hydrothermal aging modeling for scr catalysts · and a scr using ifp-exhaust library coupled with a...
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Renewable energies | Eco-friendly production | Innovative transport | Eco-efficient processes | Sustainable resources
Hydrothermal aging modeling for SCR catalysts
Simon Dosda 2015 CLEERS WORKSHOP
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Simon Dosda – Hydrothermal aging modeling for SCR catalysts – 2015 CLEERS WORKSHOP
Interest of SCR modeling for control purpose
Urea-SCR is one of the most common technology used by car and truck manufacturers to meet the latest NOX emission standards
requires to optimize urea injection in order to limit ammonia slip while keeping a good NOX reduction efficiency
2
In this context, system simulation has significant advantages to set up optimal injection strategy:
Physical modeling: modeling level is adapted for control laws design in order to obtain accurate and consistent results in every real life case
Fast calculation time: about 10 times faster than the real time for a complex exhaust line coupled with a high frequency control
Adblue injector
NOX sensor
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Simon Dosda – Hydrothermal aging modeling for SCR catalysts – 2015 CLEERS WORKSHOP
Importance of aging on SCR performances
During engine lifetime, performance degradation of the SCR catalyst is observed due to harsh exhaust conditions
frequent filter regeneration subjects the SCR catalyst to high temperatures
hydrothermal aging will strongly decrease DeNOx and NH3 storage properties of the catalyst
Modeling hydrothermal aging impact on the catalyst allows to adapt urea injection strategy and avoid excessive amount of ammonia slip
only way to adapt injection strategy over the complete vehicle lifetime
3
Is there a way to model efficiently hydrothermal aging impact on a SCR catalyst ?
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Simon Dosda – Hydrothermal aging modeling for SCR catalysts – 2015 CLEERS WORKSHOP
Approach: from fresh to aged SCR model
1 - Fresh SCR model set up and validation:
a - SCR model is calibrated on specific Synthetic Gas Bench tests
b - SCR model is integrated in a complete exhaust line simulator and validated on chassis dynamometer on test cycles
2 - Aging model set up from SGB tests for various aging conditions
3 - Aging model validation on dyno on test cycles using an aged SCR
4
1 - Fresh SCR model
2 - Hydrothermal aging model SGB data
3 - Aged SCR model validation
dyno cycle data
a - Calibration SGB data
b - Validation dyno cycle data
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Simon Dosda – Hydrothermal aging modeling for SCR catalysts – 2015 CLEERS WORKSHOP
Approach: from fresh to aged SCR model
1 - Fresh SCR model set up and validation:
a - SCR model is calibrated on specific Synthetic Gas Bench tests
b - SCR model is integrated in a complete exhaust line simulator and validated on chassis dynamometer on test cycles
2 - Aging model set up from SGB tests for various aging conditions
3 - Aging model validation on dyno on test cycles using an aged SCR
5
1 - Fresh SCR model
2 - Hydrothermal aging model SGB data
3 - Aged SCR model validation
