International Journal of Mining Science and Technology 28 (2018) 933–940

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International Journal of Mining Science and Technology

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

Spontaneous combustion of coals and coal-shales

M. Onifade, B. Genc ⇑
The School of Mining Engineering, University of the Witwatersrand, South Africa

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

Article history: Spontaneous combustion of coal is a well-known phenomena around the globe. Apart from the coal itself,
Received 8 November 2017 burning coal-shales is becoming a problem in the South African coal mines. Serious incidents of sponta-
Received in revised form 24 January 2018 neous combustion have been reported as a result of self-heating of reactive coal-shales. The intrinsic
Accepted 15 May 2018
properties and spontaneous combustion tests of 28 selected coal and coal-shale samples were conducted
Available online 18 May 2018
and a relationship between the two has been established. Intrinsic properties were obtained by using the
proximate and ultimate analysis, and spontaneous combustion liability tests results were obtained by
Keywords:
using the Wits-Ehac and Wits-CT indices. The experimental results show that intrinsic properties of these
Spontaneous combustion
Coal-shales
materials complement to the spontaneous combustion liability tests results. Comparative analyses of
Proximate and ultimate analysis intrinsic properties and spontaneous combustion characteristics indicate similarities between the mech-
Wits-Ehac index anism of coal oxidation and that of the oxidative processes undergone by coal-shales. For the tested sam-
Wits-CT index ples, coal samples have a higher intrinsic spontaneous combustion reactivity rating than the coal-shales.
Furthermore, an increase in carbon, moisture, hydrogen, volatile matter, nitrogen and a decrease in ash
content indicate an increased proneness to self-heating. The concentration of pyrite found in the
coal-shales accelerates self-heating. The event of spontaneous combustion can occur if coal-shales absorb
sufficient oxygen when subjected to atmospheric conditions.
Ó 2018 Published by Elsevier B.V. on behalf of China University of Mining & Technology. This is an open
access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).

1. Introduction compounds and ash is the non-carbonaceous matter and mineral

The sedimentary rock which comprises a lot of organic matters
is a reactive porous media. This includes coal, shale and oil sand
[1–7]. Reactive porous medium is sedimentary materials with pore
spaces embedded in the solid, together with a certain amount of a
carbon-rich element [8–14]. This enables the rock to be permeable
to different fluids like water, air and considerably increases its sur-
face area. Therefore, making the organic particles reactive as it per-
mits oxidation to occur once oxygen is supplied [15]. Such reactive
material might experience spontaneous heating. Many investiga-
tions have been carried out on self-heating characteristics of coal
both experimentally and computationally but with limited studies
on coal-shales self-heating [16–19]. There have been no studies
conducted to understand the self-heating characteristics of coal-
shales when subjected to atmospheric conditions.
Coal is a readily combustible rock consisting more than 70% by
volume and 50% by weight of carbonaceous material [20]. The
inorganic non-combustible compounds which produce sulphur
⇑ Corresponding author at: Wits University, School of Mining Engineering, P.O.
WITS, 2050 Johannesburg, South Africa.
E-mail addresses: 1519496@students.wits.ac.za (M. Onifade), Bekir.Genc@wits.
ac.za (B. Genc).
matter in coal. Carbonaceous shales are sedimentary rocks which
possibly originated from peats comprising less than 50% of organic
material [21]. Coal seam, spoil heaps and waste dumps comprise of
weathered coal, clays, pyritic shales, coal-shales and other strata
associated with them. The chemical reactions between oxygen
and external active structures of coal particles which releases heat
are the required constituents of self-heating [1,2,13].
Spontaneous combustion is a process in which oxidation reac-
tion takes place without the interference of an external heat
source. The increase in temperature is caused by the heat liberated
by coal through chemical reactions [22]. The spontaneous heating
of coal with a potential transition into endogenous fires constitutes
a direct risk to the safety of the working conditions and unfavour-
ably influence the mine environments. There are two points of con-
cern when investigating the self-heating rate of carbonaceous
materials due to the presence of oxygen. Firstly, the accumulation
of overburden materials (such as shale and sandstone etc.) on the
coal surface when a new coal seam is exposed to atmospheric con-
ditions. This is common in coal mining operations both in the past
and present. The second is geology of the material, particularly
during the formation of the deposits.
The self-heating of coal-shale has been reported to be the likely
source of spontaneous combustion in selected bands of a coal

