Fuel Processing Technology 121 (2014) 104–113

Contents lists available at ScienceDirect

Fuel Processing Technology

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

A review of the correlations of coal properties with

elemental composition
Jonathan P. Mathews a,b,1,⁎, Vijayaragavan Krishnamoorthy a,b,1, Enette Louw a,b,1, Aime H.N. Tchapda a,b,1,
Fidel Castro-Marcano a,b,1, Vamsi Karri a,b,1, Dennis A. Alexis a,b,1, Gareth D. Mitchell b,1
a
John and Willie Leone Family Department of Energy and Mineral Engineering, The Pennsylvania State University, 126 Hosler Building, University Park, PA 16802, USA
b
The EMS Energy Institute, The Pennsylvania State University, 126 Hosler Building, University Park, PA 16802, USA

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

Article history: The spatial arrangement and abundance of the elements: C, H, N, O, S often correlate or directly influence a
Received 11 December 2012 plethora of coal properties. For N 90 years, attempts have utilized the ultimate (elemental) analysis of coal to
Received in revised form 15 January 2014 predict a wide variety of properties such as: calorific value (higher heating value), volatile matter, vitrinite reflec-
Accepted 16 January 2014
tance (mean maximum), Hardgrove grindability index, helium density, aromaticity, etc. While many relation-
Available online 3 February 2014
ships resulted in graphical plots that have utility even today, numerical values can also be directly calculated
Keywords:
utilizing the correlations. These have the potential to allow rapid predictions and low-cost approaches to coal
Ultimate analysis property determination. Here the many correlations addressing multiple coal properties were reviewed and
Correlation where possible evaluated against a sampling of the Pennsylvania State University Coal Sample Bank and Database
Statistical analyses of coal for vitrinite-rich (N80% by point counting) United States coals. Over 42 correlations were found in the literature.
Coal properties While some correlations, such as calorific value predictions are accurate over a wide range of compositions,
others are restricted in applicability to a select rank range. For many correlations, there are challenges to predict
the property accurately, over a wide range, but may capture the trends.
© 2014 Elsevier B.V. All rights reserved.

1. Introduction
The structure and resultant property/behavior of coals are often
dependent on the spatial arrangement and abundance of the elements:
C, H, N, O, S, also water and cations in low-rank coals, mineral matter
and process conditions: particle size, mass, heating rate, etc. If we ignore
the latter components and focus on the elemental composition, it is
possible to predict a large number of coal parameters. Even if there is
no direct cause–effect link between composition and properties, the
systematic transformations accompanying coalification often permit
correlations. Thus, while causation and correlation need to be separated,
there is an opportunity to build on the remarkable extended studies of
coal that have been 70 plus years in preparation. These studies often
generated graphical plots which still serve the needs of the coal science
community, for example Seyler's plot [1], van Krevelen diagrams [2],
etc. and the many collections of graphical representations [3–5]. Recent-
ly, the trends are often accompanied by predictive equations. Gathering
these relationships will improve their utility and may offer considerable
synergy. This paper attempts to determine if indeed “coal is elementary”
and examines the predictive capability from a literature review and
where possible tests predictions against the Penn State Coal Sample
Bank Database for a subsample (N80%) of vitrinite-rich coals from the
United States [6].
⁎ Corresponding author.
E-mail address: jmathews@psu.edu (J.P. Mathews).
1
Tel.: +1 814 863 6213.
The Penn State Coal Sample Bank and Database currently houses
1058 coals of the 1579 samples collected over the past 45 years. While
most of these samples are historical in nature, 38 are DECS-series sam-
ples protected from deterioration using foil/polyethylene laminate bags
under argon gas and another 22 are premium samples contained in
glass vials under nitrogen. Significant data have been collected on
about 1270 of these coals including chemical, petrographic, mechanical
and thermoplastic properties in addition to geologic and geographic in-
formation [6,7]. Unless otherwise noted, the predictions are applicable
only for vitrinite-rich coals. Other maceral-rich coals differ significantly
in composition, structure and behavior [3,8–11]; thus, many of the
correlations here may have limited applicability to non-U.S. coals.
Predictions using the Penn State Coal Sample Bank and Database were
restricted to coals of vitrinite composition N80% determined by point
counting approach.
2. Predicting coal parameters
2.1. Calorific value
Calorific value of coal is one of the most important parameters for
predicting coal behavior, defining rank (for much of the rank range),
for evaluating its potential use in combustion systems [12] and for
evaluating pollution compliance. Calorific value can be determined ex-
perimentally by measuring the enthalpy change of a sample in a bomb
calorimeter by either isothermal or adiabatic methods [13]. However,
there are numerous correlations for predicting higher heating values

