Environ Sci Pollut Res (2017) 24:26310–26323
https://doi.org/10.1007/s11356-017-0480-6
REVIEW ARTICLE
Purification of Hg0 from flue gas by wet oxidation method
and its mechanism: a review
Yi Xing 1,2 & Bojun Yan 1,2 & Pei Lu 1,2 & Xiaoxu Cui 1 & Liuliu Li 3 & Mengsi Wang 1
Received: 23 August 2017 / Accepted: 12 October 2017 / Published online: 23 October 2017
# Springer-Verlag GmbH Germany 2017
Abstract The vast majority of Hg2+ can be removed while
elemental mercury (Hg0) can hardly be removed due to its
characteristic of high volatility and insolubility in water. Till
now, how to oxidize Hg0 to Hg2+ is the key for the purification
of Hg0, especially when there are others pollutants, such as
HCl, SO2, and NOx. In this review, the method and mecha-
nism of Hg0 purification from flue gas by H2O2, KMnO4,
NaClO2, and O3 are reviewed comprehensively. It is conclud-
ed that the oxidation of Hg0 mainly depends on the electronic
supply efficiency from the solution. The Fenton reagent, com-
posed of H2O2 and metal cations, is superior to O3 and the
solution of KMnO4 and NaClO2. Moreover, HCl, SO2, and
NOx in the flue gas can influence the oxidation and purifica-
tion mechanism of Hg0. It is found that HCl in flue gas had
obvious auxo-action on the oxidation of mercury, and SO2 and
NOx have different effects on the oxidation of Hg0 with the
change of compositions and concentration of pollutants in the
flue gas. In general, SO2 and NOx can slightly promote the
oxidation of Hg0 due to the synergistic effect.
Bojun Yan contributed equally to this work.
Responsible editor: Bingcai Pan
* Pei Lu
cnlupei@163.com; lupei@ustb.edu.cn
1
School of Energy and Environmental Engineering, University of
Science and Technology Beijing, Beijing 100083, China
2
Beijing Key Laboratory of Resource-Oriented Treatment of
Industrial Pollutants, University of Science and Technology Beijing,
Beijing 100083, China
3
School of Environmental Science and Engineering, Hebei University
of Science and Technology, Shijiazhuang 050018, China
Keywords Hg0 . Flue gas . Wet oxidation method .
Purification . Mechanism
Introduction
Mercury (Hg) is very stable and can be evaporated at room
temperature. The vapor is highly toxic due to its bioaccumula-
tion and can be transferred worldwide. Moreover, mercury can
be turned into methylmercury (CH3Hg) under complicated con-
ditions by the action of microorganisms (Schmeltz et al. 2011).
Mercury and its compounds are highly toxic pollutants which
can cause serious damage to the human nervous system (Meng
et al. 2011). Mercury emissions from human activities are esti-
mated to be 2000–6000 t/a all over the word, which accounts to
about 30–55% of global atmospheric mercury emissions (Yang
et al. 2007; Yan et al. 2004). Mercury pollution is mainly caused
by the burning of fossil fuels (Xu et al. 2008). With the increase
of global consumption of coal resources, mercury emission is
also increasing (Pacyna et al. 2006, 2010). Therefore, mercury
emission is becoming a global problem (Rallo et al. 2012).
The efficiency of methods for removing mercury depends
greatly on the species composition of mercury (Pavlish and
Mann, 2003). Mercury in the flue gas usually exists in varying
percentages of three basic chemical forms: elemental mercury
(Hg0), oxidized mercury (Hg2+), and particle-bound mercury
(Hg (p)) (Wu et al. 2008; Gale et al. 2008; Yuan et al. 2012).
Hg0 is very difficult to be removed because of its high volatility
and low solubility in water (Wang et al. 2014a; Driscoll et al.
2013). Therefore, the mercury pollution control technology is
mainly focused on the Hg0 purification (Pavlish and Mann,
2003).
In recent years, a number of elemental mercury removal tech-
nologies have been developed, which can be divided into two
main methods (Liu and Wang, 2014). The first one is to convert
Environ Sci Pollut Res (2017) 24:26310–26323
Hg0 to Hg2+ by oxidizing (Presto and Granite, 2006; Li et al.
2011; Xu et al. 2015), such as catalytic oxidation, photochemical
oxidation, ozonation (O3), photocatalytic oxidation, potassium
permanganate (KMnO4), sodium chlorite (NaClO2), and UV/
H2O2 oxidation (Chen and Mathur, 2006; Snider and Ariya,
2010; Liu, 2011, Liu et al. 2015a; Byun et al. 2014; McLarnon
et al. 2005; Nick et al. 2008); the other one is to adsorb Hg0 from
the flue gas (Huang et al. 2015; Lee et al. 2008; Qu et al. 2015).
Till now, the oxidation technology is becoming the most feasible
way to control mercury emissions due to its high efficiency. In
detail, there are dry and wet methods for Hg0 oxidation.
The process of removing mercury through dry method does
