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Fuel 87 (2008) 14461452

Electron beam ue gas treatment (EBFGT) technology for

simultaneous removal of SO2 and NOx from combustion of liquid fuels
Ahmed A. Basfar a,*, Osama I. Fageeha b, Noushad Kunnummal b, Seraj Al-Ghamdi b,
Andrzej G. Chmielewski c, Janusz Licki d, Andrzej Pawelec c,
Bogdan Tyminski c, Zbigniew Zimek c

King Abdulaziz City of Science and Technology, Atomic Energy Research Institute, Radiation Technology Center, P.O. Box 6086,
Riyadh 11442, Saudi Arabia
Saudi Arabian Oil Company (Saudi Aramco), Environmental Protection Department, P.O. Box 12772, Dhahran 31311, Saudi Arabia
Institute of Nuclear Chemistry and Technology, 03-195 Warsaw, Dorodna 16, Poland
Institute of Atomic Energy, 05-400 Otwock-Swierk, Poland
Received 22 July 2007; received in revised form 15 September 2007; accepted 18 September 2007
Available online 15 October 2007

Electron beam ue gas treatment technology was applied for removal of SO2 and NOx from ue gas, emitted from combustion of
high-sulfur fuel oils. The detailed study of this process was performed in a laboratory by irradiating the exhaust gas from the combustion
of three grades of Arabian fuels with an electron beam from accelerator (800 keV, max. beam power 20 kW). SO2 removal is mainly
dependent on ammonia stoichiometry, ue gas temperature and humidity and irradiation doses up to 8 kGy. NOx removal depends primarily on irradiation dose. High removal eciencies up to 98% for SO2 and up to 82% for NOx were obtained under optimal conditions.
The ue gas emitted from combustion of high-sulfur fuel oils, after electron beam irradiation, meets the stringent emission standards for
both pollutants. The by-product, which is a mixture of ammonium sulphate and nitrate, can be used as a fertilizer as such or blended with
other components to produce commercial agricultural fertilizer.
 2007 Elsevier Ltd. All rights reserved.
Keywords: High-sulfur oil combustion; Flue gas purication; Electron beam; SO2 removal; NOx removal

1. Introduction
The highest percentage of electrical energy and heat
(88% [1]) is produced by the combustion of fossil fuels like
coal, oil and natural gas. Many pollutants are released in
the combustion process. These pollutants aect air quality,
human health, environment, economy and contribute to
climate change. 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,
northeastern States USA. Number 2 and No. 6 oils are the
most commonly used liquid fuels. Heavy fuel oil (HFO) is a

Corresponding author. Tel.: +966 1 4813648; fax: +966 1 4813640.

E-mail address: (A.A. Basfar).

0016-2361/$ - see front matter  2007 Elsevier Ltd. All rights reserved.

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, reneries, industrial boilers, pulp and paper industry and metallurgical operations which generally pre-heat
the fuel oil.
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; additionally, the combustion
process creates various forms of nitrogen oxides. Flue gas
emitted from heavy fuel oil-red 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. Post-combustion technologies have been maturely

A.A. Basfar et al. / Fuel 87 (2008) 14461452

developed and widely used. Until now, most of these technologies have been performed individually, i.e. one technology controls only one pollutant. Simultaneous
removal technology for multiple pollutants will become
increasingly useful.
Electron beam ue gas treatment technology is among
the most promising advanced technologies of a new generation. It is a simultaneous dry-scrubbing of SO2 and NOx,
where no waste, except a useful by-product, is generated.
The irradiation of ue gas with fast (300800 keV) electrons initiates chemical changes that make removal of sulfur and nitrogen oxides easier. After irradiation, fast
electrons interact with the main components of ue gas
(N2, O2, H2O and CO2) and generate the same oxidants
(*OH, HO2 , O, O3) which are produced by UV sunlight
in the free atmosphere, but at concentration levels several
orders of magnitude higher. The oxidants convert NOx
and SO2 to nitric and sulfuric acids which form a solid
powder of ammonium nitrate and sulfate in the presence
of ammonia which is added to ue gas before its irradiation. The ltered by-product is usable as an agricultural
fertilizer. Overviews of the process chemistry and model
calculations were given by Tokunaga et al. [2], Matzing
[3] and Namba [4]. The application of this method for
treatment of coal-red ue gas has been developed from
laboratory scale to pilot and large demonstration scale
through research and development projects in Japan, Germany, Poland [5,6], China, Bulgaria and USA. High
removal eciencies of SO2 up to 95% and NOx up to
85% were simultaneously obtained at the optimal conditions for electron beam ue gas treatment. Three industrial
installations have already been built at coal-red Thermal
Power Plants Chengdu and Hangzhou [7] in China and
Pomorzany [8] in Poland. The tests demonstrated the ability of the technology for highly ecient removal of SO2


