The Rate of Temperature Rise of a Subbituminous Coal during

Spontaneous Combustion in an Adiabatic Device: The Effect of

Moisture Content and Drying Methods
W. E. VANCE, X. D. CHEN* and S. C. SCOT1TM
Department of Civil and Resource Engineering (formerlyDepartment of Mining Engineering) (W.E. V., S.C.S.),
Department of Chemical and Materials Engineering (X.D.C.), The Universityof Auckland, Auckland City,
New Zealand

This work investigates the effect of the moisture content of coal on its spontaneous ignition in oxygen
(40°C-140°C). It has been found that the highest heating rate is achieved at a m e d i u m moisture content of
~ 7 wt% for an initial inherent moisture content of the coal before drying (in dry nitrogen at 65°C) of - 20
wt%. This is particularly noticeable at temperatures below 80°C and tends to support previous studies
showing that a m a x i m u m oxidation rate occurs at such a moisture content in the same temperature range.
Two drying m e t h o d s have been adopted in the current work and the effects of their operating conditions on
the heating rates are described.

INTRODUCTION absorption and desorption of water vapor in

The important role of moisture on the devel-
opment of spontaneous combustion of coal is
now well recognized. However, the effect of
moisture has not yet been fully comprehended
and quantified [1, 2]. This paper is an attempt
to investigate further the effect of moisture
content on the spontaneous combustion of a
subbituminous coal.
Role of Moisture in Spontaneous Combustion
In general, one can divide the overall effect of
moisture content (and its transfer inside a coal
stockpile pile or during mining of coal under-
ground) into two aspects [2, 3], namely (i) the
effect of moisture transfer (evaporation, con-
densation, diffusion and convection) on the
overall heat balance; (ii) the effect of moisture
(at equilibrium or during drying or wetting) on
the rate of coal oxidation. The complex nature
of the above effects hindered a comprehensive
mathematical modeling of spontaneous corn-
bustion, as well as a comprehensive practical
application of the information generated over
some 70 years since Winmill [4] and Graham
[5]. The effect of moisture transfer i.e., (i) was
initially emphasized by Berkowitz [6] and Stott
and Baker [7]. They showed how the heat of
* Corresponding attthor,
COMBUST1ON AND FLAME 106:261-270 (1996)
Copyright © 1996 by The Combustion Institute
Published by Elsevier Science Inc.
coal is a very strong controlling factor in the
spontaneous heating of coal. Bannerjee [8],
summarized the major conclusions from these
earlier studies. Others [9-18] have published
further related experimental and theoretical
work.
With respect to the effect of moisture con-
tent on the oxidation rate, i.e., (ii), it has been
found that a coal reacts with oxygen more
rapidly when wet than when dry, at room tern-
perature [19]. Other studies [20, 21], however,
suggested that stripping moisture from coal
exposes more fresh active sites on the coal's
surface for contacting oxygen and thereby ac-
celerates oxidation. The work carried out by
Mukherjee and Lahiri [22], later summarized
by Beier [19], showed that, at temperatures
above 70°C, the oxidation of coals occurs more
readily in dry than in moist air. This could be
explained by noting that Berkowitz [23] pub-
lished evidence to show that the mechanism of
coal oxidation was not the same above 70°C as
at lower temperatures. Below 70°C the oxida-
tion rate is low enough to be unaffected by
restrictions on the supply at the coal surface.
Only acid functions and peroxides are gener-
ated [23] and a higher moisture content pro-
motes these reactions. Above 70°C but lower
than 150°C, however, moisture plays a differ-
ent role as peroxides form only transiently or
not at all.
0010-2180/96/$15.00
SSDI 0010-2180(95)00276-6
262
Sondreal and Ellman [27] showed conclu-
sively that the oxidation rate of a lignite in-
creased as the moisture was being removed
until a moisture content of ~ 20 wt% was
reached, when it fell as the moisture was fur-
ther driven off. However, in their experiments,
this trend becomes less conspicuous when the
temperature increases to 70°C. Chen and Stott
[3] studied the effect of changes in the mois-
ture content of a subbituminous coal with
"near-equilibrium" drying and wetting at 50°C.
Similar behavior as that found by Sondreal and
Ellman [24] was obtained, although the mecha-
nism described was slightly different from the
work by Chen and Stott [3].
It has also been found by Unal et al. [25]
that different drying methods can affect the
oxidation rate, Chen and Stott [3] used a near-
equilibrium drying procedure (very low rate of
drying) with nitrogen; this gave different trends
