Characterisation of Exhaust Particulate Emissions from Road Vehicles

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1 PARTICULATES Characterisation of Exhaust Particulate Emissions from Road Vehicles Deliverable 12: Particulate and PM characterisation in non-legislative conditions (sub-zero ambient temperatures) Final Version 04/2005 A project sponsored by: In the framework of: EUROPEAN COMMISSION Directorate General Transport and Environment Fifth Framework Programme Competitive and Sustainable Growth Sustainable Mobility and Intermodality

2 Contractors LAT/AUTh: Aristotle University of Thessaloniki, Laboratory of Applied Thermodynamics - EL CONCAWE: CONCAWE, the oil companies' European organisation for environment, health and safety - B VOLVO: AB Volvo - S AVL: AVL List GmbH - A EMPA: Swiss Federal Laboratories for Material Testing and Research - CH MTC: MTC AB - S TUT: Tampere University of Technology - FIN TUG: Institute for Internal Combustion Engines and Thermodynamics, Tech. University Graz - A IFP: Institut Français du Pétrole - F AEA: AEA Technology plc - UK JRC: European Commission Joint Research Centre - NL REGIENOV: REGIENOV - RENAULT Recherche Innovation - F INRETS: Institut National de Recherche sur les Transports et leur Securité - F DEKATI: DEKATI Oy - FIN SU: Department of Analytical Chemistry, Stockholm University - S DHEUAMS: Department of Hygiene and Epidemiology, University of Athens Medical School - EL INERIS: Institut National de l Environment Industriel et des Risques - F LWA: Les White Associates - UK TRL: Transport Research Laboratory - UK VKA: Institute for Internal Combustion Engines, Aachen University of Technology - D 2

3 Publication data form 1. Framework Programme European Commission DG TrEn, 5 th Framework Programme Competitive and Sustainable Growth Sustainable Mobility and Intermodality 3. Project Title Characterisation of Exhaust Particulate Emissions from Road Vehicles (PARTICULATES) 5. Deliverable Title Particulate and PM characterisation in non-legislative conditions (cold start effects) 7. Deliverable Responsible 8. Language EMPA English 10. Author(s) Urs Mathis, Martin Mohr, with contributions of Claes DeServes (MTC-AVL) 2. Contract No 2000-RD Coordinator LAT/AUTh 6. Deliverable No Publication Date 8 April Affiliation EMPA 12. Summary Particle measurements were performed in the exhaust of five light-duty vehicles (Euro-3) at +23 C, - 7 C, and -20 C ambient temperatures. The characterization included measurements of particle number, active surface area, number size distribution, and mass size distribution. We investigated two port-injection spark-ignition (PISI) vehicles, a direct-injection spark-ignition (DISI) vehicle, a compressed ignition (CI) vehicle with diesel particle filter (DPF), and a CI vehicle without DPF. To minimize sampling effects, particles were directly sampled from the tailpipe with a novel porous tube diluter at controlled sampling parameters. The diluted exhaust was split into two branches to measure either all or only non-volatile particles. Effect of ambient temperature was investigated on particle emission at cold and warmed up engine. For the gasoline vehicles and the CI vehicle with DPF, the main portion of particle emission was found in the first minutes of the driving cycle at cold engine start. The particle emission of the CI vehicle without DPF was hardly affected by cold engine start. For the PISI vehicles, particle number emissions were superproportionally increased in the diameter size range from 0.1 µm to 0.3 µm during cold start at low ambient temperature. Based on the particle mass size distribution, the DPF removed smaller particles (dp< 0.5 µm) more efficiently than larger particles (dp> 0.5 µm). No significant effect of ambient temperature was observed when the engine was warmed up. Peak emission of volatile nanoparticles only took place at specific conditions and was poorly repeatable. Nucleation of particles was predominately observed during or after strong acceleration at high speed and during regeneration of the DPF. 13. Notes This is the final version. 14. Internet reference Key Words subzero temperatures, cold start, passenger cars 17. No of Pages 18. Price 64 FREE 16. Distribution statement FREE 19. Declassification date 8 April Bibliography NO 3