and NOx from ue gas from coal combustion process.

New industrial plants are under construction in China
and Bulgaria. The primary objective of this paper is to
demonstrate the feasibility of the electron beam ue gas
treatment process for simultaneous removal of SO2 and
NOx from ue gas from combustion of heavy liquid fuels.
This study was performed in a laboratory with combustion
of three grades of Arabian fuels.
2. Experimental test facility
The experiments have been performed in the laboratory-scale EBFGT installation at Institute of Nuclear
Chemistry and Technology (INCT) in Warsaw, Poland.
For this study, the installation was equipped with fuel oil
combustion unit. A schematic ow chart of the test facility
is shown in Fig. 1. The ue gas emitted from fuel oil burner
(2 in Fig. 1), passed through the conditioning system and
was irradiated by electron beam in the process vessel. A
near-stoichiometric amount of ammonia (7 in Fig. 1) was
added to ue gas before its inlet to process vessel. By-product from irradiated gas was separated in a bag lter and
puried ue gas was exhausted through a stainless steel
stack (14 in Fig. 1) to the atmosphere. Flue gas ow rate
at 5m3/h was controlled by buttery valve (1 h in Fig. 1)
and draft of the ID fan and was measured by an orice.
The laboratory test facility consists of the following technological units: fuel oil combustion unit, ue gas conditioning system, electron beam irradiation of ue gas,
ltration unit, monitoring system and exhaust of puried
ue gas.
Fuel oil combustion unit. Three grades of Arabian liquid
fuels were combusted: Arabian Medium Crude Oil (AM),
Arabian Heavy Crude Oil (AH) and Arabian Heavy Fuel
Oil (HFO). Table 1 presents properties of these fuels.

Fig. 1. Schematic diagram of laboratory scale electron-beam ue gas treatment installation. (1) Thermostated fuel oil; (2) oil burner; (3) particulate and
soot lters; (4) orice; (5) dosage of water vapor; (6) gas sampling point-process inlet; (7) ammonia injection; (8) process vessel; (9) electron beam
accelerator; (10) retention chamber; (11) bag lter; (12) gas sampling point-process outlet; (13) induced-draught fan (ID fan); (14) stack; (15) concrete
shielding wall; (16) concrete shielding door.


A.A. Basfar et al. / Fuel 87 (2008) 14461452

Table 1
Properties of Arabian liquid fuels
Density at 15 C
Gross heating value
Kinematics viscosity at 50 C
Sulfur content
Ash content









