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ARTICLE IN PRESS

Radiation Physics and Chemistry 71 (2004) 439442

Operational experience of the industrial plant for electron


beam ue gas treatment
Andrzej G. Chmielewskia,b, Janusz Lickic, Andrzej Paweleca,*,
Bogdan Tyminskia, Zbigniew Zimeka
a

Institute of Nuclear Chemistry and Technology, Dorodna 16, 03-195 Warsaw, Poland
Warsaw University of Technology, Faculty of Chemical and Process Engineering, Warynskiego 1, 00-645 Warsaw, Poland
c
Institute of Atomic Energy, 05-400 Otwock-Swierk, Poland

Abstract
Electron beam ue gas treatment technology is one of the most advanced technologies among new generation
processes for air pollution control. The process, which has been developed in Japan, the United States, Germany and
Poland allows simultaneous removal of SO2 and NOx with high efciency and by-product generated can be applied as
fertilizer. Two industrial installations using this technology have been constructed in the world, one in China and the
second in Poland. Other plants are constructed in Japan and China. Chinese installation is mostly SO2 removal oriented
(since the NOx emission limits in China are not imposed up to now), so Polish plant one is as a matter of fact the rst
installation for simultaneous desulfurization and denitrication of ue gases. The plant located in EPS Pomorzany in
Szczecin treats the ue gases emitted from two Benson boilers of 65 MWe and 100 MWth each. The ue gases of
maximum ow of 270 000 N m3/h are irradiated by four accelerators of 700 keV electron energy and 260 kW beam
power each. Description of the plant and the results obtained have been presented in this paper. The plant has been in
operation for more than 2500 h (5500 h including one accelerator set operation). Removal efciencies up to 95% for
SO2 and up to 70% for NOx were achieved. Several thousand tons of the by-product was sold in the form of NPK
fertilizer. Economically, the technology is competitive with the conventional ones.
r 2004 Elsevier Ltd. All rights reserved.
Keywords: Electron beam technology; Flue gas treatment; SO2 removal; NOx removal

1. Introduction
The fossil fuel combustion process involves high
emission of acidic pollutants like SO2 and NOx that
creates a major world environmental problem. In
Poland the biggest sources of pollution are located in
south west region of the country where industrial centers
are located. In spite of this over 45% of the total SO2
and about 70% of NOx pollutants distributed over
Polish territory come from external sources. Poland,
where the energy is generated mainly from pit and
*Corresponding author. Fax: +48-22-811-15-32.
E-mail address: pawelec@orange.ichtj.waw.pl (A. Pawelec).

brown coal, is deeply involved in the reduction of


pollutants emission.
There are several methods of ue gas purication
known, but until now no one (demonstrated in the
industrial scale) was able to remove both SO2 and NOx.
In order to purify the ue gases, two separate installations have to be used. The most common solution
consists of wet ue gas desulfurization (FGD) systems
(Srivastava et al., 2001) combined with selective catalytic
reduction (SCR) for NOx removal. Although the
purication level achieved in such systems is high,
there are still many problems such as wastes generated (gypsum, waste water and spent catalyst), double
costs for both pollutants removal and high space

0969-806X/$ - see front matter r 2004 Elsevier Ltd. All rights reserved.
doi:10.1016/j.radphyschem.2004.03.020

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A.G. Chmielewski et al. / Radiation Physics and Chemistry 71 (2004) 439442

440

requirements that complicates modernization of the


retrot installations.
In the case of electron beam ue gas treatment
method both SO2 and NOx are removed in one dry
process. Moreover, in this process the removal of other
acidic pollutants were HCl and VOC decomposition
takes place (Chmielewski et al., 2002a). In this way, the
ue gas purication proceeds in only one installation,
that simplies the construction and reduce space
requirements, that allows using it in the modernized
plants. Moreover, the total cost of two main pollutants
removal does not exceed the cost of desulfurization in a
conventional installation. The great advantage of this
installation is the lack of wastes. The only by-product
generated in the process is the mixture of ammonium
sulfate and nitrate, that can be used as fertilizer and
sold.
The laboratory facility for electron beam ue gas
treatment was set in Institute of Nuclear Chemistry and
Technology in Warsaw at the end of 80-ties. Soon after
the laboratory trials, the pilot plant has been constructed at the Kawe-czyn Power Station (Chmielewski
et al., 1992). Three new elements have been tested in this
facility: double-stage irradiation, longitudinal irradiation and air curtain under the reaction chamber window.
Also, three different by-product ltration systems have
been tested: bag lters, gravel-bed lter and electrostatic
precipitator. The results of the tests performed in the
laboratory facility and pilot plant allowed the design of
full scale industrial plant.

