Procedia Engineering 84 ( 2014 ) 330 – 339
1877-7058 © 2014 Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/3.0/).
Peer-review under responsibility of scientific committee of Beijing Institute of Technology doi: 10.1016/j.proeng.2014.10.441
ScienceDirect
“2014ISSST”, 2014 International Symposium on Safety Science and Technology
Experimental analysis of minimum ignition temperature of coal dust
layers in oxy-fuel combustion atmospheres
Dejian WU
a, Frederik NORMAN
b, Filip VERPLAETSEN
b, Jan BERGHMANS
a,
Eric Van DEN BULCK
a*
aKatholieke Universiteit Leuven, Department of Mechanical Engineering, Celestijnenlaan 300A, B3001 Leuven, Belgium bAdinex NV, Brouwerijstraat 5/3, B 2200 Noorderwijk, Belgium
Abstract
An experimental investigation into the hot surface ignition of coal dust layers has been undertaken in oxy-fuel combustion atmospheres, with the oxygen mole fractions in the range of 21-50 vol. % (21%, 30%, 40% and 50%). Three coals were used to determine the minimum layer ignition temperature (MLIT) with a hot surface ignition apparatus according to the European EN50281-2-1 norm. In addition, thermal and kinetic parameters were also determined. Layer thicknesses of 5, 12.5, 15, 20 and 30mm were investigated. Firstly, 5 and 12.5mm thick coal dust layers were used to investigate the influence of the oxygen mole fraction on the MLIT, and the steady state dust layer temperature profile of a 30mm thick coal dust layer was used to estimate the thermal conductivity (k) at a low hot surface temperature. Secondly, the South African coal was used in this study to determine the kinetic parameters on the basis of the Frank-Kamenetskii theory. Results show that oxygen concentration has a significant influence on the MILT, (i.e., MLIT decreases with increasing oxygen concentration). It also shows that replacing N2 in the combustion air with CO2 a small increase of the MLIT will occur. The estimated k of the coal dust samples is respectively 0.1, 0.11 and 0.1W m -1K-1for South African coal, Sebuku coal and Pittsburgh coal. The region of the kinetic parameters of South
African coal changes when there is a shift in the test from air to oxy-fuel combustion atmospheres,which means that the reaction mechanism of self-heating or ignition changed somewhat.
© 2014 The Authors. Published by Elsevier Ltd.
Peer-review under responsibility of scientific committee of Beijing Institute of Technology.
Keywords: oxy-fuel combustion; minimum ignition temperature; dust layer; hot surface; thermal and kinetic parameters
* Corresponding author. Tel.: +0032 16 322 509; Fax: +0032 16 322 985.
E-mail address: [email protected]
© 2014 Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/3.0/).
1.Introduction
Self-heating of coal is the process by which coal achieves temperatures higher than ambient caused by exothermic reactions when coal is exposed to surrounding atmosphere without an external ignition source [1-3]. Self-ignition or spontaneous combustion, also defined as supercritical self-heating or thermal runaway, is quite hazardous in many powder industrial processes and in applications such as storage of porous bulk materials [4-7] and dust accumulations on a hot surface [8-14]. Self-ignition may cause fires and even dust explosions in the worst case [15]. Self-ignition of a dust layer depends on many factors, which can be divided into two main types: properties of coal (internal factors) and the environmental conditions (external factors) [16]. Previous researchers have investigated the effect of layer shrinkage [8], inerts [9], heat flux [10], air flow [11] and the estimation of thermo-kinetic parameters [12], as well as confinement geometry [13] and ignition position [14]. Despite the vast studies on self-ignition of coal, only a few works have investigated the effect of oxygen concentration on self-ignition [4, 6].
Oxy-fuel combustion, as one of the most promising technologies for CO2 emissions, has been advancing in recent
years [17-19]. In the oxy-fuel combustion system, dust may be processed or deposited in oxygen-enriched environments where little or nothing is known about the spontaneous ignition risk. The minimum ignition temperature of coal dust layers is studied with various oxygen concentrations by means of a heated surface. In addition, one test series was carried out to determine the thermal and kinetic parameters that are necessary in mathematical modeling.
