Particle and metal emissions
of diesel and gasoline engines Are particle filters appropriate measures?
A. Ulrich1, A. Wichser1, A. Hess1, 2, N. Heeb1, L. Emmenegger1,
J.Czerwinski3, M. Kasper4, J. Mooney5, A. Mayer6
1Empa,
Swiss Federal Laboratories for Material Testing and Research, 8600 Dübendorf, Überlandstrasse 129, Switzerland
École Polytechnique Fédérale de Lausanne, Switzerland
3AFHB, Abgasprüfstelle Biel, Gwerdtstr. 5, CH – 2560 Nidau, Switzerland
4ME, Matter Aerosol AG, Bremgarterstr. 62, CH – 5610 Wohlen, Switzerland
5585 Colgate Ave Wyckoff, NJ, USA
6TTM, Fohrhölzlistrasse 14b, CH – 5443 Niederrohrdorf, Switzerland
2EPFL
Corrosponding author: [email protected]
Introduction
Not only diesel, but also gasoline fueled internal combustion engines can emit particulate matter.
The following figure compares different vehicle types in terms of particle number concentration
(PN). The studied vehicles are listed below:
1.
2.
3.
4.
5.
6.
7.
MPI gasoline = gasoline vehicle with multiport injection
DI gasoline = gasoline vehicle with direct injection
CNG = compressed natural gas vehicle
diesel = diesel vehicle without particle filter
DPF = diesel vehicle with diesel particle filter system (wall flow)
load = diesel vehicle with diesel particle filter system during the loading phase
reg = diesel vehicle with diesel particle filter system during regeneration phase
Particle Number PN [1/km]
1.E+14
1.E+13
PN increase
PN reduction
> 99 %
1.E+12
> 98 %
1.E+11
MPI
Gasoline
DI Gasoline
Diesel
Diesel/DPF Diesel/DPF
load
reg
CNG
Figure 1: Particle number concentration (PN) of different vehicle types (adopted from Empa Report
2007 (Novatlantis) “Emissionsvergleich verschiedener Antriebsarten in aktuellen
Personenwagen) [1]
The diesel vehicle equipped with particle filter system showed the lowest PN emissions which
represent a filtration efficiency of over 99 % in the loading and over 98 % during the regeneration
phase. Gasoline vehicles especially with direct injection show significantly higher PN emissions
than those with multiport injection.
Particle Number Concentration in PN/km
«Auch neue
Benziner brauchen
strenge Grenzwerte
- Testergebnisse:
Benzinmotoren mit
Direkteinspritzung
VCD + Umwelthilfe
PN Limit for
Diesel Euro 5
and Gasoline
Euro 6
Particle Mass Concentration in g/km
PN Limit for
Diesel Euro 5b
Figure 2: Particle number (PN) and particle mass concentration in emissions of two gasoline vehicles
adopted from VCD and Umwelthilfe Study „Auch neue Benziner brauchen strenge
Grenzwerte - Testergebnisse: Benzinmotoren mit Direkteinspritzung“ [2]
Also a recently published study from Verkehrsclub Deutschland VCD and Umwelthilfe described
similar observations for gasoline vehicles with direct injection and claimed stricter particle
number restrictions also for gasoline vehicles (Figure 2). They carried out tests using different
driving cycles.
A solid particle number emission limit of 6 × 1011 #/km becomes effective at the Euro 5b and 6
stage for all categories of diesel vehicles (compression injection) as well as for Euro 6 gasoline
vehicles (positive injection). All vehicles tested in the studies presented in figure 1 and 2
significantly exceeded these PN limits.
Previous studies shown, that ultra-fine particulate emissions often contain metal oxides, which can
originate from various sources such as engine wear, lubrication oil, fuel ashes, fuel additives or
coatings from exhaust gas after-treatment systems. The main possible sources are summarized in
the following table.
Tab. 1: Possible sources for metals
1. Abrasion from piston ring, cylinder liner, valve cams, valves, bearings
(e.g. Fe, Al, Cr, Ni, Cu, Pb ...)
=> abraded metal mass ca. 0.1 to 1 mg/km
2.
