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Article history: In this study, external flue gas recirculation was considered to reduce nitrogen oxides (NOx) emissions in the
Received 29 February 2016 heating flues of a coke oven battery. The thermal and prompt NO formation was numerically investigated
Received in revised form 4 June 2016 employing an accurate 3-D representation of the heating flue geometry that the most popular Polish coke
Accepted 8 July 2016
oven battery. Originally the developed model was experimentally validated as a transient coupled model for
Available online 19 July 2016
the representative heating flue and the two coke ovens. Then the coupled model was simplified to the heating
Keywords:
flue model only with realistic boundary conditions on the heating flue and coke oven interface. As a result of
Coke oven battery the heating flue model simulations, the range of the reversed flue gas ratio was found for typical thermal loadings
Heating flue of the heating wall to effectively reduce NOx formation. The obtained results showed the significant effect of the
Coke oven gas considered flue gas recirculation on NOx formation reduction. Namely, the recirculation ratio of 0.2 resulted in
NOx reduction 50% of the NOx reduction efficiency.
External flue gas recirculation © 2016 Elsevier B.V. All rights reserved.
1. Introduction profiles of the temperature, density and porosity for a semi-coke bed.
However, this approach does not accurately include the impact of the
Coke is a fuel that is used in various technical processes, e.g., in iron combustion process in a combustion chamber. Therefore, numerical
production in the blast furnace [1]. Thus, the coke production technolo- coupled models of the coke and combustion chambers have also been
gy in coke ovens is still an important branch of industry. However, those developed. Smolka et al. [4,5] introduced a numerical model with
production processes may be fairly harmful for the environment. There- time-dependent heat flux profiles transferred from the heating flues
fore, it is important to monitor and reduce the emissions from coke oven to the coke bed. Jin et al. [6] also developed a three-dimensional tran-
gas (COG) combustion. sient mathematical model that included coupled coking and combus-
The coke oven battery, where the coke is produced, consists of coke tion chambers.
chamber charged by blends of coking coals and adjacent heating flues. In coke oven operations, in addition to effective coke heating, a low-
In the combustion chamber, the thermal energy, which is necessary emission combustion process is essential. To predict the quantity of gen-
for the process of the dry distillation of coal, is produced by burning gas- erated NOx, an appropriate mathematical model of NOx formation
eous fuel. The blast furnace gas (BFG) or purified COG is often used in needs to be employed. Loffler et al. [7] considered the influence of differ-
this application [2]. In the coking process, the most important problem ent mechanisms of NOx generation on the overall NOx emissions for the
is to obtain the appropriate final value and uniform distribution of the premixed combustion of natural gas in a one-dimensional plug flow re-
coke temperature within the whole space of the entire coking chamber. actor. As a result, a simplified model of thermal NOx was presented. The
The desired coke temperature in the centre of the coking chamber is NOx content was computed based on the temperature and species dis-
1273 K, which requires a high temperature combustion process. Such tribution. Weiss et al. [8] ran calculations of NOx generation in a coke
conditions generate a large amount of NOx, which is harmful to the oven using BFG and COG as a fuel. For this purpose, the prompt and
environment. thermal NOx fields were predicted, and a non-premixed combustion
Numerical simulations of thermal processes in coke oven batteries model was employed. The aim of that work was to examine the impact
using computational fluid dynamics (CFD) modelling have been used of various combustion conditions on NOx generation. Rieger et al. [9]
in various works. A great deal of attention has been paid to modelling modelled the formation of NOx in a blast stove for the combustion of
the coking chamber, where the coal-to-coke conversion occurs. Guo enriched blast furnace gas. That work considered two methods for
and Tang [3] presented numerical results of the COG flow pattern and modelling the turbulence-chemistry interaction: the eddy dissipation
concept (EDC) and a PDF-flamelet model. The NOx emission simula-
⁎ Corresponding author. tions using EDC produced more accurate results when compared to
E-mail address: jacek.smolka@polsl.pl (J. Smolka). the actual plant emission values.
http://dx.doi.org/10.1016/j.fuproc.2016.07.010
0378-3820/© 2016 Elsevier B.V. All rights reserved.
