www.ingentaselect.com=titles=02638762.

htm

02638762/03/$23.50+0.00 # Institution of Chemical Engineers Trans IChemE, Vol 81, Part A, October 2003

SIMULATION OF COAL COMBUSTION IN A BUBBLING FLUIDIZED BED BY DISTINCT ELEMENT METHOD

H. ZHOU1 , G. FLAMANT1 , D. GAUTHIER1 and Y. FLITRIS2
1

Institut de Science et de Genie des Materiaux et Procedes, CNRS-IMP Odeillo-Font-Romeu, France , 2 University of Thessaly, Volos, Greece

he distinct element method (DEM) is used to model combustion of coal particles in a bubbling uidized bed. The gas phase is modeled as a continuum and the particle phase is modeled by DEM. The chemical reactions consist of the heterogeneous reactions of char with O2, CO, CO2, NO and N2O and in the homogeneous reactions involving CO, O2, NO and N2O. The colliding particleparticle heat transfer is based on the analysis of the elastic deformation of the spheres during their contact. The model predicts the particle heterogeneous ow structure, the thermal characteristics of burning coal particles, and the gaseous emissions from a uidized binary mixture. Results show that the instantaneous contribution of the collision heat transfer ranges from 0 to about 1.0% of the total heat transfer during the coal combustion. The mean excess of coal temperature is approximately 140K, and the maximum excess of coal particle temperature is approximately 270 K after 2 s. Keywords: uidized bed; coal combustion; distinct element method; large eddy simulation.

INTRODUCTION Coal combustion in a uidized bed is one of the main research topics in the eld of solid fuel treatment since the combustion itself and the resulting gaseous emissions are in uenced by the fuel properties, but also by the gas particle hydrodynamics and the bed temperature. Models proposed in the literature to predict the performance of a uidized bed coal combustors have been extensively reviewed (Adanez and Abanades, 1992). Most of them are based on the two-phase theory of uidization, which views the uidized bed as consisting of a bubble phase and an emulsion phase. However, two-phase models are unable to predict the gas back mixing and the recycle peak in solids mixing. Models of computational uid dynamics of uidized bed coal combustion are rather scarce due to the complex mathematical modeling and to the unsteady character of the numerous equations (Peirano and Lekner, 1998; Rong and Horio, 1999; Lathouwers and Bellan, 2001). The distinct element method (DEM) model has been used to simulate gasparticle uidization since the 1990s, and phenomena such as bubbling, slugging and particle transport within the bed can be simulated (Tsuji et al., 1993; Hoomans et al., 1996; Zhou et al., 2002). The DEM model describes accurately not only the particle motion (particle rotation, collision with other particles, etc.) but also the chemical reactions, heat and mass transfer etc. at the individual particle level. This paper presents the DEM model that was developed for analysing the thermal characteristics of burning coal particles and the gaseous emissions from a uidized mixture of sand and coal.

THEORY The gasparticle hydrodynamics model is based on the following assumptions: (1) the uidized bed is twodimensional; both front and back walls are frictionless; (2) gas motion due to the convective interfacial transfer uxes of mass and momentum between the particle and the gas are negligible in front of the total uidizing gas ow rate (Lathouwers and Bellan, 2001); (3) the particle is isothermal; and (4) all reactions are rst order reactions. Gas Phase Hydrodynamics Filtering the two-phase NavierStokes equations of continuity and momentum conservations in a two-dimensional uidized bed derives the large eddy simulation equations for the gas ow: ~ @(erf ) @(erf uf ,i ) 0 @t @xi ~ ~ ~ @(erf uf ,i) @(er f uf ,i uf ,j ) @t @xj ~ t @(esij ) @(e~ ij ) e@~ p @xi @xj @xj (1)

erf g C

(2)

where the overbar denotes the application of the ltering operation, e is the porosity, rf is the gas density (kg m3 ), uf is the gas velocity (m s1 ), i, j 1, 2, and represent the x and y directions, p is the gas pressure (Pa), g is the gravitational acceleration vector (m s2 ), t is the time (s), C is the ~ volumetric particlegas interaction (N m3 ). tij is the sub ~ ~ ~ grid scale (SGS) stress, sij rf nf (Sf,ij 2=3Sf ,kk dij ), and

