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2008-01-2487
Michael B. Viola
General Motors R&D Center
Copyright © 2008 GM Global Technology Operations, Inc. Published by SAE International with permission.
ABSTRACT
Federal Tier 2 Emissions Bins
The two most common NOx reducing technologies, in an Beyond MY 2008
oxygen abundant exhaust stream, are urea selective
Full Useful-Life FTP Stds. Light-Duty Intermediate FTPStds.
catalytic reduction urea-SCR and lean NOx trap (LNT) in g/mi @ 120K miles in g/mi @ 50K miles
catalysts. Each technology has advantages and BIN NOx NMOG CO HCHO PM NOx NMOGCO HCHO
disadvantages. Another selective catalytic reduction 0.20 0.125 4.2 0.018 0.02 Opportunity for
8 0.14 0.100 3.4 0.015
Hi-NOx Technology
7 0.15 0.090 4.2 0.018 0.02 0.11 0.075 3.4 0.015
(SCR) catalyst that uses hydrocarbons (HC-SCR), 6 0.10 0.090 4.2 0.018 0.01 0.08 0.075 3.4 0.015
specifically diesel fuel, as the reductant to reduce NOx 5 0.07 0.090 4.2 0.018 0.01 0.05 0.075 3.4 0.015 Tier 2 Fleet Average
( Same as LEV2 )
4 0.04 0.070 2.1 0.011 0.01 also qualifies for ULEV2
emissions was investigated. This catalyst is a result of a 3 0.03 0.055 2.1 0.011 0.01
for Cars & Trucks
up to 8500 GVWR
high throughput discovery project and conducted in 2 0.02 0.010 2.1 0.004 0.01 & MDPV > 8500
1 0.00 0.000 0.0 0.000 0.00
cooperation with BASF, Accelrys and funded by the
Department of Energy (DOE.) Several full size 5.0L
monolith catalysts were made and evaluated using a V6
turbo charged diesel engine connected to a dynamometer
running light-duty transient test cycles. The NOx efficiency
on the HWYFET and US06 tests were measured to be Figure 1. Federal Tier 2 Emissions Standards.
92% and 76% respectively. The FTP was 60% on a
weighted basis. An alternative technology to reduce engine-out NOx
emissions is to use hydrocarbons along with a selective
catalytic reduction catalyst (HC-SCR) to reduce NOx
INTRODUCTION emissions. Schmieg, Lee and Oh found that using a
simulated diesel fuel made up of 67% n-dodecane and
There is greater interest in diesel engines today due to 33% m-xylene, both on a volume basis, as the reductant
their advantage in fuel efficiency and lower carbon dioxide over a HC-SCR catalyst reduced NOx emissions by as
(CO2) emissions compared to gasoline vehicles. Also, much as 75% in laboratory reactor work (2). Also, GM
rising fuel costs are an additional incentive to investigate working with BASF and Accelrys on a high throughput
diesel engines especially in the North American market. discovery project funded by the department of energy
However, diesel powered vehicles will need to meet the (DOE) discovered a HC-SCR catalyst which showed
same stringent TIER II BIN 5 emissions standards, shown promise for reducing NOx emissions using simulated
in Figure 1, that gasoline vehicles are required to meet (1). diesel fuel as the reductant (3). Two catalyst samples
Typically urea-SCR and LNT catalysts have been used to were scaled up to 5.0L in size for transient testing in a test
reduce NOx emissions. Each system has advantages and cell.
disadvantages depending on the application. In order for a
urea-SCR system to be used an infrastructure is required, A 4.9L V6 turbo diesel engine connected to a test cell
currently not in place. Also, the eutectic point for a 32.5 dynamometer was used for testing. The highway fuel
wt% liquid urea solution is 11°F, so freezing is a problem economy test cycle (HWYFET), US06 cycle and federal
which would need to be solved. A drawback of the LNT test procedure 75 (FTP) were programmed to run in the
system is the high PGM utilization required resulting in a test cell. A HC-SCR catalyst system was installed and
cost penalty which can be quite high due to the volatile ultra low sulfur diesel fuel ULSD was used as the
PGM market. Additionally, due to the required LNT reductant and was injected into the exhaust upstream of
regenerations, providing a fuel rich air-to-fuel ratio (A/F) to the HC-SCR catalyst with a fuel injector. Emissions were
convert the NOx to N2 and water, there is also a fuel sampled at various locations throughout the aftertreatment
economy penalty. system and the NOx reduction efficiency was determined
on each test cycle.
