Chemical Engineering Science 235 (2021) 116467

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Chemical Engineering Science

journal homepage: www.elsevier.com/locate/ces

Green and efficient sulfur dioxide removal using hydrogen peroxide in

rotating packed bed reactor: Modeling and experimental study
Yu-Ning Dong a, Wen-Cong Chen a, Liang-Liang Zhang a,⇑, Bao-Chang Sun a, Hai-Kui Zou a, Yong Luo a,
Guang-Wen Chu a,b, Jian-Feng Chen a,b
a
Research Center of the Ministry of Education for High Gravity Engineering and Technology, Beijing University of Chemical Technology, Beijing 100029, PR China
b
State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029, PR China

h i g h l i g h t s g r a p h i c a l a b s t r a c t

A mathematic model was first

developed to describe mass transfer
process in RPB.

The outlet SO2 concentration was
ultra-low, below 35 mg/m3.

The predicted desulfurization
efficiency agreed well with the
experimental result.

The HTU for RPB is one order of
magnitude lower than that of
conventional reactors.

a r t i c l e i n f o a b s t r a c t

Article history: In order to reduce SO2 emissions and achieve green utilization of sulfur resources, a desulfurization
Received 27 September 2020 method of SO2 removal using hydrogen peroxide (H2O2) in rotating packed bed (RPB) is proposed. It
Received in revised form 12 December 2020 can not only achieve the efficient removal of SO2, but also lead to the effective utilization of sulfur
Accepted 16 January 2021
resources. A mathematic model was first developed to describe the reaction and mass transfer process
Available online 29 January 2021
between H2O2 and SO2 in RPB. The influences of different operating conditions including RPB rotating
speed, H2O2 mass fraction, gas–liquid volumetric flow rate ratio, gas flux, and inlet SO2 concentration
Keywords:
on desulfurization performance were studied. Under the optimized conditions, it turned out that the
SO2 removal
Hydrogen peroxide
desulfurization efficiency was above 99% and the outlet SO2 concentration was ultra-low, below
Rotating packed bed 35 mg/m3. The validity of the model was confirmed by the fact that most of the predicted desulfurization
Mathematic model efficiency agreed well with the experimental result with a deviation within 5%. The height of mass trans-
fer unit HTU for RPB is calculated to be 1.60–2.07 cm, which is one order of magnitude lower than that of
conventional reactors, indicating the investment of the desulfurization reactor can be greatly reduced by
using RPB.
Ó 2021 Elsevier Ltd. All rights reserved.

1. Introduction
Sulfur dioxide (SO2) is one of the major atmosphere pollutants
which causes destructive effects on environment and human
⇑ Corresponding author.
E-mail address: zhll@mail.buct.edu.cn (L.-L. Zhang).
health (Qian et al., 2018). Via reaction with oxidant and water
vapor in the atmosphere, SO2 converts into sulfuric acid, leading
to acid rain problem that ruins water resource and corrodes build-
ings (Dahlan et al., 2009; Vidal et al., 2007). SO2 will cause respira-
tory tract illnesses if the concentration of SO2 exceeds a certain
level (Karagoz et al., 2018). Recently, it has been found that sulfate
and other secondary aerosol productions caused by SO2 emissions