2.Experiments
Hot plate ignition tests of 3 coal dust layers from different locations were conducted at various gas environments:
South African coal, Indonesian Sebuku coal, and Pittsburgh No.8 coal. Hereafter these coals are referred to as “SA
coal”, “IS coal”, and “P8 coal” respectively. 5 stainless rings of different height (5, 12.5, 15, 20 and 30mm) were employed and corresponding thermocouples were placed at the specified heights for each ring as shown in Table 1. Specifically, the results of the coal samples from the 5 and 12.5mm layer were used to estimate the influence of the oxygen concentration on the minimum ignition temperature of dust layer. The steady state temperature distribution in the 30mm layer was used to determine the thermal conductivity. The Kinetic parameters of SA coal were determined with the results of the MLIT experiments with 5 different thicknesses.
Table 1.The experimental outline and objectives.
Ring with thermocouples Gas environment Ring height L (mm) Thermocouple height (mm) air 21 vol.% O2 in CO2 30 vol.% O2 in CO2 40 vol.% O2 in CO2 50 vol.% O2 in CO2 5 2 3 samples 12.5 4, 7 and 10 3 samples - 15 3, 6, 9 and 12 SA SA SA SA - 20 5, 10 and 15 SA SA SA SA - 30 6, 12, 18 and 24 3 samples (steady state) - - SA - SA
2.1.Coal dust samples and gas composition
The coal samples were first milled or sieved (SA coal and IS coal were milled and sieved < 63 μm, and
Pittsburgh No.8 coal was milled < 200 μm). Next these coals were dried in a vacuum oven at 80 °C and 0.1 bar until
the moisture content was maximum 3%. Proximate and ultimate analysis data are given in Table 2. According to their compositions, IS coal can be classified as a subbituminous coal, while SA coal and P8 coal are bituminous coals.The gas mixtures consisted of air and various oxygen mixtures with carbon dioxide. Beginning with 21 vol. %
O2 and 79 vol. % CO2, the oxygen mole fraction was increased in increments of 10% from 30 vol. % up to 50 vol. %
O2 in CO2 with an accuracy of ± 1%.
Table 2. Properties of the coal dust samples.
Properties Coal Samples
IS P8 SA Proximate analysis (wt. %) Fixed carbon 47 55.6 56.6 Volatile material 38.2 31 27.1 Moisture content 3 3 2.1 Ash 11.8 10.4 14.2 Ultimate analysis (%) Carbon 65.7 73.8 67.5 Hydrogen 5.22 4.82 4.26 Nitrogen 1.58 1.29 1.76
Oxygen (by difference) 27.5 20.09 26.48 Gross calorific value (MJ kg 1) 27.65 29.78 27.37 Packing density (kg m 3) 645±5 620±5 600±5
2.2.Experimental apparatus and procedure
The fundamental apparatus and procedure of the dust layer test on a constant hot surface are similar to the European EN50281-2-1 norm [20]. A dust layer is placed on a hot plate, its temperature controlled by an automated control system. In order to carry out the test at oxy-fuel combustion atmospheres, an isolation glass box (about 400L) with two gloves is added as shown in Fig. 1. The experimental setup consisted of a circular stainless steel plate
25.4mm in thickness and 203mm in diameter, and stainless steel rings with an internal diameter (D) of 100mm.
The rings were placed at the center of the temperature-controlled plate with a thermal stability of 1°C. The thermocouples were set in the specified rings (see in Table 1) in order to measure the temperature profile of the dust layer. Once the hot plate temperature is stable at a predetermined temperature, the ring was gently filled with dust sample and was leveled with a spatula without compressing. Any extraneous dust on the hot plate was removed. The thermocouples were connected to the data collection system. It should be noted that all coal samples were put in the
corner of the glass box that was already flushed by the premixed O2/CO2 gas. All the operations were conducted in
the isolation glass box with vacuum chamber gloves.
When the test starts, the mixture gas was blown into the oven at a rate of 270 L/h measured by a rotameter. Ventilation was provided to exhaust any gases released from the dust sample. The concentration of oxygen in the box was adjusted by the gas flow controller. An iterative procedure was used to determine the ignition temperature within 5°C. The temperatures were recorded simultaneously every 10 seconds. Ignition is considered to have occurred if visible glowing or flaming is observed, a temperature of 450°C is reached, or a temperature rise of 250°C above the hot surface temperature is measured. If none of these conditions is satisfied after a delay (e.g. 30 min for 5 mm layer), ignition is considered to have not occurred.
3.Experimental results and discussion
3.1.Dust Layer temperature evolutions: 5mm
Typical temperature profiles for self-heating and ignition of dust layers are shown in Fig.2 (a) for 5mm layers.