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EXPERIMENTAL HC-INJ
TEX 2
NOx 2
TEX 1
Turbo NOx 1 MIXER HC-SCR
The engine used for testing was a 4.9L V6 turbo diesel HC-SCR
ENGINE DOC
engine essentially the same as the 6.6L V8 Duramax
engine with two less cylinders. The engine was connected
to a dynamometer in a test cell controlled by an ADAPT 37 in
General Motors Research and Development Center HIGHWAY FUEL ECONOMY TEST CYCLE RESULTS -
(GMR&D) working with BASF and Accelrys on a high Testing on the HWYFET with two catalyst bricks 10.14L of
throughput discovery project funded by the department of catalyst resulted in 40% NOx efficiency, 68% with 15.21L
energy (DOE) discovered an SCR catalyst which showed and 92% after 20.28L as shown in Figure 3. The tailpipe
promise for reducing NOx emissions using simulated NOx emissions with 20.28L of HC-SCR catalyst resulted in
diesel fuel as the reductant. The catalysts were scaled up 24 mg/mile. The HWYFET emissions standard for Tier 2
to 7.5 inch in diameter and 7.00 inch long resulting in BIN 5 on a LDT3 weight class vehicle certified to 120,000
5.07L in catalyst volume. A catalyst containing 2 wt% miles is 70 mg/mile. This indicates that with 20L of catalyst
Ag/Al2O3 with a washcoat loading of 2.7 g/in3 was selected hydro thermally aged, Tier 2 BIN 5 NOx emissions on the
for testing. A 400 cells per square inch (CPSI) cordierite HWYFET can be achieved. With 15L of catalyst 97
monolith substrate which was hydro thermally aged (HTA) mg/mile was measured and does not meet the standard.
in air and 10% water at 650ºC for 16 hours was used. The The instantaneous NOx efficiency shown in brown at the
temperature of 650ºC correlates to DPF regeneration top of the graph is after 20.28L and remains quite high
temperatures on a vehicle. The time of 16 hrs is based on throughout the cycle and only dropped under heavy
some internal catalyst aging work conducted at GMR&D accelerations. The fuel economy penalty on the cycle was
Center. There were four bricks in the system. Two bricks determined to be 2.4%. Also, note the second y-axis
canned together in each can with space between the shows negative numbers on all graphs indicating vehicle
bricks for emissions sampling. Sampling between and speed in MPH. The MPH trace was offset in order to plot
after catalyst bricks correlates to different space velocities. MPH on the same graph as emissions without any of the
The aftertreatment system also consisted of a diesel curves interfering with each other. This enables the reader
oxidation catalyst upstream of the SCR catalyst and the to assess emissions or temperatures anywhere on the test
system is shown in Figure 2. cycle.
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6 120 100
110 95
100 90
5 90 10.14L
85
80 80 15.21L
70
3
CUM NOX 20L 30 60
600 10
The data indicates that as long as the space velocity is 400
0
-10
kept below 10,000 1/hr the NOx performance remains 200 -20
-30
high. Additional catalyst volume may allow more time for 0
-40
-200
reactions to occur in turn increasing NOx efficiency. The -50
-400 -60
NOx efficiency more than doubles from 10L to 20L of -600 -70
-80
catalyst. The temperature is slightly lower for the rear -800 -90
bricks compared to the front and may be the reason. -1000 -100
800 900 1000 1100 1200 1300 1400 1500 1600
However, S. Schmieg (3) shows that space velocity plays Time Sec
275 250
concentration. It is clear that the lower the space velocity
vehicle speed (MPH), NOx eff. (%)
200
Exh. Flow
150 to drop off is reduced as more catalyst is added, or as
175 B1 B2 B1 B2
150 100 space velocity, is reduced. With 10L of catalyst the NOx
125
50
efficiency is only 50% on average with approximately 8.5%
100 T_SCR1_GAS_IN T_SCR1_BK1_FRONT T_SCR1_BK2_REAR T_SCR2_BK1_FRONT
oxygen compared to 6.8% oxygen with 15L of catalyst and
75 0
T_SCR2_BK2_REAR T_SCR2_GAS_OUT mph Total System NOX Eff
the NOx efficiency never drops below 55% even at 4.4%
50
25
-50
oxygen with 20L of catalyst.
