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NUKLEONIKA 2010;55(3):271−277 REVIEW PAPER
Introduction
Most the world-wide of energy (88%) is produced by
the combustion of fossil fuels like oil, natural gas and
coal [2]. All of these fuels are composed of major con-
stituents such as carbon, hydrogen and oxygen and other
components including sulfur and nitrogen compounds
and metals. During the combustion process, different
pollutants are emitted such as fly ash (containing diverse
trace elements (heavy metals)), SOx (SO2 and SO3),
NOx (NOx = NO + NO2), Hg and VOCs. Air pollution
caused by particulate matter and other pollutants not
only directly impacts the atmospheric environment but
also contaminates water and soil, leading to their deg-
radation. The exhaust gases released into atmosphere
are irradiated by ultraviolet (UV) sunlight and undergo
photochemical transformations. Wet and dry deposi-
tion of inorganic pollutants leads to acidification of the
environment. These phenomena affect human health,
increase corrosion and destroy crops and forests. VOCs
emissions to the atmosphere can lead to ground level
photochemical ozone formation and can have toxic or
carcinogenic effects on human health.
Among conventional technologies for flue gas
treatment aimed at removal of SO2 and NOx are wet,
dry and semi-dry flue gas desulfurization (FGD) and
selective catalytic reduction (SCR) of NOx. VOCs are
usually adsorbed on active carbon, but this process is
rarely used for lean hydrocarbon concentrations. All
A review on electron beam flue gas
treatment (EBFGT) as a multicomponent
air pollution control technology
Ahmed A. Basfar,
Osama I. Fageeha,
Noushad Kunnummal,
Andrzej G. Chmielewski,
Janusz Licki,
Andrzej Pawelec,
Zbigniew Zimek,
Jerzy Warych
A. A. Basfar
King Abdulaziz City of Science and Technology,
Atomic Energy Research Institute,
Radiation Technology Center,
P. O. Box 6086, Riyadh 11442, Saudi Arabia,
Tel.: +9661 481 3648, Fax: +9661 481 3640,
E-mail: abasfar@kacst.edu.sa
O. I. Fageeha, N. Kunnummal
Environmental Protection Department,
Saudi Arabian Oil Company (SAUDI ARAMCO),
P. O. Box 12772, Dhahran 31311, Saudi Arabia
A. G. Chmielewski
Institute of Nuclear Chemistry and Technology,
16 Dorodna Str., 03-195 Warsaw, Poland
and Faculty of Chemical and Process Engineering,
Warsaw University of Technology,
1 Waryńskiego Str., 00-645 Warsaw, Poland
J. Licki
Institute of Atomic Energy, 05-400 Otwock-Świerk, Poland
A. Pawelec, Z. Zimek
Institute of Nuclear Chemistry and Technology,
16 Dorodna Str., 03-195 Warsaw, Poland
J. Warych
Faculty of Chemical and Process Engineering,
Warsaw University of Technology,
1 Waryńskiego Str., 00-645 Warsaw, Poland
Received: 5 March 2010
Accepted: 31 May 2010
Abstract. Electron beam flue gas treatment (EBFGT) technology for coal-fired boilers has been implemented on an
industrial scale in two thermal power plants in China and at the Electropower Station (EPS) Pomorzany in Poland. The
plants in China have been designed mainly for desulfurization while the plant in Poland for a simultaneous removal of
SO2 and NOx from flue gases. The successful operation of these plants has demonstrated the advantages of using this
technology for removing SO2 and NOx from flue gas under varying conditions. At present, the plant in Poland is the
only operational installation at an international level. Recent tests performed at an EBFGT industrial pilot plant in
Bulgaria have demonstrated feasibility of application of this technology for treatment of high sulfur and high humidity
lignite fired boilers. Further laboratory tests have been performed for model flue gases similar to those emitted from
a copper smelter and flue gases originated from different types of high sulfur heavy fuel oils. In all cases, dry-scrubbing
process with ammonia addition has been tested. The removal efficiency of pollutants is as high as 95% for SO2 and
70–80% for NOx. The by-product of this process is a high quality fertilizer component. Additional laboratory studies
have shown that volatile organic compounds (VOCs) emitted during combustion of fossil fuels, can be degraded as
well. Therefore, EBFGT can be considered as a multicomponent air pollution control technology which can be applied
to flue gases treatment from coal, lignite and heavy fuel oil-fired boilers. Other thermal processes like metallurgy and
municipal waste incinerators are potential candidates for EBFGT technology application.
Key words: fossil fuel combustion • heavy fuel oil • electron beam irradiation • plasma processes • flue gas treatment
• SO2 and NOx removal
272 A. A. Basfar et al.
these technologies are complex chemical processes,
and wastes, like wastewater, gypsum and used catalyst
or adsorber, are generated [20].
EBFGT technology is among the most promising
advanced technologies of new generation. This is a
dry-scrubbing process of simultaneous SO2 and NOx
removal, where no waste, except a by-product, is gen-
erated. The application of electron beam irradiation
to initiate chemical reactions to remove SO2 and NOx
was first investigated by joint research of the Japan
Atomic Energy Research Institute (JAERI) and Ebara
Corporation in the early 1980s. The method has been
developed since then from the laboratory to pilot and a
large demonstration scale by research and development
projects in Japan, USA, Germany, China and Poland
[11]. The final engineering design technology for indus-
trial applications was achieved at pilot plants operating
in Nagoya, Japan [17] and at Kawęczyn, Poland [6]. In
the case of the latter, new engineering solutions were ap-
plied: double-longitudinal gas irradiation, an air curtain
separating the secondary window from corrosive flue
gases and modifications of humidification and ammonia
injection system (high enthalpy water or steam injection,
ammonia water injection) and others. A high irradiation
dose is required for NOx removal, while SO2 is removed
in proper conditions at low energy consumption [6].