S. Gamrat et al. / Fuel Processing Technology 152 (2016) 430–437 431
The methods that have been applied for reducing NOx emissions results of this work demonstrate some tendencies and potential of
can be mainly divided into primary and secondary methods [10,11]. the EFGR technology. In particular, the results with a gradually mod-
Among the primary methods that relay on a proper operation of ified amount of the recycled flue gas are discussed and compared
combustion process, the most significant are staging air in the com- with cases without EFGR. In general, this primary NOx reduction
bustion process, reburning and flue gas recirculation processes method exhibited a very promising effect in the coke oven heating
[12–15]. Currently, recirculation is applied in the considered coke system for recirculation ratios ranging from 0.2 to 0.25.
oven battery as an internal process that occurs through the recircula-
tion window between the upward and downward heating flues. This 2. Numerical model
method of recirculation works well, however, the amount of recycled
flue gas cannot be controlled. Usually, this process does not allow for 2.1. Heating flue model
the effective reduction in the generation of NOx. Another problem is
the uncontrolled mixing of flue gas with air and COG. To overcome In general, a coke oven battery consists of a series of heating flues ar-
these deficiencies, external flue gas recirculation (EFGR) can be con- ranged in rows on both sides of the coke ovens. Heating flues are sup-
sidered. This method is used in many different industrial units [16– plied from the bottom with air and the purified COG. The air and COG
18]. These authors reported a positive impact on the NOx emission are preheated in a ceramic heat exchanger that works as a regenerator
reduction and temperature uniformity in the combustion domain. by accumulating heat from the hot flue gases from the combustion
This technology can be installed on an existing object, which is an ad- chamber. As shown in Fig. 1, a single combustion chamber is divided
ditional advantage. into two heating flues: an upward heating flue, where air and fuel are
In this paper, a numerical model of NOx reduction using EFGR in supplied, and a downward heating flue, where the flue gas outlet is
the heating system of a coke oven battery is proposed. Hence, the located.
main contribution of this paper is to provide the results of an appli- In the upper part of chamber, there is a bridge window, where the
cation of a well-established method of NOx emission reduction to gases change their flow direction. In the lower part of the heating flue,
the most popular coke oven battery in Poland. To predict the influ- there is a recirculation window designed for internal recirculation be-
ence of the coking chamber on the combustion chamber operation, tween both flues. The combustion cycle for one direction inside the
the heat flux profile was introduced as a boundary condition. Typical chamber lasts approximately 20 min. Then, the flow direction is re-
values of the heat flux were obtained from previous work [4] using versed, i.e., the air inlet becomes the flue gas outlet and vice versa. The
coupled models at various instants of the coking process, and the whole coking process takes approximately 15 to 20 h.
model was finally formulated as a steady-state process. Due to the Therefore, every numerical analysis of the heating system opera-
high temperatures that occur in the combustion chamber, the tion in the coke oven battery should be performed as a time varying
model described by Loffler et al. [7], in which the thermal mechanism case. This type of approach was presented in the previous authors'
of the NOx generation has a prevailing role, was also employed in work [4]. The developed model the whole heating system was for-
this study. In EFGR, changes in flow, species and the temperature of mulated as a transient coupled model of the heating flue and coke
the air and flue gas mixture are taken into account. The presented oven. On the other hand, the combustion process itself can be a
steady-state process if a single reverse period is taken into account. heat transfer was modelled using the Discrete Ordinates (DO) model,
Changes in this process originate from the intensity of heat transfer where the Radiative Transfer Equation (RTE) is defined as [19]:
through the heating walls only. Then, a steady-state mathematical
model can be employed that includes different values of the heat ∇ ðIλ ðr; sÞsÞ þ ðaλ þ σ s ÞI λ ðr; sÞ
flux as a boundary condition on the heating walls. In this study, Z4π
σs
such a formulation was used to simulate the NOx emission from ¼ aλ n2 I bλ I λ ðr; s0 ÞΦðs s0 ÞdΦ0 ð6Þ
þ 4π
the heating flue model. 0
2.2. Governing equations where I is the intensity, which is defined as a function of the place where
the ray starts r and its direction s, a is the absorption coefficient, σ is the
The general governing equations that describe the combustion pro- Stefan-Boltzmann constant, n is the refractive index, Ibλ is the black
cess in the heating flue are [5] now discussed. body intensity, s' is the scattering direction vector, and Φ is the phase
coefficient. The spectral radiation properties of the optically active gas-
• Energy: es, i.e., CO2 and H2O, were calculated using the Weighted Sum of Gray
Gases (WSGG) model. In this approach, the radiation from the gases is
approximated by a finite number of gray gases of different absorption
!