0378-3820/$ – see front matter © 2014 Elsevier B.V. All rights reserved.
http://dx.doi.org/10.1016/j.fuproc.2014.01.015
 J.P. Mathews et al. / Fuel Processing Technology 121 (2014) 104–113
(HHV) for various fuels and wastes [12,14–26]. The earlier relationships
are well reviewed by Selvig and Gibson [27]. For the well known, and
still used Dulong formula, from 1820, (Eq. (1)) the errors are expected
to be small for the bituminous and anthracite (b1%) with larger nega-
tive values for coals of subbituminous (− 1.4%) and lignite rank
(− 3.1%) [27]. With the Penn State Coal Sample Bank and Database
coals (circa 1980) supplemented by the Bureau of Mines data, Mason
and Ghandi [28] also reported a higher variance for lignite. There,
however, the mean differences were negative for both anthracite and
bituminous coal.
HHV ðBTU=lbÞ ¼ 145:44½C  þ 620:28½H þ 40:5½S–77:54½O
The elemental content is in weight percent on a dry basis.
Most of the coal-specific relationships were developed for regional
coals. They often follow the approach of Dulong, and later Dryden
[14], utilizing heat of combustion summation approaches with varia-
tions [29] mostly based on multivariate regression analyses. Neavel
et al. developed an empirical correlation based on 66 low mineral mat-
ter vitrinite-rich North American coal samples ranging in rank from
lignite to low-volatile bituminous [16]. According to this correlation
(Eq. (2)), HHV (dry basis) is a function of carbon, hydrogen, oxygen,
total sulfur, and ash yield. In their analysis with a set of 120 coal
samples, ranging from peat to anthracite yielded a mean error of
86 Btu lb−1.
HHV ðBTU=lbÞ ¼ 145:9½C  þ 569:6½H –53:89½O þ 43:08½S–6:3½ASH ð2Þ
Values in square brackets indicate mass basis values.
Singh and Kakati developed empirical models to predict HHV for
Indian coal samples [12]. They obtained four different models by corre-
lating O, O/C, O/H, and O/C and O/H atomic ratios to HHV for 160 Indian
coal samples. Of all the developed correlations, the authors found Eq. (3)
to be most applicable. The HHV is calculated on a dmmf basis. Their
correlation predicted 160 Indian coal samples with an average error of
0.9%.
HHV ðMJ=kgÞ ¼ 37:4541−14:2040ðO=C Þ−21:2929ðO=HÞ
Mazumdar developed a correlation that relates theoretical oxygen
requirement for complete combustion of coal (Ord), ash yield, and H/C
ratio of coal to HHV (dry basis) (Eq. (3)) [17]. Where HHV is calorific
value in dry basis, H/C (wt.%/wt.%) is the hydrogen to carbon ratio.
The correlation was found to predict HHV of 31 vitrinite-rich North
American coal samples from lignite to low-volatile bituminous coals
with an average absolute deviation of 0.45% (Eq. (4)).
HHV ðMJ=kgÞ ¼ 13:03½Ord  þ ð100−MMÞ
 ð0:238  ðH=C Þ−0:0065Þ−0:007 ½ASH 
Channiwala and Parikh went a step further and developed a unified
correlation for estimating HHV of solid, liquid and gaseous fuels from
elemental analysis (Eq. (5)) [18]. The correlation was derived using
225 elemental compositions and ash yields, and was validated with 50
fuels: coals, cokes, municipal wastes, chars, and various gaseous fuels.
The HHV in the correlation is the higher heating value on a dry basis.
The elements C, H, O, N, S and ash are in dry wt.%. The authors claim
that the model was reasonable in estimating HHV of fuel having ele-
mental composition (wt.%): C from 0 to 92.25%, H from 0.43 to 25.15%,
O from 0 to 50%, N from 0 to 5.6%, S 0 to 94.8%, and ash ≤71.4%. However,
the range is wide enough to cover most of the fuels used in industry.
HHV ðMJ=kg Þ ¼ 0:3491½C  þ 1:1783½H
þ 0:1005½S−0:1034½O−0:0151½N−0:0211½ASH 
Parikh et al. developed a unified correlation for estimating HHV of
solid, liquid and gaseous fuels from proximate analysis (Eq. (6)) [20].
105
The correlation was obtained from 450 proximate analyses covering
a wide range of fuels: industrial wastes, coals, cokes, municipal
wastes, chars, and manufactured fuels. The parameters FC , VM and
ASH are fixed carbon, volatile matter and ash yield all on a dry
basis. When the correlation was tested with 100 data points of fuel
ranging from coal, coke, chars and biomass, along with 450 data points
used in derivation of the correlation, the average absolute error was
found to be 3.74%.
HHV ðMJ=kgÞ ¼ 0:3536½ F C  þ 0:1559½V M −0:0078½ASH  ð6Þ
ð1Þ Sheng and Azevedo reviewed correlations to predict HHV of biomass
based on its ultimate, proximate analysis, and biochemical composition
(such as cellulose component) [21]. The models based on ultimate
analysis were more accurate than proximate analysis or biochemical
composition. Their correlation (Eq. (7)) calculates the higher heating
value in dry basis. C and H are carbon and hydrogen, in dry wt.%. An
additional correlation (not shown) icorrected for ash yield.
HHV ðMJ=kgÞ ¼ −1:3675 þ 0:3137 ½C  þ 0:7009 ½H  þ 0:0318 ½O ð7Þ
Majumdar et al. [26] developed a correlation based on proximate
analysis (A, M, VM , and F C ) of 164 Indian coal samples to predict
HHV (as received basis) (Eq. (7)). Where A, M, VM, and FC are ash,
moisture, volatile matter, and fixed carbon in wt.%, respectively.
The model was shown to predict HHV of 79 Indian coal samples
with an average error of 13.1%. However, with a different set of 86
Indian coal samples, the average absolute error was significantly re-
duced to 1.46%. The authors attributed the poor prediction of 79
Indian coal samples to experimental errors involved in measuring
HHV of too few coal samples.
HHV ðMJ=kg Þ ¼ −0:03 ½ASH −0:11½M  þ 0:33 ½V M  þ 0:35 ½ F C  ð8Þ
Selected models, based on elemental composition (and ash yield),
were tested and compared for their predictability on 971 coal samples,
ð3Þ ranging from lignite to anthracite, obtained from the Penn State Coal
Sample Database. However, it should be noted that the validity of
the published equations holds only for the rank-range for which they
were derived. With exception of the Sheng and Azevedo model [21],
all were coal-derived expressions. The Sheng and Azevedo model was
compared to test the validity of the biomass-based model for coal.
Hence, the comparison was academic. All the models were corrected
to dry-ash-free basis. Comparison of the models, for various coal
ranks, is shown in Table 1. As expected, the predictability of models
specifically developed for coal performed better. Surprisingly, the
Sheng and Azevedo model [21] predicted anthracite with better accura-
ð4Þ cy than other coal models (Table 1). The Sheng and Azevedo model
however had considerable scatter. The general under prediction with
higher carbon content happens to match the slight drop in the HHV of
anthracite due to the reduced hydrogen content. The Singh and Kakati
model was derived for Indian coal samples and tends to slightly over
estimate HHV. This may be attributed to differences in petrography
(Gondwana inertinite-rich coals vs. U.S. vitrinite-rich coals). The models
of: Neavel et al., Channiwala and Parikh, and Mazumdar predict equally
well as shown (Fig. 1 and Table 1). The Dulong formula was poor as
indicated by the deviation from 45° for the regression line (Fig. 1) and
the deviation (Table 1). However, the wide applicability makes the uni-
versal correlation of Channiwala and Parikh [18] attractive. Given et al.
also considered calorific value with the Penn State Coal Bank and Data-
base (circa 1986) and also proposed relations with the improvement of
including the term related to the enthalpy of decomposition [15]. His
ð5Þ breakdown included a relationship clustered into six subsets to capture
coal rank transitions and regional (Eastern/Interior/Rocky Mountain)
influences. Van Krevelen considers the Neavel et al. and the Given
et al. relationships to be the better ones [4]. Although not covered
106 J.P. Mathews et al. / Fuel Processing Technology 121 (2014) 104–113