Technology status
EBFGT technology for coal-fired boilers has been
implemented on an industrial scale at the Thermal
Power Plants (TPPs) at Chengdu [9] and Hangzhou [16]
in China and at the EPS Pomorzany [4] in Poland. At
present, the EBFGT installation in Poland is the only
operational installation in the world. Table 1 presents
the main parameters of these installations.
The plants in China were designed mainly for SO2
removal, while the plant in Poland was designed for
simultaneous SO2 and NOx removal. The flue gases from
two Benson boilers (65 MW(e) and 100 MW(th) each))
are purified at the EPS Pomorzany in Poland (see Fig. 1).
The maximum flow rate of the gases is 270 000 Nm3
/h
and the total electron beam power is equal to 1 MW.
There are two process vessels over which two electron
accelerators are installed in series (700 keV, 260 kW
each). The applied dose is in the range 7–12 kGy
(kJ/kg). At these doses, the removal efficiency ap-
proaches 85–95% for SO2 and 50–70% for NOx. The
by-product is collected by an electrostatic precipitator
and shipped to a fertilizer plant.
The most often applied conventional technology for
flue gas treatment is a combination of wet FDG and SCR
processes. A comparison of the costs of various emission
Table 1. Main parameters of industrial EB installations
Parameter Unit Chengdu TPP, China Hangzhou TPP, China Pomorzany EPS, Poland
Flue gas flow rate Nm3
/h 300 000 305 400 270 000
Inlet flue gas temperature °C 150 145 140
Inlet SO2 concentration mg/Nm3
5150 2770 2000
Inlet NOx concentration mg/Nm3
820 410 600
SO2 removal efficiency % 80 85 90
NOx removal efficiency % 18 55 70
EB 800 keV, 320 kW×2 800 keV, 320 kW×2 700 keV, 260 kW×4
Fig. 1. Flow diagram of the industrial plant at the EPS Pomorzany, Poland.
273A review on electron beam flue gas treatment (EBFGT) as a multicomponent air pollution...
control methods for a 120 MW(e) unit is presented in
Table 2.
The operation of the EBFGT industrial plants in
China and Poland for the last few years has demon-
strated advantages of using this technology for simul-
taneous removal of SO2 and NOx from flue gas under
varying conditions. EBFGT has to be competitive with
the conventional ones both from economic and techni-
cal point of view. Therefore, any development concern-
ing cost reduction and technological improvements
regarding technical components, especially reliability
of electron accelerator plays a very important role for
further EBFGT process implementation.
Potential applications for industrial off-gases
Combustion of fuel oil
Liquid fuels are used in some limited applications, but
are more prevalent in certain areas of the world such
as South America, central and eastern Canada, north-
eastern USA. No. 2 and no. 6 oils are most commonly
used liquid fuels. Heavy fuel oils (HFO) are a mixture
of hydrocarbons composed of residual fractions from
distillation and processing of crude oil. It is essentially
an industrial fuel that is suitable for use in thermal
power plants, refineries, industrial boilers, pulp and
paper industry, marine applications and metallurgi-
cal operations which generally preheat the fuel oils.
Depending on the source, the sulfur content in the
HFO could be as high as 4.0 wt.%. Sulfur is converted
to sulfur dioxide when oil is burnt. Flue gas emitted
from such heavy fuel oil-fired boiler contains high SO2
and NOx concentrations, many times exceeding the
permissible emission limits, which necessitates the use
of add-on control devices for the reduction of SO2 and
NOx emissions.
A study of EBFGT on flue gas from combustion of
high sulfur heavy fuel oils was performed at the labo-
ratory plant at the Institute of Nuclear Chemistry and
Technology (INCT) in Warsaw [1]. Figure 2 presents
the flow diagram of the laboratory plant. Three types
of high sulfur (about 2.9 wt.% of sulfur) heavy fuel oils
with different viscosities were combusted. The flue gases
contain high concentrations of SO2, above 1100 ppmv
and NOx above 150 ppmv. These flue gases were irradi-
ated by an EB from an accelerator (800 keV, 20 kW) in
the presence of gaseous ammonia. Figure 3 presents the
dose dependence of SO2 and NOx removal efficiencies
Table 2. Costs of various emission control methods for retrofit 120 MW(e) unit [14]
Emission control method
Investment cost
USD/kW(e)
Annual operational cost
USD/MW(e)
Wet flue gas desulphurization 120 3000
Selective catalytic reduction 110 4600
Wet FGD + SCR 230 7600
EB treatment EBFGT 160 7350
Fig. 2. Schematic diagram of laboratory EB installation. 1 – termostated fuel oil; 2 – oil burner; 3 – particulate and soot filters;
4 – orifice; 5 – dosage of water vapor; 6 – gas sampling point-process inlet; 7 – ammonia injection; 8 – process vessel; 9 – elec-
tron beam accelerator; 10 – retention chamber; 11 – bag filter; 12 – gas sampling point-process outlet; 13 – induced-draught
fan (ID fan); 14 – stack; 15 – concrete shielding wall; 16 – concrete shielding door.
274 A. A. Basfar et al.
from flue gases from combustion of Arabian Medium
Oil with 2.81 wt.% of sulfur. High removal efficiencies
up to 98% for SO2 and 80% for NOx were simultaneously
obtained under optimal irradiation conditions. All these
flue gases after adequate electron beam irradiation meet
the stringent emission regulations for both pollutants.
The by-product, which is a mixture of ammonium sulfate
and nitrate, can be used for production of commercial
agricultural fertilizers, like NPK (i.e. fertilizer containing
nitrogen, phosphorous and potassium as nutrients) or
NPKS (i.e. fertilizer containing nitrogen, phosphorous,
potassium and sulfur as nutrients).
