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Sustainable Energy Technologies and Assessments 47 (2021) 101451

Contents lists available at ScienceDirect

Sustainable Energy Technologies and Assessments


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

Review article

A review of removing SO2 and NOX by wet scrubbing


Mengjing Zhao a, Peng Xue a, *, Junjie Liu b, Junhua Liao a, Jiamin Guo b
a
Beijing Key Laboratory of Green Built Environment and Energy Efficient Technology, Beijing University of Technology, Beijing, China
b
Tianjin Key Laboratory of Indoor Air Environmental Quality Control, School of Environmental Science and Engineering, Tianjin University, Tianjin, China

A R T I C L E I N F O A B S T R A C T

Keywords: Air pollution has intensified in recent years. The rates of sulfur dioxide (SO2) and nitrogen oxides (NOx)
Wet scrubbing contributing to air pollution have risen annually, imposing huge burdens on human health and industrial pro­
Gaseous pollutants duction. Among gas separation techniques, wet scrubbing exhibits superior economical and application value to
Removal efficiency
simultaneously remove SO2 and NOX. This paper summarizes the mechanism, study approaches, and application
Energy saving
status of wet scrubbing to remove SO2 and NOX. Given the results of previous experiments, the factors are split
Compound technology
into three categories: operating parameters, equipment parameters, and additional conditions. With the mech­
anism and degrees of each factor considered, a wet scrubbing optimization scheme for enhancing the absorption
efficiency is presented. In order to improve the removal efficiency while maintaining sustainability, this study
also introduces the method of waste heat recovery and water recycling in the wet scrubbing system. In view of
the current conditions, the development trend of wet scrubbing should be optimized as well as combined with
other new technologies.

Introduction separation [21], and biomass [22], and some technologies among them
are already mature in terms of industrial applications for the removal of
As the industrial structure has been adjusted, the release of partic­ SO2 and NOX. Considering the different requirements of gas control in
ulate matter has been controlled in many places [1–3], while SO2 and various industrial environments, technical implementation conditions,
NOX have become the predominant influential factors in the atmo­ and economic constraints, these treatment methods are more suitable
sphere. SO2, NO, and NO2 are the primary components in the flue gas of for applications in several specific scenarios. Selective catalytic reduc­
coal burning [4–6], and NO2 is gradually comprising a larger proportion tion (SCR) plays an essential role in flue gas denitrification technology
in the natural air, as indicated by meteorological data analysis [7]. SO2 owing to its high efficiency and seasoned technology [23,24]. Mem­
and NOX concentrations in specific ranges will significantly impact in­ brane separation technology is applied to fertilizer plant extracts and
dustrial production and human health, such as the body’s respiratory recover some of the gases in the tail gas, thereby increasing production
system, especially in children and the elderly [8–11]. SO2 and NOX and saving energy [21]. Because activated carbon absorbs gas well at
combined with water molecules in the air could generate corrosive low concentrations, this method is often adopted in hospitals and
acidic substances that damage equipment and products in industrial semiconductor factories to remove gaseous pollutants from fresh air
plants [4,12]. With the development of the electronics industry and the [25]. Wet scrubbing technology is commonly used in industrial thermal
tightening of production environmental requirements, the control of power plants to treat sulfides in exhaust gas because of its high
gaseous pollutants in natural air has become a decisive factor in throughput and simple structure [26]. To compare the four methods
restricting the quality of products [13,14]. In order to control SO2 and mentioned above, this article lists the advantages and limitations of
NOX, some country has issued emission standards for gas pollutants from these methods in Table 1.
thermal power plants to limit the concentration of these gases [15], and Table 1 shows that the Selective catalytic reduction is a mature
it is necessary to study technologies for the simultaneous removal of SO2 process for denitrification, but it doesn’t have the ability to remove SO2.
and NOX due to the severe demand for clean gas. Selective catalytic reduction requires complex operating conditions,
Common gas separation methods include combustion [16], absorp­ such as the applicable temperature of NH3-SCR should ranges 200–400
tion [17], adsorption [18], catalytic conversion [19,20], membrane ℃ with the aid of a catalyst bed [35]. In addition to high temperatures,

* Corresponding author at: Room 308, Green Building, No.100 Pingleyuan, Chaoyang District, 100124 Beijing, China.
E-mail addresses: xp@bjut.edu.cn (P. Xue), jjliu@tju.edu.cn (J. Liu), liaojunhua1111@emails.bjut.edu.cn (J. Liao), guojm@tju.edu.cn (J. Guo).