∂ðρuÞ X coefficients and one transparent gas. The most accurate and theoretical-
þ ∇ ðρvhÞ ¼ ∇ ðk∇T þ τ vÞ−∇ hi J i þ Sh ly sound procedure for evaluating the values of the WSGG model coeffi-
∂t i
ð1Þ cient is to use the spectral emissivity data of CO2 and H2O molecules
X ZT
p stored in an appropriate database such as HITEMP 2010 [20]. The proce-
J i ¼ −ρDi ∇yi h¼ hi yi hi ¼ cpi dT u ¼ h−
i
ρ dure for computing the radiation constants is cumbersome and time
T ref
consuming. The data available in Ansys FLUENT are those proposed by
[21]. These data are limited to H2O and CO2 partial pressure ratios equal
where ρ is the density, u is the internal energy, t is the time, h is the spe-
to 1 and 2, respectively. Several research groups are focusing on the im-
cific enthalpy, k is the effective thermal conductivity, v is the velocity
pact of the atmosphere on radiative transfer and are developing compu-
vector, T is the temperature, τ is the effective stress tensor, J is the diffu-
tation tools suitable for addressing ratios smaller than one, as can
sion mass flux, S is the source term in the transport equation of the sca-
happen when large amounts of flue gases are recirculated.
lar quantity, D is the mass diffusion coefficient, m is the mass fraction, cp
is the isobaric specific heat and p is the pressure.
2.3. Combustion model
• Momentum:
For the combustion process modelling, the global reaction mecha-
nism was used [5]. The turbulent-chemistry interaction was modelled
∂ðρvÞ using EDC [22]. The two-step COG oxidation reaction mechanism was
þ ∇∙ðρvvÞ ¼ −∇p þ ∇∙τ þ ρg þ S ð2Þ assumed.
∂t
where g is the gravitational acceleration vector, and S is the source term CH 4 þ 1:5O2 ¼ CO þ 2H2 O ð7Þ
in the momentum transport equation.
CO þ 0:5O2 ¼ CO2 ð8Þ
• Continuity:
H 2 þ 0:5O2 ¼ H2 O ð9Þ
Table 1
μ Material properties of the flue gases and heating flue walls (temperatures in K).
ρðv∇κ Þ ¼ ∇ μ þ T ∇κ þ Sðμ T ; κ; vÞ−ρε
Pr k
ð5Þ Quantity Gaseous subdomain Solid subdomain
μ ε ε2
ρðv∇ε Þ ¼ ∇ μ þ T ∇ε þ C ε1 Sðμ T ; κ; vÞ−C ε2 ρ Density Ideal gas model ρ = 1800
Pr ε κ κ
Specific heat Polynomial function of the c = 0.25116 ∙ T + 768.633
Thermal temperature and the mass-weighted k = 0.000628 ∙ T + 0.9334
conductivity average for the mixture
where κ is the turbulent kinetic energy, μ is the dynamic viscosity, Pr is Dynamic –
the Prandtl number, ε is the dissipation rate of the turbulent kinetic en- viscosity
ergy, and Cε1 and Cε2 are constants. The gaseous phase was modelled as Diffusivity –
an absorbing-emitting medium of the temperature and composition Absorption Weighted sum of gray gas model –
coefficient
that depend on the absorption coefficient. In this work, the radiative
S. Gamrat et al. / Fuel Processing Technology 152 (2016) 430–437 433
The air and COG compositions, mass flow rates and temperatures
that were defined at both inlets of the heating flue for the case without
EFGR are listed in Table 2.