4 Table of Contents Publication data form... 3 Table of Contents Introduction Experimental Set up Vehicles Tests Fuel / lube oil Results and discussions Steady state tests (warm start) CADC (warm start) NEDC (cold and warm start) ACU (cold start) Summary Steady state tests Warm start at transient test cycles Cold start at transient test cycles

5 1 Introduction The PARTICULATES programme aims to improve the understanding of particulate emissions and to develop representative emission factors for road vehicles. In the first stage, a harmonised exhaust particulate sampling and testing protocol has been developed. This protocol has then been used to evaluate particulate emissions with a range of engine and vehicle technologies, exhaust aftertreatment technologies and fuels. This report describes the investigations on particulate emissions at subzero ambient temperatures and the cold start effect at these temperatures. The experimental studies were carried out on several light duty vehicles of different combustion technologies at EMPA and at MTC within the worktask 550. There has been some deviation in extent from the Technical Annex because of cancellation of AEAT s testing in this worktask. 2 Experimental 2.1 Set up The set up used at EMPA and MTC AVL is shown in Figure 1. To the standard set-up of the PARTICULATES programme a CPC (TSI model 3022) was added in the wet branch at EMPA. The instruments were operated according to the protocol as defined in Deliverable Figure 1. Overall experimental set-up: 1 Mass flow controller for the dilution air, 2 Probe, 3 Secondary diluter at the dry line, 4 Thermodesorber, 5 CPC (3022) (at EMPA only), 6 ELPI, 7 Ageing chamber for residence time, 8 Impactor for mass measurement at the wet line, 9 Secondary diluter at the wet line, 10 Diffusion charger (Matter Engineering), 11 CPC (3022), 12 DMA + CPC (for steady state tests instead of CPC). 5

6 2.2 Vehicles The vehicles tested at EMPA and MTC AVL are listed in Table 1 and Table 2. All vehicles were constructed 1998 or later and thus, they represent current engine and aftertreatment technologies. We especially investigated two direct-injection spark-ignition (DISI) vehicles and a particle trap equipped diesel vehicle. It is supposed that these technologies will achieve the market breakthrough in the next years. In this study, the Honda represents normal gasoline. However, from previous studies this ULEVvehicle is known to show considerably lower emissions as compared to other normal gasolines for both gaseous compounds as for particle emissions. Table 1. The tested vehicles at EMPA. vehicle 1 (Renault Mégane 16V) vehicle 2 (Alfa 406 TS 16V) vehicle 3 (Ford Galaxy TD) displacement [cm 3 ] number of cylinder maximum power at engine speed [kw] / [rpm] maximum torque at engine speed [Nm] / [rpm] 79 / / / / / / 1900 aftertreatment system three way catalyst three way catalyst oxidation catalyst emission class Euro 3 Euro 3 Euro 3 fuels Artemis Artemis D3 year of immatriculation odometer [km] combustion type spark ignition spark ignition compressed ignition injection type MPI MPI direct 6

7 vehicle 4 (Peugeot 406 HDI/FAP) vehicle 5 (Toyota Avensis) displacement [cm 3 ] number of cylinder 4 4 maximum power at engine speed [kw] / [rpm] maximum torque at engine speed [Nm] / [rpm] aftertreatment system 79 / / / / 4000 Oxi cat & particle trap three way catalyst emission class Euro 3 Euro 3 fuels D3 Artemis year of immatriculation odometer [km] combustion type compressed ignition spark ignition injection type direct direct stochiometric 7