for how the oxidation rate was influenced by
moisture content from that investigated using
a vacuum drying procedure [26]. Vacuum dry-
ing was believed [26] to have damaged the solid
structure of coal, thereby causing the variation,
The Adiabatic Methods
In practice, one is usually concerned about the
overall effect of moisture on the spontaneous
combustion of coal, i.e., the effect over the
whole process of ignition. The adiabatic system
to be described later is well-suited for such a
purpose. In order to label the coal's propensity
to fire spontaneously, many devices have been
built to try to enable a thorough evaluation,
e.g., the adiabatic method [27], the crossing
point method [28, 29], the isothermal method
[10] and the ignition temperature method [30].
Of these methods, the adiabatic one appears to
be used more often, due to the small sample
size and simplicity of the system. However, this
does not mean that the test can represent
comprehensively spontaneous combustion in
TABLE 1
Proximate Analysis of Renown Seam Coal, Huntly East
(Provided by Coal Research Association of New Zealand Ltd.)
Moisture Ash Fixed carbon
20.5 wt% 3.9 wt% 39.5 wt%
W. E. VANCE ET AL.
practice, e.g., this test would not provide a full
picture of heat and mass transfer during heat-
ing. This test can, at least, be used to study
the effects of oxidation rate, reabsorption of
water vapour, degree of dryness on sponta-
neous combustion of coal. The adiabatic sys-
tern used in the current study is a modified,
robust version of that developed by Humphrey
et al. [31]. The work focused on the effect of
moisture content and the effects of the two
drying methods.
EXPERIMENTAL PROCEDURES
Sample Preparation
A fresh sample of Renown Seam coal was
obtained from the Huntly East mine in New
Zealand. It was stored in an airtight container
for transportation to our laboratory. To simu-
late the behaviour of freshly crushed coal par-
titles, the large coal lumps were reduced in
size to about 210 /zm in a three-stage opera-
tion involving: Jaw and cone crusher and ham-
mer mill. The coal particle sizes were also
limited by the small volume of the test vessel
and the size of the adiabatic oven. The crushed
coal was then sealed in airtight bags at room
temperature until required. To prevent exces-
sive preoxidation before subsequent experi-
ments, once the coal was reduced to the final
size, the coal was bagged separately in approxi-
mately 150 g lots. The coal is of subbituminous
rank and the proximate analysis is given in
Table 1. In order to study the effect of differ-
ent drying methods and the effects of moisture
content on spontaneous heating rate, several
samples with different moisture content had to
be obtained by following two different drying
methods:
(D1) Drying tube method. A sample of ~ 150
g of coal each time was placed in a drying
tube. The drying tube was placed in a stan-
dard laboratory oven which previously had
Volatile Matter Calorific Value Sulphur
36.1 wt% 22.71 M J / k g 0.2 wt%
EFFECT OF MOISTURE ON COAL COMBUSTION
been heated to 110°C. A nitrogen flow of
about 600 m l / m i n at 20°C and 1 atm was
passed through the sample, with the oven
maintained at 110°C. Upon completion of
each drying trial of typically 8-12 h, the
tube was removed from the oven and the
coal was allowed to cool in an inert atmo-
sphere of dry nitrogen,
(D2) Minimum free space drying method. The
oven was designed so that coal could either
be dried in a vacuum or an atmosphere of
nitrogen. The oven consists of a cast alu-
minium chamber with a front lifting vacuum
seal door. Inside the oven is a rack that can
take up to 6 trays. A coal sample is placed
on these trays for drying. Heating is pro-
vided by elements at the bottom of the
oven. Preheating chambers are provided in
the side and top of the oven for nitrogen
flow. In the current study, nitrogen ( ~ 3000
m l / m i n at 20°C and I a t m ) was passed
through these chambers via a flow meter,
20-
'" (
16-
I
i~ 102
4- / ~
/
2-
0 f
Time (hrs)
Fig. 1. Typical drying curves using different drying methods.
263
The temperature is controlled by an insu-
lated thermocouple (at the top of the oven)
connected to a PID controller. Two temper-
atures were used, i.e. for two separate dry-
ing runs; they were 65 ° and 110°C. The first
one was expected to give minimum damage
to the coal sample prepared. Samples of
different moisture contents were prepared
using the two drying methods for various
purposes of the current study to be de-
scribed later. Figure 1 shows the typical
drying curves for the different methods of
drying. It can be seen that the drying tube
method gives a much slower drying than the
minimum free space oven at either 110° or
