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Oil & Gas Science and Technology Rev. IFP Energies nouvelles, Vol. 66 (2011), No. 4, pp. 655-665
Copyright 2011, IFP Energies nouvelles
DOI: 10.2516/ogst/2011104
IFP Energies nouvelles International Conference
Rencontres Scientifiques dIFP Energies nouvelles
E-COSM'09 - IFAC Workshop on Engine and Powertrain Control, Simulation and Modeling
E-COSM'09 - Colloque IFAC sur le contrle, la simulation et la modlisation des moteurs et groupes motopropulseurs
Rsum Commande des systmes de RCS lure destins aux applications Diesel US Cet
article a pour objet de qualifier les dfis en matire de commande des systmes de rduction catalytique
slective (RCS) dans une solution base dure, pour la conversion des NOx au sein de groupes
motopropulseurs Diesel. Nous montrons limportance de la matrise du stockage dammoniac ainsi que
les difficults lestimer face aux incertitudes du systme. Les dynamiques de stockage lentes du
catalyseur de RCS savrent constituer un facteur de limitation majeur quant aux performances des
systmes de RCS au cours dun fonctionnement transitoire. Enfin, nous montrons leffet de lincertitude
des capteurs sur les performances du systme et comment les capteurs de NOx peuvent tre utiliss en
association avec une corrlation dentre pour distinguer une dviation de NOx dun glissement
dammoniac.
Abstract Control of Urea SCR Systems for US Diesel Applications This paper sets out to qualify
challenges in the control of urea selective catalytic reduction systems for NOx conversion in Diesel
powertrains. We show the importance of ammonia storage control, and the difficulties in estimating it in
the face of system uncertainties. The slow storage dynamics of the SCR catalyst are shown to be a major
limiting factor on the performance of SCR systems in transient operation. Lastly we show the effect of
sensor uncertainty on system performance and how NOx sensors can be used in conjunction with input
correlation to distinguish NOx slip from ammonia slip.
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656 Oil & Gas Science and Technology Rev. IFP Energies nouvelles, Vol. 66 (2011), No. 4
M van Nieuwstadt and D Upadhyay / Control of Urea SCR Systems for US Diesel Applications 657
4 NH 3 + 4 NO + O 2 4 N 2 + 6 H 2 O
Figure 2 2 NH 3 + NO + NO 2 2 N 2 + 3H 2 O (2)
Heavy duty diesel exhaust layout. 8 NH 3 + 6 NO 2 7 N 2 + 12 H 2 O
658 Oil & Gas Science and Technology Rev. IFP Energies nouvelles, Vol. 66 (2011), No. 4
2.0
3.1 Ammonia Storage
1.8 NH3 storage capacity, 75 ppm
NOx conversion on SCR catalysts is to a large degree determined 1.6 NH3 storage capacity, 350 ppm
by the amount of stored ammonia, especially at low tempera-
tures, see Figure 4. Figure 5 shows that SCR catalysts can 1.4
store an enormous amount of ammonia. While we can control 1.2
the increase in stored ammonia by injection of urea, we have 1.0
no direct control action to decrease stored ammonia.
0.8
Ammonia can only be released from the SCR by oxidation,
thermal desorption or reaction with NOx. Oxidation cannot 0.6
be directly controlled, thermal desorption results in large 0.4
ammonia concentrations of the tailpipe exhaust gas, and with
0.2
feedgas NOx concentrations typical of 2010 diesel applica-
tions, it is hard to remove ammonia at high rates. A typical 0
100 150 200 250 300 350 400 450 500 550
feedgas NOx number is on the order of 0.5 to 1.0 g/mile. Temperature (C)
Typical ammonia storage is on the order of 1 g/L, so for a 10 Figure 5
liter catalyst, total ammonia stored is 10 grams. Assuming Ammonia storage in g/L as a function of temperature, for
the standard reaction in Equation (2), 10 grams of ammonia different gas phase ammonia concentrations.
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M van Nieuwstadt and D Upadhyay / Control of Urea SCR Systems for US Diesel Applications 659
can store more ammonia for higher gas phase ammonia con- 25
centrations. Figure 4 shows that NOx conversion is to a
NOx pre SCR1 (g)
large degree determined by ammonia storage, especially at
20 NOx post SCR1 (g)
lower temperatures, and that NOx conversion increases to a
lesser degree with increasing ratio of gas phase ammonia NOx post SCR2 (g)
to NOx. 15
0
NOx conversion and NH3 slip as a fcn of NH3 storage (g/L) 0 200 400 600 800 1000 1200 1400 1600 1800
100 Times (s)
80 Eff. after SCR1 (%) Figure 8
Eff. after SCR2 (%)
60 Integrated NOx mass before, between and after the 2 SCR
40 bricks from Figure 3. Initial NH3 storage is 2.18 g/L.