The critical ignition temperature (the MLIT orTc) is supposed to be at the region between the maximum subcritical
and the minimum supercritical, e.g. 235-240°C for the IS coal, and 240-245°C for the SA coal and the P8 coal in the case of Figure 2 (a). It is clear that the critical ignition temperature of the IS coal is a bit lower than that of the others, which may result from IS coal’s higher volatile contents (see in Table 2). The observation that IS coal was more likely to produce smoke can also support this result. Even so, the induction time to ignition of the IS coal is much longer than that of the others. One of the possible reasons is that the ignition reaction of the IS coal occurs more slowly than the other coals due to the higher activation energy at the same conditions at which it was determined in a previous study [21].
Fig. 2 (b) illustrates the influence of oxygen concentration on the thermal behavior of the 5mm thick SA coal. The temperatures in the sample rise rapidly following ignition and large quantities of smoke are present, especially
at the higher concentrations of oxygen. Similarly, more visible glowing was found in 40 vol. % O2 in CO2.
Moreover, the results show that both the induction time to ignition and minimum ignition temperature decrease with increasing oxygen concentration, while the maximum temperature can be reached after ignition increases with oxygen concentration. 0 10 20 30 100 200 300 400 Tem perature, q C Time, min SA coal (a) Tp=245qC Tp=235qC Tp=240qC Tp=240qC 30 vol. % O2 in CO2 Tp=250qC Tp=245qC Tp=240qC P8 coal IS coal 0 10 20 0 100 200 300 400 Tp=265qC Tp=230qC Time, min Temper at ur e, q C 40 vol. % O2 in CO2 30 vol. % O2 in CO2 (b) Tmax=366qC Tmax=394qC Tp=455qC Tp=245qC SA coal air
Fig. 2. Thermal behaviour of the 5mm coal dust layer: (a) the subcritical and supercritical of three coal dust layers at 30 vol. % O2 in CO2; (b) the SA coal at various oxygen concentrations.
3.2.Dust Layer temperature evolutions: 12.5mm
Temperature evolutions at different heights in the 12.5mm dust layer are shown in Fig. 3. The subcritical and supercritical conditions were also determined at various oxygen concentrations. It shows that the maximum
temperature can be reached after ignition (Tmax) elevates with increasing ambient oxygen concentration. It is
heights for all the subcritical conditions (the dash lines in Figure 3). However, crossing points can be found for all the supercritical conditions (the solid lines in Figure 3), e.g., the temperature at the height of 10mm overtakes that of the 4mm and 7mm height in 12.5mm SA layer. Therefore, the crossing point might be also regarded as a criterion to judge if ignition will occur or not [11].
0 20 40 60 0 100 200 300 400 (a) Tmax=469qC Tp=215qC air Temper at ur e, q C Time, min 4mm, 215qC 7mm, 215qC 10mm, 215qC Tp=210qC 4mm, 210qC 7mm, 210qC 10mm, 210qC 0 10 20 30 40 0 100 200 300 400 (b) 21 vol. % O2 in CO2 Tmax=442qC Tp=215qC Tp=220qC Temper at ur e, q C Time, min 4mm, 220qC 7mm, 220qC 10mm, 220qC 4mm, 215qC 7mm, 215qC 10mm, 215qC 0 20 40 60 0 100 200 300 400 500 Tmax=540qC Tp=210qC Time, min Temper at ur e, q C 4mm, 210qC 7mm, 210qC 10mm, 210qC (c) 30 vol. % O2 in CO2 Tp=205qC 4mm, 205qC 7mm, 205qC 10mm, 205qC 0 20 40 60 0 100 200 300 400 500 600 Tp=200qC Time, min Temper at ur e, q C 4mm, 200qC 7mm, 200qC 10mm, 200qC (d) Tmax=655qC Tp=195qC 40 vol. % O2 in CO2 4mm, 195qC 7mm, 195qC 10mm, 195qC
Fig. 3.Temperature profiles of SA coal of thickness of 12.5mm: (a) air; (b) 21 vol. % O2 in CO2; (c) 30 vol. % O2 in CO2; (d) 40 vol. % O2 in CO2.
3.3.Influence of the combustion environment on the MLIT
The MLIT of three different coal samples with a height of 5mm and 12.5mm were determined at various oxygen concentrations. The results are plotted in Fig. 4 (a) and (b), respectively. As already illustrated by the temperature profiles, it is clear that oxygen concentration plays an important role in the self-heating or self-ignition process. The MLIT of the three coal samples decreases with increasing oxygen concentration, which agrees with the previous observation of the MCIT (minimum ignition temperature of dust cloud) at oxy-fuel atmospheres [22]. Specifically, the MLIT decreases dramatically when the oxygen concentration increases from 21 vol. % to 30 vol. % and then the MLIT goes down gradually with further increasing oxygen concentration as shown in Fig. 4 (a). In contrast, the influence of oxygen concentration is more moderate and the MLIT shows an approximate linear correlation with oxygen concentration from 21 vol. % to 40 vol. % as shown in Fig. 4 (b).