https://doi.org/10.1016/j.ijmst.2018.05.013
2095-2686/Ó 2018 Published by Elsevier B.V. on behalf of China University of Mining & Technology.
This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).
934 M. Onifade, B. Genc / International Journal of Mining Science and Technology 28 (2018) 933–940
seam, highwalls and spoil heaps in Witbank, South Africa (as
shown in Figs. 1–3). Spontaneous combustion of coal has been
extensively studied in underground and opencast mines of South
African mines using small-scale test [23–27]. There is no sufficient
information to predict the spontaneous heating of coal-shales.
However, these are materials that contain the fuel for spontaneous
combustion in coal mines. This paper presents the results of intrin-
sic properties and spontaneous combustion tests conducted on
highly reactive coal and coal-shales in South African coal mines.
This will be useful to establish significant relationships between
coal and coal-shale in terms of spontaneous combustion.
2. Sample collection and preparation
2.1. Sample collection
The coal and coal-shale samples used for this work were taken
from four coal mines in Witbank area of South Africa and kept in
airtight bags to avoid oxidation. Representative in situ samples
were obtained from the affected areas in respect of their high
propensity to oxidation. Twenty-eight coal and coal-shale samples
were collected at selected bands of a coal seam, highwalls and
coal-shales for testing. Eight coal and coal-shale samples were
taken from the same coal seam at different bands and the remain-
ing 20 from another three different coal seams.
2.2. Sample preparation
In order to reproduce the characteristics of freshly crushed coal,
the samples lumps were reduced to suitable sizes to obtain repre-
sentative samples as required for each experimental test. This was
done with the use of a crusher and ball mill. The coal particle sizes
were limited by the volume required for each test (coal-
characterization tests and spontaneous combustion tests). The
determinations of the volatile matter, ash content and moisture
content of the coal and coal-shale samples were also carried out
according to the American Society for Testing and Material Stan-
dards (ASTM) standards [28–30]. The carbon, hydrogen, nitrogen
and sulphur were determined using a LECO TruSpec CHNS analyser
after calibration with sulfamethazine based on the ISO standards
[31]. The results are given in percentage of carbon, hydrogen and
sulphur in the sample. The analyses were repeated three times
and the average values were recorded. The results for proximate,
elemental analysis (percent air-dried) and spontaneous combus-
tion tests (Wits-Ehac and Wits-CT index) carried out on each sam-
ple are presented in Tables 1 and 2. Similar sample preparations
were previously reported [32–35].
2.3. Wits-Ehac tests
The Wits-Ehac test at the School of Mining Engineering,
University of Witwatersrand is a small-scale test in which freshly
Fig. 1. Self-heating of run-of-mine and spoil heaps at Tweefontein Mine, Witbank,
South Africa.
Fig. 2. Self-heating of highwalls and coal-shales in Witbank, South Africa.
Fig. 3. Symptoms of self-heating in mine face and inseam shale in Witbank, South
Africa.
pulverized (<212 mm) and dried coal samples of 20–25 g in weight
are used. The testing apparatus consists of an oil bath, six coal and
inert material cell assemblies, an oil circular, a heater, a flowmeter
used for airflow monitoring, an air supply compressor and a com-
puter. The temperatures are recorded every 20 s by the microcom-
puter during an average four hours of testing. The test apparatus is
used to test coals under predefined conditions and combustibility
index is obtained by Wade et al., as shown in Fig. 4 [36].
Twenty-eight tests were conducted by using this apparatus.
2.4. Wits-CT tests (new apparatus)
A device for predicting the self-heating characteristics of coal,
coal-shale and other carbonaceous materials under the influence
of airflow without any heating system was recently developed in
the School of Mining Engineering, University of Witwatersrand.
This apparatus has been used to test coals and coal-shales and an
index has been obtained. This index is called the Wits-CT index.
The experimental process represents a well-insulated system rela-
tive to actual conditions in situ. The results obtained from this
apparatus are in-line with work done by Sensogut et al. in coal
stockpiles [37,38]. The experimental investigations were carried
out immediately after the samples were collected from the mine
sites to avoid oxidation. To emulate the characteristics of freshly
crushed coal samples, the lumps were reduced in size (<6.39
mm) on the same day that spontaneous combustion tests for each
sample were carried out. The particle size used is based on the
study reported by Kunni and Levenspiel to determine the
surface-volume average particle size from the size distribution of
coal [39]. A representative sample was weighed and loaded into
the autoclave. The system is sealed at the base and loaded with a
sample from the top. The lid of the system was detached during
the loading of the sample. The process was repeated till the column
was filled to the marked point. The lid was fixed and fastened as
soon as the system was filled with the sample. This technique of
preparation gives a closely sized sample that would be preferable
to measure the rate of oxidation and it ensures the samples are
representatives of the coal beds. Each temperature probe was
 M. Onifade, B. Genc / International Journal of Mining Science and Technology 28 (2018) 933–940 935

Table 1
Results of intrinsic properties and spontaneous combustion tests for coal samples.

Sample Mad Vad Aad Cad Had Nad Sad Pad Oc WE WC

CA 2.3 23.2 28.0 54.4 3.33 1.34 1.91 0.95 8.72 4.64 6.29
CB 2.3 21.0 20.0 61.4 3.36 1.48 1.11 0.59 10.4 4.64 6.96
CC 2.2 24.1 33.8 47.5 3.20 1.35 3.96 2.73 7.99 4.52 5.31
CD 2.3 25.5 20.5 61.4 3.78 1.53 0.86 0.28 9.63 4.6 6.80
CE 2.3 24.3 28.6 53.6 3.41 1.25 1.08 0.43 9.76 4.76 5.42
CF 2.5 23.6 46.9 35.9 3.01 0.89 3.42 2.33 7.38 4.49 3.97
CG 2.5 20.0 16.8 66 3.64 1.58 0.64 0.13 8.84 4.91 7.53
CH 2.4 26.9 18.8 65.2 4.21 1.55 2.19 1.13 5.65 4.69 7.51
CI 2.1 16.7 48.4 36.1 2.55 0.85 1.22 0.22 8.78 3.82 4.05
CJ 1.9 25.7 28.1 52.4 3.13 1.35 5.30 4.13 7.82 4.46 6.61
CK 1.6 22.1 13.7 69.7 4.02 1.60 0.76 0.36 8.62 4.44 9.10
CL 1.6 26.1 22.5 58.9 3.57 1.45 3.88 3.22 8.10 4.87 9.59
CM 1.6 22.0 17.0 66.7 3.77 1.57 0.59 0.30 8.78 4.76 7.27
CN 1.6 23.9 17.0 65.8 4.2 1.63 2.92 2.30 6.85 4.84 7.91

Note: Mad, Vad, Aad, Cad, Had, Nad, Sad, Pad, Oc, WE and WC are the air-dried moisture (%), air-dried volatile matter (%), air-dried ash (%), air-dried carbon (%), air-dried
hydrogen (%), air-dried nitrogen (%), air-dried sulphur (%), air-dried pyrite (%), calculated oxygen (%), Wits-Ehac index and Wits-CT index.

Table 2
Results of intrinsic properties and spontaneous combustion tests for coal-shales samples.

Sample Mad Vad Aad Cad Had Nad Sad Pad Oc WE WC

SA 1.4 11.2 78.5 11.5 1.34 0.34 0.54 0.21 6.39 3.09 1.33
SB 0.9 13.9 77.2 11.0 1.27 0.40 1.56 1.01 7.67 3.06 1.30
SC 1.1 12.7 74.6 13.8 1.60 0.42 0.35 0.15 8.13 0.91
SD 1.6 13.3 77.3 10.8 1.43 0.32 2.53 1.43 6.02 3.27 0.70
SE 1.7 15.9 68.4 15.8 1.78 0.41 6.90 4.26 5.01 3.73 1.60
SF 0.9 13.5 76.9 11.8 1.40 0.43 0.46 0.19 8.11 3.10 1.36
SG 0.8 10.7 84.3 6.02 1.04 0.29 0.73 0.22 6.83 0.67
SH 0.8 8.5 88.7 2.66 0.96 0.09 0.41 0.15 6.38 0.27
SI 1.0 11.9 79.6 9.12 1.41 0.26 0.22 0.05 8.39 0.95
SJ 0.9 11.9 86.9 3.42 0.75 0.08 0.75 0.43 7.19 0.42
SK 1.0 11.7 79.1 9.75 1.73 0.41 0.16 0.10 7.85 2.98 1.18
SL 1.0 16.0 74.0 10.5 2.14 0.39 0.12 0.04 11.85 2.99 1.34
SM 0.8 11.7 76.9 12.5 1.61 0.52 0.24 0.16 7.43 1.44
SN 1.5 16.6 51.5 33.7 2.87 0.96 0.31 0.12 9.16 3.77 3.99

3. Results and analysis

3.1. Results

The results for proximate, elemental analysis and spontaneous

combustion tests carried out on coal and coal-shale samples are
presented in Tables 1 and 2.

