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Proceedings of the Combustion Institute 31 (2007) 19051912

Combustion Institute
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Ignition and devolatilization of pulverized bituminous coal particles during oxygen/carbon dioxide coal combustion
Alejandro Molina *, Christopher R. Shaddix
Hydrogen and Combustion Technologies, Combustion Research Facility, Sandia National Laboratories, Livermore, CA 94550, USA

Abstract Oxygen/carbon dioxide recycle coal combustion is actively being investigated because of its potential to facilitate CO2 sequestration and to achieve emission reductions. In the work reported here, the eect of enhanced oxygen levels and CO2 bath gas is independently analyzed for their inuence on single-particle pulverized coal ignition of a U.S. eastern bituminous coal. The experiments show that the presence of CO2 and a lower O2 concentration increase the ignition delay time but have no measurable eect on the time required to complete volatile combustion, once initiated. For the ignition process observed in the experiments, the CO2 results are explained by its higher molar specic heat and the O2 results are explained by the eect of O2 concentration on the local mixture reactivity. Particle ignition and devolatilization properties in a mixture of 30% O2 in CO2 are very similar to those in air. 2006 Published by Elsevier Inc. on behalf of The Combustion Institute.
Keywords: Coal; Ignition; Devolatilization; Enhanced oxygen; CO2 recycle

1. Introduction The reduction of pollutant emissions and the potential for lower-cost CO2 separation have prompted the study of oxygen/carbon dioxide recycle (O2/CO2) ring for existing pulverized coal (pc) systems. As opposed to new, compact boiler units that may be designed for the use of strongly oxygen-enriched oxidizer mixtures; the retrot of existing air-based pc boilers to O2-ring is limited by the maximum temperature that the burners and boiler can tolerate. For temperature control

* Corresponding author. Present address: School of Process and Engineering, Faculty of Mines, National University of Colombia, Medelln. Fax: +57 42341002. E-mail address: amolinao@unal.edu.co (A. Molina).

and to maintain the necessary convective heat transfer to steam tubes, O2-ring in existing boilers requires the recycling of substantial quantities of CO2 into the boiler. Recent reviews [1,2] agree that O2/CO2 pc combustion is economically promising and technically feasible with current technologies, decreasing the risk associated with the development of new technologies. However, successful implementation of the O2/CO2 technology in conventional pc boilers depends on fully understanding the dierences that result from replacing N2 with CO2 in the oxidizer stream. Previous results have shown that the application of O2/CO2 combustion can cause dierences in furnace operation parameters such as burner stability, char burnout, heat transfer and gas temperature proles [37]. For example, a pilot-scale furnace test with a low-NOx burner showed that

1540-7489/$ - see front matter 2006 Published by Elsevier Inc. on behalf of The Combustion Institute. doi:10.1016/j.proci.2006.08.102

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the burner needs to be operated with a greater oxygenfuel stoichiometry to produce a stable ame when red with an O2/CO2 mixture [5]. Part of the diculty of burner operation on O2/CO2 mixtures originates from the lower ame temperatures associated with CO2 use because of its higher heat capacity. This diculty can generally be overcome by increasing the oxygen concentration of the oxidizer to values varying from 30 to 32% that give comparable ame temperatures to pc combustion in air [1,2,6]. Nevertheless, some studies have found that coal ignition is retarded in an enhanced CO2 environment, even for a comparable gas temperature prole. Liu et al. [7] reported increased coal ignition delay in pilot-scale tests of O2/CO2 coal combustion. Kiga et al. [3] performed microgravity measurements of the combustion of coal clouds in 40% O2 with N2, CO2 and Ar as balance gas and found that the ame speed increased in the order Ar > N2 > CO2. A number of studies have been previously conducted on coal particle ignition [813]. Most studies have focused on ignition of particles considerably larger than those associated with pc-ring (typically <150 lm). This does not come as a surprise, given the diculties in accurately measuring the fast ignition of pc particles ($10 ms) in hightemperature, oxidizing environments. Information on the eect of elevated levels of CO2 on the ignition of coal particles is important both for understanding how to switch existing burners from operation on air to operation on O2/CO2 mixtures, and for computational uid dynamic (CFD) modeling of the performance of pc burners in O2/CO2 systems. To examine these issues, we have studied the eects that the presence of CO2 and enhanced O2 levels have on the ignition of pulverized coal in a laminar ow reactor. The experimental technique used also yielded measurements of the total devolatilization time in CO2 and N2 gas combustion atmospheres. 2. Experimental 2.1. Gas composition and temperature Experiments were carried out in the laminar, optical entrained-ow reactor at Sandia National Laboratories [14,15]. Figure 1 shows a schematic of the facility. The reactor operates at 1 atm and uses a non-premixed-amelet Hencken burner to provide a high-velocity ow of combustion product gases. Solid fuel particles are injected at the furnace centerline through a 0.75 mm stainlesssteel tube. A 5 cm 5 cm quartz chimney isolates the reacting particles and burner products from the surrounding air and allows optical measurements on the particles injected into the ow. The eect of the presence of CO2 on coal ignition was evaluated by entraining coal into mix-