1144

SIMULATION OF COAL COMBUSTION ~ Sf ,ij @~ f ,i =@xj @uf ,j =@xi is the resolvable strain tensor. tij is u ~ ~ ~ ~ ~ ~ modeled as: tij rf nt (Sf,ij 2=3Sf,kk dij ) 2=3rf ks dij (Koutmos, 2000). nf mf =rf is the gas kinematic viscosity (m2 s1 ), mf is the gas viscosity (Pa s), vt is the SGS gas kinetic viscosity (m2 s), dij is the Kronecker delta, ~ and ks is the SGS kinetic energy (m2 s2 ). The SGS kinetic energy is obtained from equation (2). Terms higher than the third order for the SGS and pressure correlation terms are neglected. Therefore, the SGS kinetic energy equation can be obtained as: ~ ~ ~ ~ @(erf ks ) @(erf uf ,j ks ) @{erf (nf nt =Pr)@ks =@xj } @t @xj @xj 3=2 ~ er C ks 1 f e ~ ij Sij ) ~ D 2erf nt (S
0:687 3pdp mf (1 0:15Rep ) n~ nt @ n 2 ks (~ f,j vp, j ) u (aTL 1) Sc @xj

1145

where vp is the particle velocity (m s1 ), F is the sum of forces acting on the particle (N) (F Fc Ff ), Fc is the particleparticle interaction force (N), o is the angular velocity (s1 ), T is the net torque caused by the contact force (N m), I is the moment of inertia of the particle (kg m2 ), and mp is the particle mass (kg). GasParticle Interaction Force The source term C is composed of two parts, the mean velocity generation term Fm and the turbulence generation term Ft . Fm and Ft are: ~ Fm
n X F ~f ~ Ff ~ and Ft V v u ~rel n0 (~ 0f v0p ) i1 grid

(8)

(3)

where n0 is the particle number uctuating concentration (m3 ), v0p is the particle uctuating velocity (m s1 ), u0f is the gas uctuating velocity (m s1 ), vrel is the relative gas particle velocity (m s1 ), and Vgrid is the computational cell volume (m3 ). Heat and Mass Transfer The colliding particleparticle heat transfer is modeled according to the heat conduction analysis developed for impinging particle by Sun and Chen (1988). In this model, the collision heat transfer is based on the analysis of the elastic deformation of the spheres during their contact. The rate of change of the particle internal energy is due to the heat exchange with the surrounding gas resulting from convection, Qc (J s1 ), to the thermal radiation, Qr (J s1 ), to the heat of combustion, Qcomb (J s1 ), and to the energy exchanged during the collision, Qcoll (J s1 ): dTp Qcomb Qc Qr Qcoll (9) dt where Cp is the heat capacity at constant pressure (J kg1 K 1 ). For sand particle, Qcomb 0. mp Cp Coal Pyrolysis, Combustion and Other Reactions The coal pyrolysis model of Donskoi and McElwain (1999) is used. This model predicts the evolution of different species from coal during its thermal decomposition. The shrinking core model is adopted to describe the evolution of coal particles during combustion. Both the homogeneous and heterogeneous reactions are summarized in Table 1. Energy Balance for Gas Species in a Cell The energy balance is written as the following equation: ~ @(erf Cf Tf ) @(erf Cf uf ,i Tf ) @t @xi @{e(lf rf nt =Pr) @Tf =@xi } @xi q

The turbulent viscosity is evaluated from the SGS kinetic energy as (Koutmos, 2000): q ~ nt Ck Lt ks (4)

where the overbar denotes the mean value in a computational = cell, D is the characteristic length (m), D (Dx Dy)1 2 , Dx and Dy are the mesh spacing in x and y directions (m), Lt is the turbulent length scale (m) (Lt D), Ck and Ce are empirically assigned constants, Ck 0:1 and Ce 0:5 (Yuu et al., 2001). Pr is the turbulent Prandtl number, Pr 1:0, Sc is the turbulent Schmidt number, Sc 0.7, a is the inverse of the particle relaxation time (s 1 ), 36mf a 2 (1 0:15Re0:6807) (2r r )d
p f p p