65°C. The high temperature of 110°C used
above in drying was intended to see if there
was any difference in the behaviour of coals
dried at the low temperature. The results
from this high-temperature drying may be
closely related to commercial coal drying,
which employs elevated temperatures.
ng Tube llO o c
264
The Adiabatic System for Spontaneous
Combustion Test
In this study, an adiabatic oven was designed
like that by H u m p h r e y et al. [31]. The oven was
built by the Electric Furnace Company Auck-
land and consists of three essential parts: the
reaction vessel, the oven, and the controller. A
coal sample is filled in the reaction vessel. This
is illustrated in Fig. 2 and is a 500-ml vacuum
thermal flask. The top of the flask is fitted with
a Teflon plug. The Teflon plug is held in place
by two springs. These springs, in conjunction
with a rubber washer, ensure an airtight seal
when the apparatus is in use. The vessel is
fitted on the inner side wall of the oven door
by a supporting bracket to allow easy access to
the vessel and its attachments. Passing through
the Teflon plug are two glass tubes, one of
these tubes is 150 mm long with an internal
diameter of 3 mm. The end of this tube is
pointed to allow easy access through the coal.
A type K thermocouple monitors the tempera-
ture rise. The second tube of the same diame-
ter is used as an exhaust to allow reaction
product gases to be released,
To investigate a spontaneous heating, the
controller mode was initially set to "manual"
and the oven was preheated to 40°C. The reac-
tion vessel was clamped in place. Nitrogen (50
m L / m i n at 20°C and 1 atm) was passed to
allow stabilization of the coal at 40°C. The
oven was then set at the "automatic" mode
and the data acquisition system was activated
to follow the heating (recording temperature
rise) once every minute. This mode of opera-
tion allowed the oven temperature to follow, as
closely as possible, the temperature of the coal
(measured by a thermocouple located in the
reaction vessel, as shown in Fig. 2) as heating
progressed. The gas supply was then switched
to oxygen flowing at similar rate to initiate
oxidation. The gas stream was preheated in a
copper coil of ~ 16 m long, also located on
the inner wall of the oven door. A heat balance
calculation on the oven an oxygen flow inside
the copper tube (assuming a low heat transfer
coefficient of 2 W / m 2 K between the oven and
the tube) indicates that the length of the cop-
per tube ( ~ 16 m) is sufficient to allow the
oxygen (50 m L / m i n at 20°C and 1 atm) to be
W . E . V A N C E E T AL.
heated to the oven temperature, very quickly
on entry to the reaction vessel. The oven safety
shut-off was activated at 150°C; this stopped
the flow of oxygen and hence allowed the oven
and coal sample to cool.
The absolute error in heating time has been
found to be + 0.3 h for a test that completes
the heating up to 140°C within 5 h, but the
error deteriorates to +_.1.5 h if the process lasts
more than 15 h. However, the reproducibility
of each experiment between the start and the
temperature of 100°C was found to be better
than + 0.2 h, if the whole experiment stops in
5 h.
RESULTS AND DISCUSSION
The Effect of Moisture Content on
Spontaneous Ignition of Coal
To study this effect, several coal samples of
different moisture contents were prepared by
the drying method D2 at 65°C (see Table 2).
Drying at this fairly low temperature was ex-
pected to cause minimum structural damage to
the coal, compared with vacuum drying or the
same type of drying at a much higher tempera-
ture, e.g., l l 0 ° C [3]. In all the tests performed,
as soon as the temperature went beyond 140°C,
thermal run away became evident. The tem-
p e r a t u r e - t i m e profiles as influenced by the
initial moisture contents are shown in Fig. 3.
One can see that the time required to reach
140°C varied with initial moisture contents of
the samples. There is a medium moisture con-
tent of ~ 7 wt%, beyond or below which the
rate of temperature rise decreases. The times
to reach 80°C and 140°C can also be found in
Table 2 for each sample (Instead of 40°C, 42°C
was used in the calculations as the initial tern-
perature; this is to avoid error caused by the
initial operation that switched the gas flow
from nitrogen to moist oxygen.) The rates of
temperature rise for all the samples in Table 2
were calculated between temperature intervals
45°-60°C, 60°-80°C and 80°-100°C are plotted
in Fig. 4. The data provided in Table 2 as well
as the heating rates shown in Fig. 4 illustrate
that the considerable differences in rate of
temperature rise started to occur right from
the beginning of the experiments, which have
EFFECT OF MOISTURE ON COAL COMBUSTION 265