dyno cycle data
a - Calibration SGB data
b - Validation dyno cycle data
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Simon Dosda – Hydrothermal aging modeling for SCR catalysts – 2015 CLEERS WORKSHOP
Fresh SCR model presentation – Reactor scale
LMS Imagine.Lab Amesim model of SGB SCR using IFP-Exhaust library
reactions considered: NH3 adsorption/desorption, DeNOx reactions
(standard, fast & NO2 SCR) and NH3 oxidation
isolated sample: no thermal exchanges considered
SCR sample geometry: length = 3 inches, diameter = 2 inches, 350 cpsi
Synthetic Gas Bench - SCR
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Simon Dosda – Hydrothermal aging modeling for SCR catalysts – 2015 CLEERS WORKSHOP
SCR modeling set up for NH3 storage on SGB test
From NH3 TPD observation, two adsorption sites can be considered
NH3 adsorption reaction for each adsorption site:
NH3 + 𝐒𝐢 ↔ NH3−𝐒𝐢
𝒓𝒂𝒅 = 𝒌𝒂𝒅 × 𝑵𝑯𝟑 × (𝟏 − 𝜽𝑵𝑯𝟑) - 𝒌𝒅𝒆 × 𝒆−
𝑬𝒅𝒆 ×(𝟏−𝒂𝒍𝒑𝒉𝒂×𝜽𝑵𝑯𝟑)
𝑹×𝑻𝒔 × 𝜽𝑵𝑯𝟑
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0
50
100
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300
100 200 300 400 500 600ou
tlet
NH
3 m
ola
r co
nce
ntr
atio
n [
pp
m]
inlet temperature [°C]
SGB test - NH3 TPD - Tinlet 175°C
bench
site 1
site 2
site 1 + 2
Site 1
Site 2
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Simon Dosda – Hydrothermal aging modeling for SCR catalysts – 2015 CLEERS WORKSHOP
0 500 1000 1500 2000 2500 30000
50
100
150
200
250
300
350
SGB test - NH3 TPD - Tinlet 375 °C
Time [s]
NH
3 m
ola
r co
nc
en
trati
on
[p
pm
]
0 500 1000 1500 2000 2500 30000
100
200
300
400
500
600
700
Inle
t T
em
pe
ratu
re [
°C]
Bench - inlet
Bench - outlet
Model - outlet
Temperature
0 500 1000 1500 2000 2500 30000
50
100
150
200
250
300
350
SGB test - NH3 TPD - Tinlet 175 °C
Time [s]
NH
3 m
ola
r co
nc
en
trati
on
[p
pm
]
0 500 1000 1500 2000 2500 30000
100
200
300
400
500
600
700
Inle
t T
em
pe
ratu
re [
°C]
Bench - inlet
Bench - outlet
Model - outlet
Temperature
0 500 1000 1500 2000 2500 3000 35000
50
100
150
200
250
300
350
SGB test - NH3 TPD - Tinlet 550 °C
Time [s]
NH
3 m
ola
r co
nc
en
trati
on
[p
pm
]
0 500 1000 1500 2000 2500 3000 35000
100
200
300
400
500
600
700
Inle
t T
em
pe
ratu
re [
°C]
Bench - inlet
Bench - outlet
Model - outlet
Temperature
150 200 250 300 350 400 450 500 5500
0.02
0.04
0.06
0.08
0.1
0.12
0.14
0.16
0.18
0.2
Inlet temperature [°C]
NH
3 q
ua
nti
ty [
g]
SGB test - NH3 TPD
Bench - adsorbed
Bench - desorbed
Model - adsorbed
Model - desorbed
SCR model calibration for NH3 storage on SGB test
NH3 storage calibration is done on NH3 TPD tests with various inlet temperature
8
Good results consistency for the overall test
data
0 500 1000 1500 2000 2500 30000
50
100
150
200
250
300
350
SGB test - NH3 TPD - Tinlet 275 °C
Time [s]
NH
3 m
ola
r co
nc
en
trati
on
[p
pm
]
0 500 1000 1500 2000 2500 30000
100
200
300
400
500
600
700
Inle
t T
em
pe
ratu
re [
°C]
Bench - inlet
Bench - outlet
Model - outlet
Temperature
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Simon Dosda – Hydrothermal aging modeling for SCR catalysts – 2015 CLEERS WORKSHOP
SCR model calibration for DeNOx reaction on SGB test
Standard SCR reaction calibration:
4 NH3-Si + 4 NO + O2 4 N2 + 6 H2O + 4 Si
𝒓𝒔𝒕𝒅 = 𝒌𝒔𝒕𝒅 × 𝒆−
𝑬𝒔𝒕𝒅𝑹×𝑻𝒔 × 𝑵𝑶 × 𝜽𝑵𝑯𝟑