https://doi.org/10.1016/j.seta.2021.101451
Received 30 January 2021; Received in revised form 18 April 2021; Accepted 3 July 2021
Available online 10 July 2021
2213-1388/© 2021 Elsevier Ltd. All rights reserved.
M. Zhao et al. Sustainable Energy Technologies and Assessments 47 (2021) 101451

there have the problems of leaking catalysts and reducing agents in this transfer are replaced by a single simplified factor (e.g., film thickness,
process [23]. The membrane technology is employed for the removal of residence time, surface renewal rate). Some novel models are proposed
a specific gas with a largish pressure drop in the process of separation, on that basis with more variables, such as the modified surface update
and new membrane materials is necessary to adapt more stringent model [41] and vortex model [42]. The modified surface renewal model
conditions, such as temperature, pressure and corrosive media [29]. introduces the distribution function of different surface residence time,
Owing to SO2 and NOX exist in the atmosphere and industrial exhaust and the vortex model bring the surface tension in vortex momentum
gases at the same time, the technology of removing SO2 and NOX variation.
simultaneously is more in line with economic needs. Activated carbon Gas–liquid mass transfer models have two main functions, and the
has a great removal efficiency of SO2 and NOX, whereas the preparation first is to lay a theoretical basis for assessing the rate of absorption. Kuo
of adsorption materials is costly and the adsorption rate drops rapidly. et al. [44] built a theoretical model of gas scrubbing efficiency assess­
Although the removal efficiency of wet scrubbing technology is medium, ment and explained the relationship between the inlet concentration
the operating equipment is relative simple and inexpensive. Fig. 1 de­ and removal efficiency based on this model. Brogren and Karlsson [45]
picts the schematic diagram of wet flue gas desulfurization (WFGD), calculated the dynamic absorption rate of SO2 in limestone droplets in
which is a common form of equipment in wet scrubbing. Removal SO2 accordance with a model of permeation theory. Chang and Rochelle
and NOX can be achieved by changing the sprayed liquid in that device [46] calculated the liquid-phase mass transfer rate applicable to SO2
(e.g., Fe(II)-EDTA solution [36] and urea solution [37]), and it is not absorption in exhaust gases based on surface renewal theory. Darake
required to attain high temperature and concern catalysts. In view of the et al. [47] enhanced the ability of the spray tower model to assess the
above analysis, wet scrubbing technology has superiority in the situa­ desulfurization efficiency using the droplet fluid dynamics model. The
tions that removing SO2 and NOX with no strict requirement or pre- second function is to interpret the effect of the parameters during mass
removing SO2 and NOX as a part of filtration system with low cost. transfer. Zheng et al. [48] adopted the formula to calculate the effect of
This article summarizes the mechanism and research methods of wet the mass transfer coefficient and effective gas–liquid contact area on the
scrubbing technology and the current application of wet scrubbing purification. Bandyopadhyay and Biswas [49] built a simple and prac­
technology. According to the existing problems in development, this tical model to ascertain the effects of valid parameters (e.g., droplet size,
research analyzes the previous research and makes suggestions for ef­ velocity, surface gas velocity, and liquid flow rate) on mass transfer. Zhu
ficiency improvements and energy sustainability. In addition, prospects et al. [50] studied the absorption of SO2 by limestone-gypsum and
for the future development of wet scrubbing technology combined with determined that the absorption height decreased with the increase in the
new technologies are proposed. liquid/gas ratio and pH value of the absorption liquid. It can be seen that
the gas–liquid mass transfer theoretical model is the basis of subsequent
Wet scrubbing technology research about low-consumption and high-efficiency mass transfer
process, and in order to further explore the mechanism of the wet
Principle of wet scrubbing scrubbing process, experiments and simulations are both efficient ap­
proaches of to clarify the state of the actual absorption.
Many researchers have proposed theories to describe the mass
transfer between gas and liquid phases. The two-film theory proposed by Research approaches
Whitman [38] assumes that layers exists at the interface of the two
fluids, and the mass transfer between the gas and the liquid acts as Experimental methods
steady-state molecular diffusion. The mass transfer diagram of the two- The most common approaches to studying wet scrubbing are ex­
film theory hypothesis is shown in Fig. 2. However, most industrial mass periments and simulations. Over the past few years, numerous re­
transfer is considered an unsteady process. As inspired by Whitman’s searchers have explored the factors affecting the absorption rate of wet
study, Higbie [39] proposed the theory of infiltration given the time scrubbing using experimental methods and provided considerable
required to form a concentration gradient, which is valid only when the experimental data under different working conditions. Fang et al. [51]
contact time between the two phases is too short to reach a steady state. exploited a urea solution to absorb SO2 and NOX, and the effects of the
Based on these studies, Danckwerts [40] abandoned the concept of urea concentration, temperature, and initial pH on the removal effi­
“stagnant film” and proposed a surface renewal theory, stating that the ciency were ascertained. With the improvement of precision in­
surface will be constantly replaced by fresh liquid. The common feature struments, the expanded the measurement range of experimental
of the above three classic models is that multiple factors that affect mass parameters and improvement in the accuracy lead to more valid and

Table 1
Comparison of several conventional methods for removing SO2 and NOX.
Method Medium Efficiency Advantages Constraint Limitations
rating

