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Die Ressourcenuniversität. Seit 1765.
TU Bergakademie Freiberg I Department of Energy Process Engineering and Chemical Engineering
Reiche Zeche I 09596 Freiberg I Germany I Phone +49(0)3731/39-4511 I Fax +49(0)3731/39-4555
Email [email protected] I Web www.iec.tu-freiberg.de
Department of Energy Process Engineering
and Chemical Engineering
Influence of Coal Blend Component Kinetics on
Entrained-Flow Gasification Performance
Lars-Erik Gärtner*, Martin Gräbner, Danny Messig, Wolfgang Heschel, Bernd Meyer
*Email: [email protected], Phone: +49 3731 39 4774
2
Content
1 Project and task description
2 Gasifier model development
3 Gasifier model verification
4 First results and discussion
5 Next steps
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600 °C
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1300 °C
600 °C
1250 °C
1000 °C
1200 °C
1350 °C
1300 °C
600 °C
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1000 °C
1200 °C
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600 °C
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0.0 0.2 0.4 0.6 0.8 1.0
0.0
0.2
0.4
0.6
0.8
1.00.0
0.2
0.4
0.6
0.8
1.0
Carbon Conversion in %
CR
C252
CR
C299 (C
har)
CRC274 (Char)
30 32 34 36 38 40 42 44 4646< 46
Maximum Gasifier Temperature
Maximum Carbon Conversion (45.4%)
Carbon Conversion Contour Lines
No ignition zone
▲
1 4
4 3
,
1 1
R Rsm s
m
mR M
x
1
3
1 ibi - Project description
Concept of a staged process chain for integral non-energetic
utilization of lignite with high wax content (Central Germany)
Gasifier must be able to process fuel blends
with varying composition depending on plant
operation
▲ 1
4
1 ibi – Description of modeling task
Influence of fuel blend composition on carbon conversion,
cold gas efficiency and temperature profile inside the gasifier
Entrained-flow
gasifier
Dried lignite
VM (waf) = 64%
FC (waf) = 36%
Extraction residue
VM (waf) = 58%
FC (waf) = 42%
Char (cat.-crack.)
VM (waf) = <15%
FC (waf) = >85%
Ternary
fuel blend
Syngas
Mathematical gasifier model with ability to process ternary fuel blends
Detailed flow sheet model of entire process chain
Blend composition
varies during plant
operation
▲ 1
5
2 Gasifier model development ▲
Modeling environment of choice: Aspen Plus
• Integratability of detailed gasifier model in complex flow sheet
model of the ibi process chain (plant optimization)
• Availability of physical and thermodynamic properties database
Reactor model properties
• First stage: drying and devolatilization (product yield)
• Second stage: kinetic 1D plug flow gasification reactor (rate and
product yield)
• Processing of ternary fuel blends
• Isothermal or adiabatic process mode
• Radial temperature und gas composition gradients are neglected
• Particle inherits temperature of gas phase
• Robust convergence behavior
2
6
2 Gasifier model development ▲
Considered heterogeneous gasification reactions
Considered homogeneous gas phase reactions
1
2 2
1 1 22 1 1
RC O CO CO
2
2 2 R
C CO CO
3
2 2 R
C H O CO H
4
2 42 R
C H CH
5
2 2
1
2
RCO O CO
6
2 2 2
1
2
RH O H O
7
4 2 2 22 2R
CH O CO H O
8
2 2 2 R
CO H O H CO
9
2 2 2 R
H CO CO H O
2
7
2 Gasifier model development ▲
5 91 4
4 3 9
,
1 1 5
( ) ( )R RR Ri
i i m i i i m i
m m
mR M R M
x
1 9
9 3
, ,
1 1
R R
m m
m
HR h
x
Conservation of mass
Conservation of energy
1 4
4 3
,
1 1
R Rsm s
m
mR M
x
Capital letters
m Mass flow ( kg / s )
x Length ( m )
R Reaction rate ( kmol / m / s )
M Molar weight ( kg / kmol )
Stoichiometric coefficient
H Enthalpy flow ( kJ / s )
h Heat of reaction ( kJ / kmol )
Subscripts
s Solid
m Reaction index
Fuel index
i Gas species index
Superscripts
Reactant gas
Product gas
´
´´
2
8
2 Gasifier model development ▲
Calculation of reaction rates
Heterogeneous
Homogeneous
1 4 1 4
, , , , , ,mnR R R R
m m p t S m mR a p k ,5 9 5 9
1
m i
NnR R R R
m m i
i
R k c
1 4 1 4 ,
, , exp
mR R R R
m m
p
Ek A
T5 9 5 9 exp
R R R R mm m
p
Ek A
T
,int, ,int, ,0 0( ) (1 ) 1 ln(1 )p C p C Ca X a X X
, , ,int, , , p t p p exa a a
,
, , ,
3 1 1
tanh
m
m m m
,1 41
, , , , ,int, ,,
,
, , ,
1
3 2
mnR R
m m p m p g S mp
m
s i eff p
n k a T pr
M D
[2]
[1]
[1]
[1]
[1] Laurendeau, N.M.; Heterogeneous Kinetics of Coal Char Gasification and Combustion; Progress in Energy and Combustion Science 1978(4):221-270.
