Chinese Journal of Chemical Engineering 27 (2019) 426–443

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Chinese Journal of Chemical Engineering

journal homepage: www.elsevier.com/locate/CJChE

Review

Advances in reduction of NOx and N2O1 emission formation in an oxy-

fired fluidized bed boiler☆
Khalid El Sheikh 1,2,⁎, Mohammad Jakir Hossain Khan 2, Mahar Diana Hamid 2, Siddhartha Shrestha 3,
Brahim Si Ali 2, G.A. Ryabov 4, Lya A. Dolgushin 4, Mohd Azlan Hussain 2,
Tatiana V. Bukharkina 1, Elena A. Gorelova 4
1
Dmitry Mendeleev University of Chemical Technology of Russia, Moscow 125047, Russia
2
Department of Chemical Engineering, Faculty of Engineering, University of Malaya, Kuala Lumpur 50603, Malaysia
3
Laboratory for Simulation and Modelling of Particulate Systems, Department of Chemical Engineering, Monash University, Victoria 3800, Australia.
4
All-Russian Thermal Engineering Institute, VTI, 14/23 Avtozavodskaya str, Moscow, Russia

a r t i c l e i n f o a b s t r a c t

Article history: Fossil fuel combustion is one of the major means to meet the mounting global energy demand. However, the in-
Received 11 January 2018 creasing NOx and N2O emissions arising from fossil fuel combustion process have hazardous effects. Thus, mitigating
Received in revised form 10 June 2018 these gases is vital to attain a sustainable environment. Interestingly, oxy-fuel combustion in fluidized bed for car-
Accepted 30 June 2018
bon capture and minimized NOx emissions is strongly sustainable compare to the other approaches. It was assessed
Available online 23 July 2018
that NOx formation and fuel-N conversion have significant limitation under oxy-fluidized bed compared to air mode
Keywords:
and the mechanism of NOx formation is still deficient and requires further development. In addition, this review
Oxy-fuel combustion paper discussed the potential of primary measure as low emission process with others supplementary techniques
Fluidized bed technology for feasible NOx reduction. The influences of combustion mode, operating parameters, and reduction techniques
Biomass blend such as flue gas recirculation, oxygen staging, biomass co-firing, catalyst, influence of fluidized bed design and struc-
Primary/ secondary measures ture, decoupling combustion and their merges are respectively evaluated. Findings show that significant minimiza-
NOx emission tion of NOx emission can be achieved through combination of primary and secondary reduction techniques.
© 2018 The Chemical Industry and Engineering Society of China, and Chemical Industry Press. All rights reserved.

1. Introduction
The current bulk production of energy to meet the needs of the
society is primarily dependent on the combustion of fossil fuels, such as
natural gas, petroleum products, and coal. Among these fuels, the use of
coal for power generation is dominant because of its abundance and
low cost compared with other non-conventional methods of power gen-
eration. However, the combustion process of the coal is always associated
with the release of harmful air pollutants, such as CO2, SOx, and NOx. Ni-
trogen oxides from coal combustion consist of nitric oxide (NO), nitrogen
dioxide (NO2), and nitrous oxide (N2O). NOx is a generic term for NO and
NO2 collectively. These derivatives of nitrogen oxides can cause a wide
range of health and environmental damages. One of the major effects is
acid rain; when NOx and SOx react with other substances in the air to
form acids and fall to the earth as rain, snow, fog or dry particles, they
can directly damage the buildings and historical monuments, besides,
☆ Supported by the University of Malaya, Ministry of Education Malaysia under the
grant FP064-2015A (FRGS) and IPPP grant number : PG101-2015B.
⁎ Corresponding author at: Department of Chemical Engineering, Faculty of
Engineering, University of Malaya, Kuala Lumpur 50603, Malaysia.
E-mail addresses: khalid51@siswa.um.edu.my (K. El Sheikh),
Mahar.diana@um.edu.my (M. Diana Hamid).
they can cause lakes and water streams to become acidic and dangerous
for human purposes and other living organism [1]. In addition, this in-
creased nitrogen loading in water bodies, particularly coastal estuaries,
upsets the chemical balance of nutrients used by aquatic plants and ani-
mals. Secondly, the nitrogen oxides also play a major role in Global
Warming. The continuous accumulation of NOx and N2O in the atmo-
sphere may cause gradual rise in earth's temperature, which causes the
rise of the sea level as well as affects the plant and animal habitat ad-
versely [2–6]. The impact of N2O on global warming of the atmosphere
is almost 300 times higher than that caused due to effect of CO2 [7]. More-
over, the toxic chemical in the air occurring by NOx and, N2O reacts with
ozone and common organic chemicals which may lead the biological mu-
tations and can deeply harm visibility [8–12]. By considering their haz-
ardous effects, the standards for regulations on NOx and N2O emission
levels from combustion plants have been set worldwide [13, 14].
Table 1 shows the NOx emission standards in several EU countries [15].
These emission standards are met by undertaking measures to control
NOx and N2O emission, which also raised the global awareness and the
need for extensive research toward the utilization of coal in an
environment-friendly manner.
The major sources of the NOx and N2O emissions are the coal-fired
power plants, such as pulverized, fixed, moving, and fluidized bed
boilers. Three mechanisms are considered for the formation of nitrogen

