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Article history: Since the complexity of sulfur capture and release during solid fuel combustion in circulating fluidized bed (CFB)
Received 16 December 2014 boilers, especially in the oxycombustion conditions is still not sufficiently recognized, the development of a simple
Received in revised form 30 March 2015 SO2 emission model for wide range of operating conditions is of practical significance.
Accepted 2 April 2015
The paper introduces the artificial neural network (ANN) approach for the prediction of SO2 emissions from CFB
Available online 22 April 2015
boilers. The model considers a wide range of parameters influencing SO2 emissions. The [16-1-6-1] ANN model
Keywords:
was successfully applied to predict SO2 emissions from coal combustion in several large- and small-scale
Modeling CFB boilers, over a wide range of operating conditions, both in air-firing as well as oxygen-enriched and
Circulating fluidized bed oxycombustion conditions.
Oxycombustion Since the method constitutes a quick and easy to run technique this approach makes a complementary tool in
SO2 emissions relation to the experimental procedures and the programmed computing approach. Therefore, the model can
Artificial neural networks be easily applied by scientists and engineers for simulations and optimizations of CFB units.
© 2015 Elsevier B.V. All rights reserved.
1. Introduction A widely used method for SO2 capture during solid fuel combustion
in CFBC is a dry flue gas desulfurization (FGD) technology, based on
Sulfur dioxide is the main S-based flue gas compound. Although thermal decomposition of limestone, followed by the sulfation reaction.
other sulfur species, such as SO3 H2S, CS, CS2, COS, SH, can be also detected This method belongs to the first of all four groups which are discussed in
in flue gas, their amount is much lower than SO2 [1–7]. the paper [8].
The source of SO2 in air-fired conditions constitutes the fuel-bound The possibility of the in situ SO2 emissions control by the addition of
sulfur. In combustion recycled flue gas, particularly in oxycombustion a sorbent, usually limestone or dolomite, directly into the combustion
conditions, SO2 from the recycled gas makes an additional sulfur source chamber, due to the low combustion temperature, is considered to be
[6]. one of the main advantages of fluidized bed boilers [5,9–12]. The
The emission of SO2 is affected by complex factors and when its con- process of dry flue gas desulfurization can proceed via indirect or direct
centration is too high the need for desulfurization of flue gas appears. sulfation [9,13–17].
An extensive review of sorbent systems for removal of sulfur oxides The investigations presented in the paper are limited to the cases
from flue gases is given in [8]. The authors distinguished four categories when if used, limestone is applied as a sorbent to retain SO2 from flue gas.
of the oxide materials intended for SO2 removal: single oxides, mixed During conventional air-fired conditions indirect sulfation of lime-
oxides, oxides supported on carbonaceous materials and oxides sup- stone occurs, including calcination (1) and CaO–SO2 sulfation (2) reac-
ported on porous silica-based materials. tions [17]:
⁎ Corresponding author at: Jan Dlugosz University in Czestochowa, Faculty of CaCO3 →CaO þ CO2 ð1Þ
Mathematics and Natural Science, Institute of Technical Education and Safety, 13/15
Armii Krajowej Av., Czestochowa, Poland. Tel./fax: + 48 343615970.
E-mail address: jkrzywanski@tlen.pl (J. Krzywanski). CaO þ SO2 þ 0:5O2 →CaSO4 : ð2Þ
http://dx.doi.org/10.1016/j.fuproc.2015.04.012
0378-3820/© 2015 Elsevier B.V. All rights reserved.
J. Krzywanski et al. / Fuel Processing Technology 137 (2015) 66–74 67
overcomes the shortcomings of experimental procedures as well as Such prepared neural network constitutes a tool for making non-
the programmed computing approach. iterative and quick calculations, giving accurate results (e.g. in extrapo-
The present work deals with the ANN technique to predict SO2 lation or interpolation problems) as an answer to new stimuli, not
concentration in flue gas from coal combustion in different, pilot and previously seen by the neural network [65].