not produce waste water, the flue gas temperature after purifi-
cation is high; no need for secondary heating. Zhao found that
combination of selective catalytic reduction (SCR) and flue gas
desulfurization (FGD) is considered as one of the most effective
methods to remove Hg from flue gas (Zhao et al. 2015). At
present, the sintering flue gas denitrification in China is still in
the initial stage. For most steel companies, the SCR system
needs to be rebuilt. Although the pollutant purification efficien-
cy is high, but it needs huge energy consumption and space and
configure expensive catalytic systems. Meanwhile, the wet ox-
idation system can be easily made replacements and technical
innovations on current desulfurization system. It is very simple
and feasible to purify the flue gas discharged by coal-fired
power plants and steel mills, especially for developing coun-
tries. Therefore, oxidation and purifying Hg0 from flue gas by
wet method are specially discussed in this study.
Wet mercury removal method mainly refers to the absorp-
tion of mercury using desulfurization absorbing liquid. Wet
FGD (WFGD) system can remove nearly 90% of the Hg2+ but
essentially none of the Hg0 (Wang et al. 2007; Zhuang et al.
2004). Thus, according to the status of wet mercury removal, a
lot of efforts have been conducted to oxidize Hg0 to Hg2+ for
the purpose of increasing the mercury removal efficiency
(Diaz-Somoano et al. 2005). The forms of mercury and their
conversions in flue gas are illustrated in Fig. 1 (Fernández-
Miranda et al. 2014).
This review mainly focused on the purification of mercury
in flue gas by wet oxidation method, and different techniques
of mercury oxidants are summarized and compared compre-
hensively. The impact and mechanism of flue gas components
on the oxidation of mercury are also discussed. Finally, rea-
sonable suggestions were given for the study of mercury re-
moval in flue gas.
Methods and different oxidants
Oxidation by H2O2
Under different reaction conditions, H2O2 can be decomposed
and produce the following four substances: ·OH + OH, HO2· +
26311
H·, H2O + O2, and H2O + HO2·. ·OH is an ideal oxidizer with
strong oxidability and high reaction rate. The redox potential
of ·OH is up to 2.80 V and the oxidation reactions with ·OH
can be carried out fast and completely (Li et al. 2009; Liu and
Wang, 2014). The decomposition of H2O2 and the generation
of ·OH were mainly through two ways: (1) excitation under
high temperature (higher than 500 °C) (Cooper et al. 2002);
(2) factor addition under low temperature (room temperature
to 90 °C), by adding metal ions to the H2O2 such as: Fe2+ and
Cu2+ or applying ultraviolet (UV) light or ultrasound (Liu
et al. 2013; Ding et al. 2014). In the situation of the rapid
decomposition of H2O2 in the role of the relevant catalyst such
as Fe2+ and production of ·OH (Li et al. 2013), these following
reactions will take place.
Fe2þ þ H2 O2 →Fe3þ þ OH− þ ∙OH ð1Þ
−
Fe 3þ
þ H2 O2 þ OH →Fe 2þ
þ H2 O þ ∙OH ð2Þ
Fe3þ þ H2 O2 →Fe2þ þ Hþ þ HO2 ð3Þ
HO2 þ H2 O2 →H2 O þ O2 ↑ þ ∙OH ð4Þ
2þ
=Fe3þ
Hg0 þ H2 O2 →Fe HgO þ H2 O ð5Þ
According to reactions (1)–(5), it can be found that the
main function of Fe3+ or Fe2+ is to act as a catalyst to accel-
erate the decomposition of H2O2. Liu has studied the oxida-
tion of mercury by Fenton solution (Liu, 2011, Liu et al.
2014a, Liu et al.2015a) by adding metal ions and ultraviolet
light. The mechanism of mercury oxidation by UV/H2O2 is
shown as Fig. 2. Hg0 can be easily oxidized to HgO by ·OH
through the following reaction in UV/H2O2 system.
Hg0 þ ∙OH→HgðOHÞ2 →heat HgO þ H2 O ð6Þ
When the concentration of the H2O2 is high enough, Hg0
can also be oxidized by H2O2 according to the following re-
action.
Hg0 þ H2 O2 →HgO þ H2 O ð7Þ
Meanwhile, Dennis (2007) has carried out an interesting
study to remove Hg0 from flue gas. The results show that 75%
of the Hg0 can be oxidized by Fenton solution and the best
reaction pH is 1.0~3.0 (Burbano et al. 2005). Furthermore,
many researchers have studied the oxidation by H2O2; the
comparison studies in different reaction systems have been
carried out and the results are summarized in Table 1.
Table 1 and reactions (1)–(7) illustrate that H2O2 has a
strong oxidizing effect on Hg0, the removal efficiency of
Hg0 is high and the oxidation process does not produce other
pollutants. Moreover, the removal efficiency of Hg0 can be
greatly affected by the experimental condition. In Fenton re-
agent, the removal efficiency of Hg0 mainly depends on the
26312 Environ Sci Pollut Res (2017) 24:26310–26323

