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ReceiVed May 30, 2007. ReVised Manuscript ReceiVed December 25, 2007
In order to reduce overall fuel consumption, or partially substitute a “valuable” fuel with a poor one, in
electric power plant boilers, oxygen enrichment of combustion air can be very effective. Combustion
characteristics of three Chinese pulverized coals, Shenmu bituminous, Tianhushan anthracite, and Duolun lignite,
and three different particle sizes, under high oxygen concentrations more than 21%, have been investigated
using thermogravimetric/differential scanning calorimetry analysis (TG/DSC) and a drop-tube furnace. Results
showed that the ignitability, the combustion property, and the burnout were largely improved when added
oxygen was used, especially for small particles, the influence of oxygen on the bituminous coal was greater
than the lignite and the anthracite, and the suitable O2 concentration for the ignition of pulverized coal flow
should be controlled below 40%.
Table 2. Mean Weight Diameter and Specific Surface Area of runs.31,32 About 10 mg of each sample was heated at 10 °C min-1
Coal Samples from ambient temperature up to 1100 °C, with a flow rate of 100
coal sample THSH SM-1 SM-2 SM-3 DL mL min-1 for mixture of nitrogen and oxygen. Data on time,
residual weight, temperature close to the sample, rate of weight
mean weight diameter (µm) 96.18 71.30 60.68 53.38 181.14 loss or differential weight loss, and the nature and extent of
BET surface area (m2 g-1) 34.077 13.176 14.438 16.156 7.239
endothermic or exothermic reactions during thermochemical con-
version were recorded simultaneously to produce combustion
producing a higher temperature source in boilers to ignite profile. From the combustion profile, the following characteristic
subsequent pulverized coal flow. temperatures (Illustrated in Figure 4) were obtained:33,34 Ti, initial
temperature where the rate of weight loss accelerates due to the
A number of laboratory techniques have been used to onset of combustion (almost equivalent to the first DSC peak); Tp,
determine the ignition and flame stability of pulverized coal. peak temperature at maximum weight loss rate; Tb, burnout
Thermogravimetric/differential scanning calorimetry analysis temperature where DTG reaches a 1% combustion rate at the tail
(TGA/DSC) and a drop-tube furnace (DTF) were widely used end of the profile; Tcb, complete burnout temperature, the point
to investigate the reactivity of pulverized coal. In this paper, where the derivative of the DSC curve inflects to zero gradients.
the ignition of pulverized coal at high O2 concentrations It should be kept in mind that the Ti is not the ignition
temperature. Experimental factors such as the sample mass, the
(21-100% vol) was studied with a thermogravimetric analyzer particle-heating rate, and the condition of surrounding gases
to continuously measure the temperature of the coal during the influence the initial temperature. Therefore, the initial temperature
ignition and combustion, and a DTF was used to simultaneously is not a physical property of a fuel.35 Our aim was not to propose
measure the temperature and the content of the pulverized coal method for initial temperature evaluation. This study was based
flow. on comparison purpose, i.e., we kept the same burnoff procedure
to see the impact of high oxygen on the ignition and combustion
2. Experimental Setup characteristics of pulverized coal.
2.3. Drop-Tube Furnace Analysis. A DTF can simulate the
2.1. Samples. Three different rank coal samples were taken from combustion conditions in industrial pulverized coal combustion
Tianhushan (THSH) anthracite, Shenmu (SM) bituminous, and more closely than a thermogravimetric analyzer.36 A heating rate
Duolun (DL) lignite of China. Coals were first pulverized to the of 104-105 °C s-1 and maximum temperature of 1300 °C can be
needed particle size with a ball mill. The ultimate and proximate achieved in a DTF. In addition, the particles are in a dynamic, dilute
analyses of the three coals are given in Table 1. The mean weight phase. Fewer studies on ignition behavior and flame stability of
diameters of samples were measured by the sieving method and pulverized coal in DTF have been done than in TGA,34 especially
listed in Table 2. Three different size distribution samples were under high oxygen concentration.
prepared for SM coal. The measurement techniques available in DTFs for studying
The multimode scanning probe microscope was used here to particle combustion may be divided into “internal” and “external”
analyze the surface characteristics of pulverized coal. The amplifi- classes.14 The former one usually uses probes to take samples for
catory multiple is 500. Photos of the test samples are shown in analysis. Of the external methods, the optical technique is the most
powerful, which is usually nonperturbing and results can be obtained
Figures 1-3. From photos, we can see that the particle size of the
immediately in situ. The two methods above were accepted here.
