Fuel Processing Technology 125 (2014) 217222

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Fuel Processing Technology

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

Mercury emission characteristics from coal combustion by supplying

oxygen and carbon dioxide with limestone injection
Ha-Na Jang a, Jeong-Hun Kim b, Seung-Jae Jung a, Seung-Ki Back a, Jin-Ho Sung a, Seong-Heon Kim a,
Yong-Chil Seo a,, Sang-In Keel c, Xiaowei Liu d
a

Dept. of Environmental Engineering, Yonsei University, Wonju 220-710, Republic of Korea

Air Quality Research Division, National Institute of Environmental Research, Inchon 404-708, Republic of Korea
Environment & Energy System Research Division, Korea Institute of Machinery and Materials, Daejeon 305-343, Republic of Korea
d
State Key Labaratory of Coal Combustion, Huazhong University of Science and Technology, Wuhan 430074, China
b
c

a r t i c l e

i n f o

Article history:
Received 1 December 2013
Received in revised form 2 April 2014
Accepted 5 April 2014
Available online 3 May 2014
Keywords:
Particulate mercury
Oxidized mercury
Sulfur dioxide
Limestone injection
Desulfurization
Oxy-fuel combustion

a b s t r a c t
Coal combustion experiments at a lab-scale furnace with a capacity of 10,000 kcal/h were conducted in order to
investigate the speciation changes and mass distribution of mercury with limestone injection in conditions of air
and oxy-fuel combustion. Mass distribution and concentration of mercury in ue gas at oxy-fuel combustion
were higher than those at air combustion. With limestone injection, the reduction of mercury from ue gas by
adsorption into limestone could be clearly observed at both air and oxy-fuel combustion conditions. In the speciation of mercury, the particulate mercury in ue-gas was dominant with around 50% and the portion of elemental mercury was higher than that of oxidized mercury as shown at other coal combustion cases. At oxy-fuel
combustion, most of particulate mercury seemed to be bounded to limestone more easily in comparison to air
combustion, so that the elemental mercury in ue gas resulted to be more dominant at oxy-fuel combustion.
2014 Elsevier B.V. All rights reserved.

1. Introduction
In oxy-fuel combustion which fuel is combusted at O2 and CO2 supplying condition, the emission trend of pollutants in the ue gas should
be different than in the conventional air combustion. In the conventional
air combustion, the ue-gas from the coal-red power plants includes
various air pollutants such as ne particulate, toxic trace metals, mercury
compounds, sulfur oxides, and nitrous oxides. Linak et al. [13] have reported several studies on the chemical properties of the ne particulates
formed in the coal combustion process. According to Linak et al., ne particulate are thought to originate from metal vapor at high combustion
temperatures and they are formed via nucleation, condensation, and coagulation processes. The coal combustion resulted in ne particulate
emissions which were primarily enriched by trace metals such as mercury. The temperature of the furnace and the residence time were the controlling factors and the particle size distribution depended on the
interaction between the chemical reactions, nucleation, condensation,
and coagulation [4]. Coal power plants release ne particulate enriched
by trace metals such as mercury due to the limited removal efciency

Corresponding author. Tel.: +82 10 5373 2114; fax: +82 33 760 2571.
E-mail address: seoyc@yonsei.ac.kr (Y.-C. Seo).

http://dx.doi.org/10.1016/j.fuproc.2014.04.003
0378-3820/ 2014 Elsevier B.V. All rights reserved.

of the existing air pollutants control devices for these ne particulates

[5]. Mercury can exist as elemental mercury (Hg0), oxidized mercury
(Hg2+) and particulate mercury (Hgp). Once in the air, mercury can be
widely dispersed and transported thousands of miles from the emission
sources. Mercury undergoes a series of complex chemical and physical
transformations as it cycles among the atmosphere, land, and water [6,
7]. Lee et al. [8] investigated the speciation and mass distribution of mercury at bituminous coal-red power plant. The facility was equipped with
an electrostatic precipitator (ESP) and a wet ue gas desulfurization
(FGD) as air pollution control devices (APCD). According to this study, elemental mercury was dominant at the outlet of FGD because oxidized
mercury was primarily absorbed in the lime/limestone solution due to
the solubility of oxidized mercury in water. Pudasainee and Kim et al.
[912] compared the variation of mercury emission and speciation in
APCD at various coal power plants in Korea. Those plants were equipped
with selective catalytic reactor (SCR), ESP, and FGD and the conguration
was different at each coal power plant. The removal efciency of mercury
was different at each coal power plant and depends on the conguration
of APCD. The removal of mercury increased at the facility equipped with
SCR, ESP, and wet FGD because the oxidization of elemental mercury by
SCR enhanced the removal of oxidized mercury in the downstream of
wet FGD. Researchers have proposed the use of several sorbent materials
such as limestone for metal control. Owens et al. [13] performed