Combustion of high-sulfur lignite
In many countries large amounts of low-quality, high-
-sulfur coal is used in the power industry. The TPPs
in the Maritsa-East region (Bulgaria) are supplied by
low calorific with high sulfur content Thracian lignite.
This is a low-grade Bulgarian lignite with the follow-
ing quality parameters: ash content (as received base)
up to 20 wt.%, moisture up to 52.5 wt.%, combustible
sulfur up to 2.7 wt.%, carbon up to 20 wt.%, and low
calorific value up to 6711 kJ/kg. The 215 MW unit of
TPP Maritsa-East 2 consumes 350 ton/h of lignite. The
pilot plant for EBFGT of the flue gas from lignite-fired
boiler was constructed in the TPP Maritsa-East 2 [10].
Table 3 presents the main technological parameters of
the plant. High simultaneous removal efficiency of SO2
up to 99% and NOx up to 90% was achieved at low doses
4–6 kGy. The by-product collected at the electrostatic
precipitator, is a mixture of ammonium sulfate and
nitrate with a moisture content of about 0.8 wt.% can
be used directly as fertilizer or as component for mixed
fertilizers used in agriculture. The positive results of
the plant operation were the basis for preparation of a
feasibility study for an industrial plant in Bulgaria.
Purification of exhaust gases from copper smelter
Exhaust gases with high SO2 concentration up to 15 vol.%
are emitted from a copper smelter [21]. In conventional
worldwide smelter practices, these gases with an SO2
content higher than 4 vol.% are fed to sulfuric acid
plants that provide SO2 abatement. In the metallurgical
industry, there is no consistent trend for the treatment
of flue gas with low SO2 content (smaller than 4 vol.%).
The gases with a low SO2 content are released from
varied smelter sources such as: fugitive gases from differ-
ent stages of the process, gases from secondary process
(electric furnaces, etc.) and tail gas from sulfuric acid
plants. The applicability of the EB-FGT for controlling
copper smelter off-gases has been demonstrated at two
plants in Poland: the EPS Kawęczyn pilot plant for flue
gas with concentration of SO2 up to 3200 ppmv (an ad-
ditional SO2 was dosed to the flue gases from a coal fired
boiler) and the INCT laboratory installation with a model
gas with an SO2 content up to 15 vol.% SO2 removal ef-
ficiency up to 90% was achieved (see Fig. 4) in the INCT
Fig. 3. Effect of irradiation dose on SO2 and NOx removal from
flue gases formed during combustion of Arabian Medium Oil
with 2.81 wt.% of sulfur.
Table 3. The main technological parameters of the Maritsa-East 2 pilot plant
Parameter Unit Value
Flow rate of flue gas Nm3
/h 10 000
Inlet gas temperature to PV % °C 66
Ammonia stoichiometry 0.90
Inlet SO2 concentration mg/Nm3
17 190
Inlet NOx concentration mg/Nm3
217
EB parameters 800 keV, 35 kW×3
Absorbed dose kGy 3.94
Obtained removal efficiency
SO2 % 97.8
NOx % 86.3
Fig. 4. Dose dependence of SO2 removal from model gases
with extremely high SO2 (15 vol.%). The experimental condi-
tions: gas humidity (14.5 vol.%), ammonia stoichiometry (0.90)
and gas temperature (105–114°C).
275A review on electron beam flue gas treatment (EBFGT) as a multicomponent air pollution...
laboratory installation at a dose of 17.5 kGy, when the
temperature and humidity (see Fig. 5) of irradiated gases
and ammonia stoichiometry were properly adjusted [15].
Both exhaust gases with a weak SO2 content as well as
with high SO2 content can be desulfurized in the EBFGT
process with high efficiency.
Removal of polycyclic aromatic hydrocarbons (PAHs)
PAHs are emitted from coal or oil-fired boiler. Some of
them are carcinogenic, mutagenic or both. The United
States Environmental Protection Agency (US EPA)
has fixed 16 PAHs as priority pollutants. The studies
of PAHs removal during simultaneous SO2 and NOx
removal from flue gas using EB irradiation have been
carried out at EBFGT pilot plant at EPS Kawęczyn
using coal as fuel [5]. Concentration of 16 PAHs in the
flue gas, emitted from a coal-fired WP-120 boiler, was
measured at the plant inlet and outlet by gas chromatog-
raphy-mass spectrometry (GC-MS) technique. During
the plant operation with irradiation dose of 8 kGy, two
tests were performed as follows:
The first test was with a gaseous ammonia addition–
to the flue gas before its inlet to the process vessel
(PV). The ammonia stoichiometry was 0.90. It was
a typical condition for simultaneous SO2 and NOx
removal in the EBFGT process.
The second test was without ammonia addition.–
The removal efficiencies of 5 PAHs obtained in both
tests are presented in Fig. 6. The results of both tests
can be concluded as follows:
Removal efficiencies of 14 PAHs ranged from 2%–
for the four-ringed benzo(b+k)fluoranthene up to
96.5% for the two-ringed acenaphthene were ob-
tained in typical conditions for SO2 and NOx removal
in the EBFGT process,
The concentrations of the 2 three-ringed com-–
pounds: anthracene and fluoranthene increased
after EB irradiation. Probably they are the products
of decomposition of higher-ringed PAHs. This phe-
nomenon is now under investigation.
Ammonia addition to the flue gas has a positive–
influence on the removal efficiencies of 16 PAHs.