Fig. 1 The schematic diagram of

the forms of mercury and its
conversions in flue gas
(Fernández-Miranda et al. 2014)

decomposition rate of H2O2 and it can be accelerated by another important work on Fenton oxidation technology
adding catalysts or applied energy to the system, which results industrialization.
in the significant enhancement on Hg0 removal efficiency.
Due to its low price and high efficiency on purifying Hg0, Oxidation by NaClO2
H2O2 with some metal cation (Fenton solution) is desirable
for purifying Hg0 from flue gas. The development of photo- Till now, NaClO2 is widely used in many chemical fields as an
chemical reactor can be used to effectively remove Hg0 like oxidizing agent due to its strong performance on oxidation
UV/H2O2/O2 system (Liu and Wang, 2014). (Byun et al. 2014; Qian et al. 2007). Strong oxidizing agents
Till now, purifying by H2O2 has been studied for more than of ClO and Cl can be generated by the reaction between
10 years, and the influence of removal conditions, such as NaClO2 and SO2 or/and NO. Meanwhile, chlorine (Cl2) will
temperature, catalyst, and UV, have been studied in detail. be generated at the same time. The reactions are shown as
Though it has been found that Fenton reagent is a good oxi- (8)–(10).
dizer for Hg0, it is still necessary to develop more effective
OClO þ NO→NO2 þ ClO ð8Þ
methods to accelerate the decomposition of H2O2 to enhance
the removal efficiency of Hg0 in the future work. At the same ClO þ NO→NO2 þ Cl ð9Þ
time, lowing the cost of H2O2 applied in the removal of Hg0 is Cl þ Cl→Cl2 ð10Þ

Fig. 2 Reaction mechanism of

Hg0 removal by UV/H2O2
process (Liu and Wang, 2014)
Environ Sci Pollut Res (2017) 24:26310–26323 26313

Table 1 Removal efficiencies of mercury in different reaction systems

Reaction systems Experiment conditions Removal Reference

efficiency (%)
Hg0 SO2 O2 (%) NO H2O2 UV pH Fe2+
(μg/m3) (ppm) (ppm) (mol/L) (nm) (mol/L)

UV/H2O2/Fe3+ 30 800 6 400 0.40 254 3.4 0.006 67.9 Liu et al., 2015a
UV/H2O2 30 1500 6 400 0.50 254 3.97 – 50.6 Liu et al., 2014a
UV/H2O2/O2 30 1500 6 400 0.50 254 3.97 – 83.5 Liu et al., 2014a
H2O2/O2 30 1500 6 400 0.50 – 3.97 – 9.8 Liu et al., 2014a
2+
Fenton solution (Fe /H2O2) 40 1000 6 400 1.2 – 3.4 0.06 100 Liu et al., 2015a
H2O2/O2 30 – 6 – 0.50 – 3.97 – 11.7 Liu and Wang, 2014
UV/H2O2 30 – 6 – 0.50 254 3.97 – 52.7 Liu and Wang, 2014
UV/H2O2/O2 30 – 6 – 0.50 254 3.97 – 85.1 Liu and Wang, 2014

It is well known that Hg0 can be easily oxidized to Hg2+ by
Cl2, which can be shown as reaction (11).
Hg þ Cl2 →HgCl2
According the experimental results reported by Byun et al.
(2010), NaClO2 has a significant oxidation effect on Hg0
when the concentration of Hg0 is 260 μg nm−3 and the con-
centrations of NaClO2 are 0.1, 0.18, and 0.36 g nm−3, respec-
tively. The experiment procedure is shown in Fig. 3 (Byun
et al. 2010). The reported experimental results show that
NaClO2 added into the sintering flue gas can greatly promote
the oxidation of Hg0, and the oxidation rate of Hg0 increases
with the concentration increasing of NaClO2 (Nick et al.
2008). When the concentration of ClO is 3 mmol/L, the re-
moval efficiency of Hg0 is as high as 100% (Jin et al. 2011).
With the reactions between NaClO2 and other reducing com-
ponents in flue gas, amount oxidants will be generated, such
as ClO, Cl, and Cl 2 , which will greatly accelerate the
oxidation of Hg0 (Byun et al. 2009). On considering the dif-
ference of reactions between NaClO2 and these reducing com-
ponents in flue gas, the efficiencies of purifying Hg0 and its
ð11Þ mechanism will also be different (Nick et al. 2008). According
to the reported results of Zhao et al., the acid condition of
solution is beneficial to the oxidation of Hg0 (Zhao et al.
2009).
Though NaClO2 can obtain significant oxidation efficiency
of Hg0, this method generates a number of new pollutants (Cl−
and Cl2) into absorbing solution or flue gas (Fan and Deng,
2012), which is dangerous to the environmental protection
device and environment. Therefore, NaClO2 and its solution
should be carefully used for removing Hg0 from flue gas.
Oxidation by KMnO4
Potassium permanganate (KMnO4) solution is one kind of
effective absorbents for oxidizing Hg0 from flue gas, and the

