aeronet workshop berlin, 16-17 sep 2002 leonidas ntziachristos mech. eng, phd post-doc research...
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Aeronet Workshop
Berlin, 16-17 Sep 2002
Leonidas Ntziachristos
Mech. Eng, PhD
Post-Doc Research Fellow
SamplingSampling
& Instrumentation & Instrumentation TechniquesTechniques
for Automotive Exhaust for Automotive Exhaust Particle EmissionsParticle Emissions
Aeronet WorkshopBerlin,
16-17 Sep 2002
The “PARTICULATES
”
project team
” PARTICULATES „ Characterisation of Exhaust Particulate
Emissions From Road Vehicles
A 5 FP European research programmesponsored by the Directorate General
on TRansport and ENergy
Partners: Associate partners:Aristotle University (GR) – Coord. Renault (F) Concawe (B) INRETS (F) Volvo (S) Dekati (FIN) Tampere University (FIN) Stockholm Univ. (S) EMPA (CH) Athens Uni. (GR) AEAT (UK) TRL (UK)IFP (F) INERIS (F) AVL (AUT) LWA (UK) MTC (S) Graz University (AUT)Aachen University (D) ConsultantsJRC (NL) D. Kittelson G. Reischl
Aeronet WorkshopBerlin,
16-17 Sep 2002
The“PARTICULATES
”
relevant info
Project started April 2000 3-year duration (end March 2003) Total cost: 3,6 M€, EU contribution:
2,5 M€ (70%) http://vergina.eng.auth.gr/mech/
lat/particulates
Aeronet WorkshopBerlin,
16-17 Sep 2002
The “PARTICULATES
”
targets
Definition of the exhaust aerosol properties which will be examined and evaluation of available measurement instruments and techniques
Development and introduction of a harmonised protocol for the definition of exhaust aerosol sampling conditions
Examination of the particulate emissions of current light duty vehicles and heavy duty engines
Investigation of the influence of engine technology, fuel quality and after-treatment on particulate emissions
Aeronet WorkshopBerlin,
16-17 Sep 2002
Nature of ICEExhaust Particles
Primary particles Soot - elemental carbon
(mostly on diesel engines) Heavy HC (PAHs, >C20)
Ash (metal oxides):• Lube oil and fuel (Ca, Mg, Zn, ...)• Engine component wear (Fe, Cu, Cr,
Al,…)• Fuel additives (Ce, Fe, Cu, Mn,…)
Secondary particles Sulphates (from S in fuel and lube
oil) Condensable organic material Water
Aeronet WorkshopBerlin,
16-17 Sep 2002
Size definitions and
morphology
(diesel engine)
Df~3Df~3
Df~2.4Df~2.4
+secondary particles
Aeronet WorkshopBerlin,
16-17 Sep 2002
Why do we need to shift from mass to
other metrics?
Legislative, mass-based method seemed not to be sensitive enough for future vehicle technologies- 1992: 0.14 g/km, 2005: 0,025 g/km Work by ISO, US and EU authorities increased
sensitivity and reproducibility of traditional method
Evidence from medical research calls for a wider reporting of emissions
To better understand (and control) pollutant formation
Occasion: Report of HEI (1996) raised concerns that mass-based measures do not control number concentrations evidence after that never confirmed
such a finding in a consistent way
Aeronet WorkshopBerlin,
16-17 Sep 2002
Main Issues in ICE
Particle Analysis
Issue 1: What to measure? … instrument Particle property Size range Resolution (time, size) Applicability / cost
Issue 2: How to measure? … sampling method Dilution factor Residence time Temperature RH Hydrocarbon concentration of background air
Decisions to be taken on: Requirements from health and environment
experts Potential for evaluation of technology
measures
Aeronet WorkshopBerlin,
16-17 Sep 2002
Issue 1
What to measure
Candidate Metrics
Mass of particles <10 μm (respirable fraction) is the legislation requirement
Size: Determines lung deposition profiles and cell interactions and behaviour in atmosphere Aerodynamic diameter (> 100 nm) Mobility diameter (< 100 nm)
Surface: Carrier of chemical species, medium for all interactions Geometric Fuchs “Active” surface
Number: Sensitive metric to boundary condition changes
Nature/chemistry: Behaviour in atmosphere and in human body
Aeronet WorkshopBerlin,
16-17 Sep 2002
Issue 1
What to measure
Instruments
(most widespread techniques - non exhaustive list)
Metric Technique Property Size RangeSize
ResolutionTime
ResolutionRemarks
Mass Filter Method Total mass <10 um None None Standard method for PM determination
ImpactorMass / aerod.
