Article

pubs.acs.org/IECR

Absorption of Sulfur Dioxide with Sodium Hydroxide Solution in

Spray Columns
Zhanke Wang, Yu Peng, Xiaocong Ren, Shaoyong Gui, and Guangxu Zhang*

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School of Chemistry, Chemical Engineering and Life Science, Wuhan University of Technology, Wuhan 430070, Hubei, China
ABSTRACT: The absorption of sulfur dioxide into highly concentrated sodium hydroxide in a spray column from simulated
ue gas was investigated. The inuences of dierent operating conditions on the SO2 removal eciency, such as sodium
hydroxide concentration, liquid-to-gas ratio, gas velocity and SO2 concentration, were examined. The overall volume transfer
coecients (kGa), under moderate conditions, were obtained by introducing the instantaneous and irreversible chemical reaction
into the two-lm theory to establish a model that allowed the calculation of theoretical values of the overall volume-transfer
coecient. It was found that the absorption process was controlled by diusion through gas lm when a highly concentrated
caustic soda solution was adopted. The overall volume-transfer coecient was essentially independent of concentration of SO2 in
gas phase and positively related to the gas and liquid ow rates. The formula of kGa was tted for the process and found to be in
good agreement with experimental results.

1. INTRODUCTION
Air pollution caused by sulfur oxides (SOX) in exhausted gas
from marine diesel engine has been a global issue and a hot
research topic. The emission limits for SOX has been dictated in
International Maritime Organization (IMO) Regulation 14.
However, naturally occurring low-sulfur fuel is insucient and
rening to remove sulfur content is expensive. It is an
alternative method of mitigating SOX emissions by the lessexpensive high-sulfur-content oil in combination with an
exhaust gas scrubber.1,2 Attributed to the low-cost advantage
of the raw material source, desulfurization with limestone
gypsum system has been a common ue gas desulfurization
(FGD) technique mainly used in coal power stations. However,
the practical marine application of this treatment is limited by
the large cubage, easy blockage, and the produced large amount
of solid waste. Wet ammonia FGD is prevalent for its
byproduct of ammonium sulfate fertilizer recently,3 but it is
swept aside for the ammonia escape and the constraint of the
discharge of wastewater containing the ammonia nitrogen. As
an important industrial absorption process to reduce air
pollution, removing sulfur dioxide from gas mixtures by
contacting it with an aqueous alkali hydroxide solution has
been considered to minimize scaling, plugging, and erosion
problems in the absorbent circuit.4,5
Several studies were reported previously about the chemical
absorption mechanism for the SO2OH ion system.612 The
transfer mechanism,6,7 theoretical calculation approaches,8,9
and some experiment researches about various types of reactors
on a laboratory scale1012 have been investigated. However,
only few studies involving the overall volume-transfer
coecient of absorption SO2 with sodium hydroxide solution
in a spray column were reported. Zidar6 discussed desulfurization in the NaOHSO2H2O system on a laboratory scale
using a falling lm reactor to scale down criteria for the spray
columns, which reported the enhancement factor and the
overall mass-transfer coecients and presented the gasliquid
equilibrium operation graphically in the low concentration of
caustic soda solution. However, in a practical application of
XXXX American Chemical Society

ships, the concentrated sodium hydroxide solution would be

adopted to increase the absorption rate.13
The main purpose of this study is the overall volume-transfer
coecient of the purication of euent gases containing sulfur
dioxide with high concentration sodium hydroxide solution in a
spray tower. Furthermore, the signicant rate of SO2 reduction
aected by the dierent operation conditions in the system was
also investigated.

2. THEORETICAL BACKGROUNDS
2.1. Physical and Chemical Properties of the System.
When sulfur dioxide is absorbed into aqueous alkaline solution,
the diusion of sulfur dioxide molecules from current gas phase
core to the gas/liquid interface and the dissolution in the
washing agent should be considered initially, according to the
equality of the chemical potentials in the phases, which could
be described by eq 1. It is often thought that the dissolution
process obeys Henrys Law in low concentrations of the sulfur
dioxide predominant in euent gases in practice. Some
dissolved acid gas molecules would be dissociated according
to eq 2, and others react with hydroxide ion directly, according
to eq 3, whereby hydrogen sulte reacts, in turn, with the
additional hydroxide ion to sulte, as shown in eq 4. The
hydrogen sulte could also react with the dissolved sulfur
dioxide molecules, according to eq 5. The above processes
would have something with the dissociation of the water
(according to eq 6), the caustic soda (according to eq 7), and
the products of the processes (according to eqs 810).
Dissolution:
SO2 (g ) SO2 (l)