https://doi.org/10.1016/j.ces.2021.116467
0009-2509/Ó 2021 Elsevier Ltd. All rights reserved.
Y.-N. Dong, W.-C. Chen, L.-L. Zhang et al.
Notation
a gas–liquid effective interfacial area, m2/m3
at specific area of packing per unit volume, m2/m3
c H 2 O2 concentration of H2O2 in absorbent solution, mol/L
cSO2 concentration of SO2 in liquid phase, mol/L
cSO2 ;O SO2 concentration at gas–liquid interface, mol/L
cH2 SO4 concentration of H2SO4 in liquid phase, mol/L
d diameter of spheral droplet, m
dp effective diameter of the packing = 6(1-e)/at, m
DSO2 diffusivity of SO2 in absorbent, m2s1
DG diffusivity of SO2 in gas phase, m2s1
g0 characteristic centrifugal acceleration (100 ms2),
ms2
G gas flux, m3m2s1
GI inert gas molar flow rate, molh1
h axial height of packing, m
H henry constant of SO2 in absorbent, kPam3kmol1
HTU the height of mass transfer unit, cm
k kinetic constant of reaction (4), Lmol1s1
kov pseudo first order rate constant, s1
kG gas-side mass transfer coefficient, kmolkPa1m2h1
kL liquid-side mass transfer coefficient, ms1
KG overall mass transfer coefficient, kmolkPa1m2h1
L liquid flux, m3m2s1
Dl distance between two packing layers in RPB, m
MG mole mass of gas mixture, g/mol
Mi mole mass of component i, g/mol
N the rotating speed, rpm
NTU the number of mass transfer unit
N
 SO2 mass transfer flux of SO2 into absorbent, molm2s1
NSO2 average mass transfer rate, molm2s1
P experimental operating total pressure, kPa
r quadratic mean radius of packing, m
are mainly responsible for the severe urban haze formation (Guo
et al., 2014b; Heo et al., 2016; Ma et al., 2018).
SO2 mainly exists in the flue gas of power plants, metallurgical
furnaces, sulfuric acid plants or some chemical plants. To control
the SO2 emission, several industrial flue gas desulfurization (FGD)
methods have been developed. Although these methods have been
used for several decades, they are still accompanied by some inher-
ent shortcomings. For example, the lime-limestone process, which is
the foremost used technology, has the problem of a solid by-product
waste (CaSO4) (Scala and Salatino, 2010). At the same time, if the
concentration of sulfur dioxide in the emission gas is high, the desul-
furization efficiency is difficult to meet the requirements of environ-
mental regulation. Sodium hydroxide desulfurization can greatly
improve the removal efficiency, but it generates a large number of
wastewater which increases the load of subsequent water treatment
process. Capture SO2 with organic amines, such as ethylene diamine,
will bring about the volatile organic compounds (VOC) pollution
because of the significant solvent evaporation (Wei et al., 2014).
The ammonia scrubbing technology realizes the utilization of the
SO2, but it will also cause secondary pollution due to the NH3
volatilization and aerosol formation (Pan et al., 2016; Pan et al.,
1991). In general, the current desulfurization methods couldn’t ade-
quately solve the problems of difficult utilization of by-products and
secondary pollution. Nowadays, green chemistry technology,
defined as the chemical products and processes that lessen or pre-
vent waste substances (Kinidi and Salleh, 2017) has become more
and more significant because it’s beneficial to both environment
and economy. There are massive researches about green chemistry
methods in various application areas including wastewater treat-
ment (Kinidi and Salleh, 2017; Sepehri et al., 2019; Sepehri and
2
Chemical Engineering Science 235 (2021) 116467
rin the inner radius of packing,m
rout the outer radius of packing, m
r SO2 reaction rate of SO2, molL1s1
R radius of spheral droplet, m
Rg gas constant, Jmol1K1
S renewal frequency, s1
t mean lifetime of liquid film, s
T experimental operating temperature, K
u liquid flow rate per unit area, m/s
u0 characteristic flow rate per unit area (1 cm/s), m/s
ur liquid mean radial velocity, m/s
yi mole fraction of component i in gas phase
yin SO2 concentration of inlet gas
yout SO2 concentration of outlet gas
ySO2 mole fraction of component SO2 in the gas
ySO2 equilibrium mole fraction of component SO2 in the gas
Greek letters
e voidage of packing
eL liquid hold-up in RPB, m3m3
lG viscosity of gas, kgm1s1
qG density of gas, kgm3
q density of liquid, kgm3
r surface tension of the liquid, N/m
ʋ kinematic viscosity of liquid, m2/s
ʋ0 characteristic kinematic viscosity (106 m2/s), m2/s
ɷ (H2O2) = H2O2 mass fraction, %
Dimensionless Groups
ReL ¼ aLt tWeL ¼ qrLat Fr L ¼
2
L2
ReG
lG
¼ aGtqlG ScG ¼ q
ð2pN=60Þ2 rdp G G DG
Sarrafzadeh, 2018), solid waste disposal (Jun et al., 2016) etc. For
SO2 removal, the development of desulfurization technology based
on green chemistry is also of great importance.
The use of hydrogen peroxide (H2O2) provides an attractive
option for SO2 removal. SO2 can directly convert into valuable pro-
duct, H2SO4, through the oxidation of H2O2 without generating other
by-products. This route achieves the utilization of sulfur resource
and avoids the secondary pollutants. From the standing point of
green chemistry and atom economy (Trost, 1991), these advantages
make H2O2 desulfurization methods an attractive way to capture
SO2 from industrial flue gas. However, the traditional implementa-
tion in conventional reactors makes this method unpopular. First,
with the growing concerns on environmental issues, the allowable
emission index of SO2 is continuously reduced. For example, now
in China, SO2 emission standards for new chemical enterprises and
coal-fired power plants are reduced to 100 mg/m3 and 35 mg/m3,
respectively (Han et al., 2017). At the same time, the desulfurization
efficiency of hydrogen peroxide oxidation method is slightly lower
as in comparison with the alkaline-based absorption method. Some-
times, it is difficult to meet the ever-increasing desulfurization
requirement. Second, it requires a huge traditional reactor to imple-
ment this H2O2 scrubbing process. Considering the existence of
H2SO4 and H2O2 in the absorbent, the building material for the
equipment must be resistant to corrosion and oxidation, which
increases the total investment of the equipment. Therefore, it’s
important to develop a process intensification technology to
improve desulfurization efficiency and to reduce equipment size
and investment.
The rotating packed bed (RPB), also known as Higee (High grav-
ity) is a novel process intensification device, which was first devel-
Y.-N. Dong, W.-C. Chen, L.-L. Zhang et al.
oped by Ramshaw and Mallinson (1981). It has been applied as a
key reactor or contactor for various chemical processes including
chemical absorption (Guo et al., 2014a; Joel et al., 2017; Pei
et al., 2017; Xie et al., 2017), oxidation (Chen et al., 2004; Chang
et al., 2009; Zeng et al., 2013), reactive crystallization (Chen
et al., 2003; Sun et al., 2011), and cationic polymerization (Chen
et al., 2009) etc, which are generally fast or instantaneous reactions
limited by the gas–liquid mass transfer. RPB is designed to gener-
ate high acceleration via the use of the centrifugal field to simulate
the high-gravity environment (Su et al., 2018). In RPB, liquids are
split into thin liquid films or tiny liquid droplets (Neumann et al.,
2018), which leads to large gas–liquid contact interface resulting
in enhanced gas–liquid mass transfer. It has been reported that
mass transfer coefficient of RPB is at least an order of magnitude
higher than that of conventional packed column (Zhang et al.,
2013; Chen and Liu, 2002).
In this work, we proposed a green and efficient approach for
SO2 removal by using H2O2 absorption in RPB. This approach
combines the advantage of RPB as a high effective reactor and
H2O2 as green absorbent to achieve efficient and green utiliza-
tion of sulfur resources. A mathematic model was first developed
to describe the reaction and mass transfer process between H2O2
and SO2 in RPB. The experiment was conducted to verify the
model in a wide range of operating conditions including RPB
rotating speed, H2O2 mass fraction, gas–liquid volumetric flow
rate ratio, the gas flux, and inlet SO2 concentration. Moreover,
the SO2 removal performance between conventional reactors
and RPB was compared.
2. Model development
2.1. Chemical reaction
The SO2 absorption process with H2O2 solution can be described
by the following steps:
(1) Diffusion of SO2 from gas phase into liquid phase. The pro-
cess is expressed as:
SO2 ð g Þ $ SO2 ðlÞ ð1Þ
(2) Reaction of SO2 and H2O. SO2 reacts with H2O, forming sul-
furous acid.
SO2 ðlÞ þ H2 O $ H2 SO3 ð2Þ
(3) Oxidation of H2SO3. Considering the existence of H2O2,
H2SO3 is oxidized, producing H2SO4 as a by-product.
H2 SO3 þH2 O2 ! H2 SO4 þH2 O ð3Þ
This oxidation reaction promotes the SO2 hydration process.
Thus, SO2 is absorbed into H2O2 solution continuously.
The SO2 absorption process is described by the following overall
reaction:
SO2 þH2 O2 ! H2 SO4 ð4Þ
Based on the research of Thomas et al. (Thomas et al., 2003a;
Colle et al., 2005; Colle et al., 2008; Colle et al., 2004; Thomas
et al., 2003b), reaction (4) is fast and considered to be first order
to both SO2 and H2O2. The kinetic equation is written as:
r SO2 ¼ kcSO2 cH2 O2 ð5Þ
3
Chemical Engineering Science 235 (2021) 116467
Compared with the SO2 input, if the hydrogen peroxide is highly
excess, the concentration of H2O2 will have little change. So H2O2
concentration can be regarded as a constant. And the reaction (4)
is thought to be pseudo-first order reaction. The rate equation is:
rSO2 ¼ kov cSO2 ð6Þ
where kov is pseudo-first order rate constant and defined as
kov ¼ kcH2 O2 ð7Þ
2.2. Basic assumptions
Compared with conventional packed bed, the hydrodynamic
characteristics in rotating packed bed are more complicated.
According to visual study in RPB (Burns and Ramshaw, 1996), film
flow and droplet flow are commonly observed in packing zone. The
rotating speed is an important parameter affecting the liquid flow
pattern in RPB. In Burns’ study (Burns and Ramshaw, 1996), dro-
plet flow is the main form of liquid flow in RPB when the rotating
speed is approximately above 800 rpm (the high gravity is 70g
based on the arithmetic mean radii of the RPB) Visual study con-
firmed that there were film, droplet and ligament form flow in
the RPB and the liquid flew mostly as film attaching the packing
when the rotating speed was low, but mostly as droplet filling
the voids of the packing when the rotating speed was high
(Burns and Ramshaw, 1996). The liquid flow pattern not only
affected the form of molecular diffusion depth, but also affected
the interfacial area of gas–liquid mass transfer. In order to simplify
the model, we assumed that the liquid existed only in one form at a
special RPB rotating speed. The detailed basic assumptions of this
model are listed as follow:
(1) In RPB, liquid flows in the film form when the high gravity
level is below 70g (the rotating speed is 200–800 rpm based
on the quadratic mean radii of the RPB) and in the droplet
form when high gravity level is above 70g (rotating speed
is 1000–1400 rpm).
(2) The volatilization of absorbent is ignored and the inert gas
nitrogen is not dissolved into H2O2 aqueous solution. So
the flow rate of the inert gas is regarded as constant in the
absorption process.
(3) The gas pressure drop in RPB has been extensively studied
through experimental method and CFD simulation (Wang
et al., 2019). It’s found that pressure drop of counter-flow
RPB is in the range of 10–3000 Pa, concentrated in 10–
300 Pa (Hu et al., 2013). Besides, in our SO2 absorption
experiment, SO2 partial pressure is less than 100 Pa. So the
gas pressure drop can be neglected in RPB in this work.
(4) The reaction between SO2 and H2O2 is exothermic. But the
concentration of H2O2 in aqueous solution of this work is rel-
atively low, and the temperature increase of the absorption
is very small. So the variation of temperature of the reactant
system is ignored and the SO2 absorption in RPB is regarded
as isothermal absorption process.
2.3. Model development
Fig. 1(a) displays a typical structure of RPB. The liquid phase
enters RPB through a liquid distributor with 4 holes and is sprayed
towards the inner edge of the packing. The liquid phase flows out-
wards through packing via a centrifugal force. Meanwhile gas
phase moves inward from outer edge of RPB. Then SO2 is absorbed
from gas phase into the liquid phase.
The overall gas–liquid mass transfer coefficient (KGa) is one of
the important parameters to evaluate mass transfer performance.
Y.-N. Dong, W.-C. Chen, L.-L. Zhang et al. Chemical Engineering Science 235 (2021) 116467