Table 1
Comparison of errors for different HHV models for PSU Sample Bank coals.

Coal rank N Average absolute error (AAE) %

Neavel Singh and Kakati Channiwala Sheng and Mazumdar Dulong

et al. correlation and Parikh Azevedo correlation correlation
correlation correlation correlation

Lignite 51 1.63 4.08 1.92 10.71 1.66 15.45

Subbituminous 114 1.54 3.59 1.71 12.43 1.72 12.22
High-vol. bituminous 622 1.03 2.18 0.98 16.80 1.47 14.69
Medium-vol. bituminous 74 0.98 2.68 0.92 10.04 1.65 14.62
Low-vol. bituminous 83 0.95 2.78 0.82 17.50 1.59 16.66
Anthracite 27 1.31 5.23 1.42 8.18 1.30 17.89
Total 971 1.12 2.62 1.11 15.27 1.53 14.70




ðExperimental HHV−Predicted HHV Þ

Σ

x100


Experimental HHV
AAE ð% Þ ¼
n

here, recent work has utilized a more sophisticated neural network are percentages of vitrinite, “exinite” (liptinite) and inertinite. The sym-
approach [24,25,30]. bols x, y, and z are their volatile matter values for “pure” macerals. Com-
parison of their calculated and experimental data was considered
“statistically insignificant” by those authors.
2.2. Volatile matter