Fig. 1. Entrained-ow reactor and associated optical diagnostics.

Table 1 Calculated composition of combustion products (mol %) N2 _21 CO2 H2O N2 O2 1.65 12.27 65.08 21.00 N2 _30 1.65 12.34 56.00 30.00 CO2 _21 65.31 13.69 0.00 21.00 CO2 _30 57.02 12.98 0.00 30.00

tures with N2 or CO2 as balance gas at two dierent oxygen concentrations (21 and 30%). Table 1 shows the composition of the four gas mixtures studied. The dierent gas compositions were obtained by burning mixtures of C2H4, H2, O2 and CO2/N2 in the at ame. The total ow of products was 65.0 standard (298 K, 101,325 Pa) liters per minute (slpm). The gas used for entraining the particles at the centerline was the same as the balance gas and had a ow of 0.03 slpm. The particle feeding rate was kept low ($0.02 g/min) to guarantee that the gas temperature and velocity proles were not aected by particle combustion and the particles ignited and burned as isolated particles. The gas temperature prole along the reactor centerline was measured with a 76-lm, type R thermocouple and corrected for radiative losses [16]. The gas temperature was the same for the four cases, within the uncertainty of the measurements (Fig. 2). The higher uncertainty in the gas temperature measurements at low heights (see inset in Fig. 2) occurs because of the relatively high radial temperature gradient near the centerline resulting from the mixture of the particle feed gas and the hot burner products. 2.2. Particle imaging The rst 10 cm of the reactor were imaged with a charged-coupled device (CCD) camera. In some experiments an interference lter centered at 431 nm (10 nm FWHM) was used to collect chemiluminescent time-averaged CH* emission. The exposure times were 1 and 0.08 s with and without the lter, respectively. The dierent exposure times were designed to maximize the signal,

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1300 1250 1200 1150 1100 T (K) 1050 1000 950 900 850 800 0 2 4 6 8 h (cm)
Fig. 2. Measured centerline gas temperature proles in the entrained ow reactor. Triangles, N2; circles, CO2. Open symbols, 21% O2; closed symbols, 30% O2. Expanded gure shows detail of rst 5 cm.

1300 1200 T (K) 1100 1000 900 800 0 1 2 3 h (cm) 4 5

10

12

14

16

18

without saturation. CH* chemiluminescent imaging was attempted for single entrained particles, but was found to be too weak to be detected. Similarly, an intensied CCD camera and a 431nm lter were used in conjunction with a bellows to provide high magnication images of individual reacting particles, but CH* chemiluminescence was too weak to be detected. The use of CH* chemiluminescence as a tool for the detection of ame sheet and ignition regions has been previously described [17]. 2.3. Fuel Pittsburgh seam high-volatile bituminous coal was used in the experiments. The proximate analysis showed 0.8%w moisture, 8.8%w ash, 34.9%w
2.60 2.40 2.20 combustion products

volatiles and 55.6%w xed carbon. The coal was sieved to a 106125 lm size fraction. 2.4. Gas and particle velocity The velocity of the entrained particles was measured with the optical diagnostic system described in Ref. [14]. Figure 3 shows the measured velocity prole. As the entraining gas mixes with the combustion products, the centerline velocity increases and the furnace ow develops from the at prole at the reactor exit to a characteristic parabolic prole of laminar pipe ow, increasing the centerline velocity. 3. Results Figure 4 shows examples of time-averaged images obtained for coal and char igniting in 21% O2 in N2. Comparable images were observed for the other cases. In Fig. 4a, after a certain distance, coal particles ignite, typically producing a non-premixed ame of volatile gases that surrounds the particle (producing bright soot emission). After devolatilization ends, the ignited char particles appear as low-intensity traces that extend upward with the gas ow. This description for the initial stages of the oxidation of a bituminous coal particle agrees with that of McLean et al. [18] for coal from the same seam and similar experimental conditions. McLean et al. found that the observation of condensed matter surrounding the coal particle coincided with ignition, suggesting that homogeneous ignition of volatiles occurs before any signicant phase of heterogeneous

v (m/s)