Fig. 1. (a) Schematic diagram of an RPB, (b) Sketch of packing in RPB, (c) Vertical view of packing micro element.

The desulfurization efficiency can be obtained by the calculating of 2.3.1. Liquid-side mass transfer coefficient
KGa. Based on our assumption, when the high gravity level is below
The overall mass transfer rate under a steady condition can be 70g, liquid phase flows only in the film form. The mass balance of
written as SO2 diffusion into a liquid film can be expressed as

 8
@cSO @ 2 cSO
NSO2 a ¼ K G a  P ySO2  ySO2 ð8Þ >
> 2
¼ DSO2 @x2 2  kov cSO2
>
> @t
<
0 < x < 1; t > 0
Fig. 1(b) is the sketch of packing in RPB with inner radius, outer ð13Þ
>
> cSO2 ðx; 0Þ ¼ 0
radius, and axial height of rin, rout, and h respectively. Considering >
>
:
an annular element of packing with an axial height of h and radial B:C: cSO2 ð0; t Þ ¼ cSO2 ;0 ; cSO2 ð1; tÞ 6 0
thickness of dr, as presented in Fig. 1(c), the mass balance can be
given as cSO2 ;O is the SO2 concentration at the gas–liquid interface. Consider-
ing the reaction (4) is fast and irreversible, equilibrium concentra-
!
ySO2 tion of SO2 in liquid phase is close to zero.
NSO2 a  2prhdr ¼ GI d ð9Þ Letting cA ¼ cSO2 , an ordinary differential equation is obtained
1  ySO2
by using Laplace transform.
Combining equations (8) and (9), it can be obtained 8 2 
< DSO2 d 2c A  ðs þ kov Þc A ¼ 0
! dx ð14Þ