https://doi.org/10.1016/j.cjche.2018.06.033
1004-9541/© 2018 The Chemical Industry and Engineering Society of China, and Chemical Industry Press. All rights reserved.
 K. El Sheikh et al. / Chinese Journal of Chemical Engineering 27 (2019) 426–443
Table 1
NOx emission standards in some EU countries for coal and biomass [70]
Total rated thermal Coal, lignite and other Biomass (Straw)①
input/MW solid fuels
Finland
50–100 400 400
100-300 300 300
N300 150 150
①
6% O2.
②
7%–11% O2.
③
11% O2.
④
In case of fluidized bed combustion.
oxide: (i) thermal-NOx, (ii) prompt-NOx, and (iii) fuel-NOx. Thermal-
NOx is formed by the reaction of atmospheric nitrogen with oxygen
atoms, especially at higher temperatures (T N 1000 °C). The prompt-
NOx also forms at higher temperatures, but is induced by fuel radicals
under fuel-rich conditions. The fuel-NOx originates from the oxidation
of nitrogen compounds chemically bounded in the fuel. Compared
with the conventional power plants (pulverized, fixed, and moving
beds), fluidized beds have more advantages because they offer rela-
tively high mixing and reaction rate and can be scaled up to medium
and large sizes [16, 17]. Moreover, fluidized beds are suitable for wide
varieties of feed-stocks (from anthracite to lignite, petroleum coke,
biomass, and so on) [18, 19]. The operating temperature range in fluid-
ized bed combustors is fairly low (800–900 °C) [20]. The formation of
thermal and prompt NOx is less than 5% of the total NOx emitted and
can thus be considered negligible; only NOx formed from fuel-N is
important.
Although the use of fluidized bed for power generation is relatively
efficient and emits relatively less amount of NOx compared with pul-
verized combustion, it is still below the requirement set by the legis-
lated emission standards. To meet the imposed emission standards,
NOx reduction technologies play an important role. The NOx reduction
techniques are classified into two broad categories, namely, primary
and secondary measures. Primary measures are applied during the
combustion process, whereas secondary measures are operated in
the downstream of the combustion process. Secondary measures,
often referred as post combustion treatment or flue gas treatment,
are techniques designed to remove NOx from flue gas. Several second-
ary measures are available including (i) selective catalytic reduction,
(ii) selective non-catalytic reduction, (iii) non-selective catalytic reduc-
tion, (iv) pulsed corona discharge, and (v) electron beam flue gas
treatments [21–23]. Although NOx reduction achieved from secondary
measures is competent, it is not economical because the process is
energy extensive and requires periodic replacement of expensive
catalysts [24].
Meanwhile, primary measures are techniques that aim to adjust
the combustion parameters to reduce NOx formation during combus-
tion. Several experts have suggested that primary measures can be
an efficient way to mitigate NOx emissions [25–27]. Primary measures
are cost effective but are rather challenging and largely dependent
on the process parameters, such as temperature, fluidizing velocity,
excess air, air staging, and flue gas recirculation (FGR). Aside from
modification of the combustion parameters, advancement of the tech-
nology has also led to the realization in the modification of combus-
tion technology.
The oxy-fuel combustion technology has recently been regarded
as an emerging technology and has been under extensive research.
This technology also has numerous benefits over other technologies,
mostly toward CO2 capture [28–32]. Oxy-fuel combustion is a process
in which fuel is combusted in a stream of pure oxygen instead of air.
The combustion byproducts mainly consist of CO2 and water vapors,
where CO2 can be easily separated and sequestrated. In addition to
427
Peat① Coal and Low-high contamination Clean solid Co-firing non clean
lignite② Wood③ biomass① solid biomass①
Germany Netherland
④
300 300 250-400 100 100
300 300④ – 100 100
400–500
– – 200 200 200
CO2 capture, oxy-fuel combustion is also gaining importance in NOx re-
duction studies because this technology is always associated with low
NOx emission [27]. NOx emission from the oxy-fuel system is less than
about one-third that of combustion in air [33, 34]. Given that pure oxy-
gen is used to combust the fuel, oxy-fuel combustion is always associ-
ated with higher temperatures than conventional air combustion.
Therefore, moderation in temperature is required, which is generally ac-
complished by recirculation of flue gas (mainly CO2 and water vapor).
Similar to air combustion, oxy-fuel combustion can also be performed
in any type of combustors: pulverized, fixed, moving, and fluidized
bed. Oxy-fuel combustion in fluidized bed has been reported to have
the following additional advantages [16, 35, 36]:
(1) Fuel flexibility
(2) Operable under high oxygen concentration
(3) Reduction in area up to 50% can be achieved given the better con-
trol of combustion temperature by solid recirculation.
(4) Significant reduction in the amount of recirculation of flue gas
(5) Increased SO2 capture.
Currently, the oxy-fuel technology has been undergoing a rapid ad-
vancement. A number of pilot plants have been established and under
study to scale-up the process for commercialization [37, 38]. However,
this method is still considered to be under development and requires
more insight for advancement. Several reviews have been published
discussing the oxy-fuel technology as viable, efficient, and environment
friendly emerging technology for sustainable development [39, 40].
However, the process of oxygen separation from air to generate pure
oxygen stream is energy extensive and requires higher operational
cost. The emission units are generally expressed in terms of milligram
per mega joule (mg·MJ−1).
Although this technology is preferred and has been extensively
studied for the implementation of CO2 capture, studies on NOx emis-
sion are limited. Similar to NOx emission from fluidized bed air-
fired combustors, NOx emission from oxy-fuel fluidized bed is also
affected by several parameters [41–43]; the major control parameters
include temperature, fluidizing velocity, excess percentage of oxygen
presence, oxygen staging, types of Fluidized Bed Gasification Reactor
(FGR), catalyst, and so on. These parameters significantly affect the
NOx reduction and remain as challenges in the application of oxy-fuel
fluidized bed because they largely vary with the process conditions
[20, 25, 35, 44, 45].
The objective of this review paper is to discuss the formation of
nitrogen emission in fluidized bed conditions during the last two
decades. The first part discusses the reaction mechanism for the
formation of NOx and N2O and the effect of key parameters during flu-
idization. The second part summarizes the current research conducted
on the reduction of NOx and N2O emission from coal. Both lab and
pilot scale research works have been critically reviewed by consider-
ing the influence of operating conditions. The effect of controlling
the amount of biomass and catalyst dosages was also taken into
428 K. El Sheikh et al. / Chinese Journal of Chemical Engineering 27 (2019) 426–443

account. Lastly, the third part summarizes the recent studies on the
role of combination primary and certain secondary measures for re-
duction NO emissions.
2. The Mechanism of Formation and Destruction of NOx and N2O
The formation and destruction of NOx is a complex mechanism
where series of reactions take place and are highly influenced by
combustion conditions and forms intermediate radical compositions
[20]. Under typical fluidized bed conditions, temperatures are usually
kept low, around 800–900 °C. Therefore, the amount of formation
of NOx is acceptable as the outcome of nitrogen presents in the fuel
(i.e., fuel-N). The mechanism is a function of several factors including
the amount, phase, and volatility of the nitrogen present in the fuel,
oxy/fuel ratio (stoichiometry), bed temperature, and fixed carbon/
volatile matter ratio [30]. Nevertheless, the formation of NOx is reliant
on O and OH radicals instead of O2. Moreover, the formation of N2O
dependent on the presence of cyanides than ammonia was discussed
in details by Aemand et al. [47].
2.1. Reaction mechanism of Fuel-N
volatile-N (mainly HCN and NH3) and char-N (nitrogen remained in
the char) [52], based on nitrogen conversion during devolatilization
of fuel nitrogen. The fraction of volatile-N formed depends on the
devolatilization temperature, heating rate, and coal type. The formation
of NOx depends on the subsequent reactions of volatile-N and char-N
[53].
2.1.1. Decomposition of N through volatilization
Volatile-N is mainly decomposed into intermediate species of nitro-
gen, such as HCN and tar-N [54-56]. Other species, such as NH3 and
CNO, are also available in relevant concentrations. These species
more readily form fuel-NOx than thermal NOx because the N–H and
N–C bonds in fuel-N are weaker than the triple bond in molecular ni-
trogen that needs to be dissociated to produce thermal NO. Moreover,
the formation of fuel-NOx depends on the type of volatile nitrogen
compounds formed and proceeds with the subsequent reactions.
The process is relatively complex and results in a large number of ho-
mogenous and heterogeneous reactions. In general, the formation of
NOx and N2O from volatile-N is attributed to HCN and NH3 shown in
Table 3 [46, 57-59].