0 -100
800 900 1000 1100 1200 1300 1400 1500 1600
Time Sec
100
95 10.14L NMOG standard of 0.4 g/mile for Tier 2 BIN 5 with a LDT3
90 15.21L
85 20.28L
vehicle. Since 0.149 g/mile of NOx is only 37.25% of the
80
75
0.4 NOx +NMOG standard this should be enough
70
65
compliance for adding in NMOG emissions and still meet
60 the standard.
NOx eff. (%)
55
50
45
40
35
10 100
30
9 90
25
8 80
20
7 70
15
10 6 60
5 50
Cumulative NOx g
O2% 2 20
20L HC-SCR 76%
1 10
0 0
-1 -10
Figure 7. HWYFET Impact of Oxygen Concentration. -2 -20
-3 -30
-4 -40
CUM EO NOx
-5 -50
CUM NOx 10L
-6 -60
CUM NOx 15L
US06 TEST CYCLE RESULTS - Testing was also -7
CUM NOx 20L
-70
-8 -80
conducted on the US06 test cycle with the same -9
mph
-90
Total System NOx eff
aftertreatment architecture. The US06 cycle resulted in -10
700 800 900 1000 1100 1200 1300 1400
-100
29% NOx efficiency with two catalyst bricks 10.14L, 56% Time Sec
250
completion as on the HWYFET. However, at high 225
Exh. Flow
B1 B2 B1 B2
150
200
temperatures like on the US06, reactions would be 175 100
expected to go to completion. The space velocity is so 150
50
125
much higher on the US06 cycle that the reactions may not 100
0
reach completion and results in lower overall cycle 75
50
efficiency. 25
-50
0 -100
700 800 900 1000 1100 1200 1300 1400
100
95 10.14L COLD START FTP TEST CYCLE RESULTS - The
90 15.21L
85
20.28L
catalysts were moved closer to the engine for faster light-
80
75 off on a cold start and both cans were put together to
70
65
60
better simulate 20L of catalyst in one can and minimum
NOx eff. (%)
55
50
temperature loss as shown in Figure 13. Since the
45
40 temperatures on a FTP are too low throughout the test for
35
30 the HC-SCR catalyst to operate, a heat strategy was
25
20 developed to heat the catalysts to a temperature greater
15
10
5
than 300°C. Temperatures on the HWYFET were on
0
average 310°C and provided 92% NOx reduction on the
0
00
00
00
00
00
00
00
00
00
00
00
00
00
00
00
00
00
,0
,0
,0
,0
,0
,0
,0
,0
,0
,0
,0
,0
,0
,0
,0
5,
10
15
20
25
30
35
40
45
50
55
60
65
70
75
80
85
Space Velocity 1/hr
same and with several idles on the FTP, where space
velocity is low and oxygen concentration is high, NOx
Figure 10. US06 Impact of Space Velocity on NOx
performance on the FTP cycle is expected to be very
Efficiency.
good.
100 TEX 2
95 10.14L HC-INJ NOx 2
TEX 1
90
15.21L Turbo NOx 1 MIXER
85
80 20.28L HC-SCR HC-SCR
75
70
ENGINE DOC
65
60
20 in
NOx eff. (%)
55
50
45
40
35
30
EMISSIONS EMISSIONS EMISSIONS EMISSIONS
25
20
15
Figure 13. Cold FTP Aftertreatment Architecture.
10
5
0
0 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25
O2%
The heat strategy used was post injection from the engine
which would develop an exothermic reaction over the
DOC to produce heat in the exhaust stream to heat the
Figure 11. US06 Impact of Oxygen Concentration on
HC-SCR catalyst to the desired temperature. Once the
NOx Efficiency.
exhaust gas temperature just upstream of the DOC
reached 190°C, post injection was started which occurred
5000 100 at 170 seconds into the test at the start of cycle two in the
90
4000 80
first bag of the FTP as shown in Figure 14. However, HC
70 injection for NOx reduction does not start until the exhaust
3000 60
50 gas temperature upstream of the HC-SCR catalyst
vehicle speed (MPH), NOx eff. (%)
2000 40
30
reaches 280°C which does not occur until 224 seconds
1000 20 into the test. Catalyst light-off of 50% for the HC-SCR
HC ppm C1
10
0 0 system of 20L occurred at 309 seconds into test which is
-10 near the end of cycle two. The FTP exhaust temperatures
-1000 -20
-30 and instantaneous NOx efficiency is shown in Figure 15.
