assessment of particulate matter emission from diesel vehicles … › 2014_eth-npc-18 ›...

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1 Université de Lyon, Institut de Recherches sur la Catalyse et l’Environnement de Lyon, UMR 5256, CNRS, Université Claude Bernard Lyon 1, 2 avenue A. Einstein, 69626 Villeurbanne, France 2 IFP Energies nouvelles - Direction Techniques d'Applications Energétiques, Etablissement de Lyon, Rond-point de l'échangeur de Solaize - BP 3, 69360 Solaize - France e-mail: [email protected] B. R’Mili 1 , A. Boréave 1 , N. Charbonnel 1 , A. Même 1 , M.N. Tsampas 1 , M. Leblanc 2 , L. Noel 2 , S. Raux 2 , P. Vernoux 1 , B. D’Anna 1 Assessment of particulate matter emission from Diesel vehicles equipped with DPF Introduction Experimental set up Results: Acknowledgements II: regeneration Conclusions MAAP 5012 o BC measurement Since 2011, all Diesel cars are equipped with a Diesel Particulate Filter (DPF) and respect European standards (Euro 6) for particulate matter emissions which combine a limit number (PN: 6.0×10 11 part/km) with a limit mass (PM: 4.5 mg/km). However, vehicle emission during cold start and regeneration are known to be higher and not yet regulated. Otherwise, there is limited data concerning particle number, mass, morphology, chemical composition during these two phases. In this study we propose a new approach based on the combination of three technique namely, AMS, MAAP and MPS to characterize particles emitted from one Diesel Euro5 vehicles equipped with Fuel Born Catalyst Filter (FBCF). Collections were carried out during cold and hot start NEDC driving cycle and during regenerations phase. I: Transient test o NEDC cycle : cold start Dilution ratio FPS : o DR = 6,4 (PD (hot)=1,2 – ED (ambiant) =5,8) FPS 4000 o Two stages diluter MPS o TEM grid sampling TOF-AMS o Aerosol mass spectrometer Citroen C4 o Equipped with DPF (FBCF) exhaust Chassis dynamometer Exhaust samples were analyzed during NEDC driving cycle as well as during regenerations phases TEM/EDX analysis o Soot : C, S o Big droplet : C, Fe, Ni, Cr, S, Si, Ca, Mn, P, K, Na TEM/EDX analysis o Soot : C, S TEM/EDX analysis o Big droplet : C, Fe, Ni, Cr, S, Si, Ca, Mn, P, K, Na Start regeneration End regeneration -1- -2- -3- -1- -1- -1- Soot cake formation in DPF TEM analysis Soot : C, S (adsorbed) TEM analysis Soot : C, S Small droplets : S TEM analysis Soot : C, S Small droplets : S Diesel engines equipped with DPF mainly emit particles during cold start and DPF regenerations. o During cold start, in the first ten minutes, the particles emitted are mainly carbon soot. Later, big droplets with metal content appear especially during heavy acceleration o During hot start, is observed only large droplets especially during heavy acceleration. It seems that the increase of engine speeds during cycles resulted in increase of fractions of metal contents in particulate matters. Sources of droplet and metal emissions : Abrasion from piston ring, cylinder liner, valves (abraded metal) Lubrication oil Trace metals in Fuel o During the DPF regenerations, PM size distributions are classified as bimodal, mainly consisting of the nucleation and accumulation modes. Typically, these particles are composed of a complex mixture of soot and small droplet like particles. These results are repeatable o MAAP-multi-angle absorption photometry (A. Petzold et al. 2004, 2005) Joint d’étanchéité + Grille MET Entrée Aérosol Sortie Aérosol Interception Impaction inertielle Diffusion brownienne Lignes de courant membrane 0% 10% 20% 30% 40% 50% 60% 70% 80% 90% 100% 1 10 100 1000 Collection efficiency (%) Diameter (nm) Experimental points (NaCl) Experimental points (Cu) Theory o NEDC cycle : Hot start o Porous TEM grid (Quantifoil) o Cappilary tube model (Rubow & liu 1981) o Collection efficiency (B. R’mili et al. (2011)) Particle collection technique based on filtration through on class of TEM dedicated technique support, namely porous TEM grids o MPS - Mini Particles Sampler (B. R’mili et al. 2011) Aerosol is introduced into the instrument through an aerodynamic lens focusing the particles through a skimmer and an orifice onto the vaporizer. Particle vapor is ionized and the ions are guided into the TOF-MS, which generates mass spectra at 83.3 kHz repetition rate. For particle size measurement the particle beam is chopped with a mechanical chopper and the detection is synchronized with the chopper opening time (F. Drewnick et al. (2005)) o Schematic of the Time-of-Flight Aerosol Mass Spectrometer (TOF-AMS). This method measure the black carbon mass concentration by measuring the aerosol light absorption from the simultaneous measurement of radiation passing through and scattered back from a particle-loaded fiber filter . Correction methods for an artifact found to affect the instrument accuracy (A. P. Hyvärinen et al. (2012)) TEM/EDX analysis o Big droplet : C, Fe, Ni, Cr, S, Si, Ca, Mn, P, K, Na TEM/EDX analysis o Big droplet : C, Fe, Ni, Cr, S, Si, Ca, Mn, P, K, Na TEM/EDX analysis o Big droplet : C, Fe, Ni, Cr, S, Si, Ca, Mn, P, K, Na Nothing was measured with the MAAP during the hot start Literature: A.P. Hyvärinen et al. Atmos. Meas. Tech., (2013) 6, 81-90 A. Petzold & M. Schönlinner, Aerosol Science (2004) 421-441 A.Petzold et al., Aerosol science and technology, (2005) 39:1, 40-51 B. Rmili et al. Aerosol science and Technology, (2013) 47:7, 767-775 F. Drewnick et al. (2005) 36:637-658 K.L. Rubow and B.Y.H. Liu Gas. Vol. 1 ASTM (1986) p. 975