TL is theptime scale of average sub grid scale vortices ~ 1= TL D= 2ks 2 ), and n, dp , rp and Rep are the mean particle concentration(m3 ), the mean particle diameter (m), the mean particle density (kg m3 ), and the mean particle Reynolds number in the computational cell, respectively. Particle Phase Hydrodynamics Cundall and Strack (1979) opened up new possibilities of using DEM to calculate dense phase ows such as uidized beds. In the DEM model, particleparticle contact forces are described in terms of a mechanical model involving a spring, a dashpot and friction. The drag force on a suspended particle is given by: 1 2 ~ Ff pdp Cd enp 2 rf j~ f ~p j(~ f ~p ) u n u n (5) 8 where np is the porosity factor (np 4:7) and Cd is the drag coef cient. Equations of translation and rotation particle motions are: ~ n Vp d~p F g ~ mp mp H~ p dt ~ ~ do T I dt (6) (7)

(10)

where q is the heat source in a unit volume [J (m2 s)1 ]. The heat source consists of the heat transfer between the particle and the gas, plus the heat release of burning CO. Cf is the heat capacity of gas [J (kg K)1 ] and Tf is the local gas temperature (K).

Trans IChemE, Vol 81, Part A, October 2003

1146

ZHOU et al.
Table 1. Reactions included in the model (Chen et al., 2001; Chan et al., 1983; De Soete et al., 1999; Hobbs et al., 1992).

Reaction 2 kA a1 2a 2 C O2 ! CO CO , a2 a2 a2 2 where: a 750exp(7200=Tp ) b 1 kB (char) O2 bNO C O ! 2

kC (char)

Reaction rate (mol m3 s1) RA kA CO2

Kinetic constant (s1) kA KOXDN Tp exp(21578=Tp ) fp KOXDN 35 kB 2(a 1) bkA , b 1 a2

Heat release (J mol1) 4:04 105 [2a=(a 2)] Negligible Negligible Negligible Negligible Negligible Negligible Negligible 2:82 105

C N

RB kB CO2 RC kC CNO RD kD CNO RE kE CNO RF kF CN2 O RG kG CN2 O RH kH CN2 O RI kI CCO

C N NO N2 O C !
kD (char) 1 NO C ! N2 CO 2 k E (char) 1 NO CO ! N2 CO2 2

kC bk0 fp exp(9000=Tp ), k0 3:0 ( 0:159fp exp(6255=Tp ) Tp 973 K kD 555:6fp exp(14193=Tp ) Tp > 973 K kE 5:67 103 Tf exp(13952=Tf )p kF 13:36fp exp(16677=Tp ) kG 1:75 108 exp(23800=Tf ) kH 2:51 108 exp(23180=Tf )CCO,avre
0:5 kI 1:254 1010 F(CO2 =2)0:25 CH2 O exp(20130=Tf ) F 7:93exp(2:48CCO =CO2 )

N2 O C N2 CO ! 1 N2 O N2 O2 ! 2
kG

kF

N2 O CO N2 CO2 !
kI 1 CO O2 CO2 ! 2

kH (char)

Mass Balance for Gas Species in a Cell The mass balance for the gas species i (where i represents CO2, CO, N2O, NO, H2O and O2) is derived as: ~ ~ ~ ~ @(erf Yi ) @(erf uf j Yi ) @{erf (Di nt =s) @Yi =@xj } @t @xj @xj Gi

(11)

where Yi is the local mass fraction of species, and Di is the molecular diffusion coef cient (m 2 s1 ); i 16 corresponds to the gas species in the transport gas. The last term on the right of equation (11) is the average mass source arising from reaction. The thermophysical properties of air, sand and coal can be seen in Flamant et al. (1993), and the calculation of the molecular diffusion coef cients Di is in Canu (2001) and Massman (1998). COMPUTATION CONDITIONS The well-known semi-implicit method for pressure-linked equations scheme of Patankar (1980) was used to solve equations (1), (2), (3), (10) and (11). The computation scheme has been detailed previously (Zhou et al., 2002). The total number of particles N (thus the size of the simulated uidized bed) is limited by the computer power since the CPU time is proportional to N 2 . Here, 1480 particles (1460 sand particles of diameter 1 mm and 20 coal particles of diameter 0:8 mm) were put in the bed at initial stage. The ratio number of coal particles over number of sand particles is based on the mass ratio of the coal over the inorganic materials in uidized bed combustors. Generally, this ratio is less than 24%; in the simulation it is approximately 0.3% to avoid any burning of coal particles at the bed surface because of possible segregation. For the validity of the simulation of coal combustion in uidized bed, a heterogeneous structure must be