-2000 -40
EO HC ppm -50
The catalyst temperatures with the heat strategy are
HC ppm 10L
-3000 HC ppm 15L -60 controlled to 290°C to 350°C from cycles two through 18.
HC ppm 20L -70
-4000 mph
Total System NOx eff
-80 The heat strategy is also used in bag 3 of the FTP, starting
-90
-5000 -100
at 1,975 seconds and turned off at 2,395 seconds.
700 800 900 1000 1100 1200 1300 1400 Temperatures in bag 3 reach almost 400°C due to the hot
Time Sec
restart after the soak. This was a first attempt at a heat
strategy and would require further development and
Figure 12. US06 Hydrocarbon Emissions. optimization.
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30 100
T_DOC_IN T_SCR1_GAS_IN T_SCR1_BK1_FRONT
28 90
T_SCR1_BK2_REAR T_SCR2_BK1_FRONT T_SCR2_BK2_REAR
T_SCR2_GAS_OUT mph Total System NOx eff 26 80
500 100 24 70
SCR1 SCR2 90 22 60
450 Flow
20 50
Cumulative NOx g
350 50 14 20
Figure 14. Cold FTP Bag 1 Heat Strategy. Total System NOx eff
mph
SV
100 16000
90
T_DOC_IN T_SCR1_GAS_IN T_SCR1_BK1_FRONT 80 14000
T_SCR1_BK2_REAR T_SCR2_BK1_FRONT T_SCR2_BK2_REAR
70
T_SCR2_GAS_OUT mph Total System NOx eff
500 100 60
12000
50
40 0
300 30 -10 6000
250 20 -20
Exhaust T C
10 -30
200 0 4000
-40
-10
150 -50
-20 2000
-60
100 -30
-70
SCR1 SCR2 -40
Flow -80 0
50 -50
DOC B1 B2 B1 B2 -90
-60
0 -70 -100 -2000
-80 0 200 400 600 800 1000 1200 1400 1600 1800 2000 2200 2400
-50
-90 Time Sec
-100 -100
0 200 400 600 800 1000 1200 1400 1600 1800 2000 2200 2400
Time Sec
Figure 17. Cold FTP Impact of Space Velocity on NOx
Efficiency.
Figure 15. Cold FTP Heat Strategy.
Total System NOx eff
mph
INLET SCR O2 %
100 22
The NOx efficiency on the cold start FTP on a weighted 90
20
80
basis was determined to be 60% and resulted in a fuel 70
18
60
economy penalty, for HC injection for NOx reduction only, 50
16
vehicle speed (MPH), NOx eff. (%)
-40
throughout the cycle is relatively high especially on idles -50
6
-60
where it is 98% or better. In Figure 17 the impact of space -70
4
The NOx efficiency is shown as a function of both space In the future, improvements need to be made in catalyst
velocity and oxygen concentration in Figures 19 and 20 formulation to reduce operating temperatures below 300°C
respectively. In both cases the data starts at the point of and to reduce catalyst volume. In addition, reduce
catalyst light-off, it does not include the first 308 seconds hydrocarbon slip past the HC-SCR catalyst to reduce or
of the FTP.
eliminate the need for a DOC downstream of the HC-SCR
catalyst.
100
95 20L HC-SCR
90
85
80 ACKNOWLEDGMENTS
75
70
65
60 The author would like to thank Steven J. Schmieg in the
NOx eff. (%)
55
50
Chemical and Environmental Science Laboratory for many
45
40
useful conversations while conducting tests. The author
35
30
thanks Edward E. Klusendorf in the Chemical and
25
20
Environmental Science Laboratory for developing the FTP,
15 HWYFET and US06 transient test cycles in the test cell.
10
5 The author would also like to thank Chris C. Crellin and
0
0 2,000 4,000 6,000 8,000 10,000 12,000 14,000 Dennis J. Upton in the Chemical and Environmental
Space Velocity 1/hr Data starts at Catalyst lightoff
Science Laboratory for conducting the tests and
maintaining the test cell. The author also thanks David B.
Figure 19. Cold FTP Space Velocity vs. NOx Efficiency. Brown and Michael Paratore, both from GM Powertrain,
for providing the diesel oxidation catalysts along with other
hardware needed for testing. The author also thanks
100 Michael Paratore for his help with the catalyst heating
95
90 strategy.
85
80
75
70
REFERENCES
65
60
NOx eff. (%)
CONTACT