Mathematical modeling of coke combustion

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Mathematical modeling of coke combustion

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∂εs ρs hs ∂εs ρs us hs

Abstract—We describe behavior of the moving coke bed + = Shs ,

combustion in a cupola furnace, based on balance equations for ∂t ∂x

big coke particles and oxygen enriched blast. The undergoing where εs is solids’ volume fraction (εs = 1 − εg where εg

chemical reactions are described by the Arrhenian kinetics is void fraction), ρs is particle density of coke, us is descent

E

(reaction rate proportional to e− RT for homogeneous reactions)

as well as diffusion limited rate chemistry for heterogeneous

velocity (which is constant for all particles at given time), Srs

reactions on the coke surface. We also consider the heat is mass source term due to coke combustion and gasification,

transfer among solid and gas phases and furnace water jacket. hs is specific enthalpy of coke particles and Shs is energy

The system of PDEs is discretized using the finite volume source term due to combustion, gasification and heat transfer

method (FVM) and time integration is performed via Euler to the surrounding gas and walls. For flue gases we have

explicit scheme together with point-implicit preconditioning of

species balance equations. Simulation results are compared with

mass, heat and components’ mass fractions balances:

experimental ones. ∂εg ρg ∂εg ρg ug

+ = Srg ,

Index Terms—coke combustion, reactive flow modeling, het- ∂t ∂x

erogeneous combustion ∂εg ρg hg ∂εg ρg ug hg

+ = Shg ,

∂t ∂x

I. I NTRODUCTION

∂εg ρg ug Yj ∂εg ρg ug Yj

OMBUSTION of large particles constitutes one of

C the major problems in modeling of industrial scale

combustion. The rate of combustion is limited by two com-

∂t

+

∂x

= SYj ,

peting processes, the kinetic limited and the diffusion limited

where ρg is gas density, ug is actual velocity, Srg is mass

combustion. While kinetic limited combustion is the case

source term due to coke combustion and gasification, hg

for small particles and homogeneous reactions in the gas

is specific enthalpy, Shg is energy source term due to

phase, the diffusion limited combustion takes place during

combustion and heat transfer to the coke particles and walls,

surface heterogeneous reactions on the large particles. Main

Yj is mass fraction of j-th component of flue gas and SYj

products of such reactions are carbon dioxide and carbon

is source term due to homogeneous reactions in flue gases.

monoxide whose concentrations in exhaust gases are to be

Gas phase is considered to be in a state of plug flow, and its

controlled and in the latter case limited to the minimum.

superficial velocity is computed from known blast volumetric

When coke burns, extensive amounts of carbon monoxide

flux, rate of combustion and barotropic condition inside the

can be released in flue gases due to e.g. Boudouard reaction.

cupola furnace.

However in some cases this is necessary part of industrial

Chemical reactions considered in the model are:

process (as in the case of a blast furnace) in other cases

this is strictly unwanted. We develop a 1D model of large 1) Heterogeneous gasification of fuel

coke particles combustion in a cupola furnace, together 2

RCO

with essential chemical reactions and heat and mass transfer C(s) + CO2 (g) −−−−→ 2CO(g),

relations which can be further used for simulation of other RH O

industrial processes where the coke combustion is main C(s) + H2 O(g) −−−2−→ H2 (g) + CO(g),

source of heat and emissions. Model itself is based on heat RCO s

and mass balance laws for counter current tubular reactor. C(s) + O2 (g) −−−−2→ CO2 (g),

Comparison of simulated and experimental results shows 1 RO2

good agreement [1] and the model was incorporated into the C(s) + O2 (g) −−−→ CO(g).

2

bigger project of rock melting cupola simulation tool [2]. 2) Homogeneous combustion

II. M ATHEMATICAL MODEL 1 R

CO(g) + O2 (g) −−CO−→ CO2 (g),

Moving bed consists of two phases, flue gases and solid 2

coke particles, for the solid phase we have following mass 1 RH2

and heat balances: H2 (g) + O2 (g) −−−→ H2 O(g).

