Fuel Processing Technology 92 (2011) 349355

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Fuel Processing Technology

j o u r n a l h o m e p a g e : w w w. e l s ev i e r. c o m / l o c a t e / f u p r o c

Estimation of free-swelling index based on coal analysis using multivariable

regression and articial neural network
S. Chehreh Chelgani a,, James C. Hower b, B. Hart a
a
b

Surface Science Western, University of Western Ontario, London, Ont., Canada N6G 0J3
Center for Applied Energy Research, University of Kentucky, 2540 Research Park Drive, Lexington, KY 40511, USA

a r t i c l e

i n f o

Article history:
Received 13 November 2009
Received in revised form 22 August 2010
Accepted 26 September 2010
Available online 20 October 2010
Keywords:
Free-swelling index (FSI)
Proximate and ultimate analysis
Regression
Articial neural network

a b s t r a c t
The effects of proximate, ultimate and elemental analysis for a wide range of American coal samples on
Free-swelling Index (FSI) have been investigated by multivariable regression and articial neural network
methods (ANN). The stepwise least square mathematical method shows that variables of ultimate analysis are
better predictors than those from proximate analysis. The non linear multivariable regression, correlation
coefcients (R2) from ultimate analysis inputs was 0.71, and for proximate analysis input variables was 0.49.
With the same input sets, feed-forward articial neural network (FANN) procedures improved accuracy of
predicted FSI with R2 = 0.89, and 0.94 for proximate and ultimate analyses, respectively. The ANN based
prediction method, as a rst report, shows FSI is a predictable variable, and ANN can be further employed as a
reliable and accurate method in the free-swelling index prediction.
2010 Elsevier B.V. All rights reserved.

1. Introduction
Coke is an expensive component in the steel-making process [1]
where about 90% of the coke produced from blends of coking coals is
used to maintain the process of iron production in the blast furnace
[2]. The plasticity of coal during heating, measured by rheological tests
of coals in their softened state [3], is the major factor responsible for
coke formation [4].
The uid and swelling properties of coals relate to the ability of the
reactive components in a coal to fuse with the inert material in the
coal, thereby making a strong coke. Impurities present in coke affect
its performance in the blast furnace by decreasing its role as a fuel in
terms of carbon available for direct and indirect reduction roles and its
role as a permeable support. These impurities include moisture,
volatile matter, ash, sulfur, phosphorous, and alkali contents [2].
In spite of the relative smallness in the amount of inorganic mineral
content, the rank and chemistry of the parent coal strongly inuences
the optical textures of cokes [58]. Some mineral matters (for example,
calcium-containing substances) deteriorate the thermoplastic properties of coals, decrease their swelling and simultaneously favor the yield
of solid residue (coke) [9,10].
Because the inorganic components of the coal remain in the coke,
the ash content of the coal can have an adverse affect on the coke
quality. Coke properties decrease in proportion to increasing ash
content of the coal [11,12]. Diez et al. investigated how coke reactivity
is affected by ash components, especially Fe2O3 and K2O [2]. The alkali
Corresponding author. Tel.: + 1 519 702 9356.
E-mail address: Sos4552@gmail.com (S.C. Chelgani).
0378-3820/$ see front matter 2010 Elsevier B.V. All rights reserved.
doi:10.1016/j.fuproc.2010.09.027

content of coal, which is measured by ash composition, will accelerate

coke reactivity [3]. Goscinski and Patalsky emphasized the importance
of Fe2O3 and CaO contents [13]. When these oxides are present in
eutectic proportions the catalytic effect of the ash on coke reactivity is
enhanced [11]. In addition, approximately 75% of the sulfur in coal
remains in the coke [3] and as it increases, coke productivity in the
blast furnace decreases [2].
Fluidity, dilatation, and free-swelling index (FSI) are all useful
indicators to predict the strength of coke that can be made from a parent
coal [1]. FSI (determined according to ASTM D 720) is a test that rates a
coal's ability to swell during heating [3], and denotes the caking capacity
of coal [14,15]. FSI is determined by comparing the size and shape of the
resulting solid button with a series of standards and assigning a value
from 1 to 9 at intervals of 0.5 [14]. According to the test, standard FSIs are
classied into weakly (02), medium (24), and strongly (49) caking
ranges [16].