20
0
0.2 0.3 0.4 0.5 0.6 0.7 0.8
200
Table 1 summarizes the trade off between NOx conversion
Max. NH3 slip after SCR1 (ppm)
and ammonia slip for the strategies considered so far.
150
Max. NH3 slip after SCR2 (ppm)
100 TABLE 1
NOx conversion and ammonia slip for different urea injection strategies
50
Strategy Initial storage No. conversion NH3 slip
0
0.2 0.3 0.4 0.5 0.6 0.7 0.8 g/L pct ppm
NH3 stored (g/L)
Figure 6 No urea injection 0.6 62 75
NOx conversion and ammonia slip over an EPA75 cycle, for FF, low storage 0.08 88 25
different initial storage levels, with 0 urea injection during
FF, high storage 2.18 97 5 981
the cycle.
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660 Oil & Gas Science and Technology Rev. IFP Energies nouvelles, Vol. 66 (2011), No. 4
6 000 W839 Fresh DOC/SCR/DPF, VERL Warm 1FTP74, 07Dec2006 - NH3 Storage Control
3.0
NH3 in (ppm) urd_NH3_mstor_des_scr
5 000
NH3 SCR1 out (ppm) 2.5 urd_calc_NH3_stor_scr_gm
NH3 SCR2 out (ppm)
4 000 2.0
3 000 1.5
g
2 000 1.0
1 000 0.5
0 0
0 200 400 600 800 1000 1200 1400 1600 1800 0 200 400 600 800 1 000 1 200 1 400
Times (s) Times (s)
Figure 9 Figure 10
NH3 concentrations before, between and after the 2 SCR Performance of an ammonia storage controller. Experimental
bricks from Figure 3, corresponding to the NOx traces in data. The red trace is desired storage, the blue line is achieved
Figure 8. storage.
3.3 Ammonia Storage Control storage level to within around 0.1 g/L. This controller
achieves between 92 and 98% conversion efficiency on
In Upadhyay (2006) we presented the following simplified repeated hot FTP74 cycles.
control oriented model of an SCR catalyst. The three states To study the issues involved in ammonia storage we
represent gas phase NOx concentration, ammonia storage and simulate a storage controller on our simulation depicted in
gas phase ammonia concentration. The reaction rates Rxxx Figure 3. A simple PI controller on ammonia storage is added
(xxx = ADS, DES, OX, RED) follow an Arrhenius equation to the stoichometric feed forward controller of Section 3.2. In
with a strong temperature dependence, where ADS stands this simulation we control to the average ammonia storage of
for adsorption, DES stands for desorption, OX stands for the different longitudinal slices in the first brick. Clearly, we
oxidation, RED stands for NOx conversion. The control cannot measure this quantity in a real system, but the assump-
input U is the ammonia from injected urea, the feedgas tion is useful to point out some fundamental limitations of
NOx concentration is disturbance d: storage control. Figure 11 shows that even if we know the
See Equation (3) ammonia storage level, the slow bandwidth of the storage
To give and example of storage control, Figure 10 shows dynamics force a oscillation around the storage target, with a
the experimental performance of an ammonia storage controller period of around 20 minutes. This behaviour is qualitatively
based on this model, on a 5 liter catalyst over an EPA75 very similar to the experimental data in Figure 10.
cycle. After the initial transient resulting from a start at zero It should be noted here that the stored ammonia is a
ammonia storage, the controller can control the ammonia calculated quantity, and as such the feed forward could be
C R
NO ( RRED + F ) + OX F
C NO Vcat Vcat 0
R Vcat
= ( RADS CNH 3 + RDES + RRED CNO + ROX ) + ADS CNH 3 + 0 U + 0 d (3)
SC SC
CNH 3 C F 0
R
NH 3
Vcat
( RADS (1 ) + F ) + V
DES Vcat
cat
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M van Nieuwstadt and D Upadhyay / Control of Urea SCR Systems for US Diesel Applications 661
C R
NO ( RRED + F ) + OX F
C Vcat Vcat
NO 0
Vcat 0
= R C + R + R C + R + RADS C + 0
(
ADS NH 3 DES RED NO OX
SC
NH 3 )
U + 0 d + K
(
CNH 3 CNH 3 ) (4)
C SC
F 0 0
NH 3
CNH 3
Vcat
V
cat
( R
)
RADS (1 ) + F + DES
V cat
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662 Oil & Gas Science and Technology Rev. IFP Energies nouvelles, Vol. 66 (2011), No. 4
500 1.5
300 0
0 200 400 600 800 1 000 1 200 1 400 1 600 1 800
250
200 800
50 200
0 0
0 0.5 1.0 1.5 2.0 2.5 0 200 400 600 800 1 000 1 200 1 400 1 600 1 800
Stored NH3 (g/L) Times (s)
Figure 13
Figure 14
Simplified ammonia slip model for single state observer. This
Estimated and real NH3 storage. Predicted and measured NH3
graph depicts the function f(.,.) in Equation (5).
slip after the first brick. Around 1500 s, the feedback action
results in significant NH3 slip and the observer can catch up
with the real storage.