After EBFGT with an irradiation dose of 8 kGy,
the total concentration of all 16 PAHs was lowered
by 26.5%. The PAHs are characterized by their car-
cinogenic factors related to benzo(a)pyrene. Such
factors are proposed by EPA in the USA [18]. The
overall toxicity of flue gas was calculated as a sum of
concentration and carcinogenity factor product for
each PAH measured in the flue gas. Such calculations
indicate that after EBFGT with an irradiation dose of
8 kGy, the overall toxicity of flue gas was decreased by
47.5%. The concentration of organic pollutants in the
solid by-product is several times lower in comparison
to commercial ammonium sulfate being a by-product
of caprolactam or coke production processes.
This test confirms that the EBFGT process ensures
simultaneous removal of SO2, NOx and PAHs with
high efficiencies from coal-fired flue gas. Therefore,
EBFGT is the multicomponent air pollution control
technology.
Reduction of dioxin emission from municipal waste
incinerators
Dioxins are very toxic to human body due to their endo-
crine disrupting character, carcinogenity and mutagen-
icity. Dioxins include polychlorinated dibenzo-p-dioxins
(PCDDs), polychlorinated dibenzofurans (PCDFs) and
coplanar polychlorinated biphenyls (PCBs). Dioxins are
emitted from the incineration (especially of municipal
solid waste and medical waste), metallurgical processes
(steel and iron, copper, aluminum and zinc metallurgy),
manufacturing of paper and pulp and combustion of
fuels with high content of chlorine. In addition, dioxins
are typically formed during cooling of the off-gases. The
EBFGT was applied to reduce the emission of dioxins
in flue gas from the municipal solid waste incinerator
at the Takahama Clean Center (Japan) [12]. More
than 90% decomposition of dioxins was obtained after
EB irradiation with a dose of 14 kGy. The treated flue
gas meets the stringent emission standards for dioxins
Fig. 6. Removal efficiencies of 5 PAHs obtained in the
tests with and without ammonia addition to the irradiated
flue gas. The experimental conditions: flue gas flow rate
(10000 Nm3
/h), dose (8 kGy), gas humidity (6.5 vol.%),
ammonia stoichiometry (0.90), gas temperature at PV inlet
(65°C). Simultaneous SO2 removal (92%) and NOx removal
(75%) were obtained.
Fig. 5. Effect of gas humidity on SO2 removal. The experimen-
tal conditions: inlet SO2 concentration (1000–3200 ppm), dose
(11.5 kGy), gas temperature (60–64°C), NH3 stoichiometry
(0.85–0.95).
276 A. A. Basfar et al.
established by the Government of Japan, the USA and
the EU. Low-toxicity of irradiated gas was confirmed
in terms of endocrine disrupter using enzyme immu-
noassay.
VOCs removal from exhaust gases
VOCs are released into the atmosphere from vari-
ous industrial processes. Their main emission sources
are: the mobile combustion sector, organic solvent
application, petroleum industry, combustion of fossil
fuels (industrial and non-industrial), waste treatment
and disposal. Several types of VOCs are very harmful
to human health and the environment. When exhaust
gases containing VOCs mixed with nitrogen oxides are
released into the atmosphere and irradiated by UV
component of sunlight, a complex chain of reactions
converts them into photochemical pollutants (ozone,
aldehydes, hydrogen peroxide, peroxyacetyl nitrate, or-
ganic and inorganic acids and fine particles) [7]. Among
these pollutants, ozone is considered to be the most
important because it is produced in high concentrations
and its wide range of effects may have on human health,
plant growth and material corrosion. Ozone is formed
in the lower layer of the troposphere. The hydrocarbon
reactivity is expressed in terms of photochemical ozone
creation potential (POCP), units calculated with respect
to ethylene as a reference compound (POCP = 100)
[8]. The alkenes and aromatic hydrocarbons represent
classes of VOCs with high POCP. VOCs released to
the atmosphere affect large areas during long-distance
redistribution through atmospheric pathways. The
reduction of VOCs emission is a subject of growing
interest in the international conventions.
EBFGT technology is a promising method for treat-
ment of VOCs at low concentrations. Many studies on
EBFGT of individual VOC in air have been performed
at laboratory installations in Japan, Germany, the USA,
South Korea and Poland [13]. It is very important to
clarify how much EB energy is required to destroy
VOCs in the flue gas from oil-fired boilers. Such studies
are carried out at the INCT laboratory plant, Poland.
Equipment and process engineering
The main components of the process are: spray cooler,
ammonia injection system, process vessel with ac-
celerators and electrostatic precipitator (ESP). The
process control system is based on industrial computer
monitoring system. Most of the used systems are based
on conventional process engineering design principles.
However, they were adopted, tested and optimized at
the EPS Pomorzany installation in Poland. The con-
struction of PV was developed by the INCT, Poland
[3]. Most crucial for plant operation in harsh industrial
conditions is engineering and reliability of high power
accelerators and their shut downs were the main draw-
back of recently constructed industrial plants. A new
high power machine (400 kW) installed and operated
at a wastewater plant, Korea, [19] is a breakthrough in
accelerator construction which can solve the problems
observed in EBFGT installations.
Conclusions
The EBFGT technology is very competitive in compari-
son with the conventional ones and usually is applied
as a combination of wet FGD + ammonia based SCR.
The process is dry and the by-product is a good qual-
ity fertilizer. EBFGT allows simultaneous removal of
SO2, NOx and VOCs, and this cannot be achieved in
other technologies. The technology can be applied for
air pollution control in the case of different fuels; coal,
lignite, heavy fuel oil, municipal wastes and to treat
other industrial off-gases, e.g. lean gases emitted from
copper smelters. Further development of high power
electron accelerators is a crucial factor for technology
implementation on industrial scale.
Acknowledgment. This work was partly financed by the
Saudi Arabian Oil Company (SAUDI ARAMCO), Envi-
ronmental Protection Department and partly by the Polish
Ministry of Science and Higher Education – Project no.
