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Abstract
To evaluate trace element emissions from modern coal-fired power plants into the atmospheric environment in Japan, trace
elements in the coal used in electric utility boilers, stack concentrations, emission rates and emission ratios of coal-fired power plants,
and proportions of trace elements in coal-fired power plants were studied. The elements were As, B, Be, Cd, Co, Cr, F, Hg, Mn, Ni, Pb,
Sb, Se and V, which are designated in the Law of Pollutant Release and Transfer Register. The particulate trace elements were
collected in an electrostatic precipitator and a wet desulfurization scrubber. Emissions into the atmosphere were lower than 1% of the
quantity in coal, but the volatile trace elements showed somewhat higher emission ratios. For mercury, the mean concentration in coal
was 0.045 ppm, the mean emission rate was 4.4 Ag/kW h, and the mean emission ratio was 27%, the highest ratio among all elements
in this study. The total annual emission of mercury from coal-fired power plants of the electric power industry in Japan was estimated
to be 0.63 t/y. On the basis of these data, the atmospheric environment loads from a coal-fired power station were investigated. The
calculation of stack gas dispersion showed that maximum annual mean ground level concentrations were in the order of 10 2 to 10 5
of the background concentrations, and that the adverse effect of the emissions from the coal-fired power station was small.
D 2005 Elsevier B.V. All rights reserved.
Keywords: Coal; Power plant; Trace element; Mercury; Emission; Environmental load
NOx PM SOx
FBC+DeNOx 2.4% Others 1.2% None 3.6%
In furnace DeSOx 2.4%
Comb. control 3.1% Wet ESP
7.5% Wet scrubber (MgOH 2)
LNB 13.7% 1.4%
Dry FGD (CaCO 3)
SCR 5.0% Extra cold ESP 0.9%
Cold. ESP
23.1% 51.1%
SCR+LNB Wet scrubber (CaCO 3)
75.7% Hot ESP 91.6%
17.1%
equipped with particulate control, and more than 96% 2. Trace elements in coal
perform FGD mostly using wet scrubbers.
These flue gas treatments are also considered effec- Nowadays all the coal consumed in Japan is
tive for emission control of trace elements, as well as imported. In 2000, 59.9% of the total steam coal was
mercury. The electric power industry in Japan has imported from Australia, 16.2% from China, 13.8%
measured trace element concentrations in the coal from Indonesia, 3.6% from USA, and very small
used in utility boilers and in the stack gases, voluntarily, amount from Canada and South Africa. The amount
to comply with the notification of the Agency of Nat- of import varies year by year, but Australian coal
ural Resources and Energy, or to fulfill agreements with exceeds 50% normally and Chinese and Indonesian
local governments. Recently, the government imple- coals follow it.
mented a new law called the Pollutant Release and The data of trace element concentrations in coal
Transfer Register (PRTR). The PRTR aims to promote were collected from 13 power stations for 81 brands
the voluntary improvement of business in the manage- of coal, most of which were bituminous coal. The
ment of specific chemical substances and to prevent any shipping countries of the coal were Australia (for 41
impediment of environmental protection. Under this brands), USA (13), Canada (3), South Africa (10),
Law, owners of business that deal with chemical sub- China (5), Indonesia (11) and Russia (3). Although
stances in amounts exceeding stipulated values must some brands of coal had plural set of data, individual
calculate the quantity of the substances they release into sets of data were treated independently, since the var-
the environment and notify the government of the iation in data for one brand exceeded the difference
result. As for the trace elements in coal, As, B, Be, between brands in some cases. As shown in Fig. 2, the
Cd, Co, Cr, F, Hg, Mn, Mo, Ni, Pb, Sb, Se and V have data seem to approximately follow the lognormal dis-
been designated in the PRTR. The amounts of those tribution. In the case of the lognormal distribution, the
elements treated in a coal-fired power plant were lower geometric mean is generally selected as the represen-
than the reference quantities that the PRTR requires to tative quantity. However, it is lower than the arithmetic
be reported. However, CRIEPI collected the data on mean and may cause underestimation when estimating
these elements from 10 electric utility companies and the total amount. Therefore Table 1 shows the arith-
the Electric Power Development Company (EPDC), metic means of the data as the representative values.
and analyzed the emissions into the atmosphere, except For mercury, the total number of datums was 181 and
for Mo for which the amount of data was very small. the arithmetic mean was 0.045 mg/kg. Some coal
The data of trace element concentrations in coal and brands of China and South Africa showed higher
stack gases were obtained from modern coal-fired mercury concentrations with the maximum concentra-
power plants, all of which employed ESPs and wet tion of 0.21 mg/kg observed in this study. The con-
FGD using lime slurry; all but one employed SCR. centration in coal may be rather affected by the degree
Using these emission data, the effect of coal-fired of coal cleaning and the product lot. The data of a
power station emissions on the local atmospheric envi- brand was limited and the variation in data for a brand
ronment was also investigated. Based on the calculation was sometimes higher than the difference between
of stack gas dispersion, the ground level concentrations brands, it was not possible to find the correlation
of trace elements due to diffusion were estimated and between mercury concentration distributions and the
compared with the background concentrations. coal origin.