For the boundary conditions at the heating walls, the heat flux
resulting from the coking chamber neighbourhood was assumed. The
value of the heat flux profile was the same for both heating walls and
was determined on the basis of the results obtained from the coupled
model of the heating flue and coking chamber. These results were consis-
tent with the heat demand monitored in the typical coke oven battery. In
the first hours of the coking process, when intensive evaporation occurs,
the average value is 5000 W/m2. In the second stage, the average heat
flux drops to 2000 W/m2. Therefore, the following average values of the
heat flux boundary conditions were employed in this study: 2000, 3000,
4000 and 5000 W/m2. It has to be noted that in the first minutes after
the coke oven charging with wet hard coal, the heat demand is much
higher than the mentioned values. This period was taken into account
in this study.
2.6. External flue gas recirculation Fig. 2. Scheme of the EFGR system.
where Hin, Hair and Hrec are the mixture inlet, the air inlet and the
where m _ in , m
_ air and m
_ rec are the total (mixture) inlet, air inlet and the
recirculated flue gas total enthalpies, respectively, Tair and Tout are the
recirculated flue gas mass flow rates, respectively. The mass flow rate
air inlet and flue gas outlet temperatures, respectively, and cpairi and cpouti
of the recirculated flue gas was computed on the basis of the recircula-
are the air inlet and flue gas outlet specific heats of the ith component
tion ratio that was defined as
gas.
_ rec
m In the last step, the mixture inlet temperature was determined on
R¼ ð15Þ the basis of the inlet enthalpy, the mass flow rate, and the mass-aver-
_ out
m
aged specific heat of the mixed air and flue gas:
_ out is the flue gas outlet mass flow rate.
where m
H in
T in ¼ ð20Þ
_ in ∙cpave
m
Table 2
The mass flow rates, temperatures and mass fractions of the air and the COG inlets of the
heating flue. where Tin is the mixture inlet temperature, and cpave is the mass-aver-
Air COG
aged specific heat of the mixture that was computed from
specific heat and temperature for the air-heating flue mixture were increase with the increase in the recirculation ratio. This was expected
computed. These values were then prescribed to the air inlet boundary because with the higher recirculation ratio, more flue gases, of which
condition (see Fig. 1). CO2 and H2O are the main components, are recirculated. The changes
The base case for the comparison purposes was computed for the in these fractions in comparison with other recirculation ratios can be
zero recirculation ratio. Since the mass flow rate of the air-flue gas mix- clearly observed near the air inlet because the recirculated flue gas is
ture was assumed constant at the inlet of the heating flue model, more added to the air. Moreover, visible changes can be observed in the
flue gas recirculated resulted in a lower value of the air excess ratio. downward flue where triatomic gases are well mixed with other flue
Then the recirculation ratio was increased until the value of 0.3 that gas components. The increases in the CO2 and H2O fractions cause an
corresponded to the air excess ratio near unity. Moreover, numerical abatement of the O2 mole fraction. This causes a decrease in the air ex-
simulations were performed for the mentioned recirculation ratios in- cess ratio. A recirculation ratio of 0.3 results in nearly 0% of the O2 mole
volving heat flux values ranging from 2000 W/m2 to 5000 W/m2 as fraction, so further analysis of the higher recirculation ratio was aban-
the boundary conditions for both heating walls. doned. In this case, the maximum CO2 mole fraction reached approxi-
All the computations were performed employing high-performance mately 9%, and H2O mole fraction reached a value of approximately 24%.