VM ¼ ða  xÞ=100 þ ðb  yÞ=100 þ ðc  zÞ=100 ð9Þ

Volatile matter is an integral part of the ASTM classification system
[31] and is indicative (along with other parameters) of coals' suitability
for combustion and carbonization. The standard method for determin-
ing volatile matter is the ASTM D3175 [32]; however, the instrumental
proximate approach is now more common (recently (2010) replaced
by a macro thermal analysis approach [33]), but there are differences in
yields between the two classic and modern approaches for some ranks
[34]. Various attempts have been made to estimate its value from other
coal parameters such as elemental composition [16], maceral composition
[35], and vitrinite reflectance [36]. Chatterjee et al. [35] used maceral
composition to estimate the volatile matter (Eq. (9)) where a, b, and c
The Borrego et al. [36] formula (Eqs. 10–13) used a combination
of maceral composition and vitrinite reflectance. A summary of
their formula is shown in Table 2. The fractional volatile matter con-
tent of the residual maceral in coal (φi) was determined according to
the formula. Then, the volatile matter contribution of each maceral is
determined by multiplying the fractional content of the residual
maceral φi , by the percent content of the residual maceral (X i ) in
coal. The volatile matter yield is the sum of the individual maceral
volatile matter contributions.

Fig. 1. Models of Neavel et al., Singh and Kakati, Channiwala and Parikh, Sheng and Azevedo, Mazumdar, and Dulong formula.
 J.P. Mathews et al. / Fuel Processing Technology 121 (2014) 104–113 107

Table 2 Fig. 2 shows the calculated versus measured volatile matter. The
Equations of Borrego et al. for volatile matter prediction from maceral composition. top left graph shows how Neavel et al. equation performs for all
Maceral Range (Rr) φi VMi ranks. As expected, Neavel's equations fail to predict the volatile
v1 matter content of high-rank coals; their equations were derived for
Vitrinite 0.42–6.08% φv ¼ v v (10) VMv = φv*Xv
Rr 2 −Rr 3 −v4 þv5
   
i
lignite to subbituminous rank. Their equation gave negative values
Rr 3
Inertinite 0.42–6.08% φi ¼ i1 exp − i2 (11) VMi = φi*Xi when the volatile matter yield of the coal was low (high-rank
I 1 þRr2
I coals). When applied to lignite and subbituminous coals, their re-
Liptinite 0.42–1.40% φl ¼ I I
(12) VMl = φl*Xl
Rr3 −Rr4 −I 5 þI 6
v1
sults improved. The bottom graphs of Fig. 2 give the results of
1.40–6.08% φv ¼ (13) VMv = φl*Xl
v v
Rr 2 −Rr 3 −v4 þv5 Borrego et al. equations. Borrego's equations that are restricted to
v1, v2, v3, v4, v5, i1, i2, i3, I1, I2, I3, I4, I5, and I6 are constants and Rr is the random vitrinite
the random vitrinite reflectance of 0.46–6.08 give a fairly good pre-
reflectance, predicted VM value is the sum of the maceral contributions. diction for high-rank coals. It is noteworthy that in 1916, there was
work on achieving the reverse, the prediction of elemental data from
proximate analysis [37]. For completeness, Koba [38] also provided
VM predictions for coking coals mostly using variations of the H/C
Neavel et al. [16] produced the simplest equation to estimate the ratio or hydrogen content.
volatile matter, using ultimate analysis data for low-rank coals. Their
equations were segregated into a sulfate-free ash group and an uncor-
rected ash group. 2.3. Vitrinite reflectance

Whole dataset and applying an intercept to the analysis
VM ¼ 94:160−1:350½C  þ 10:630½H−1:780½N−0:845½Ash
VM ¼ 92:380−1:34½C  þ 10:440½H  þ 0:366½S−0:963½Ash
Selected samples of the dataset and applying an intercept to the
analysis
VM ¼ 94:670−1:345½C  þ 10:590½H−2:290½N−0:825½Ash
VM ¼ 93:670−1:363½C  þ 10:430½H þ 0:396½S−0:964½Ash
Selected samples without intercept
VM ¼ −0:408½C  þ 11:250½H  þ ½O þ 1:3½S
VM ¼ −0:417½C  þ 11:520½H  þ 0:912½O þ 1:260½Ash
VM*: Ash uncorrected, otherwise sulfate-free ash
Vitrinite reflectance (mean maximum) (R0) is often used as a coal
rank or basin thermal maturation indicator. The R0 value is determined
ð14Þ
by measuring the amount of incident light reflected from the polished
surface of a statistically significant number of vitrinite particles and
ð15Þ
reporting the mean value. Reflectance values are collected from a micro-
scope system capable of plane polarized, white light illumination
between ×400 and ×750 magnification, 360° stage rotation and having
a photoelectric system standardized to a known reflectance range that
can record the maximum amount of incident light through a 360°
ð16Þ
rotation. Flueckinger et al. determined correlation tables for mean max-
imum vitrinite reflectance and found a strongly negative correlation
ð17Þ
with hydrogen and a strongly positive correlation with carbon as ex-
pected [39]. Koba also developed various R0 correlation parameters for
coking coals [38]. McCartney and Teichmüller [40] conducted a compre-
hensive study of European and U.S. coals with N75% vitrinite content
ð18Þ
and H/C atomic ratios ranging from 0.6 to 1.2. The R0 values correlate
well with other commonly used rank parameters such as volatile
ð19Þ
matter, carbon content, and H/C ratios. They indicated that generally
vitrinite aromaticity increases with increasing rank, raising the refrac-
tive index and consequently the reflectance. Several correlations have