The major percentage of NOx formed in oxy-fluidized bed condition

Table 3
is caused by the oxidation of nitrogen content that is chemically bound Formation and decomposition NOx, N2O in fluidized bed conditions
to the fuel. [47]. The N content in coal can range from 0.5 wt%–2.5 wt%,
Reaction Comment
whereas 0.1 wt% (wood)–0.5 wt% (agricultural residues) in biomass
[49], as shown in Table 2. Nitrogen is chemically bounded in the 1 HCN þ 12 O2 →CNO þ 2H HCN considered as main source of N2O
form of pyridines, quinolones, iso-quinolines, amines, indoles, and 2 CharN þ 12 O2 →CNO
carbazoles. The formation of NOx is divided into two fractions, namely, 3 CNO + NO → N2O + CO2
4 N2 O→N2 þ 12 O2 On bed/char N2O is stable below 800 °C
5 N2O + Char C → N2 + CO
6 N2O + CO → N2 + CO2
Table 2 7 N2 O þ 12 O2 →N2 þ O2 Thermal deposition
Chemical composition of varieties of biomass (dry basis) and solid fuel types based on 8 HCN þ 12 O2 →CNO þ H
volatility fuel-N content [25, 50] 9 CNO þ 12 O2 →NO þ CO
No. Fuel type Proximate Ultimate analysis daf 10 CNO + H → NH + CO
analysis db 11 NH + OH → NO + H2
12 NH3 þ 34 O2 → 12 N2 þ 32 H2 O
Biomass VM FC A C O H N S 13 NH3 þ 54 O2 →NO þ 32 H2 O Formation reaction
①
1 Oak sawdust 86.3 13.4 0.3 50.1 43.9 5.9 0.1 0.01 14 NO þ CO→ 12 N2 þ CO2 Char in bed zone
2 Sugar cane bagass②③ 85.5 12.4 2.1 49.8 43.9 6.0 0.2 0.06 15 NO þ H2 → 12 N2 þ H2 O
3 Sawdust① 84.6 14.3 1.1 49.8 43.7 6.0 0.5 0.02 16 NO + NH3 → N2 + H2O
4 Mixed waste paper④ 84.2 7.5 8.3 52.3 40.2 7.2 0.2 0.08 17 NO þ CharC→ 12 N2 þ CO Heterogeneous destruction
5 Wood① 84.1 15.7 0.2 49.6 44.1 6.1 0.1 0.06
6 Pine sawdust① 83.1 16.8 0.1 51.0 42.9 6.0 0.1 0.01
7 Furniture waste④ 83.0 13.4 3.6 51.8 41.8 6.1 0.3 0.04
8 Pine pruning① 82.2 15.1 2.7 51.9 41.3 6.3 0.5 0.01
9 Fire mil residue① 82.0 17.5 0.5 51.4 42.5 6.0 0.1 0.03
10 Sorghastrum grass② 81.6 14.2 4.2 49.4 44.0 6.3 0.3 0.05 2.1.2. Formation of Char-N
11 Bamboo whole② 81.6 17.5 0.9 52.0 42.5 5.1 0.4 0.04
12 Spruce wood① 81.2 18.3 0.5 52.3 41.2 6.1 0.3 0.10
Besides volatile-N, a part of the total fuel-N persists in char after
13 Miscanthus grass② 81.2 15.8 3.0 49.2 44.2 6.0 0.4 0.15 devolatilization, which is known as char-N. During char combustion,
14 Oat straw② 80.5 13.6 5.9 48.8 44.6 6.0 0.5 0.08 char-N results in the formation of NOx and N2O. The formation of NOx
15 Poplar bark① 80.3 17.5 2.2 53.6 39.3 6.7 0.3 0.10 and N2O from char-N under fluidized bed conditions depends mostly
16 Wood residue (Min)① 69.5 12.3 0.1 48.7 32.0 5.4 0.1 0.01
on the quality and quantity of char [60-62]. Dong et al. [63] studied
17 Wood-straw residue(Min)3 69.4 15.9 3.3 50.9 33.1 5.9 0.4 0.04
18 Wheat straw (Min)② 64.3 13.6 4.7 48.5 40.1 5.6 0.5 0.08 the influence of operating conditions on char texture by pyrolysis
19 Biomass [51] (min)② 59.3 12.4 0.9 42.2 34.2 3.2 0.1 0.01 and concluded that char reactivity increases with heating rate
20 Walnut shells (min)② 59.3 12.4 1.4 42.2 34.2 3.2 0.1 0.01 and coal category. This increase is attributed to enhanced NO hetero-
21 Wood yard waste (min)④ 48.0 0.5 3.6 45.4 16.4 6.0 0.2 0.01 geneous reduction on the char surface [64]. Meanwhile, nitrogen dis-
Solid Fossil Fuel
tribution between char and volatiles during coal pyrolysis is weakly
1 Peat 67.6 28.5 3.9 56.3 36.2 5.8 1.5 0.0.2
2 Coal (Max) 51.8 71.8 52.0 86.9 29.9 6.3 2.9 9.8 dependent on coal rank [62]. According to Wójtowicz et al. [65],
3 Lignite 36.7 28.7 34.6 64.0 23.7 5.5 1.0 5.8 approximately 60% of the initial fuel-N remains in the char during coal
4 Sub-bituminous 36.4 37.2 26.4 74.4 17.7 5.6 1.4 0.9 combustion.
5 Coal 32.8 46.3 20.9 78.2 13.6 5.2 1.3 1.7
The study of Czakiert et al. [66] identified the noticeable drawbacks
6 Bituminous coal 30.0 54.3 15.7 83.1 9.5 5.0 1.3 1.1
7 Coal (Min) 12.4 20.0 5.7 62.9 4.4 3.5 0.5 0.2 of application of the oxy-fuel combustion in the case of fuel-N conver-
①
sion to NOx. Nevertheless, it has been identified that compared to air
Wood and woody biomass.
②
Herbaceous and agricultural biomass [51].
firing technique, NOx formation is lower during oxy-coal combustion
③
17-Wood-straw residue(Min)3 because of the additional reduction in NO by reaction with carbon
④
Contaminated biomass. dioxide [52, 67, 68].
 K. El Sheikh et al. / Chinese Journal of Chemical Engineering 27 (2019) 426–443 429

2.2. Influence of operation parameters
2.2.1. Bed temperature
Coal devolatilization as well as the formation of volatile-N/char-N
are strongly dependent on bed temperature. Glarborg et al. [69] re-
ported that higher bed temperature resulted in higher NO emissions.
Tourunen et al. [61] investigated the dependency of CO, NO, and N2O
emissions on bed temperature and oxygen concentration in circulating
fluidized bed combustion (CFB). Their study mainly focused on nitrogen
emission formation in the lower furnace area. Their experiments
showed that NO emissions above the dense bed decreases, whereas
N2O emission increases with decreasing temperature or oxygen concen-
tration. These trends can be explained by the heterogeneous reactions
between NO and char that decreased with temperature or oxygen con-
centration and increased the bed char inventory. Oxygen concentration
and temperature also affected NO emissions directly. Correlations for
CO, NO, N2O, NH3, and HCN concentrations at the exit of dense bed
were also developed [61]. Recently, Roy et al. [70] confirmed N2O forma-
tion is high under oxy-fuel combustion than an air. However, N2O de-
creased with an increase in bed temperature.
Duan et al. [25] studied the effect of bed temperature on NO emission
for bituminous and anthracite coals under different combustion atmo-
spheres in CFB. As a result, NO emission increased with bed tempera-
ture, which can be explained in three points:
(1) The coal char burnt more completely, and more char-N was re-
leased from the N site in the coal matrix into the gas phase to
form NO precursors.
(2) Active O and OH radicals were produced from molecular O2, and
the precursors were easier to oxidize to NO.
(3) The char and CO concentrations in the combustor decreased, and
the NO reduction reaction was suppressed.
Lasek et al. [72] studied the influence of temperature and pressure
on NOx, N2O emissions in pressurized fluidized bed combustion. They
reported significant decrease in nitrogen emissions with the increase
of pressure. These results are shown in Fig. 1,
2.2.2. Excess oxygen
Excess oxygen (λ) is stoichiometric oxygen ratio, which can be
controlled by varying fluidizing gas flow rate or fuel flow rate in
oxy-fired condition. Several researchers have studied the effect of ex-
cess oxygen ratio on NOx formation in oxy-fired fluidized bed condi-
tion [25, 35, 73]. Lupianez et al. [20] investigated the effect of excess
oxygen in 90 kWth BFB. The range of oxygen concentrations in the
O2/CO2 (25:75, 55:45) atmospheres was varied to change the excess
oxygen percentage; whereas, other parameters, such as bed tempera-
ture and catalyst, were maintained constant. Their results showed
significant rise of NO emission at higher range of excess oxygen
(ƛ = 1.5–1.7) compare to the lower range (ƛ = 1.1–1.3). The NOx
emission increased from 590 mg·Nm− 3 to 685 mg·Nm− 3 when ƛ
was increased from 1.1 to 1.7. Tan et al. [20, 74] also observed similar
trend from their experiments in a 0.1 MWth oxy-fuel CFB. These results
suggest that at higher ‘excess oxygen’ ratio the formation of NO in-
creased, which may depend on the coal type used during fluidization.
Duan et al. [25] studied the effect of excess oxygen ratio (ƛ = 1.1–1.3)
by using two different coal types in recator. Their results are shown
in Fig. 2.

De diego et al. [71] showed the increment of NO emission with de-

velopment in bed temperature. In their experiments, NO emission in-
creased until the bed temperature was 900 °C and remained constant
up to 950 °C. The increase in NO emission with bed temperature was
attributed to reduced char and CO concentrations, which led to the
heterogeneous reduction of NO on the char surface. Moreover, higher
temperature tended to promote NCO oxidation to NO.
Lupianez et al. [43] studied NOx emissions from bituminous and lig-
nite coal under oxy-firing in bubbling fluidized bed (BFB). They found Fig. 2. Effect of excess oxygen on NO emission [2].
that the effect of bed temperature on NOx emissions is less intense
and without a clear tendency. They suggested that fuel-NOx formation
is mainly controlled by the oxygen partial pressure in the surroundings
of the burning particle. Moreover, the temperature influence is not The figure shows that the NO emission from bituminous coal in-
significant, and the differences on emissions relied on the coal type. creased from 116 mg·MJ−1 to 130 mg·MJ−1, whereas emmission rate
However, the effect of temperature increased. was 72 mg·MJ−1 to 97 mg·MJ−1 from anthracite, when the value of

Fig. 1. Influence of the pressure on NO during the air/oxy condition [1].