2

∂εs ρs us 3) Water gas shift

= Srs ,

∂x

w R

Manuscript received December 28, 2013; revised May 7, 2014. This work

CO(g) + H2 O(g) −−→ CO2 (g) + H2 (g).

was supported by the research project No. 15.11.110.239 from the budget for

science at Faculty of Metals Engineering and Industrial Computer Science, Heterogeneous reactions take place in the vicinity of the coke

AGH University of Science and Technology. particles creating thin film, away from this film homoge-

R. Straka and T. Telejko are with the Department of Heat Engineering neous combustion of carbon monoxide and hydrogen occurs

and Environment Protection, Faculty of Metals Engineering and Industrial

Computer Science, AGH University of Science and Technology, Aleja together with water gas shift reaction. Combination of source

Mickiewicza 30, 30-059, Cracow, Poland; email:straka@metal.agh.edu.pl. terms R∗ yields the overall source terms Srs , Srg and SYj

for appropriate phase and specie, these terms are described with λg gas heat conduction coefficient and Res is Reynolds

in the following section. number based on particle diameter. System of equations is

Heat transfer among gas, particles and walls is given by accompanied with following relations:

following relations: X X Z Tg/s

p = ρRTg , ρ = ρj , hg/s = cp,j/s (T )dT.

X

Shg = − ηk ∆Hk Rk − Sh,het + as hgs (Ts − Tg ) T0

j j

k

+as σes (Ts4 − Tg4 ) + Qgw ,

III. H ETEROGENEOUS AND HOMOGENEOUS

X COMBUSTION

Shs = − (1 − ηk )∆Hk Rk + Sh,het

k Mass source terms for balance equations are derived from

−as hgs (Ts − Tg ) − as σes (Ts4 − Tg4 ) + Qsw , stechiometric equations from previous section and read:

where first terms are due to chemical reactions with ηk being Srg = MC (RCO2 + RH2 O + RCO2 (s) + 2RO2 ),

portion of energy ∆Hk released by homogeneous reaction MC

Rk transferred to gas phase, Sh,het is energy released from Srs = − r (RCO2 + RH2 O + RCO2 (s) + 2RO2 ),

C

heterogeneous reactions, third terms is combined convective SYO2 = −MO2 RO2 + RCO + RH2 + RCO2 s ,

and conductive heat transfer hgs between gas and particles

SYH2 O = MH2 O 2RH2 − RH2 O − Rw ,

surface as with Tg gas- and Ts solid temperatures, next

terms provide radiative heat exchange between gas and solid SYCO = MCO 2(RCO2 + RO2 − RCO ) + RH2 O − Rw ,

(effective emissivity of coke es is assumed to be 0.9) and SYCO2 = MCO2 −RCO2 + 2RCO + RCO2 s + Rw ,

last terms represent heat losses to walls, σ = 5.67 · 10−8

SYH2 = MH2 RH2 O − 2RH2 + Rw ,

is Stefan-Boltzmann constant. Note that summing up those

two equations and dropping first and last terms yields zero, where MC is molar mass of carbon and C r is mass fraction

i.e. non-chemical energy is conserved in the model when the of carbon in coke as given by ultimate analysis of fuel

system is adiabatically insulated. Energy exchange term for sample. Reactions terms are described by Arrhenian kinetic

heterogeneous reactions reads: for homogeneous reactions i.e. the reaction rate k is given

Sh,het = RO2 (MO2 hO2 (Tg ) − 2MCO hCO (Ts )) by:

Ek

−R

+RCO2 s (MO2 hO2 (Tg ) − MCO2 hCO2 (Ts )) kkhom = Ak e 0T ,

+RCO2 (MCO2 hCO2 (Tg ) − 2MCO hCO (Ts )) where frequency factors Ak and activation energies Ek for

+RH2 O (MH2 O hH2 O (Tg ) − MH2 hH2 (Ts ) reactions are taken from [5]. Heterogeneous reactions are

−MCO hCO (Ts )). diffusion-kinetic limited i.e. their rates are evaluated as:

Overall heat transfer coefficient hgs is given by relation [3]: kkhet = min(kkkin , kkdiff ),