3.2. Analysis

The determination of moisture, volatile matter and ash content

Fig. 4. Wits-Ehac test apparatus setup [36].
inserted into the column as the correct sample level was reached.
The position of each temperature probe to the column was place
vertically and uniformly spaced to the centre as soon as the coal
level was reached. Oxygen was supplied and controlled at a fixed
flow rate (20 mL/min) by means of a flowmeter before being fed
into a manifold attached below the lid of the autoclave. The logging
began and the variation in temperatures distribution of the sensors
was stored to a computer file every minute. The test period lasts for
24 h. At the end of each experiment, samples are discarded and the
autoclave is cleaned. The conditions in which the experimental
tests were carried out closely resembled the situation in the mine
environment. Twenty-eight tests were conducted with the use of
this new apparatus to bring better definition for the Wits-Ehac
index. An illustration of the experimental setup is indicated in
Fig. 5a while Fig. 5b shows the apparatus setup.
of both coal and coal-shale samples is carried out. Tables 1 and 2
provide the results of the proximate analysis of coal and coal-
shale samples. The air-dried moisture content varies between
1.6% to 2.5% and 0.8 to 1.7% for coal and coal-shales respectively.
The lower moisture content in the tested coal samples could be
due to the depth of burial and age of the coal seam. It was observed
that most of the coals with lower moisture content show high lia-
bility to spontaneous combustion. This is in-line with the study
reported by McPherson and Beamish and Hamilton [40,41]. Slight
differences are observed in the moisture content of the samples
which is in-line with the study described by Gurdal et al. [42,43].
The variations in moisture content (drying or wetting) of different
bands within a seam have noticeable influences on spontaneous
combustion. The interaction between coal and water in the studied
area can be due to two opposing processes. Firstly, the heat of
evaporation occurs in the first process when the moisture content
of the coal is driven by evaporation at the early heating phase.
Secondly, the process involves adsorption of water vapour from
936 M. Onifade, B. Genc / International Journal of Mining Science and Technology 28 (2018) 933–940
Fig. 5. Wits-CT experimental setup and apparatus.
the air which caused an increase in the coal temperature. The influ-
ence of these two processes is dependent on which process domi-
nates significantly to coal oxidation. The behavior of the moisture
content of the investigated samples are in-line with the study
reported by Pone et al. [45]. Fig. 6 indicates an increase in moisture
occurring on the coal surface layers during spontaneous heating.
Previous studies reported a similar coal comportment [45–51].
The coal-shales have low moisture contents similar to the
tested coal samples. The air-dried moisture content of seam CG
to CJ varies between 1.9% and 2.5%, CA to CC ranges between
2.2% and 2.3%, CD to CF between 2.3% and 2.5% and CK to CN have
the same moisture content (1.6%) respectively. Seams CK to CN
have the lowest moisture content while seam CF and CG have
the highest moisture contents. Seam CF and CG have the highest
moisture content than others followed by CH and those from CA,
CB, CD and CE respectively. It was observed from the study that
the samples have roughly the same moisture contents and are
more prone to self-heating except for samples CF and CI, with
lower liability indices. Coal-shales SE, SD and SN have roughly
the same moisture contents among the coal-shale samples. Coal-
shale SN is more prone to spontaneous combustion from the result
of the liability indices compared to other coal-shales. This may be
due to the presence of the mineral matters that promotes the self-
heating rate. Literature studies revealed that moisture content
increases the liability of coal to spontaneous combustion in addi-
tion to parameters like oxygen, organic matter type, surface area
exposed, mineral content (particularly pyrite) and rank [44,52].
The study shows that an increase in moisture content of coal and
coal-shales is enough to provide a high heat loss from evaporation,
as the samples temperature increases during oxidation reaction.
The air-dried volatile matter content varies between 16.7% to
26.9% and 6.5% to16.6% for the coal and coal-shale samples respec-
tively. The volatile matter for the coals is not less than 20%, except
for sample CI (16.7%). Seams with the high volatile matter have
high liability to spontaneous combustion as indicated in Table 1.
This supports the study reported by Banerjee [53]. Seam CH has
the highest volatile matter content than the other seams. The high-
est volatile matter among all the coal-shales is found in samples SN
and SE as shown in Table 2. The two coal-shales have high sponta-
neous combustion liability index compared to other coal-shales. It
Fig. 6. Moisture occurrence on the surface of the coal at Khwezela Mine (Bokgoni
Pit), Witbank, South Africa.
was found that coal-shales with high volatile matter are more
liable to spontaneous combustion. This characteristic of coal-
shales with high volatile matter corresponding to high liability
indices are similar to coals with the high volatile matter contents.
It is observed that coal and coal-shales with high volatile matter
are liable to spontaneous combustion compared to other samples
with lower values of volatile matter content.
The air-dried ash content ranges between 13.7% to 48.4% and
51.5% to 88.7% for both coal and coal-shale samples respectively.
This confirms with the characteristic of South African coals
[54–57]. The ranges of the results are much related to properties
of some Indian coals with ash contents greater than 45% [58].
The cause of this high ash content is due to the peat depositional
environment where the condition of flooding of the paleomire
occurs periodically during deposition. This is in-line with the study