430 K. El Sheikh et al. / Chinese Journal of Chemical Engineering 27 (2019) 426–443

ƛ was 1.1 to 1.3. The NOx emission from bituminous coal was higher at
lower value of ƛ. The reason behind this is the remarkable amount of ni-
trogen retained in the unburnt char of anthracite coal which was greater
amount than the bituminous coal.
Reduction in conversion of nitrogen species from char or solid fuel
using reasonable reduction techniques can minimize the formation of
NOx and N2O. The next sub-section reviews the different reduction
techniques together with optimized operating parameters in oxy-fired
in CFB conditions.
3. The NOx Reduction Emission Systems
Numerous studies have been conducted on NOx and N2O emission
reduction technologies in oxy-fuel fluidized bed in lab and pilot scale

Table 4
Review techniques of NOx emission issues in air and oxy firing fluidized bed

Techniques Fuel Properties Reactor configuration Operating modes Finding Ref.

Oxygen staging • Bituminous Coal 50 kWth CFB Air CO2 suppresses NH3 formation Duan et al. [83]
(dp = 0.545 mm) H = 4.2 m 21%, 30%, 40% O2/60% CO2 and increases HCN. In comparison
• Anthracite (PZ① = 0.8 m, TZ① = λ = 1.2 with conventional combustion,
(dp = 0.829 mm) 0.2 m, SZ① = 3.2 m) Primary stream fraction = 0.7 NO increase with O2 concentration.
ID
PZ = 0.122 m
SZ = 0.15 m
Catalyst and • Central Europe bituminous BFB OF The excess oxygen is the dominant Lupiáñez et al. [84]
combustion coal H = 2.5 m AF variable influencing NOx emissions,
conditions • Spanish high-sulfur lignite ID = 0.2 m OF with RFG both for AF/OF-firing. Nitrogen
Blend AF: O2 = 21% conversion rates to NOx are within
OF: O2/CO2 (%) 5%–25%, being significantly dependent
40/60, 25/75 on fuel volatiles/char split and
Bed Temperature: 820–900 °C excess oxygen.
Fluidization velocity
0.88–1.71 m·s−1
Load (kWth)
25–71
Catalyst and • Anthracite (700–1200 μm) 90 kWth AF The higher the excess oxygen, and Lupiáñez et al. [79]
combustion BFB OF bed temperature, the higher the
conditions H = 2.5 m O2/CO2: 25%, 40% and 55% O2 NO emissions.
ID = 0.2 m T = 800–950 °C oxy-fuel FB combustion optimization
λ = 1.1–1.7 of the desulfurization efficiency, but
Ca:S = 0,2.5,4 the increase of free CaO enhances
NO emissions
Steam staging • Distilled spirit lees FB reactor N2/O2 Added steam lowered the NOx at low Zhu et al. [85]
• Char (900 °C) H = 0.76 m O2 concentrations (e.g., b35 vol-%)
• Char (950 °C, steam) ID = 0.068 m and steam addition amount (mass
ratio below 0.8).
At high O2, added steam cause higher
NOx formation than without steam
addition.
steam added (mass ration of 1.0)
NOx decreased, O2 no effect
Gas-staging • Synthetic coal char M6 Lab scale fixed bed OF High level CO and temperature Wang et al. [86]
Catalyst (prepared in tubular quartz reactor T 950 °C results in an increase reduction N2O,
quartz reactor) Fe2O3 promotion on N2O reduction
with high concentration CO
Recycling Flue Gas • Bituminous American, Chinese 50 kWth T = 857–891 °C NOx emission was much lower Duan et al. [15]
(warm) • Petroleum coke Chinese CFB O2 = 21%–23% in oxy-fuel than that in air combustion.
The reduction by gas phase in
reaction in flue seem to be to take the
dominant role.
Blending fuel • Municipality solid waste BFB T = 700 °C, 800 °C, 900 °C At 30% MSW addition to the coal, Lu et al. [16]
(MSW) H = 1.1 m λ = 1.3 both NO and N2O emissions showed
• Lignite ID = 0.077 residence time = 1.5–2 s the lowest values (391.85 ppm and
Blending ratio: 10%, 20% 55.33 ppm, respectively at 900 C).
and 30% MSW
Oxygen staging • Chinese coal –Datong (DT) 0.1 MWth O2 concentration: 40%–50% Result of Increasing secondary flow Tan et al. [17]
(high O2 CFBC Secondary air: H = 1.5 m ratio, SO2 emission increases and NO
concentration) H=6m emission decreases.
ID = 0.10 (bot)
ID = 0.14 (top)
Gas-staging • Low volatile anthracite 90 kwth Primary air at distributor plate NOx control is depending on the Lupianez et al. [18]
(700–1200 μm) BFB Secondary air at: 0.4 and 0.80 m volatile content of the coal.
• High sulfur lignite H = 2.5 m (above distributor plate) Coal rank different content CO and
(700–1200 μm) ID = 0.2 m Secondary gas ratio SO2, there concentration effect NO
(%) = 0,10,20 formation/depletion mechanisms
Ca:S = 4
Fluidization medium:
Air
oxy (O2/CO2) = 28/72, 45/55
T = 850, 925 °C
λ = 1.4, 1.5
①
PZ — Primary zone; TZ — Transition zone; SZ — Secondary zone.
 K. El Sheikh et al. / Chinese Journal of Chemical Engineering 27 (2019) 426–443 431