Fig. 2. Calculated versus measured volatile matter.

108 J.P. Mathews et al. / Fuel Processing Technology 121 (2014) 104–113
been derived for estimation of R0 from elemental composition data
[40–44]. Sweeny and Burnham developed a simplified Arrhenius reac-
tion model (EASY %R0) that incorporates a distribution of activation
energies to calculate vitrinite maturation with changing time and tem-
perature [45]. Neavel [41] proposed an exponential fit to the data of
McCartney and Teichmüller [40] (Eq. (20)).
R0 ¼ 15:64  exp½−3:6  ðH=C Þ
An improved correlation based on results given by McCartney and
Teichmüller [40] was obtained by Burnham and Sweeny [42] recognizing
that oxygen content also tends to reduce the refractive index (Eq. (21)).
R0 ¼ 12  exp½−3:3  ðH=C Þ−ðO=C Þ
George et al. [43] used samples from the Permian Greta seam in the
Sydney Basin (Australia) with H/C atomic ratios N0.85 (Eq. (22)).
R0 ¼ 2:12–1:71  ðH=C Þ
Smith and Smith [44] developed correlations (Eq. (23)) for Australian
coals with 80–95 %C (dmmf).
R0 ¼ −5:035 þ 0:0804½C –0:184½H 
Recent regression analysis approach generated Eq. (24) with an R2
value of 0.77 for 1012 Kentucky coals by Chelgani et al. [30]. An im-
proved R2 value of 0.84 was obtained with the feed-forward artificial
neural network approach.
2 equation proposed by George et al. [43] exhibited the best agreement
R0 ¼ 9:096−0:129½C  þ 0:001½C  −0 : 03½O−0:021½VM−0 : 081Ln½S
2
−0 : 738½H  þ 0:077½H 
Fig. 3 shows R0 values computed from Eqs. (20 to 24), with respect to
carbon content, utilizing PSU Coal Sample Bank and Database for N80%
Fig. 3. R0 values computed from Eqs. (20 to 24), with respect to carbon content.
vitrinite coals and experimental values for comparison. As seen, Neavel
[41] and Burnham and Sweeney [42] relationships are able to predict
the increase in R0 for %C N 91%. George et al. [43], and Smith and Smith
[44] correlations showed consistency with experimental trends for
carbon content of 75–85%. The fit was poor for Chelgani et al. outside
of the bituminous range as expected for a bituminous correlation.
Fig. 4 shows a comparison between calculated and measured values
ð20Þ for these equations. Neavel and also Burnham and Sweeney exhibit a
reasonable agreement with experimentally determined R0 values,
whereas George et al. and the Smith and Smith approach had higher de-
viations for these coals. Recent work used the combination of proximate
and ultimate analyses with a neural network approach to predict
maceral composition for Indian coals with significantly improved
ð21Þ results over multivariate regression analyses [46]. Their prediction
(Eq. (25)) for vitrinite had a coefficient of determination of 0.6495 vs.
0.9684 for the equivalent neural work determination.
Vitriniteð% Þ ¼ 65:1470 þ ð0 : 131 ½MÞ þ ð0 : 4832 ½VMÞ–ð0 : 8263½AshÞ
ð22Þ
ð25Þ
Average absolute deviation values obtained from correlations ap-
ð23Þ
plied to PSU Coal Sample Bank and Database are compared in Table 3.
As expected, these correlations exhibit lower deviations for high- and
mid-rank coals since they were developed using vitrinite reflectance
data from these ranks. Specifically, for anthracite and high-volatile
bituminous rank, Burnham and Sweeney [42] correlation showed the
lowest deviation. For medium- and low-volatile bituminous rank, the
with the experimental values, whereas for lignite and subbituminous
ð24Þ rank, the experimental data were best correlated by the Burnham and
Sweeney relationship. The results obtained suggest that the equation
developed by Burnham and Sweeney better correlates overall with the
PSU Coal Sample Bank and Database.
 J.P. Mathews et al. / Fuel Processing Technology 121 (2014) 104–113 109

Fig. 4. Comparison between calculated and measured values.