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Page 1: Assessment of particulate matter emission from Diesel vehicles … › 2014_ETH-NPC-18 › Badr_R_Mili.pdf · 2015-06-04 · aerosol light absorption from the simultaneous measurement

1Université de Lyon, Institut de Recherches sur la Catalyse et l’Environnement de Lyon, UMR 5256, CNRS, Université Claude Bernard Lyon 1, 2 avenue A. Einstein, 69626 Villeurbanne, France 2IFP Energies nouvelles - Direction Techniques d'Applications Energétiques, Etablissement de Lyon, Rond-point de l'échangeur de Solaize - BP 3, 69360 Solaize - France

e-mail: [email protected]

B. R’Mili1, A. Boréave1, N. Charbonnel1, A. Même1, M.N. Tsampas1, M. Leblanc2 , L. Noel2, S. Raux2 , P. Vernoux1, B. D’Anna1 Assessment of particulate matter emission from Diesel vehicles equipped with DPF

Introduction Experimental set up

Results:

Acknowledgements

II: regeneration

Conclusions

MAAP 5012 o BC measurement

Since 2011, all Diesel cars are equipped with a Diesel Particulate Filter (DPF) and respect European standards (Euro 6) for particulate matter emissions which combine a limit number (PN: 6.0×1011part/km) with a limit mass (PM: 4.5 mg/km). However, vehicle emission during cold start and regeneration are known to be higher and not yet regulated. Otherwise, there is limited data concerning particle number, mass, morphology, chemical composition during these two phases. In this study we propose a new approach based on the combination of three technique namely, AMS, MAAP and MPS to characterize particles emitted from one Diesel Euro5 vehicles equipped with Fuel Born Catalyst Filter (FBCF). Collections were carried out during cold and hot start NEDC driving cycle and during regenerations phase.