−0.41

ug where diffusion rate:

hgs = 1.061δhgs ds ρg ρg ug cp,g Prg−2/3 ,

µg Shj Dj

kkdiff =

where δhgs is a correction coefficient established during ds

validation, µg is gas dynamic viscosity, cp,g is gas specific is evaluated using Sherwood number (Shj ) correlations by

heat and Prg is Prandtl number. Particle diameter ds , surface Dwivedi and Upadhyay [6]:

area as and volume fraction εs change during combustion

and gasification and are computed from: 1/3 0.765 0.365

Shj = Scj Res + ,

r

εs ρs us Res0.82 Res0.386

ds = ds,in 3 ,

(εs ρs us )in where Scj and Dj are Schmidt number and diffusion coef-

6εs ficient for O2 , CO2 and H2 O [7]:

as = ,

φs d s

Tg

1.75

101325

εs =

ρs,bulk

, DO2 = 2.2 · 10−4 ,

ρs 1000 p

1.75

where φs is sphericity of coke particles. Non-conserved −5 Tg 101325

DH2 O = 1.6 · 10 ,

energy terms due to interaction with surrounding walls are: 395 p

1.75

Qsw = Aσ(ξs es Ts4 − ew Twall

4 Tg 101325

), DCO2 = 2.2 · 10−5 .

273 p

the correction parameter ξs must be determined from mea-

surements and wall emissivity is set to ew = 0.85, IV. N UMERICAL ALGORITHM

Qgw = Aσeg (Tg4 − Twall

4

) + Ahgw (Tg − Twall ), Furnace chamber is divided into finite control volumes and

where heat transfer coefficient from gas to wall is given by finite volume method approximation of spatial derivatives to-

[4]: gether with simple explicit Euler scheme for time derivatives

is applied:

λg 1 − εg 0.815 −0.5 Tg 0.73 ∂U ∂F

hgw = 0.07659 Res Prg , + =S

ds εg Twall ∂t ∂x

τ

Ui+1 − Uiτ 1 TABLE I

+ (∂ΩU )i+1/2 − (∂ΩU )i−1/2 = Si , S IMULATION SETUP.

∆τ |Ωi |

where following notation is used: Hot blast volume 169.8 Nm3 /h

Blast temp. 80 ◦ C

Srg

εg ρg εg ρg ug Oxygen enrichment 0 Nm3 /h

εg ρg hg εg ρg ug hg Shg Coke bulk density 500 kg/m3BED

εg ρg YO

εg ρg ug YO

SY Coke diameter 0.04 m

2 2

O2

εg ρg YCO εg ρg ug YCO S Carbon content 71.3 %

2 2

YCO2

Cupola diameter 0.2 m

U = εg ρg YCO , F = εg ρg ug YCO , S = SYCO .

εg ρg YH εg ρg ug YH SYH2

Cupola height 1.37 m

2 2

37 ◦ C

εg ρg YH O εg ρg ug YH O

SYH O Wall temp.

2 2

2

0 εs ρs us

Srs

εs ρs hs εs ρs us hs Shs

carbon monoxide and carbon dioxide were measured. At each

When fast (chemical reactions) and slow (heat transfer, slow level, three samples were taken at near wall, midpoint and

chemical reactions) processes are coupled, above system center locations. Accuracy of the tuned model is surprisingly

of equations has great disparity in Jacobian’s eigenvalues high.

which leads to extremely small time steps in order to keep

positivity and accuracy of the solution. One remedy is to VI. C ONCLUSION

apply point implicit preconditioning of time derivatives of

The complex model of coke combustion and gasification

species equations [8]:

in moving bed was developed. Data from simulations were

∆τ τ compared with experimenal data and are in good agreement.