Selective catalytic Ammonia, liquid ammonia, urea, and the like are used High High NOX removal efficiency Incapable of removing SO2
reduction [23,27] as a reducing agent, and metal oxide is supported as the Reliable operation Complicated system and operating
catalyst conditions (high temperature)
Ammonia slip
Membrane separation Inorganic and organic polymers with a microporous High High efficiency Difficult to prepare membrane
[28,29] structure No secondary pollution materials
Removal of a specific contaminant
High pressure drop
Activated carbon Activated carbon and surface impregnated chemical High Remove multiple gases simultaneously Surface catalyst is natural to
adsorption components High removal efficiency for low inactivate and difficult to
[24,30–32] concentration pollutants regenerate
The waste catalyst is hard to
handle
High cost
Wet scrubbing Absorbent liquid Medium Remove multiple gases simultaneously Inefficient
[17,33,34] (water, alkaline solution, etc.) Suitable for high air volume systems Cause secondary pollution
Low cost

2
M. Zhao et al. Sustainable Energy Technologies and Assessments 47 (2021) 101451

Fig. 1. Schematic diagram of wet flue gas desulfurization (WFGD) device [26].

novel conclusions, and some experimental studies are summarized in


Table 2.
Table 2 shows some experimental methods with new instruments
under different operating conditions. In terms of measurement range,
PIV, laser doppler and phase doppler measurements can obtain
gas–liquid two phases’ velocities in wet scrubber, and ultraviolet
analyzer and chemiluminescence analyzer could measure the concen­
tration of SO2 and NOx instantly with the accuracy of ppm. Laser and
phase doppler measurements can measure the size of droplets in the
spray state with high accuracy (accurate to millimeters), and the new
equipment can produce the velocity field without any contact. The
experimental results could be more reliable with a higher cost, and it is
necessary to explore the simulation method to study the wet scrubbing
process.

Simulation methods
Because simulation technology has the advantages of low cost and
short calculation period, using a simulation method to study the ab­
sorption of gaseous pollutants can remedy the defects of experimental
techniques. With the large application of fillers in wet scrubbers, a
growing number of researchers are beginning to study the gas–liquid
Fig. 2. Standard two-film theory (STFT) schematic representation [43]. mass transfer on the surface of the filler and build physical models for
simulation calculations. For instance, Rahimpour et al. [55] built a
mathematical model to simulate the absorption of acid gases with
corrugated plate fillers. This approach allows the adoption of the
Navier–Stokes equations and convection–diffusion and heat–conduction
equations to express the transport phenomena under the gas–liquid
Table 2
condition in an entire separation column. Sebastian-Saez et al. [56]
Experimental methods of wet scrubbing.
established a three-dimensional numerical model based on the volume-
Equipment Flow Absorbent Purpose Ref. of-fluid (VOF), and reported that the surface texture of the filler sheet
rate type
could affect the wetted area and the mass transfer rate of the liquid. As
Particle image 360 water Obtained the vector [52] revealed from the simulation results, the rough surface positively
velocimetry (PIV) m3/h velocity of the fluid impacted the liquid film thickness and the wetted area. It is an
in different area by
tracing particles and
economical way to get results quickly by modifying the calculation
high-speed camera model and input parameters in the software. In order to compare the
Laser doppler and 5.85 water Analyzed the [53] calculation functions, different software for removal of SO2 and NOX by
phase doppler m3/s droplets size and wet scrubbing are shown in Table 3.
measurements movement trajectory
Table 3 shows three simulation ways to analyze the process of wet
of the droplets and
gas sprayed by scrubbing remove SO2 and NOx. Aspen Plus can calculate the energy
different nozzle consumption and removal efficiency of each device in the system
models through establishing the system flow model, Fluent is able to describe
Ultraviolet analyzer 2.45 acidic Measured the [54] the process of mass transfer of entire device dynamically and visually
and × solutions concentration of SO2
chemiluminescence 10− 4 containing and NOx at the input
under different parameter conditions, while OpenFOAM can draw the
analyzer m3/s H2O2 and output ports result of the velocity and mass changes of tiny droplets in contact with

3
M. Zhao et al. Sustainable Energy Technologies and Assessments 47 (2021) 101451

Table 3
Simulation methods on SO2 and NOX removal by wet scrubbing.
Software Reactant Contaminant Variable parameters Purpose Ref.

Aspen Plus O3 and water SO2 and NO flow rate Calculated the power cost, removal efficiency, temperature and pressure changes of each [57]
gas components of flue device in the system
gas
Fluent NaSO3 NO2 liquid/gas ratio, Explored the influence of liquid/gas ratio, solution concentration and NO2 concentration on [58]
solution solution concentration removal efficiency
NO2 concentration
OpenFOAM seawater SO2 alkaline concentrate Modeled the mass exchange of droplet and SO2 [59]
SO2 concentrate