Lubrication oil: e.g. Zn: 0.1 – 0.2 %, Ca: 0.5 %,
B: 0.09 %. Mg: 0.002-0.004 %,...
old vehicles: up to 1 % oil of fuel consumption
3. Fuel: several metals in traces, heavy metals (Pb, Mn,)
have limits (e.g. in Germany BzBIG 1971: Pb <150 mg/kg fuel)
The metal content in most of the conventional on-road fuels is usually relatively low, whereas
lubrication oils often contain much higher metal concentrations. Engine wear metals occur in all
internal combustion engines. Metal compounds collected in lubrication oil can be re-entrained into
the cylinder and then oxidized during combustion. Some metals might be vaporized and re-nuclide
forming ultra-fine particles in a size range typically below 30 nm. These metal oxide particles can
be present in the exhaust aerosol either as free metal oxide particles or attached to larger soot
particles. The toxicological effect of nanoparticles was proved in several studies. Hence, these
nanoparticulate emissions need to be avoided. Full wall-flow particle filter systems are effective
measures to reduce particulate emissions and they are already well established in diesel engine
technology. These filter technology might be also beneficial especially for direct injection gasoline
engines.
Toxicological effects of nanoparticles
Particle emissions of diesel vehicles can cause acute and chronic harm at lung and cardiovascular
system. The biological impact depends on the particles' ability to defeat the human body defense.
Crucial factors are particle size and solubility. Almost insoluble particles are hazardous especially
in small size ranges. Toxicological studies have shown increased toxicity of nanoparticles
compared to micrometer particles of the same composition, which has raised concern about the
impact on human health. Nanoparticles can enter alveoli in the lungs, pass biological barriers
including placenta and blood–brain barrier, and enter cells. The high surface area and chemical
composition of the nanoparticles (NPs) play an important role in biological activity and toxicology,
but toxicology depends also on cell types. The binding of NPs to bacterial proteins can inhibit
enzymatic activity. Epidemiological studies on ultrafine particles have shown increased cancer risk
after long-term exposure of diesel vehicle drivers enhanced allergy tendency at traffic burdened
sites and enhanced risk of heart attack.[3-16]_ENREF_1
Figure 3 shows that particles < 10 μm can intrude deep into the lung. Particles smaller than
100 nm show a high deposition rate in the alveoli, which increase with decreasing particle
diameter. Tissue penetration from alveoli to the blood vessels, too, is highly dependent on particle
size. Therefore, the particle dosage should be weighted with this size influence.
Deposition
Rate
in %
deposition
rate [%]
Particle deposition rates in the respiratory tract
Metal Soot
100
100
oxides
total
80
80
54%
(15 nm)
60
60
48%
(10 nm)
40
40
nasal region
20%
(100 nm)
20
20
00
11
1010
tracheobronchial
region
alveolar region
100
100
1000
1000
10000
10000
particle diameter [nm]
Particle
Diameter in nm
Fig. 3: Deposition of inhaled particles in the alveoli. The main particle sizes are: Diesel soot about
100 nm; SI soot about 50 nm and metal oxides about 10-15 nm.
Experimental
The vehicle characteristics as well as the sampling procedures and analysis are displayed in the
following graphs and tables. Online particle analysis has been performed with SMPS. Size
fractionated chemical analysis of nanoparticles in vehicle emissions were carried out by sampling
with an electrical low pressure multi-stage impactor ELPI with subsequent acid digestion in a
microwave system and chemical analysis with plasma mass spectrometry ICPMS. Further details
can be found elsewhere.[16-27]
Fuel / Lube oil
Sampling
Parameter Methods
Fuel supply
Engine
Metals,
Sulphur,
Chlorine
ICP-MS,
ICP-OES,
XRF
CO
CO2
HC
NO
NOx
O2
Opacity
NDIR
NDIR
FID
CLD
CLD
Magnos
Opacity
Meter
Major components
T, p
catalytic
DPF
T, p
Particulate Matter
PM Number/
Surface
Air
Filter
Partial Dilution
Tunnel
NanoMet
Size
Distribution
SMPS
Mass
Gravimetry
Metals
ICP-MS
VOC
GC-FID
VOCOX
LC-UV/VIS
V
ELPI
Fig. 4:
Flow-proportional
Sampling
Constant Volume
Sampling CVS
Toxic trace components
V
Bag
Air
Impinger
PAH
Dioxin Train
V
Test and sampling setup
(A) for passenger cars and 2-wheelers
(B) for diesel engine tests
n-PAH
PCDD/F
}
GC-HR-MS
Tab. 2: Operation points for vehicle and diesel engine tests
ISO 8178/4 C1-cycle for construction site engines
5
Torque
0.10
Load
100 %
6
1
0.15
0.10
75 %
2
7
0.15
0.10
50 %
3
0.15
Idling
Intermediate
RPM
8
0.15
10 %
4
0.10
60 %
100 %
RPM
N. Heeb, EMPA Report 167985
Fig. 5:
Used Test cycle ISO 8178/4 C1
Tab. 3: Characteristics of lubrication oils for cars and 2-wheelers
Tab. 4: Lubrication oil 15 W/40 and fuel for Liebherr D934S and D914T diesel engine
Fig. 6: CVS Background: Lab air and CVS tunnel only
Results
The investigation within this study focused on the particle emissions. Gaseous emissions are not
reported. Sampling was carried out according to PMP Protocol at 300 °C. The particle mass
emissions and their composition are summarized in table 5. Figure 7 shows the particle size
distribution (measured by scanning mobility particle sizer SMPS) for Liebherr 924 engine without
DPF and with DPF at the 8 tested operation points. At the point 8, i.e. idling at 800 RPM, the
particle number concentration in the smaller size range is relatively low. A possible explanation for
this fact might be the lower soot generation at idling point 8. Hence, possibly emitted metal species
are emitted as free metal oxides, whereas at the other operating points the concentration of soot
particles is much higher that the metals can be bounded to the soot particles like shown as an
example in Fig. 8.