Fig. 3 Temporal profile of Hg0

concentration obtained by the
injection of NaClO2(s) (Byun
et al. 2010)
26314
removal efficiency is very desirable due to the strong oxidiz-
ing performance of KMnO4, especially for the low concentra-
tion of Hg0. Acidic KMnO4 is suggested to be used as an
absorbing solution for purifying Hg0 in the gas phase by the
US Environmental Protection Agency (EPA) as absorbent
method 29 (Liu and Wang, 2014), and KMnO4 solution can
also be used to collect mercury from flue gas during the puri-
fication process (Hara 1975). Ye et al. also reports that
KMnO4 has a strong action for the removal of Hg0 (Ye and
XH, 2007).
Zhao (1999) reports that the reactions of Hg0 and KMnO4
can be influenced by the pH of the KMnO4 solution. Mn2+ can
be used to produce catalytic agents to speed up reactions,
especially under acidic conditions. The H+ can increase its
redox potential while the produced Mn2+ can play a catalytic
role. The reactions of KMnO4 under different pH values are
shown as follows (Liu and Wang, 2014; Ye and XH, 2007).
Under strongly acidic condition:
5Hg0 þ 2MnO4 − þ 16Hþ →5Hg2þ þ 2Mn2þ þ 8H2 O ð12Þ
Under weakly acidic condition:
3Hg0 þ 2MnO4 − þ 8Hþ →3Hg2þ þ 2MnO2 þ 4H2 O ð13Þ
Under neutral condition:
3Hg0 þ 2MnO4 − þ H2 O→3HgO þ 2OH− þ 2MnO2
Under strongly alkaline condition:
Hg0 þ 2MnO4 − þ 2OH− →HgO þ 2MnO4 2− þ H2 O
In order to study the performance of KMnO4 in Hg0 oxi-
dation, oxidant solutions of KMnO 4, NaClO 2 , NaClO,
K2S2O8, and H2O2 are comprehensively studied in WFGD
system by Ping et al. (2012). In Table 2 (Ping et al. 2012), it
can be found that when there is no interference of other con-
ditions, KMnO4 solution can yield the highest oxidation and
removal efficiency on Hg0.
Moreover, according to the results reported by Liu and
Wang, 2014), pH is a key factor in the oxidation of Hg0 by
KMnO4. With the increase of pH value, the removal efficiency
Table 2 The effect of oxidant on Hg0 removal efficiency (Ping et al.
2012)
Oxidant solution Experimental conditions Removal
efficiency (%)
KMnO4 Qgas 1 L/min 96.70
NaClO2 pH 5.2; 69.09
Oxidant 1 mmol/L;
NaClO 60.65
Hg0 50 μg/m3;
K2S2O8 Treaction 55 °C 51.45
H2O2 5.14
Environ Sci Pollut Res (2017) 24:26310–26323
will be firstly decreased and then increased, just like a semi-
waveform. The pH value has a significant effect on the oxida-
tion kinetics and reaction pathways of KMnO4, which results
from the difference of the standard electrode potential (φ0) and
reaction rate. The redox potential of KMnO4 solution can be
illustrated as the following equation:
φ ¼ φ0 þ 0:01184lg½cðHþ Þ ð16Þ
where c is the concentration of H+ in KMnO4 solution.
It is clear that the redox potential will increase with the
decreasing of pH and the oxidizing ability of KMnO4 solution
will be enhanced. Therefore, it can yield the highest removal
efficiency of Hg0 under the condition of strong acid (Liu,
2011). When it is under strong alkaline condition, OH− can
also be oxidized to ·OH, which is also helpful for the
oxidization and removing of Hg0 (Hara 1975). The redox
reactions and their various potentials are summarized and
shown in Table 3.
According to the results of Tables 2 and 3, the removal
efficiency of Hg0 by KMnO4 solution is obviously higher than
that of the others. However, the cost of the method is very
high, and the reaction is difficult to be controlled. Therefore,
how to control the reaction process of KMnO4 exactly and
decrease its cost is still a tough task and need be further
studied.
ð14Þ
Oxidation by O3
It is different from other oxidants that O3 has the unique char-
ð15Þ
acteristic and very high oxidation-reduction potential (ORP),
only slightly below to that of Cl (Jin et al. 2011). Moreover, it
can exist with a long oxidation life in the flue gas (Biswajit
and Ariya, 2003).
Wang et al. (2007) adds O3 into flue gases of WFGD to
remove Hg0. It is found that O3 will firstly react with NO
when there is NO in flue gas and when the ratio of O3 and
NO is 2:1, the removal efficiency of Hg0 can reach as high as
95% without the generation of secondary pollutants (Wang
et al. 2007). However, HgO will be decomposed into Hg
and O 2 when the temperature is higher than 371 °C.
Therefore, Wang suggests that the optimal temperature for
Table 3 Redox reactions and their potentials of various couples of
KMnO4 ions (Liu et al. 2011)
Half-cell reactions Standard electrode pH
potential φ0 (V)
Mno4‐ + 8H + 5e‐ → Mn2+ + 4H2 O 1.51 < 3.5
Mno4‐ + 4H+ 3e‐ → MnO2 + 2H2 O 1.70 3.5–7
Mno4‐ + 2H2O + 3e‐ → MnO2 + 4OH‐ 0.6 7–12
Mno4‐ + e‐ → MnO42‐ 0.56 > 12
Environ Sci Pollut Res (2017) 24:26310–26323 26315

Hg0 oxidation should be 245–273 °C. The oxidation property

by ozone at different temperatures is shown in Fig. 4. The
reactions of Hg0 oxidation by O3 are shown as the following
equations.
Hg þ O3 →HgO þ O2 ð17Þ
Hg þ O→HgO ð18Þ

On the oxidation mechanism of Hg0 by O3, Wang et al.

(2007) reports that Hg0 can be effectively oxidized by O3 in
flue gas, and the content of NO3 is a key factor to Hg0 oxida-
tion. The reactions can be shown as (19) and (20).