gas component by writing new solver. Compared with experiments, the respectively by using limestone–gypsum. The chemical reaction be­
simulation method could break the limitations of measuring in­ tween the solution and the pollutant gas can greatly improve the
struments, and dramatically reduce the time consuming and resource removal efficiency, but exothermic heat is produced during the chemical
consumption. However, the calculation formulas applied in the simu­ reaction, which is mostly ignored.
lation calculation are mostly modified semi-empirical formulas under When natural air is the pollution source, the wet scrubbing process is
the imperfect theoretical foundation, and the assumptions in the method applied as the make-up air unit in a clean air-conditioning system [61].
may result in errors in the simulation results, adversely affecting the If additives are introduced to absorb SO2 and NOX in the make-up air
accuracy of the simulation. Therefore, the effectiveness of the simulation units, a certain amount of acid and alkali ions may be carried in the air,
model should be verified experimentally, and the verified results exhibit thereby causing secondary pollution to the cleanroom. Accordingly, the
high credibility and can guide subsequent operations. wet scrubber for cleanrooms can only use deionized water or pure water
to dissolve and absorb the gaseous pollutants. Existing studies have
suggested that many researchers have made some progress in exploiting
Current application status
water to remove SO2 and NOX from the atmosphere. Xi’an Institute of
Engineering and Technology proposed multiple rows of a spray scrubber
According to the source of pollutants, wet scrubbing technology is
to remove SO2 and NO2 from outdoor air. According to the results, the
adapted to remove industrial exhaust gas and natural gas (Fig. 3). When
improvement of the liquid/gas ratio makes the purification effect
flue gas acts as the pollution source, typically, a wet scrubbing absorp­
visible, with the removal rates of NO2 and SO2 of 52% and 43%,
tion device will be adopted to treat the exhaust gas in the factory [28].
respectively [62]. Therefore, the removal efficiency of wet scrubbing is
For a large concentration of SO2 and NOX in the exhaust gas, additives
generally low when removing natural air.
should be added to enhance the efficiency of absorption. Hao et al. [20]
Wet scrubbing technology can absorb multi-component gaseous
developed a composite additive (HA-Na/NaClO2) to absorb SO2 and NO
pollutants with different concentrations, and the equipment is flexible.
in coal-fired flue gas. The results indicated that the desulfurization ef­
These characteristics make wet scrubbing technology widely demanded
ficiency was 98–99.8%, and the NO conversion efficiency reached 98%.
and applied in many industrial fields, such as thermal power plants,
The method to adopt the solution for exhaust gas absorption in wet
textiles plants, ships [63], and electronics factories. However, it can be
scrubbers has been extensively used in the exhaust systems of factories.
concluded from the above that wet scrubbing technology has the
For instance, Ma et al. [60] achieved the first industrial-scale application
problems of energy waste and low removal efficiency in the application.
of this technology in a 100,000 ton/year carbon black production line
Overall, the theoretical basis for wet scrubbing is incomplete. With the
(with a gas volume of 60,000 Nm3/h), and the desulfurization and
advancement of research methods and technology, the technique has
denitrification efficiencies of the system can be up to 98% and 85–90%

Fig. 3. Schematic diagram of gaseous pollutant source during wet scrubbing process.

4
M. Zhao et al. Sustainable Energy Technologies and Assessments 47 (2021) 101451

been further understood, but there are still some problems in practical Equipment parameters
applications. Therefore, research and analysis should be conducted on
the key problems that currently exist regarding efficiency and energy. From the experimental results of changing the equipment parame­
ters, both fillers and nozzles significantly impact the results. The primary
Factors affecting the removal efficiency of wet scrubbing function of the filler is to expand the contact area of the absorption
device with the gas. The selection of fillers primarily considers three
The rate at which a wet scrubber removes gaseous contaminants criteria. The first is the surface area per unit volume of filler. The second
from an air stream is determined by the degree of saturation at the is the surface wetting properties of the filler, covering the hydrophilic
interface of the gaseous phase and the solvent within the absorber (as properties of the filler and the microstructure of the surface, among
shown in Eq. (1)). It is therefore suggested that the gas removal effi­ others [79,80]. The third refers to the effect of airflow resistance [81].
ciency is limited to a specific size of the absorber plant and a particular Overall, the larger the specific surface area of the filler, the better the
airflow rate [64]. Accordingly, even identical removal efficiencies have wetting property will be, and the smaller the opposition to the gas flow,
different implications under varied experimental conditions. According the better the performance of the fillers. From the experimental results,
to the conclusions of existing studies, numerous factors (e.g., gas–liquid changing the packing (type, thickness, etc.) can increase the NOX
contact time, gas–liquid contact area, and liquid temperature) can affect removal efficiency by 5% to 36%. Because smaller droplets can form
the final mass transfer effect. This paper divides these factors into three larger interfacial contact areas, the key factor in the nozzle parameters
categories: operating parameters, equipment parameters, and additional affecting the removal efficiency is the spray particle size [82]. The ideal
parameters. Operating parameters refer to conditional settings other nozzle is characterized by uniform spray, small droplet size, and high
than the system structure that can usually be regulated during operation, spray rate [83]. The optimization of the nozzle increased the efficiency
such as the speed of the inlet gas and the liquid/gas ratio. Equipment of SO2 removal by 10% to 45%, and the efficiency change of NOX
parameters are defined as the structural parameters of the wet scrubber removal by 7%. The existing nozzle technology to produce small particle
determined during the design process, covering the structure of the sizes is mature, and the material selection and structural form of the
packing and the type of nozzle. Additional parameters refer to the pa­ filler are under continuous exploration. In the design of the wet
rameters of other equipment in the system that impact the wet scrubber. scrubber, the nozzles should be distributed reasonably, and the appro­
To determine methods to enhance the efficiency of SO2 and NOX priate type should be used according to the system requirements. The
removal by a wet scrubber, the experimental results of related articles use of fillers should be considered to reduce the resistance, while the
are listed in Table 4. Fig. 4 clearly expresses the impact degree of each efficiency should not be lower than required. The experimental results
parameter on the removal efficiency. indicate that the spray particle size and the structure of the filler criti­
cally affect the removal efficiency. Accordingly, selecting a more suit­
N = KL(Ci − CL) (1) able filler structure based on a small particle size nozzle is one of the
2
where N is mass transfer rate, kmol/(m .s); KL is the liquid phase mass processes to optimize the wet scrubber.
transfer coefficient, m/s; Ci–CL is the concentration difference between
gas and liquid phases, kmol/m3. Additional parameters