THSH anthracite is the smallest, its configuration polyhedron is
First, at the sidewall of the DTF, 10 optical windows were designed
similar to a globe body, and, most DL lignite with the largest
to reveal the actual combustion flame situation. Second, the optical
diameters and smallest specific surface areas (SSA), present a kind window sections, fitted with an access port, allowed insertion of a
of spheroid shape. The configurations of SM bituminous present a sampling tube that can be easily changed for future experiments.
kind of atactic shape. Through the sampling tube, reaction products of different combus-
The SSA of the test samples are listed in Table 2. The samples tion stages can be elicited into the sampling probe. The solids were
were first heated and placed under vacuum to remove the moisture removed by filtration and the exhaust gases were analyzed for CO,
and other contaminants. Then when measured, the BET specific CO2, NOx, etc. with the help of an online analyzer (the GASMET
surface area demonstrated the order of PC based on SSA from the Fourier transform infrared gas analyzer, manufactured by Temet
minimum to maximum to be DL, SM, and THSH, which was Instruments in Finland). Meanwhile, a pump thermocouple is
different from the order by mean weight diameter of the test located in the sampling probe to measure the gas temperature.
samples. The reason is that distinct agglomerating phenomena
occurred between the particles of THSH pulverized coal, which
(31) Morgan, P. A.; Robertson, S. D.; John, F. U. Fuel 1986, 65, 1546–
can be observed by microscope. Many small particles tended to 1551.
swarm and be hard to separate by the sieving method, thus easily (32) Chen, Y.; Shigekatsu, M.; Pan, W. P. Thermochim. Acta 1996, 275,
building up in the feeding pipe of drop-tube furnace apparatus. Table 149–158.
2 also revealed that the SSA increased as the mean weight diameter (33) Pisupati, S. V.; Scaroni, A. W.; Stoessner, R. D. The Influence of
Weathering and Low-Temperature Oxidation on the Combustion Behaviour
decreased for the same kind of pulverized coal, because more and of Bituminous Coals. In 13th Annual Energy-Sources Technology Confer-
more small pores inside particles are exposed when the particle ence and Exhibition. Petroleum Division of ASME: New Orleans, 1990;
diameter is reduced. p 87.
2.2. Thermogravimetric (TG) Analysis. Temperature-pro- (34) Artos, V; Scaroni, A. W. TGA and drop-tube reactor studies of
grammed combustion tests were performed in a thermogravimetric the combustion of coal blends. Fuel 1993, 72 (7), 927–933.
(35) Perry, J. H. Chemical Engineers’ Handbook, 4th ed.; McGraw-
apparatus (Netzsch-STA 409C). In order to compare the samples, Hill: New York, 1963; Vol. 3–93.
factors such as sample mass, heating rate, and gas flow rate were (36) Su, J. H.; Pohl, D; Holcombe, J. A. Progr. Energy Combust. Sci.
well determined to ensure good repeatability between experimental 2001, 27, 75–98.
894 Energy & Fuels, Vol. 22, No. 2, 2008 Fan et al.
oxygen, 1.65% for 30% oxygen, 6.21% for 60% oxygen, and
6.88% for 100% oxygen, respectively. The higher the chemi-
sorbed O2, the greater the chemical reaction rate on the surface
of coal. Namely, higher oxygen concentrations can improve the
ignition characteristic of pulverized coal.
This phenomenon can also be observed in Figure 8 of DL
but is not obvious for THSH. From Figures 6-8, another
conclusion can be obtained: the hole structure of SM bituminous
coal is more helpful for oxygen adsorption than DL lignite and
THSH anthracite, since it holds the biggest chemisorptions heat
peak.