2. Industrial installation
The rst industrial installation for simultaneous
removal of SO2 and NOx was located in Electropower
Station Pomorzany in Szczecin, north of Poland
(Chmielewski et al., 2001). The installation puries ue
gases from two Benson boilers of 65 MWe and
100 MWth each, the total maximum ow rate is
270 000 N m3/h. With its 1.05 MW total beam power
installed it is the biggest accelerator facility in the world.
The installation consists of four main, separated
systems:
*
*
*
*

ue gas conditioning unit,


ammonia storage and injection unit,
reaction chambers,
by-product collecting and storage unit.

Before entering the installation, the ue gases from


boilers are dedusted in electrostatic precipitators and
divided into two streams. About half of the total ue gas
amount is directed to the installation, while the rest is
bypassed to the mixer before the stack. The puried part
of the gases enters the dry bottom spray cooler, where

the water evaporation process takes place. As a result of


this process the temperature of the gases lowers to 65
80 C and the humidity rises up to 1014% vol. In this
way, the temperature and the humidity of the gases are
correlated with each other to a high degree. If the inlet
ue gas temperature is low, the humidity may be too low
for the proper course of the process. In this case there is
a possibility of increasing this parameter by adding
steam over the gas outlet from the cooling tower.
Ammonia, the main process reagent, is stored as an
ammonia water. It may be dosed to the installation in
two ways
*

gaseous ammonia after the evaporation may be


injected upstream the irradiation chamber (variant I),
ammonia water may be sprayed straight to the spray
cooler using the separate system of nozzles
(variant II).

Ammonia may be also dosed both in the form of


ammonia water to spray cooler and gaseous ammonia
before the irradiation chamber (mixed variant). The
tests carried on the industrial installation showed, that
the way of ammonia adding affects the pollutants
(especially, SO2) removal efciency. Depending on the
process conditions the ammonia water consumption is in
the range of 150600 kg/h.
After the ammonia injection the ue gases are guided
to reaction unit, where the irradiation and main
reactions take part. The reaction unit consists of two
parallel irradiation chambers equipped with two accelerators (260 kW, 700 keV) installed in series . The double
titanium foil window with air curtain was applied
(Chmielewski et al., 1995). In this device the doses in
the range of 712 kGy were used. The energy of
electrons induces the sequence of reactions that effects
in oxidizing of SO2 and NO and creation of ammonium
sulfate and ammonium nitrate aerosol (Person and
Ham, 1988; Namba, 1993; Chmielewski et al., 2002b).
Other acidic pollutants such as HCl are removed by
straight reaction with ammonia.
The by-product aerosol is collected by the electrostatic
precipitator and after granulation and storage is shipped
to the NPK fertilizers production plant. The by-product
consists mainly of ammonium sulfate and ammonium
nitrate. Apart of them occurs ammonium chloride (from
the carbon contained chloride) and other impurities as
ammonium uoride, insoluble parts (residual y ash and
rust) etc. The impurities content (especially heavy
metals) is much lower, than the fertilizers concerning
standards, so the by-product has a very good quality for
the agricultural uses. The by-product yield is up to
300 kg/h.
The ue gases after purication are mixed with the
unpuried part of gases and leaded to the stack. Gas
temperature after mixing exceeds 110 C, what avoids
wet stack problems.

ARTICLE IN PRESS
A.G. Chmielewski et al. / Radiation Physics and Chemistry 71 (2004) 439442

3. Operational experiences

450.0

Removal [mg/Nm ]

400.0

350.0

300.0

250.0
6 kGy
8 kGy
200.0

10 kGy
12 kGy

150.0
300

400

500

600

700

800

900

1000

1100

NOx inlet concentration [mg/Nm ]

Fig. 2. NOx removal vs. inlet NOx concentration (calculated).


Ammonia stoichiometry 0.5.