Operating parameters Additional parameters refer to the other equipment parameters in


the system that are likely to affect the absorption ability of the wet
From the analysis of the effect of the operating parameters on the scrubber. For instance, a cooling coil after the wet scrubber will
removal efficiency of SO2 and NOX, the following conclusions can be condense the moist air to partially remove gaseous contaminants.
drawn. The absorbent is split into a chemical solvent and water However, the experimental results suggest that these additional pa­
depending on whether an additive is added. It can be seen that the rameters have a slight effect on the removal efficiency.
removal NOX efficiency can be elevated from 21% to 25% by using This section summarizes the effects of the operating parameters,
chemical solvent in the Table 4. The rates of water absorption of SO2 and equipment parameters, and additional parameters on the removal effi­
NOX vary from 8% to 18% within different water quality. The inlet gas ciency of SO2 and NOX. By analyzing the previous experimental data, the
concentration determines the concentration difference between the gas liquid/gas ratio, inlet gas velocity, and spray are parameters that have a
and liquid phases, and this rise could up-regulate the diffusion rate of the greater impact on efficiency. During the operation of the system, in
gas on the liquid [38]. The gas velocity at the inlet will lead to variations addition to the absorption efficiency, the energy consumption of the
in the gas–liquid contact time, which significantly impacts efficiency system must also be considered. Integrated air quality management is a
[78]. In contrast, under the requirement of the outlet airflow speed, the combination of technical and economic measures [84], and considering
inlet gas velocity can only be regulated within a small range. Up- the energy saving method is a key direction worth studying.
regulating the water flow means varying the liquid/gas ratio, which is
easy to achieve during operations. According to the experimental re­ Research on sustainability
sults, altering the liquid/gas ratio can elevate the removal SO2 efficiency
by 14% to 47%, the removal NOX efficiency by 10% to 32%, demon­ Heat recovery
strating that changing the liquid/gas ratio can effectively up-regulate
the removal efficiency of the wet scrubber. The greater the amount of In addition to improving the absorption efficiency, using energy
water, the higher the ability will be within a specific range. An increase sustainability is also an important aspect of optimizing wet scrubbing.
in the amount of water results in an increase in energy consumption. There is a considerable waste of energy in a wet scrubber (e.g., waste of
Thus, the liquid/gas ratio should be reasonably elevated under eco­ heat energy caused by the excessive temperature of the treated gas and
nomic conditions. The liquid temperature affects the removal efficiency waste of water resources attributed to large water consumption [85]).
by changing the solubility of the gas in the liquid. Lower liquid tem­ Some studies have proved that using heat recovery device can effectively
peratures can increase solubility, whereas lowering the temperature reduce the energy consumption in air conditioning system [86]. Fig. 5 is
requires additional equipment, which increases operating costs. a schematic diagram of an exhaust heat recovery type air cleaner system
for a semiconductor manufacturing cleanroom. In a study on recovering
heat from waste gas, Song et al. [87] investigated a heat exchanger to
link the wet scrubber in the exhaust gas treatment system to the reheater
of the fresh air system. As indicated by the calculation results, a good

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M. Zhao et al. Sustainable Energy Technologies and Assessments 47 (2021) 101451

Table 4
Effect of parameters in wet scrubber on SO2 and NOX removal efficiency.
Influencing factors Experimental operating conditions Pre- Post- Efficiency Pre- Post- Efficiency
efficiency efficiency increase (%) efficiency efficiency increase (%)
(SO2) (%) (SO2) (%) (NOX) (%) (NOX) (%)