Gas InletPipe ~----x

ThermocoupleLeadsTo
Controller/DataLogger. " I GasOutletPipe
~ f / j BrassFlange

TeflonPlug

~ .~ l RubberGasket
~/ I Seal

I I
i I
i
SpringsFor
SecuringPlug

, ApproximateCoal
j Level
I
i

'-4---- ~ VacuumFlask

I ..~ Type K

' ' 4// TeflonSupporting

j Lk __ Cup
I I

'~' SupportBracketsOnOvenDoor
Fig. 2. The adiabatic system.

shown the great importance of the oxidation
rates at these low temperatures. It can be seen
that the maximum rate appears to shift, as
temperature increases, towards a higher mois-
ture removal (i.e. small amount of residual
moisture). More drastic changes in heating
rates with increasing moisture removal oc-
curred at high residual moisture contents. If
this trend was due to a change in the specific
heat (Cp) and the density of coal ( p ) with
moisture, it would require that their product
(pCp) in the energy balance of self-heating
266 W. E. V A N C E E T AL.

TABLE2
Coal Sampleswith Different Moisture Contents Obtained Using the Minimum Free Space Oven Method Operated
Under Nitrogen Flow at 65°C; Time to 80~Cand Time to 140°C.
Moisture Content (wt%)a Time to reach 80~C(h) Time to reach 140~C(h)
15.7 10.1 16.2
14.3 8.1 12.4
11.7 6.0 8.6
9.5 4.5 6.2
8.3 3.2 4.7
5.0 4.0 4.9
4.5 4.2 5.0
Retained moisture content based on inherent moisture content of 20.5 wt% of the crushed coal before drying; the
crushing did not appear to alter this value to more than +0.5%.

[14] possessed a minimum value at the corre-
sponding moisture content. A coal sample with
zero moisture content has the lowest density
(due to dry pores) and with any increase in
moisture content without swelling (due to in-
teraction with water) this density must in-
crease. Similarly, the specific heat of coal
should increase from that of the dry coal with
addition of moisture inside the pores. As a
result, ( p C p ) should increase monotonically
with increasing moisture content. This, there-
fore could not have caused the maximum tem-
perature rise at a medium moisture content,
Previous studies [3, 24] have demonstrated the
effect of moisture content on oxidation rate
under isothermal conditions at or below 70°C.
A maximum oxidation rate occurs at a medium
moisture content, for a very similar sub-hi-
tuminous coal investigated by Chen and Stott
[3]. These previous findings are therefore sup-
ported by the current study. The current study
is more significant in the sense that it gives, for
the first time, the integrated effect of moisture
on the whole ignition process (from about 40 °
to 140°C).
The Effect of Drying Methods on
Spontaneous Ignition
As shown in Table 3, several samples were
prepared to show a comparison between the
performance of various drying methods
adopted in the current study. Table 3 shows
that the drying method D2 at 110°C did not
give reproducible results; this may be caused
by the nonuniform temperature distribution in
the minimum free space oven as detected.
However, a lower temperature, e.g., 65°C, gave
fairly consistent results. The drying method D1
at l l 0 ° C also produced reproducible results. It
is interesting to note that the heating rate
obtained using D1 at l l 0 ° C was at least twice
as much as that when using D2 at 65°C while
only a difference in moisture content of ~ 2
wt% between the two. To explain this observa-
tion, it would have been desirable to have full
chemical analyses before and after drying. Pro-
cedure D2 at l l 0 ° C consistently gave the lower
rates of heating compared with D1 at ll0°C.
The explanation is not dear. One apparent
reason causing a slower rate for D2 at l l 0 ° C
was that the dried coal samples reabsorbed
moisture from the ambient air while cooling in
open air. In one case recorded, a sample picked
up 1% moisture in 40 min. During this period,
the coal started at a temperature of ~ 100°C,
which should lead to a fast rate of preoxida-
tion. Normal stockpiling is unlikely to produce
a drying process as severe as that described for
D1 and D2 at 110°C. Laboratory studies car-
ried out using such a high temperature may
not be relevant to practice. On the other hand,
drying at low temperatures would not give in-
formation related to the handling of commer-
cial coals dried at elevated temperatures.
Observations on the Effects of Weathering
and Gas Humidity
With its inherent moisture content, the coal
could not self-heat and a maximum tempera-
ture rise of about 3°C was observed. A fresh
 ~
.~" Temperature (oc) Temperature (°C) ~'J