Table 1
The number of samples for different states.
State

Number of samples

State

Number of samples

Alabama
Illinois
Kansas
Iowa
New Mexico
Oklahoma
Tennessee
Virginia
Wyoming

733
16
21
53
29
29
51
320
16

Colorado
Indiana
Kentucky
Missouri
Ohio
Pennsylvania
Utah
West Virginia

96
97
798
65
581
354
66
366

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S.C. Chelgani et al. / Fuel Processing Technology 92 (2011) 349355

Table 2
The ranges of proximate and ultimate analysis of coal samples (as received).
Variables

Minimum

Maximum

Mean

Std. deviation

Moisture
Volatile matter
Ash
Hydrogen
Carbon
Nitrogen
Oxygen
Pyritic sulfur
Organic sulfur
Hydrogen exclusive
Oxygen exclusive
SiO2
Al2O3
CaO
MgO
MnO
Na2O
K2O
Fe2O3
TiO2
P2O5
SO3

0.90
25.70
1.00
3.60
46.70
0.60
2.00
0.00
0.00
3.08
1.12
0.00
0.00
.0.00
0.20
0.00
0.00
0.00
0.00
0.00
0.00
0.00

11.10
45.30
20.00
6.10
82.20
2.00
19.50
7.26
3.57
5.74
13.38
73.00
39.00
30.00
2.90
0.94
8.40
4.40
69.00
3.20
2.80
19.00

3.89
34.03
11.73
5.06
68.39
1.40
11.72
.8472
0.72
4.63
8.26
45.48
24.71
2.91
0.85
.032
0.50
1.85
14.15
1.27
0.42
2.64

1.55
3.02
4.82
0.34
5.41
0.26
2.55
1.32
0.48
0.37
1.62
13.05
7.61
3.91
0.40
0.07
0.72
0.98
14.66
0.55
0.42
3.01

Some problems associated with the test method (ASTM D 720)

include variability in heating rates, variability in the degree of oxidation
or weathering of the coal sample, and, an excess of ne coal in the
analysis [16]. If the FSI can be predicted from basic coal characterization
data, there may be an opportunity to provide a predictive to assess the
coking capacity of a particular coal.
The aim of the present work is the assessment of properties of a wide
range of American coals with reference to the determined FSI and
possible variations with respect to proximate, ultimate and ash analysis
of coals using regression and articial neural networks. To our
knowledge, this is the rst cited issue that investigates the predictability
of FSI, and relationship between common coal analyses with free
swilling index.

2. Experimental data
Data used to test the proposed approaches are from U.S. Geological
Survey Coal Quality (COALQUAL) database, open le report 97-134 [17].
The database includes the determined proximate and ultimate analysis,
as well as free-swelling index (FSI) on an as received basis. The samples
with more than 20% ash, and volatile matter (dry ash free) less than 32%,

Fig. 1. Distribution of difference between actual and estimated FSI from Eq. (3) according to coking ranges.

S.C. Chelgani et al. / Fuel Processing Technology 92 (2011) 349355

as well as the samples with proximate and/or ultimate analysis different

from 100, were excluded from the database. A total of 3691 set of coal
sample analysis were used, the number of samples for different states
shown in Table 1.

351

higher K2O contents in coal (0.20) results higher FSI. No other elemental
analysis parameters were signicant. The ranges of proximate and
element analysis of coal samples are shown in Table 2. The best
multivariable equations between the proximate and element analysis
and FSI can be presented as the following equations:

3. Result and discussion

FSI = 15:3450:535 M0:205 VM:11A
The stepwise variable selection procedure was used to prepare
regression equations. As input sets for the regression, traditional
analyses of coal (proximate, ultimate and element analysis) were used
and different combinations of variables were examined.