reported by Životić et al. [59–61]. It is known that the physical and
chemical properties of coal changes during coal oxidation [62]. The
variations in ash contents for samples of the same seam may be
attributed to changes in combustion. Gurdal et al. observed
changes in ash content when compared with un-oxidized coals
[42,43]. It was observed that the ash content of samples within a
selected band of a seam varies significantly. Seam CK has very
low ash content compared to samples CL, CM and CN from the
same seam. Seam CG and CH also have ash content lower than
samples CI and CJ from the same seam. The ash content of seam
CF and CI are considerably high compared to the other seams. Sam-
ple CI with the highest ash content has the slowest self-heating
rate while coal samples with low ash content sample have the fast-
est self-heating rate. The slow and fast self-heating of the coal
could be due to the influence of heat sink on existing mineral
within a coal. This is in-line with the study reported by Humphreys
et al. [63,64]. It was observed that the liability of coal to sponta-
neous combustion decreases with increasing ash content and vice
versa. Coal-shales SN and SE have the lowest ash contents com-
pared with other coal-shales and have the highest self-heating
rate. It is shown that coal-shales SH, SJ and SG have high ash con-
tents and displayed slow self-heating rate. This characteristic is
related to those exhibited by coal samples. Coal-shales with low
ash contents indicate a high propensity to spontaneous combus-
tion than coal-shales of higher ash contents. Therefore, coal and
coal-shale samples display similar ash behaviour with respect to
spontaneous combustion.
Proximate analyses of the tested coal samples have a similar
range of moisture, ash and volatile matter contents, compared to
other values found in a reported study [40,41,56–58,65,66]. This
demonstrates that the obtained results are in-line with the previ-
ous studies in this regard. No studies have previously been
reported on the proximate analysis of coal-shales.
The major elemental constituents present in the coal and
coal-shale samples are determined using a LECO TruSpec CHNS
 M. Onifade, B. Genc / International Journal of Mining Science and Technology 28 (2018) 933–940
analyser. The air-dried carbon content varies between 36.1% to
69.7% and 2.66% to 33.7% for coal and coal-shales respectively as
shown in Tables 1 and 2. Seam CI has the lowest carbon and the
slowest self-heating rate while seams with high carbon contents
have high self-heating rates. Coal-shales SN and SE contained the
higher carbon self-heating rate compared to other coal-shales.
Seam CL, CK, CN, CG and coal-shales SN and SE show higher liabil-
ity indices compared to other coal and coal-shales. Most of the coal
seams displayed high self-heating rate due to the high carbon con-
tents compared to the coal-shales with considerably low carbon
contents. Seam CI and coal-shale SH indicate the lowest liability
indices. The capacity to self-heat appears to be directly related to
the amount of carbon and ash content present in the samples. Most
of the coals with high carbon and low ash content indicate high lia-
bility index while the coal-shales which contain more than 15%
carbon and less than 70% ash content shows a high propensity to
spontaneous combustion (see Tables 1 and 2). It is shown that
coal-shales with high carbon and low carbon contents show simi-
lar characteristics to coal samples having high and low carbon con-
tent with respect to spontaneous combustion. There is a
relationship between the spontaneous combustion characteristics
and carbon contents of the coal and coal-shales from the experi-
mental studies. Coal-shales with a low carbon content of 13% can
be described as a weakly reactive porous medium with respect to
self-heating when compared to coal which contains a higher car-
bon content.
The air-dried hydrogen, nitrogen and calculated oxygen content
varies between 2.55–4.21%, 0.85–1.63%, 5.65–10.35% and 0.75–
2.87%, 0.08–0.96% and 5.01–11.85% for the coals and coal-shales
respectively. Seam CI has the lowest hydrogen of 2.55% and also
the slowest self-heating rate compared to other coal seams. Seam
CN and CH have hydrogen contents of 4.20% and show a high lia-
bility to spontaneous combustion. The highest nitrogen content
of 1.63% is found in seam CN and it shows high liability to sponta-
neous heating. Seam CI has the lowest nitrogen content of 0.85%
and indicates a very slow self-heating rate compared to other coal
samples. This indicates that coal and coal-shales with high hydro-
gen and nitrogen content show a high propensity to spontaneous
heating and vice versa. Coal-shale SN has the highest hydrogen
and nitrogen content of 2.87% and 0.96% respectively. It is moder-
ately prone to spontaneous heating based on the liability indices.
Coal-shale CJ with the lowest hydrogen (0.75%) and nitrogen con-
tent (0.08%) shows a low propensity to spontaneous heating. Seam
CH has the lowest oxygen of 5.65% and the highest oxygen content
is found in seam CB (10.35%). Coal-shale SE has the lowest oxygen
content of 5.01% while coal-shale SL has the highest oxygen con-
tent of 11.85%. This study indicates that the influence of calculated
oxygen from the obtained results of ultimate analyses has no
effects on the liability indices used to evaluate spontaneous com-
bustion. The percentage oxygen by itself does not seem to indicate
the ability of coal to absorb oxygen. The oxygen content of coal
does not seem to show a direct relation to the avidity with which
coal and coal-shales absorb oxygen. Coal-shales with a high
propensity to spontaneous combustion in this study appears not
to contain high oxygen content. Hence, the percentage oxygen con-
tents do not seem to indicate the liability of the tested samples to
self-heating.
The study shows that coal and coal-shales with high carbon,
hydrogen and nitrogen contents are more liable to spontaneous