[2] Bhatia, S.K., Perlmutter, D.D.; A Random Pore Model for Fluid-Solid Reactions: I. Isothermal, Kinetic Control; AIChE Journal 1980;26(3):379-386.
2
, , ,4 p ex pa r( ²)
( )
( / ² / / ) (1/ )
( / ² / / ) ( / ³ / )
( / )
n
n
Effectivness Factor
a Surface area m
p Partial pressure atm
k Reaction rate constant
kg m s atm or s
A Frequency factor
kg m s atm or kmol m s
E Activation energy kJ kmol
n Order of reaction
Particle roughnes
( )
( ² / )
C
eff
s factor
X Carbon conversion
Particle structural parameter RPM
Thiele modulus
Stoichiometry coefficient
D Effective diffusivity m s
2
9
2 Gasifier model development ▲
Schematic structure of gasifier model in Aspen Plus
2
Drying,
Devolatilization &
Char Decomposition
Volatile
Combustion
VMFuelβ
Gasification
Charβ
O2/Air
Combustion
Products
RYield+RStoic RGibbs
RPlug
Physical &
Thermodynamic
Properties Database
Aspen Plus Graphical User Interface
Ash
Charβ
Kinetics Subroutine
Solid Residence
Time
Calculator
Qdevol. + Qdecomp.
Additional
User Input
Calculator
Prox./Ult./Sulf.
Analysis
rp,ψβ,ap,0,β,nβ,Aβ,Eβ,
εma,β,εme,β,εmi,β,Ωβ,λ
External FORTRAN77
dr,lr,reactor type (adiabatic or
isothermal), numerical
convergence parameters
dr*
Solver
dr,lr
assume Rep,in < 2,τS
Raw Gas
Aspen Simulation Engine Aspen Properties
km,β,Rm,β,ap,t,β,ap,int,β,ap,ex,β,ηm,β,φm,β,Di,eff,p,β,dm/dx,dH/dx
Check, if Rep,out < 2
Steam
10
3 Gasifier model verification ▲
Verification data from single coal gasification experiments (1)
• Case setup data taken from PEFR experiments of CSIRO [3]
• Devolatilization product distribution data derived from wire mesh
reactor experiments [4]
• 3 Australian coals where investigated (CRC252, CRC274, CRC299)
[3] Hla, S., Harris, D.J., Roberts, D.G.; Gasification Conversion Model – PEFR: Research Report 80, Pullenvale, Australia; 2007.
[4] Mill, C.; Pyrolysis of Fine Particles at High Heating Rate and Pressure, PhD-Thesis, Sydney; 2000.