 :  cSO
2 ;0

ySO2 B:C: c A ð0; sÞ ¼ ; c A ð1; sÞ 6 0
K G a  P  ySO2  ySO2  2prhdr ¼ GI d ð10Þ s
1  ySO2
The solution to equation (14) is
For a fast chemical reaction, ySO2 is usually close to zero and it sffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi!
 cSO2;0 s þ kov
can be negligible. Then KGa can be obtained by integrating equation c A ðx; sÞ ¼ exp x ð15Þ
s DSO2
(10)

   The function of SO2 concentration to time and depth in the liq-

GI yin ð1  yout Þ yin yout uid film is deduced by using Laplace inverse transform.
KGa ¼    ln þ 
pPh r2out  r 2in yout ð1  yin Þ 1  yin 1  yout  qffiffiffiffiffiffiffi  pffiffiffiffiffiffiffiffiffi
cSO
ð11Þ cSO2 ¼ 2
2 ;0
exp x kov
DSO
erfc p ffiffiffiffiffiffiffiffi
x ffi  k ov t
2 2 DSO t
2
 qffiffiffiffiffiffiffi  pffiffiffiffiffiffiffiffiffi ð16Þ
It should be noted that the calculated KGa represents the aver- cSO ;0
þ 22 exp x DkSOov erfc 2pffiffiffiffiffiffiffiffi
x ffi þ kov t
ages KGa of the packing (Sheng et al., 2016) According to equation D t
2 SO2

(11), when KGa is calculated, outlet SO2 concentration yout is

obtained and desulfurization efficiency can be inferred. And based on first Fick law, the interface mass transfer rate
Based on two-film theory, the overall mass transfer coefficient (x = 0) is written as
(KGa) is determined by the following equation @cSO2
RSO2 ¼ DSO2 jx ¼ 0
@x
"rffiffiffiffiffiffiffiffiffi #
1 1 H qffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
pffiffiffiffiffiffiffiffiffi
¼ þ ð12Þ DSO2
¼ cSO2 expðkov tÞ þ kov DSO2 erf kov t ð17Þ
K G a kG a kL a pt
where kLa is liquid-side mass transfer coefficient and kGa is gas-side where erfc(x) is the excess error function and erf(x) is the error
mass transfer coefficient. H is the Henry’s constant of SO2 in absor- function. In RPB, liquid film is renewed every time it passes through
bent solution. one layer of packing. The renewal frequency is calculated by
4
Y.-N. Dong, W.-C. Chen, L.-L. Zhang et al. Chemical Engineering Science 235 (2021) 116467

ur pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi 
S¼ ð18Þ d sinh kov =DSO2 R
Dl cSO2 ¼ cSO2 ;0 pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi  ð28Þ
2R sinh kov =DSO2 ðd=2Þ
where Dl is the distance between the two packing layers in RPB. ur
is liquid mean radial velocity and is determined by empirical equa- Furthermore, the liquid-side mass transfer coefficient (kL) can
tion(Guo et al., 1997) be calculated according to the following equation
" 2 #0:5448 
2p N dcSO2 
ur ¼ 0:0217L0:2279 r ð19Þ kL cSO2 ;0 ¼ DSO2 R ¼ d=2 ð29Þ
60 dR 

For the smooth liquid film with constant lifetime, the Higbie age Therefore, the mass transfer coefficient of SO2 in droplet can be
distribution function of mass transfer in the film can be defined as expressed as

1  "sffiffiffiffiffiffiffiffiffi sffiffiffiffiffiffiffiffiffi ! #
wðtÞ ¼  ; 0<t<t ð20Þ kov kov d d
t kL ¼ DSO2 =tanh  ð30Þ
DSO2 DSO2 2 2
The mean lifetime of liquid film is calculated by
When the rotating speed is high, liquid flow pattern is droplet
 1
t¼ ð21Þ flow in the void of packing. The mass transfer interfacial area of
S droplet depends on operating conditions and characteristics of liq-
With equations (17) and (20), the average mass transfer rate is uid phase. It’s obtained by liquid hold-up and the diameter of dro-
obtained plet. The liquid hold-up is evaluated using correlation proposed by
Burns et al. (2000)

Z 
t
NSO2 ¼ RSO2 wðt Þdt " #0:5    
ð2pN=60Þ2 r m 0:22
0:6
u
0
pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi 2 sffiffiffiffiffiffiffiffiffiffi eL ¼ 0:039 ð31Þ
kov DSO2 4
qffiffiffiffiffiffiffiffiffiffi




g0 u0 m0
t ð22Þ
¼ t erf k ov t þ exp kov t

t pkov The diameter of droplets in packing zone is regressed as follows
qffiffiffiffiffiffiffiffiffiffi (Yi et al., 2009)
1 
þ erf kov t  cSO2 ;0 " #0:630
2kov
r
d ¼ 12:84 u0:201 ð32Þ
And the liquid-side mass transfer coefficient (kL) can be ð2pN=60Þ2 rq
deduced
 And mass transfer interfacial area is calculated by the equation
NSO2 ¼ kL  cLSO2 ;0 ð23Þ
eL
a¼6 ð33Þ
pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi 2 sffiffiffiffiffiffiffiffiffiffi d
qffiffiffiffiffiffiffiffiffiffi 