(1)

Received: June 15, 2015

Revised: August 17, 2015
Accepted: August 24, 2015

DOI: 10.1021/acs.iecr.5b02146
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Dissociation:
SO2 + H 2O HSO3 + H+

(2)

Reaction:
SO2 + OH HSO3

(3)

Consecutive Reaction:
HSO3 + OH SO32 + H 2O

(4)

Reaction:
SO2 + SO32 + H 2O 2HSO3

(5)

Dissociation:

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H 2O H+ + OH

(6)
Figure 1. Concentration distribution of instantaneous and irreversible
reaction.

Dissociation:
NaOH Na + + OH

(7)

DS,L
NS =
cS,i = L kLcS,i
1
1

Dissociation:
Na 2SO3 2Na + + SO32

(8)

The diusing rate of NaOH is expressed as

D N,L
D N,L
NN =
c N,L
c N,L = L
2 L
2

Dissociation:
NaHSO3 Na + + HSO3

(9)

(10)

In the case of the scrubbing process in the spray tower, which

acts as a multiple-staged feeding reactor, the fresh sodium
hydroxide solution is fed at dierent stages, which leads to the
sucient fresh reactants and lower concentration of SO2
3 in
the column. In addition, the fresh sodium hydroxide solution is
the strong alkaline with high ionization equilibrium constant,7
because of eq 7, which will provide the surplus of the hydroxide
ion. The result of the circumstance is that eq 5 could be ignored
and eq 4 follows close behind eq 3. Therefore, the overall
reaction in the scrubber is described as shwn in eq 11. Besides,
eq 3 is very fast with a rate constant exceeding 109 (mol1 s1
L), and the eq 4 has a very much higher rate constant because
of the proton transfer reaction.9 As a result, the reaction 11
could be regarded as an instantaneous and irreversible reaction
under the condition of high concentration of reactants.6,14
SO2 + 2OH SO32 + H 2O

(13)

Regarding eq 11, 2NS = NN is obtained for the relationship of

stoichiometry. Therefore, eq 12 can be converted to the form of
eq 15, with the removal of the factors 1 and 2, using the
following relationship between L, 1, and 2:

Dissociation:

HSO3 H+ + SO32

(12)

L = 1 + 2

(14)

D N,L c N,L
kLcS, i
NS = 1 +
(2DS,L cS, i)

(15)

D N,L c N,L
L
=1+
1
2DS,L cS,i

(16)

According to eqs 15 and 16, the increase in cN,L will promote

the absorption of sulfur dioxide for the decrease of 1, and the
limiting case of cS,i = 0 would occur when the absorbent
concentration is high enough. In this case, the absorption
process conducts with the maximum rate expressed by eq 17,
and the appropriate critical concentration is calculated by eqs
1820:

(11)

2.2. Absorption Model. A comparison was made between

the predicted eects of chemical reaction on the absorption
process for some of the rigorous models (including penetration
theory, lm theory, eddy diusion theory, and surface theory)
and approximate methods by Glasscok and Rochelle.15 They
concluded that the steady-state model (for example, lm
theory) was the most eective for illustrating experimental data
and conducting the numerical simulation of acid gas-treating
process. On the basis of the lm theory, the instantaneous
irreversible reaction occurs only on the specic plane in liquid
lm and the plane is called the reaction surface.16 As shown in
Figure 1, in order to supply the plane with reactants, the sulfur
dioxide molecules diuse from the gas/liquid interface and the
sodium hydroxide molecules diuse from the liquid bulk. The
diusing rate of SO2 is expressed as

NS = k GpS,G

(17)

D N,L
NN =
(c N,L,C 0) = 2NS = 2k GpS,G
L

(18)

kL =

DS,L
L

2k DS,L
p
c N,L,C = G
kL D N,L S,G

(19)

(20)