possible, and the coal particles must have the opportunity to move in both the bubble phase and the emulsion phase. Thus the size of the cells was chosen to be big enough to contain enough particles, approximately 12 particles (mean value), to have signi cant interaction effects, but be small enough for allowing averages. The resulting bed size was 4.84 7.26 cm in width and height. For the gas calculation, the bed was divided into 9 13 cells (width height). It is a good compromise since the effects of the bed size and particle number on the coal combustion in uid bed are small. The coal and sand densities were 1100 and 2600 kg m3, respectively. The initial bed temperature was 1123:15K; the uidization gas was air at 1123:15K, and the gas velocity was 0:6 m s1 (1:5umf ; umf is the minimum uidization velocity of 1 mm diameter sand). The time step for particle motion was 2 105 s. The fuel analysis of coal was (wt% dry): C (83.0), H (5.4), O (9.0), N (1.4), S (1.2), ash (3.0), moisture (2.6).

RESULTS AND DISCUSSION When coal is fed into a hot uidized bed, each coal particle undergoes heating and combustion. It takes several seconds to burn out the coal, depending on the coal diameter, oxygen concentration, uidizing velocity, etc. However, the simulation showed that most coal particles oat and burn at the bed surface after 1:5 s. To study the effect of the particle heterogeneous ow structure on the coal combustion, the heating process was calculated rst (the initial coal temperature is set as 423:15K). The temperature range of the coal particles is very narrow after 2 s, from 1137.2 to 1140:6K. The combustion process is calculated afterwards (the initial coal temperature is set as 1123:15K). Trans IChemE, Vol 81, Part A, October 2003

SIMULATION OF COAL COMBUSTION

1147

Figure 1. Particle structure at different times.

Figure 3. Contributions of the different heat transfer modes for all the coal particles.

Figure 1 shows snapshots of the particle ow structure. There exists an impulsive start-up process at initial stage (t < 0:25 s). The instantaneous break-up of the inter-particle locking leads to a signi cant increase of bed height. Then, a stable succession of bubble formation and disappearance in the uidized bed is established. The temperature of coal particles is always higher than the bed temperature (Figure 2). The maximum excess temperature is 65:50K at 1 s and it increases up to 273:87K at 2 s. The mean excess temperature increases with time, whereas the bed temperature remains almost constant (it varies from 1123.29 to 1125:54K, i.e. less than 2% variation). The mean excess temperatures is 60.56 and 142:54K at 1 and 2 s, respectively. The temperature of coal particles can vary widely, and the range increases with time. It is 10:94K at 1 s and 198:10K at 2 s. The big temperature difference results from the different routes followed by coal particles, where the O2 concentration, the gas velocity and the in uence of other coal particles etc. may vary greatly. Figure 3 plots the instantaneous contributions of the four heat transfer modes, i.e. heat of coal combustion, radiation, convection and collision) for all the coal particles during the combustion process. The heat of combustion is the largest whereas the collision heat transfer is the smallest, and the radiation and the convection contributions are similar. The collision heat transfer uctuates with time because of the discontinuous coalparticle collisions, and its instantaneous contribution ranges from 0 to 1.10%. Thus, the simulation shows that the heat transfer due to particle collisions is always weak during coal combustion. Moreover, all the heat transfer modes depend strongly on the type of coal particles: the absolute values for the same heat transfer mode may