S. Ito et al. / Science of the Total Environment 368 (2006) 397–402 399
40 30 20 40
Cumulative (%)
Cumulative (%)
Cumulative (%)
Cumulative (%)
60% 60% 60% 60%
25
30 50% 50% 15 50% 30 50%
20
40% 40% 40% 40%
20 15 10 20
30% 30% 30% 30%
10 20%
20% 20% 20%
10 5 10
10% 5 10% 10% 10%
0 0% 0 0% 0 0% 0 0%
-3 -2
-1
-1
0
0
1
1
2
2
310
3
10
-1
-1
010
0
10
1
1
102
2
10
3
3
-1 -1
010 0 11 22 3 3 -3
10 -2
10 -110 -1 010 0 110 1
10 10 10 10 10 10 10 10
Concentration [mg/kg-dry] Concentration [mg/kg-dry] Concentration [mg/kg-dry] Concentration [mg/kg-dry]
10 40 40
Cumulative (%)
Cumulative (%)
Cumulative (%)
Cumulative (%)
60% 60% 50 60%
60%
Cumulative (%)
Cumulative (%)
Cumulative (%)
Cumulative (%)
10 50
60% 12 60% 60% 60%
0 0% 0 0% 0 0% 0 0%
-1 0 1 2 3 -1 0 1 2 3 -1 0 1 2 3 -2 -1 0 1 2
-1
10 010 1
10 2
10 3
10 -1
10 010 1
10 2
10 3
10 -1
10 0
10 1
10 2
10 3
10 -210 -110 010 110 210
Concentration [mg/kg-dry] Concentration [mg/kg-dry] Concentration [mg/kg-dry] Concentration [mg/kg-dry]
40 100% 40 100%
90% 90%
35 35
Se V
80% 80%
30 30
70% 70%
Number of datums [-]
Cumulative (%)
Cumulative (%)
25 25
60% 60%
20 50% 20 50%
40% 40%
15 15
30% 30%
10 10
20% 20%
5 5
10% 10%
0 0% 0 0%
-2 -1 0 1 2 -1 0 1 2 3
10
-2 10
-1 10
0 10
1 10
2 -1
10 010 1
10 2
10 3
10
Concentration [mg/kg-dry] Concentration [mg/kg-dry]
Fig. 2. Trace element concentrations in coal used in coal-fired power plants in Japan.
Clarke and Sloss (1992) and Davidson and Clarke lands and gave 0.11 mg/kg as the mean concentration
(1996) showed the typical concentrations and the with the range 0.02 to 1.8 mg/kg. Kilgroe et al.
concentration range of trace elements in coal. Accord- (2002) summarized the mercury content in coal used
ing to them, the typical concentration of mercury was in coal-fired utility electric boilers in the US and
0.1 mg/kg and its range was from 0.02 to 1 mg/kg. showed that the mean concentration in bituminous
Meij et al. (2001) studied the content of mercury in coal was 0.11 mg /kg and the range was from 0.0
coal used in coal-fired power plants in the Nether- to 1.3 mg/kg.
400 S. Ito et al. / Science of the Total Environment 368 (2006) 397–402
Table 3
Proportions of trace elements in coal-fired power plant (%, 3 plants of 2 stations)
Clinka ESP FGDa Stack Total Number of datums
FGD (Gypsum and sludge) (Waste water)
As 1.9 67.2 4.3 4.26 0.02 1.6 75.0 9
Be 7.6 63.7 1.6 1.48 0.12 0.54 73.4 9
Cd 1.8 69.7 16.3 15.73 0.54 1.4 89.2 9
Cr 8.2 58.7 1.9 1.91 0.03 1.2 70.1 9
F 0.37 7.2 67.1 63.64 3.4 13.1 87.7 9
Hg 0.18 51.7 21.9 21.78 0.15 27.6 101.4 9
Ni 9.9 80.6 1.6 1.50 0.05 0.08 92.1 7
Pb 2.8 79.7 5.5 5.47 0.01 1.2 89.2 9
Sb 14.0 69.8 5.0 4.79 0.23 0.06 88.8 2
V 8.5 63.2 2.5 2.45 0.05 0.61 74.8 9
B, Co, Mn and Se were eliminated since mass balances were insufficient.
a
Wet scrubber. The numerical figure of FGD is the sum of (gypsum and sludge) and (waste water).
plant configurations and operation conditions are pos- proportions and the total values are distributed around
sibly the major factors affecting the emission character- 100%. To show the errors in mass balance, proportions
istics. However, they could not be discussed here are not corrected to total 100%. Mercury evaporated
because of the incompleteness of the data set. almost completely in the boiler and did not remain in
Meij et al. (2001) reported 3 Ag/m3N for the mean the clinker ash. When the temperature was decreased,
stack concentration of mercury in Dutch coal-fired some mercury attached to fly ash particles and was
power plants with high efficiency ESPs and wet FGD. collected in the ESP. Some gaseous mercury was cap-
Kilgroe et al. (2002) showed various sets of data from tured by FGD and was finally fixed in the gypsum and
different kinds of US coal-fired power plants. The stack sludge, with a very small quantity in the waste water.