When cN,L cN,L,C, as shown in Figure 2, the absorption

process is controlled by gas lm mass transfer, and the rate can
be calculated by eq 17 under the consideration of cS,i = 0.16
B

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3. EXPERIMENTAL METHODS AND DATA

INTERPRETATION
3.1. Experimental Work. A schematic diagram of the
experimental setup for the desulfurization is shown in Figure 3.
The experimental system consists of a mixing tank, an air
heater, a scrubber column, a spraying system, a demister, and an
instrumentation section. An air-mixing chamber simulates
dierent air velocities in the range of 3.05.0 m/s and SO2
concentrations of exhaust gas from diesel engine. The system is
equipped with a SO2 gas tank, a mixing section, and an air
compressor. SO2 concentrations can be controlled by the ow
of SO2 in the system with the rotameter. The SO2-laden air
ows to the vertical spray column and contacts counter-current
with the absorption solvent, which is pumped into the tower
through the atomizing nozzles and rotameter. The scrubber is a
cylindrical stainless steel column with a diameter of 0.125 m
and a height of 1.8 m. There are three nozzles with the interval
distance of 0.4 m inside the column. Figure 4 shows
information about the scrubber.
In the experiment, the concentration of SO2 ranged from 0
to 800 ppm. Experiments were performed by keeping the liquid
ow rate constant and varying the gas ow rate (100200 m3
h1), and by keeping the gas ow rate constant and varying the
liquid ow rate (7502000 L h1). The liquid recirculation
duration was controlled to be less than half an hour and the
change of liquid concentration could be ignored, resulting from
the presence of little SO2 and a large sum of NaOH in each run.
The pressure drop (p) between points A and B shown in
Figure 3 was measured to evaluate the ow resistance of the
equipment.
3.2. Data Interpretation. The mass-transfer coecient
(kG) is an important parameter, but it is dicult to measure,

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Figure 2. Concentration distribution of instantaneous and irreversible

reaction (in the case of cN,L cN,L,C).

When cN,L < cN,L,C, the absorption is governed by both gas lm

and liquid lm. The absorption rate of sulfur dioxide is obtained
with the help of gas lm transfer rate expressed by eq 21 and
the equilibrium condition of gas/liquid interface described by
eq 22.

NS = k G(pS,G pS,i )

(21)

cS,i = HpS,i

(22)

NS =

pS,G + D N,L /(2HDS,L )c N,L

1/(HkL) + 1/k G

(23)

Figure 3. Schematic diagram of the experimental setup.

C

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k Ga =

MS
VR pS,G,lm t

(30)

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4. RESULTS AND DISCUSSION

Experiments on the SO2 scrubbing have been conducted by
altering various process operating parameters, including sodium
hydroxide concentration, liquid-to-gas ratio (L/G), gas velocity,
and SO2 concentration. The scrubber SO2 removal eciencies
for eld tests are calculated using eq 31:
cSO2,out cSO2,in
(%) =
100
cSO2,out
(31)
where cSO2,in and cSO2,out are the concentrations of SO2 at the
inlet and outlet of the column, respectively.
4.1. Inuence of Sodium Hydroxide Concentration on
the Sulfur-Removal Eciency. Based on the preceding
description, the critical concentration of the sodium hydroxide
solution is the key point to determine the controllability of the
SO2 absorption process via gas-phase mass transfer. Figure 5
Figure 4. Brief schematic view of the spray column.

because of the diculty involved in determining the interface

area. However, the volume-transfer coecient (kGa) is easier to
obtain, by interpreting the global data from the measurements
at the inlet and outlet of the device. Based on the description
given in Section 2, because of the instantaneous and irreversible
reaction, the absorption of SO2 with concentrated NaOH
solution is governed by the diusion of SO2 through gas lm, if
the concentration of the solution is considerably higher than
the critical concentration. The equilibrium concentration of
SO2 at the gas/liquid interface is equal to 0 and the absorption
ux can be calculated using eq 17.
As a result, the absorption rate per unit volume is given as

NS = k GapS,G

Figure 5. Inuence of sodium hydroxide concentration on the sulfurremoval eciency (L/G = 5.55 L m3, cSO2,in = 300 ppm, Tab = 30 C).