2.4. Aromaticity tars, and gases.

Coal properties can often be predicted by the degree of aromaticity.
van Krevelen and colleagues determined molar volumes and aromaticity
via a graphical densimetric method via a group contribution approach
[47]. Mazumdar used corrected values (Eq. (26)) with X = 0.115 when
H/C ≥ 0.7 and 0.125 when H/C is less [48]. The Mc/d value is a molar
volume per carbon atom (via group addition approach with assignment
assumptions) with an estimated helium density prediction to obtain
mean values around 11.33.
f a ¼ ð0:0159½C Þ–0:564 ð27Þ
Aromaticity, determined through single pulse excitation 13C NMR,
correlated the aromaticity to the atomic H/C ratio for coals in the
bituminous rank range Maroto-Valer et al. [52,53]. The correlation
gave reasonably accurate results for 39 different coals. Mazumdar in a
follow-up letter further discussed applicable ranges and locations of
the transformation between linear ranges [54].

f a ¼ 1:22−0:58  ðH=C Þ ð28Þ

f a ¼ ½1–ðH=C Þ þ X ½ðMc =dÞ−5:34 ð26Þ

2.5. Physical parameters

A linear correlation was also generated by Niksa [49] based on
Gerstein et al. [50] data (Eq. (27)). The goal in that work (Flashchain)
and in the Chemical Percolation Devolatilization model [51] was to
utilize various NMR parameters in describing the coal structure and
subsequent breakup upon devolatilization to determine yields of char,
There is the expectation that “the macroscopic physical properties of
a substance depend to some extent on its density because the interac-
tion between the molecules is a function of the intra-molecular
distance” [47]. Coal density (daf/dmmf) is an important property

Table 3
Comparison of average errors for different vitrinite reflectance models PSU Coal Sample Bank and Database.

Rank Average error (%)

Neavel (1981) Burnham and Sweeney (1989) George et al. (1994) Smith and Smith (2007)

Lignite −132 36 94 67
Subbituminous −91 39 86 54
High-volatile bituminous −23 9 29 14
Medium-volatile bituminous −20 −9 2 −22
Low-volatile bituminous −21 −12 −3 −37
Anthracite −54 −8 10 −66
110 J.P. Mathews et al. / Fuel Processing Technology 121 (2014) 104–113
as it can provide structural information and is used in porosity
determinations [55]. The helium density is determined through helium
picnometry. While the analysis is not challenging, it can be time con-
suming; however, modern analytical devices are now highly automat-
ed, and the determination is becoming trivial. X-ray techniques can
also be used for a true density determination. Coalification transitions:
loss of oxygen, hydrogen etc. with reorientation and enhanced stack-
ing are partially responsible for the general trend of density decreasing
then increasing with rank parameters. The inflection point is around
85% C (daf basis) [47]. Many correlations have been developed to re-
late organic density (also termed true density, or the helium density es-
timate) to the elemental composition. Parkash [55] developed a
correlation (Eq. (29)) to estimate true density from the elemental com-
position by performing a multivariate analysis of the data from 32 Al-
berta (Canada) subbituminous coals.
True Density ¼ 3:5742−ð00:0197½C  þ 0:0192½OÞ−0:0691½H 
Neavel et al. [56] developed a similar equation based on the data
obtained by analyzing 66 fresh, vitrinite-rich U.S. coals (Eq. (30)).
True Density ¼ 0:023½C  þ 0:0292½O−0:0261½H 
þ 0:0225½S−0:765
Neavel et al. [16] also developed a multivariate correlation to predict
density (He pycnometry) from the elemental composition by using
analytical data from 66 samples starting from lignite to low-volatile
bituminous coals (Eq. (31)).
Density ¼ 0:01556½C −0:04117½H þ 0:02247½O þ 0:02049½S
þ 0:0208½Ash
Additionally, they also developed a correlation to estimate the den-
sity of organic matter in coal on a dry-ash-free basis (Eq. (32))
Densityorganic ¼ 1:534−0:05196½H  þ 0:007375½O–0:02472½N
þ 0:003853½S
Mazumdar [57] used the modified H/C atomic ratios to calculate
helium density from the elemental composition. This correlation is
generally applicable to lignite to semianthracite (Eq. (33)).
20 ’ 2
d 4 ¼ 1:714−0:686½H=C  þ 0:5½ðH=C−0:6Þ
Walker et al. [58] conducted experiments on a large number of coal
macerals of different ranks with He, Hg, methanol, water and CO2 to
determine densities, porosities and surface areas. Subsequently they
developed a correlation to estimate the densities from elemental com-
position (Eq. (34)).
ρHe ¼ 0:033½C  þ 0:036½O−0:031½H  þ 0:009½S−1:577
Strugala [59] developed correlations to determine the “real” density
of hard coals by using ultimate and proximate analysis data of coal
samples obtained from different seams of Polish coal mines. The “true”
density (dHe) was expressed as a combination of the density of mineral
matter (dM) and the density of organic matter (do) where, Md is the per-
centage of mineral matter in dry coal (Eq. (35)).
   