2.00 1.80 1.60 1.40 1.20 1.00 0

entraining flow 2 4 6 h (cm) 8 10 12

Fig. 3. Particle velocity prole along the reactor. The solid line shows a polynomial t of the optical measurements (points). The horizontal lines indicate the calculated initial velocities of the cold (298 K) particle feed gas and the hot combustion products.

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Fig. 4. Example of images obtained for coal particle ignition in 21% O2 in N2. The luminosity at the bottom corresponds to the burner face. The height from the burner to the top of the image is 10 cm.

ignition of the char. Figure 4b shows images through the 431 nm lter. The devolatilization zone appears as a region of chemiluminescent CH* emission. To get statistical information on the dierences in ignition and devolatilization for the dierent cases, 250 images of blackbody emission (i.e., lterless imaging) and 100 images of CH* chemiluminescence were analyzed. To perform a consistent and statistically meaningful analysis of the signal strengths with height above the burner, an average was calculated of the central 40 pixels in each row for each image. Figure 5a presents examples of blackbody emission, where each axial prole corresponds to the results from one image. A region of higher intensity that corresponds to soot emission during volatiles oxidation can be readily distinguished from the succeeding low-intensity char oxidation zone. Figure 5b shows proles for CH* chemiluminescence. Although the CH* signal is lower than the blackbody emission, the CH* axial intensity proles show less variation than the blackbody proles, probably because of

the longer exposure time (and therefore more extensive particle averaging) for the CH* measurements. The onset of CH* emission occurs closer to the burner than that for blackbody emission, as expected considering the nite inception time for soot following ignition of the volatiles cloud. Negligible blackbody emission penetration through the 431 nm lter was veried at temperatures up to 1200 K by imaging a 76-lm thermocouple placed inside the reactor using the same camera settings as for the CH* measurements. Analysis of the image intensity through the CH* lter in the char combustion region suggests that a minor amount of blackbody emission (from higher temperature soot and char) may contribute to some of the CH* images. The CH* chemiluminescence signals should provide a superior indicator for the onset of coal ignition than blackbody emission (from soot or hot char), as explained above. Figure 6 shows the axial prole for the central rows superimposed on a typical CH* chemiluminescence image. The burner emission signal is used to set the time of

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10

distance from burner (cm)

b
intensity (a.u.)

0.1

10

distance from burner (cm)

Fig. 5. Centerline proles for coal particle ignition in 21% O2 in N2. (a) Blackbody emission, (b) CH* emission.

particle injection. Ignition, dened as the onset of the CH* signal, occurs around pixel # 560. The CH* chemiluminescence can be represented as a second-order polynomial (thick line) centered at the maximum peak intensity. Although use of higher-order polynomials gave a more exact representation of the CH* prole, a second-order polynomial captured the sharp intensity rise as the particle ignited and was less sensitive to the less-uniform CH* emission toward the end of devolatilization (see Fig. 6). From the intersection of the second-order polynomial with the baseline, the onset of ignition (assumed to correspond to the onset of devolatilization) and the end of volatiles oxidation can be estimated. The pixel count and the particle velocity can be used to estimate the particle ignition time, si, and the particle devolatilization time, svol. Analysis of 100 images such as the one in Fig. 6 for the four cases in Table 1 gives estimates of si and svol, which are presented in Fig. 7. The results do not show any statistically signicant dierence in svol for the four cases analyzed. However, for both the CO2 and N2 atmospheres, ignition occurs faster for the higher oxygen concentration (30%). For the same oxygen concentration, ignition takes longer in the presence of CO2. Although the dierences are minor, Fig. 7 gives evidence of the importance that the presence of CO2 can have on particle ignition. It is important to note that dierences in the adiabatic ame temperature between CO2 and N2 atmospheres cannot explain the trend observed in Fig. 7 for a constant O2 concentration. Figure 2 shows that in the controlled conditions of this experiment, the gas temperature prole was the same for different gas mixtures. The dierences in ignition, therefore, are not caused by variations in gas temperature.

intensity (a.u.)