PBZ-MEiN-3/2/2006 “Process engineering for the abate-
ment of harmful and greenhouse gas emissions and their
utilization”.
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A review on electron beam flue gas treatment (ebfgt)

  • 1. NUKLEONIKA 2010;55(3):271−277 REVIEW PAPER Introduction Most the world-wide of energy (88%) is produced by the combustion of fossil fuels like oil, natural gas and coal [2]. All of these fuels are composed of major con- stituents such as carbon, hydrogen and oxygen and other components including sulfur and nitrogen compounds and metals. During the combustion process, different pollutants are emitted such as fly ash (containing diverse trace elements (heavy metals)), SOx (SO2 and SO3), NOx (NOx = NO + NO2), Hg and VOCs. Air pollution caused by particulate matter and other pollutants not only directly impacts the atmospheric environment but also contaminates water and soil, leading to their deg- radation. The exhaust gases released into atmosphere are irradiated by ultraviolet (UV) sunlight and undergo photochemical transformations. Wet and dry deposi- tion of inorganic pollutants leads to acidification of the environment. These phenomena affect human health, increase corrosion and destroy crops and forests. VOCs emissions to the atmosphere can lead to ground level photochemical ozone formation and can have toxic or carcinogenic effects on human health. Among conventional technologies for flue gas treatment aimed at removal of SO2 and NOx are wet, dry and semi-dry flue gas desulfurization (FGD) and selective catalytic reduction (SCR) of NOx. VOCs are usually adsorbed on active carbon, but this process is rarely used for lean hydrocarbon concentrations. All A review on electron beam flue gas treatment (EBFGT) as a multicomponent air pollution control technology Ahmed A. Basfar, Osama I. Fageeha, Noushad Kunnummal, Andrzej G. Chmielewski, Janusz Licki, Andrzej Pawelec, Zbigniew Zimek, Jerzy Warych A. A. Basfar King Abdulaziz City of Science and Technology, Atomic Energy Research Institute, Radiation Technology Center, P. O. Box 6086, Riyadh 11442, Saudi Arabia, Tel.: +9661 481 3648, Fax: +9661 481 3640, E-mail: abasfar@kacst.edu.sa O. I. Fageeha, N. Kunnummal Environmental Protection Department, Saudi Arabian Oil Company (SAUDI ARAMCO), P. O. Box 12772, Dhahran 31311, Saudi Arabia A. G. Chmielewski Institute of Nuclear Chemistry and Technology, 16 Dorodna Str., 03-195 Warsaw, Poland and Faculty of Chemical and Process Engineering, Warsaw University of Technology, 1 Waryńskiego Str., 00-645 Warsaw, Poland J. Licki Institute of Atomic Energy, 05-400 Otwock-Świerk, Poland A. Pawelec, Z. Zimek Institute of Nuclear Chemistry and Technology, 16 Dorodna Str., 03-195 Warsaw, Poland J. Warych Faculty of Chemical and Process Engineering, Warsaw University of Technology, 1 Waryńskiego Str., 00-645 Warsaw, Poland Received: 5 March 2010 Accepted: 31 May 2010 Abstract. Electron beam flue gas treatment (EBFGT) technology for coal-fired boilers has been implemented on an industrial scale in two thermal power plants in China and at the Electropower Station (EPS) Pomorzany in Poland. The plants in China have been designed mainly for desulfurization while the plant in Poland for a simultaneous removal of SO2 and NOx from flue gases. The successful operation of these plants has demonstrated the advantages of using this technology for removing SO2 and NOx from flue gas under varying conditions. At present, the plant in Poland is the only operational installation at an international level. Recent tests performed at an EBFGT industrial pilot plant in Bulgaria have demonstrated feasibility of application of this technology for treatment of high sulfur and high humidity lignite fired boilers. Further laboratory tests have been performed for model flue gases similar to those emitted from a copper smelter and flue gases originated from different types of high sulfur heavy fuel oils. In all cases, dry-scrubbing process with ammonia addition has been tested. The removal efficiency of pollutants is as high as 95% for SO2 and 70–80% for NOx. The by-product of this process is a high quality fertilizer component. Additional laboratory studies have shown that volatile organic compounds (VOCs) emitted during combustion of fossil fuels, can be degraded as well. Therefore, EBFGT can be considered as a multicomponent air pollution control technology which can be applied to flue gases treatment from coal, lignite and heavy fuel oil-fired boilers. Other thermal processes like metallurgy and municipal waste incinerators are potential candidates for EBFGT technology application. Key words: fossil fuel combustion • heavy fuel oil • electron beam irradiation • plasma processes • flue gas treatment • SO2 and NOx removal