Calibration is done on DeNOx SGB test with an upstream NO2/NOx ratio of 0 %
0 1000 2000 3000 4000 5000 60000
50
100
150
200
250
300
350
SGB test - DeNOx - Tinlet 175 °C / NO2/NO
X 0 %
Time [s]
NO
X m
ola
r co
nc
en
trati
on
[p
pm
]
0 1000 2000 3000 4000 5000 60000
100
200
300
400
500
600
700
Inle
t T
em
pe
ratu
re [
°C]
Bench - inlet
Bench - outlet
Model - outlet
Temperature
0 500 1000 1500 2000 2500 3000 3500 4000 45000
50
100
150
200
250
300
350
SGB test - DeNOx - Tinlet 275 °C / NO2/NO
X 0 %
Time [s]
NO
X m
ola
r co
nc
en
trati
on
[p
pm
]
0 500 1000 1500 2000 2500 3000 3500 4000 45000
100
200
300
400
500
600
700
Inle
t T
em
pe
ratu
re [
°C]
Bench - inlet
Bench - outlet
Model - outlet
Temperature
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Simon Dosda – Hydrothermal aging modeling for SCR catalysts – 2015 CLEERS WORKSHOP
SCR model calibration for DeNOx reaction on SGB test
Fast SCR reaction calibration:
2 NH3-Si + NO + NO2 2 N2 + 3 H2O + 2 Si
𝒓𝒇𝒂𝒔𝒕 = 𝒌𝒇𝒂𝒔𝒕 × 𝒆−
𝑬𝒇𝒂𝒔𝒕
𝑹×𝑻𝒔 × 𝑵𝑶 × 𝑵𝑶𝟐 ×
𝜽𝑵𝑯𝟑
calibration is done on DeNOx SGB test with an upstream NO2/NOX ratio of 50 %
0 500 1000 1500 2000 2500 3000 3500 4000 4500 50000
50
100
150
200
250
300
350
SGB test - DeNOx - Tinlet 275 °C / NO2/NO
X 50 %
Time [s]
NO
X m
ola
r co
nc
en
trati
on
[p
pm
]
0 500 1000 1500 2000 2500 3000 3500 4000 4500 50000
100
200
300
400
500
600
700
Inle
t T
em
pe
ratu
re [
°C]
Bench - inlet
Bench - outlet
Model - outlet
Temperature
0 200 400 600 800 1000 1200 1400 16000
50
100
150
200
250
300
350
SGB test - DeNOx - Tinlet 275 °C / NO2/NO
X 100 %
Time [s]
NO
X m
ola
r co
nc
en
trati
on
[p
pm
]
0 200 400 600 800 1000 1200 1400 16000
100
200
300
400
500
600
700
Inle
t T
em
pe
ratu
re [
°C]
Bench - inlet
Bench - outlet
Model - outlet
Temperature
10
NO2 SCR reaction calibration:
4 NH3-Si + 3 NO2 5,5 N2 + 6 H2O + 4 Si
𝒓𝑵𝑶𝟐 = 𝒌𝑵𝑶𝟐 × 𝒆−
𝑬𝑵𝑶𝟐𝑹×𝑻𝒔 × 𝑵𝑶𝟐 × 𝜽𝑵𝑯𝟑
calibration is done on DeNOx SGB test with an upstream NO2/NOX ratio of 100 %
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Simon Dosda – Hydrothermal aging modeling for SCR catalysts – 2015 CLEERS WORKSHOP
150 200 250 300 350 400 450 500 5500
10
20
30
40
50
60
70
80
90
100
Inlet temperature [°C]
NO
x c
um
ula
tiv
e e
ffic
ien
cy [
%]
DeNOx efficiency - inlet NO2/NO
X ratio 100 %
Bench
Model
150 200 250 300 350 400 450 500 550 6000
10
20
30
40
50
60
70
80
90
100
Inlet temperature [°C]
NO
x c
um
ula
tiv
e e
ffic
ien
cy [
%]
DeNOx efficiency - inlet NO2/NO
X ratio 0 %
Bench
Model
150 200 250 300 350 400 450 500 5500
10
20
30
40
50
60
70
80
90
100
Inlet temperature [°C]
NO
x c
um
ula
tiv
e e
ffic
ien
cy [
%]
DeNOx efficiency - inlet NO2/NO
X ratio 50 %
Bench
Model
SCR model calibration for DeNOx reaction on SGB test
Ammonia oxidation reaction calibration:
4 NH3-Si + 3 O2 2 N2 + 6 H2O + 4 Si
𝒓𝑵𝑯𝟑𝒐𝒙 = 𝒌𝑵𝑯𝟑𝒐𝒙 × 𝒆−
𝑬𝑵𝑯𝟑𝒐𝒙𝑹×𝑻𝒔 × 𝑶𝟐 × 𝜽𝑵𝑯𝟑
calibration is done on DeNOx SGB test with an high upstream temperature
Standard SCR Fast SCR NO2 SCR
This calibration allows to obtain consistent results on the overall test data
0 500 1000 1500 2000 2500 30000
50
100
150
200
250
300
350
SGB test - DeNOx - Tinlet 555 °C / NO2/NO
X 0 %
Time [s]
NO
X m
ola
r co
nc
en
trati
on
[p
pm
]
0 500 1000 1500 2000 2500 30000
100
200
300
400
500
600
700
Inle
t T
em
pe
ratu
re [
°C]
Bench - inlet