large-scale CFB boilers over a wide range of operating conditions, both
in air-fired, oxygen-enriched and oxycombustion conditions. The neces- 2.2. Application of neural network and calculating conditions
sary training samples to learn the ANN model are taken from the exper-
imental as well as calculated data reported in literature, similar to the A highly accurate model for the prediction of SO2 emissions needs
methods described in [65,66,68–72]. some detailed information not only of each combustion process condi-
tions but also about coal-fired CFB combustors, as they are different in
2. Material and methods size; they have different height and cross-section of the combustion
chamber, e.g. circular, square and rectangular, some of them are large-
2.1. Neural network modeling scale/industrial boilers while others pilot-scale combustors. Most of
them have been fitted with cyclones but e.g. the 261 MWe COMPACT
The neurocomputing approach is applied in the paper since artificial CFB boiler operated in Turow Power Station in Poland is equipped
neural networks have the ability to simulate uncertain, ill-defined, big with two compact separators, as it constitutes the example of the boiler
and complex systems. Because of the fact, that ANNs can learn from of the second generation design [33,35,76]. The fuel properties and op-
the relationship between the input and output variables from given erating parameters for both, air-fired oxygen-enriched and oxy-
examples/stimuli, they do not need any detailed information about combustion conditions should also be taken into account to accurately
the studied processes. They operate in a similar way to a “black box” train the ANN model. All possible factors that can affect the SO2 emis-
and their learning process resembles a human brain operation. The sions are used making the model as complete as possible. Therefore,
ANN models have also the ability to ignore redundant and excess data, the set of the input parameters consists also of some operation condi-
use incomplete data sets, concentrate on more important inputs as tions, the fuel properties and geometry factors describing the combus-
well as generalize the complex relationships between input and output tion chamber. However, it is worth mentioning, that the range of the
data [65–67,73,74]. Since a single neuron has a limited memorizing input parameters set is limited due to the fact that the accessible train-
capacity, the neural network constitutes a group of interconnected (by ing data set, applied in the model, is also not so large.
so-called weights) neurons (perceptrons). The knowledge of the pro- The input parameters are: the atmosphere tag IDatm defining the
cess is acquired by the network during the learning stage, called also atmosphere mode (‘1’ for O2/N2, ‘2’ for O2/CO2 and ‘3’ for O2/Recycled
the training epoch, and it is stored in ANN structure, i.e. weights [65, Flue Gas (RFG) mode), the Ca/S molar ratio, the oxygen concentration
69]. The examined process determines the architecture of ANN, the in the inlet gas CO2, the excess oxygen EO, the primary gas ratio Pg,
activation function of neurons, the number of perceptrons in hidden the average gas velocity in the riser U, the average temperature T in
layers and sometimes the type of ANN. Therefore, there are e.g. recur- the riser, the Sauter mean diameter of the coal particles df and limestone
rent, feed-forward, Kohonen, Hopfield, Bayesian–Gaussian, probabilistic particles dl, the inlet gas pressure p, coal feed rate ṁf, sulfur (S) as well as
neural networks [63–65,67,75]. Some of them refer to supervised ones, ash content (A) in the coal (air dried basis) and three geometrical
others — unsupervised or self-organizing NN. factors describing the feeding points of limestone and secondary gas
The feed-forward type of ANN was applied in the paper [65], where in relation to the height of the combustion chamber, i.e.: height of the
neurons are arranged in three kinds of layers and form input, interme- combustion chamber H, height of secondary gas inlet/height of the
diate (so-called hidden) and output layers. The feed-forward type of combustion chamber Hsg/H, height of the limestone injection point/
ANN can contain one or more hidden layers. height of the combustion chamber Hl/H. For the cases when a boiler
In order to be a useful tool, the neural network needs to be previously was neither supplied by secondary gas nor limestone, the parameters
prepared by the following principal steps: setting of ANN architecture HSG and Hl are assumed to be 0 for calculation purposes. The input
and initial values of weights (between 0 and 1), normalization of parameters are given in Table 1.
input and output signals, the training (learning) and testing process The average temperature in the riser is considered to be the temper-
[65,74]. A suitable architecture and the proper number of hidden neu- ature defined in a similar way as it is given in [18,47,48,77]. In large scale
rons must be established to achieve the required accuracy of neural units the temperature used in simulations was the average temperature
network estimation. The learning stage with the supervised learning is
based on repeatedly presented input data and corresponding output Table 1
pattern, simultaneously. For example, during the overall heat transfer The input parameters used for training and testing the ANN model.
calculations the data sets consisted of 64, 29 and 69 input and output
Input parameter Value
sets (data patterns), for membrane-walls, SH I and SH II, respectively
a
[65]. The learning process makes it possible to modify the connection Atmosphere tag IDatm , – 1, 2, 3
Calcium to sulfur molar ratio Ca/S, – 0–9.494
weights by a suitable learning method and to adjust them to produce
Oxygen concentration in the inlet gas CO2, % 21.0–45.0
the desired output. A simple, powerful and reliable supervised training Oxygen excess EO, % 0–100
method of feed-forward neural networks is the Back Propagation (BP) Primary gas ratio Pg – 0.4–1.0
scheme [68,73]. The BP algorithm constitutes an iterative gradient Average gas velocity in the riser U, m s−1 2.28–6.2
algorithm for minimization of the mean square error, between the Average riser temperature T, K 1073–1262
Mean diameter of coal particles df, mm 0.000756–11.096
desired and predicted output. In the BP scheme the difference between
Mean diameter of limestone particles dl, mm 0.024–1.1
outputs and the pattern constitutes the measure of the weights modifi- Gas inlet pressure p, atm 1.0–9.0
cation rate. Coal feed rate ṁf, kg s−1 0.0008–71.3
The logarithmic sigmoid and the hyperbolic tangent sigmoid func- Sulfur content Sad, wt.% 0.20–6.00
Ash content Aad, wt.% 0.48–35.7
tion are the most commonly used activation functions in such ANN.
