation for the ith species and was detailed
in Equation (12) (Baukal, 2000).
(12)
where, CSO2 is the concentration of SO2 for mass transfer which is
th
solved iteratively up to the i species at the last element of the
column, D is the diffusion coefficient, represents average velocity
that the gas is moving, and R represents the quantity of SO2
produced (R>0) or destroyed (R<0) after the chemical reaction.
4. Experimental System
The line diagram of the experimental system consisting of two
storage tanks, packed column, rotameters, pump, heat exchanger,
and SO2 gas sensors is shown in Figure 1.
The gaseous mixture was made up of SO2 and air, supplied by
SO2 cylinder and air compressor respectively. SO2 gas flow rate was
maintained between (00.5 Lph) and mixed with air at a flow rate
of 40 m3/hr. The mixed gas is entered at the bottom of the packed
column. The concentration of SO2 at inlet and outlet were mea
sured by two SO2 gas sensors. Two SO2 transmitters transmitted
sensor readings to the computer through VMAT Data Acquisition
Card (DAQ), and the sample readings were recorded for every 0.1 s
interval. Process tank (or) recirculation tank was filled with H2O2 of
required volume (10 L) and pumped with the flow rate of (150 Lph)
Maheswari et al. Atmospheric Pollution Research (APR)
to the top of the packed column through VFD (Variable Frequency
Drive). A heat exchanger was connected on the liquid loop to
maintain the temperature of the recirculated liquid constant
during experiments. The rotameters connected in liquid and gas
loop were used to show the flow rate of liquid and gas.
Figure 1. Line diagram of the experimental system.
The SO2 gas fed from the cylinder was mixed with compressed
air and required concentration of SO2 (5 000 ppm) was produced.
This mixed gas was then supplied from the bottom of the packed
column. The scrubbing liquid was fed from the process tank and
was entered at the top of the packed column. Inside the packed
column, mass transfer takes place between gas and liquid
depending on the amount of packed area. After the chemical
absorption between gas and liquid, the treated flue gas is
transferred to the top of the packed column. The absorbed
solution at the bottom of the column is collected by the process
tank and recirculated. The recirculated liquid temperature was
maintained at a constant rate by a heat exchanger connected to
the liquid loop and was supplied with cold water from the water
tank with the flow rate of 150 Lph.
5. Results and Discussions
5.1. CFD simulation results
From the CFD model described in the Section 3, simulation
results were carried out for water as an absorbent and H2O2 (with
different concentrations) as an absorbent. CFD analysis was carried
out with the operating parameters are given as: pressure101.325
KPa, SO2 mass flow rate0.029193 Kg/s, H2O2 mass flow rate
0.0604 Kg/s, inlet molar concentration of SO20.0727 Kmol/m ,
3 simulation study was carried out a number of iterations till the
and Inlet molar concentration of H2O20.4 Kmol/m3.
Simulation runs were carried out for water as an absorbent
and the simulated CFD model is shown in Figure 2. The figure
illustrates that the concentration of SO2 changes throughout the
length of the absorber. In the gas phase, the air stream enters in to
the column with a SO2 composition of 0.0727 Kmol/m3 and leaves
the absorber with a composition of 0.0327 Kmol/m3, with a small
increase in absorption rate towards the top of the absorber. Since
water was used as an absorbent, reaction between water and
sulfur dioxide is immediate and permanent. The enhancement of
mass transfer between SO2 and water in the packed column is less
due to fractional absorption takes place between them. Resultantly
water absorbent produces an average SO2 removal efficiency of
55.02%.
467
Figure 2. SO2 outlet molar concentration profile using water as an
absorbent in a packed column (kmol/m ).
3
To enhance the SO2 removal efficiency further, simulation
study was carried out using H2O2 as a reactant as shown in
Figure 3.
When H2O2 is used as an absorbent the following reaction
takes place:
(13)
For the above oxidation reaction, 2 M of SO2 was mixed with
1 M of H2O2 to make equilibrium solubility between SO2 and H2O2
and 3 M of H2SO4 was produced. Hence the requirement of H2O2 is
half that of the SO2 concentration. Since maximum SO2 inlet
concentration to the packed column was considered as 5 000 ppm,
a little quantity of H2O2 is enough to make a kinetic mass transfer
reaction. In this simulation study, mass flow rate of H2O2 was
0.0604 Kg/s, when it reacts with SO2, during continuous recircula
tion, more and more concentrated in H2SO4 is produced and SO2
depleted in H2O2 in the course of time. This is mainly due the
equilibrium between SO2 and H2O2 (Henrys law constant) and
enhancement effect on the absorption of SO2 in to H2O2. The
convergence.
As shown in Figure 3, mass transfer takes place mainly in the
packed area (at the middle of the packed column). The air stream
enters in to the packed column with a SO2 composition of
0.0727 Kmol/m3 [CSO2(in)] and leaves at the outlet of the column
with a composition of 0.00364 Kmol/m3 [CSO2(out)], then the SO2
removal efficiency ( ) was calculated as =[CSO2(in)CSO2(out)/
CSO2(in)]x100. The SO2 removal efficiency obtained from the
simulation was 94.99%. Since the wall effect was not considered
for analysis there was a high SO2 concentration gradient shown at
the wall of the column (Figure 3).
Maheswari et al. Atmospheric Pollution Research (APR) 468

Absorption performance with H2O2 tremendously increases

relative to the pure water. This is due to the enrichment effect
taking place during the chemical reaction between SO2 and H2O2
which increases the mass transfer. H2O2 with 0.1 M involves in
increasing the absorption rate with SO2 up to nth iterations
simulated using CFD and the removal efficiency obtained was
94.99%. Similarly for H2O2 concentrations 0.01 M, and 0.05 M
results were obtained and produces 82%, and 85%, removal
efficiency respectively.