Bench - outlet
Model - outlet
Temperature
11
© 2
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Simon Dosda – Hydrothermal aging modeling for SCR catalysts – 2015 CLEERS WORKSHOP
Approach: from fresh to aged SCR model
1 - Fresh SCR model set up and validation:
a - SCR model is calibrated on specific Synthetic Gas Bench tests
b - SCR model is integrated in a complete exhaust line simulator and validated on chassis dynamometer on test cycles
2 - Aging model set up from SGB tests for various aging conditions
3 - Aging model validation on dyno on test cycles using an aged SCR
12
1 - Fresh SCR model
2 - Hydrothermal aging model SGB data
3 - Aged SCR model validation
dyno cycle data
a - Calibration SGB data
b - Validation dyno cycle data
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Simon Dosda – Hydrothermal aging modeling for SCR catalysts – 2015 CLEERS WORKSHOP
Exhaust line model presentation
LMS Amesim model of a complete exhaust line composed of a DOC, a DPF and a SCR using IFP-Exhaust library coupled with a Simulink control platform
Upgrade from SGB models:
convective and radiative heat transfer modeled
light adjustment of catalysts calibration
13
chassis dynamometer bench – DOC + DPF + SCR
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Simon Dosda – Hydrothermal aging modeling for SCR catalysts – 2015 CLEERS WORKSHOP
0 200 400 600 800 1000 12000
50
100
150
200
250
300
Time [s]
NO
X m
ola
r co
nc
en
trati
on
[p
pm
] NEDC cycle
Bench - Inlet SCR
Bench - Outlet SCR
Model - Outlet SCR
0 200 400 600 800 1000 12000
200
400
600
800
1000
1200
1400
1600
Time [s]
NO
X c
um
ula
tiv
e m
as
s f
low
[m
g]
Bench - Inlet SCR
Bench - Outlet SCR
Model - Outlet SCR
Fresh SCR cycle simulation results on NEDC cycle
NOX reduction is well represented by the model
Almost no NH3 slip on this cycle with a fresh SCR
14
0 200 400 600 800 1000 12000
10
20
30
40
50
60
70
Time [s]
NH
3 m
ola
r co
nc
en
trati
on
[p
pm
]
NEDC cycle
Bench - Inlet SCR / 100
Bench - Outlet SCR
Model - Outlet SCR
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Simon Dosda – Hydrothermal aging modeling for SCR catalysts – 2015 CLEERS WORKSHOP
Approach: from fresh to aged SCR model
1 - Fresh SCR model set up and validation:
a - SCR model is calibrated on specific Synthetic Gas Bench tests
b - SCR model is integrated in a complete exhaust line simulator and validated on chassis dynamometer on test cycles
2 - Aging model set up from SGB tests for various aging conditions
3 - Aging model validation on dyno on test cycles using an aged SCR
15
1 - fresh SCR model
2 - Hydrothermal aging model SGB data
3 - Aged SCR model validation
dyno cycle data
a - Calibration SGB data
b - Validation dyno cycle data
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Simon Dosda – Hydrothermal aging modeling for SCR catalysts – 2015 CLEERS WORKSHOP
Hydrothermal aging effects on SCR catalyst : Cu-Zeolite
Catalyst changes with aging:
at low aging, copper migrates from exchanged positions to form copper oxide aggregates in the zeolite porosity
during this phase, copper in exchanged positions protects the zeolite structure against dealumination
with increasing aging, copper is completely removed from exchanged positions and dealumination occurs.