A pressure jet oil burner, type Jet 4.5EV, produced by

Korting Hannover AG (Germany), was installed in the
front wall of an air-cooled cylindrical combustion chamber
(1d in Fig. 1) 800 mm long and 400 mm in diameter. The
chamber was lined with high-temperature chamotte bricks
to assure good combustion of sprayed oils. Flue gas temperature was reduced in the air cooler (1f in Fig. 1). Temperature of gas leaving the cooler was about 420540 C
depending on the type of fuel burned. The ue gas was
divided into two streams: one (xed at 5 m3/h) was drawn
to the laboratory installation by the ID fan and the rest was
released through the stack (1g in Fig. 1) to atmosphere. For
HFO burning, it was necessary to lower its viscosity to
manageable level by preheating the oil further and blending
it with 10% wt. of light fuel oil (type Ekoterm Plus). This
light fuel oil (LO) was also burnt for conditioning the laboratory installations before and after combustion of Arabian liquid fuels.
Flue gas conditioning unit. Flue gas from the burner was
directed to the process vessel through stainless steel pipes.
These tubes were wrapped with heating tapes and thermal
insulation to keep the ue gas temperature above its dewpoint to avoid condensation. The soot and y ash were
removed from ue gas at the inlet to the installation to
assure good quality of by-product. A two-step ltration
system was applied. The rst lter (3a in Fig. 1) was
installed at the inlet to the facility where ue gas temperature at the cross-section was above 400 C. This lter was
made from needled cloth with prime coat glass ber. The
second lter (3b in Fig. 1) was installed in the colder part
of installation and was made from Goretex bag with a teflon coat. The water vapor dosage system (5 in Fig. 1) was
applied to increase the ue gas humidity to the desired
level. NH3 was injected to the ue gas upstream of process
vessel from gas cylinder. A temperature controller was used
to adjust the gas temperature at the inlet to the process
Electron beam irradiation of ue gas. The process vessel
was constructed as a cylinder with diameter of 200 mm and
length of 850 mm. Electron beam was introduced into the
process vessel perpendicularly to the axis of the vessel. It
passes through a thin titanium (Ti) entrance window
installed on top of the vessel. The active dimensions of
the Ti foil were 350 120 mm2 and thickness of 50 lm.
The electron beam was generated by an electron accelerator ILU-6. It is a single cavity high frequency, pulsed resonant accelerator. Average beam power was up to 20 kW

and electrons energy 800 keV. The dose applied to the ue

gas was changed by varying the repetition rate of the electron pulse. The ue gas ows through the process vessel,
where it was irradiated by the beam of fast electrons in
the presence of a near-stoichiometric amount of ammonia.
Essential changes in ue gas composition occur as a result
of physicochemical processes subsequent to ue gas irradiation. The magnitude of changes in its composition
depends on the process parameters.
Filtration unit. Gas leaving the process vessel ows
through a retention chamber (10 in Fig. 1) to provide
enough residence time for the formation of the by-product.
These salts were recovered as a dry powder using bag lter
(11 in Fig. 1). Goretex bags with a teon coat were used for
collection of by-product.
Exhaust of treated ue gas. Treated ue gas leaving the
bag lter was drawn through duct by ID fan and was discharged to the atmosphere through a stack. The measurement point (12 in Fig. 1), designed for monitoring of SO2
and NOx concentration in the treated ue gas, was located
at the outlet of the bag lter.
Monitoring system. The ue gas contained high concentrations of SO2, NOx, H2O and CO2 In order to assure
accurate measurements of ue gas components the following selections were made:
Type of gas analyzers: a UV pulsed uorescent SO2 analyzer Model 40 and a chemiluminescent NO/NOx analyzer with molybdenum converter Model 10 A/R,
manufactured by Thermo Electron Corporation (TEC,
USA), were used.
Continuous emission monitoring (CEM) system operates by utilizing the sample gas dilution unit. The heated
sample gas dilution and conditioning Model 900 (TEC)
was applied with dilution ratio 20:1.
The gas leaving bag lter may contains un-reacted
ammonia. The heated ammonia scrubber from Shimadzu (Japan) was used for selective absorption of ammonia gas from the sample gas without changing the
concentration of the other components.
Two extractive multi-gas monitoring systems were
installed for continuous measurement of SO2 and NOx
concentration in the ue gas: one at the process inlet
(before irradiation, point 5 in Fig. 1) and second at the process outlet (after bag lter, point 12 in Fig. 1).
The portable ue gas analyzer type Lancom II, manufactured by Land Combustion (UK), measures the concentrations of CO, CO2, O2, SO2, NO, NO2, NOx, and
hydrocarbons in the ue gas. Such measurements were performed in the ue gas at outlet of oil burner and occasionally at process inlet and outlet to check readings of both
CEM systems. The temperature of ue gas at six essential
points of experimental set-up was measured and controlled
using K thermocouples. The humidity of ue gas was determined by manual analytical method based on EPA method
4 using u-tubes lled with granular silica gel.