Operating Water quality Solute:urban water and pure water, air 95 82 8 / / /


parameters [65] volume = 1000 CMHGas velocity = 2 m/
s, Liquid/gas ratio = 0.6
Water quality Solute: water (conductivity), air volume 73–79 55–68 11–18 / / /
[66] = 120000 CMHLiquid/gas ratio = 0.5,
Inlet concentration of SO2 = 5.9 ug/m3
Solution Solute: Na2SO3 solution, Gas flow rate = / / / 75 96 21
concentration 400 ft3/minLiquid flow rate = 3000 Ib/ft2
[67] hrInlet concentration of NO = 200 ppm
Solution Solute: Na2S2O8 solutionInlet 94 94 0 60 85 25
concentration concentration of SO2 = 1000 μl/LInlet
[33] concentration of NO = 500 μl/L
Liquid/gas ratio Solute: city waterLiquid/gas ratio = 65 95 30 / / /
[68] 0.2–0.4
Liquid/gas ratio Solute: water, air volume = 10000 m3/ 59.58 73.9 14 / / /
[69] hLiquid/gas ratio = 0.08–0.12Inlet
concentration of SO2 = 9.30 ± 3.34 ppb
Liquid/gas ratio Solute: Fe(II)-EDTA solution, Gas flow / / / 74 84 10
[36] rate = 0.1 m/sLiquid/gas ratio =
27.52–58.98 L/m3Inlet concentration of
SO2 = 375 ± 25 ppmInlet concentration
of NO = 155 ± 20 ppm
Liquid/gas ratio Solute: seawater, Liquid flow rate = 1–4 43 90 47 / / /
[47] L/minInlet concentration of SO2 = 1500
ppm
Liquid/gas ratio Solute: Na2SO3 solutionGas flow rate = 100 100 0 58 90 32
[67] 400–900 ft3/minLiquid flow rate =
3000–4000 Ib/ft2 hrInlet concentration of
NO = 200 ppm
Inlet gas Solute: water, air volume = 120000 55 65 10 / / /
concentration CMHLiquid/gas ratio = 0.5
[66]
Inlet gas Solute: water, Liquid flow rate = 1.25 94.5 97.8 3 / / /
concentration dm3/sInlet concentration of SO2 = 0.8 –
[70] 15.5 g/m3
Gas velocity [71] Solute: Cu2+/Fe3+ solutionGas flow rate 100 100 0 30.6 83.8 53.2
= 300–800 mL/minInlet concentration of
SO2 = 2000 mg/m3Inlet concentration of
NO = 400 mg/m3
Gas velocity [72] Solute: waterInlet concentration ofSO2−
4
75 92 18 24 61 37
= 7000 ng/m3Inlet concentration ofNO−3
3
= 1500 ng/m
Gas velocity [67] Solute: Na2SO3 solution, Gas flow rate = / / / 59 90 31
400–900 ft3/minLiquid flow rate = 3000
Ib/ft2 hrInlet concentration of NO = 200
ppm
Gas velocity [73] Solute: HNO3 solution, Liquid flow rate = / / / 65 88 23
0.048 m/sInlet concentration of NO =
400 ppm
Liquid Solute: Mg–Al oxide slurry, Gas flow rate 99 99 0 4 14 10
temperature [74] = 1.3 mL/minInlet concentration of SO2/
NO = 150 ppm
Liquid Solute: Na2S2O8 solutionLiquid 94 99 5 / / /
temperature [33] temperature = 35, 55, 65, 75, 85, and 90
℃Inlet concentration of SO2 = 1000 μl/
LInlet concentration of NO = 500 μl/L
Liquid Solute: HNO3 solution, Liquid flow rate = / / / 81 93 12
temperature [75] 0.12 m3/hInlet concentration of NO =
800 ppm

Equipment Two-stagewet Solute: water, Gas velocity = 4.2 m/sInlet 87 93 6 26 32 6


parameters scrubbing [72] concentration ofSO2− 3
4 = 7000 ng/m Inlet
concentration ofNO−3 = 1500 ng/m3
Two-stagewet Solute: Fe(II)-EDTA solution, Gas flow 96 96 0 83 96 13
scrubbing [36] rate = 0.1 m/sLiquid/gas ratio = 58.98 L/
m3Inlet concentration of SO2 = 375 ± 25
ppmInlet concentration of NO = 155 ±
20 ppm
Filler type [73] Solute: HNO3 solution, Gas flow rate = / / / 91/95 100 5–9
0.061 m/sLiquid flow rate = 0.048 m/
sInlet concentration of NO = 400 ppm
/ / / 22 58 36
(continued on next page)

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M. Zhao et al. Sustainable Energy Technologies and Assessments 47 (2021) 101451

Table 4 (continued )
Influencing factors Experimental operating conditions Pre- Post- Efficiency Pre- Post- Efficiency
efficiency efficiency increase (%) efficiency efficiency increase (%)
(SO2) (%) (SO2) (%) (NOX) (%) (NOX) (%)

Filler thickness Solute: Fe(II)-EDTA solution, Gas


[62] velocity = 1.83 m/s
Spray particle Solute: Fe(II)-EDTA solutionGas flow rate 50 95 45 / / /
size [36] = 0.1 m/s, Liquid/gas ratio = 58.98 L/
m3Inlet concentration of SO2 = 375 ± 25
ppmInlet concentration of NO = 155 ±
20 ppm
Nozzle style [47] Solute: seawater, Liquid/gas ratio = 12 L/ 20 42 22 / / /
m3Inlet concentration of SO2 = 1500 ppm
Nozzle style [62] Solute: water, air volume = 1000 52 42 10 35 42 7
CMHGas velocity = 2 m/s, Liquid/gas
ratio = 0.6

