Paper-Abstract Form. Title: Reduction of exhaust nanoparticles by retrofitted after-treatment systems in diesel passenger cars

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12 th ETH-Conference on Combustion Generated Nanoparticles June 23 rd 25 th 2008 Paper-Abstract Form Name of Author: Liisa Pirjola 1,2 Co-Authors: Topi Rönkkö 3, Heikki Parviainen 1, Annele Virtanen 3, Jorma Keskinen 3 Affiliation: 1 Department of Technology, Helsinki Polytechnic, Finland 2 Department of Physics, University of Helsinki, Finland 3 Department of Physics, Tampere University of Technology, Finland Mailing address: 1 P.O. Box 4020, FIN-00099 Helsinki, Finland 2 P.O. Box 64, FIN-00014 Helsinki, Finland 3 P.O.Box 692, FIN-33101, Tampere, Finland Phone / Fax : +358-9-31083245/ +358-9-31083350 E-mail : liisa.pirjola@stadia.fi, liisa.pirjola@helsinki.fi Title: Reduction of exhaust nanoparticles by retrofitted after-treatment systems in diesel passenger cars Abstract: (min. 300 - max 500 words) The abstracts for papers and posters should contain unpublished information on the research subject, the investigation methods and results obtained so far. Graphs and references are very welcome. During your presentation at the conference you may expand on this with additional data and results. General information on products which are already commercially available are not the focus of the presentations but are very welcome at the exhibition. Vehicle exhaust emissions constitute an environmental and health hazard Recent investigations on climate change have made apparent that traffic based CO 2 emissions should be restrained. Since diesel vehicles emit less CO 2 than gasoline vehicles, we can expect that the number of diesel vehicles will increase. Consequently, particle emissions will enhance due to higher soot mode compared to gasoline vehicles. Before the more strict Euro standards force car manufacturers to equip all diesel vehicles with particle filters, nanoparticle reduction could be accomplished by retrofitted after-treatment systems, especially if the car fleet renews very slowly as in Finland (18.3 years). A retrofitted after-treatment system (oxidizing catalyst and diesel particle filter DPF by Twintec) were installed into two test diesel passenger cars (BMW 530d year 2002, VW Passat 2.0 TDI year 2007). The nanoparticle emissions were studied in the real-world conditions. The vehicles were chased by a mobile laboratory van Sniffer (Pirjola et al., 2004a; Pirjola et al., 2004b) with a distance of 4 m. The measurements were performed with high and low engine loads. The driving speed was constant 40 km h -1. To control the activity of the DPF the temperature and pressure sensors were installed before and after the after-treatment system. Particle size distributions were measured by the electrical low pressure impactor (ELPI, Dekati Inc.) and two scanning mobility particle sizers (SMPS); one equipped with DMA 3085 and CPC 3025 (Nano-SMPS, TSI Inc.) and the other with DMA 3071 and CPC 3775 (SMPS, TSI Inc.) nearly similar as in Rönkkö et al. (2007). Particle volatility was studied by using a thermodenuder. Also recorded were the gaseous species such as CO, CO 2, NO, NO 2, and NO x as well as the driving parameters and fuel consumption. To determine the dilution ratio, the raw exhaust CO 2 concentrations with the same engine loads were measured on the chassis dynamometer by Helsinki Polytechnic. The particle number and volume size distributions in the raw exhaust were derived based on the measurements with and without the filter. A clear reduction was seen indicating the benefit of the filter. For the older car BMW,

the total number concentration decreased by ~63% for high load and ~42% for low load whereas for Passat the values were 26% and 9 %, respectively (Figure 1). By using the filter, the CO 2 emissions were not significantly enhanced. Effects of exhaust temperature on particle properties will be discussed. Particle reduction 100 % 90 % 80 % 70 % 60 % 50 % 40 % 30 % 20 % 10 % 0 % BMW 530d low engine load high engine load VW Passat 2.0 TDI Figure 1. Reduction percent of soot particles due to the retrofitted after-treatment systems. Pirjola, L., Parviainen, H., Hussein, T., Valli, A., Hämeri, K., Aalto, P., Virtanen, A., Keskinen, J., Pakkanen, T., Mäkelä, T., Hillamo, R. (2004a). Atmospheric Environment 38, 3625-3635. Pirjola, L., Parviainen, H., Lappi, M., Hämeri, K. and Hussein, T. (2004b). SAE-paper no 2004-01-1962. Rönkkö, T., Virtanen, A., Kannosto, J., Keskinen, J., Lappi, M., and Pirjola, L. (2007). Environmental Science and Technology, 41, 6384-6389. Short CV: Liisa Pirjola - degree of Ph. D. at University of Helsinki, Dept. of Physics, in 1998 - Docent (Adj. Prof.) at University of Helsinki since 2000 - principal lecturer at Helsinki Polytechnic, Dept. of Technology, since 2001 - more than 60 peer reviewed papers - research interests include aerosol dynamic modelling, atmospheric particles, atmospheric chemistry, traffic pollution, exhaust and non-exhaust particles, mobile laboratory measurements Return by Email latest 28 th of March 2008 to ttm.a.mayer@bluewin.ch 2

12th ETH-Conference on Combustion Generated Nanoparticles June 23rd 25th 2008, ETH Zentrum, Zûrich Reduction of exhaust nanoparticles by retrofitted after-treatment systems in diesel passenger cars Liisa Pirjola 1,2, Topi Rönkkö 3, Heikki Parviainen 1, Annele Virtanen 3 and Jorma Keskinen 3 1 Department of Technology, Helsinki Polytechnic (Stadia), P.O. Box 4020, FIN-00099 Helsinki, Finland 2 Department of Physics, University of Helsinki, P.O. Box 64, FIN-00014 Helsinki, Finland 3 Department of Physics, Tampere University of Technology, P.O.Box 692, FIN-33101 Tampere, Finland