(24)

and, overall, the eective volume of column is given as

MS = VR k GapS,G

shows that the absorption eciency of SO2 increases with the

aqueous alkali concentration. At the beginning, the rate of
desulfurization increases rapidly and then slowly when the
concentration of absorbent is >0.4 mol/L. This phenomenon
indicated that, when the cNaOH is low, the process is governed
by both gas lm and liquid lm mass transfer, and the sulfurremoval eciency increases as cNaOH because of the decrease in
1. Under the high concentration of sodium hydroxide solution
(for example, >0.9 mol/L), however, the distance between the
interface and the reaction surface is innitesimal, and the trend
of increasing sulfur-removal eciency slows for the control
process of gas lm mass transfer. Therefore, the critical
concentration can be supposed to be between 0.05 mol/L and
0.41 mol/L, which can be armed by eq 20, where kG and kL
can be calculated using the correlation obtained by Zidar.6
Furthermore, Schultes17 also reported that the rapid mass
transfer rate was so dominant that resistance lay exclusively in
the gas phase at a large mole fraction of sodium hydroxide
solution.
4.2. Inuence of Liquid-to-Gas Flow Rate Ratio on
Sulfur-Removal Eciency. The liquid-to-gas ratio (L/G)
refers to the ratio between the spraying volume ow rate and
the gas ow rate. It is a signicant parameter to report the
scrubbing performance, because a high ratio leads to high

(25)

The total amount of SO2 absorbed within the residence time

of gasliquid countercurrent in the eective volume of the
scrubber can be obtained as
MS = VR k Ga

pS,G dt

(26)

where t is calculated by

t =

VR
VG

(27)

pS,G dt = pS,G,lm t

(28)

where pS,G,lm is the logarithmic mean partial pressure of SO2,

which is dened by the expression
pS,G,in pS,G,out
pS,G,lm =
ln(pS,G,in /pS,G,out )
(29)
As a consequence, the volumetric overall mass-transfer
coecient is obtained as
D

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sulfur-removal eciency but high energy consumption and
operation costs. To ensure the desulfurization eciency, the
value of L/G usually ranges from 8 L m3 to 25 L m3.
Considering the high absorption ability of the strong base
solution, the inuence of a lower L/G value (varying from 5 L
m3 to 10 L m3) on the eciency of SO2 removal and the
total pressure drop were studied under the xed values of
absorbing temperature and concentrations of SO2 and alkaline
liquor. The results are shown in Figure 6. To keep the same

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Figure 7. Inuence of SO2 concentration on sulfur-removal eciency

and absorption rate (L/G = 5.55 L m3, cNaOH = 0.4 mol L1, Tab = 30
C).

results of the eect of inlet gas velocity on the removal

eciency are displayed in Figure 8. To keep the same

Figure 6. Inuence of liquid-to-gas ratio (L/G) on () sulfur-removal

eciency and () total pressure drop (VG = 200 m3 h1, cSO2,in = 575
ppm, cNaOH = 1 mol L1, Tab = 25 C).

residue time, the experiments were carried out at a constant gas

ow rate (VG), while the liquid ow rate (VL) was changed
according to the requested L/G value.
Figure 6 shows that the percentage removal of SO2 increases
sharply as the value of L/G increases at the beginning and then
slowly at L/G > 8 L m3, whereas the growth trend of pressure
drop is totally opposite. When the L/G increases at a xed
value of VG, VL rises in the scrubber and, thus, the contact area
of gasliquid also increases. Meanwhile, the pressure drop
increases for the highly loaded demister. When the ratio
exceeds 8 L m3, the droplet surface area is large enough, and
further increases in this ratio become meaningless, whereas the
load of the mist eliminator surges as a result of more droplets in
the gas ow. The result is consistent with the report by
Bandyopadhyay and Biswas.4
4.3. Inuence of SO2 Concentration on SulfurRemoval Eciency. The concentration of sulfur dioxide in
diesel exhaust varies with the sulfur content of fuels and the
operation points of engine. It is meaningful to consider the
eect of SO2 concentration in the feeding gas (cSO2,in) on the
sulfur-removal eciency. The results are shown in Figure 7. It
shows that higher removal eciency is achieved at lower initial
SO2 concentration. However, this does not mean higher
absorption rate. Actually, the absorption rate is proportional to
the initial SO2 concentration due to the increasing mass transfer
driving force: the partial pressure of SO2 in gas bulk. This
observation is in good agreement with eq 20 and it suggests
that some measures (e.g., increasing L/G) should be taken to
achieve higher sulfur removal eciency in the case of high
initial SO2 concentration.
4.4. Inuence of Inlet Gas Velocity on the SulfurRemoval Eciency. The velocity of inlet gas will aect both
the volume of the scrubber and the total pressure drop, with
regard to the cost of the device and operation, respectively. The