35 30 25 time (ms) 20 15 10 5 0 N2_21 N2_30 CO2_21 CO2_30

Fig. 6. Example of intensity analysis of the chemiluminescence during coal particle ignition. The gure shows the second-order polynomial t of the peak and the derived si and svol values superimposed on the analyzed image.

Fig. 7. Estimated values of si (circles) and svol (squares) using CH* lter and CCD camera. Vertical bars represent 98% condence statistical error.

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4. Discussion To explain the observed variation in coal ignition and devolatilization with gas composition it is important to distinguish the dierent phenomena that occur after coal injection into the ow reactor. The rst phenomenon is particle heat up from ambient temperature to a gas temperature at which volatiles begin to be released. For the case of a non-reactive particle, this process can be described by the following equation: i dT p 3 h erT 4 T 4 hT p T g ; 1 p w C p qp rp dt where Tp, Tw, and Tg are the particle, wall, and gas temperatures, respectively. Cp, qp, rp, and e are the particle heat capacity, density, radius and emissivity, respectively; r is the Stefan Boltzmann constant and h is the coecient for convection heat transfer. The contribution of gas-to-particle radiant transport (originating from hot CO2 and H2O) is neglected, as the small dimensions of our reactor make this a small factor. In Eq. (1), the only parameters that depend on the gas properties are Tg and h. Because Tg was kept constant for the dierent gas compositions, the only possible eect of the dierent gas mixtures on initial particle heating resides in the coecient for convection heat transfer, h. For the present experimental conditions with low particle slip velocity, h can be calculated assuming a Nusselt number (Nu = hDk1) of 2 [19], where D is the particle diameter and k the gas thermal conductivity. Hence, the only gas property that aects the initial particle heat up is the thermal conductivity. Figure 8 compares the ratios of several thermophysical properties and some non-dimensional groups for N2 and CO2, as calculated for a temperature of 1200 K using CHEMKIN [20]. Figure 8 shows that the ratio of thermal conductivities for CO2 and N2 is close to one. In fact, when Eq. (1) is applied for the dierent gas compositions in Table 1 and integrated over the gas temperature proles in Fig. 2, there are negligible

Fig. 8. Comparison of the ratio of dierent thermophysical properties and non-dimensional groups for CO2 and N2 at 1200 K.

dierences in the temperature rise of an inert particle. Following initial particle heat up, two processes can occur, the onset of heterogeneous ignition of the coal particle or the release and ignition of volatiles [8,11,21]. In some cases, initial heterogeneous ignition may be quenched by the eruption of volatiles [8]. In our experiments, there is no discernible heterogeneous ignition stage prior to devolatilization and ignition of the volatiles, so the governing ignition process is homogeneous ignition of the volatiles cloud, consistent with the image analysis of McLean et al. [18]. Therefore, the relevant process following particle heat up is that of volatiles release. Coal devolatilization is an endothermic process whose rate is strongly dependent on particle temperature and particle heating rate. If, as was discussed earlier, the particles have similar heating proles before the onset of devolatilization for the dierent gas mixtures, one can expect a similar onset time for coal devolatilization. Once coal devolatilization begins, the light hydrocarbons and tar material released during devolatilization ignite when they come into contact with hot oxidizer gases. The process of homogeneous gas-phase ignition is dependent on the transport properties of the surrounding gas and on the combustion heat release and reactivity of the local fueloxidizer mixture. For coal particles introduced into a hot atmosphere, ignition presumably occurs in a localized region where the combination of gas temperature, oxygen concentration, and volatile concentration rst undergoes autoignition. In this situation the oxidizing gas is at a higher temperature than the coal volatiles, so ignition will occur at a leaner mixture than would occur for isothermal mixtures [22]. In general, ignition time decreases as the mixture reactivity and heat release increase and increases as the product of heat capacity and density (qCp) increasesqCp gives a measure of the thermal sink for any heat that is chemically released. Figure 8 shows that the density and (molar) heat capacity of CO2 are signicantly higher than those for N2 (the heat capacity on a mass basis is only 7% higher). Therefore, it can be expected that the volatiles released into an N2 atmosphere will ignite more quickly than those released into a CO2 environment. A higher O2 concentration decreases si by increasing the characteristic reaction rate of the local mixture (the product of qCp for O2 has a value similar to that of N2). Once the volatiles cloud is ignited, a nonpremixed ame provides additional heating of the particle and consumes the evolved volatiles. In quasi-steady droplet combustion theory [23], the mass consumption rate is expressed as m = (4prs) qsD ln (1 + B) where rs is the droplet diameter, qs is the fuel vapor density at the particle surface, D the fuel mass