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Ref. « Hydrothermal aging effects on Cu-zeolite NH3-SCR catalyst » M. Valdez Lancinha Pereira, A. Nicolle, D. Berthout, IFPEN doi:10.1016/j.cattod.2015.03.027
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Simon Dosda – Hydrothermal aging modeling for SCR catalysts – 2015 CLEERS WORKSHOP
Hydrothermal aging effects on SCR catalyst : Cu-Zeolite
Aging model description:
loss of copper and aluminum ions contributes to a loss of catalytic sites: modeled by a coefficient on active surface and on NH3 capacities
𝑺𝒂𝒄𝒕𝒊𝒗𝒆𝒂𝒈𝒆𝒅 = 𝑪𝒐𝒆𝒇𝒇𝑪𝒖 × 𝑺𝒂𝒄𝒕𝒊𝒗𝒆 𝒇𝒓𝒆𝒔𝒉
𝛀𝑵𝑯𝟑𝒔𝒊𝒕𝒆𝟏𝒂𝒈𝒆𝒅 = 𝑪𝒐𝒆𝒇𝒇𝒔𝒊𝒕𝒆𝟏 × 𝛀𝑵𝑯𝟑𝒔𝒊𝒕𝒆𝟏 𝒇𝒓𝒆𝒔𝒉
𝛀𝑵𝑯𝟑𝒔𝒊𝒕𝒆𝟐𝒂𝒈𝒆𝒅 = 𝑪𝒐𝒆𝒇𝒇𝒔𝒊𝒕𝒆𝟐 × 𝛀𝑵𝑯𝟑𝒔𝒊𝒕𝒆𝟐𝒇𝒓𝒆𝒔𝒉
17
CuO aggregates promote NH3 oxidation: modeled by a coefficient on NH3 oxidation activation energy
𝒓𝑵𝑯𝟑𝒐𝒙 = 𝒌𝑵𝑯𝟑𝒐𝒙 × 𝒆−
𝑪𝒐𝒆𝒇𝒇𝑪𝒖𝑶
×𝑬𝑵𝑯𝟑𝒐𝒙𝑹×𝑻𝒔 × 𝑶𝟐 × 𝜽𝑵𝑯𝟑
no other changes in the calibration of the kinetic constants (kj, Eaj) determined on the fresh sample
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Simon Dosda – Hydrothermal aging modeling for SCR catalysts – 2015 CLEERS WORKSHOP
Aging impact set up for NH3 storage - Reactor scale
NH3 storage capacity reduction with aging is observed on SGB NH3 TPD tests
hydrothermal impact on NH3 capacity is higher on “low temperatures” NH3 storage sites
Desorption reaction rate reduction due to active surface reduction with hydrothermal aging temperature is well modeled
18
0
10
20
30
40
50
60
70
80
90
100
active surface NH3 capacity site 1 NH3 capacity site 2co
rrec
tive
co
effi
cien
t [%
]
Parameters variation
5h 800°C 5h 900°C 5h 1000°C
250 300 350 400 450 500 550 6000
50
100
150
200
250
Temperature [°C]
NH
3 m
ola
r co
ncen
trati
on
at
SC
R o
utl
et
[pp
m]
SCR aging impact on NH3 slip - Tinlet 225 °C
Bench - 5h 800°C
Model - 5h 800°C
Bench - 5h 900°C
Model - 5h 900°C
Bench - 5h 1000°C
Model - 5h 1000°C
SGB NH3 TPD tests
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Simon Dosda – Hydrothermal aging modeling for SCR catalysts – 2015 CLEERS WORKSHOP
Aging impact set up for DeNOx reaction - Reactor scale
At low hydrothermal aging temperature, main aging impact is a loss of catalyst efficiency at high temperature due on NH3 oxidation
impact of CuO aggregates
DeNOx reactions rates reduction is well represented by the reduction of the active surface in the model
19
0
20
40
60
80
100
120
active surface NH3 oxidation activation energy
corr
ect
ive
co
eff
icie
nt
[%]
Parameters variation
5h 800°C 5h 850°C 5h 900°C 5h 1000°C
100 150 200 250 300 350 400 450 500 5500
10
20
30
40
50
60
70
80
90
100
Temperature [°C]
SC
R D
eN
Ox e
ffic
ien
cy [
%]
SCR aging impact on DeNOx efficiency
Bench - 5h 800°C
Model - 5h 800°C
Bench - 5h 850°C
Model - 5h 850°C
Bench - 5h 900°C
Model - 5h 900°C
Bench - 5h 1000°C
Model - 5h 1000°C
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Simon Dosda – Hydrothermal aging modeling for SCR catalysts – 2015 CLEERS WORKSHOP
Approach: from fresh to aged SCR model
1 - Fresh SCR model set up and validation:
a - SCR model is calibrated on specific Synthetic Gas Bench tests
b - SCR model is integrated in a complete exhaust line simulator and validated on chassis dynamometer on test cycles
2 - Aging model set up from SGB tests for various aging conditions
3 - Aging model validation on dyno on test cycles using an aged SCR
20
1 - fresh SCR model