Low soot
Free metal NPs
OP 8
Fig. 7: Particle size distribution (SMPS) for Liebherr 924 engine (A) without DPF and (B) with DPF
at 8 operation points (OP) according to test cycle ISO 8178/4 C1. OP 8 is idling at 800 RPM.
Sampling according to PMP Protocol: 300°C, Dilution Ratio DR=100
Fig. 8: SEM image of metal NPs, here cerium oxide, bound to soot particles
Tab 5: Particle mass emissions of filter samples for vehicles
If metal emissions lead to nanoparticulate emissions at very low size ranges, it was suspected that
the phenomenon is also visible for petrol engines. The following graph shows the size distribution
measured by SMPS for measurement of two cars and two 2 weelers. All measurements were
carried out at two different steady-state conditions, i.e. at a constant speed of 50 km/h and at
idling. The Renault R18 car has, both at the medium load point and at idling, relatively high particle
emissions. A bimodal distribution was observed at part load. For the Honda 450 CWR Motorbike
modality of the size distribution is clearly evident and the emissions are relatively high. Also the 1cylinder/4-stroke scooter engine of the Piaggio Scooter showed significant particle emissions at 50
km/h which were even higher than for the Honda motorbike. However, the bimodal distribution is
less evident. The .particle emission at idling operation was lower than expected. The second car
Nissan Qashqai, which was of newer engine technique showed relatively low particle emissions
which hardly exceed the background, neither at 50 km/h nor at idling. Further investigations on
metal oxide emissions of different vehicle types have been already published [16, 18, 19, 27].
Fig. 8: Particle distribution (SMPS) at 50 km/h and idle for cars: (A) Renault R18 and
(B) Nissang Quahqai motorbikes: (A) Honda 450 and (B) Scooter Piaggio
Mechanism
In figure 9 a schematic of possible reactions in the exhaust gas are given. Metals, present in the
exhaust can be adsorbed to other particles e.g. soot, but in absence of this particles also nucleate
with itself. Therefore, a lower soot generation at idling point 8 like in figure 7 might lead to a
higher amount of self-nucleation and is therefore emitted as metal species (metal oxides). A
particle filter enables to lower this emissions significantly.
Vehicle
Emissions
Fig. 9: Schematic mechanisms of emission and particle formation in exhaust (partly adopted from
Schneider et al.) [26]
Conclusion
Emissions of metal oxide particles can occur for all types of internal combustion engines. Even if
clean fuels are used, lubrication oil remains as a potential source for metal oxide particles. Fullwall-flow particle filter systems have shown high filtration efficiency in diesel exhaust gas aftertreatment. However, this study demonstrated that they can be also useful to remove metal oxide
emissions from other engine types. An effective filtration of metal particles is important to reduce
toxic potential of nanosized particles and metals. Hence, filtration technology is promising not only
for diesel engines (soot filtration) but for all types of combustion engines. The filtration efficiency
for metals should be further investigated in future projects.
Acknowledgements:
The authors like to thank the Swiss Federal Office for Environment BAFU, the VERT Assoziation
and our industry partners for support.
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(4)
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Personenwagen. - Untersuchung der Emissionen von aktuellen Personenwagen mit konventionellen und
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Conference on Combustion Generated Nanoparticles, August 2007 (2007).
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tract to study the interaction with particles. American Journal of Respiratory Cell and Molecular Biology 32,
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Jeng, H. A. & Swanson, J. Toxicity of metal oxide nanoparticles in mammalian cells. Journal of environmental
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Mayer et al, SAE 2012-01-0841.