O3 þ NO2 →NO3 þ O2 ð19Þ

Fig. 5 Reaction routes of elemental mercury oxidization in flue gases by
Hg þ NO3 →NO2 þ HgO ð20Þ ozone (Wang et al. 2007)

Moreover, Dai and Tao, 2014) reports that the oxidation of

decompose (Wei et al. 2007) and the oxidation rate of Hg0
Hg0 can be greatly enhanced with the concentration ratio of
begins to decrease. Meanwhile, the generation of O3 is very
O3/NO or/and the temperature of flue gas increasing. The
expensive. Therefore, demercuration by O3 is not suggested
reaction routes of oxidization of Hg0 in flue gases by ozone
for large-scale industrial applications. Obtaining ozone with
are illustrated as Fig. 5(Wang et al. 2007). Calvert (2005) has
low-cost and high efficiency and enhancing its oxidation effi-
studied the mechanism of the removal Hg0 in atmospheric
ciency are the keys in future research and application in
environment by O3 and finds that reaction (17) cannot occur
demercuration by O3.
in the atmosphere. Hg0 and O3 will firstly react and generate
HgO3, which is a metastable compound. After that, HgO3 will
be decomposed to HgO and O2. Other researches find that a
combining gas-phase oxidation method, ozone and alkali ab- Effects of experimental conditions
sorption included, will significantly improve the oxidizing
and removal of Hg 0 (Zhang et al. 2014; Glomba and Influence by the constituents of flue gas
Kordylewski, 2014).
However, the demercuration by O3 can be affected by tem- The composition of industrial flue gas is complex, and differ-
perature easily. When the temperature is over 150 °C, O3 will ent compositions have significantly different impacts on the

Fig. 4 Mercury oxidation

property by ozone at different
temperature (Wang et al. 2007)
26316
removal of Hg0. However, due to lack of oxidant, Hg0 can not
be fast oxidized in gas phase components, though there are
SO2, HCl, and NOx in the flue gas. Up to now, it has been
demonstrated that the oxidation and removal of Hg0 mainly
occurs during the gas-liquid mass transfer process (Fuente-
Cuesta et al. 2012). Therefore, the effect of SO2, HCl, and
NOx on the oxidization of Hg0 in flue gas with wet oxidation
method are mainly discussed in the following part.
Effect of SO2
Sulfur dioxide is amount discharged by coal-fired factory, such
as power plants and steel mills, and it has been reported that SO2
can influence the oxidation of Hg0 under different reaction con-
ditions (Fernández-Miranda et al. 2014; Liu et al. 2014a, b;
Eswaran and Stenger, 2008; Ghorishi and Kilgroe, 1999; Xu
et al. 2013). Fernández-Miranda et al. (2014) finds that SO2
can enhance the oxidation of Hg0, and the oxidation rate can
only be increased 3–5% when the concentration of SO2 is 1000–
2000 ppm. The oxidation of Hg0 is shown as reaction (21).
Hg0 þ SO2 þ O2 →HgO þ SO3 ð21Þ
0 due to the reaction between NO and O2 in flue gas, NO can be
Liu has found that when both SO2 and NO exist with Hg
in flue gas, the oxidation rate of Hg0 will be decreased (Liu
et al. 2014a, b). When there is no other oxidizing gases (such
as Cl2) in the flue gas, the presence of SO2 has a slight en-
hancement to the oxidation of Hg0. But in the coal-fired flue
gas, the concentration and oxidation rate of Hg0 in flue gas are
always much lower than that of SO2 (Eswaran and Stenger,
2008). Moreover, the addition of SO2 in the flue gas will
inhibit the formation of Cl atoms and Cl2, which results in
the fact that SO2 will compete with Hg0 for oxidizing agent.
It will reduce the rate of oxidation of Hg0 (Ghorishi and
Kilgroe, 1999; Xu et al. 2013). The oxidation inhibition mech-
anism of Hg0 by SO2 is shown as the following reactions.
Cl2 þ SO2 þ H2 O→2HCl þ SO3 ð22Þ
2Cl þ SO2 þ H2 O→2HCl þ SO3 ð23Þ
Effect of HCl
In the process of coal combustion, Cl− contained in flue gas
can partially exist in the status of HCl, and it can oxide Hg0
from flue gas by the following reaction.
2HCl þ Hg →HgCl2 þ H2
0
ð24Þ
Hall, 1995) studies the removal of Hg0 from simulated flue
gas and finds that within a certain temperature range, Hg0 can
rapidly react with HCl. When the temperature of flue gas is
900 °C, about 90% of the reactions can be completed within
0.7 s. The contents of Hg2+ will increase with the increase of
Environ Sci Pollut Res (2017) 24:26310–26323
the concentration of HCl in the simulated flue gas. On the
other hand, HCl can react with O2 in the simulated flue gas
to generate Cl2, and it is very feasible for the oxidation of Hg0.
The oxidation reaction can be shown as reaction (25).
1
2HCl þ O2 →catalyst Cl2 þ H2 O ð25Þ
2
Gao et al. 2004has conducted an experiment on the two
types of flue gas system (13% CO 2 –7% O 2 –80% N 2 –
800 ppm NO system and 13% CO 2 –7% O 2 –80% N 2 –
800 ppm NO–1200 ppm SO2 system) for exploring the impact
of different concentrations of HCl on Hg0 oxidation, respec-
tively. It is found that HCl can effectively promote the oxida-
tion of Hg0 in flue gas. The oxidation of Hg0 is heavily de-
pendent on Cl as a medium in the oxidation, and the concen-
tration of Hg2+ is linear positive correlation with the concen-
tration of HCl. Thermodynamic calculation results are consis-
tent with that of experiments carried out by Gao et al. (2004).
Effect of NOx
About 90% NOx in the flue gas is NO in flue gas. Meanwhile,
partially oxidized to NO2. Therefore, when the influence of
NOx on the oxidation of Hg0 is analyzed, both NO and NO2
must be considered.
The influence on removal mechanisms of Hg0 oxidation in
the flue gas by NOx is similar to that by SO2. Xue reports that
when there are no other oxidizing gases in flue gas, the pres-
ence of NO has a slight influence on the catalytic oxidation of
Hg0 and the enhancement effect is a little less than that of SO2.
When the concentration of NO is controlled within 0–500 mg/
m3, Hg0 oxidation efficiency can increase to about 4%, which
results in the generation of NO2, generated by NO oxidization.
It is a stronger oxidizing agent for Hg0. When the concentra-
tion of NO continues to increase, the oxidation rate of Hg0 will
be decreased because of the competition between NO and Hg0
and the change of the pH value of the absorption solution (Xue
2014). Therefore, excess of NO will inhibit the oxidation of
Hg0. The main reactions between NO and Hg0 can be sum-
marized as below.
2NO þ O2 →2NO2 ð26Þ
NO2 þ Hg0 →HgO þ NO ð27Þ
Other researchers have found similar phenomena. The ox-
idation effect of NO on Hg0 primarily depends on the concen-
tration of NO in oxidation experiments of Hg0 by Fenton
reagent, and the oxidation of Hg0 can be hindered due to the
reaction between NO and ·OH (Liu, 2011). However, accord-
ing to the results reported by Gao, the oxidation efficiency of
Hg0 is always higher in the presence of NO in flue gas than
that in the absence of NO (Gao et al. 2004).
Environ Sci Pollut Res (2017) 24:26310–26323 26317