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H.-N. Jang et al. / Fuel Processing Technology 125 (2014) 217222

equilibrium calculations for a number of toxic metal species reacting with

sorbents in order to establish the relative efciencies. For a specic sorbent and toxic metal, there is a temperature range over which it is most
effective. Wu et al. [14] extended their earlier studies to the development
of a multifunctional sorbent for the capture of sulfur dioxide, alkali
metals, and lead. This aluminosilicate sorbent was effective in the simultaneous removal of the species and no loss of activity was observed due to
competitive reactions. Zheng et al. [15] concluded that the coal oxy-fuel
combustion had an effect on the amount and type of trace metals such
as mercury emissions in the vapor phase. These ne particulate and
trace metals such as mercury from oxy-fuel combustion would be
difcult to capture by the APCD of the conventional coal power plant.
Therefore, it would be necessary to gure out the emission trend of ne
particulate and trace metals such as mercury from the oxy-fuel combustion. In this study, the speciation of the mercury compound was predicted
both in the conditions of conventional air combustion and in the conditions of oxy-fuel combustion by a chemical equilibrium and applications
(CEA) simulation code. Also, a lab-scale furnace experiment was carried
out in order to compare the emission characteristics of mercury in the
conditions of oxy-fuel combustion with that of conventional air combustion with limestone injection. The mass distribution and speciation of
mercury in the ue-gas, y ash and bottom ash were investigated in
order to compare the transformation characteristics of mercury in the
conditions of oxy-fuel combustion with those of air combustion with
limestone injection.
2. Experimental methods
The experiments were conducted in a 10,000 kcal/h oxy-fuel combustion reactor, which based on the low-heating value of coal-fuel.
Fig. 1 shows the schematic diagram of the lab-scale consisting of an air
and gas supply, a coal feeding, a control box, two combustion chambers,
a heat exchanger and a bag lter. The air and oxy-fuel combustion
experiments were conducted by using the bituminous coal as fuel. The
basic characteristics of the coal fuel are presented in Table 1. With coal
elemental analysis, CEA code simulation was conducted in order to
predict the speciation of mercury such as elemental mercury (Hg0)
and oxidized mercury (Hg2 +) in the ue gas from air and oxy-fuel

Table 1
Basic characteristics of coal fuel in lab-scale experiment.
Low heating value, kcal/kg
Proximate
analysis (%)
Elemental
analysis (%)

Volatile
Fixed carbon
Ash
C
H
N
S
O

5966
35.5
56.7
7.7
76.5
4.6
0.2
0.170.3
18.4

Major element
composition
(wt.%)

Al
K
Ca
Ni
Zn
Ni
Hg
Cl

1.113
0.085
0.861
0.002
0.001
0.002
0.046E04
0.7

combustion. Comparative studies of coal combustion in air and oxyfuel combustion were carried out with the stoichiometric ratio of
1.265 and 1.165, respectively. The limestone injection to the furnace
was conducted in the conditions of air and oxy-fuel combustion for
the desulfurization test. Sampling points of gaseous, bottom ash and
y ash were presented in Fig. 1. The combustion temperature in the
lab-scale furnace was approximately 900 C. The experimental conditions are summarized in Table 2. The mercury sampling in the ue-gas
and the analysis were conducted in the outlet of the combustor by the
Ontario Hydro Method ASTM D6784 [16]. The Ontario Hydro Method
was developed in order to measure elemental mercury, oxidized mercury, particulate mercury, and total mercury from combustion sources.
Solid samples were pre-treated by US EPA Method 7470A [17]. A cold
vapor atomic absorption spectroscopy (CVAAs) mercury analyzer (RA915+, LUMEX) was used to determine the mercury speciation in the
ue-gas and the mass distribution in the gaseous and solid samples
such as the bottom ash and y ash.
3. Results and discussion
3.1. Desulfurization process and mercury transformation
The essential problem with ue gas desulphurization (FGD) from
coal combustion is its inefciency. Limestone is typically used to capture

Fig. 1. Schematic diagram of experimental oxy-fuel combustion facility.