  • 2. 272 A. A. Basfar et al. these technologies are complex chemical processes, and wastes, like wastewater, gypsum and used catalyst or adsorber, are generated [20]. EBFGT technology is among the most promising advanced technologies of new generation. This is a dry-scrubbing process of simultaneous SO2 and NOx removal, where no waste, except a by-product, is gen- erated. The application of electron beam irradiation to initiate chemical reactions to remove SO2 and NOx was first investigated by joint research of the Japan Atomic Energy Research Institute (JAERI) and Ebara Corporation in the early 1980s. The method has been developed since then from the laboratory to pilot and a large demonstration scale by research and development projects in Japan, USA, Germany, China and Poland [11]. The final engineering design technology for indus- trial applications was achieved at pilot plants operating in Nagoya, Japan [17] and at Kawęczyn, Poland [6]. In the case of the latter, new engineering solutions were ap- plied: double-longitudinal gas irradiation, an air curtain separating the secondary window from corrosive flue gases and modifications of humidification and ammonia injection system (high enthalpy water or steam injection, ammonia water injection) and others. A high irradiation dose is required for NOx removal, while SO2 is removed in proper conditions at low energy consumption [6]. Technology status EBFGT technology for coal-fired boilers has been implemented on an industrial scale at the Thermal Power Plants (TPPs) at Chengdu [9] and Hangzhou [16] in China and at the EPS Pomorzany [4] in Poland. At present, the EBFGT installation in Poland is the only operational installation in the world. Table 1 presents the main parameters of these installations. The plants in China were designed mainly for SO2 removal, while the plant in Poland was designed for simultaneous SO2 and NOx removal. The flue gases from two Benson boilers (65 MW(e) and 100 MW(th) each)) are purified at the EPS Pomorzany in Poland (see Fig. 1). The maximum flow rate of the gases is 270 000 Nm3 /h and the total electron beam power is equal to 1 MW. There are two process vessels over which two electron accelerators are installed in series (700 keV, 260 kW each). The applied dose is in the range 7–12 kGy (kJ/kg). At these doses, the removal efficiency ap- proaches 85–95% for SO2 and 50–70% for NOx. The by-product is collected by an electrostatic precipitator and shipped to a fertilizer plant. The most often applied conventional technology for flue gas treatment is a combination of wet FDG and SCR processes. A comparison of the costs of various emission Table 1. Main parameters of industrial EB installations Parameter Unit Chengdu TPP, China Hangzhou TPP, China Pomorzany EPS, Poland Flue gas flow rate Nm3 /h 300 000 305 400 270 000 Inlet flue gas temperature °C 150 145 140 Inlet SO2 concentration mg/Nm3 5150 2770 2000 Inlet NOx concentration mg/Nm3 820 410 600 SO2 removal efficiency % 80 85 90 NOx removal efficiency % 18 55 70 EB 800 keV, 320 kW×2 800 keV, 320 kW×2 700 keV, 260 kW×4 Fig. 1. Flow diagram of the industrial plant at the EPS Pomorzany, Poland.
  • 3. 273A review on electron beam flue gas treatment (EBFGT) as a multicomponent air pollution... control methods for a 120 MW(e) unit is presented in Table 2. The operation of the EBFGT industrial plants in China and Poland for the last few years has demon- strated advantages of using this technology for simul- taneous removal of SO2 and NOx from flue gas under varying conditions. EBFGT has to be competitive with the conventional ones both from economic and techni- cal point of view. Therefore, any development concern- ing cost reduction and technological improvements regarding technical components, especially reliability of electron accelerator plays a very important role for further EBFGT process implementation. Potential applications for industrial off-gases Combustion of fuel oil Liquid fuels are used in some limited applications, but are more prevalent in certain areas of the world such as South America, central and eastern Canada, north- eastern USA. No. 2 and no. 6 oils are most commonly used liquid fuels. Heavy fuel oils (HFO) are a mixture of hydrocarbons composed of residual fractions from distillation and processing of crude oil. It is essentially an industrial fuel that is suitable for use in thermal power plants, refineries, industrial boilers, pulp and paper industry, marine applications and metallurgi- cal operations which generally preheat the fuel oils. Depending on the source, the sulfur content in the HFO could be as high as 4.0 wt.%. Sulfur is converted to sulfur dioxide when oil is burnt. Flue gas emitted from such heavy fuel oil-fired boiler contains high SO2 and NOx concentrations, many times exceeding the permissible emission limits, which necessitates the use of add-on control devices for the reduction of SO2 and NOx emissions. A study of EBFGT on flue gas from combustion of high sulfur heavy fuel oils was performed at the labo- ratory plant at the Institute of Nuclear Chemistry and Technology (INCT) in Warsaw [1]. Figure 2 presents the flow diagram of the laboratory plant. Three types of high sulfur (about 2.9 wt.% of sulfur) heavy fuel oils with different viscosities were combusted. The flue gases contain high concentrations of SO2, above 1100 ppmv and NOx above 150 ppmv. These flue gases were irradi- ated by an EB from an accelerator (800 keV, 20 kW) in the presence of gaseous ammonia. Figure 3 presents the dose dependence of SO2 and NOx removal efficiencies Table 2. Costs of various emission control methods for retrofit 120 MW(e) unit [14] Emission control method Investment cost USD/kW(e) Annual operational cost USD/MW(e) Wet flue gas desulphurization 120 3000 Selective catalytic reduction 110 4600 Wet FGD + SCR 230 7600 EB treatment EBFGT 160 7350 Fig. 2. Schematic diagram of laboratory EB installation. 1 – termostated fuel oil; 2 – oil burner; 3 – particulate and soot filters; 4 – orifice; 5 – dosage of water vapor; 6 – gas sampling point-process inlet; 7 – ammonia injection; 8 – process vessel; 9 – elec- tron beam accelerator; 10 – retention chamber; 11 – bag filter; 12 – gas sampling point-process outlet; 13 – induced-draught fan (ID fan); 14 – stack; 15 – concrete shielding wall; 16 – concrete shielding door.