kov DSO2 4  t 
kL ¼ t erf k ov t þ exp kov t

t pkov
ð24Þ 2.3.2. Gas-side mass transfer coefficient
qffiffiffiffiffiffiffiffiffiffi
1  In Chen’s study (Chen and Liu, 2002), it’s pointed that gas phase
þ erf k ov t in RPB flows in a similar way with that in packed bed. The gas-side
2kov
mass transfer coefficient (kG) in RPB is not significantly influenced
According to Burns’ visual study (Burns and Ramshaw, 1996), by the rotating speed. Similarly, the value of gas-side mass transfer
liquid travels over the surface of the packing when it flows as a thin coefficient (kG) in RPB is estimated by the equation proposed by
film. Hence, the mass transfer interfacial area in RPB is not only Onda’s work (Onda et al., 1968)
related to the operating conditions, but also to the special area of
the packing. In this model, mass transfer interfacial area of liquid kG Rg T 1=3  2:0
¼ 2Re0:7
G Sc G at dp ð34Þ
film is calculated by Rajan’s (Rajan et al., 2011) empirical equation at DG
a In the experiment, absorbent solution used is diluted and H2O2
¼ 54999ReL2:2186 Fr 0:1748
L WeL1:3160 ð25Þ
at mass fraction is below 0.63%. The effect of H2O2 molecule on the
However, when the rotating speed of RPB is high, liquid phase physical parameters of liquid phase including density, viscosity
flows only in droplet form based on our assumption. The mass and surface tension is ignored. Hence, the physical parameters of
transfer of SO2 in a single spheral droplet can be expressed as: water are used in this model. The rest of physical properties,
  kinetic and equilibrium parameters are listed in Table 1.
@cSO2 DSO2 @ @cSO2 The process to calculate the desulfurization efficiency in RPB is
¼ 2 R2  kov cSO2 ð26Þ
@t R @R @R illustrated in Fig. 2.
Because the reaction between SO2 and H2O2 is fast and irre-
versible, it requires a very short time to reach a stable state. Thus, Table 1
@cSO2 =@t can be ignored. The equation (26) is converted into Physical properties, kinetic and equilibrium parameters.

8
dc  Parameter Expression
>
<
DSO
R2 dR 2  kov cSO2 ¼ 0
2 SO
d
3
R 2 dR DG 1:75
DG ¼ 110 T 1=3ð1=MA þ1=M BÞ
1=2

 dcSO 
 ð27Þ p½ðRA ti Þ þðRB ti Þ1=3 
2 (Fuller et al., 1966)
>
: B:C: cSO2 2d ¼ cSO2 ;0 R¼0 ¼0
dR  lG
2
lG ¼ RRyyi lMi M1=2i
1=2

i i

qG qG ¼ MRgGTP
The solution to equation (27) is

k k293:15K ¼ 46541exp 0:1187c2H2 SO4  1:4229cH2 SO4 (Thomas
et al., 2003a)

5
Y.-N. Dong, W.-C. Chen, L.-L. Zhang et al. Chemical Engineering Science 235 (2021) 116467

Fig. 2. Flow chart of desulfurization efficiency calculation.

3. Experimental section The simulated industrial flue gas is prepared by mixing N2 and
SO2. N2 gas (purity 99.9%) is purchased from Beijing Ruyuan-
3.1. Materials ruquan Technology Co., Ltd., China. And SO2 (purity 99.9%) is
obtained from Beijing Beiwenqiti Technology Co., Ltd., China.
The hydrogen peroxide (H2O2) with 50.3% mass fraction, sup-
plied by Solvay (Zhenjiang) Chemicals Co., Ltd., China., is diluted
3.2. Experimental procedure
by adding deionized water to prepare the absorbent solution. The
deionized water is obtained from our laboratory water purification
The schematic diagram of the experimental set up for SO2
system (Shanghai Hitech Instruments Co., Ltd., China) with the
absorption is shown in Fig. 3. The SO2 from gas cylinder is mixed
specific resistivity of >15 MX/cm.
with N2 to simulate the industrial flue gas. And the SO2 concentra-
6
Y.-N. Dong, W.-C. Chen, L.-L. Zhang et al.
Fig. 3. Schematic diagram of the experimental set up.
tion in the mixture gas is adjusted to 1000–2000 mg/m3. The lean
absorbent H2O2 aqueous solution is prepared with 50.3% H2O2
solution and deionized water. The liquid flow rate is controlled
by a peristaltic pump. The gas mixture is sampled in both inlet
and outlet of RPB and SO2 concentration is measured by the flue
gas analyzer (Testo 350, Testo Company, Germany, SO2 volume
fraction ranging from 0 to 5000 ppm).
To prevent H2O2 decomposing, all metal equipment including
RPB, liquid pipelines and liquid storage tank have been degreased,
pickled and passivated. In the absorption process, the H2O2 absor-
bent is pumped from the lean absorbent tank into RPB through a 4-
holes liquid distributor. The liquid phase flows from inner edge of
packing to outer edge via a centrifugal force. Meanwhile, the gas
phase moves inward from the outer edge of the RPB. Gas phase
and liquid phase contact counter-currently in the RPB. SO2 dis-
solves in the liquid phase and reacts with H2O2. The gas phase
leaves from gas outlet of RPB and the liquid phase is collected in
the rich solvent tank through liquid outlet.
The RPB used in the experiment with a horizontal shaft is com-
prised of a rotating motor, a stainless steel shell, gas inlet, gas out-
let, liquid inlet, liquid outlet and a mesh packing. The stainless
steel shell is designed with a jacket structure which can be con-
nected to a circulating water to control the temperature. The spec-
ification of packing in RPB is listed in Table 2. In the experiment,
H2O2 concentration of absorbent is high enough to ensure H2O2
mole flow rate is excessive compared to that of SO2.
In this work, the H2O2 mass fraction of absorbent is in the range
of 0.13–0.63%. The total gas flux is 0.024–0.073 m3m2s1 and
inlet SO2 concentration is set to 1000–2000 mg/m3. The gas–liquid
Table 2
Specification of packing in RPB.
Item Value
Inner radius of packing rin 0.025 m
Outer radius of packing rout 0.10 m
Axial height of packing h 0.025 m
Special surface area of packing at 500 m2/m3
Voidage of packing e 0.95
Distance between the two packing layers Dl 0.003 m
7
Chemical Engineering Science 235 (2021) 116467
volumetric flow rate ratio varies from 200 to 600. RPB rotating
speed increases from 200 rpm to 1400 rpm in the experiments to
determine the optimized operating condition. All the experiments
are carried out under normal pressure and 293.15 K if there is no
special explanation. And all experimental data, such as SO2 concen-
tration and temperature, are obtained after reaching a steady state.
To reduce the errors, experimental data are collected by averag-
ing the testing values of repeated measurements. And standard
deviation (SD) is used for descriptive error bars to show how the
data are spread. SD is calculated by the following formula:
sffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
Rð X  M Þ 2
SD ¼ ð35Þ
n1
where X is the individual data, M represents the mean value and R
refers to the sum for all the n data points.
4. Results and discussion
4.1. Effect of different operating conditions on desulfurization
efficiency
The desulfurization performance is evaluated by the desulfur-
ization efficiency g, which can be computed from the definition,
as equation (36) shows