I: Transient test o NEDC cycle : cold start

Dilution ratio FPS :

o DR = 6,4 (PD (hot)=1,2 – ED (ambiant) =5,8)

FPS 4000 o Two stages diluter

MPS o TEM grid

sampling

TOF-AMS o Aerosol mass

spectrometer

Citroen C4 o Equipped with DPF (FBCF)

exhaust

Chassis dynamometer

Exhaust samples were analyzed during NEDC driving cycle as well as during regenerations phases

TEM/EDX analysis o Soot : C, S o Big droplet : C, Fe, Ni, Cr,

S, Si, Ca, Mn, P, K, Na

TEM/EDX analysis o Soot : C, S

TEM/EDX analysis o Big droplet : C, Fe, Ni, Cr,

S, Si, Ca, Mn, P, K, Na

Start regeneration End regeneration

-1- -2- -3- -1- -1- -1-

Soot cake formation in DPF

TEM analysis Soot : C, S (adsorbed)

TEM analysis Soot : C, S

Small droplets : S TEM analysis

Soot : C, S Small droplets : S

Diesel engines equipped with DPF mainly emit particles during cold start and DPF regenerations. o During cold start, in the first ten minutes, the particles emitted are

mainly carbon soot. Later, big droplets with metal content appear especially during heavy acceleration

o During hot start, is observed only large droplets especially during heavy acceleration. It seems that the increase of engine speeds during cycles resulted in increase of fractions of metal contents in particulate matters.

Sources of droplet and metal emissions : Abrasion from piston ring, cylinder liner, valves (abraded metal) Lubrication oil Trace metals in Fuel

o During the DPF regenerations, PM size distributions are classified as bimodal, mainly consisting of the nucleation and accumulation modes. Typically, these particles are composed of a complex mixture of soot and small droplet like particles.

These results are repeatable

o MAAP-multi-angle absorption photometry (A. Petzold et al. 2004, 2005)

Joint d’étanchéité +

Grille MET

Entrée Aérosol

Sortie Aérosol

Interception

Impaction inertielleDiffusion brownienne

Lignes de courant

membrane

0%

10%

20%

30%

40%

50%

60%

70%

80%

90%

100%

1 10 100 1000

Col

lect

ion

effic

ienc

y (%

)

Diameter (nm)

Experimental points (NaCl) Experimental points (Cu) Theory

o NEDC cycle : Hot start

o Porous TEM grid (Quantifoil)

o Cappilary tube model (Rubow & liu 1981)

o Collection efficiency (B. R’mili et al. (2011))

Particle collection technique based on filtration through on class of TEM dedicated technique support, namely porous TEM grids

o MPS - Mini Particles Sampler (B. R’mili et al. 2011)

Aerosol is introduced into the instrument through an aerodynamic lens focusing the particles through a skimmer and an orifice onto the vaporizer. Particle vapor is ionized and the ions are guided into the TOF-MS, which generates mass spectra at ∼ 83.3 kHz repetition rate. For particle size measurement the particle beam is chopped with a mechanical chopper and the detection is synchronized with the chopper opening time (F. Drewnick et al. (2005))

o Schematic of the Time-of-Flight Aerosol Mass Spectrometer (TOF-AMS).

This method measure the black carbon mass concentration by measuring the aerosol light absorption from the simultaneous measurement of radiation passing through and scattered back from a particle-loaded fiber filter .

Correction methods for an artifact found to affect the instrument accuracy (A. P. Hyvärinen et al. (2012))

TEM/EDX analysis o Big droplet : C, Fe, Ni, Cr,

S, Si, Ca, Mn, P, K, Na

TEM/EDX analysis o Big droplet : C, Fe, Ni, Cr,

S, Si, Ca, Mn, P, K, Na

TEM/EDX analysis o Big droplet : C, Fe, Ni, Cr,

S, Si, Ca, Mn, P, K, Na

Nothing was measured with the MAAP during the hot start

Literature: A.P. Hyvärinen et al. Atmos. Meas. Tech., (2013) 6, 81-90 A. Petzold & M. Schönlinner, Aerosol Science (2004) 421-441 A.Petzold et al., Aerosol science and technology, (2005) 39:1, 40-51 B. Rmili et al. Aerosol science and Technology, (2013) 47:7, 767-775 F. Drewnick et al. (2005) 36:637-658 K.L. Rubow and B.Y.H. Liu Gas. Vol. 1 ASTM (1986) p. 975

Page 2: Assessment of particulate matter emission from Diesel vehicles … › 2014_ETH-NPC-18 › Badr_R_Mili.pdf · 2015-06-04 · aerosol light absorption from the simultaneous measurement

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