H.-N. Jang et al. / Fuel Processing Technology 125 (2014) 217222

219

Table 2
Summary of experimental condition and ue-gas emissions.
Parameters

Air combustion

Oxy-fuel combustion

Mixing ratio by volume

Coal feeding (g/min)
Limestone injection (CaCO3g/min)
Air to fuel ratio (A/F)
Combustion temp (C)
Sampling point temp (C)
Gas ow rate (Sm3/h)
Operation time (hr)

Air (21% O2, 79% N2)

26
1.78
1.265
900
6070
11.57
3.844.2

27% O2, 73% CO2

26
1.78
1.165
900
7480
7.66
3.66

Flue-gas analysis

w/o limestone

w/ limestone

w/o limestone

w/ limestone

CO2 (%)
O2 (%)
SO2 (ppm)

14.8 to 17.2
4.23 to 6.23
190 to 290

15.1 to 16.6
4.52 to 6.03
70 to 140

91.7 to 93.2
5.28 to 7.27
230 to 310

92.1 to 93.2
5.30 to 6.78
70 to 120

w/o limestone: without limestone injection.

w/ limestone: with limestone injection.

SO2 which is normally described by the following two-step overall

process [18]:
CaCO3S CaOs CO2g
H 182:1 KJ=mol;

CaOS SO2g 1=2O2g CaSO4s

H 481:4 KJ=mol:

The stable form of the chloride at a high combustion temperature is

HCl. With the cooling of the gases, the diatomic and molecular form of
the chloride becomes stable according to the Deacon type of reaction
as follows [19,20]:
4HCl O2 2H2 O 2Cl2 :

of the air combustion at the temperature of 900 K and the elemental

mercury from oxy-fuel combustion was higher than that of the air combustion at the temperature of 1100 K. The dominant species below 900 K,
which is the boiler outlet temperature, is predicted to be the HgCl2 in
both the conditions of air and oxy-fuel combustion.

3.3. Mass distribution of total mercury in the process

Table 3 shows the mass distribution of the total mercury in the bottom ash, y ash and ue-gas. As shown in the table, the concentration
of the total mercury from air combustion was 0.87 and 1.16 g/h in the
bottom ash, 27.68 and 33.61 g/h in the y ash, and 8.13 and 3.86 g/h
in the ue-gas without limestone injection and with limestone injection,

Hg0 in fuel reacts with Cl species to form Hg2+ in Eqs. (4)(7). Sulfur
in fuel and SO2 in ue gas have been reported to promote Hg2+ and
decrease Hg0 formation as follows [21,22]:
Hg ClHgCl

HgCl Cl2 HgCl2 Cl

Hg Cl2 HgCl2

2Hg 4HCl O2 2HgCl2 2H2 O

HgCl2 g SO2 g O2 gHgSO4 s Cl2 g:

3.2. Mercury species prediction by CEA code

Fig. 2 illustrates the equilibrium distribution of mercury species in the
conditions of air and oxy-fuel combustion as a function of temperature
when CaO and SO2 are not included in the calculation. The CEA simulation code was used in order to predict the mercury compound speciation,
and more importantly, the fractions of the vapor-phase species as a function of the temperature. In the conditions of air combustion, HgCl2 was
dominant as the oxidized mercury below the temperature of 900 K and
elemental mercury was dominant above the temperature of 1100 K.
Also, other oxidized mercury speciation such as HgCl and HgO was predicted in the range of low concentrations. In the conditions of oxy-fuel
combustion, the speciation of the mercury compounds in the ue gas
was similar with that of the conditions of air combustion. The oxidized
mercury concentration from oxy-fuel combustion was higher than that

Fig. 2. (a). Speciation of mercury from air combustion. (b). Speciation of mercury from
oxy-fuel combustion.

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Table 3
Mass distribution of mercury with and without limestone injection [unit: g/h].
ID

Bottom ash
Fly ash (BF)
Gaseous

Air-combustion

Oxy-fuel combustion

w/o limestone

w/ limestone

w/o limestone

w/ limestone

0.87
27.68
8.13

1.16
33.61
3.86

0.69
26.05
12.84

1.23
36.27
5.19

w/o limestone: without limestone injection.

w/ limestone: with limestone injection.
BF: bag lter.