since 2005. Carbon Capture and Storage (CCS) technology has been
intensively studied in large scale to improve with the passage of
time by some research centers such as: VTT in Finland, CIRCE
in Spain, Alstom in USA and others. In lab scale, Czakiert et al. [66]
studied the fuel behavior under oxy-fired CFB conditions and their
effect on NOx emissions; they found an increase nitrogen conversion
with increase in excess oxygen. Jia et al. [75] investigated the effect
of recycling flue gas on reduction NOx, and also extended their
studies on SOx emission. Their results exhibited low NOx emissions
for the oxy-fired condition, even at higher temperature. Moreover,
they showed that high oxygen concentration can increase the rate
of NOx reduction. Thereafter, Li et al. [76] studied NOx and SOx emis-
sions under CFBC under high oxygen, and observed higher NOx
(ppm) in oxy-condition compared to the air combustion condition.
On the other hand, Duan et al. [77] studied NOx emission during co-
firing biomass with coal under oxy-fuel condition and noticed that
the addition of biomass can have a positive effect on NOx reduction.
Another study by Stewart et al. [42] and Tan et al. [78, 79] using lab
and pilot scale power plant CFBC under air and oxy-fuel mode exam-
ined the effect of H2O (g) on SOx, formation and NOx emission with
adding limestone to optimize the reduction process with tempera-
ture. In addition, Hofbauer et al. [80], Duan et al. [77] and Li et al.
[81] investigated the effect of recycling flue gas on emissions. They
confirmed higher reduction in wet and dry recycling flue gases.
Li [76] and Li et al. [82] investigated the effect of steam with various
oxygen concentration on NOx, and achieved significant reduction in
high oxygen concentration. However, N2O decreased by height of
the boiler.
According to these researches, the formation of NOx greatly depends
on combustion parameters, such as the characteristics of solid fuel,
operating temperature, oxygen availability, combustor design, and
firing configuration. All the combustion parameters need to be moni-
tored to develop an effective reduction technique. This process may
be developed by implementing the primary measures that aim to
adjust the combustion operating parameters (temperature, oxygen Fig. 3. Effects of combustion atmosphere on nitrogen emissions [3].
availability, and so on), either to reduce the formation of NOx or de-
formed the NOx formed inside the furnace.
Internal modifications of combustion system and conducting reac-
tions at minimum reaction temperature and/or the reducing contact
period of nitrogen to the fuel along with oxygen in the reaction phase, [73] observed by recycling flue gas the fractional conversions of fuel-N
while creating a fuel-rich zone. These techniques reduce NOx emissions into NOx and N2O in oxy-mode to be significantly lower than in the air
around 50%–80%, and are simple and cost effective. The available litera- combustion. They explained the effect of RFG on NOx, N2O, can extend
ture discussed on NOx reduction techniques in air/oxy-firing techniques the reduction from 80% to 95% including the fractional contributions
has been shown in Table 4. of CO2 and H2O.
The effect of FGR in Bubbling Fluidized Bed (BFB) combustor
3.1. NOx and CO2 recirculation profile was studied by De Diego et al. De Diego et al. [71] used various gases
(CO2, SO2, and NO) on dry base at two different temperatures (850 °C,
Flue Gas Recycle (FGR) is known as an effective method in emis- 950 °C) to simulate different compositions of dry recycle flue gas.
sions reduction. In (FGR) the flue gas is recycled back to the combus- Their experimental results showed that the recycled flue gas with
tion zone to reduce the formation of NOx, either by reducing the flame 650 vppm reduced NO concentration at 850 °C from 60%–70%. How-
temperature and overall excess oxygen or by increasing the concen- ever, Hu et al. [26] confirmed that further reduction results could be
tration of CO2 [34, 87]. The effect of recycling flue gas (O2/CO2) and achieved when recycling NO or NO2 in recycle flue gas. Compared to
(NOx/CO2) on NOx, N2O has been studied in fluidized bed condition De Diego et al. [71] showed that the result of dry recirculation was
by several authors [34, 42, 50, 71, 77, 88]. Qian et al. [88] investigated 65% NOx to N2. Moreover, they mentioned 850 °C as an optimum tem-
the effect of RFG on NOx reduction in a vortex fluidized bed under perature. In addition, the recycled flue gas can be dry or wet. De Diego
air condition. They reported that recycling NOx not only minimized et al. [71] compared the result between dry and wet FGR in oxy-fuel
but also inhibited the formation NOx by reducing the combustion condition at 950 °C and suggested that Wet FGR could be more effec-
temperature. tive in reducing NOx. Stewart et al. [42] and Zhu et al. [89] have stud-
The effects of FGR on nitrogen emissions have been investigated at ied the effect of wet FGR on NOx concentration in (ppm) and fuel-N
different compositions under air and oxy-fuel combustion conditions conversion to NO x in percentage using (30% O 2 –70% CO 2 ) oxygen
as shown in Fig. 3(a) and (b) [50]. The results indicated that the imple- concentrations at varied temperatures. Results of Zhu et al. [89, 90]
mentation of FGR in air firing mode tends to increase the formation are shown in Fig. 4.
of NOx, whereas it seems to increase the formation of N2O in oxy- Reduction in both NOx and N2O was observed using steam. The use
combustion. The formation of N2O increased at the inlet of the reactor of steam may be significant for nitrogen emission; however, its utiliza-
because of recirculation of N2O; however, its contribution was lessened tion requires more insight toward corrosion, combustion efficiency,
along the height, as shown in Fig. 3(b). Moreover, Hosoda and Hirama and formation of N2O [42].
432 K. El Sheikh et al. / Chinese Journal of Chemical Engineering 27 (2019) 426–443

Fig. 4. Conversion ratios of fuel-N to (a) NO and (b) N2O with different temperatures (BC and inlet gas composition: 30%O2þ70%CO2) [4].

Yoshiie et al. [42, 50] investigated the formation of NOx and N2O 3.2. Oxygen staging
in a drop tube furnace by varying the combustion mode and fuel-N
content in their experiments. Their results are summarized in Table 5. Staging in typical fluidized beds refers to a method in which the total
air supplied in the reactor is divided into ratios at different locations,
usually as primary (under-fire) and secondary (over-fire). This investi-
Table 5 gation has focused on oxy-fuel combustion because the O2 concentra-
Fuel-N content and NOx, N2O formation for different types of coal [19] tion is limited to 21% and can be varied independently, which is
Coal type Fuel-nitrogen/% Release in air Release Release in referred as oxygen staging. This process is in contrast to combustion
condition/ppm inO2/CO2 oxy-fuel with air, in which the formation of NOx is a function of oxygen concen-
condition/ppm condition/ppm tration although the air is staged. Various lab and pilot scale experi-
NOx N2O NOx N2O NOx N2O ments with different solid fuels have been conducted to investigate
Coal O 1.05 – – 53 80 55 95 the effect of oxygen concentration in the formation of NOx and N2O
Coal E 1.88 25 150 10 160 15 170 [25, 43, 44, 51, 74, 91].
Coal M 2.52 – – 12 245 18 260
3.2.1. Oxygen staging in primary flow
NOx emission increases with oxygen concentration in primary
stream. At low temperature and oxygen concentration in the dense
bed, the concentration of CO2 and CO increases, consequently reducing
The authors elaborated that the relationship of char-N to coal-N NOx to N2 [74]:
ratio was dominated by the nitrogen conversion ratio from NO and
N2O. However, the N2O emission at the exit point was a function of HCN þ OH→HCO þ H2 O ð1Þ
nitrogen content in the original coal. Therefore, the N2O emission
concentration seems to be high in oxy-CFB, and RFG cannot minimize HCO þ O→NO þ CO ð2Þ
such concentration. Thus, the use of different types of catalyst may
be applicable. NCO þ NO→N2 þ CO ð3Þ
 K. El Sheikh et al. / Chinese Journal of Chemical Engineering 27 (2019) 426–443
In addition, NO is reduced by CO as follows:
1
CO þ NO→CO2 þ N2
2
Char-N conversion was low with O2 concentration in the primary
stream because the volatile consumed a lot of oxygen. Incomplete
oxidization of carbon, together with CO2 gasification, produced large
amount of char and CO, which enhanced the NO/Char reduction reac-
tion. However, the NOx emission increased slightly with increasing O2
concentration in the primary flow [74]. The similar trend was ob-
served by Duan et al. [25] for two different types of coal as shown in
Fig. 5.
Fig. 5. Effect of oxygen staging on NOx using different type of coal [2].
At 14% O2 concentration in the primary stream, the NOx emission
was similar for both bituminous and anthracite coals. Meanwhile, NOx
emission for bituminous coal was higher by 50 and 40 mg·MJ− 1
at 30% and 40% O2 concentration, respectively. Recently, Li et al. [82]
studied the effect primary and secondary staging on formation N2O.
They showed increased in excess oxygen concentration in primary
Fig. 6. Normalized NOx emission from Anthracite (Left) and Lignite (right): effect of secondary gas ratio [5].
433
stream increases N2O. However, with increasing combustion tempera-
ture concentration of N2O decreased.
ð4Þ
3.2.2. Oxygen staging in secondary flow
Secondary oxygen staging is applied at non-rich fuel area to regulate
formation of NO with height of gasifier or combustor [25]. Lupianez et al.
[51] investigated the effect of staging on NOx formation in lab scale
BFB under two different secondary/total ratios (S/T) of 0%–10% and
10%–20%. The staging results showed higher reduction in NOx emission
at S/T ratio of 0%–10%. Experiments were carried using coal in bubbling
fluidized bed reactor at 90 kWth station to compare anthracite and lig-
nite at same atmosphere 45/55 O2/CO2. The result showed significant
NOx reduction only on Lignite coal due to higher amount of volatiles
released in Fig. 6 [51, 67].
However, in Fig. 7 shows NOx emission from anthracite coal at
different atmospheres, the first concentration under 30/70 O2/CO2,
NOx emission reduced around 37%. However, under 50/50 O2/CO2
the variation is minor, the no advantages obtained by the secondary
staging in this case. That explains the limitation of oxygen second-
ary staging on NOx emission in different types of fuel and various
atmospheres.
Li et al. [76] studied the effect of oxygen concentration in secondary
flow in 1 MWth pilot scale oxy-CFB. They considered different oxygen
concentrations (30%, 40%, and 55%,) in secondary flow, their result
showed that NOx concentration decreased gradually to 55, 50, and
42 mg·MJ− 1, respectively. Another experiment was conducted by
Mingxin et al. [92] in circulating fluidized bed to study the relation be-
tween primary and secondary staging ratios on NOx emission. Their
results are shown in Fig. 8 which delineate the change in axial profile
of NO concentration in combustor. It can be seen clearly that the
50/50 staging gave the lowest emissions at FG1. Reduction of NOx by
secondary air (S.A) is more obvious at higher temperature due to the
intensified NOx emission [93].
4. Influence of Fluidized Bed Design and Structure
Fluidized Bed Technology (FBT) has been considered as one of the
best options to reduce the NOx emission because of its user-friendly and
flexible operating and design facilities such as, excellent heat and mass
transfer uniformity, lower temperature requirement for operations and
434 K. El Sheikh et al. / Chinese Journal of Chemical Engineering 27 (2019) 426–443
Fig. 7. Normalized NOx emission from Anthracite: effect of secondary gas ratio [6].
opportunities of conducting multiphasic reactions for energy production
[94-101].
4.1. Effects of design and structure variations of reaction systems
The process design and structures provide control to the fluidized bed
boiler which is beneficial for dynamic performance, efficiency, imple-
mentation cost and emission control [102]. Sirisomboon et al. [103] com-
pared biomass firing in pilot combustors with advanced conical fluidized
bed at the same operating condition. They concluded that the greater res-
idence time and more uniform distribution of the combustion air across
the bed allowed operation to be lower in NOx emissions. The details of
fluidization state specification (FSS) have been reviewed by Runxia Cai,
et al. [101]. They have discussed to achieve ultra-low NOx emission,
some design principles have been followed and modified such as:
(1) the separators and ash coolers were improved,
(2) the position of discharging ports was modified
(3) the particle size distribution of feeding coal was reduced
Fig. 8. Effect of SG and location on NO emission profile along the combustor [8].
In addition, the reduced particle size of fly ash has proven to
give higher efficiency and finer bed material. Hence, compared with tra-
ditional CFB boilers, the pressure drop of the dilute zone increased to
over 1.0 kPa. Higher-pressure drop indicated the higher solid concen-
tration in the dilute phase and the higher solid inventory. As a result,
the NOx emission was significantly reduced. The influence of nozzle
structure in NOx emission was investigated by Zhu et al. [104]. They
studied pulverized coal combustion in circulating fluidized bed boiler
by using 3 different types of secondary air nozzle structure (center, an-
nular, and circular ports), with various ratios and tertiary air position of
the boiler. Fig. 9 shows the results obtained from their study. The varia-
tion in NOx concentration is identical under both annular and circular
secondary air nozzles. The released-N remained stable in the reducing
zone. When tertiary air position changed from 600 mm to 1200 mm
below the top, i.e., the length of the reducing zone was greater, NOx con-
centrations decreased during combustion. Concentrations of reduced
NOx increased because the reducing ratio of NOx increased in tandem
with the length of the reducing zone, resulting in a marked drop in
NOx emissions.
Fig. 9. NOx emission with different secondary air Nozzle structure only/uniformly injected,
at 600/1200 mm blew the top down-fired combustor [9].
 K. El Sheikh et al. / Chinese Journal of Chemical Engineering 27 (2019) 426–443 435