concentration in Table 2 is lower than many of their The stack gas contained approximately one quarter of
values but the mean emission ratio is almost the same as the mercury in coal. Fluorine was also evaporated al-
the value of 25% reported by Meij et al. (2001). Kilgroe most completely in the boiler. A small amount of fluo-
et al. (2002) also obtained 25% for the pulverized coal rine adhered to fly ash particles and the remainder was
boilers with cold side ESPs and wet FDG using bitumi- removed by wet FGD. Arsenic and lead are volatile at
nous coal. The difference among stack gas concentra- high temperatures, but were captured on fly ash particles
tions was probably due to the use of high quality coal in upstream of the ESP. Other elements existed in fly ash
the Japanese electric power industry. On the basis of the particles and were also collected in the ESP.
emission rate, the total annual emission from the coal-
fired power plants of the Japanese electric power indus- 4. Atmospheric environment loads of trace elements
try was estimated to be 0.63 t/y in 2000 with some from a coal-fired power station
degree of uncertainty. This quantity is less than the
emissions in many other countries, e.g., 72.9 t from To evaluate the effect of emissions during coal-fired
coal-fired power plants in China reported by Wang et power generation on the local atmospheric environ-
al. (2000), emission amounts from EU energy industries ment, stack gas dispersion was calculated for a hypo-
reported in the Position paper (2001), and 48 t from US thetical coal-fired power station consisting of two 1000
coal-fired power plants reported by Kilgroe et al. (2002). MW plants. Table 4 shows the operation conditions of
this plant. The calculation was performed using the
3.2. Proportions of trace elements
Table 4
Specifications of hypothetical coal-fired power station
The proportions of trace elements in coal-fired power
plants are shown in Table 3. These values are the means Output 1000 MW 2
Coal consumption 360 t/h 2
of a limited amount of data which varied depending on Height of stack 200 m
factors such as the plant type and the type of coal. The Stack gas temperature 90 8C
values in the table do not represent the average for coal- Discharge velocity 30 m/s
fired power plants in Japan, but show the general trends. Volume flow rate (wet) 3,400,000 m3N/h 2
The value in the column under bTotalQ is the sum of Availability factor (annual) 83.9% (305 days/year)
402 S. Ito et al. / Science of the Total Environment 368 (2006) 397–402
Cr 1.41 10 3
7.4#1 1.9 10 4 of annual emissions were investigated.
F 1.87 NA – The concentrations in coal used in electric utility
Hg 3.71 10 3
2.6#1 1.4 10 3
coal-fired boilers in Japan were equal to or lower than
3
Mn 3.25 10 34#1 9.6 10 5
the typical concentrations generally reported, probably
4
Ni 8.57 10 6.4#1 1.3 10 4
due to the use of high quality coal. The concentrations
3
Pb 3.02 10 51#2 5.9 10 5
Sb 1.59 10 4
6.6#2 2.4 10 5 in stack gases and the emission ratio were also equal to
Se 1.10 10 2
1.1#2 9.8 10 3 or lower than the data reported from other countries.
V 5.73 10 3
4.6#2 1.2 10 3
The use of air pollution control facilities in addition to
#1: Local public entities in 2000, #2: National Atmospheric Monitor- the use of high quality coal are thought to be effective
ing Stations in 1996. for reducing trace element emissions.
As to the proportion of trace elements in coal-fired
plume and puff model specified in the manual of total power plants, the particulate trace elements were col-
pollutant load control for nitrogen oxides by the Min- lected in an ESP and by wet FGD, and the emission
istry of the Environment in Japan. Since the diameter ratio was lower than 1%. To remove volatile elements,
and density of particulates were not well known, the wet FGD is effective, but these elements showed some-
effect of gravitational sedimentation, and the amounts what higher emission ratios than did the particulate
of dry and wet depositions were not considered. In a elements. Mercury had the highest emission ratio
modern coal-fired power plant, the average particle size among the trace elements in this study, with a fraction
in the stack gas is often of the scale of sub-micrometer of about 27%.
to approximately a few micrometers. Hence the effect The calculation of stack gas dispersion yielded the
of sedimentation is expected to be small. To obtain the ground level concentrations of the trace elements emit-
ground level concentrations, the dilution factor was ted from a hypothetical power station. The impact on
calculated and multiplied with the stack gas concentra- the local atmospheric environment of emissions from
tions calculated using the emission rates in Table 2 and the coal-fired power station was found to be small since
the volume flow rate of flue gas in Table 4. In the the maximum ground level concentrations of trace ele-
calculation we used meteorological data and geograph- ments emitted from the station were much lower than
ical data of an actual coal-fired power station where the the background concentrations.
calculated maximum ground level concentration was
higher than those of other stations.
References
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background concentrations in Japan. The background tion and gasification, IEACR/49. IEA Coal Research; 1992.
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local public entities in 2000 or at National Atmospheric Coal Research; 1996.
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loe SA. Control of mercury emissions from coal-fired electric
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