Additional Cooling coil Solute: city water, air volume = 9000 94 95 1 / / /


parameters location [76] CMHGas velocity = 2.1 m/s, Liquid/gas
ratio = 0.6
Whether the exit Solute: DI water, air volume = 1000 95 92 3 / / /
iscooling coil CMHGas velocity = 2 m/s, Liquid/gas
[77] ratio = 0.6

Fig. 4. Impacting degree of each parameter on the removal efficiency.

energy saving effect could be achieved, and the energy saving in winter energy for multi-effect distillation (MED) technology. The calculations
is twice that in summer. In addition to the waste heat recovery of the of the investment and income have indicated that this is a promising
exhaust gas, the heat recovery unit exhibits potential applications in technical scheme. Therefore, recycling the heat of the wet scrubbing
fresh air systems. Cianfrini et al. [88] developed an integrated energy system is not only beneficial to save energy, but also to economic profit.
saving system consisting of an air scrubber, an indirect evaporative
cooling unit, and a cooling reheat unit. The humid air passing through Water recycling
the air scrubber enters the indirect evaporative cooling device to achieve
evaporative cooling, and the indirect evaporative cooling device ex­ In the wet scrubbing system, the exhaust gas contains vast water
changes the heat with the use of a cooling and reheating unit. After molecules when the pollutant gas is discharged, and the waste liquid is
adding the evaporative cooling device for heat recovery and utilization, let off directly after the solution absorbs the gas. Thus, the water in the
the energy consumption of the system is down-regulated by 40%–60%. wet scrubbing system needs to be recycled owing to the large amount of
Cohen et al. [89] recovered the waste heat from flue gas desulfurization water consumption, especially in areas with scarce water resources. In
and set up a heat recovery device to heat water to provide thermal the wet scrubbing process, the inlet high-heat flue gas is unsaturated at

7
M. Zhao et al. Sustainable Energy Technologies and Assessments 47 (2021) 101451

sprayed into the evaporator of the FEC device and begins to obtain pure
water under a vacuum condition, which can be employed as a system
water supplement. The calculations show that the volume of the
recovered purified water is greater than the amount of replenished water
2−
in the system. What’s more, the component of contains NH+ 4 , SO3 ,
2−
HCO3 all meet the Chinese national recycling water standard [93],
ensuring the quality of circulating water.
Coal-fired power plants consume numerous coal and water resource,
so heat and water saving are the major issues should be considered. The
heat recovery and water recycling process can effectively reduce the
energy consumption of the wet scrubbing system, whereas these
methods have not been widely applied because of the increasing initial
investment and floor space caused by the additional equipment.

Prospective research

In current application of wet scrubbing system, the disadvantage of


resource waste could be optimized by heat recovery and water recycling.
However, the removal efficiency could not be easily achieved with
above technologies and wet scrubbing technology alone, and consid­
Fig. 5. Schematic diagram of an exhaust air heat recovery type air washer ering the combined use of other technologies is a critical topic explored
system for semiconductor manufacturing cleanrooms [90]. at present.
Fueled by the advancement of science technology, a range of
the beginning, and the moisture contained in the slurry will evaporate advanced methods to remove SO2 and NOX have been developed
into the flue gas continuously. In the process of spraying water contact, continuously, including electrochemical [94], complex absorbent
the flue gas temperature keep decreases, and the flue gas moisture will adsorption [95], liquid-phase oxidation [21], ultrasonic [96], photo­
increases until it reaches saturation. After that, the temperature of the chemical [97,98], plasma [99], and ozonation [100]. These methods
saturated flue gas continues to decrease, and the flue gas will generate focus more on enhancing the removal efficiency and restricting by-
condense water due to supersaturating [91]. Therefore, the comparison product generation than conventional removal methods. However,
of the evaporated and condensed water is the basis for evaluate whether these methods have significant shortcomings in terms of investment cost
the system saves water. and technology maturity. All the single techniques for removing SO2 and
Xiong et al. [91] compared the water consumption of three NOX exhibit limitations and applicability. For instance, the electron
commonly used solution desulfurization methods. The water consump­ beam (EB) method displays high removal efficiency for SO2 and NOX,
tion of the limestone-gypsum method is the largest, followed by the and the by-products can be recycled. However, the energy use rate of EB
magnesium method, and the natrium-alkali method has the lowest water is low, and the X-ray shielding problem is difficult to solve [101]. To
consumption. They also established the influence of a series of operating overcome the disadvantages of using a single method, the idea of
parameters on water consumption (Fig. 6), confirming that zero-water combining multiple arrangements has begun to arouse attention [102].
consumption can be accomplished under certain conditions. Because It was found that the wet scrubbing method combined with other
the presence of impurities in the water during the process of recovering methods can achieve high efficiency and environmental protection re­
water from flue gas (e.g., SO2, NOX, heavy metals, etc.), and it may quirements and lower the operating cost of the entire system. Accord­
corrode the pipeline or affect further utilization of recovery water, some ingly, the study of wet scrubbing combined with the plasma method and
researchers have tested the water quality after recycling. Li et al. [92] photocatalytic oxidation method is described below.
established a flash evaporation and condensation (FEC) device to
recover and recycle the water in the system, and the waste liquid is

Fig. 6. Test facility of zero-water consumption [91].