NOx &
NO2

Cyclone
Hopper

Fluidization
Reactants Zone

Gas
chromatography
Carrier
U-type valve
gas
Distributor

Fig. 10. Schematic of a decoupled fluidized bed reactor with NOx and NO2 testing facility.

4.2. Decoupling combustion
Decoupling of fluidized bed reactors for combustion has been
considered as a developed new clean technology for the purpose
of NO x and N 2O emission reduction [105, 106]. Devolatilization
and fuel combustion takes place in during traditional fluidized
bed combustion, whereas in the decoupled fluidization the com-
bustion process go through three steps: (1) pyrolyzation of fuel
particle takes place at the bottom section of the reactor (2) in the
second stage the pyrolyzed products are burned in the reactor col-
umn at fully fluidized conditions and (3) the unburned particles
are separated form gas by passing the gas–solid fluid through a cy-
clone and send back to the system again. This extra step plays a
vital role for the reduction of NOx and NO 2 [107] The schematic
of a standard decoupled fluidized bed reactor has been shown in
Fig. 10.
As consequence, the idea of decoupling reactions actually provides op-
timization on the reaction behaviors and performances. Number of
researcher's had been studied decoupled combustion in last decade. Li
dong et al. [107] used coal and biomass and achieved around 19% NOx
emission less than traditional way of combustion intensely NOx reduction
till 33% by merging decoupling combustion with air-staging and
reburying. The comparison is shown in Fig. 11 [108]. Moreover Zhennan
Han et al. [83, 109] compared to the direct combustion of DSL in CFB com-
bustion, the operating mode of first pyrolysis or partial gasification of fuel
and then combustion of fuel gas can bring a stable combustion easily, and
effectively inhibit the produced NOx, reaching the level of 50 μl·L−1 com-
pared to 160 μl·L−1 in old-style combustion.

Fig. 11. Comparison of NOx emissions during direct combustion and decoupling combustion [10].
436 K. El Sheikh et al. / Chinese Journal of Chemical Engineering 27 (2019) 426–443

Fig. 12. NOx emission pathways.

5. Influence of Biomass and Catalyst Additives on NOx Emissions
5.1. Co-firing coal and biomass
Biomass is a promising renewable source of CO2 neutral fuel.
Co-firing or blending biomass with coal can be a cost-effective and
environment-friendly method for minimizing the existing pollution
problems [110-117]. Given that the biomass is composed of higher
volatile and lower nitrogen content, co-firing may lead to the reduction
of NOx emission [118-120]. Moreover, biomass is highly reactive be-
cause of the presence of cellulose, hemicelluloses, and lignin contents
with weaker bonds and higher alkali/alkaline earth metallic species,
which plays a key role in the thermal chemical process [121-123].
The main objectives of blending biomass and coal are to reduce NOx
emissions in fuel content, improve boiler efficiency, and reduce fuel
cost. During co-firing, knowledge on fuel properties and qualities is re-
quired because of their significant effect on NOx emission. However,
combustion conditions, for example, bed temperature, freeboard

Fig. 13. NOx emission for different biomass bituminous coal blends.
 K. El Sheikh et al. / Chinese Journal of Chemical Engineering 27 (2019) 426–443 437

Table 6
Proximate and ultimate analysis of bituminous possible blend with different biomass on % wet basis [20]

N Parameter Bituminous Coal/% Wood chips/% Sugarcane/% Coconut shell/% Bagasse/% Lignite/%