combustion. Therefore, the influence of these elements might play
a significant role in evaluating the incidents of spontaneous com-
bustion. It was observed that the carbon, hydrogen and nitrogen
contents present in the tested coal samples are in-line with the
study reported by Czaplicki and Smolka; Department of Minerals
and Energy South Africa (DME) and Roberts [65–67].
937
The air-dried total sulphur content varies from 0.59% to 5.30%
and 0.12% to 6.90% for the coals and coal-shales respectively. Six
of the coal samples have sulphur content more than 2% as shown
in Table 1, CC (3.96%), CF (3.42%), CH (2.19%), CJ (5.30%), CL
(3.88%) and CN (2.92%) respectively. The presence of high sulphur
content can be related to the peat depositional environment and
conditions, regional volcanic activity (tuff deposits are interbedded
in the coal-bearing sequences) and alkaline depositional environ-
ments with concentrated sulphide mineralization. Another cause
is that marine influenced peat when the sulphate ions in seawater
provide sufficient amount of sulphur. This is supported in the study
reported by Casangrande et al. [68–70]. It is also reported by
Teichmüller and Teichmüller [71] that fresh-water coal deposited
in the calcium-rich environment is usually sulphur-rich and this
may cause the presence of high sulphur content in some coals
[70]. Seam CM has the lowest total sulphur of 0.59% while seam
CJ has the highest sulphur of 5.30%. The spontaneous combustion
tests on the samples show that both samples are liable to sponta-
neous combustion. Coal-shales SE (6.90%) and SD (2.53%) have high
sulphur content compared to other coal-shales. Coal-shale SL has
the lowest sulphur concentration of 0.12% while coal-shale SE
has the highest sulphur content of 6.9%. The high sulphur content
in coal-shale SE increases with increasing self-heating rate while
coal-shale SL with low sulphur content shows a slow self-heating
rate as shown in Table 2. This may be caused by the high sulphur
minerals occurring in the tested samples.
Comparing the total sulphur content to other coal samples
around the world, the study shows that South African coal can be
considered as low sulphur coal. The values of the total sulphur
analysed in the tested coal samples are in-line with the study
reported in previous studies [65–67,72–76].
The pyrite content in coal is known to be one of the main factors
accelerating the self-heating rate. The pyrite present in the coal
and coal-shales was investigated using the inductively coupled
plasma optical emission spectrometry (ICP-OES). The concentra-
tion of the total sulphur and pyritic sulphur varied considerably
from one sample to another due to other sulphur forms occurrence.
The high amounts of pyrite are observed in seams CJ, CL, CN and CC
while the lowest in seams CG and CI respectively. Seam CJ has the
highest concentration of total sulphur while the lowest total sul-
phur is found in seam CM. The sulphur forms analysed show that
the pyritic contents vary between 0.13% to 4.13% and 0.038% to
4.26% for the coals and coal-shales respectively. The high liability
indices observed in coal-shales SN and SE compared to all other
coal-shales can be associated with the existence of pyrite which
reacts with oxygen and moisture. The reason for the self-heating
rate of coal-shale SE to be higher than other coal-shale samples
except for SN may be due to pyrite concentration of 6.9%. This pyr-
ite content might have considerable effects on the spontaneous
combustion process. This supports the study reported by Stach
et al. [77]. The results certainly illustrate the advance effects of
pyrite oxidation on coal and coal-shales spontaneous combustion.
Furthermore, the results show that the oxidation of sulphide min-
erals might favour the self-heating rate. The results from the tested
coal and coal-shales are in-line with the study reported on coal by
Pone et al. [44,52,78].
The analysed results show that the concentration of pyrite in
the coal and coal-shales accelerates the self-heating rate. The burn-
ing areas as seen in Figs. 7 and 8 indicate that the areas of self-
heating are causes of severe ingress of oxygen into the coal seam.
The distribution of different minerals is formed where gas streams
may appear on the coal surface. These conditions allow sulphur
deposits in the form of crystals and their aggregate, crust, dendrites
and other forms of native sulphur and ammonium chloride to be
found. The occurrence of fumarolic acid mineral deposits are signs
938 M. Onifade, B. Genc / International Journal of Mining Science and Technology 28 (2018) 933–940
Fig. 7. Forms of crystals and ammonium chloride present on the surface of coal-
shales at iMpunzi Mine, Witbank, South Africa.
Fig. 8. Blooms of sulphur and ammonium chloride on the surface of coal-shale at
Tweefontein Mine, Witbank, South Africa.
of the oxidation stage of coal. This study indicates a similar expe-
rience in the burning areas as seen in Fig. 7.
Fig. 8 shows a light-yellow to straw coloured sulphur deposits
and white powdeish ammonium chloride appeared on the coal sur-
face in one of the studied areas. The presence of sulphur deposits
on the coal-shale surface indicates that coal fire may be located
deep underground. Figs. 7 and 8 show that pyrite reacts exother-
mally with oxygen to liberate heat and oxidizes to form sulphuric
acid which significantly increases the rate of low-temperature oxi-
dation. The crystals of these hydrated sulphates on the exposed
coal surfaces are shown in Figs. 9 and 10. The formation of these
hydrated iron crystal sulphates is exothermic and should be con-
trolled effectively to avoid consistent self-heating of coal seams.
If the self-heating rate of carbonaceous materials is associated
with the heat generated and heat dissipated from a single process,
it is expected that the rise in temperature would basically increase
the reaction rate of that process. The carbon contents found in the