3.1.1. Proximate and element analysis

By a least square mathematical method, the correlations of variables
(moisture and elemental analysis) with FSI value were determined.
According to relationships, higher moisture contents (a rank parameter
at low rank coals) can result in lower FSIs (0.60). Similarly, volatile
matter can have a somewhat less adverse affect on FSIs (0.26), and

FSI = 15:7430:542 M0:232 VM0:3 SiO2

+ 0:637 Na2 O0:235 P2 O5 + 0:014 Fe2 O3 + 0:041 CaO
+ 0:172 K2 O0:176 MgO

3.1. Regression

R2 = 0:45

R2 = 0:47

FSI = 15:7171:001M + 0:034M2 0:201VM0:029SiO2

+ 0:024CaO0:217MgO + 0:179K2 O
+ 0:627Na2 O0:252P2 O5 + 0:012Fe2 O3

Fig. 2. Distribution of difference between actual and estimated FSI from Eq. (7) according to coking ranges.

R2 = 0:49

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S.C. Chelgani et al. / Fuel Processing Technology 92 (2011) 349355

where M is moisture, A is ash, and VM is volatile matter. The distribution

of difference between FSI predicted from Eq. (3) and actual determined
amounts of it according to their coking ranges is shown in Fig. 1.

FSI = 3:459 + 1:498 Oex0:362 Oex + 0:017 Oex

+ 0:534 Hex + 0:123 C + 0:011 SiO2 0:12 Sp1:241N

+ 0:168 K2 O + 0:143 Na2 O + 0:067 P2 O5 0:465 TiO2

3.1.2. Ultimate and element analysis

According to inter correlations, oxygen exclusive of moisture (Oex),
oxygen, organic sulfur, and hydrogen have negative effect on FSI; their
values are 0.74, 0.75, 0.23, and 0.18, respectively. In addition,
the rank parameters carbon (0.60) and hydrogen exclusive of moisture
(Hex) 0.35 have positive effects on FSIs. Final equations, using a stepwise
procedure, between the ultimate parameters and FSI can be shown as
follows:

FSI = 33:3790:779 O0:23 C1:787 N

4

+ 0:437 H0:362 Sp0:318 A0:361 SoR = 0:62

FSI = 2:9070:815 Oex + 0:172 C1:299 N

+ 0:07 A0:515 Hex0:127 SpR = 0:68

FSI = 1:0240:9 Oex + 0:132 C1:379 N + 0:173 K2 O

6

+ 0:209 Na2 O0:515 TiO2 + 0:012 SiO2

+ 0:504 Hex0:134 Sp + 0:123 P2 O5

R = 0:69

Fig. 3. Predicted FSI by neural network using proximate analysis versus actual measured
FSI in testing and validation process.

R = 0:71

Where Sp is pyritic sulfur, and So is organic sulfur. The distribution of

difference between FSI predicted from Eq. (7) and actual determined
amounts of it according to their coking ranges is shown in Fig. 2.
3.2. Articial neural network
Articial neural networks (ANN) are simplied systems simulating
the intelligent behavior, as the computational (mathematical) models
try to solve complicated functional aspects. An ANN usually consists of a
hierarchical structure of three different layers described as input,
hidden, and output layers. Each node in the input layer is linked to all the
nodes in the rst hidden layer using weighted connections. Similar
weighted connections exist between nodes of hidden layers, as well as
between the last hidden layer and nodes in the output layer [1823].
In this study, feed-forward articial neural network (FANN) was
used to improve the accuracy of FSI prediction for each state, using the
experimental data FANNs have been applied to many elds of coal
processing in recent years [2428] (Fig. 3).
Based on the regression analysis the best variables for the prediction
of FSI are given in Eqs. (3) and (7). These variables were used as inputs to
FANN for the improvement of FSI prediction. Neural network training

Fig. 4. Predicted FSI by neural network using ultimate analysis versus actual measured
FSI in testing and validation process.

S.C. Chelgani et al. / Fuel Processing Technology 92 (2011) 349355

353

Fig. 5. Distribution of difference between actual and FANN predicted FSI in testing phase using proximate analysis according to coking ranges.

can be made more efcient if certain preprocessing steps (normalizing

processes) are performed on the network inputs and targets. Before
training, it is often useful to scale the inputs and targets so that they
always fall within a specied range. For ANN work, all input and output
data were scaled using the following model:
Np =

Ap meanAps
stdAp

where, Ap is actual parameter, meanAps is the mean of actual

parameters, stdAp is standard deviation of actual parameter and Np is
normalized parameter (input) [29]. By using the above model the inputs
and targets have the mean of zero and a standard deviation of 1.
The number of neurons in the hidden layers was obtained by the trial
and error method so that the error between the desired and estimated
outputs was minimized. Based on these, the most suitable neural
network with a minimum number of neurons in hidden layers to
correlate the input and output parameters was selected as 22331
arrangement for both input data sets. From the total data set (3691);
2591 data were used for training, 700 for validation, and 400 for testing
the FANN model.