  • 4. 274 A. A. Basfar et al. from flue gases from combustion of Arabian Medium Oil with 2.81 wt.% of sulfur. High removal efficiencies up to 98% for SO2 and 80% for NOx were simultaneously obtained under optimal irradiation conditions. All these flue gases after adequate electron beam irradiation meet the stringent emission regulations for both pollutants. The by-product, which is a mixture of ammonium sulfate and nitrate, can be used for production of commercial agricultural fertilizers, like NPK (i.e. fertilizer containing nitrogen, phosphorous and potassium as nutrients) or NPKS (i.e. fertilizer containing nitrogen, phosphorous, potassium and sulfur as nutrients). Combustion of high-sulfur lignite In many countries large amounts of low-quality, high- -sulfur coal is used in the power industry. The TPPs in the Maritsa-East region (Bulgaria) are supplied by low calorific with high sulfur content Thracian lignite. This is a low-grade Bulgarian lignite with the follow- ing quality parameters: ash content (as received base) up to 20 wt.%, moisture up to 52.5 wt.%, combustible sulfur up to 2.7 wt.%, carbon up to 20 wt.%, and low calorific value up to 6711 kJ/kg. The 215 MW unit of TPP Maritsa-East 2 consumes 350 ton/h of lignite. The pilot plant for EBFGT of the flue gas from lignite-fired boiler was constructed in the TPP Maritsa-East 2 [10]. Table 3 presents the main technological parameters of the plant. High simultaneous removal efficiency of SO2 up to 99% and NOx up to 90% was achieved at low doses 4–6 kGy. The by-product collected at the electrostatic precipitator, is a mixture of ammonium sulfate and nitrate with a moisture content of about 0.8 wt.% can be used directly as fertilizer or as component for mixed fertilizers used in agriculture. The positive results of the plant operation were the basis for preparation of a feasibility study for an industrial plant in Bulgaria. Purification of exhaust gases from copper smelter Exhaust gases with high SO2 concentration up to 15 vol.% are emitted from a copper smelter [21]. In conventional worldwide smelter practices, these gases with an SO2 content higher than 4 vol.% are fed to sulfuric acid plants that provide SO2 abatement. In the metallurgical industry, there is no consistent trend for the treatment of flue gas with low SO2 content (smaller than 4 vol.%). The gases with a low SO2 content are released from varied smelter sources such as: fugitive gases from differ- ent stages of the process, gases from secondary process (electric furnaces, etc.) and tail gas from sulfuric acid plants. The applicability of the EB-FGT for controlling copper smelter off-gases has been demonstrated at two plants in Poland: the EPS Kawęczyn pilot plant for flue gas with concentration of SO2 up to 3200 ppmv (an ad- ditional SO2 was dosed to the flue gases from a coal fired boiler) and the INCT laboratory installation with a model gas with an SO2 content up to 15 vol.% SO2 removal ef- ficiency up to 90% was achieved (see Fig. 4) in the INCT Fig. 3. Effect of irradiation dose on SO2 and NOx removal from flue gases formed during combustion of Arabian Medium Oil with 2.81 wt.% of sulfur. Table 3. The main technological parameters of the Maritsa-East 2 pilot plant Parameter Unit Value Flow rate of flue gas Nm3 /h 10 000 Inlet gas temperature to PV % °C 66 Ammonia stoichiometry 0.90 Inlet SO2 concentration mg/Nm3 17 190 Inlet NOx concentration mg/Nm3 217 EB parameters 800 keV, 35 kW×3 Absorbed dose kGy 3.94 Obtained removal efficiency SO2 % 97.8 NOx % 86.3 Fig. 4. Dose dependence of SO2 removal from model gases with extremely high SO2 (15 vol.%). The experimental condi- tions: gas humidity (14.5 vol.%), ammonia stoichiometry (0.90) and gas temperature (105–114°C).
  • 5. 275A review on electron beam flue gas treatment (EBFGT) as a multicomponent air pollution... laboratory installation at a dose of 17.5 kGy, when the temperature and humidity (see Fig. 5) of irradiated gases and ammonia stoichiometry were properly adjusted [15]. Both exhaust gases with a weak SO2 content as well as with high SO2 content can be desulfurized in the EBFGT process with high efficiency. Removal of polycyclic aromatic hydrocarbons (PAHs) PAHs are emitted from coal or oil-fired boiler. Some of them are carcinogenic, mutagenic or both. The United States Environmental Protection Agency (US EPA) has fixed 16 PAHs as priority pollutants. The studies of PAHs removal during simultaneous SO2 and NOx removal from flue gas using EB irradiation have been carried out at EBFGT pilot plant at EPS Kawęczyn using coal as fuel [5]. Concentration of 16 PAHs in the flue gas, emitted from a coal-fired WP-120 boiler, was measured at the plant inlet and outlet by gas chromatog- raphy-mass spectrometry (GC-MS) technique. During the plant operation with irradiation dose of 8 kGy, two tests were performed as follows: The first test was with a gaseous ammonia addition– to the flue gas before its inlet to the process vessel (PV). The ammonia stoichiometry was 0.90. It was a typical condition for simultaneous SO2 and NOx removal in the EBFGT process. The second test was without ammonia addition.– The removal efficiencies of 5 PAHs obtained in both tests are presented in Fig. 6. The results of both tests can be concluded as follows: Removal efficiencies of 14 PAHs ranged from 2%– for the four-ringed benzo(b+k)fluoranthene up to 96.5% for the two-ringed acenaphthene were ob- tained in typical conditions for SO2 and NOx removal in the EBFGT process, The concentrations of the 2 three-ringed com-– pounds: anthracene and fluoranthene increased after EB irradiation. Probably they are the products of decomposition of higher-ringed PAHs. This phe- nomenon is now under investigation. Ammonia addition to the flue gas has a positive– influence on the removal efficiencies of 16 PAHs. After EBFGT with an irradiation dose of 8 kGy, the total concentration of all 16 PAHs was lowered by 26.5%. The PAHs are characterized by their car- cinogenic factors related to benzo(a)pyrene. Such factors are proposed by EPA in the USA [18]. The overall toxicity of flue gas was calculated as a sum of concentration and carcinogenity factor product for each PAH measured in the flue gas. Such calculations indicate that after EBFGT with an irradiation dose of 8 kGy, the overall toxicity of flue gas was decreased by 47.5%. The concentration of organic pollutants in the solid by-product is several times lower in comparison to commercial ammonium sulfate being a by-product of caprolactam or coke production processes. This test confirms that the EBFGT process ensures simultaneous removal of SO2, NOx and PAHs with high efficiencies from coal-fired flue gas. Therefore, EBFGT is the multicomponent air pollution control technology. Reduction of dioxin emission from municipal waste incinerators Dioxins are very toxic to human body due to their endo- crine disrupting character, carcinogenity and mutagen- icity. Dioxins include polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs) and coplanar polychlorinated biphenyls (PCBs). Dioxins are emitted from the incineration (especially of municipal solid waste and medical waste), metallurgical processes (steel and iron, copper, aluminum and zinc metallurgy), manufacturing of paper and pulp and combustion of fuels with high content of chlorine. In addition, dioxins are typically formed during cooling of the off-gases. The EBFGT was applied to reduce the emission of dioxins in flue gas from the municipal solid waste incinerator at the Takahama Clean Center (Japan) [12]. More than 90% decomposition of dioxins was obtained after EB irradiation with a dose of 14 kGy. The treated flue gas meets the stringent emission standards for dioxins Fig. 6. Removal efficiencies of 5 PAHs obtained in the tests with and without ammonia addition to the irradiated flue gas. The experimental conditions: flue gas flow rate (10000 Nm3 /h), dose (8 kGy), gas humidity (6.5 vol.%), ammonia stoichiometry (0.90), gas temperature at PV inlet (65°C). Simultaneous SO2 removal (92%) and NOx removal (75%) were obtained. Fig. 5. Effect of gas humidity on SO2 removal. The experimen- tal conditions: inlet SO2 concentration (1000–3200 ppm), dose (11.5 kGy), gas temperature (60–64°C), NH3 stoichiometry (0.85–0.95).