~ •

• r.~

5 u • ,-1 0
g~ g z
[ " •

g ~

b~
268 W . E . V A N C E E T AL.

40,

35"

30"

"t:l
O
"" 20"

taO
15"

10-
,- [c,0.-80d~g.

~ 5 - ~ deg-C I

Moisture Content (wt%)

Fig. 4. Rate of temperature rise in different temperature ranges as influenced by moisture content.

TABLE 3 sign of spontaneous heating. Two dried sam-

Coal Sampleswith Different Moisture Contents Obtained ples obtained using D2 at l l 0 ° C with similar
using the Two Drying Methods (DI and D2); Time moisture removal ( ~ 18.5 wt%) were tested
to 140°c. separately. One was exposed to saturated oxy-
Moisture Removed Time to reach gen and another reacted with dry oxygen (in
(wt%) Drying Method 140°C(11) both cases, the dry oxygen flow rates remained
18.6 D1, ll0°C 1.5 the same). The former gave a faster rate of
18.9 D1, ll0°C 1.8 heating as expected, since the reabsorption of
18.8 D1, ll0°C 1.8 water vapour released the latent heat of water
18.4 D2, ll0°C 3.6 vaporization (as shown in Fig. 6). In this moist
18.5 D2, ll0°C 2.8 case, a saturated oxygen flow was required. All
18.5 D2, ll0°C 5.2
16,0 D2, 65°C 4.9 these observations reconfirm previous findings,
15.4 D2, 65°C 4.4 e.g., those by Guney and Hodges [27] and Stott
15.5 D2, 65°C 5.0 [29] etc.

sample with inherent moisture content and an
old sample with similar moisture content, after
4 months of exposure to air at room tempera-
ture, were tested for their tendency to self-heat,
The t e m p e r a t u r e - t i m e profiles are shown in
Fig. 5, the old coal sample did not show any
CONCLUSIONS
For the first time, the integrated effect of
moisture of a subbituminous coal on its self-
ignition process (40" to 140°C) has been stud-
ied. It has been found that, at a medium mois-
ture content of ~ 7 wt%, the self-heating rate
EFFECT OF MOISTURE ON COAL COMBUSTION 269

42-

40-~ / Fresh Sample

38.-

36-

:32-

30- ~ _ Ola Sample

28 , i , ~ ...... "~
2 4 6 S llO ll2 14 16

Time (hrs)
Fig. 5. The effect of pre-oxidation on temperature-time profile.

160 .

140-

120.

o
,~ lO0-

Wet

E- 80-
Dry Oxygen

60-

4O I
0 015 i 115 2 215 3

Time (hrs)
Fig. 6. The effect of wetting on temperature-time profile.
270
( r a t e o f t e m p e r a t u r e rise) is a m a x i m u m . T h i s
is most pronounced at temperatures below
80°C. This supports the previous work on oxi-
d a t i o n r a t e as i n f l u e n c e d b y m o i s t u r e c o n t e n t .
The drying method adopted, when using a rela-
tively h i g h t e m p e r a t u r e o f 110°C, gave less
reproducible results. This may be attributed to
"thermal damage" on the solid structure and
un-controlled re-absorption of moisture, by a
v e r y dry coal.
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Received 3 January 1995; accepted 10 December 1995