The validation and testing phase results show the capability of the
model. The R2 values for validations were R2 = 0.88 for proximate
analysis input data seta, and 0.94 using ultimate analysis. The results
show the model has an ability to reliably predict FSI values (Figs. 4, 5). In
the testing stage, samples (n = 400) over a wide range of FSI values were
applied to certify the potential of FANN model. Figs 4 and 5 show the
relationship between estimated FSIs by FANN model from testing phase
and the FSI value determined by the traditional ASTM method. The R2
values for the testing sets were 0.89 for proximate analysis input data
seta, and 0.95 using ultimate analysis inputs. Upon comparison with the
regression results, the FANN model was shown greater accuracy to
predict FSI values from the same inputs, and (as a rst report) were
convinced FSI is predictable. According to Figs. 5 and 6, that show the
distribution of differences between FANN calculated FSIs and actual
determined FSIs, it can be seen that ultimate rather than proximate
analysis parameters, provide a much better estimation of the FSI values.
4. Conclusion
Inter correlations between ultimate and proximate analysis with FSI
show that with the increase content of ash, moisture, volatile matter,

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S.C. Chelgani et al. / Fuel Processing Technology 92 (2011) 349355

Fig. 6. Distribution of difference between actual and FANN predicted FSI in testing phase using ultimate analysis according to coking ranges.

oxygen exclusive of moisture, and organic sulfur in coal, the FSI

decreased (negative effect). Higher amounts of carbon and hydrogen
exclusive in coal have positive effects on FSI. Also the results show that
higher K2O content in coal results higher FSI. These relationships were
not cited before.
The nonlinear equations have shown greater accuracy than linear ones
where they can predict FSI with the correlation coefcients (R2) of
0.49 thereby R2 = 0.47 in the linear using proximate parameters, and
R2 = 0.71 versus R2 = 0.69 in the linear using ultimate analysis inputs.
Ultimate analysis beside ash oxides are much greater predictors than
proximate analysis for the estimation of FSI by both linear and non
linear multivariable regression methods. These precisions were not
reported in the previous published works.
The FANN procedures used to improve the correlation coefcients
between predicted FSIs and actual determined FSIs, with a good
resulting R2 of 0.88 and 0.89 using proximate analysis inputs in the
testing and validation, respectively, and also R2 = 0.94 and 0.95 using
ultimate analysis data set inputs in the testing and validation,
respectively, had not been previously mentioned.
The ability of both regression and ANN model were investigated
according to the coal coking ranges (FSI ranges 02, N24, N49). As a

comparison with the regression method, articial neural network was

capable to predict FSI with signicant accuracy.
References
[1] D. Barry, B.C. Rayan, T. John, The predicted coke strength after reaction values of
British Columbia coals, with comparisons to international coals, Geological eldwork
(1993) 507516.
[2] M.A. Dez, R. Alvarez, C. Barriocanal, Coal for metallurgical coke production:
predictions of coke quality and future requirements for coke making, International Journal of Coal Geology 50 (2002) 389412.
[3] H.D. Huntington, Coal propertiesmeasurement and application to coke making,
Iron and Steel Engineer (November 1997) 27.
[4] N.H. Bostick, T.A. Daws, Relationships between data from rock-eval pyrolysis and
proximate, ultimate, petrographic, and physical analyses of 142 diverse U.S coal
samples, Organic Geochemistry 21 (1) (1994) 3539.
[5] H. Marsh, Metallurgical coke: formation, structure and properties, Proc. 41st
Ironmaking Conf., ISS-AIME, 1982, pp. 211.
[6] H. Marsh, The coke making process, Proc. 51st Ironmaking Conf., ISS-AIME, 1992,
pp. 569580.
[7] H. Marsh, D.E. Clarke, Mechanisms of formation of structure within metallurgical
coke and its effects on coke properties, Erdohle Kohle Erdgas Petrochemie 39
(1986) 113122.
[8] Q. Zhang, X. Wu, A. Feng, M. Shi, Prediction of coke quality at Baosteel, Fuel
Processing Technology 86 (2004) 111.
[9] N. Tsubouchi, Y. Ohtsuka, Fuel 81 (2002) 1423.