  • 6. 276 A. A. Basfar et al. established by the Government of Japan, the USA and the EU. Low-toxicity of irradiated gas was confirmed in terms of endocrine disrupter using enzyme immu- noassay. VOCs removal from exhaust gases VOCs are released into the atmosphere from vari- ous industrial processes. Their main emission sources are: the mobile combustion sector, organic solvent application, petroleum industry, combustion of fossil fuels (industrial and non-industrial), waste treatment and disposal. Several types of VOCs are very harmful to human health and the environment. When exhaust gases containing VOCs mixed with nitrogen oxides are released into the atmosphere and irradiated by UV component of sunlight, a complex chain of reactions converts them into photochemical pollutants (ozone, aldehydes, hydrogen peroxide, peroxyacetyl nitrate, or- ganic and inorganic acids and fine particles) [7]. Among these pollutants, ozone is considered to be the most important because it is produced in high concentrations and its wide range of effects may have on human health, plant growth and material corrosion. Ozone is formed in the lower layer of the troposphere. The hydrocarbon reactivity is expressed in terms of photochemical ozone creation potential (POCP), units calculated with respect to ethylene as a reference compound (POCP = 100) [8]. The alkenes and aromatic hydrocarbons represent classes of VOCs with high POCP. VOCs released to the atmosphere affect large areas during long-distance redistribution through atmospheric pathways. The reduction of VOCs emission is a subject of growing interest in the international conventions. EBFGT technology is a promising method for treat- ment of VOCs at low concentrations. Many studies on EBFGT of individual VOC in air have been performed at laboratory installations in Japan, Germany, the USA, South Korea and Poland [13]. It is very important to clarify how much EB energy is required to destroy VOCs in the flue gas from oil-fired boilers. Such studies are carried out at the INCT laboratory plant, Poland. Equipment and process engineering The main components of the process are: spray cooler, ammonia injection system, process vessel with ac- celerators and electrostatic precipitator (ESP). The process control system is based on industrial computer monitoring system. Most of the used systems are based on conventional process engineering design principles. However, they were adopted, tested and optimized at the EPS Pomorzany installation in Poland. The con- struction of PV was developed by the INCT, Poland [3]. Most crucial for plant operation in harsh industrial conditions is engineering and reliability of high power accelerators and their shut downs were the main draw- back of recently constructed industrial plants. A new high power machine (400 kW) installed and operated at a wastewater plant, Korea, [19] is a breakthrough in accelerator construction which can solve the problems observed in EBFGT installations. Conclusions The EBFGT technology is very competitive in compari- son with the conventional ones and usually is applied as a combination of wet FGD + ammonia based SCR. The process is dry and the by-product is a good qual- ity fertilizer. EBFGT allows simultaneous removal of SO2, NOx and VOCs, and this cannot be achieved in other technologies. The technology can be applied for air pollution control in the case of different fuels; coal, lignite, heavy fuel oil, municipal wastes and to treat other industrial off-gases, e.g. lean gases emitted from copper smelters. Further development of high power electron accelerators is a crucial factor for technology implementation on industrial scale. Acknowledgment. This work was partly financed by the Saudi Arabian Oil Company (SAUDI ARAMCO), Envi- ronmental Protection Department and partly by the Polish Ministry of Science and Higher Education – Project no. PBZ-MEiN-3/2/2006 “Process engineering for the abate- ment of harmful and greenhouse gas emissions and their utilization”. References Basfar AA, Fageeha OI, Kunnummal N1. et al. (2008) Electron beam flue gas treatment (EBFGT) technology for simulations removal of SO2 and NOx from combustion of liquid fuels. Fuel 87:1446–1452 Baukal CE (ed) (2004) Industrial combustion pollution2. and control. Marcel Dekker, Inc., New York Chmielewski AG (1995) Technological development of3. EB flue gas treatment based on physics and chemistry of the process. Radiat Phys Chem 46:1057–1062 Chmielewski AG, Licki J, Pawelec A, Tymiński B, Zimek4. Z (2004) Operational experience of the industrial plant for electron beam flue gas treatment. 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