yout ð1  yin Þ
g¼ 1  100% ð36Þ
yin ð1  yout Þ
where the yin represents the SO2 concentration of inlet gas, yout is
the SO2 concentration of outlet gas. The effects of various operating
conditions including RPB rotating speed, H2O2 mass fraction, gas–
liquid volumetric flow rate ratio, gas flux and inlet SO2 concentra-
tion on the desulfurization efficiency g are investigated.
4.1.1. RPB rotating speed
Fig. 4 shows the experimental and predicted g under different
rotating speed (N). The Savitzky-Golay smoothing method is used
to smooth the curve. The gas flux G is 0.073 m3m2s1 and gas–
liquid volumetric flow rate ratio G/L is set at 300. The SO2 concen-
Y.-N. Dong, W.-C. Chen, L.-L. Zhang et al. Chemical Engineering Science 235 (2021) 116467

0.073 m3m2s1. The gas–liquid volumetric flow rate ratio G/L is

100 selected to 300. The SO2 concentration of inlet gas is 2000 mg/
m3. The H2O2 mass fraction varies from 0.13 to 0.38%. As shown
in Fig. 5, the increase of H2O2 mass fraction promotes the SO2
95 absorption process. This phenomenon is in accordance with the
results in many gas–liquid absorption processes (Wu et al., 2017;
Zheng et al., 2015). Additionally, the experimental results show
90
(%)

that the removal efficiency can easily exceed 98.25% by controlling

85 (H2O2)=0.19%, Experimental
(H2O2)=0.19%, Predicted
80 (H2O2)=0.38%, Experimental
(H2O2)=0.38%, Predicted
75
200 400 600 800 1000 1200 1400
N (rpm)
Fig. 4. Effect of RPB rotating speed on desulfurization efficiency.
tration of inlet gas is 2000 mg/m3. According to Fig. 4, predicted
desulfurization efficiency g is in good agreement with the experi-
mental data. It’s found that the desulfurization efficiency g fast
increases when rotating speed increases from 200 rpm to
1000 rpm. But the desulfurization efficiency is tending towards sta-
bility when the rotating speed beyond 1000 rpm. This is because the
intensification effect of RPB depends highly on the liquid flow pat-
tern (Wu et al., 2017). It has been observed in visual experiments
(Sang et al., 2017a; Sang et al., 2017b) that film flow, droplet flow
etc. exist in RPB. The increase of rotating speed enhances the shear-
ing and breaking effect of packing, leading to smaller liquid ele-
ments, including thinner liquid film and tinier liquid droplet. It
gives rise to the increase of gas–liquid contact area which is benefit
for SO2 removal. On the other hand, the increase of rotating speed
reduces the residence time of liquid in packing and weakens the
SO2 absorption. This effect weakens the contribution of RPB in mass
transfer enhancement, and results in no obvious increase in SO2
removal efficiency when rotating speed is beyond 1000 rpm. It can
be found that when the absorbent contains 0.38% H2O2 and the
rotating speed of RPB is higher than 1000 rpm, the SO2 removal effi-
ciency can reach above 98.25%, which means the SO2 concentration
of outlet gas is within 35 mg/m3, realizing SO2 ultra-low emission.
4.1.2. H2O2 mass fraction
Fig. 5 illustrates the effect of H2O2 mass fraction on desulfuriza-
tion efficiency at different rotating speed (N). The gas flux is
the rotating speed of RPB even when very low concentration of
absorbent (H2O2 concentration absorbent of 0.25–0.38%) is used.
Considering that high concentration of H2O2 is explosive, this
method can control the concentration of H2O2 in a very lower
range, which can not only improve the safety of the process, but
also reduce the volatilization loss of H2O2.
4.1.3. Gas-liquid volumetric flow rate ratio
Fig. 6 exhibits the effect of gas–liquid volumetric flow rate ratio
G/L on desulfurization efficiency. In order to ensure the molar ratio
of H2O2 to SO2 does not decrease with the increasing of the gas–liq-
uid volumetric flow rate ratio G/L, the concentration of H2O2 is
changed to 0.63% in this part of experiment. The gas flux is set to
0.073 m3m2s1 and gas–liquid flow rate ratio is adjusted by con-
trolling the absorbent flow rate. The SO2 concentration of inlet gas
is 2000 mg/m3. It’s shown that desulfurization efficiency g
decreases with the increasing of the gas liquid volumetric flow rate
ratio G/L within the experimental range. This phenomenon can be
attributed to two reasons. Firstly, increasing G/L means a relatively
less liquid flow rate, leading to a decrease of liquid hold up, which
decreases gas–liquid contact area. Secondly, the less liquid flow
rate decreases liquid turbulent degree and weakens the update
speed of liquid surface, decreasing the liquid-side mass transfer
coefficient. So the larger G/L is more difficult to keep high desulfu-
rization efficiency. As shown in Fig. 6, for gas–liquid volumetric
flow rate ratio of 600, by increasing H2O2 absorbent concentration
to 0.63% can ensure the removal efficiency higher than 98.25%
under optimized rotating speed. For industrial processes, increas-
ing the gas–liquid ratio means reducing the liquid circulation,
which is beneficial to reduce process energy consumption. Hence,
desulfurization by H2O2 in RPB is of great significance for industrial
process in view of the excellent desulfurization efficiency under
high volumetric flow rate ratio in RPB.
4.1.4. Gas flux
Fig. 7 presents the effect of gas flux on desulfurization effi-
ciency. The H2O2 mass fraction in the experiment is 0.13%. The