1 Moisture 5.55 7 4 6.5 50 48.5

2 Ash 34 0.37 1.75 6.50 1.5 7.0
3 Carbon 44.14 48.80 49.00 49.75 23.5 29.06
4 Fixed 34.5 38.11 38.27 38.85 18.35 22.69
carbon
5 Hydrogen 3.23 6.37 5.85 5.8 3.25 2.35
6 Sulfur 0.59 0 0 0.05 0 0.5
7 Oxygen 11.58 44.4 43.36 36.7 21.75 12.31
8 Nitrogen 0.91 0 0 1.2 0 0.28

extension, and excess oxygen, are key to successful operational con-
trol. The present paper aims to establish the effect of biomass addition
on fuel-N reduction and oxygen availability under various operating
conditions.
During co-combustion, synergistic effects of coal and biomass
blending can lead to reduction in emitted pollutant, especially NOx.
The co-combustion mechanism of fuel can be divided into two stages:
the initial stage of devolatilization and then the combustion of the re-
maining char. During volatilization, some of the fuel-N will be released
as volatile-N, while others will remain as char-N. Based on the first
Fig. 14. NOx emission during staging in co-combustion [11].
assumption for co-firing made by Glarborg et al. [48], HCN and NH3
are the dominant species formed as nitrogen-bearing intermediates.
The formation ratio of both species is dependent on specific combus-
tion condition and nitrogen content of fuel. For biomass combustion,
only NH3 as nitrogen intermediate species can be considered based
on the second assumption made by Álvarez et al. [68]. NOx emission
pathways from co-combustion of coal and biomass are shown in
Fig. 12.
NOx emissions were dependent on biomass volatility and the oper-
ating conditions, shown in Fig. 13, Tables 2 and 6 [124].
Fig. 13 shows drop in NOx emission by their highest ratio in blends
with coal. Some studies have been conducted to analyze the effect of
biomass and coal co-combustion on NOx and N2O emissions in oxy-
fuel fluidized beds [38, 125-129], as well experiments have been carried
out in small and large scale [125, 130-133]. The conducted test on
thermo-gravimetric analysis [134, 135] suggested that co-firing can be
an effective NOx reduction technique. In addition co-combustion of
coal and biomass can be adopted to reduce N2O emission in high
nitrogen-content coal [136]. However Duan et al. [84] recently reported
that burning biomass alone has higher NOx emission than coal. Lower
nitrogen concentration was evidently observed by Duan et al. in co-
combustion oxy-fuel by shifting to 30% oxygen staging in 10 kWth
CFBC shown in Fig. 14.
Similar results were also observed by blending wood pellets at
different ratios with different ranks of coal, as shown in Fig. 15.
Furthermore, oxygen staging reduces NOx emission in co-firing
mode during oxy-fuel combustion. Table 7 summarizes several experi-
ments and their results under air/oxy firing/CO2-firing in fluidized bed
combustor.

Fig. 15. Effect of biomass ration on NOx emission in oxy-fuel combustion [12].
438 K. El Sheikh et al. / Chinese Journal of Chemical Engineering 27 (2019) 426–443

Table 7
Review of NOx studies on air/oxy co-firing fluidized beds

Reactor type Coal and biomass Conditions Effects Ref.

Temperature/°C Fluid

BFB Lignite and anthracite 850 Air NOx emission decreased as the percentage of olive [21]
Olive cake (dried) cake fuel blending increased.
BFB High volatile bituminous 850 Air Accumulation of sludge ash will exhibit the NOx emission. [22]
Medium volatile bituminous Sludge ash only plays minor role in N2O emission.
Semi-anthracite
Dry sludge
BFB Central Europe bituminous 800–900 Air Nitrogen conversion rate significantly dependent [134]
Spanish high sulfur lignite 25/75 O2 RFG on fuel volatile/ char.
Excess O2 favor NOx emissions and plays dominant
role compared to bed temperature and CO concentration.
BFB Wet sludge 830–870 Air RFG led to a decrease in NOx emission [23]
Dry sludge 21/79 O2/N2 RFG Semi-dried and wet sludge exhibit a tendency of
Semi-dried sludge NOx reduction with increase in O2 while dry sludge
gives an opposite effect
CFB Eastern bituminous 750–950 Air 30/70 O2 RFG① Recycle ratio shows significantly lower than [24]
Kentucky bituminous 35/65–45/55 O2 RFG oxy-fuel pulverized fuel combustion required.
Petroleum coke NOx emissions exhibit lower in oxy –firing
compared to air firing even at high temperature
(950 °C) in fluidized bed.
CFB Sub-bituminous (Puertollano) 575–875 Air Excess O2 favor NOx emission [25]
Bituminous (Carbocol) NOx emission reduced as Ca/S ratio increased.
CFB Bituminous 800–1000 Air Excess O2 favor NOx emission. [26]
28/72 O2/N2
35/65 O2/N2
CFB Lignite 565 Air NOx emission decreased with fraction of biofuel
Willow all for type of biomass.
Forest biomass
Sunflower husk
CFB Bituminous 800–1000 Enriched air (35%) Higher partial pressure of O2 in oxy-firing favor [27]
21/79–35/65 O2/CO2 conversion of fuel-N
High temperature in air firing shows strong effect
toward NOx emission.
CFB Polish coal 830–860 Air Type of biomass plays vital role on NOx emission as [28]
Wood amount of char contribute to NO reduction.
Sewage sludge Advanced air staging method contributes a strong
reduction of CO and NO concentration compared to
normal air staging.
DFB Wood 848–890 Air Nitrogen exclusively reals in gasifier [29]
MSW And need two stage producer gas cleaning
Bark equipment to implement
①
Recycling flow gas.

An experimental study on the conversion of Fuel-N to NOx was
carried out by G. Pu, et al. [137] in a bubble fluidized bed under high
oxygen concentration at different temperatures — first for coal alone
(Antharcite) where the NOx conversion rate increased by 1.98%.
Secondly by coal mixed with 20% pine powder where the nitrogen
emission was decreased by 3.39%.
Lowering the fuel-N content, biomass produces significant amount
of ash compared with coal, which has been shown to induce catalytic
effect [138-140]. Kalembkiewicz [141] reviewed ashes from co-
combustion of coal and biomass and termed it as an industrial
waste. However, other researchers [142, 143] reported that the ash
is composed of constituents, such as AL2O3, CaO, and TiO2, which
are considered catalytically active compounds that reduce SOx and
NOx emissions during the combustion processes. In addition, the
ash of biomass also exhibits strong catalytic activity toward the oxi-
dation of emission gas precursors, such as HCN, CO, and CH4. The
selectivity of HCN to produce NO is higher than that of N2O forma-
tion [144].
5.2. Influence of catalytic reduction
Reduction in SOx, NOx and N2O by absorption–desorption using
sorbent/catalyst such as bauxite, quartz sand, dolomite, limestone
and other bed material has been in practice for the last two decades,
been proven to reduce emission gases. But the challenges were in
the selection of catalyst for NOx reduction in fluidized bed reactor.
There are other factors like temperature variation, chemical stability
and reaction retention time that are also proven to be considered
as effective operation conditions [2, 6, 145]. The opportunities for
in-situ catalyst/s as bed material to reduce of NOx in FBC have been
studied by number of researchers and classified catalyst in groups,
shown in Table 8.
5.2.1. Thermal stability
The catalyst groups mentioned in Table 8 have been classified
by Khanh-Quang Tran et al. [146] such as zeolites, noble metals and
metals oxides; all were effective toward HC-SCR of NOx at different
temperature ranges (800–900)°C in fluidized bed [147, 148]. Suggested
Cu–Fe/ZSM-5 as catalyst, which showed higher NOx conversion in lower
temperature and better performance will be achieved by varying the
amount of cooper and iron [147, 148].
5.2.2. Mechanical stability
The second major concerns in fluidized bed include excessive sor-
bent attrition and short residence time of catalyst. Therefore, catalysts/
sorbents that are mechanically stable and have higher capability
of absorption are anticipated. Nevertheless, an internal circulation
fluidized bed (i-CFB) was suggested by Cheng et al. [149] to in-
crease the residence time and minimize iteration of the catalysts.
The hydrodynamic behavior coupled with the reaction kinetics to simu-
late the performance of i-CFB for NOx reduction was also studied [149-
151].
 K. El Sheikh et al. / Chinese Journal of Chemical Engineering 27 (2019) 426–443 439

Table 8
Classification Catalysts used to reduction NOx from Fluidized bed combustion [30]

Catalyst name Sample Activation T/°C Activity notes Others remarks

Zeolites Cu-ZSM-5 500 Most active catalyst. This type desorbed NOx at Active research to improved
higher temperature
Noble Metal Pt, alloys, Pt-AL2O3 700 Add silver and Gold enhance the catalyst activity Long life time, highest resistance against O2, SO2
to Pb-La2O3 to 827 °C
Metal Oxides Cr, Fe, Co, Ni, 750 Activity increase by addition Silver to cobalt oxide Quite Stable for long term ‘Perovskite catalyst”,
Ba2Cu3O7, La2CuO4 high thermal stability, but low surface area and
inferior, catalyst under development