d d
1=dHe ¼ 1−M =100  ð1=do Þ þ M =100  ð1=dM Þ
The density of mineral matter (dM) can be calculated if the composi-
tion of different minerals is known by using a simple arithmetic summa-
tion of the product of their respective densities and fractions. See
citation for a detailed discussion [59]. The density of organic matter
in coal (do) is expressed as the arithmetic sum of the product of the
fraction of the ‘hydrocarbon moieties’ and the ‘oxygen plus nitrogen
moieties’ (Eq. (36)) where, x(C–H), x(O + N) are the mass fractions of
‘hydrocarbon moieties’ and ‘oxygen plus nitrogen moieties’ respectively
and d(C–H), d(O + N) are the real densities of ‘hydrocarbon moieties’ and
‘oxygen plus nitrogen moieties’ respectively.
   
1=do ¼ xðC−HÞ =dðC−HÞ þ xðOþNÞ =dðOþNÞ ð36Þ
Based on the dependency of the specific volume of hydrocarbon
moieties (1/d(C–H)) on different characteristics the linear variation
of specific volume of oxygen plus nitrogen moieties (1/d(O + N))
with (O + N) content and subsequently calculating regression coeffi-
cients using measured organic matter density data they were able to de-
termine the density of organic matter (Eq. (37)).
ð29Þ h i
2
1=do ¼ 0:6625–0:5696 C =ðC þ HÞ–0:4820C þ H þ 1:0494½C  ð37Þ
Fig. 5 shows the plots of Cwt.% (dmmf) versus density (particle or
organic density). The general expected trend for the variation of coal
ð30Þ density with carbon is to observe a gradual reduction as the carbon
content increases until about 85% then increases rapidly for carbon
values greater than approximately 93% as shown in Fig. 5. There is lim-
ited experimental density data available so Gan et al. [60] and Walker
et al. Penn State Coal data [58] was plotted for reference. For Neavel
et al.'s [16] correlations, the point of inflexion is around 85% for the den-
sity curve, but it fails to rise sharply enough after 90% C. The Walker et al.
[58] correlation captures the expected trend. Mazumdar [57] used a
ð31Þ modified H/C ratio to calculate density. The modified (H/C) ratio calcu-
lation used functional group distribution estimates for heteroatoms.
Here the standard H/C ratio was used for density predictions as func-
tional group distribution data was not readily available. The density fol-
lows the trend but less effectively in comparison to other correlations.
Parkash's [55] trend does not capture the trend initially; predictions
ð32Þ are scattered between 70% and 90% carbon, increasing after Strugala's
[59] correlation for the organic density shows a relatively flat correla-
tion for low-ranks with considerable scatter. A steep increase occurs
after 90% C and is similar to the experimental observations [60,61].
3. Predicting behavior
ð33Þ
3.1. HGI
The Hardgrove grindability index (HGI) is an important practical
measure for coal handling and utilization, especially for pulverized-
coal-fired boilers [62]. HGI reflects the characteristics of coal in terms
of fracture, hardness, and tenacity and is related to coal rank, petrogra-
phy, moisture, and mineral composition [63]. HGI is experimentally de-
ð34Þ termined and even though the equipment is not expensive, the process
is tedious and therefore there is an interest in predicting its value [64].
Attempts have been made to correlate HGI with coal properties such
as moisture content, ash yield, vitrinite reflectance, etc. [65–68]. By
means of an empirical modeling tool, Chelgani et al. [64] evaluated the
complex relationship between HGI and elemental analysis (Eq. (38)).
Data for 600 Kentucky (presumably all bituminous) coals were used
to determine this correlation, and a fraction of variance (R2) of 0.75
was achieved [64].
ð35Þ HGI ¼ 77:162 þ 3:994  ln½S−10:920½H 
þ 1:904½M −0:424½ASH−11:765  lnð½O þ N=C Þ ð38Þ
3.2. Thermal swelling
The free swelling index (FSI) is an empirical value that can be used to
determine the caking characteristics of coals. It is measured by heating
 J.P. Mathews et al. / Fuel Processing Technology 121 (2014) 104–113
Fig. 5. Plots of Cwt.% (dmmf) versus density (particle or organic density).
particulate coal in a closed crucible to 820 °C and measuring the volume
of the agglomerated mass after devolatilization. By definition, only
bituminous coals possess caking abilities, and therefore the test is
often used to evaluate coking coals. Neavel et al. attempted to correlate
the free swelling index to the oxygen content and total non-plastic com-