100 100
95
98
90
96
(%)
(%)

85
N= 400 rpm, Experimental 94 N= 400 rpm, Experimental
80 N= 400 rpm, Predicted N= 400 rpm, Predicted
N=1000 rpm, Experimental N=1000 rpm, Experimental
75 N=1000 rpm, Predicted 92 N=1000 rpm, Predicted

70 90
0.10 0.15 0.20 0.25 0.30 0.35 0.40 200 300 400 500 600
(H2O2) (%) G/L
Fig. 5. Effect of H2O2 mass fraction on desulfurization efficiency. Fig. 6. Effect of gas–liquid volumetric flow rate ratio on desulfurization efficiency.

8
Y.-N. Dong, W.-C. Chen, L.-L. Zhang et al. Chemical Engineering Science 235 (2021) 116467

SO2 concentration of inlet gas is 2000 mg/m3. The gas flux varies
from 0.024 to 0.073 m3m2s1. And the gas–liquid volumetric 100
flow rate ratio is fixed to 200. As shown in Fig. 7, the desulfuriza-
tion efficiency decreases with the rise of the gas flux. Increasing
95
gas flux means the decreasing of gas–liquid contact time in RPB,
which is detrimental to the absorption process. But for RPB, it is
shown that increasing rotating speed can reduce the influence of 90

(%)
gas flux change on desulfurization effect. For example, when RPB
rotates at 1000 rpm, with the gas flux increasing from 0.024 m3-
N= 400 rpm, Experimental
m2s1 to 0.073 m3m2s1 the SO2 removal efficiency decreases 85
N= 400 rpm, Predicted
from 99.6% to 98.8%, which is almost negligible. But when RPB N=1000 rpm, Experimental
rotates at 400 rpm, the SO2 removal efficiency decreases from N=1000 rpm, Predicted
97.7% to 87.9% with the gas flux rise. This indicates that the gas– 80
liquid mass transfer process has been fully strengthened at high
rotating speed. In a very short residence time, the mass transfer 75
process of SO2 from gas phase to liquid phase and consequent reac- 1000 1200 1400 1600 1800 2000
tion has been completed. Therefore, the change of residence time
of gas and liquid in RPB has negligible effect on desulfurization effi- Inlet SO2 concentration (mg/m3)
ciency. However, at low rotating speed, the two-phase mass trans-
Fig. 8. Effect of inlet SO2 concentration on desulfurization efficiency.
fer process is not strengthened sufficiently and the mass transfer
rate of SO2 from gas phase to liquid phase is not high enough to
cover up the effect of the decrease of gas residence time. For indus-
tively precise predictions with a deviation within 5% compared
trial processes, RPB exhibits good operational flexibility to flue gas
to the experimental values, which indicates the reliability of the
flow rate fluctuations.
model to predict desulfurization efficiency.

4.1.5. Inlet SO2 concentration

4.3. Comparison with conventional reactors
Fig. 8 shows the effect of SO2 concentration of inlet gas on
desulfurization efficiency at different rotating speed. The gas flux
The height of mass transfer unit HTU is an important parameter
is 0.073 m3m2s1 and 0.25% H2O2 solution is used. The gas–liq-
to evaluate the size of reactor. The values of HTU are calculated
uid volumetric flow rate ratio is set to 300. As illustrated in
based on experimental data.
Fig. 8, the desulfurization efficiency has no significant change with
The number of mass transfer unit NTU can be derived as
increase of inlet SO2 concentration. At a higher SO2 volume frac-
tion, more SO2 molecules transfer into liquid phase within unit  
yin ð1  yout Þ yin yout
time. This is ascribed to that the reaction rate increases with SO2 NTU ¼ ln þ  ð37Þ
yout ð1  yin Þ 1  yin 1  yout
concentration. When inlet SO2 concentration varies from 1000 to
2000 mg/m3, desulfurization efficiency is above 98.5% at In the experiment, the gas phase and liquid phase countercur-
1000 rpm rotating speed. RPB displays great operation flexibility rent contact along the radial direction of the packing. So the HTU
to variation of flue gas SO2 concentration. can be expressed as
r out  rin
4.2. Model validation HTU ¼ ð38Þ
NTU
Table 3 illustrates the comparison of SO2 absorption perfor-
According to Figs. 4–8, it’s concluded that proposed model can
mance in different reactors including packed column, cables-
well predict the effects of operating conditions on desulfurization
bundle scrubber and RPB. It’s reported that desulfurization effi-
efficiency. Fig. 9 presents the comparison of predicted and experi-
ciency is 85–94.99% for packed column (Maheswari et al., 2014)
mental desulfurization efficiency of SO2 absorption using H2O2
solution in RPB. It can be found that proposed model offers rela-
100
Predicted desulfurization efficiency (%)

100
95
95
90
+5%
90
85
85
(%)

80 -5%
80 75
N= 400 rpm, Experimental
N= 400 rpm, Predicted
75 70
N=1000 rpm, Experimental
N=1000 rpm, Predicted
70 65

65 60
0.02 0.03 0.04 0.05 0.06 0.07 0.08 60 65 70 75 80 85 90 95 100
G (m3 m-2 s-1) Experimental desulfurization efficiency (%)
Fig. 7. Effect of gas flux on desulfurization efficiency. Fig. 9. Comparison of predicted and experimental desulfurization efficiency.