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diusivity and the Spalding transfer number, B, is given by B = Cp (T1 Ts) + (Yo,1/OF)hc/hv where T1 is the bulk gas temperature, Ts the particle surface temperature, Yo,1 is the mass fraction of oxygen in the bulk gas, OF is the stoichiometric mass oxygenfuel ratio, hc is the heat of combustion of the fuel vapor, hv is the heat of vaporization (or devolatilization, in the case of coal) of the drop, and the relevant Cp here is that of the volatilized fuel, Therefore, the use of CO2 in place of N2 only inuences the consumption rate of the volatiles through its impact on the fuel vapor diusivity. Figure 8 shows that the diusivity of CH4 (used to represent the volatiles) in CO2 is 20% lower than in N2, so that the volatile consumption rate in the CO2 environment is expected to be slightly slower. Similarly, the volatiles should be consumed more rapidly for higher oxygen content in the oxidizer. However, the results from Fig. 7 show that the eect of the gas environment on the consumption rate of volatiles is negligible, under the conditions investigated here. Our results have signicance for coal combustion in utility boilers because they show that differences in coal ignition and in the time required for volatile oxidation during O2/CO2 pc coal combustion are not only aected by the lower adiabatic ame temperature when CO2 is present in the system, but also by the high specic heat and the lower mass diusivities of the CO2 mixtures. As it turns out, by increasing the oxygen concentration to 30% (at which point the ame temperatures are similar), pc combustion in the presence of CO2 can achieve similar ignition and devolatilization properties as for traditional coal/air combustion. 5. Conclusions Experiments in a combustion-driven laminar ow reactor show that the presence of CO2 retards coal particle ignition but has no measurable eect on the duration of volatile combustion. Increasing oxygen concentration accelerates particle ignition for both N2 and CO2 atmospheres. Although the changes in particle ignition time are minor, they illustrate the importance of the dierent thermophysical properties of gas mixtures during O2/ CO2 pc coal. For homogeneous ignition, such as observed in the experiments, the eect of CO2 can be explained by its higher specic molar heat and the eect of O2 can be explained by its eect on mixture reactivity. The results in this paper suggest that an increased oxygen concentration for CO2 recycle combustion, if correctly selected, should produce ignition times and volatile ames similar to those obtained under coal/air combustion.

Acknowledgments This research was sponsored by the U.S. Department of Energy through the National Energy Technology Laboratorys Power Systems Advanced Research Program, managed by Dr. Robert Romanosky. Susan Maley serves as the NETL technical monitor for this project. Sandia is a multi-program laboratory operated by Sandia Corporation, a Lockheed Martin Company, for DOEs National Nuclear Security Administration under Contract DE-AC0494AL85000.

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Comment
Jerry Lee, UTRC/UTC, USA. Can you rule out the eects of CO2 on the heterogeneous kinetics on the particle surface? Using the Nagle-stoichiometric-combustion rate expression O2 attacks on carbon surface produces CO + CO2. The ratio of CO/CO2 produced by the heterogeneous mixtures can be shifted due to the higher CO2 in your system. The spectral interaction of CO2 with the particle (especially in the infrared range) is very dierent from that of air. Can you assess its role? Reply. Concerning the rst question, it is true that the presence of a high concentration of CO2 may aect the heterogeneous kinetics of char oxidation and the CO/CO2 ratio of the oxidation products. However, for the conditions investigated here, the predominant coal ignition process was homogeneous in nature, for both N2 and CO2 diluents. Therefore, any eect of the CO2 on the heterogeneous kinetics did not inuence the ignition delay and is unlikely to have aected the devolatilization time observed in the experiments. Our analysis suggests that the dierences in ignition delay in high CO2 environments may be entirely attributed to the high heat capacity of CO2. Concerning the second question, the use of elevated CO2 environments clearly aects the radiant heat transfer in large-scale combustors and furnaces, including the radiant heat transfer incident.

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