computing cluster installed at ITT, Gliwice, Poland. The approximate The volume-averaged and maximum gas temperatures in the com-
time consumption for a typical case run in parallel on 20-node machine bustion chamber are presented as a function of the recirculation ratio
was 30 h. The convergence of the numerical computations was moni- in Fig. 4. A general observation is that the average gas temperature in-
tored using the governing equation residuals and the field values. creased with the growing recirculation ratio. This phenomenon has
two causes. The first cause is the rise of the hot flue gas fraction at the
2.7. NOx formation mixture inlet. The second is the higher content of triatomic gases in
the flue gas mixture, which are not transparent to radiation. Simulta-
During the gaseous fuel combustion process, NOx is mainly pro- neously, this caused a drop in the maximum gas temperature. Obvious-
duced due to prompt and thermal mechanisms. The first mechanism ly, the highest changes in the maximum gas temperature for the
is mostly focused on modelling hydrocarbon radicals such as CH and particular recirculation ratio were obtained for the case with the highest
CH2. that react very rapidly with nitrogen and, in consequence, NOx heat flux value of 5000 W/m2, which was transferred from the heating
are generated. In the present work, the global kinetic parameters were flue to the coke oven. The average temperature was practically the
used to control the rate of NOx formation without modelling the same for that case. In contrast, the maximum temperature of approxi-
many subsequent reactions [23,24]. The second mechanism contributes mately 2500 K was almost constant for a heat flux of 2000 W/m2. This
more to the overall NOx formation. The source of NOx is nitrogen pro-
vided to the combustion chamber with an oxidiser. This path is
governed by three reactions:
O þ N 2 →N þ NO ð22Þ
N þ O2 →O þ NO ð23Þ
N þ OH→H þ NO ð24Þ
The first reaction requires very a high activation energy that is used
to break the triple bonds of N2 to atomic nitrogen and nitric oxides. For
this reason, the thermal mechanism becomes important only at temper-
ature higher than 1800 K [25]. In NOx modelling using this mechanism,
the third reaction is also important. This reaction should be taken into
account for stoichiometric and fuel rich regions. The thermal NOx mech-
anism assumes that the rate of formation and consumption of N atoms
are equal, so that the NOx formation can be defined as
where kf,1, kf,2 and kf,3 are the rate constants for the forward reactions,
and kr,1 and kr,2 are the rate constants for the reverse reactions. To
solve this equation, the concentrations of O and OH must be deter-
mined. In this study, the O and OH radicals were modelled using a par-
tial-equilibrium model [26]. This model accounts for the participation of
the third-body in the creation of the oxygen radicals that is important
when high temperature differences occur within the computational
domain.
In Fig. 3, the mole fractions of the gas mixture species such as CO2
and H2O are presented as a function of the recirculation ratio. The field
is depicted in the cross-sectional view through burners (see Fig. 1). In Fig. 3. Mole fraction fields in the cross-sectional view shown in Fig. 1 for (a) CO2 and (b)
Fig. 3, it can be observed that the amounts of CO2 and H2O generally H2O.
S. Gamrat et al. / Fuel Processing Technology 152 (2016) 430–437 435
Fig. 4. (a) Volume-averaged and (b) maximum temperatures in K of gases in the heating Fig. 5. Temperatures in K of gases at the (a) inlet and (b) outlet of the heating flue.
flues.
Fig. 7. (a) The NOx emissions in PPM and emission reductions and (b) the mole fraction
fields of NOx in the cross-sectional view shown in Fig. 1 as a function of the
recirculation ratio.
Fig. 6. Temperature field in K in the cross-sectional view shown in Fig. 1 for wall heat used, the NOx pollution abated linearly with EFGR intensification. For
fluxes of (a) 2000 W/m2 and (b) 5000 W/m2.
a recirculation ratio of 0.3, the recirculation efficiency exceeded 80%.
Therefore, EFGR also appears to be a crucial primary method to reduce
practice, a case with 20% recirculated flue gas should be considered. A NOx emissions in the coke industry.
NOx generation reduction of nearly 50% in the emissions can be obtain-
ed in that case. In this case, the flue gas recirculation led to the oxygen Acknowledgements
content decrease in a primary combustion zone and it ensured a more
uniform distribution within the whole combustion zone. As a result of The authors gratefully acknowledge the financial support of the pro-
the oxygen dilution that substantially slowed down the NOx forming re- ject Competent mechanical engineers for energetic sector no
actions, the NOx reduction was observed. The other aspect that influ- POKL.04.01.02-00-131/12. The work of JS and WA was partially sup-
enced the NOx reduction was lowering the peak flame temperature ported by the statutory research fund of the Faculty of Power and Envi-
which led to a reduction of the thermal NOx formation as well. Fig. ronmental Engineering.
7(b) shows the molar fraction fields of NOx. It can be observed that
the recirculation implementation eliminated the generation of large References
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