8 Table 2. Vehicles tested at AVL MTC and their respective fuels. vehicle 6 vehicle 7 vehicle 8 vehicle 9 (Honda Accord) (Mitsubishi Carisma) (Peugeot 406 HDI) (VW Golf, TDI) Year of construction Mileage (km) Displacement (cm 3 ) Cylinders Max. power (kw/rpm) 110/ / / /4000 Aftertreatment TWC TWC, NO x # Oxidation cat Oxidation cat Emission class ULEV* Euro III Euro II Euro III Fuels G1, G3 G3 D2, D5 D2, D5 Combustion type SI SI CI CI Injection type MPI DISI common rail unit injectors * California ARB, Lev-1 # NO x adsorption catalyst 2.3 Tests The conducted test programme is listed in Table 3 and Table 4. All tests were usually run twice. If the results of these two test did not coincide a third or eventually a forth test was carried out. The real world CADC and the ACU cycle from the ARTEMIS project are depicted in Figure 2. While the CADC consists of an urban, road, and highway part, the ACU cycle composes of a sequence of 190 s with a speed up 45 km/h that is repeated 15 times. The NEDC composed of four ECE and an EUDC parts is depicted in Figure 3. For the ACU and NEDC the tests were started with the same lube oil temperature as the room temperature, i.e. so-called cold starts were run. For the steady state tests and the CADC the lube oil temperature was increased to at least 80 C by preconditioning, i.e. warm starts. At MTC the instrumentation was placed inside an insulated and heated box in order to keep the temperature constant at +20 C during the cold test cell tests. At EMPA the instrumentation was placed outside of the climate chamber at ambient temperature of about 20 C. 8

9 Table 3. Test programme at EMPA. Temperature in climate chamber [ C] Driving cycles Warm start Cold start Warm start Cold start Warm start Cold start ACU x x x CADC x x x 50 km/h x x 120 km/h x x Table 4. Test programme at MTC AVL. Temperature in climate chamber [ C] Driving cycle Warm start Cold start Warm start Cold start Warm start Cold start NEDC x x x x x x 9

10 speed [km/h] speed CADC bag number bag number [-] time [s] 45 speed ACU bag number speed [km/h] bag number [-] time [s] 0 Figure 2. The transient test cycles conducted at EMPA: the CADC (above) and the ACU cycle (below). 10

11 NEDC speed speed [km/h] time [s] Figure 3. The NEDC conducted at MTC-AVL. 2.4 Fuel / lube oil Diesel and gasoline fuels were supplied within Particulates. The specifications are presented in Table 5. The gasoline fuel used at EMPA was the fuel used within the Artemis project. The supplied lube oil from the PARTICULATES programme was used. Before the tests the lube oil filter was replaced by a new one. Prior to testing the lubricating oil was changed and aged at minimum 100 km of driving. 11

12 Table 5. Specifications for diesel and gasoline fuels. Gasoline Artemis Gasoline G1 Gasoline G3 Diesel D2 Diesel D4 Diesel D5 Density (g/l at 15 C) Viscosity (mm 2 /s) Flash point ( C) Cetan index Octan number (MON) Octane number (RON) Sulphur (ppm) Polyaromatics (mass-%) <0.1 Monoaromatics (mass-%) Aromatics (volume-%) EMPA MTC AVL MTC AVL MTC AVL EMPA MTC AVL 3 Results and discussions The data evaluation was conducted by means of the latest software version of an MS-Excel macro provided by LAT. The data of each instrument was evaluated for the whole cycle. The total particle concentration of the ELPI was considered for the lower seven stages. The total SMPS particle concentration was summed in the size range from 10 nm to 430 nm. The cascade impactor DGI divides the collected mass on five stages with the following size ranges: <0.2 µm, 0.2 to 0.5 µm, 0.5 to 1.0 µm, 1.0 to 2.5 µm and >2.5 µm. 3.1 Steady state tests (warm start) Vehicle 1 (Gasoline, MPI, 1.6 l) The particle concentration was low and neither a clear nucleation nor accumulation mode could be detected at both investigated constant speeds. An example of the number size distribution can be seen in Figure 4 at 20 C. No significant difference of the number size distribution was found at other chamber temperatures. The total particle concentrations as measured with DC, CPC, ELPI and SMPS are shown in Figure 5. The results of the gravimetric mass measurements with a conventional filter holder at the CVS tunnel and with the DGI filter holder at the wet branch are shown in Figure 6. The particle emissions were low at 50 km/h and no clear dependence of the chamber temperature could be identified. For most instruments a slight increase of the particle emissions were observed for the two lower temperatures 7 and 20 C. DC and DGI gravimetric mass do not show this trend. However, it is questionable if this observation is a real effect as the signal for all instruments were very close to the noise level. 12

13 1.40E E E+11 dn/dlogdp [1/km] 8.00E E E E+10 0E particle diametre dp [nm] Figure 4. Number size distribution for the vehicle 1 at 120 km/h steady state and -20 C. Two SMPS scans and the mean value of the particle number size distribution measured by ELPI are presented. 13

