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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
c
Institute of Nuclear Chemistry and Technology, 03-195 Warsaw, Dorodna 16, Poland
d
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
Abstract
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
*
0016-2361/$ - see front matter 2007 Elsevier Ltd. All rights reserved.
doi:10.1016/j.fuel.2007.09.005
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
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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.
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Table 1
Properties of Arabian liquid fuels
Property
Density at 15 C
Gross heating value
Kinematics viscosity at 50 C
Sulfur content
Ash content
Unit
3
kg/m
MJ/kg
cSt
%wt
ppmw
AM
AH
HFO
878
43.29
7.33
2.81
115
890
43.31
15.45
2.90
268
980
43.43
175.0
3.10
45
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Table 2
Composition of ue gas from combustion of three Arabian fuels measured
at process inlet
Parameter
Unit
AM
AH
HFO + 10% LO
SO2
NOx
O2
H2O
CO
CO2
CxHy
Sulfur content in oil
ppmv
ppmv
% vol.
% vol.
ppmv
% vol.
% vol.
% wt.
1215
153
4.40
8.48
0
12.4
0.18
2.81
1270
168
3.42
9.06
0
15.5
0.16
2.90
1250/1355a
169
3.78
9.58
36
13.6
0.17
2.7/3.1
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Fig. 3. SO2 and NOx removal eciency as a function of dose with and
without ammonia for the combustion of Arabian Medium Oil.
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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:
Parameter
AM
AH
HFO +10%
LO
0.77
2.4
1.39
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
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
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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.
09.005.
References
[1] Baukal ChE. Industrial combustion pollution and control. New
York: Marcel Dekker; 2004.
[2] Tokunaga O, Suzuki N. Radiation chemical reactions in NOx and
SO2 removals from ue gas. Radiat Phys Chem 1984;24:14565.
[3] Matzing H. Chemical kinetics of ue gas cleaning by irradiation with
electron. Adv Chem Phys 1991;80:315402.