2 - Hydrothermal aging model SGB data
3 - Aged SCR model validation
dyno cycle data
a - Calibration SGB data
b - Validation dyno cycle data
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Simon Dosda – Hydrothermal aging modeling for SCR catalysts – 2015 CLEERS WORKSHOP
5h 1000°C aged SCR cycle simulation results - NOx
NEDC cycle is realized with an aged SCR
hydrothermal aging of 5h at 1 000°C
Coefficients from previous aging model are used:
Active surface: 2 %
NH3 capacity of site 1: 0,5 %
NH3 capacity of site 2: 1 %
NH3 oxidation activation energy: 85 %
Impact on DeNOx efficiency is well modeled
21
0 200 400 600 800 1000 12000
50
100
150
200
250
Time [s]
NO
X m
ola
r co
nc
en
trati
on
[p
pm
] NEDC cycle
Bench - Inlet SCR
Bench - Outlet SCR
Model - Outlet SCR
0 200 400 600 800 1000 12000
500
1000
1500
2000
2500
3000
Time [s]
NO
X c
um
ula
tiv
e m
as
s f
low
[m
g]
Bench - Inlet SCR
Bench - Outlet SCR
Model - Outlet SCR
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Simon Dosda – Hydrothermal aging modeling for SCR catalysts – 2015 CLEERS WORKSHOP
5h 1000°C aged SCR cycle simulation results - NH3
Impact on NH3 slip is well modeled : right timing and level of release
While NH3 slip for the fresh SCR was almost inexistent, more than half of NH3 injected quantity is released in the atmosphere for the aged SCR
Injection strategy can be optimized
22
0 200 400 600 800 1000 12000
500
1000
1500
Time [s]
NH
3 m
ola
r co
ncen
trati
on
[p
pm
]
NEDC cycle
Bench - Inlet SCR
Bench - Outlet SCR
Model - Outlet SCR
0 200 400 600 800 1000 12000
100
200
300
400
500
600
700
Temps [s]
NH
3 c
um
ula
tive m
ass f
low
[m
g]
Bench - Inlet SCR
Bench - Outlet SCR
Model - Outlet SCR
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Simon Dosda – Hydrothermal aging modeling for SCR catalysts – 2015 CLEERS WORKSHOP
Summary
Simple hydrothermal aging model with reduced parameterization:
one coefficient for active surface reduction
two coefficients for NH3 storage capacities, close to active surface
coefficient
one coefficient for NH3 oxidation activation energy
Need only SGB data
Consistency in results on NOX and NH3
Efficient methodology to model SCR aging impact from a fresh SCR
calibration
This hydrothermal aging model will be integrated in IFP-Exhaust
library for the next LMS Amesim release
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© 2
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IF
P E
nerg
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Simon Dosda – Hydrothermal aging modeling for SCR catalysts – 2015 CLEERS WORKSHOP
Renewable energies | Eco-friendly production | Innovative transport | Eco-efficient processes | Sustainable resources
www.ifpenergiesnouvelles.com
For further questions, please contact: Simon Dosda [email protected] Engine and Vehicle Modeling Department IFP Energies nouvelles 1 et 4 avenue de Bois-Préau 92852 Rueil-Malmaison Cedex - France
© 2
013 -
IF
P E
nerg
ies n
ouvelle
s
Simon Dosda – Hydrothermal aging modeling for SCR catalysts – 2015 CLEERS WORKSHOP
Back up: IFP-Exhaust Library
Heat transfer (free and forced convection)
Pneumatic flow (pipes, orifices, volumes.)
Sensors and Sources (temperature, pressure,
species)
Catalysts and Filters (DOC, DPF,LNT,SCR, SCR-F & 3WC)
Library dedicated to the after-treatment devices modeling
MiL, SiL and HiL capabilities