A.A. Basfar et al. / Fuel 87 (2008) 14461452

Electron-beam energy absorbed in the ue gas, dened

as an absorbed dose in units of gray (Gy = J/kg), was estimated using a cellulose triacetate (CTA) tape of 8 (w)
0.125 (t) mm (Fuji photo lm, FTR-125) [9].
3. Results and discussion
During this investigation three types of Arabian liquid
fuels were combusted. Measurement of the emission of
SO2 and NOx from the burning of these fuels was the rst
task of this work. The measurements of ue gas composition were performed at the process inlet for each grade of
fuel. Table 2 summarizes averaged volumetric emission
concentrations for all tested fuels.
Observations from these measurements are as follows:
Very high level of SO2 emission. All SO2 concentrations
were above 1200 ppmv while the sulfur content in the
burned oils was above 2.7% wt.,
NOx emissions ranged from 150 to 170 ppmv,
oxygen content in the analysed ue gases ranged from
3.4 to 4.4% vol.,
natural humidity of ue gas was higher than 8.48% vol.
To evaluate SO2 and NOx emissions under comparable
conditions, the measurements were normalized at 3% vol.
oxygen and dry gas basis conditions. The data indicate that
SO2 emissions from combustion of these high-sulfur fuel
oils were very high, about 1220 ng/J, which if released
untreated, will adversely impact the ambient air quality
standards. Emissions of NOx were also high, in the range
of 110120 ng/J. In order to meet air quality standards,
these ue gases require post-treatment with high SO2 and
NOx removal eciencies.
The applicability of the electron beam technology for
removal of SO2 and NOx from these ue gases was the
main objective of this investigation. In previous studies of
this technology it was demonstrated that removal eciencies of both pollutants depend on the following process
parameters: absorbed dose (D), ammonia stoichiometry
(aNH3 ), gas temperature at inlet to process vessel (TinletPV),
gas humidity (H) and inlet NOx concentration (NO0x ). The
parametric study of SO2 and NOx removal eciency was


performed for ue gas obtained from combustion of each

Arabian fuel.
Eect of electron beam dose on SO2 and NOx removal.
Fig. 2 presents the dose dependence of SO2 and NOx
removal eciency. The absorbed dose is the primary factor
inuencing NOx removal eciency. The reaction starts at
zero eciency for zero dose and indicating a saturation
at high dose. This demonstrates that NOx removal is a
radiation-induced process. Higher NOx removal was
achieved with higher absorbed doses because the amount
of NOx molecules removed corresponds to the amount of
active species formed by electron beam irradiation of ue
The SO2 removal is based on two dierent pathways:
thermal process and radiation-induced process. At zero
dose, SO2 removal is caused by thermal reaction of SO2
and NH3 in the presence of moisture. These reactions take
place in the gas phase as well as on the surface such as
those on the lter cake of bag lter. Sulfur dioxide removal
increases sharply with increase of electron beam dose up to
8 kGy and then attens out at high doses.
Eect of ammonia stoichiometry. Fig. 3 presents the SO2
and NOx removal eciency obtained in two experiments
with combustion of Arabian Medium Oil. First experiment
was performed with electron beam treatment of the ue gas
without any additives (without NH3). Low SO2 and NOx
removal eciencies were obtained. In the second experiment, gaseous ammonia was added to ue gas before its
inlet to process vessel. The NH3 stoichiometry was equal
to 0.90. In this case higher removal eciency of SO2 and
NOx were obtained. Ammonia addition signicantly inuences SO2 removal.
Fig. 4 shows eect of ammonia stoichiometry on SO2
and NOx removal eciency.
Eect of gas temperature at the inlet to process vessel.
Fig. 5 presents the eect of gas temperature on SO2 and
NOx removal eciency. The gure shows that higher gas
temperatures yielded higher NOx removals. This is in contrast with the SO2 removal, which decreases with higher gas

Table 2
Composition of ue gas from combustion of three Arabian fuels measured
at process inlet




HFO + 10% LO

Sulfur content in oil

% vol.
% vol.
% vol.
% vol.
% wt.