Diameter~20 nm -
10 um10 - 15 stages
None Small size range is problematic
TEOMTotal mass of
solids< 10 um None s
Only suitable where solids dominate
Number CPC Total number > 3 nm None s Can be reference
instrument for total number
Number & size
SMPSNumber, mobility
diameter 7 nm - 1 um
64 channels per decade
min
Mobility relevant for small sizes, most
widespread technique
ELPINumber,
aerodynamic diameter
7 nm - 10 um
14 size bins s
Aerodynamic relevant for
accumulation, most suitable for solids
SurfaceEpiphanio-
meterFuchs surface > 7nm None s
Until lately the only technique for on-line
surface determination
Diffusion charger
"Active" surface > 7nm None sCheap altenative to
epiphaniometer
ChemistryAnalytical
techniquesChemical
informationNone
Standard chemical analysis, time consuming
Depending on classification method
Aerosol Mass Spectrometer
Size, chemical information
30 nm - 3 um
10 part / s sState of the art high-
cost application
Aeronet WorkshopBerlin,
16-17 Sep 2002
How do exhaust aerosol looks
like after atmospheric
dilution?
Data from SAE 2000-01-2212, Kittelson et al.
Aeronet WorkshopBerlin,
16-17 Sep 2002
Issue 2
How to measure
Sampling Parameters
Dilution is required: To avoid water condensation To approach atmospheric process Because particle concentration is usually
above instrument max range
0.E+00
2.E+08
4.E+08
6.E+08
8.E+08
1.E+09
1.E+09
1.E+09
1 10 100 1000
electrical mobility particle diameter dp [nm]
dN
/dlo
g d
p [
cm-3
] 40 °C
30 °C
19 °C
17 °C
Dilution Parameter: Temperature
0.0E+00
5.0E+08
1.0E+09
1.5E+09
2.0E+09
2.5E+09
3.0E+09
1 10 100 1000
electrical mobility particle diameter dp [nm]
dN
/dlo
g d
p [
cm-3
]
41
24
15
Dilution ratio
Dilution Ratio
0.0E+00
5.0E+08
1.0E+09
1.5E+09
2.0E+09
2.5E+09
1 10 100 1000
electrical mobility particle diameter dp [nm]
dN
/dlo
g d
p [
cm-3
]
0.6 s
3.1 s
Residence time
Residence Time
0.0E+00
5.0E+08
1.0E+09
1.5E+09
2.0E+09
2.5E+09
1 10 100 1000
electrical mobility particle diameter dp [nm]
dN
/dlo
g d
p [
cm-3
]
50
38.8
26
14.4
10
2.4
relative humidity [%]of dilution air
RH of dilution air
Aeronet WorkshopBerlin,
16-17 Sep 2002
Issue 2
How to measure
Vehicle effects
Vehicle Effect: THC concentration
0.0E+00
5.0E+07
1.0E+08
1.5E+08
2.0E+08
2.5E+08
3.0E+08
3.5E+08
4.0E+08
4.5E+08
5.0E+08
1 10 100 1000
electrical mobility particle diameter dp [nm]
dN
/dlo
g d
p [
cm-3
] 506
390
238
99.2
25
13.6
THC concentration ofdilution air [ppm]
0.0E+00
5.0E+08
1.0E+09
1.5E+09
2.0E+09
2.5E+09
1 10 100 1000
electrical mobility particle diameter dp [nm]
dN
/dlo
g d
p [
cm-3
]
250 ppm
<10 ppm
Sulphur content of fuel
Sulphur concentration
0.0E+00
2.0E+08
4.0E+08
6.0E+08
8.0E+08
1.0E+09
1.2E+09
1 10 100 1000
electrical mobility particle diameter dp [nm]
dN
/dlo
g d
p [
cm-3
]
0 min.