vary up to almost 10-fold when the properties of particles changed. The temperature of coal particles and their heating rates varied considerably during the uidization process, as illustrated by two examples of particles (Figure 4). Both considered particles behave similarly in the rst second; then particle 2 was heated very quickly, especially after 1:5 s (870K s1 at 2 s), whereas particle 1 is not heated and its heating rate even became negative. This results in a very large difference in particle temperature (1380K for particle 2, 1240K for particle 1, after 2 s). This points out that the thermal characteristics of burning coal particles may different strongly, even if the initial conditions are almost the same. Figure 5 shows the non-uniform distributions of the gas species at 1 s in the uidized bed. O2 concentration is higher at the bottom (air injection) and it decreases along the bed, especially in the center where combustion is higher. Conversely, CO2 concentration is very low at the bottom and it is always higher in the upper center of the bed. CO concentration was high in the regions of coal particles. NO concentration is always higher than N2O concentration. The local maximum concentrations of NO and N2O are 77.4 and 19:0 ppm at 1 s, respectively. Figure 6 plots the gas species concentrations at the outlet of the uidized bed vs. time. O2 concentration decreases regularly with time, contrary to CO2 and NO, which increase regularly. CO concentration uctuates a lot and increases. There exists a sharp peak in the rst tenths of

Figure 2. Excess temperature of coal particles at different times.

Figure 4. Variations of coal temperatures and heating rates with time.

Trans IChemE, Vol 81, Part A, October 2003

1148

ZHOU et al.

Figure 5. Instantaneous gas species distributions (mass fraction, time

1.0 s).

later it will be possibly implemented at larger scales, following the increase of calculator power.

NOMENCLATURE
A, B, C, D Ap Cf CH2 O CNO CN2 O CCO CO2 Cp Di dp EA fp G Gi hp kA, kB, . . . , kJ k0 m mp N Qc Qcoll Qcomb Qr r R RA, RB, . . . , RJ Sc t Tb Tf constants in Equation (2) particle surface area, m2 heat capacity of the gas, J (kg K) 1 oxygen concentration, mol m 3 NO concentration, mol m 3 N2O concentration, mol m 3 CO concentration, mol m 3 O2 concentration, mol m 3 heat capacity of particle, J (kg K) 1 diffusion coef cient, m2 s 1 particle diameter, m apparent activation energy, J mol 1 speci c internal surface area of the char, m average Youngs moduli, GPa Young moduli, GPa s heat transfer coef cient, J (m2 s) 1 rate constant of reactions, s 1 pre-exponential factor in Equation (1), s 1 average mass of particle, kg mass of particle, kg order of reaction in Equation (1) convective heat transfer, J s 1 collision heat transfer, J s 1 heat of combustion, J s 1 radiation heat transfer, J s 1 average radius, m ideal gas constant, (8.314 J mol 1 K 1) reaction rate, mol m 3 s 1 turbulent Schmidt number, Sc 0:7 time, s bed absolute temperature, K gas absolute temperature, K

Figure 6. Gas species at the outlet of the uidized bed.

second, due to coal pyrolysis. N2O concentration always remains very small, although increasing slightly with time. CONCLUSION Coal combustion was numerically studied at the particle level in a uidized bed. The mathematical model was based on the DEM model with heat transfer and chemical reactions (kinetics). The dynamic simulation predicted the particle heterogeneous ow structure, the thermal characteristics of burning coal particles, in particular coal particles overheating, and the gaseous emissions from a uidized binary mixture of sand and coal. It was planned to validate these results with experimental data. This method, now developed at small scale, cannot yet simulate industrial reactors, but

Trans IChemE, Vol 81, Part A, October 2003

SIMULATION OF COAL COMBUSTION

Tp TR u ~f umf vpn Vpyrol Vpyrol Wi Yi Ymi
Greek symbols a e gi nt rf rp sSB lf lp Bp Dt DT Dx Dy
Subscripts c s 0

1149

particle absolute temperature, K heating rate, K s 1 ltered gas phase velocity, m s 1 minimum uidization velocity, m s 1 normal relative velocity, m s 1 mass fraction of volatiles evolved up to time t limit value of Vpyrol as t molecular weight, kg mol 1 local mass fraction of species local mole fraction of species
primary CO=CO2 product ratio porosity in uid cell Poisson ratio SGS kinetic gas viscosity, m2 s 1 gas density, kg m 3 particle density, kg m 3 StefanBoltzmann constant gas conductivity, J (s m K) 1 particle conductivity, J (s m K) 1 emissivity of the particle time step, s mean excess temperature, K x direction mesh spacing, m y direction mesh spacing, m
coal sand initial