Nuria Fernández-Miranda
Though NO2 is a more active oxidizing agent than NO, it

Liu and Wang, 2014

has no effect or a slight effect in promoting the oxidation of
Hg0 because of its low concentration. The reaction of the

Zhou et al. 2015

Gao et al. 2004
et al. 2014

Hutson 2008
oxidation of Hg0 by NO2 can be shown as reaction (27).

Reference
After summarizing a number of literatures which men-
tioned the influence of different constituents of the flue gas
on Hg0 oxidation process, it can be concluded that under nor-
mal circumstances, HCl can always promote the oxidation and

Effects on mercury
removal of Hg0, and the related experimental results are sum-

suitable amounts
Slight promotion
Slight promotion

Promotion under
marized in Table 4.

Promotion

Promotion

Promotion
Promotion
Promotion
oxidation

Inhibition
Inhibition
Inhibition
No effect
Influence by the constituents of H2O2

As discussed above, H2O2 solution can be used for wet oxi-

dation and removing of Hg0 from flue gas. In order to increase

84.5 Decrease to 78.8

85.1 Decrease to 81.4
the discharge of ·OH and enhance the removing efficiency of

92 Decrease to 90
Hg0, the optimization of the excitation and decomposition of

oxidation %
H2O2 by metal cation is very important (Zhou et al. 2015;

9.8–82.8

80–100
81–100
Hutson 2008; Zepp et al. 1992; Malato et al. 2007).

94–99
40–81
Hg0

4–5
18

92
45
48
–
Classical Fenton solution

127–827
The Fenton reaction mainly describes the activation of H2O2 by
T °C

150
150

150
300
300

50
50
50

50
50

55
55
50
ferrous ions (Fe2+) to generate ·OH (Cheves Walling 1973;
Pignatello et al. 2006), and the reaction equations can be sum-
marized as reactions (1)–(3) (Liu and Wang, 2014; Dranga et al.
(%)
O2

2012; Granite et al. 2007). Fe3+ can react with OH− to form
4
4

8
8
4
4
4
7
6
6

–
–
insoluble ferric hydroxide [Fe(OH)3] in neutral pH conditions
HCl (ppm)

(Neyens and Baeyens, 2003). Therefore, the pH of the solution

should be maintained in an acidic environment. The relation-
Effects of different factors in different experiments on mercury oxidation

ship between the forms of iron species in aqueous and the pH of

25

60
60
–
–

–
–
–
–
–
–

–
–
the solution could be shown as Fig. 6 (Bokare and Choi, 2014).
Main experimental conditions

According to the reported results (Liu and Wang, 2014; Pouran

NO (ppm)

et al. 2014; Pham et al. 2010; Umar et al. 2010), the optimum 100–500
0–2000

0–500
1000

working pH value of Fenton reaction is 2.8–3.2. When the

800
800
800
400

400

200
–

–
concentration of H2O2 remains constant, appropriately enhanc-
ing the concentration of Fe2+ can be favorable to accelerate the
decomposition rate of H2O2 and the oxidation of Hg0.
SO2 (ppm)

1000–2000

500–1000
0–3000

0–1500

However, some research (Kang et al. 2002; Ashraf et al.

1200
1200
1200

1500

1500
1500

2006; Zazo et al. 2005) also find that when Fe2+ is excessive
–
–

–
–

in Fenton solution, the following reaction (28) will occur with a

high reaction rate and it will reduce the concentrations of ·OH
Catalyst dosage

and Fe2+. Therefore, the removal process of Hg0 will be limited.