coal-shales varied from one sample to the other, hence, this might
indicate that different reactions with different activation energies
might take place in the spontaneous combustion process. When
the carbon contents for the coal-shales were compared with each
other, shales SN and SE are more reactive under the two sponta-
neous combustion tests than other coal-shales. The Wits-Ehac val-
ues of coal-shales SC, SG, SH, SI, SJ and SM could not be determined
due to their low reactivity.
The results of Wits-CT index obtained from tested samples are
in-line with the Wits-Ehac index. The Wits-CT index varies
between 3.97 to 9.59 and 0.27–3.99 for the coal and coal-shales
respectively as shown in Tables 1 and 2. Seam CL has the highest
Wits-CT values while seam CF has the lowest Wits-CT value.
Coal-shale SH has the lowest Wits-CT and coal-shale SN has the
highest Wits-CT index among the coal-shale samples. It is shown
from the analysed results that high-risk coal and coal-shales have
higher Wits-CT and Wits-Ehac index values. Most of the fires
caused by spontaneous combustion in the affected areas of this
Fig. 9. Hydrated iron sulphates on exposed coal surfaces, iMpunzi Mine, Witbank,
South Africa.
Fig. 10. Crystals of hydrated iron sulphates on exposed coal surfaces, iMpunzi
Mine, Witbank, South Africa.
study have been identified as having high Wits-Ehac and Wits-CT
values. As can be seen from Table 1, seam CL, CK, CH, CN and CG,
(which were taken from Khwezela at Bokgoni Pit and Arthur Taylor
Mine at iMpunzi mines) showed the highest risk value in the two
liability indices. The records of the mines revealed that an incident
of spontaneous combustion happened in the seam. These areas are
assigned as being high-risk zone and are the zones from which
samples were collected. The event of spontaneous combustion in
coal mines may be caused by various organic and inorganic con-
stituents of coal-shale within a coal seam. Coal-shales can initiate
self-heat when it absorbs sufficient oxygen and moisture when
exposed to atmospheric conditions. The heat generated due to
the influence of oxygen may exceed the heat dissipated to the sur-
rounding via conduction, convection and radiation and accumu-
lates causing spontaneous combustion of coal-shales to arise.
4. Conclusions
This study has established a detailed experimental methodol-
ogy to evaluate the self-heating characteristics of coal and coal-
shales under the field conditions. The study illustrates that the
tested coals have a high intrinsic spontaneous combustion reactiv-
ity rating than the coal-shales. Both materials show that an
increase in carbon, moisture, hydrogen, volatile matter, nitrogen
and decrease in ash content can complement the proneness to
spontaneous combustion. The proximate and ultimate analysis of
the samples tested shows that these properties may be used as a
tool to measure the liability of spontaneous combustion. Further
research on petrographic analysis and detailed geotechnical study
of coal and coal-shales is underway to evaluate their influences in
predicting and minimizing the event of spontaneous heating.
Acknowledgments
The authors would like to thank the staff of Glencore and Anglo
American mines for their devoted help during sample collections.
The authors wish to express gratitude to Coaltech for their financial
support. The work presented here is part of a PhD research study in
the School of Mining Engineering at the University of the
Witwatersrand.
References
[1] Oliveira ML, Navarro OG, Crissien TJ, Tutikian BF, da Boit K, Teixeira EC, et al.
Coal emissions adverse human health effects associated with ultrafine/nano-
particles role and resultant engineering controls. Environ Res 2017;158:450–5.
[2] Oliveira MLS, da Boit K, Pacheco F, Teixeira EC, Schneider IL, Crissien TJ, et al.
Multifaceted processes controlling the distribution of hazardous compounds in
the spontaneous combustion of coal and the effect of these compounds on
human health. Environ Res 2018;160:562–7.
[3] Gredilla A, de Vallejuelo SFO, Gomez-Nubla L, Carrero JA, de Leão FB,
Madariaga JM, et al. Are children playgrounds safe play areas? Inorganic
analysis and lead isotope ratios for contamination assessment in recreational
(Brazilian) parks. Environ Sci Pollut Res 2017;24:24333–45.
[4] Dutta M, Saikia J, Taffarel SR, Waanders FB, de Medeiros D, Cutruneo CM, et al.
Environmental assessment and nano-mineralogical characterization of coal,
overburden and sediment from Indian coal mining acid drainage. Geosci Front
2017;8:1285–97.
 M. Onifade, B. Genc / International Journal of Mining Science and Technology 28 (2018) 933–940
[5] Agudelo-Castañeda DM, Teixeira EC, Schneider IL, Pereira Felipe N, Oliveira
MLS, Taffarel SR, et al. Potential utilization for the evaluation of particulate and
gaseous pollutants at an urban site near a major highway. Sci Total Environ
2016;43:161–70.
[6] Agudelo-Castañeda DM, Teixeira EC, Schneider IL, Lara SR, Silva LF. Exposure to
polycyclic aromatic hydrocarbons in atmospheric PM 1.0 of urban
environments: carcinogenic and mutagenic respiratory health risk by age
groups. Environ Pollut 2017;224:158–70.
[7] de Vallejuelo SFO, Gredilla A, da Boit K, Teixeira EC, Sampaio CH, Madariaga JM,
et al. Nanominerals and potentially hazardous elements from coal cleaning
rejects of abandoned mines: environmental impact and risk assessment.
Chemosphere 2017;169:725–33.
[8] Saikia BK, Dalmora AC, Choudhury RD, Tonkeswar, Taffarel SR, Silva, et al.
Effective removal of sulfur components from Brazilian power-coals by
ultrasonication (40 KHz) in presence of H2O2. Ultrason Sonochem
2016;32:147–57.
[9] Civeira M, Oliveira MLS, Hower JC, Agudelo-Castañeda DM, Taffarel SR, Ramos
CG, et al. Modification, adsorption, and geochemistry processes on altered
minerals and amorphous phases on the nanometer scale: Examples from
copper mining refuse, Touro, Spain. Environ Sci Pollut Res Int
2016;23:6535–45.
[10] Civeira M, Pinheiro RN, Gredilla A, de Vallejuelo S, Oliveira MLS, Ramos CG,