Table 3 lists the MLIT of South African coal at different thicknesses. This table shows that MLIT decreases dramatically from 5mm to 12.5mm thick rings, and then this trend continues on gradually. With an increased thickness in the dust layer, oxygen diffusion to the bottom of the layer becomes difficult, which is the reason why the maximum temperature of self-ignition occurred at the top surface where oxygen is easily available. At first, the thermal decomposition or oxidation reactions occur at the bottom of the layer and generate gas products such as carbon oxides and volatiles, which can slow down the oxygen diffusion from the top surface layer.
18 20 25 30 35 40 45 50 220 230 240 250 260 270 280 (a) 5mm MLI T , q C O2 concentration, vol. % Sebuku coal South African coalPittsburgh coal
Air 18 20 25 30 35 40 200 210 220 230 (b) 12.5mm MLI T , q C O2 concentration, vol. % Sebuku coal South African coal
Pittsburgh coal
Air
Fig. 4. The influence of oxygen concentration on the MLIT for 5mm (a) and 12.5mm (b) dust layers. Table 3. The MLIT of South African coal at different thicknesses.
Oxygen concentration the MLIT (°C) 5mm 12.5mm 15mm 20mm 30mm air 255-260 210-215 205-210 196-200 180-185 21 vol.% 260-265 215-220 208-213 197-201 - 30 vol.% 240-245 205-210 200-205 190-195 - 40 vol.% 230-235 198-200 190-195 185-188 170-173
4.Estimation of thermodynamic and kinetic parameters
4.1.Steady state energy conservation
With the assumption of negligible reactant depletion, a one dimensional steady state heat conduction equation for the dust layer can be written as [1, 12]:
2 b 2 exp( ) 0 T E k HA x U RT w ' w (1)
whereUbis the packing density (
-3
kg m ),
k
is the thermal conductivity of a dust layer (W m K -1 -1), and 'His theheat of reaction (J kg -1) which is assumed to equal the gross calorific value in this paper.
According to the experimental procedure, the dust layer equals the ambient room temperature at time t=0:
0
t
, T Ta (2) Boundary conditions of constant temperature at the bottom surface and convective and radiative cooling on the top surface are0 x , T Tp (3) x r, d ( s a) d T k h T T x (4) whereh hrhcis the total heat transfer coefficient (W m K -2 -1) accounting for the convective and radiative heat
temperature.
4.2.Estimation of thermal conductivity
Effective thermal conductivity plays an important role in the heat transfer in the dust layer. Therefore, some tests were carried out to estimate thermal conductivity using the method described by Park et al [12] and based on the assumption that heat generation can be neglected at low temperature. Then Equation (1) can be rewritten as
2 2 0 T x w w (5)
which implies a the linear temperature profile in the dust layer (d
d
T
x =constant). Rearranging equation (4) yields
a s a s s p 2 ( ) d ( ) d ( ) rh T T x k h T T T T T (6)
wheredx is the thickness of the dust layer (30mm). Tscan be obtained from the steady state experiment. hcan be
calculated by the following equations:
0.25 a a c 0.54R k h l (7) 2 2 s a s a ( )( ) r h HV T T T T (8)
wherelis characteristic length equal to the side of a square having the same area as the dust layer surface (l=0.09m
in this case), 3
a ( s a) / ( a)
R g TE T l vD , g is the gravitational constant, E 2 / (TsTa), vis the kinematic viscosity
of air, Dais thermal diffusivity of air,
k
ais the thermal conductivity of air,H
is the coal emissivity=0.9, andV
is the Stefan-Boltzmann constant (5.67×10-8W m K -2 -4).In order to evaluate the value of Ts, 4 thermocouples were used to measure temperatures at heights of 6, 12, 18
and 24mm in the 30mm dust layer exposed at a hot surface at 50°C. The temperature profiles of the locations are shown in Fig. 5 (a). After 5000s, the average temperatures at 0, 6, 12, 18 and 24mm in the South African coal dust layer were 49.6, 44.3, 39.8, 34.7 and 30.9°C, respectively. A linear extrapolation from the 5 temperatures yields the temperature of the top surface (25.9°C) of the dust layer as shown in Fig. 5 (b). Then the effective thermal
conductivity of the dust layer (0.1W m -1
K-1) can be obtained. Similarly, the thermal conductivity of IS coal andP8 coal are 0.11 and 0.1W m -1
K-1, respectively.4.3.Estimation of kinetic parameters
Previous work [21] found that to determine the kinetic parameters, the Frank-Kamenetzkii (F-K) method is more reliable when compared to other Arrhenius equation variations. Hence, the F-K method was used in this paper. The F-K parameterGcr, which is defined as [1]:
2 o a a c cr 2 c exp[ / ( )] r HE A E RT kRT
U
G
' (9)characteristic length of the dust sample (L/2, see Fig.1). 0 1000 2000 3000 4000 5000 6000 20 30 40 50 (a) Ta 24mm 18mm 12mm 6mm Tp South African coal
Temper at ur e, q C Time, s 0 10 20 30 20 30 40 50 (b) SA coal y=49.26-0.78x R-Square=0.99644 Tem perature, q C Distance, mm Experiment Linear approximation
Fig. 5. 30mm SA dust layer temperatures at different heights when exposed to a hot surface of 50°C: (a) temperature profiles; (b) equilibrium temperatures distribution and its linear trend line.