Figure 8. Inuence of inlet gas velocity on the sulfur-removal

eciency (L/G = 7 L m3, cSO2,in = 550 ppm, cNaOH = 0.4 mol L1, Tab
= 25 C).

absorption conditions, the trial was conducted at a xed L/G

value, which indicated that the liquid ow rate varied with the
gas ow rate, according to the given L/G value.
As shown in Figure 8, an initial increase in the SO2 removal
rate is observed from the elevation of inlet gas velocity and then
a sharp decrease occurs after the gas velocity exceeds 4.0 m s1.
There are two major factors regarding the inlet gas velocity that
inuence the absorption rate. On one hand, the resistance of
gas lm declines as the turbulence intensies when the gas ow
rate increases, as well as the droplet Stokes diameter, which is
inversely proportional to the gasliquid contact area.18 On the
other hand, as the gas ow rate increases, the residence time of
vaporliquid contact and mass transfer decreases. At the low
velocity, the former is the dominant factor, so the removal rate
of SO2 increases as the inlet gas velocity increases; at the high
velocity, the process is dependent on the latter factor.
4.5. Interpretation of the Mass-Transfer Coecient. In
order to predict the removal eciency of SO2 in an alkaline
scrubber, empirical and semiempirical correlations were
developed. Lorent et al.19 have studied the sulfur dioxide
absorption process in the sodium sulte solutions in a cable
contactor. They developed a semiempirical calculation and
found that the overall mass-transfer coecients increased with
the liquid ow rate and gas velocity and slowly with the pH.
E

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Since a high concentration of sodium hydroxide solution was
introduced in this experiment, the inuence of pH could be
considered to be negligible. However, it is necessary to take the
inlet concentration of sulfur dioxide, as well as the gas and
liquid ow rates, into consideration.
The inuence of the inlet SO2 concentration on volumetric
overall mass-transfer coecient is described in Figure 9. It

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Figure 11. Inuence of liquid ow rate on the volumetric overall masstransfer coecient.

increase completely, because of the limited liquid holdup of the

scrubber, which could also be observed through Figure 11.
Based on the results of the experiments and previous
reported studies, kGa is a function of VG and VL at a xed
temperature:
Figure 9. Inuence of the inlet SO2 concentration on the volumetric
overall mass-transfer coecient.

k Ga = AVG aVL

(32)

where A is a constant when the temperature is xed. With the

regression analysis method, those coecients were obtained at
an absorption temperature of 25 C, as follows:

shows that kGa remains constant, independent of the initial gas

phase concentration, which means that kGa is irrelevant to
cSO2,in. This fact further shows that the scrubbing process under
consideration is controlled by gas-phase mass transfer. In
contrast, the volumetric overall mass-transfer coecient has a
relationship with the gas ow rate and the liquid ow rate. As
shown in Figure 10, kGa maintains an upward tendency with

k Ga = 3.379 103VG 0.9118VL 0.3037

(33)

The comparison between predicted values and the

experimental data is presented in Figure 12. It can be seen

Figure 12. Comparison of calculated and experimental volumetric

overall mass-transfer coecient.