Materials Sci ence & Technolog y
Particle and metal emissions
of diesel and gasoline engines
Are particle filters appropriate measures?
A. Ulrich1, A. Wichser1, A. Hess1,2, N. Heeb1, L. Emmenegger1
J.Czerwinski3, M. Kasper4, J. Mooney5, A. Mayer6
1Empa,
Swiss Federal Laboratories for Material Testing and Research, 8600 Dübendorf, Überlandstrasse 129, Switzerland
École Polytechnique Fédérale de Lausanne, Switzerland
Abgasprüfstelle Biel, Gwerdtstr. 5, CH – 2560 Nidau, Switzerland
4ME, Matter Aerosol AG, Bremgarterstr. 62, CH – 5610 Wohlen, Switzerland
5585 Colgate Ave Wyckoff, NJ, USA
6TTM, Fohrhölzlistrasse 14b, CH – 5443 Niederrohrdorf, Switzerland
2EPFL
3AFHB,
Contact: [email protected]
Not only diesel, but also gasoline fueled internal combustion engines can emit particulate matter. Especially for direct injection technology an increase in particulate
emission was observed. Previous studies shown, that ultra-fine particulate emissions often contain metal oxides, which can originate from various sources such as
engine wear, lubrication oil, fuel ashes, fuel additives or coatings from exhaust gas after-treatment systems. The metal content in most of the conventional on-road
fuels is relatively low, whereas lubrication oils often contain much higher metal concentrations. Engine wear metals occur in all internal combustion engines. Metal
compounds collected in lubrication oil can be re-entrained into the cylinder and then oxidized during combustion. Some metals might be vaporized and re-nuclide
forming ultra-fine particles in a size range typically below 30 nm. These metal oxide particles can be present in the exhaust aerosol either as free metal oxide
particles or attached to larger soot particles. The toxicological effect of nanoparticles was proved in several studies. Hence, these nanoparticulate emissions need to
be avoided. Full wall-flow particle filter systems are effective measures to reduce particulate emissions and they are already well established in diesel engine
technology. These filter technology might be also beneficial especially for direct injection gasoline engines.
Comparison of Vehicles
Toxicity
1.E+14
Deposition
Rate
in %
deposition
rate [%]
Particle Number PN [1/km]
100
100
1.E+13
PN increase
PN reduction
> 99 %
1.E+12
> 98 %
total
80
80
54%
(15 nm)
48%
(10 nm)
60
60
40
40
nasal region
20%
(100 nm)
20
20
00
11
1010
tracheobronchial
region
alveolar region
100
100
1000
1000
10000
10000
particle diameter [nm]
Particle
Diameter in nm
DI Gasoline
Diesel
Diesel/DPF Diesel/DPF
load
reg
Deposition of
particles in
respiratory tract
Emissions Diesel
1.E+11
MPI
Gasoline
Emissions Gasoline Vehicles
Particle deposition rates in the respiratory tract
Metal Soot
oxides
CNG
PN for Diesel engine (Test cycle ISO 8178/4
Particle number concentration (PN) of different vehicle types
C1 from VERT VSET (SN 277 206)
adopted from Empa Report 2007 (Novatlantis)
“Emissionsvergleich verschiedener Antriebsarten in aktuellen Personenwagen
MPI = multiport injection / DI = direct injection / CNG = compressed natural gas
DPF = diesel particle filter (wall flow) / load = loading phase / reg = regeneration phase
NEDC
= New European driving cycle for cars
Euro 3-C2 = European driving cycle for bikes
Euro 3-C1 = European driving cycle for scooters
Vehicle
Renault R18
Honda 450 CBR
Nissan Qashqai
Piaggio
Cycle
50 km/h
Idling
50 km/h
Idling
50 km/h
Idling
50 km/h
Idling
Diesel
Idling
Ntotal
[P/cm3]
4.1  107
7.1  107
2.2  106
6.8  106
9.1  103
1.8  103
3.6  107
6.2  103
1.5  107
Nash
[P/cm3]
3.8  107
7.1  107
n.d.
6.8  106
n.d.
n.d.
n.d.
n.d.
1.4  107
Nsoot
[P/cm3]
3.1  106
7.1  104
n.d.
3.7  104
n.d.
n.d.
n.d.
n.d.
8.6  105
Dash
[nm]
7.9
24.4
n.d.
12.7
n.d.
n.d.
n.d.
n.d.
11.8
Dsoot
[nm]
69.6
131.6
n.d.