M van Nieuwstadt and D Upadhyay / Control of Urea SCR Systems for US Diesel Applications 663
Des storage (g/L) Est. storage (g/L) SCR1 avg storage (g/L) result in zero NOx conversion and ammonia slip for larger
1.0 additive errors.
0.8
The above account points out a fundamental limitation in
0.6
observer design for this system. While we can take action to
0.4 achieve robustness against multiplicative uncertainty, both in
0.2 modelling and sensor, it is hard to achieve robustness against
0 additive uncertainty, both in modelling and sensor, especially
0 200 400 600 800 1 000 1 200 1 400 1 600 1 800
if this uncertainty corresponds to a magnitude of the desired
level of ammonia storage.
150
Predicted NH3 slip Measured NH3 slip
post SCR1 (ppm) post SCR1 (ppm)
100
4 NOx SENSORS
50
The previous section discussed the use of an ammonia sensor
0 for observation of the ammonia storage. Since ammonia
0 200 400 600 800 1 000 1 200 1 400 1 600 1 800
Times (s) sensors are not available for large volume applications in
2010, current US diesel applications need to rely on a NOx
Figure 15
sensor. In this section we will discuss some tools to use a
Top: estimated and real NH3 storage. Bottom: predicted and
NOx sensor to detect ammonia slip. Since NOx sensors are
measured NH3 slip after the first brick. Compared to Figure
14, this simulation uses lower gain, and overestimates the heated to above 600C, any ammonia in the exhaust gas will
ammonia slip. be oxidized on the sensor element, and converted to NOx.
Hence NOx sensors are also sensitive to ammonia. The sensi-
tivity depends on the protection tube design, the exhaust tem-
NOx conversion and NH3 slip, as a fcn of NH3 sensor gain error
perature, and the microstructure of the diffusion barrier in the
100
sensor. Since the NOx sensor is not designed to sense ammo-
80 nia, the sensitivity to ammonia shows a large variability from
NOx conv., SCR2 (pct)
60 part to part and over life time.
NH3 slip, SCR2 (ppm)
40 The NOx sensor is sensitive to both NO and NO2, with
20 different gains. NO2 is a larger molecule, hence experiences a
0 larger resistance to transport through the diffusion barrier.
0.7 0.8 0.9 1.0 1.1 1.2 1.3 1.4 Additionally NO2 accounts for two oxygen atoms once it is
Gain
Figure 16 dissociated in the sensing chamber. Depending on the sensor
details the sensitivity to NO2 can be between 70% and 130%
NO x conversion and ammonia slip as a function of
multiplicative sensor error. of that to NO.
NOx conversion and NH3 slip, as a fcn of NH3 sensor offset error 4.1 Measuring Ammonia with a NOx Sensor
100
80 No conv., SCR2 (pct)
Since the NOx sensor is sensitive to both ammonia and NOx,
x
60 NH3 slip, SCR2 (ppm) one cannot a priori determine which combination of these
40 species causes a nonzero sensor reading. We propose a corre-
20 lation scheme with the urea injection input to ascertain which
0 species is registered, (Van Nieuwstadt, 2003). Suppose we
-15 -10 -5 0 5 10
Offset set are running in steady state conditions, where the SCR cata-
Figure 17 lyst is in a regime of good NOx conversion. If we increase the
NOx conversion and ammonia slip as a function of additive urea injection and see a decrease in output, we can infer that
sensor error. we were sensing NOx, since the increased ammonia in the
feedgas reacted with NOx and reduced the sensor reading. If
on the other hand we see an increase in sensor output when
we increase urea input, we can infer that we were sensing
A positive additive error causes the observer to overestimate ammonia, since the extra ammonia in the feedgas passed
ammonia storage, and hence the controller to reduce urea through the SCR and was sensed by the NOx sensor. By
injection. Specifically, if the sensor bias is greater than the correlating the change in input uhp to the change in output yhp,
ammonia slip corresponding to the desired storage level, the we can construct a metric M that is positive when we measure
storage controller will completely turn off urea injection and ammonia, and negative when we measure NOx.
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M van Nieuwstadt and D Upadhyay / Control of Urea SCR Systems for US Diesel Applications 665
ACKNOWLEDGMENTS
We thank P. Laing, J. Kim and the rest of their team for the
development of the SCR model used for all simulations in
this paper. We thank C. Lambert, G. Cavataio and the rest of
their team for the gas bench data on SCR catalysts. We thank
A. Brahma for the synthesis of the two-brick model. Finally, Final manuscript received in February 2011
E. Serban provided engine experimental data used in this paper. Published online in September 2011