Height of the combustion chamber H, m 1.8–48
Different activation functions can also be used in different layers of the Height of secondary gas inlet/Height of the combustion 0.0–0.3
network [74]. chamber Hsg/H, –
When the criterion of the mean square error is fulfilled and the Height of the limestone injection/Height of the combustion 0.0–0.38
network has a good ability to predict accurately the validation data set chamber Hl/H, –
in the combustion chamber above the secondary gas feed points. IDatm
The tag of IDatm is named 1, 2 and 3 for O2/N2, O2/CO2 and O2/Recycled
Flue Gas (RFG) inlet gas mixtures with different oxygen concentra-
Ca/S
tion, respectively. Therefore, the air-fired, oxygen-enriched and
oxycombustion conditions are taken into account by the model.
The average gas velocity U is considered to be a superficial gas veloc- CO2
ity in the riser above the secondary gas inlet level.
Since the model is in the development stage the Sauter mean diam- EO
eter of limestone particles was used only. This issue should be also taken
into consideration during further development of the model. The Sauter
mean diameter could not be sufficient to describe the real particle size Pg
distributions, since two kinds of limestone with the same mean diame-
ter but different particle size distribution would not offer the same U
sulfur capture. To be more comprehensive and precise, the model
should also take into consideration the limestone reactivity among the T
input data.
All the input parameters are easy to acquire and applied in the
model. The output variable is the SO2 concentration in flue gas. Since df
CSO2
the number of neurons in the input and output layers are the same as
the number of input and output parameters, respectively, the input dl
and output layers consist of sixteen and one neurons, respectively.
Each neural network was prepared via a supervised learning (train- p
ing) procedure, in which 16 inputs and the corresponding output
pattern were introduced to the network simultaneously.
The normalization of input and output parameters and an instance
of Back Propagation scheme called the Lee and Park's algorithm is
applied during calculations [34,65]. This algorithm consists in changing Sad
the momentum and learning rate simultaneously.
The coefficient of determination R2 of the linear regression line
Aad
between the predicted values from the neural network and the desired
output, the mean absolute error MAE as well as the mean relative error
MRE are used to select the optimal number of neurons in hidden layers, H
i.e. to choose the best ANN architecture, characterized by the highest
coefficient of determination R2 and the lowest errors: MAE and MRE. Hsg/H
On the basis of preliminary calculations and previous experience [34,
65], a hyperbolic tangent sigmoid function is applied as an activation Hl/H
function for all perceptrons.
The necessary training samples constitute the experimental data set
of 150 input–output data pairs, obtained from large-scale and pilot- Fig. 1. The structure of the [16-1-6-1] type of neural network.
scale CFB combustors, reported in the literature [3,11,16,25,26,29,47,
48,52,54–56,77,78]. The data made it possible to apply an approach
similar to the method described in [68,69,71,72]. The values correspond the highest coefficient of determination R2 = 0.9833 and the lowest
to different combustion modes since the combustors were operating number of errors: mean absolute error MAE = 64.78 and the mean
under air-fired, oxygen-enriched and oxycombustion O2/CO2 and O2/ relative error MRE = 0.09.
RFG conditions. The concentrations of SO2 have been normalized to 6% The ANN model was successfully validated against experimental
of the oxygen content of the flue gas. The Leave-one-out methodology results, using both training and the new samples, unseen before in the
was used to select data sets. Because of the fact, that the amount of network. The approach was undertaken since the comparison between
accessible data was not so large, it was necessary to use mostly the experimental and calculated data is regarded as the most difficult type
dependent data sets. The testing data included 30 whereas validation of model's validation procedure [57,58,65].
data set contained 20 samples of which 10 were independent validation The data were collected from the wide variety of boilers, both pilot-
data sets, similar to the procedure given in [34,65]. an large-scale, operating in air-firing, oxygen-enriched O2/N2 as well as
oxy-fired: O2/CO2, and O2/RFG combustion modes.