UYτi+1 = UYτi + [Res]Yi ,

1 + ∆τ ∂SYi /∂UYi From the simulated and measured data it is clear that oxygen

is consumed up to the half of the cupola with increasing con-

this technique does not affect steady-state solution which is

centrations of carbon monoxide and dioxide. The presence

the desired one. The above system of discretized equations

of high temperature, water molecules and oxygen keeps the

is then accompanied with boundary conditions, the known

concentration of carbon monoxide low. The peak temperature

volumetric flux, composition and temperature of blast at the

of flue gases is at same position as the peak carbon dioxide

bottom of the cupola and composition and temperature of

concentration indicating that at this point the combustion

solid fuel at the opposite side. The initial conditions must be

is the most intensive. After this point, oxygen is almost

carefully chosen to support startup of the combustion inside

exhausted and carbon monoxide produced by Boudouard

the cupola.

reaction cannot be burned to carbon dioxide, thus the con-

centration of carbon monoxide is increasing together with

V. R ESULTS decrease in carbon dioxide concentration and temperature

To examine model abilities, we setup the model con- decrease due to endothermic nature of Boudouard reaction.

sistently with experiment performed by Hameedullah and Nevertheless the temperature of flue gases are too high to

Chakraborty [9] (values are given in Tab. I). Character N stop Boudouard reaction and it proceeds until the end of

before m3 stands for normal conditions i.e. volume of gas cupola. High temperature of flue gases and lack of oxygen

is given at pressure equal to 1 atmosphere and temperature also cause decrease in water and increase in hydrogen

equal to 273.15 Kelvins. A bulk density is mass of material concentrations due to water gas and water gas shift reactions.

related to the volume which the material occupies i.e. in coke The extended version of the model is used in simulation tool

filled container (so called ”bed”) of volume equal to 1 m3 we of rock-melting cupola. The model can be further developed

have 500 kg of coal particles. During several runs, correction and enhanced to simulate different industrial processes which

parameters (that cannot be measured or predicted in advance) involve moving bed combustion (e.g. blast furnaces) of coal

were fine tuned until agreement between measured and particles.

computed values was established. The parameter δhgs has

great influence on temperature profiles as increasing heat R EFERENCES

flux to the wall decreases flue gas and coal temperatures [1] R. Straka and T. Telejko, “Validation of Mathematical Model of

and rather small influence on concentrations profiles (with Combustion and Rock Melting in Cupola Furnace,” May 2013, internal

observable effect on carbon dioxide concentrations shift). Report.

[2] ——, “Mathematical Model of Combustion and Rock Melting in

The parameter ξs has very strong influence on the tempera- Cupola Furnace,” Dec. 2012, internal Report.

ture profiles in the middle of the cupola (where the highest [3] B. R. Bird, W. E. Stewart, and E. N. Lightfoot, Transport Phenomena,

temperatures occur) and thus observable influence on the 2nd ed. John Wiley & Sons, 2001.

[4] E. Piwowarski, “Matematisches modell des kupolofenprozesses,”

carbon monoxide and carbon dioxide concentrations in the Giessereiforschung, vol. 2, 1973.

upper half of the cupola. Comparison of experimental data [5] NIST. (2013) Chemical kinetics database on the web. [Online].

(digitally acquired from the article [9]) with computed is Available: http://www.kinetics.nist.gov

[6] R. H. Perry and D. W. Green, Perry’s Chemical Engineers’ Handbook,

shown in Fig. 1. Computed values are depicted as lines, 8th ed. McGraw-Hill, 2008.

molar fractions of CO2 , CO, O2 , H2 O and H2 together [7] S. R. Turns, An Introduction to Combustion: Concepts and Applications,

with flue gas temperature and coal particles temperature. 2nd ed. McGraw-Hill, 2000.

[8] T. R. A. Bussing and E. M. Murman, “Finite volume method for the

Measured values taken from the paper [9] are denoted by calculation of compressible chemically reacting flows,” AIAA Journal,

symbols, there are six levels where concentrations of oxygen, vol. 26, pp. 1070–1078, 1988.

25

20

15

%,oC

10

0

0 0.2 0.4 0.6 0.8 1 1.2 1.4

distance from tuyeres [m]

XO2 Tc/100 TEMP CO2

XCO XH2 O2

Fig. 1. Simulation results, comparison of measured (symbols) and computed (lines) values. X axis denotes position from tuyeres, Y axis is scaled to

contain both temperature in Celsius and molar fractions in percents.

cupola,” Combustion Science and Technology, vol. 45, pp. 129–146,

1986.

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