Figure 10. Inuence of gas ow rate on the volumetric overall masstransfer coecient.

that the predicted values t well with the experimental values

(well within a deviation of 10%) when the absorption
temperature is 25 C and the absorbent concentration is >0.9
mol L1. In addition, an interesting phenomenon should be
given attention: experimental values that are obtained under the
conditions of higher temperature or lower absorbent
concentration diverge greatly from the calculative values.
Obviously, a lower concentration of the absorption liquid
does not conform to the model assumption. With regard to the
absorption temperature, the dissolution process of SO2 is
accompanied by an evolution of heat; therefore, sulfur dioxide
solubility decreases as the temperature increases. Actually, the
dissolved sulfur dioxide molecules in liquid begin to desorb at

the increasing gas ow rate, which may be induced by the

increase in kG. The high gas ow rate implies intensied
turbulence, which may contribute to the decreased resistance in
the gas lm and the increase in kG. Although the value of kGa
increases with the liquid ow rate, a slow tendency should be
given attention when the liquid ow rate surpasses 1600 L h1,
which can be observed in Figure 11. This phenomenon may be
attributed to the fact that the increased spray rate is likely to
lead to an increase in the spraying density and a decrease in the
droplet Stokes diameter, both of which give rise to an increase
in the specic interface area, according the equation given by
Wu et al.20 Furthermore, the specic interface area could not
F

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2 = distance between the reaction surface and liquid bulk, m

L = thickness of liquid lm, m
= sulfur-removal eciency

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20 C and the amount of desorption is proportional to the

temperature.21 In conclusion, eq 33 is applicable to the low
adsorption temperature and high concentration of absorption
solution.

Subscripts

5. CONCLUSIONS
The theoretical analysis presented and the experimental results
described reveal that the absorption of SO2 into a highly
concentrated sodium hydroxide solution in a spray tower is
controlled by gas side lm mass-transfer resistance, and the
reaction is instantaneous and irreversible. The increase in the
vaporliquid contact area and the decrease of the gas lm
resistance are benecial to increasing the sulfur-removal
eciency. The volumetric overall mass-transfer coecient
increases with the liquid and gas ow rate. The inlet sulfur
dioxide concentration has no inuence on kGa. A semiempirical
equation is in good agreement with the experimental data
under certain conditions. In addition, diesel engine exhaust
contains many dierent species that would have potential
eects on the desulfurization, so further study will focus on the
impacts of other acid species in exhaust gas, as well as
particulates, upon the removal of sulfur dioxide.

C = critical value
i = interface
G = gas or gas lm
L = liquid or liquid lm
lm = logarithmic mean
N = sodium hydroxide
R = reactor
S = sulfur dioxide

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AUTHOR INFORMATION

Corresponding Author

*Tel./Fax: +8627 87859019. E-mail address: zhanggx2002@

163.com.
Author Contributions

Concepts for research program were conceived by all authors.

Experiments were devised by G.X.Z., together with Z.K.W.,
who carried them out and performed data analysis. All authors
have given their approval to the nal version of the manuscript.
Notes

The authors declare no competing nancial interest.

ACKNOWLEDGMENTS
The authors are grateful to Yunfeng Yang, Rui Shi, Guomeng
Zhang, and Jun Deng for discussions and assistance.
ABBREVIATIONS
IMO = International Maritime Organization
FGD = ue gas desulfurization
L/G = liquid-to-gas ratio
eq = equation
eqs = equations

NOTATION
a = specic interface area, m2 m3
c = concentration, mol L1 or ppm
D = diusion coecient, m2 s1
H = Henry constant, kPa
k = lm mass transfer coecient, mol m2 kPa1 s1 or m s1
M = absorption rate of whole the column, mol s1 or mol
N = mass ux, mol m2 s1
N = absorption rate per unit volume, mol m3 s1
p = pressure, kPa
t = time, h
V = volume or volumetric ow rate, m3 or m3 h1 or L h1
= constant
= constant
= increment
1 = distance between the interface and reaction surface, m
G

DOI: 10.1021/acs.iecr.5b02146
Ind. Eng. Chem. Res. XXXX, XXX, XXXXXX

Article

Industrial & Engineering Chemistry Research

Downloaded by SUNY UPSTATE MEDICAL UNIV on August 28, 2015 | http://pubs.acs.org

Publication Date (Web): August 27, 2015 | doi: 10.1021/acs.iecr.5b02146

(21) Liu, S. Y.; Nengzi, L. C.; Qiu, W.; Xu, Y. Y.; Liu, J. Y. Process
and kinetics of SO2 absorption by carbide slag in spray tower. CIESC J.
2012, 63, 1543.

DOI: 10.1021/acs.iecr.5b02146
Ind. Eng. Chem. Res. XXXX, XXX, XXXXXX