3. Results and discussion The comparison between the predicted C pSO2 and desired C dSO2 emis-
sions of SO2 for different boilers (large- and pilot-scale) and a wide
Different ANN architectures were studied as the network's perfor- range of operating conditions, both in air-fired, oxygen-enriched and
mance depends on its structure. The number of neurons in each hidden oxycombustion atmospheres is shown in Fig. 2. The comparison for
layer varied from 1 to 16 and then the best architecture of the network new, previously unused independent data is shown in Fig. 3. Good accu-
was selected by the use of the earlier mentioned error measures. Such racy in prediction of SO2 emissions by the [16-1-6-1] type ANN model
an approach helps to reduce the risk of the memorization instead of was obtained. The calculated results are located within the range of
generalization the relationship within the data set [65,66]. ±20% compared to the experimental data.
This procedure resulted in a generation of family of neural models, Good accuracy in prediction of SO2 emissions by the model was also
including 256 networks in total. In addition, previously unused inde- observed for three of all four data points presented in [47]. However, the
pendent data were used for validating each network. prediction error for the highest value, i.e. for 14,720 ppm was too large.
The best ANN architecture turned out to be the [16-1-6-1] structure, It was due to the fact that training data set was not so large, since the
shown in Fig. 1. The ANN model consists of 7 hidden neurons forming number of accessible experimental data for oxycombustion conditions
two hidden layers. This artificial neural network was characterized by in open literature is limited. This remark has to be taken into account
70 J. Krzywanski et al. / Fuel Processing Technology 137 (2015) 66–74
Fig. 2. Comparison of the SO2 concentrations (without normalization) desired and predicted by the [16-1-6-1] type ANN. Open symbols refer to air-firing whereas closed ones apply to
oxygen-enriched and oxygen-fired conditions.
during further development of the model and the training data set The training data set, which was used to build up the model, corre-
should have been expanded. sponds to different conditions. The combustors that are considered
Figs. 2 and 3 do not indicate references, since some of the data for in the paper operated under both below and above the calcination tem-
large-scale boilers are confidential. perature. It would be difficult, especially for specific oxycombustion
Fig. 3. Comparison of the SO2 concentrations (without normalization) desired and predicted by the [16-1-6-1] type ANN for new, unused before, independent data sets. Open symbols refer
to air-firing whereas closed ones apply to oxygen-enriched and oxygen-fired conditions.
J. Krzywanski et al. / Fuel Processing Technology 137 (2015) 66–74 71
be precisely determined in this combustion mode. This is where Lower heating value (LHV) (kJ kg−1) 8200–12,100
the neurocomputing approach can overcome the shortcomings of Proximate analysis/wt.%
experimental procedures as well as the programmed computing Fixed carbon(by difference) FCar 6.50–39.90
approach. Volatile Var 17.60–22.00
Since neural networks have the ability to reproduce the process Ash Aar 6.50–31.50
Moisture War 36.00–40.00
from training samples via the learning stage, the knowledge about the
phenomenon allows ANN model to produce correct SO2 concentration Ultimate analysis/wt.%
for the given set of input variables. Carbon Car 23.90–30.40
Hydrogen Har 1.90–6.85
The obtained results show that the model is flexible enough to be
Oxygen Oar 4.57–8.61
applied for different CFB combustors [3,11,16,25,26,47,48,56,77–79]. Nitrogen Nar 0.2–0.41
Among boilers used during validation tests are three large scale Sulfur Sar 0.20–1.06
boilers, i.e.:
Table 2
Properties of bituminous coal.
Proximate analysis/wt.%
Fixed carbon(by difference) FCar 39.86–49.83
Volatile Var 24.48–29.65
Ash Aar 11.12–15.74
Moisture War 14.57–14.75
Ultimate analysis/wt.%
Carbon Cad 53.84–57.09
Hydrogen Had 4.19–44.41
Oxygen Oad 6.09–6.88
Nitrogen Nad 0.78–0.85
Sulfur Sad 0.95–1.23
Fig. 4. Schematic diagram of the 235 MWe CFB boiler [65].
72 J. Krzywanski et al. / Fuel Processing Technology 137 (2015) 66–74
Table 4
Input parameters (common data).
Table 5
Input parameters (variable data) and SO2 emissions (normalized to 6% O2 basis).
Input parameter/test no 1 2 3 4 5 6 7 8 9 10 11 12
30 kW CFB combustor
Average gas velocity in the riser U, m s−1 5.22 3.64
SO2 concentration, predicted C pSO2 , ppm 446 388 340 485 420 366 747 636 545 1170 995 845
SO2 concentration, desired C dSO2 , ppm 462
δ [%] 16
a
1 stands for: O2/N2 mode, 2 — O2/CO2 mode, 3 — O2/RFG (Recycled Flue Gas) mode
J. Krzywanski et al. / Fuel Processing Technology 137 (2015) 66–74 73
Acknowledgments
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