REFERENCES
Adanez, J. and Abanades, C., 1992, Modeling of lignite combustion in atmospheric uidized bed combustors, 1. Selection of submodels and sensitivity analysis, Ind Eng Chem Res, 31: 22862296. Canu, P., 2001, Simulation and interpretation of catalytic combustion experimental data, Catal Today, 64: 239252. Chan, L.K., Saro m, A.F. and Beer, J.M., 1983, Kinetics of NOcarbon reaction at uidized bed combustion conditions, Combust Flame, 52: 3744. Chen, Z., Lin, M., Ignowski, J., Kelly, B., Linjewile, T.M. and Agarwal, P.K., 2001, Mathematical modelling of uidized bed combustion, 4: N2O and NOx emissions from the combustion char, Fuel, 80: 12591272. Cundall, P.D. and Strack, O.D.L., 1979, A discrete numerical model for granular assemblies, Geotechnique, 29: 4765. De Soete, G.G., Croiset, E. and Richard, J.R., 1999, Heterogeneous formation of nitrous oxide from char bound nitrogen, Combust Flame, 117: 140154.

Donskoi, E. and McElwain, D.L.S., 1999, Approximate modelling of coal pyrolysis, Fuel, 78: 825835. Flamant, G., Lu, J. and Variot, B., 1993, Towards a generalized model for vertical walls to gassolid uidized beds heat transferII. Radiative transfer and temperature effects, Chem Eng Sci, 48: 24932503. Hobbs, M.L., Radulovic, P.T. and Smoot, L.D., 1992, Modelling xed-bed coal gasi er, AIChE J, 38: 681702. Hoomans, B.P .B., Kuipers, J.A.M., Briels, W.J.W. and Van Swaaij, P.M., 1996, Discrete particle simulation of bubble and slug formation in a twodimensional gas- uidized bed: a hard-sphere approach, Chem Eng Sci, 51: 99118. Koutmos, P., 2000, Simulations of localized extincition in turbulent CH4 jet ames using a Lagrangian model for reactedness, Acta Astronaut, 46: 47 53. Lathouwers, D. and Bellan, J., 2001, Modeling of dense gas-solid reactive mixtures applied to biomass pyrolysis in a uidized bed, Int J Multiphase Flow, 27: 21552187. Massman, W.J., 1998, A review of the molecular of diffusivities of H2O, CO2, CH4, CO, O3, SO2, NH3, N2O, NO, and NO2 in air, O2 and N2 NEAR STP Atmos Environ, 32: 11111127. , Patankar, S.V., 1980, Numerical Heat Transfer and Fluid Flow (Hemisphere, New York, USA). Peirano, E. and Leckner, B., 1998, Fundamentals of turbulent gassolid ows applied to circulating uidized bed combustion, Prog Energy Combust Sci, 24: 259296. Rong, D. and Horio, M., 1999, DEM simulation of char combustion in a uidized bed, 2nd International Conference on CFD in the Minerals and Process Industries (CSIRO, Melbourne, Australia). Sun, J. and Chen, M., 1988, A theoretical analysis of heat transfer to particle impact, Int J Heat Mass Transfer, 31: 969975. Tsuji, Y., Kawaguchi, T. and Tanaka, T., 1993, Discrete particle simulation of two-dimensional uidized bed, Powder Technol, 77: 7987. Yuu, S., Nishikawa, H. and Umekage, T., 2001, Numerical simulation of air and particle motions in group-B particle turbulent uidized bed, Powder Technol, 118: 3244. Zhou, H., Abanades, S., Flamant, G., Gauthier, D. and Lu, J., 2002, Simulation of heavy metal vaporization dynamics in a uidized bed, Chem Eng Sci, 57: 26032614.

ADDRESS
Correspondence concerning this paper should be addressed to Dr G. Flamant, Institut de Science et de Genie des Materiaux et Procedes, CNRS-IMP, BP 5, 66125 Odeillo-Font-Romeu Cedex, France. E-mail: amant@imp.cnrs.fr The paper was presented at the 9th Congress of the French Society of Chemical Engineering held in Saint-Nazaire, France, 911 September 2003. The manuscript was received 26 February 2003 and accepted for publication after modi cation 28 August 2003.

Trans IChemE, Vol 81, Part A, October 2003