Fig. 1: Model carbon conversion profiles and exp. data points
3
11
3 Gasifier model verification ▲
Verification data from single coal gasification experiments (2)
Fig. 4: Model CO2 mole fraction profiles and exp. data points Fig. 5: Sensitivity analysis oxygen to carbon molar ratio
model and experiment (CRC274)
Fig. 2: Model CO mole fraction profiles and exp. data points Fig. 3: Model H2
mole fraction profiles and exp. data points
3
12
4 First results and discussion ▲
Fuel system
Unit Fuel 1 Fuel 2 Fuel 3
Fuel type
CRC252
(as received)
CRC274
(char)
CRC299
(char)
HHV (Dulong) MJ/kg (wf) 28.62 29.22 20.82
Proximate analysis
Fixed carbon wt.% 39.1 86.2 61.4
Volatile matter wt.% 38.8 0.0 0.0
Ash wt.% 11.3 13.8 38.6
Moisture wt.% 10.7 0.0 0.0
Ultimate analysis
C wt.% (waf) 78.1 100.0 100.0
H wt.% (waf) 5.9 0.0 0.0
O wt.% (waf) 14.4 0.0 0.0
N wt.% (waf) 1.1 0.0 0.0
S wt.% (waf) 0.5 0.0 0.0
4
Tab. 1: Fuel system designed for binary and ternary fuel blend gasification simulations
13
4 First results and discussion ▲
Simulation results - binary fuel blend gasification
• Adiabatic reactor (PEFR geometry)
•
4
0
200
400
600
800
1000
1200
1400
0
10
20
30
40
50
0 0,2 0,4 0,6 0,8 1
Maxim
um
Gasi
fier
Tem
pera
ture
in
°C
Con
vers
ion
in
%
M ass Fraction CRC252
Carbon Conversion
Char Conversion
Tmax Gasifier
No i
gn
itio
n z
on
e
0
200
400
600
800
1000
1200
1400
0
10
20
30
40
50
0 0,2 0,4 0,6 0,8 1
M ass Fraction CRC252
Maxim
um
Gasi
fier
Tem
pera
ture
in
°C
Con
vers
ion
in
%
Carbon Conversion
Char Conversion
Tmax Gasifier
No i
gn
itio
n z
on
eFig. 6: Binary fuel blend gasification results - system CRC274-CRC252 Fig. 7: Binary fuel blend gasification results – system CRC299-CRC252
• Char LHV controls maximum gasifier temperature, thus carbon
and char conversion
• “No ignition zone” of char blend CRC299-CRC252 is larger then
blend CRC274-CRC299
, ,. ; . ; . . / ;
N O in N inm LHV const kW m const kg h T T C
2 2 2
85 0 3 36 2 200
14
4 First results and discussion ▲
Simulation results - ternary fuel blend gasification
4
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1360 °C
1340 °C
1200 °C
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600 °C
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1250 °C
1360 °C
1340 °C
1200 °C
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0.0 0.2 0.4 0.6 0.8 1.0
0.0
0.2
0.4
0.6
0.8
1.00.0
0.2
0.4
0.6
0.8
1.0
CR
C252
CR
C299 (C
har)
CRC274 (Char)
30 32 34 36 38 40 42 44 46
No ignition zone
<
Carbon Conversion in %Maximum Gasifier Temperature
Carbon Conversion Contour Lines
Maximum Carbon Conversion (46.2%)
# of single simulations: 1000
Calculation time: 12h 54min
Fig. 8: Ternary fuel blend gasification results - system CRC274-CRC252-CRC299
15
4 First results and discussion ▲
The kinetic fuel blend synergy effect in gasification
4
Fuel 1
High VM content
Fuel 2
Low to no VM content
High LHV
Fuel blend gasification
Fuel 2 benefits from Fuel 1 volatile combustion
(Fuel2 activation energy barrier is exceeded → ignition)
Fuel1 and Fuel2 char conversion is accelerated by
increased max. gasification reactor temperature
from high LHV of Fuel2
Higher total carbon conversion
16
5 Next steps ▲
Fuel blend validation experiments in new GMEQ reactor
• Fuel system: (1) Central German lignite, (2) extraction residue and
(3) char from catalytic cracking process
• Data analysis to obtain Langmuir-Hinshelwood (LHW) type kinetic
parameters
5
Model enhancement towards LHW kinetic expression
• Modification of existing gasifier model
• Implementation of measured LHW constants in gasifier model
Development of plant flow sheet model
• Integration of gasifier model in plant flow sheet
• Sensitivity study of plant process parameters
Fuel blend gasification with 2D CFD simulations
• Verification of the fuel blend synergy effect in gasification
17
Acknowledgments
We like to thank the German Federal Ministry of Education and
Research for the financial support of the present work within
the framework of the research initiative ibi – Innovative
Process Technology (R&D code 03WKBZ06C). Special thanks is
regarded to A. Laugwitz for constructive discussions during
the model development and verification phase.
▲ 5