ponents (Eqs. (39) and (40)) [16]. The non-plastic components in the
coal were defined as the sum of the mineral matter and the total
inertinite and liptinite content. Coals with N 15% oxygen were consid-
ered to have no swelling properties; hence, the correlation was devel-
oped only for coals of oxygen content between 2.5% and 15 %dmmf by
mass. In their Eq. (38), NPC is defined as the sum of ash value (weight
%) and the total inertinite content (volume %) and LIP is the total
liptinite content. The behavior however is very sensitive to the condi-
tions used; thus, applicability is limited to these specific conditions
and the rank range considered.
2
FSI ¼ 5 þ 4:68f ðOÞ−0:00395  NPC þ 0:0897  NPC−0:0601  LIP ð39Þ
f ðOÞ ¼ sinð0:2513  ½O þ 0:9505Þ ð40Þ
3.3. Direct liquefaction
Coal rank and petrographic composition are important factors in
direct liquefaction behavior [62] but yields are sensitive to the condi-
tions used, and catalyst, so these correlation attempts are also limited
to those conditions. Bright low-rank coals are generally more reactive
during non-catalyzed direct liquefaction [69–71]. Abdel-Baset et al.
[70] investigated the relationship between elemental composition and
liquefaction conversion of 68 coals ranging from lignite to high-
volatile bituminous coals. The highest yields were found for coals with
80–85% carbon (dmmf) [70]. Through multiple stepwise regression
analysis, linear equations were developed that relate conversion to sul-
fur, carbon, and the amount of reactive macerals. Since a strong
111
relationship between the sulfur content of coal and the total conversion
was observed, two separate equations were derived; one for low sulfur
coals (Eq. (41)) and one for coals with content higher than 1.6%
(Eq. (42)). Both correlations are only valid for coals with a total reactive
maceral content above 70%.
Conversion ð% Þ ¼ 3:03  ½S þ 0:27  ðtotal reactivesÞ–0:82  ½C  þ 109
ð41Þ
Conversion ð% Þ ¼ 3:40  ½S þ 0:31  ðtotal reactivesÞ–0:66  ½C  þ 91:9
ð42Þ
3.4. Others
Using full maceral reflectogram data from an automated coal petrology
approach, O'Brian et al. related (separately) various compositional data
and volatile matter for Australian coals and for a few coals coke
parameters (reactivity index and coke strength after reaction) with
graphical approaches [72]. Quick and Glick determined CO2 predictions
(kg CO2 per net GJ) for coal emissions, from regression analyses, yield-
ing a correlation for coals b69% fixed carbon (Eq. (43)) and for N 69%
(Eq. (44)) mostly based on PSU Coal Sample Bank data [73]. CVg is the
gross calorific value (MJ kg− 1) and can be predicted from elemental
composition.
2
CO2 ¼ 0:03663  ðCVgÞ —ð2:584  CVg Þ þ 136:5 ð43Þ
2
CO2 ¼ 0:0101  ðFC Þ —ð1 : 29  FC Þ þ 132 : 2 ð44Þ
Winschel had demonstrated a general reduction of CO2 emissions
with increasing S content [74]. Thus, for international coals, Quick deter-
mined equations for the CO2 emission estimates [75]. Where Sef is an S
emission factor, CV is the calorific value (m,mmf basis), FC is fixed
112 J.P. Mathews et al. / Fuel Processing Technology 121 (2014) 104–113
carbon (dmmf). Again equations differentiate between low-rank to
high-volatile bituminous coals (Eq. (45)), and for medium-volatile bitu-
minous and higher (Eq. (46)).
   
−2 2
CO2 ¼ 108:73– 1:647  Sef –ð1:085  ½CV Þ þ 1:45E  ½CV  ð45Þ
   
−2
CO2 ¼ 144:45– 0:7647  Sef –ð1:6521  ½FC Þ þ 1:228E  ½FC  ð46Þ
4. Conclusions
There is a rich history and a wide variety of predictive equations that
relate to elemental composition and coal properties. Specifically,
there have been attempts to predict the higher heating value, vola-
tile matter yield, vitrinite reflectance, aromaticity, density, the
Hardgrove Grindability Index, the free swelling index, pyrolysis
yields, direct liquefaction yields, and carbon dioxide yields. Greater
than 40 relationships were collected and where possible evaluated
for their utility broadly with a subset of the Penn State University
Coal Sample Bank and Database. For some relationships, the causa-
tion directly produces good agreement, typically however for a lim-
ited rank range that reflects the correlations creation intent. For
other correlations, the often-systematic transformations accompa-
nying coalification typically enable a reasonable proxy or reasonable
trend given the complex nature of coal.
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