respectively. In the case of oxy-fuel combustion, the concentration of

mercury was 0.69 and 1.23 g/h in bottom ash, 26.05 and 36.27 g/h in
the y ash, and 12.84 and 5.19 g/h in the ue-gas without limestone injection and with limestone injection, respectively. Fig. 3(a) shows the
mass concentration of total mercury from air and oxy-fuel combustion
with and without limestone injections. As shown in the gure, the gaseous mercury from the oxy-fuel combustion was relatively higher than
that from the air combustion. The concentration of mercury in y ash
from oxy-fuel combustion was higher than that from air combustion in
the case of limestone injection. Fig. 3(b) shows the mass distribution of
the total mercury from the air and oxy-fuel combustion with limestone
injection and without limestone injection. As shown in the gure, the
gaseous mercury from the oxy-fuel combustion was relatively higher
than that from the air combustion. It was assumed that the ue-gas
emission from the oxy-fuel combustion was relatively lower than that
of the air combustion and the mercury concentration in the ue-gas
was evaluated as accelerate concentration in the outlet. In the mass distribution of mercury in the y ash, the concentration of mercury from the
oxy-fuel combustion more rapidly increased than that from the air combustion in the case of limestone injection. In the mass distribution of

Fig. 3. (a). Mass concentration of mercury from air and oxy-fuel combustion with and
without limestone injection. (b). Mass distribution of mercury from air and oxy-fuel
combustion with and without limestone injection.

mercury in the bottom ash, the concentration of the total mercury was
relatively lower than that of the y ash and gases. It was considered
that the gaseous mercury was adsorbed, reacted with the limestone injection, and was captured as y ash by the bag lter as temperature
was decreased after heat exchange. Also, the particulate formation of
mercury from the oxy-fuel combustion was more activated than that
from the air combustion after heat exchange in the case of limestone
injection.
3.4. Mercury speciation and distribution in ue-gas
Table 4 shows the average concentration of each mercury compound in the ue-gas from air and oxy-fuel combustion at the outlet
of the combustion chamber in the case of without limestone injection
and with limestone injection. The speciation of the mercury compound
was determined as the particulate mercury, the elemental mercury, the
oxidized mercury, and the total mercury. As shown in Table 4, the concentrations of total mercury from air combustion were 0.703 g/Sm3
and 0.334 g/Sm3 on average without limestone injection and with
limestone injection, respectively. In the conditions of oxy-fuel combustion, the concentrations of total mercury were 1.677 g/Sm3 and
0.678 g/Sm3 on average without limestone injection and with limestone injection, respectively. The mercury speciation from air combustion was determined to be 0.370 g/Sm3 and 0.103 g/Sm3 as the
particulate mercury, 0.280 g/Sm3 and 0.132 g/Sm3 as the elemental
mercury, and 0.054 g/Sm3 and 0.099 g/Sm3 as the oxidized mercury
without limestone injection and with limestone injection, respectively.
In the oxy-fuel combustion, the speciation of the mercury was
determined to be 0.864 g/Sm3 and 0.109 g/Sm3 as particulate
mercury, 0.778 g/Sm3 and 0.553 g/Sm3 as elemental mercury, and
0.036 g/Sm3 and 0.016 g/Sm3 as oxidized mercury without limestone
injection and with limestone injection, respectively. The baseline
testing of the air combustion indicated that 52%, 40%, and 8% on average
of the total mercury in the ue gas was present as particulate mercury,
elemental mercury, and oxidized mercury, respectively. In comparison,
mercury speciation in the ue gas with limestone injection was 31% as
particulate mercury, 39% as elemental mercury, and 30% as oxidized
mercury. On the other hand, the baseline testing of the oxy-fuel combustion indicated that 52%, 46%, and 2% on average of the total mercury
in the ue gas were present as particulate mercury, elemental mercury,
and oxidized mercury, respectively. In comparison, mercury speciation
with limestone injection in the ue gas in oxy-fuel combustion was 16%
as particulate mercury, 82% as elemental mercury, and 2% as oxidized
mercury. Fig. 4 presents the speciation and fraction of the mercury compounds in the case of without limestone injection and in the case of
with limestone injection from air combustion and oxy-fuel combustion.
As shown in Fig. 4(a), the concentration of total mercury from the oxyfuel combustion was higher than that of the air combustion in both
cases. It was considered that the transformation mechanism of mercury
between air and oxy-fuel combustion should be different because the
boiler outlet temperature from oxy-fuel combustion was relatively
higher than that of air combustion. In the case of the speciation of the
mercury compounds in air and oxy-fuel combustion, the elemental
mercury was more dominant than the oxidized mercury in the case of
with limestone injection in the oxy-fuel combustion conditions. Also,
in the case of with limestone injection, the concentrations of the total
mercury decreased in the air and oxy-fuel combustion and the concentration of particulate mercury from oxy-fuel combustion was more rapidly decreased than that of air combustion. In the CEA prediction, the
oxidized mercury was more dominant than the elemental mercury
below the temperature of 900 K in contrast to the experimental results.
It was considered that most of oxidized mercury, which was dominant
as HgCl2, was more reactive in the condition of oxy-fuel combustion and
transformed into the particulate mercury, which was composed of
HgSO4(s), as the temperature of the ue-gas was rapidly decreased in
the boiler outlet without limestone injection. Also, sulfur dioxide was