et al. The properties of the nano-minerals and hazardous elements: potential
environmental impacts of brazilian coal waste fire. Sci Total Environ
2016;544:892–900.
[11] Civeira M, Ramos CG, Oliveira MLS, Kautzmann RM, Taffarel SR, Teiseira EC,
et al. Nano-mineralogy of suspended sediment during the beginning of coal
rejects spill. Chemosphere (Oxford) 2016;145:142–7.
[12] Schneider IL, Teixeira EC, Agudelo-castañeda DM, Silva ESG, Balzaretti N, Braga
MF, et al. FTIR analysis and evaluation of carcinogenic and mutagenic risks of
nitro-polycyclic aromatic hydrocarbons in pm1.0. Sci Total Environ
2016;541:1151–60.
[13] Sehn JL, de leão FB, da boit K, Oliveira MLS, Hidalgo GE, Sampaio CH, et al.
Nanomineralogy in the real world: a perspective on nanoparticles in the
environmental impacts of coal fire. Chemosphere (Oxford) 2016;147:439–43.
[14] Rodriguez-iruretagoiena A, de vallejuelo SF, De Diego A, de leão FB, de
Medeiros D, Oliveira MLS, et al. The mobilization of hazardous elements after a
tropical storm event in a polluted estuary. Sci Total Environ 2016;565:721–9.
[15] Dullien F. Porous media fluid transport and pore structure. Academic Press;
1979. p. 79.
[16] Bowes PC. Self-heating: evaluating and controlling the hazards. London:
HMSO; 1984.
[17] Singh RN, Demirbilek S. Statistical appraisal of intrinsic factors affecting
spontaneous combustion of coal. Int J Min Sci Technol 1987;1984(4):155–65.
[18] Morris R, Atkinson T. Seam factor and the spontaneous heating of coal. Int J
Min Sci Technol 1988:149–59.
[19] Carras J, Young B. Self-heating of coal and related materials: models,
application and test methods. Prog Energy Combust Sci 1994;20(1):1–15.
[20] Schopf JM. Definitions of peat and coal and of graphite that terminates the coal
series (Graphocite). Int J Coal Geol 1966;74(5):584–92.
[21] Jones JR, Cameron B. Modern coastal back-barrier environment: analog for coal
basin or carbonaceous black shale? Geology 1988;16:345–8.
[22] Querol X, Alastuey A, Lopez-Soler A, Plana F, Fernandez-Turiel JL, Zeng R, et al.
Geological controls on the mineral matter and trace elements of coals from the
Fuxin basin, Liaoning Province, Northeast China. Int J Coal Geol
1997;34:89–109.
[23] Genc B, Cook A. Spontaneous combustion risk in South African coalfields. J S
Afr Inst Min Metall 2015;115:563–8.
[24] Wade L. The propensity of South African coals to spontaneously combust [Ph.
D. thesis]. Johannesburg: Department of Mining Engineering, University of
Witwatersrand; 1989.
[25] Gouws MJ, Wade L, Phillips HR. Spontaneous combustion of South African
coals. In: Szwilski AB, Richards MJ, editors, Proceedings of the symposium on
underground mining methods and technology. Amsterdam: Elsevier Science
Publishers; 1987. p. 65–73.
[26] Bell FG, Bullock SET, Halbich TFFJ, Lindsay P. Environmental impacts associated
with an abandoned mine in the Witbank coalfield, South Africa. Int J Coal Geol
2001;45:195–216.
[27] Gouws MJ, Gibbo GJ, Wade L, Phillips HR. An adiabatic apparatus to establish
the spontaneous combustion propensity of coal. Min Sci Technol
1991;13:417–22.
[28] ASTM, D-3175. Standard test method for volatile matter in the analysis sample
of coal and coke. West Conshohocken, PA: ASTM International; 2017. www.
astm.org.
[29] ASTM, D-3174. Standard test method for ash in the analysis sample of coal and
coke from coal and standard classification of coals by rank. West
Conshohocken, PA: ASTM International; 2017. www.astm.org.
[30] ASTM, D-3173. Standard test methods for moisture in the analysis sample
of coal and coke. West Conshohocken, PA: ASTM International; 2017. www.
astm.org.
[31] ISO 12902:2001. Determination of total carbon, hydrogen and nitrogen.
[32] Ramos CG, Querol X, Dalmora AC, de Jesus PiresKC, Schneider IAH, Oliveira LFS,
et al. Evaluation of the potential of volcanic rock waste from southern Brazil as
a natural soil fertilizer. J Cleaner Prod 2017;142:2700–6.
[33] Wilcox J, Wang B, Rupp E, Taggart R, Hsu-kim H, Oliveira MLS, et al.
Observations and assessment of fly ashes from high-sulfur bituminous coals
939
and blends of high-sulfur bituminous and subbituminous coals:
environmental processes recorded at the macro and nanometer scale. Energy
Fuels (print) 2015;29:7168–77.
[34] Saikia BK, Ward CR, Oliveira MLS, Hower JC, de Leao F, Johnston MN, et al.
Geochemistry and nano-mineralogy of feed coals, mine overburden, and coal-
derived fly ashes from assam (north-east India): a multi-faceted analytical
approach. Int J Coal Geol 2015;137:19–37.
[35] Dalmora AC, Ramos CG, Querol X, Kautzmann RM, Oliveira MLS, Taffarel SR,
et al. Nanoparticulate mineral matter from basalt dust wastes. Chemosphere
2016;144:2013–7.
[36] Wade L, Gouws MJ, Phillips HR. An apparatus to establish the spontaneous
combustion propensity of South African Coals. In: Symposium on safety in coal
mines, CSIR, Pretoria; 1987. p. 7.1–7.2.
[37] Sensogut C, Ozdeniz AH. Statistical modelling of stockpile behaviour under
different atmospheric Conditions-Western lignite corporation (WLC) case. Fuel
2005;84:1858–63.
[38] Ozdeniz AH, Sivrikaya O, Kelebek S. Statistical modelling of spontaneous coal
combustion due to effect of the sunray’s. Energy Sources Part A
2015;37:2114–22.
[39] Kunii D, Levenspiel O. Fluidization engineering. New York: Krieger; 1991.
[40] McPherson MJ. Subsurface ventilation and environmental engineering.
University Press; 1993. p. 23.
[41] Beamish BB, Hamilton GR. Effect of moisture content on the R70 self-heating
rate of callide coal. Int J Coal Geol 2005;64:133–8.
[42] Gurdal G. Abundances and modes of occurrence of trace elements in the Can
coals (Miocene), Canakkale-Turkey. Int J Coal Geol 2011;87:157–73.
[43] Gurdal G, Bozcu M. Petrographic characteristics and depositional
environment of Miocene Can coals, Canakkale-Turkey. Int J Coal Geol
2011;85:143–60.
[44] Pone JDN, Hein KAA, Stracher GB, Annegarn HJ, Finkleman RB, Blake DR, et al.
The spontaneous combustion of coal and its by-products in the Witbank and
Sasolburg coalfields of South Africa. Int J Coal Geol 2007;72:124–40.