UV power

(1.0 g/L)

Fe2þ þ OH→Fe3þ þ OH− ð28Þ

Impact
factor

NOx

NOx

NOx

NOx
HCl
HCl
SO2

SO2

SO2

SO2

SO2
NO
Fe2.45Ti0.55O4/H2O2

NaClO2 wet system

Oxidation method

Ultraviolet/H2O2 solution
Constituents of the
flue gas

The light source can be excited under specific wavelengths of

UV/H2O2
Table 4

the UV to produce light quantum. Under the impact of light

quantum, which is full of different energies, some substances
26318 Environ Sci Pollut Res (2017) 24:26310–26323

Fig. 6 Iron species in aqueous

solution as a function of pH
(Bokare and Choi, 2009)

can be excited to break down. The production of ·OH in UV/ shorter UVeffective propagation distance will result in smaller
H2O2 solution is mainly by means of the energy provided by amount of mercury removal.
UV which can excite the decomposition of H2O2. The homo- At the same time, UV power should also be considered in
lytic reaction of H2O2 can be shown as Eq. (29) (Jeong and UV/H2O2 system. Decomposition of H2O2 cannot be com-
Jurng, 2007; Liu, 2011; Jia et al. 2010). pleted when the UV power is too low. However, when the
power is beyond the scope of the required for the oxidation
H2 O2 þ hv→2  OH ð29Þ
of Hg0, the chemical reaction may transfer to the mass transfer
Due to the hemolytic of H2O2, UV often has a significant controlling and will cause the waste of resources (Garoma and
impact on photochemical reaction. Mercury removal rate can Gurol, 2004; Song et al. 2006). The most appropriate power
be improved nearly 80% for H2O2 system under the stimula- for per unit solution is suggested as 0.006 W/mL (Liu, 2011)
tion of UV (Liu and Wang, 2014; Liu et al. 2015a). The UV in UV/H2O2 solution.
wavelength is the most influential factor for the production of
·OH in UV/H2O2 system (Cater et al. 2000;Muruganandham Non-ferrous Fenton solution
and Swaminathan, 2004). Different UV wavelengths (185,
254, and 365 nm) are used to study the effects of UV wave- In order to completely decompose H2O2 and achieving a more
length on Hg0 removal efficiency by Liu and Wang, 2014), desirable removal efficiency of Hg0, some researchers have
and it is illustrated that 254 nm is the most effective UV studied on non-ferrous Fenton system. The redox performance
wavelength in the photochemical reaction of removing Hg0. of metal or metal cation can be described by the characteristic
Some other documents also report similar conclusions of loss or gain of electrons. The ideal Fenton catalyst should
(McLarnon et al. 2005; Jia et al. 2010; Granite and Pennline,
2002). The energy of photon can be calculated by Planck Eq.
(30) (Xu 2005).
c
ε ¼ hv ¼ h ð30Þ
λ
where ε is the energy of photon, J; ν is the UV frequency, 1/s;
h is the Planck constant, 6.626 × 10−34 J s; c is the speed of
light, 2.998 × 108 m/s; and λ is the UV wavelength, 100–
380 nm.
According to Eq. (30), shorter wavelength of UV light has
the larger energy of photoelectron, and it is easier to stimulate
the decomposition of H2O2 and produce more ·OH. However,
when the wavelength of UV light is decreased, the effective
propagation distance is reduced at the same time (Xu 2005), Fig. 7 Electron transfer pathways of CeO 2 under sulfuric acid-
which will inhibit the oxidation of Hg0 in reactor. Therefore, pretreating (Wang et al. 2014a)
Table 5 Description of H2O2-based AOPs
Type of H2O2 solution
Classical Fenton
(Fe2++H2O2)
Photo-Fenton
(UV + Fe2++H2O2)
UV + H2O2
Sono-Fenton
(Ultrasonic + Fe2+ + H2O2)
Non-ferrous Fenton solution
(Ce/Al/Mn + H2O2)
Key reaction pathway
Fe2+ + H2O2 → Fe3+ + ⋅ OH + OH‐
(a) Fe2+ + H2O2 → Fe3+ + ⋅ OH + OH‐
(b) Fe3+ + H2O2 + hv → Fe2+ + ⋅ OH + OH‐
(c) H2O2 + hv → 2 ⋅ OH
H2O2 + hv → 2 ⋅ OH
(a) H2O2 + ))) → 2 ⋅ OH
(b) Fe2+ + H2O2 + Fe3+ + ⋅ OH + OH‐
(c) Fe3+ + H2O2 + ))) → Fe2+ + ⋅ OOH
(d) H2O + ))) → + ⋅ OH + OH+
(e) O2 + ))) → 2 ⋅ O
(f) ⋅O + H2O + → 2 ⋅ OH
(a) M + xH2O2 + Mx+ + x ⋅ OH + xOH‐
(b) Mn+ + xH2O2 + Mn + x+ + x ⋅ OH + xOH‐
Advantages Disadvantages References
(1) The reaction conditions require lower (1) Progress of the reaction is Liu et al. 2013
(2) No mass transfer limitations difficult to control Ding et al. 2014
(2) Large iron-containing sludge Bigda 1995
Environ Sci Pollut Res (2017) 24:26310–26323
Bigda 1996
Nesheiwat and Swanson, 2000
Mosteo et al. 2007 Venkatadri
and Peters, 1993
(1) Enhances decomposition of H2O2 (1) UV consume more energy Ashraf et al. 2006
(2) Reducing the generation of waste iron (2) Impact factors is increased, Bigda 1995
(3) Improved the efficiency of mercury reaction is instability Adewuyi 2005
removal
(1) No solid waste (1) UV consume more energy Liu and Wang, 2014
(2) The reaction condition is easy to control (2) The effectiveness is lower Liu and Wang, 2014
than photo-Fenton solution Bokare and Choi, 2009