H.-N. Jang et al. / Fuel Processing Technology 125 (2014) 217222

221

Table 4
Mercury emission from air and oxy-fuel combustion with and without limestone injection in ue-gas [unit: g/Sm3 (%)].
ID

Mercury speciation

Air-combustion

Hg
Hg0
Hg2+
Total Hg

Oxy-fuel combustion

w/o limestone

w/ limestone

w/o limestone

w/ limestone

0.370 (52.56)
0.280 (39.76)
0.054 (7.68)
0.703 (100)

0.103 (30.74)
0.132 (39.58)
0.099 (29.68)
0.334 (100)

0.864 (51.51)
0.778 (46.38)
0.036 (2.12)
1.677 (100)

0.109 (16.02)
0.553 (81.62)
0.016 (2.36)
0.678 (100)

more reactive with limestone injection in oxy-fuel combustion, and the

fraction of HgSO4(s) as the particulate mercury was more decreased in
the oxy-fuel combustion.
4. Conclusions
The air and oxy-fuel combustion experiments were performed using
a lab-scale furnace with bituminous coal as a fuel. The desulfurization
test was performed by limestone injection to the furnace in both conditions. The CEA code simulation was conducted in order to predict the
speciation of the mercury from the air and oxy-fuel combustion by
the results of the fuel elemental analysis. In the lab-scale furnace experiments, the mercury speciation in the ue-gas from the air and oxy-fuel
combustion was investigated with limestone injection. The mass distribution of total mercury in the bottom ash, the y ash, and the ue-gas at
the air and oxy-fuel combustion conditions was investigated. The
experimental results are summarized below.
1. In the literature review, mercury chlorination, the reaction of Hg0(g)
with HCl(g) or Cl2(g) to form HgCl2(g), is generally considered to be
the dominant mercury transformation mechanism in coal combustion
ue gas. It has been reported that sulfur oxide in the combustion reacts
with oxidized mercury (HgCl2) and generates particulate mercury,
which is HgSO4(s).

2. In the CEA code prediction, it was observed that oxidized mercury

such as HgCl2 was dominant below the temperature of 900 K,
which was the same as the literature review, and the elemental
mercury was dominant above the temperature of 1100 K in both
the conditions of air and oxy-fuel combustion.
3. In the mass distribution of mercury, the mercury concentration in y
ash from the oxy-fuel combustion increased more rapidly than that
from air combustion in case of limestone injection. It was indicated
that the gaseous oxidized mercury was more reacted with the
limestone injected in the conditions of oxy-fuel combustion and
the formation of particulate mercury from the oxy-fuel combustion
was more active than that from the air combustion.
4. In the case of the speciation of the mercury compounds in air and
oxy-fuel combustion, the elemental mercury was more dominant
than the oxidized mercury in the case of oxy-fuel combustion condition with limestone injection. Also, in the case of with limestone
injection, the concentration of total mercury decreased in both air
and oxy-fuel combustion and the concentration of particulate
mercury from the oxy-fuel combustion more rapidly decreased
than that of air combustion. It was considered that most of the
oxidized mercury, which was dominant as HgCl2, was mostly reacted
in the condition of the oxy-fuel combustion and transformed into the
particulate mercury, which was composed of HgSO4(s), as the temperature of the ue-gas rapidly decreased. Also, the sulfur dioxide in
ue-gas was more reactive with limestone injection in oxy-fuel
combustion, and the fraction of HgSO4(s) as the particulate mercury
decreased more in the oxy-fuel combustion.

Acknowledgments
This study was supported by a collaborative research project of the
National Research Foundation Grant (NRF-616-2011-2-D0060). This research was also supported by the R&D project titled the Environmental
Control System Design for 100MW Oxy-PC Power Plant/Development
of Environmental Control Techniques for Pollutants concentrated by
FGR in Oxy-PC Power Plant/Fluidization Combustion Technology of
Sludge and RDF using Mixture of Recirculating Flue-Gas and Oxygen
funded by the Korea Institute of Energy Technology Evaluation and
Planning (KETEP). This work was partially funded by the Korean Ministry
of Environment as the human resource development project for energy
from waste and biomass recycling.
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Fig. 4. (a). Gaseous mercury speciation from air and oxy-fuel combustion with and
without limestone injection. (b). Gaseous mercury distribution from air and oxy-fuel
combustion with and without limestone injection.

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