3.1.1. Ignition Mechanism. Extensive research on the mech-
anism of ignition of coal particles has classified the ignition Figure 9. Variation of characteristic temperature with O2 concentration.
into three types:2,3
(1) Homogeneous ignition or the ignition of the volatile matter
released from coal primary step was the initial ignition of volatile matter; following
(2) Heterogeneous ignition or the ignition of the coal particle this, the combustion of volatile matter, in a circumambient flame
surface like an oil drop, was presumed to prevent char reaction by screening
(3) Heterohomogeneous ignition, which results from simul- the solid from access by oxygen; secondary ignition, of char, then
taneous ignition of the volatile matter and the coal particle occurred as pyrolysis terminated.1
surface Obviously, one-step ignition, by direct attack of reactant gas
Distinctly, the three samples gave different combustion charac- on the whole coal, occurs in the THSH coal (Figure 6) for its
teristics. It may be observed that the DL coal (Figure 8) belonged very low concentration of volatile matter, which is true of
to homogeneous ignition1,23,32 that involved three stages. The heterogeneous ignition.1,23,32
896 Energy & Fuels, Vol. 22, No. 2, 2008 Fan et al.
Table 3. Downtrend of Ignition Temperature with Oxygen (2) As the O2 concentration increased, the characteristic
Concentrations temperatures decreased, but only the three curves of SM
O2 concentration range (vol %) bituminous gradually moved closer as O2 concentration in-
coal 21-30 30-40 40-60 60-80 creased. Namely, the influence of oxygen on the bituminous
drop in temperature coal was bigger than that on the lignite and the anthracite; the
DL lig ∆t (°C) 31 18 34 47 bituminous pulverized coal is the most suitable for the ignition
β (°C vol %-1) 3.44 1.8 1.7 2.35 system of oxygen enrichment.
SM-2 bit ∆t (°C) 131 102 51 140
β (°C vol %-1) 14.56 10.2 2.55 7.0 (3) DTF experiments indicated that the degressive rate of
ignition temperature was the largest in the range of 21-30%
O2 and the smallest in the range of 40-60%. Therefore, the
also be explained by the effect of mass concentrations of
suitable O2 concentration for the ignition of pulverized coal flow
pulverized coal or too much water content (Mar ) 34%) in DL
lignite. The evaporation of water would consume the large initial may be controlled below 40% O2.
combustion heat of the pulverized coal flow definitely, thus Since electrical utilities are highly required to reduce costs,
causing the ignition to delay and the ignition temperature to improve combustion behavior, control ash deposition, enhance
increase. Another conclusion can be made that the trend shown fuel flexibility, and extend the range of acceptable coals, ignition
by the three different size SM coals appears to be the same, and combustion technology in oxygen enrichment ambience for
and the ignition temperature decreased as the particle size pulverized coal would become possible in pulverized coal-fired
decreased. Furthermore, Figure 12 also revealed that as the power stations in the near future.
volume concentration of O2 exceeded 40%, the ignition tem-
perature of the tested SM pulverized coal flow decreased to 600 Abbreviations
°C, equivalent to the ignition temperature of the oil fuel.38 anthr ) anthracite
The β is defined as the rate of variation of ignition temperature bit ) bituminous
under every 1% oxygen concentration. Table 3 reveals that the DL ) Duolun
degressive rate of ignition temperature of bituminous coal is DSC ) differential scanning calorimetry
larger than that of lignite, that the degressive rate of ignition DTF ) drop-tube furnace
temperature is the largest in the range of 21–30% vol O2, and DTG ) derivative thermogravimetry; the rate of weight
it is the smallest in the range of 40–60% vol O2. When the O2 loss with time, as a function of temperature
concentration increased from 21 to 30%, the ignition temperature HFO ) heavy fuel oil
of SM-2 decreased by 131 °C, whereas the DL decreased by HFOF ) heavy fuel oil-fired
31 °C. Thus, O2 affects much more on bituminous than lignite, lig ) lignite
and the suitable O2 concentration for the ignition of pulverized PC ) pulverized coal
coal flow may be controlled below 40% vol O2. OPCF ) oxy-enriched pulverized coal-fired
SM ) Shenmu
4. Conclusion SSA ) specific surface area
TGA ) thermogravimetric analysis
To sum up the above discussions, we can obtain the following THSH ) Tianhushan
conclusions: Ti ) initial temperature
(1) The ignitability, combustion property, and burnout have Tp ) peak temperature at maximum weight loss rate
all been greatly improved when enrichment oxygen was added, Tb ) burnout temperature
especially for small particles. The ignition mechanism did not Tcb ) completely burnout temperature
change under the higher O2 concentrations, even under the pure Tb ) temperature of the furnace wall
O2 circumstance at the lower heating rate. Ty ) temperature of the flue gas
(38) Cao, Y. Q. Energy Eng. 2000, 5, 60–62. EF7006497