[45] Cutruneo CMN, Oliveira MLS, Ward CR, Hower JC, de brum IAS, Sampaio CH,
et al. A mineralogical and geochemical study of three Brazilian coal cleaning
rejects: demonstration of electron beam applications. Int J Coal Geol
2014;130:33–52.
[46] Oliveira MLS, Marostega F, Taffarel SR, Saikia BK, Waanders FB, Daboit K, et al.
Nano-mineralogical investigation of coal and fly ashes from coal-based captive
power plant (India): an introduction of occupational health hazards. Sci Total
Environ 2014;468–469:1128–37.
[47] Saikia BK, Colin R, Oliveira MLS, Hower JC, Braga M, Silva LF. Geochemistry and
nano-mineralogy of two medium-sulfur northeast Indian coals. Int J Coal Geol
2014;122:1.
[48] Saikia BK, Ward CR, Oliveira MLS, Hower JC, Baruah BP, Braga M, et al.
Geochemistry and nano-mineralogy of two medium-sulfur northeast Indian
coals. Int J Coal Geol 2014;121:26–34.
[49] Martinello K, Oliveira MLS, Molossi FA, Ramos CG, Teixeira EC, Kautzmann RM,
et al. Direct identification of hazardous elements in ultra-fine and
nanominerals from coal fly ash produced during diesel co-firing. Sci Total
Environ 2014;470–471:444–52.
[50] Silva LFO, Marcos LS, Oliveira MLS, Kautzmann RM, Ramos CG. Geochemistry
and mineralogy of coal-fired circulating fluidized bed combustion fly ashes.
Coal Combust Gasification Prod 2014;6:16–28.
[51] Garcia KO, Teixeira EC, Agudelo-castañeda DM, Braga M, Alabarse PG, Wiegand
F, et al. Assessment of nitro-polycyclic aromatic hydrocarbons in pm1 near an
area of heavy-duty traffic. Sci Total Environ 2014;479–480:57–65.
[52] Kaymakci E, Didari V. Relations between coal properties and spontaneous
combustion parameters. Turk J Eng Environ Sci 2002;26(1):59–64.
[53] Banerjee SC. Prevention and combating mine fires. Oxford and IBH Publishing
Co., Pvt. Ltd.; 2000. p. 33.
[54] Hagelskamp HHB, Snyman CP. On the origin of low-reflecting inertinites in
coals from the Highveld coalfield, South Africa. Fuel 1988;67:307–13.
[55] Snyman CP, Botha WJ. Coal in South Africa. J Afr Earth Sc 1993;16:171–80.
[56] Van Niekerk D, Pugmire RJ, Solum MS, Painter PC, Mathews JP. Structural
characterization of vitrinite-rich and inertinite-rich Permian-aged South
African bituminous coals’. Int J Coal Geol 2008;76:290–300.
[57] Falcon RMS, Ham AJ. The characteristics of Southern African coals. J S Afr Inst
Min Metall 1988;88(5):145–61.
[58] Choudhury N, Boral P, Mitra T, Adal AK, Choudhury A, Sarkar P. Assessment of
the nature and distribution of inertinite in Indian coals for burning
characteristics’. Int J Coal Geol 2007;72:41–152.
[59] Životić D, Stojanović DK, Gržetić I, Jovančićević B, Cvetković O, Šajnović A, et al.
Petrological and geochemical composition of lignite from the D field, Kolubara
basin (Serbia). Int J Coal Geol 2013;111:5–22.
[60] Siavalas G, Linou M, Chatziapostolou A, Kalaitzidis S, Papaefthymiou H,
Christanis K. Palaeoenvironment of Seam I in the Marathousa Lignite Mine,
Megalopolis Basin (Southern Greece). Int J Coal Geol 2009;78:233–48.
[61] Sia GS, Abdullah WH. Geochemical and petrographical characteristics of low-
rank Balingian coal from Sarawak, Malaysia: its implications on depositional
conditions and thermal maturity. Int J Coal Geol 2012;96–97:22–38.
[62] Taylor GH, Teichmüller M, Davis A, Diessel CFK, Littke R, Robert R. Organic
petrology. Berlin: Gebrüder Borntraeger; 1998. p. 704.
[63] Humphreys D, Rowlands D, Cudmore JF. Spontaneous combustion of some
Queensland coals. Proc Ignit Explos Fires Coal Min Symp 1981;5:1–19.
[64] Smith AC, Miron Y, Lazzara P. Inhibition of spontaneous combustion of coal, US
Bureau of Mines Report of Investigation; 1988, RI 9196.
940 M. Onifade, B. Genc / International Journal of Mining Science and Technology 28 (2018) 933–940
[65] Roberts DL. Chromium speciation in coal combustion by products: case study
at a dry disposal power station in Mpumalanga province, South Africa, Thesis
for Doctor of Philosophy. Johannesburg: University of the Witwatersrand;
2008. p. 60–76, 112–127.
[66] Department of Minerals and Energy South Africa (DME) Mineral Economics
Directorate (Minerals Bureau). Operating and Developing coal mines in the
Republic of South Africa. Directory; 2004, D2/2004.
[67] Czaplicki A, Smolka W. Sulfur distribution within coal Pyrolysis products. Fuel
Process Technol 1998;55:1–11.
[68] Casangrande DJ, Gronli K, Sutton N. The distribution of sulfur and organic
matter in various fractions of peat origins of sulphur in coal Geochim.
Cosmochim Acta 1980;44:25–32.
[69] Cohen AD, Spackman W, Deben P. Occurrence and distribution of sulphur in
peat forming environment of southern Florida. Int J Coal Geol 1984;4:73–96.
[70] Given PH, Miller RN. Distribution of forms of sulphur in peats from saline
environments in the Florida Everglades. Int J Coal Geol 1985;5:397–405.
[71] Teichmüller M, Teichmüller R. The geological basis of coal formation. In: Stach
E, editor, Stach’s Textbook of Coal Petrology, 3rd ed., Borntraeger, Berlin; 1982.
p. 5–86.
[72] Gryglewicz G, Rutkowski P, Yperman J. Characterization of Sulfur compounds
in Supercritical coal extracts by gas chromatography-mass spectrometry. Fuel
Process Technol 2002;77–78:167–72.
[73] Hsieh KC, Wert CA. Direct determination of organic sulphur in coal. Fuel
1985;64(2):255–61.
[74] Olivella MA, Palacios JM, Vairavamurthy AC, de las Heras FXC. A study of
sulphur functionalities in fossil fuels using destructive (ASTM and Py-GC-MS)
and non-destructive (SEM-EDX-XANES and XPS) techniques. Fuel
2002;81:405.
[75] Wagner NJ, Hlatshwayo B. The occurrence of potentially hazardous trace
elements in five Highveld coals, South Africa. Int J Coal Geol 2005;63:228–46.
[76] William HC. The chemical forms of sulfur in coal. Fuel 1994;73:475–84.
[77] Stach E, Zierke F, Taylor GH, Murchison D. Stach’s textbook of coal petrology.
2nd ed. Berlin: Gebruder Borntraeger; 1975. p. 387–8.
[78] Suarez-Ruiz I, Crelling JC, editors, Applied coal petrology. The role of petrology
in coal utilization. Elsevier; 2008. p. 388.