Rearranging equation (9) gives
2 cr c a a 2 o c ln( T ) ln( Q E A) E r k R RT G U (10)
Equation (10) also gives a linear correlation between the terms 2 2
cr c o
ln(G T /r )and 1 /Tcwith Ea/R as the slope,
which offers the possibility to determine the pre-exponential factor from the intercept of the linear correlation [1]. Fig. 6 shows the correlation between the characteristic lengths of the coal samples and the critical ignition temperature of both the upper and the lower limits using the F-K method and based on the results of the MLIT of Table 3. From Fig. 6, combined with Equation (10), the kinetic parameters of South African coal can be derived. The results are listed in Table 4. Clearly, the activation energy in air is similar with that in 21 vol. % O2 in CO2, but
smaller than those in 30 and 40 vol. % O2 in CO2 and the magnitude of the pre-exponential factor increases by a
factor of 2. Strangely both values of the kinetic parameters are the same on the whole between the 30 and 40 vol. % O2 in CO2. 1,8 1,9 2,0 2,1 2,2 20 21 22 23 24 y=52.24-14.44x 1000/Tc, Tc in K ln ( Gcr T 2 /rc 2 ), Gcr T 2 /rc 2 in k 2 /m 2 30 vol.% O2 in CO2 y=51.95-14.16x y=52.33-14.22x 40 vol.% O2 in CO2 y=52.87-14.38x y=48.24-12.67x air y=47.98-12.43x y=47.31-12.3x 21 vol.% O2 in CO2 y=46.83-11.9x
Table 4. The kinetic parameters of South African coal.
Oxygen
concentration E (
1
kJ mol ) A (s-1) lower upper mean lower upper mean Air 100.2 108.7 104.4 1.4e5 1e6 3.9e5 21 vol.% O2 in CO2 97.5 105.1 102.3 7.3e4 3.4e5 1.6e5 30 vol.% O2 in CO2 115.8 122 118.9 9.8e6 3.3e7 1.8e7 40 vol.% O2 in CO2 114.6 124 119.3 9.1e6 1.2e8 3.4e7
5.Conclusions
The experimental investigation of the minimum ignition temperature of dust layers has been performed by means
of aheated plate. The influence of oxygen concentration and dilution of air with CO2was studied. Several results of
the MLIT under various conditions arepresented to provide data and experimental basis for the assessment and prevention of coal dust fires, and explosion risks related to hot surfaces. The thermal and kinetic parameters have been estimated which can be used for further modelling work. The conclusions as follows:
(1) As the thickness of the dust layer increases, the critical temperature for ignition decreases significantly both in air and oxy-fuel combustion atmospheres.
(2) A remarkable increase in the spontaneous ignition risk of the coal dust layer has been found when increasing the ambient oxygen concentration. However, the effect of ambient oxygen concentration gradually lowers with increased thickness of the dust layer.
(3) The obvious variation in the values of the apparent activation energy and pre-exponential factor is observed when the combustion environment shifts from air to oxy-fuel atmospheres, which means that the reaction mechanism of self-heating or ignition more or less changed. Further investigation is necessary to elucidate this phenomenon.
Acknowledgements
The authors gratefully acknowledge financial support from the European FP7 project RELCOM (Reliable and Efficient Combustion of Oxygen/Coal/Recycled Flue Gas Mixtures).
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