25.6
n.d.
n.d.
n.d.
n.d.
48.1
Particle size distribution (SMPS) for Liebherr 924 engine
of aDPF
particle
filterpoints
(A) withoutEfficiency
DPF and (B) with
at 8 operation
Point 8 is idling at 800 RPM.
PN concentration dN / d log DP [cm-3]
Particle Number Concentration in PN/km
«Auch neue
Benziner brauchen
strenge Grenzwerte
- Testergebnisse:
Benzinmotoren mit
Direkteinspritzung
VCD + Umwelthilfe
PN Limit for
Diesel Euro 5
and Gasoline
Euro 6
PN Emissions of Petrol Engines
Idle with / without particle filter (PF)
Filtration efficiency > 99.9%
without PF
Particle mass emissions of filter samples for vehicles
with PF
Text
Mechanism
Particle Mass Concentration in g/km
OP 8 = idle
Sampling: 300°C,
Dilution Ratio DR=100
PN Limit for
Diesel Euro 5b
Low soot
Free metal NPs
45
1. Abrasion from piston ring, cylinder liner, valve cams, valves,
bearings (e.g. Fe, Al, Cr, Ni, Cu, Pb ...)
=> abraded metal mass ca. 0.1 to 1 mg/km
2. Lubrication oil: e.g. Zn: 0.1 – 0.2 %, Ca: 0.5 %,
B: 0.09 %. Mg: 0.002-0.004 %,...
old vehicles: up to 1 % oil of fuel consumption
3. Fuel: several metals in traces, heavy metals (Pb, Mn,) have
limits (e.g. in Germany BzBIG 1971: Pb <150 mg/kg fuel)
Soot
DPF1 1
Soot
DPF2 2
35
Soot
DPF3 3
30
Soot
DPF5 5
Soot
DPF4 4
Metals in ash and soot
collected in 5 different DPFs
(DPF 4 and 5 were operated with
CeO2 regeneration fuel additive)
25
Schematic mechanisms of emission and particle
formation in exhaust (partly adopted from Schneider et al.)
20
15
Metal NPs bound to soot
10
Soot generation at idling point
5
0
Na
Mg
Al
Si
P
S
Cl
K
Ca
Ti
V
Cr
Mn
Fe
Co
Ni
Cu
Zn
Rb
Sr
Y
Zr
Nb
Mo
Sn
Sb
Ba
La
Ce
Pt
Pb
Sources for Metal Emissions
Mass Concentration in g/100 g (%)
40
Conclusion
Emissions of metal oxide particles can occur for all types of internal combustion engines. Even if clean fuels are used,
lubrication oil remains as a potential source for metal oxide particles. Full-wall-flow particle filter systems have shown
high filtration efficiency in diesel exhaust gas after-treatment. However, this study demonstrated that they can be also
useful to remove metal oxide emissions from other engine types. An effective filtration of metal particles is important to
reduce toxic potential of nanosized particles and metals. Hence, filtration technology is promising not only for diesel
engines (soot filtration) but for all types of combustion engines. The filtration efficiency for metals should be further
investigated in future projects.
Acknowledgements:
Presented at:
Bafu for financial support;
16th Conference on Combustion Generated Nanoparticles 2012,
VERT Association
24.6.2012 – 27.6.2012 in Zürich, Switzerland
Particle distribution (SMPS) at 50
andlow
idle for
8 iskm/h
relatively
cars: (A) Renault R18 and (B) Nissang
Quahqai
=> free metal
oxides
motorbikes: (A) Honda 450 and (B) Scooter Piaggio
Literature:
A. Ulrich et al, Anal Bioanal Chem, 2003, 377, 7181.
J. Czerwinski et al: SAE Paper 2005-01-1100.
A. Mayer et al; SAE 2007-01-1112
C. Bach et al: Empa Report 2007 (Novatlantis) “Emissionsvergleich verschiedener
Antriebsarten in aktuellen Personenwagen.
N.V. Heeb, et al., SAE Paper 2005-26-014, 329-338.
N.V. Heeb, et al., Environ Sci Techn 2008, 42(10); 3773-3779.
A. Mayer et al, SAE 2010-01-0792.
N.V. Heeb, et al. Env. Sci. Tech. 44 (3), 2010, 1078 - 1084.
N.V. Heeb, et al. Atm. Env. 45, 2011. 3203-3209
A. Ulrich et al. Proceedings of PTNSS Congress 2011, June 2011
J. Schneider et al. Environ. Sci. Technol. 2005, 39, 6153-6161
A. Mayer et al, SAE 2012-01-0841.