(1) Ways to generate ·OH is increased by (1) Consume more energy Kang et al. 2002Han et al. 2007
the reaction of water and O2 (2) Experimental conditions
(2) Fe2+ catalyst is easily regenerated is complex
(1) Enhances decomposition of H2O2 (1) For some metals, the cost is high Wen et al. 2011
(2) Generate less solid waste (2) For some metals, it will Chen et al. 2012
produce more sludge Nidheesh et al. 2013
Watts et al. 2005
Zhao et al. 2006
Rodriguez-Perez et al. 2013
26319
26320
exhibit multiple oxidation states and can be easily regenerated
from an inactive form through a simple redox cycle (Bokare
and Choi, 2009). Many metals have been used as catalysts,
such as aluminum (Al), cerium (Ce), chromium (Cr), and
manganese (Mn). Among the researched metals, Ce shows
an excellent catalytic performance in non-ferrous Fenton so-
lution (Heckert et al. 2008; Mamontov et al. 2000; Wang et al.
2014a).
Cerium (Ce) is a rare earth element which can exhibit both
+ 3 and + 4 oxidation states in solution (Heckert et al. 2008).
CeO2 is widely used in wet oxidation for the presence of
oxygen vacancies which can enhance the catalytic activity
(Mamontov et al. 2000). Wang et al. 2014a) reports that the
pretreatment of CeO2 by sulfation can improve the catalytic
activity of CeO2/H2O2 system. Electron transfer from Ce3+ is
initiated under the function of the protonation of peroxide
species in the presence of sulfate groups, which acts as acidic
sites (Wang et al. 2014a; Ji et al. 2010). The reaction principle
is shown in Fig. 7. Moreover, it will enhance the decomposi-
tion of H2O2 and the removal efficiency of Hg0 will be im-
proved. When the amount of catalyst exceeds the optimal
concentration for H2O2 decomposition, removal rate of Hg0
will not change (Hua et al. 2010; Wen et al. 2011; Chen et al.
2012; Nidheesh et al. 2013; Bautista et al. 2008; Bigda 1995,
1996; Nesheiwat and Swanson, 2000; Mosteo et al. 2007).
In Table 5, some H2O2-based advanced oxidation process-
es (AOP), their individual characteristic, and fundamentals of
solutions are all summarized in detail. From Table 5, it can be
found that the key point of Hg0 removal by H2O2 system is to
enhance the decomposition of H2O2 and produce ·OH with
suitable concentrations, which can be greatly influenced by
both amount and recycling of the catalyst used in H2O2 system
(Chen et al. 2012). Though ultraviolet light can achieve a good
result, the cost on energy for generating ultraviolet is too high.
Moreover, the ultraviolet is harmful to the health of workers
and related setups. Therefore, it is still hard work to find a
suitable method to catalyze the decomposition of H2O2 and
the most desirable method should be economic and technical-
ly feasible; meanwhile, there is no secondary pollution gener-
ation (Mosteo et al. 2007; Venkatadri and Peters, 1993;
Adewuyi 2005; Bokare and Choi, 2009; Han et al. 2007;
Watts et al. 2005; Zhao et al. 2006; Rodriguez-Perez et al.
2013; Wu et al. 2008).
Conclusions
Purifying Hg0 from coal-fired flue gas has been one of the
most important environmental issues worldwide in the
twenty-first century. Up to now, there is no established tech-
nology which is suitable for large-scale applications for re-
moving Hg0 from flue gas. The method of wet flue gas desul-
furization is a new idea to remove Hg0, and the Fenton
Environ Sci Pollut Res (2017) 24:26310–26323
solution is found to be superior to the others oxidants for
removing Hg0 from flue gas in industrial applications. This
technology has obvious advantages in simultaneously purify-
ing multi-pollutants such as SO2, NOx, and Hg0, and can be
widely used for its high pollutant removal efficiency and low
energy consumption. Engineering applications only need to
improve the equipment on the basis of the original, which
can save a lot of investment costs. Meanwhile, HCl in flue
gas has clear auxo-action on the oxidation and purification of
Hg0 and it can effectively enhance the efficiency of mercury
removal especially when the chloride ion concentration is
controlled in a reasonable range in the flue gas. In the future,
the further study is suggested focus on the increasing of the
removal efficiency of multi-pollutants and lowing its cost.
Finally, the reduction of Hg2+ should be avoided as much as
possible when Hg0 is oxidized and purified from flue gas, and
it is another related important research field on purifying Hg0.
Funding This work was supported by the Joint Funds of the
National Natural Science Foundation of China (Grant No.
U1560110), the National Key R&D Program of China (No.
2017YFC0210301), Funds of Beijing Science and
Technology (D161100004516001), and Fundamental
Research Funds for the Central Universities.
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