S.C. Chelgani et al. / Fuel Processing Technology 92 (2011) 349355

[10] M.R. Khan, R.G. Jenkins, Fuel 65 (1986) 1203.
[11] B. Ryan, R. Leeder, J.T. Price, J.F. Gransden, The effect of coal preparation on the
quality of clean coal and coke, Geological Fieldwork (1999) 247275.
[12] I. Toroglu, The effects of ash and maceral composition of Azdavay and Kurucasile
(Turkey) coals on coking properties, Energy Sources, Part A 28 (2006) 263279.
[13] J.S. Goscinski, R.M. Patalsky, CSR control: a coal producers point of view, Iron Making
Proceedings, Iron and Steel Society, 48, American Institute of Mining, Metallurgical
and Petroleum Engineers, 1989, pp. 5065.
[14] B. Viswanathan, ebook of An introduction to energy source (2006) p. 66.
[15] ASTM D 720, Standard test method for free swelling index of coal, ASTM
Handbook for Coal and Coke, 1999, pp. 226230.
[16] J.G. Speight, Handbook of Coal Analysis, 2005, pp. 145148.
[17] L.J. Bragg, J.K. Oman, S.J. Tewalt, C.J. Oman, N.H. Rega, P.M. Washington, R.B.
Finkelman, U.S. Geological Survey Coal Quality (COALQUAL) Database: Version 2.0.
U.S. Geological Survey Open-File Report, 2009, pp. 97134, http://www.energy.er.
usgs.gov/products/databases/CoalQual/index.htm.
[18] S.S. Tambe, B.D. Kulkarni, P.B. Deshpande, Elements of articial neural networks
with selected applications in chemical engineering, and chemical and biological
sciences, Simulation and Advanced Controls, Louisville, KY, 1996.
[19] S. Qin, T.J. McAvoy, Nonlinear PLS modeling using neural networks, Computers
and Chemical Engineering 16 (1992) 379391.
[20] D. Dong, T.J. McAvoy, Non-liner principal component analysis-based on principal
curves and neural networks, Computers and Chemical Engineering 20 (1996) 6578.

355

[21] M.A. Kramer, Autoassociative neural networks, Computers and Chemical

Engineering 16 (4) (1992) 313328.
[22] S.U. Patel, B.J. Kumar, Y.P. Badhe, B.K. Sharma, S. Saha, S. Biswas, A. Chaudhury, S.S.
Tambe, B.D. Kulkarni, Estimation of gross caloric value of coals using articial
neural networks, Fuel 86 (2007) 334344.
[23] M.A. Kramer, Nonlinear principal component analysis using autoassociative
neural networks, AIChE 37 (2) (1991) 233243.
[24] E. Jorjani, S. Chehreh Chelgani, Sh. Mesroghli, Prediction of microbial desulfurization
of coal using articial neural networks, Minerals Engineering 20 (2007) 12851292.
[25] S. Chehreh Chelgani, J.C. Hower, E. Jorjani, Sh. Mesroghli, A.H. Bagherieh, Prediction of
coal grindability based on petrography, proximate and ultimate analysis with multiple
regression and articial neural network models, Fuel Processing Technology 89 (2008)
1320.
[26] E. Jorjani, S. Chehreh Chelgani, Sh. Mesroghli, Application of articial neural
networks to predict chemical desulfurization of Tabas coal, Fuel 87 (2008)
27272734.
[27] E. Jorjani, H. Asadollahi Poorali, A. Sam, S. Chehreh Chelgani, Sh. Mesroghli, M.R.
Shayestehfar, Prediction of coal response to froth otation based on coal analysis
using regression and articial neural network, Minerals Engineering 22 (2009)
970976.
[28] E.C. Cilek, Application of neural networks to predict locked cycle otation test
results, Minerals Engineering 15 (2002) 1095.
[29] H. Demuth, M. Beale, Neural network toolbox for use with ATLAB, Handbook, 2002.