8
M. Zhao et al. Sustainable Energy Technologies and Assessments 47 (2021) 101451

Plasma method

The plasma method primarily uses high-energy electrons to activate,


ionize, or even cleave SO2 and NOX molecules in the flue gas, and gen­
erates considerable active particles (e.g., ions and radicals). After SO2
and NOX are oxidized by the energetic particles, ammonium sulfate
((NH4)2SO4) and ammonium nitrate (NH4NO3) fertilizer are formed
when ammonia is injected [103,104]. According to the source of high-
energy electrons, the plasma method can fall into an electronic beam
accelerator and pulse corona-induced plasma chemical process [105].
The wet scrubber is critical for pre-oxidation and acid aerosol formation
of the gaseous pollutants in combination with plasma methods. Park Fig. 8. Schematic diagram of VUV method [108].
et al. [106] employed a wet scrubber and a plasma electrostatic pre­
cipitator to remove NO and SO2 gases simultaneously. SO2 and NO were destroying the UV lamp. The high-speed spray solution in the wet
absorbed and oxidized by the aerosol particles in NaClO2 in the wet scrubber clears the dirt from the surface of the tube, thereby maintaining
scrubber. Subsequently, the aerosol particles were electrostatically the spread of UV light and extending the life of the photochemical sys­
precipitated by a plasma electrostatic precipitator (Fig. 7). As suggested tem. No secondary pollution is caused during the removal, and the water
from the results, the NO and SO2 removal efficiencies of the system were can even be recycled. Under optimized conditions, the maximal removal
94.4% and 100%, respectively. Cui et al. [107] developed a compre­ efficiency of NO was 96.8%, and SO2 could be removed entirely.
hensive system to remove NO and SO2 while integrating a wet electro­ Xie et al. [109] studied the effects of experimental parameters on the
static precipitator (WESP) and dielectric barrier discharge (DBD). The simultaneous removal of SO2 and NO by the VUV/H2O2 oxidation pro­
oxidizing substances generated in the DBD oxidize SO2 and NO, and the cess in a pilot-scale photochemical spraying tower. As suggested from
oxidation product can be further converted into acid mist when water the results, under most experimental conditions, the SO2 removal effi­
vapor is present in the flue gas; the WESP can then absorb and capture ciency reached 100%. VUV irradiation intensity, H2O2 concentration,
the acid mist and residual free radicals. The system exhibited better and solution pH increase could facilitate NO removal, and the removal
removal performance with an optimal removal efficiency of 98.9% for efficiency could reach 72.9%. Comparing the investment operation cost
SO2, as well as an optimal removal efficiency of 87.1% for NO. of the system with the value of the combined process of NH3-SCR and
Combining the plasma technology can remarkably improve the removal Ca-WFGD, the system is reported to have a good economy and can be
efficiency of SO2 and NOX, but it can be seen from the system diagram used in industrial production applications.
that after the electrostatic part is added, the system is more complicated, With the improvement in the industrial level and the enhancement of
and the investment and operating costs also increase. environmental awareness, traditional gas separation technology should
be optimized to meet the new challenges. Compared with the wet
Photocatalytic oxidation method scrubbing technology alone, the combination of plasma technology and
the photocatalytic oxidation method can remarkably improve the
The photocatalytic oxidation method indicates that the photocatalyst removal efficiency of SO2 and NOX. However, hybrid methods have
will have a catalyzing effect as irradiated by a specific wavelength light some disadvantages that limit business applications, such as the system
source, and the surrounding water molecules and oxygen molecules are being more complex and the investment burden and operation cost are
excited to generate active •OH− and •O−2 free ion groups (Fig. 8). After also increased. Therefore, reducing the cost of the composite methods
the gaseous contaminants are oxidized by the free ions, they can be and simplifying the system are critical problems that need to be solved.
absorbed by the wet scrubber. Photocatalytic oxidation is advantageous At present, the research results of the composite methods have proved
in a compact structure, with no secondary pollution and a high removal that the combination of a wet scrubber with other technologies can
efficiency. Liu et al. [108] developed a novel method for the simulta­ effectively remove harmful gases and has the advantages of saving en­
neous removal of NO and SO2 using a vacuum ultraviolet (VUV)-acti­ ergy and reducing secondary pollution, which is an important direction
vated O2/H2O/H2O2 system in a wet VU-spraying reactor. Dust and dirt for the development of wet scrubbing technology.
rapidly adhere to the surface of the quartz tube during the UV (ultra­
violet)-ray drying process, blocking the transmission of UV light and

Fig. 7. Facility diagram of wet scrubber combined with plasma electrostatic precipitator [103].

9
M. Zhao et al. Sustainable Energy Technologies and Assessments 47 (2021) 101451

Conclusion 2013 and contribution of meteorological factors. Atmos Chem Phys 2015;15(22).
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