SO2 concentration recalculated for combustion of HFO only.

Fig. 2. SO2 and NOx removal eciency as a function of dose from

combustion of Arabian Heavy Fuel Oil + 10% Light Oil.


A.A. Basfar et al. / Fuel 87 (2008) 14461452

Fig. 3. SO2 and NOx removal eciency as a function of dose with and
without ammonia for the combustion of Arabian Medium Oil.

Fig. 4. Eect of ammonia stoichiometry on SO2 and NOx removal

eciency at an absorbed dose of 8.8 kGy for combustion of Arabian
Heavy Oil.

Gas temperature has a signicant impact on the SO2

removal and a small eect on the NOx removal eciency.
These phenomena are governed by equilibrium conditions for ammonium sulfate formation which depends on
the temperature; above 125 C this salt undergoes thermal
dissociation. This indicates that ue gas temperature at
inlet to process vessel can be eectively used to change
SO2 removal eciency with minimal impact on the NOx
Eect of ue gas humidity. Two experiments for electron
beam treatment of ue gas at dierent humidity levels were
preformed. Flue gas with natural humidity (9.62% vol) was
irradiated in the rst experiment. Additional water vapor
was injected to the ue gas in the second experiment to
increase its humidity to 11.57 % vol.
Fig. 6 presents the SO2 and NOx removal eciencies
obtained in both experiments. The increase of ue gas
humidity does not aect NOx removal. The SO2 removal
eciency increases markedly with the increase in humidity
of ue gas. This increase is due to the thermal reaction of
SO2 with ammonia in the absence of electron beam irradiation. The dew-point depends on gas temperature and
humidity; this is another evidence of the occurrence of heterogeneous reaction.
By-product analysis. In each experiment a by-product
was collected in the bag lter. The by-product (white solid
particles) was analyzed using ion chromatography 2000i/
SP (Dionex, USA). Table 3 presents the chemical characteristics of by-products collected in the dierent experiments with combustion of the three Arabian fuels.
The major constituents of by-products were sulfate,
nitrate and ammonium ions. The contents of these constituents varied depending on the type of fuel (AM, AH, or
HFO) used in the experiments. Ion chromatography analyses indicate that by-product consists primarily of ammonium sulfate and ammonium nitrate. The data, however,
show that the amount of ammonium nitrate collected in
this process was less than the amount of NOx removed
from ue gas. This is due to the fact that in electron beam
process, NOx is partly converted to nitrogen gas (N2) and
N2O through homogeneous gas phase reactions
NH3  OH ! NH2 H2 O
NH2 NO ! N2 H2 O
NH2 NO2 ! N2 O H2 O

Fig. 5. Eect of gas temperature on the SO2 and NOx removal at an

absorbed dose of 8.8 kGy for combustion of Arabian Medium Oil.

temperature. The SO2 removal eciency is improved as the

gas temperature approaches its dew-point temperature.

Experiments with N-15 labeled compounds, performed

at IAERI, Japan [10], proved that NOx is partly reduced
to molecular nitrogen (20%) and N2O (<10%). The smaller amount of nitrate was also caused by the additional formation of sulfate by the thermal reaction on the large
surface area of the bag lter cake. The chemical composition of by-product suggests that it is suitable as an agricultural fertilizer.
Optimization study. From the above parametric study it
was possible to deduce the value of process parameters for
optimal SO2 and NOx removal eciencies:

A.A. Basfar et al. / Fuel 87 (2008) 14461452


their deposition throughout the installation. Soot particles

tend to be sticky and can lead to clogging of duct and other
pollution treatment equipment in the facility. A two-step
ltration system was applied. This solution was successful.
The by-product collected in bag lter was a white powder
devoid of soot and other particulates. For industrial plant,
a continuous ow collector (wet or dry) should be applied.
Another diculty was in maintaining a stable bag lter
operation due to sharp increase in pressure drop over a relatively short period of operation. This leads to poor release
of by-product from the bag surface. For industrial plant it
is preferable to use the electrostatic precipitator, which
shall be specically designed for collection of sticky and
hygroscopic by-product.
Fig. 6. Eect of humidity on the SO2 and NOx removal eciencies for
combustion of Arabian Heavy Oil.