9
Y.-N. Dong, W.-C. Chen, L.-L. Zhang et al.
Table 3
Comparison of SO2 absorption performance of conventional reactors and RPB.
Packed column (Maheswari et al., 2014)
Temperature (K) 293.15
Pressure (kPa) 103
Gas-liquid flow rate ratio (m3/m3) 267
H2O2 concentration (mol/L) 0.05–0.1
Desulfurization efficiency (%) 85–94.99
KGa (molm3Pa1h1) 1.72–2.71
HTU (cm) 33.4–52.7
and 70–80% for cable-bundle scrubber (Thomas et al., 2003a). In
RPB, desulfurization efficiency is increased to 97.3–99.1% even
low concentration absorbent and high gas–liquid flow rate ratio
are used. The value of mass transfer coefficient is also greatly
improved in RPB. It’s demonstrated that RPB improves the desulfu-
rization efficiency and enhances the gas–liquid mass transfer per-
formance. Because the reaction between SO2 and H2O2 is
instantaneous, the desulfurization process is limited by mass
transfer step. In RPB, liquid is sprayed and violently collides with
rotating porous packing. Under the shearing and cutting effect of
packing, liquid is split into thin liquid films or tiny liquid droplets,
leading to large gas–liquid contact interface. Besides, liquid is cap-
tured by the rotating packing and obtains higher flow rate, which
enhances the turbulent of liquid and increases the renewal fre-
quency of liquid surface. These factors make RPB effectively inten-
sify the gas–liquid mass transfer process. The values of HTU of
different reactors are calculated and listed in Table 3. HTU is
1.60–2.07 cm for RPB, 33.4–52.7 cm for packed column and
33.6–44.9 cm for cables-bundle scrubber. It shows the value of
HTU in RPB is one order of magnitude lower than that in packed
column and cables-bundle scrubber. This result indicates the size
of RPB is expected to be reduced to less than 1/10 compared to
conventional reactors. Hence, by using RPB, it can not only obtain
higher desulfurization efficiency, but also greatly reduce the
investment of the desulfurization equipment.
Although RPB needs extra energy consumption for its rotating,
it is still possible to decrease the energy cost of the whole desulfu-
rization system (the electricity cost for the blower, the absorbent
pump and the RPB). Firstly, based on Table 3, it can be found that
when we use RPB for a desulfurization process, the absorbent flow
rate can be decreased. And the lift height of the absorbent will also
be reduced owing to the less height of RPB reactor compared to the
high packed column. Both of these two factors will decrease the
energy cost for the absorbent pump in RPB desulfurization process.
This will cover part of the energy consumption for RPB. Secondly,
the pressure drop for RPB is much less than the packed column
(Zhang et al., 2019). Hence the energy cost for the blower can be
greatly decreased. In the desulfurization process, the energy cost
for the blower occupies the major part of the whole energy cost.
The energy saving for the blower is expected to be higher than
the energy consumption for RPB in most industrial applications.
Hence, for the whole system, energy consumption can be
decreased when RPB is used.
5. Conclusions
In the present work, a desulfurization method of industrial flue
gas treatment with H2O2 using RPB is proposed. The modeling and
experimental investigations on SO2 absorption process in RPB are
presented. Experiments are carried out under different operating
conditions, including RPB rotating speed, H2O2 mass fraction,
gas–liquid volumetric flow rate ratio, the gas flux, and inlet SO2
concentration. Within the range of experiment, RPB rotating speed
and H2O2 mass fraction are benefit for desulfurization process. But
10
Chemical Engineering Science 235 (2021) 116467
Cables-bundle scrubber (Thomas et al., 2003a) RPB
293.15 293.15
103 103
78.4 300
0.05–0.1 0.04–0.09
70–80 97.3–99.1
1.35–1.81 6.07–7.83
33.6–44.9 1.60–2.07
gas–liquid volumetric flow rate ratio and the gas flux have a nega-
tive impact on desulfurization process. RPB displays great opera-
tion flexibility to variation of flue gas SO2 concentration. Under
the optimized conditions, it’s found out that the desulfurization
efficiency is above 99% and the outlet SO2 concentration is below
35 mg/m3, achieving SO2 ultra-low emission. The desulfurization
efficiency predicted by this model is in good agreement with the
experimental data, with a deviation within 5%. A comparison of
SO2 absorption performance in different reactors is presented.
Compared with conventional reactors, RPB improves the desulfur-
ization efficiency and the size of reactor can be reduced to less than
1/10 of traditional reactors.
CRediT authorship contribution statement
Yu-Ning Dong: Investigation, Formal analysis, Writing - origi-
nal draft. Wen-Cong Chen: Data curation, Formal analysis.
Liang-Liang Zhang: Conceptualization, Writing - review & editing,
Supervision, Funding acquisition. Bao-Chang Sun: Conceptualiza-
tion, Resources, Methodology. Hai-Kui Zou: Conceptualization,
Resources, Methodology. Yong Luo: Resources, Methodology.
Guang-Wen Chu: Resources, Methodology. Jian-Feng Chen: Con-
ceptualization, Resources, Methodology.
Declaration of Competing Interest
The authors declare that they have no known competing finan-
cial interests or personal relationships that could have appeared
to influence the work reported in this paper.
Acknowledgments
This work was financially supported by the National R & D Pro-
gram of China (No. 2017YFC0210900) and the National Natural
Science Foundation of China (Nos. 21978011).
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