Background for this work Particles, NOx, PAH Traffic exhaust emissions Greenhouse gases CO 2, N 2 O soot particles EU standards Adverse health effects Climate change EU biofuel directive Retrofitted filters Soot particles increase No filter Finnish tax policy for new cars Increase in diesel vehicles To restrain CO 2 emissions Passenger cars: diesel ~13% New diesels this year ~50%

Experimental method a retrofitted after-treatment system (oxidizing catalyst and particle filter) were installed into two test diesel passenger cars - EURO 3: BMW 530d, year 2002 - EURO 4: VW Passat 2.0 TDI, year 2007 on road chasing experiments were performed by a mobile laboratory Sniffer in Alastaro, Finland chasing distance 4 m driving speed 40 km/h high load and low load driving conditions one after the other several times driving parameters recorded with the KTS vehicle diagnostic system

Driving conditions - constant driving conditions Low engine load High engine load VW Passat with filter VW Passat without filter BMW with filter BMW without filter Boost pressure (kpa) Wheel power (kw) Boost pressure (kpa) Wheel power (kw) 125 5.5 168 21.6 126 5.6 169 21.7 110 6.7 160 32.7 110 6.9 160 30.8

Twintec PM-filter catalyst (PFC) open system with passive regeneration NO oxidizes to NO 2 on catalytic coated surfaces on a catalyst 1 NO + O 2 NO 2 2 NO 2 reacts with soot particles at appr. 200 o C 2NO 2 + C => CO 2 + 2NO continuous regeneration, no danger of clogging up low back pressure, no reduction of fuel mileage

- a part of flow passes directly through the fleece to the neighbouring channel - much larger part flows through the fleece in the direction of flow or along the surface of the fleece - particles are collected on the fleece surface mainly by diffusion - only as many particles are tracked as can be regenerated via NO2 (controlled by the metal PM-Metalit by Emitec) - 30-50% (even 70%) PM reduction rates

Instrumentation mobile laboratory Sniffer: a Diesel vehicle, Volkswagen LT35 designed and built by Stadia (Pirjola et al. 2004; 2006). sampling above the front bumpers ELPI (Electrical Low Pressure Impactor), aerodynamic diameter 7 nm - 6.6 μm, 12 stages,1s NanoSMPS (DMA 3085+CPC 3025), mobility diameter 3-60 nm, 90 s. SMPS (DMA 3071+CPC 3025), 10-400 nm, 90 s thermodenuder Gas analysers: CO, CO2, NO, NO2 Weather station at 2.9 m altitude, gps temperature and pressure sensors before and after the filter system

VW Passat DR-ave BMW 530d DR-ave Dilution ratio load1 368.14 load1 140.74 load2 310.98 load2 150.26 load3 753.07 load3 179.35 load4 661.86 load4 198.69 load5 571.61 load5 354.80 On road measurements for CO 2 additionally chassis dynamoter measurements performed in the emission laboratory of Helsinki Polytechnic with the same engine loads dilution ratios as a function of time as well as the averages calculated (* refers to denuder, green to filter, yellow to without filter) load6 586.06 load6 404.83 Load7 595.35 Load7 * 197.50 load 8 * 760.12 noload1 278.66 noload1 491.89 noload2 328.30 noload2 368.27 noload3 296.64 noload3 791.79 noload4 285.73 noload4 715.83 noload5 271.37 noload5 933.53 noload6 526.67 noload6 749.37 Noload7 * 514.63 Noload7 * 870.09 load8 251.17 Noload8 * 789.88 load9 355.13 load9 973.52 load10 266.94 load10 658.60 Load10b * 201.56 load11 572.33 Load11 * 607.76 Load12 * 740.26 load12 295.89 Load13 * 751.02 load13 208.36 Load14 * 657.85 Load14 * 262.86 noload9 1144.36 Load15 * 240.44 noload10 1082.50 noload9 876.57. noload11 886.86 noload10 843.45 Noload12 * 935.60 noload11 526.07 Noload13 * 1117.71 noload12 497.97 Noload14 * 641.16 Noload13 * 420.89 noload14 443.84 noload15 389.67 Noload16 * 383.09 Noload17 526.57

Results (no PFC, high vs. low load). thermodenuder 260 o C => non-volatile soot mode GMD larger for higher engine load number concentration 29% (BMW) and 22% (VW) larger for high load than for low load volume concentration 3-fold (BMW) and 2-fold (VW) compared with low load

Results (PFC, number size distribution) BMW VW.

Results (reduction percents) Particle number reduction Particle volume reduction 70 % 60 % Low load High load 70 % 60 % Low load High load 50 % 50 % 40 % 40 % 30 % 30 % 20 % 20 % 10 % 0 % BMW 530d VW Passat 10 % 0 % BMW 530d. VW Passat

Results (PFC, denuder, BMW).

Results (PFC, no denuder, BMW) No denu Rönkkö et al., 2008 submitted to EST

Results (PFC, denuder, VW Passat).

Results.

Conclusions exhaust emissions: simultaneous reduction of CO 2, NO x and PM are needed the mobile chasing measurements under real driving conditions show that retrofitted filters decreased exhaust particle number concentrations (40-60%) and mass concentrations (20-60%) however, reduction depends on driving conditions, oxidizing catalysts and vehicles more measurements are needed (several vehicles, different driving conditions, different after-treatment systems) long-time measurements are needed to follow filter s efficiency, also under winter conditions dynamometer tests effects on nucleation mode particles

Acknowledgements This work was funded by the Ministry of Transport and Communications Finland