4. Conclusions

Table 3
Chemical characteristics of by-product collected in bag lter in the
experiments with combustion of the three Arabian fuels

The investigation of the electron beam process for treatment of ue gas from combustion of Arabian liquid fuels
shows the following main advantages of this process over
currently used conventional ones:




HFO +10%

Loss of weight during

drying at 105 C
Water insoluble




0.33 0.005

0.30 0.005

0.96 0.05

74.4 3.7
1.59 0.05
23.79 1.1
0.02 0.001
0.04 0.002
0.16 0.008

74.7 3.7
0.51 0.025
24.3 1.1
0.02 0.001
0.2 0.01
0.2 0.001

Ion content in water soluble part

78.06 3.9
1.68 0.03
20.055 1.1
0.29 0.0014
0.009 0.0004
0.065 0.0033
Values of parameters are expressed in % wt.

Dose: 6 kGy only for SO2 removal and 12 kGy for SO2
and NOx removal,
ammonia stoichiometry: 0.95,
gas temperature at inlet to process vessel: 65 C,
gas humidity: 11.5 % vol.
An experiment with the selected process parameters was
performed with ue gas from combustion of Arabian
Heavy Fuel Oil + 10% Light Oil. SO2 removal eciency
of 98% and NOx removal eciency of 82% were obtained.
The obtained SO2 removal eciency is signicantly higher
than that of a conventional dry scrubber and comparable
to that of the wet lime scrubber systems employed in the
desulfurization of ue gas emitted from coal-red boilers.
Operational problems and developed solutions. During
the one year operation of INCT laboratory plant with
combustion of Arabian oils, no major failures were
noticed, indicating the reliability of the electron beam process. A major problem, encountered at the beginning of
this project, was removing particulate matter and soot
from ue gas before its introduction to the process vessel.
They should be removed to assure the suitability of byproduct for agricultural application as well as to avoid

Simultaneous removal of SO2 and NOx at high eciency

levels. SO2 removal eciency up to 98% and NOx up to
82% were obtained under optimal conditions.
It is a dry process which can be easily controlled and
operated. Only three parameters need to be regulated:
water and ammonia dosage to the ue gas and electron
beam current (i.e. dose).
The process yields a usable and valuable by-product. It
is a mixture of ammonium sulfate and nitrate which can
be used as such as a fertilizer or can be blended with
other fertilizer components to produce commercial agricultural fertilizers NPK or NPKS.
No wastewater is formed in the process.
Economic studies show that the investment and operation costs of the process are very competitive. In addition, revenue from by-product sale could lower the
costs signicantly.
This is the rst experimental conrmation of the applicability of electron beam technology for treatment of ue
gas from combustion of high-sulfur liquid fuels. During
the study, several limitations of the process were encountered as follows:
The energy consumption of the process is relatively high,
especially for application to ue gas with high NOx and
low SO2 concentrations. Further reduction of energy
consumption by process improvement is required.
Multi-stage irradiation and non-uniform dose distribution between irradiation stages are eective on DeNOx
and reduce energy consumption by 1520% [11].
Flue gas directed to the process should be cleaned o
soot and other particulates to a level lower than
50 mg/Nm3 for two reasons. Firstly, the particulates
present in the ue gas will contaminate the by-product


A.A. Basfar et al. / Fuel 87 (2008) 14461452

and decrease its agricultural value. Secondly, the particulates, under humid conditions, can get deposited in
ducts and other process components, which will complicate operation.
Filtration of by-product requires special attention due to
potential clogging of lters and its deposition in ue gas
ducts. This may be overcome by the use of electrostatic
precipitators and mechanical scrapers specially designed
for this purpose.
Appendix A. Supplementary data
Supplementary data associated with this article can be
found, in the online version, at doi:10.1016/j.fuel.2007.
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