2000

Removal [mg/Nm ]

1800
1600
1400
1200
1000
800
600
400
200
0
60

65

70

75

80

85

90

Temperature [C]

Fig. 3. SO2 removal efciency vs. dose reaction vessel


temperature.

1800
1600

Removal [mg/Nm3]

The process course and the efciency of pollutants


removal depends on various conditions. The literature
and our earlier investigations (Matzing and Paur, 1992;
Chmielewski et al., 2000) pointed out, that the NOx
removal efciency depends mainly on dose, inlet NOx
concentration and ammonia stoichiometry. In the case
of SO2 removal, temperature impact is crucial due to
radiothermal reactions (Wittig et al., 1988). The rest of
the parameters such as dose, humidity, ammonia
stoichiometry or inlet pollutant concentration play
minor, but not negligible roles. The impact of these
parameters on the SO2 and NOx removal efciency in
the industrial installation was examined.
The industrial installation highest pollutants removal
efciency may reach 95% for SO2 and 70% for NOx
(Fig. 1). Such results were obtained for low temperature
(under 70 C) and high humidity of ue gases. These
results shows good agreement with the trends previously
described in the literature (Matzing and Paur, 1992;
Chmielewski et al., 2000).
In the industrial installation, there were also observed
three main parameters having impact on the NOx
removal effectiveness: the dose, NOx inlet concentration
and ammonia stoichiometry. The empirical model
equations of NOx removal based on the multidimensional regression method was applied. As it was
previously noticed, the dose is the most important
parameter from the NOx removal point of view (Fig. 1).
The inlet concentration of NOx shows less impact on the
process efciency and the correlation is linear. It is
worth to notice, that the total removal (taken in mg/
N m3) increases (Fig. 2), while the relative removal (in
%) decreases with the increase of one of the listed
parameters. The empirical model pointed to the very
little impact of ammonia stoichiometry on the NOx
removal efciency.
In the case of SO2 removal, with no doubt, the
temperature and humidity (closeness to the dew point)
are the most important parameters (Fig. 3). The dose

1400
1200
1000
800
600

SO2
NOx

400
200
0
30.00

40.00

50.00

60.00

70.00

80.00

90.00

100.00

Ammonia stoichiometry [%]

100
90

Fig. 4. SO2 and NOx removal efciency vs. ammonia stoichiometry (observed).

SO2

80
Removal [%]

441

70
60
50

NOx

40
30
20
10
0
5.0

5.5

6.0

6.5

7.0 7.5 8.0


Dose [kGy]

8.5

9.0

9.5

Fig. 1. SO2 and NOx removal efciency vs. dose.

10.0

plays rather moderate role in this process, while opposite


to NOx, the ammonia stoichiometry seems to be
important (Fig. 4). The other factors as ue gas ow
rate or inlet pollutants concentration play minor role
according to the process effectiveness.
High impact of the ammonia injection pathway
(variant I or II) on the SO2 removal efciency was
observed (Fig. 5). Its clear view, that adding at least

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A.G. Chmielewski et al. / Radiation Physics and Chemistry 71 (2004) 439442

442

simplicity, simultaneous pollutants removal possibility,


lack of wastes and economical competitiveness.

100
90

Removal [%]

80
70
60

References

50
40
30
20
10
0
0.00

0.10

0.20

0.30

0.40

0.50

0.60

0.70

0.80

0.90

1.00

Ammonia mass fraction sprayed into cooling tower

Fig. 5. SO2 removal efciency vs. ammonia dosing way.

50% of total ammonia water amount straight to the


cooling tower increases SO2 removal efciency considerably.
The plant was operated for over 3000 h with two
accelerators and then, since June 2002, with set of all
four accelerators for over 2500 h.

4. Conclusions
The industrial electron beam ue gas treatment
installation for simultaneous removal of SO2 and NOx
has been constructed in EPS Pomorzany in Szczecin,
Poland. The installation proved high effectiveness of the
process against the pollutants removal. Among the other
parameters the dose is the most important from the NOx
removal point of view. In the case of SO2 the most
important parameters are temperature, ammonia stoichiometry and the ammonia dosing way. The accelerators of this power were not applied ever before, so
5000 h of their operation in severe industrial conditions
delivered a lot of experience for further technology
implementation.
The radiation ue gas treatment method is one of the
most attractive air pollution control processes due to its

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