5.2. Experimental results

Experimental runs were carried out in a pilot plant

experimental system as detailed in Section 4. The computed
and experimental removal efficiencies were compared with the
influence of water as an absorbent and H2O2 with different
concentrations.

From the Figure 4, it appears that during water absorption, for

constant inlet SO2 concentration of 5 000 ppm, absorption rate
was moderate up to 55% but during continuous recirculation, the
absorption rate decreases to 45%. The variation in the absorption
rate is due to instantaneous reaction of SO2 takes place initially but
during continuous runs absorption rate decreases. SO2 removal
efficiency increases with increase in H2O2 concentration. When the
concentration increases, the time taken for desulfurization process
decreases, thus it has a direct influence on the absorption. The SO2
removal efficiency obtained from the experiments were in well
agreement with CFD simulation results (Figure 5).

Simulation and experimental results were obtained for various

H2O2 concentrations such as 0.01 M, 0.05 M, 0.1 M and 0.2 M.
Figure 3. SO2 outlet molar concentration profile using 0.1 M H2O2 as an Hence the developed CFD modeling can be used for designing the
3
absorbent (kmol/m ). packed column to get the maximum removal efficiency.

Figure 4. Responses for SO2 absorption in water and H2O2.

Maheswari et al. Atmospheric Pollution Research (APR) 469

However, some limitations need to be considered when H2O2 Nomenclature

is used as a reactant. Corrosion and causticity are the major
problems which affect the experimental system. To solve this, Liquid inlet flow rate to GasLiquid absorption column
packed column with acid tanks were fabricated using acrylic Lm :
(Lph)
material and less concentrated (0.1 M H2O2) acid was used for
experiments. As compared to water as an absorbent, the system is Gas inlet flow rate to GasLiquid absorption column
Gm : 3
more economical when H2O2 is used as a reactant. After the (m /hr)
continuous recirculation of hydrogen peroxide for several hours, it SO2 : Sulfur dioxide
becomes reusable concentrated sulfuric acid.
H2O2 : Hydrogen peroxide
H2SO4 : Sulfuric acid
PSO2 : Partial pressure of SO2 (KPa)
PTOT : Total pressure of the packed column (KPa)
X : Mole fraction of the solute in equilibrium
Y : Mole fraction of gas in equilibrium with liquid
H : Henrys constant
X1 : Mole fraction of aqueous H2SO4 leaving the column
X2 : Mole fraction of aqueous H2SO4 entering the column
Mole fraction of SO2 in gas stream leaving the column
Y2 :
with time
Y1 : Mole fraction of SO2 in gas stream entering the column
K4 : Flooding factor
FLV : Pressure drop or abscissa
G : Density of SO2 gas
L : Density of aqueous H2SO4
Figure 5. Comparison of experimental and CFD simulation results. v : SO2 gas density at 20 C
L : Liquid viscosity
6. Conclusions FP : Packing factor for 25 mm polypropylene pall ring
Gas mass flow rate per unit column cross sectional
The most widely used technique to remove SO2 from flue gas Vw :
is the absorption. When H2O2 is used as a reactant in wet scrubbing area
process, it produces no resultant pollutants to the atmosphere. A : Area of the packed column
This present work was concentrated on the equipment, packed Z : Total packed height
column design using mathematical correlations and based on this,
the parameters of the packed column were calculated as: diameter HOG : Height of the transfer unit
152 mm, total height 2 500 mm, packed height 1 000 mm, inlet NOG : Number of transfer units
liquid flow rate 150 Lph and inlet gas flow rate 40 m3/hr. Based on
these parameters, CFD model of the packed column was devel CSO2 : Concentration of SO2
oped. The developed CFD model was used to estimate the gas : SO2 removal efficiency
liquid absorption rate which can be applied to the design of v : Droplet velocity vector
industrial packed columns. The model can be used as an effective
tool for the design and analysis of the packed column used for : Continuous phase density
industrial purposes. CFD and experimental analysis were carried vgi : Gas velocity at ith element
out by considering H2O2 as an absorbent. The experimental and
simulation results clearly show that, SO2 removal efficiency in : Liquid phase dynamic viscosity
creases with increasing H2O2 concentrations. The simulated model : Binary gas diffusion coefficient of SO2 in H2O2
was validated suitably with an experimental pilot plant. The
: Mass fraction of a component A in gas phase
calculated values of SO2 removal efficiency agreed well with the
experimental results. Also hydrogen peroxide can be used as an
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