3 min.
6.5 min.
10 min.
13.5 min.
16.5 min.
Consecutive SMPS scans
History effects
Aeronet WorkshopBerlin,
16-17 Sep 2002
Issue 2
How to measure
Selection of sampling
parameters
Similarity to atmospheric dilution Potential to form nucleation mode Small sensitivity to change of parameters Feasibility to reach at the lab
DR: 12.5:1DT: 32°C
RT: 1 ms+stabilisation
(~3s)
Aeronet WorkshopBerlin,
16-17 Sep 2002
SamplingConfiguration
Example: Diesel engine
emissions
Ageing Chamber
2-stage ejector Dilutor
Dilution Air Line
Sample Line
Silica Gel
CharcoalFilter
EjectorDilutor
Heater Denuder
Mass Flow
Controller
ELPI
SMPS
Diffusion
Charger
Cooling Agent Line
Fdddg kjlk
TEOM
DR 12 : 1DR 12 : 1T 30 - 40°CT 30 - 40°C
RT 1 msRT 1 ms
Pump
Throttle Valve
Grav. Impactor
DR 120 : 1DR 120 : 1T ambT amb
RT 2.5 sRT 2.5 s
DR 1200 : 1DR 1200 : 1T ambT amb
RT 2.8 sRT 2.8 s
DR 120 : 1DR 120 : 1T 40°CT 40°C
RT 3.5 sRT 3.5 s
S A M P L E IN
D IL U T E D S A M P L E O U T
Aeronet WorkshopBerlin,
16-17 Sep 2002
Example of properties
determinationin a single run
Total “active” surface [RT] Total particle number [RT]
Surface and number give mean size [RT] Size segregated solid particle number [RT] Solids particle mass [RT] Gaseous pollutants [RT] Particle mass (VF/nVF) - CVS [CYCLE] Mass weighted size distribution [CYCLE] Number weighted size distribution[SS]
RT: Real Time CYCLE: Mean value over cycle SS: Steady State
Aeronet WorkshopBerlin,
16-17 Sep 2002
Example of protocol
application
Motorcycle emissions
-400
-200
0
200
400
600
800
0 200 400 600 800 1000 1200
ECE 40 Cycle Time [s]
Ac
tiv
e S
urf
ac
e [
cm
2 s-1
]
0
20
40
60
80
100
120
Sp
ee
d [
km
h-1
]
Yamaha BWS (3.2 m²/km).
.
Speed
Yamaha BWS
1.E+07
1.E+08
1.E+09
1.E+10
1.E+11
1.E+12
1.E+13
0 200 400 600 800 1000 1200ECE 40 Cycle Time [s]
dN
/dlo
gD
p [
s-1
]
0
30
60
90
120
150
180
Sp
ee
d [
km
h-1
]
Total particles, 100 nm mob.Solid particles, 104 - 168 nm aer.
Speed
.
.Honda DIO
1.0E+10
1.0E+11
1.0E+12
1.0E+13
1.0E+14
1.0E+15
1.0E+16
1.0E+17
1 10 100 1000Mobility Diameter [nm]
dN
/dlo
gD
p [
km
-1]
55 km/h
20 km/h
Active SurfaceConcentration of totals/solidsDistribution with nucleation mode
Honda DIO
1.0E+08
1.0E+09
1.0E+10
1.0E+11
1.0E+12
1.0E+13
1.0E+14
1.0E+15
1.0E+16
1.0E+17
1 10 100 1000 10000
Aerodynamic Diameter [nm]
dN
/dlo
gD
p [
km
-1]
20 km/h
55 km/h
Solid particles distribution
Aeronet WorkshopBerlin,
16-17 Sep 2002
Conclusions
Recommendations
Candidate metrics (automotive sector): mass (will remain legislation metric) active surface total number concentration accumulation mode profile size segregated chemical fingerprints
Plume aerosol differs from engine-out one
Sampling parameters are critical if nucleation mode particles are important
Soot particles are easier to characterise (thermodenuders become widespread)
Experience from the automotive sector may also apply to ground-level aviation emissions
In-flight emissions?