5.2.3. Limestone effect
Limestone in the form of Ca and CaO is widely employed as catalyst
bed materials mainly for sulfur retention. The interaction between de-
sulfurization and NOx formation in fluidized bed combustor by lime-
stone addition has been broadly studied [126, 152-154]. Studies have
suggested that the use of Ca and CaO as catalyst aids in sulfur retention,
but results in increase of NOx emission [153]. The solid phase of CaSO4
and CaO has a negligible effect on NOx, especially CaO restrained release
from char-N [155]. However, the catalyzed limestone [156, 157] can sig-
nificantly affect the formation and destruction of NO. The formation of
NO from NH3 occurs because of the catalytic effect of CaS:
5 CaS 3 flying ash reduction, implantation of various fluidized bed designs and
NH3 þ O2 → NO þ H2 O
4 2
Similarly, CaS can also catalyze NO to N2.
CaS 1
NO þ CO → N2 þ CO2
2 and CCS systems may result in high efficiency, low (SOx, NOx) emission,
In addition, N2O reduction can also be examined with the use of Ca
and Cao as catalysts [158]. The mechanism of CaS catalytic decomposi-
tion and reduction of N2O was studied by Lingnan et al. [159] and the de-
struction of N2O occurred with Ca and CaO according to Reaction (19).
Ca þ N2 O→CaO þ N2
catalyst for adsorption/reduction of NOx. The catalyst showed a good
performance in CFB in the presence of different hydrocarbons, H2O,
and temperatures. Nickel-based catalysts are active for tar reduction
and NH3 decomposition [161]. Almost all NOx precursors were con-
verted to N2 by Ni/AL2O3 catalytic reforming at 650 °C in the presence
and absence of steam during the pyrolysis process in gasifier, with an
enrichment in hydrogen in fixed bed reactor [162]. Similarly, significant
increase in NOx reduction rate was achieved in the presence of CO and
solids, such as SiO2, Al2O3, Fe2O3, CaO, TiO2, and K2O in fluidized bed
in the absence and presence of water vapors [142].
Finally, this paper reviewed possibility of primary reduction tech-
niques such as combustion modification, renewable fuel, catalysts and
ð5Þ
structures including process decoupling combustion through oxy-fired
fluidized bed boiler to meet the requirement of ultra-low NOx, N2O
emission. These techniques as discussed earlier lead to virtuous contra-
dictory NOx reduction. However, the combination of reduction tech-
niques in oxy-fuel technology fluidized bed based power generation
ð6Þ
low energy penalty and capital costs. Nevertheless, with the important
advantages of this technology some secondary measures for NOx miti-
gation can be incorporated easily. The challenge of multi-objective opti-
mization parameter, design, control structures and further fluidized bed
modifications is necessary to encounter new strict air pollution require-
ments expected in the near future.
ð7Þ

Zhao et al. [85] studied the effect of mineral matters (Na, Ca) on NOx
reduction. Fig. 16(a) and (b) shows their results at different oxygen con-
centrations and increasing temperature for LK coal, with and without
mineral matter (LK) and (LK-de). The NOx emission from LK started at
lower temperatures and reached its maximum quickly. However, NOx
emission from LK-de started at relatively high temperature and then
changed gradually. They concluded that the mineral matter present in
the coal promotes oxidation of fuel-N.
Besides mineral matter catalyst, metal catalysts have also been studied
to analyze their performance. Yang et al. [160] prepared Fe/ZSM-5
6. Advanced Reduction
The advanced flue-gas purification technologies were imple-
mented by merging between primary and secondary measures to
meet environmental requirements of ultra-low NOx emission. The
European conditions target to estimate nitrogen emission to be less
than 200 mg·Nm− 3 for pilot scale, therefore this combination can
be considered as one of most perspective methods. A number of studies
related to the deployment of hybrid of various existing technologies
such as RFG, oxy-fuel combustion, co-combustion, SNCR, etc. can

Fig. 16. NOx evolution profiles during temperature programmed combustion of coals with various O2 concentration; (a) LK, (b) LK-de [13].
440 K. El Sheikh et al. / Chinese Journal of Chemical Engineering 27 (2019) 426–443

potentially meet the emission reduction proficiently and economically.
Recent research activity in fluidized bed condition has been targeted
to merge different combinations such as less nitrogen content biomass
combustion with reduction in NO emission by injecting NH3 [163].
They achieved around 84% NOx reduction using NH3 and urea in 58
MWth CFBC. In addition, they highlight the economic impact of
implementing SNCR. The demonstration unit known as CIUDEN CFB
pilot plant [164] has provided an experimental platform for CCS by
injecting NH3 into the cyclone to sustain concentration NOx emission
at 120 mg·m− 3. Similarly, research work have been conducted in
pulverized coal facilities on the development related to the combination
of co-firing, oxygen enrichment and SNCR [86]. Tests were carried out in
a 20 kW down-fired furnace by fixing the optimum position for ammo-
nia injection; oxygen enriched over-fired air (OFA) and optimum blend-
ing portion for two different biomass with coal. Fig. 17 shows the
significant reduction with high initial NO biomass for blending ratios
of SM with RC2.
On the other hand the new reduction emission technology applied in
China known as dry multi emission control (D-MEC) [165] for ultra-low
emissions includes the technologies of desulfurization, denitrification,
dust removal and removal of multi-component pollutants. This was
achieved through the installation of SCR (catalyst) binder in pulverized
coal boiler or CFB boiler and was targeted to NOx reduction. This tech-
nology has been applied in a number of power projects, for example:
Shanxi province power station with the capacity of 350 MW. They
have achieved NOx emissions of less than 50 mg·m-3.
7. Conclusions
This review paper demonstrated several methods and experimental
techniques applied in reducing NOx and N2O under oxy-fuel condition.
The rules and regulations on gaseous emissions are becoming stricter
each year. NOx formation and fuel-N conversion has significant limita-
tion under oxy-fluidized bed compared to air mode. However, the

Fig. 17. NOx reduction when applying NH3 with co-combustion and air staging [14].
 K. El Sheikh et al. / Chinese Journal of Chemical Engineering 27 (2019) 426–443
mechanism formation is still not fully understood and need further
studies to investigate the mechanism.
Temperature, pressure and excess oxygen are the important oper-
ating parameters influencing the NO emissions. The NO emissions
strongly dependent on bed temperature, higher bed temperature
leads to higher NO emissions. Moreover, NO emissions decreased
with the increase of pressure while it increased at higher range of excess
oxygen. However, the influence of the operating parameters on NO
emissions was found largely relying on the type of coal and the amount
of nitrogen present in it. Moreover, the formation of NOx greatly de-
pends on combustion parameters, such as the characteristics of solid
fuel, operating temperature, oxygen availability, combustor design,
and firing configuration. Depending upon the operating condition
and fluidized bed design various minimization techniques, which in
turn enhance the development of more complex technology toward
new eco-technological system are needed. The different minimization
techniques to reduce NOx and N2O emissions in oxy-FB combination
technology can be summarized as follows:
(1) Recycling NOx not only inhibits the formation NOx by reducing
the combustion temperature. In addition, reduction in both NOx
and N2O was observed using steam.
(2) Excess oxygen concentration in primary stream increases N2O.
However, with increasing combustion temperature concentra-
tion of N2O decreases. Reduction of NOx by secondary air is ob-
served at higher temperature due to the intensified NOx
emission [93]
(3) Developing stages of decoupling fluidized bed combustion tech-
nology in oxy-fuel need to be implemented for biomass as a
source of renewable energy for low emission.
(4) The role of catalyst in reducing nitrogen emissions especially on
N2O in oxy-fluidized bed condition can play a dominant role in
the future.
(5) NOx emissions can be further inhibited by nozzle structure by
rationally arranging tertiary air positions. The challenge is to im-
prove fluidized bed design control in oxy-combustion condition
toward energy efficiency and low NOx emission.
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