14 9 8 7 DC, wet +23, -20 C 50 km/h SMPS, wet +23, -20 C CPC, dry +23, -20 C ELPI, dry +23, -20 C 1.2E E+10 DC [cm 2 /km] E E E+09 CPC, SMPS, ELPI [1/km] E DC, wet 120 km/h SMPS, wet CPC, dry ELPI, dry 1.6E E E+11 DC [cm 2 /km] E E E E+10 CPC, SMPS, ELPI [1/km] 2 2.0E+10 0 Figure 5. Total particle concentration for vehicle 1. 14

15 1.8E E E-03 CVS, +23, -20 C 50 km/h DGI, +23, -20 C gravimetric mass [g/km] 1.2E E E E E E E-03 CVS, 120 km/h DGI, +23, C 2.0E-03 gravimetric mass [g/km] 1.5E E E-04 Figure 6. Gravimetric mass at CVS with conventional filter holder and wet branch with DGI filter holder for vehicle Vehicle 2 (Gasoline, MPI, 2.0 l) This vehicle showed clearly higher emissions than the other port-fuelled gasoline vehicle 1. At the constant speed of 50 km/h a weak mode in the range of about 50 nm was detected in the number size distribution for all investigated temperatures. Significant higher emission was found for 120 km/h at all temperatures, resulting in a clear mode in the size distribution. For example, the results are presented at 15

16 -20 C in Figure 7. No significant difference in the number size distribution was found at other chamber temperatures. The values for DC, CPC, total ELPI, and total SMPS concentrations are shown in Figure 8. The results of the gravimetric measurements from the CVS-tunnel with conventional filter holder and with the DGI filter holder at the wet branch are shown in Figure 9. The particle concentration were higher for the two lower temperatures at 50 km/h while there cannot be seen a trend at 120 km/h. The particle emissions at 120 km/h were more than an order of magnitude higher than at 50 km/h. 16

17 4.50E E km/h 3.50E+12 dn/dlogdp [1/km] 3.00E E E E E E+11 0E particle diametre dp [nm] 1.8E E km/h 1.4E+14 dn/dlogdp [1/km] 1.2E E E E E E particle diametre dp [nm] Figure 7. Number size distribution for vehicle 2 at 50 and 120 km/h steady state and 20 C. Three SMPS scans and the mean value of the particle number size distribution measured by ELPI are presented. 17

18 DC, wet 50 km/h SMPS, wet CPC, dry ELPI, dry 4.0E E E+12 DC [cm 2 /km] E E E E+12 CPC, SMPS, ELPI [1/km] E E+03 DC, wet SMPS, wet CPC, dry ELPI, dry 1.2E E km/h 1.0E+14 DC [cm 2 /km] 4.0E E E E E E+13 CPC, SMPS, ELPI [1/km] 1.0E E+13 Figure 8. Total particle concentration for vehicle 2. 18

19 1.4E E-03 CVS, 50 km/h DGI, +23, C gravimetric mass [g/km] 1.0E E E E E E-02 CVS, 120 km/h DGI, +23, C 1.0E-02 gravimetric mass [g/km] 8.0E E E E-03 Figure 9. Gravimetric mass at CVS with conventional filter holder and wet branch with DGI filter holder for vehicle Vehicle 3 (Diesel, DI, 1.9 l) For the conventional diesel vehicle without trap a clear accumulation mode was detected at 50 and 120 km/h for all three temperatures. Figure 10 shows the results for 20 C. No significant difference in the number size distribution was found at other chamber temperatures. The values for DC, CPC, total 19

20 ELPI, and total SMPS concentration are shown in Figure 11. The results of the gravimetric measurements from the CVS-tunnel with the conventional filter holder and with the DGI filter holder at the wet branch are shown in Figure E E E km/h dn/dlogdp [1/km] 2.50E E E E E+13 0E particle diametre dp [nm] 4.00E E E km/h dn/dlogdp [1/km] 2.50E E E E E+13 0E particle diametre dp [nm] Figure 10. Number size distribution for the vehicle 3 at 50 and 120 km/h steady state and 20 C. Three SMPS scans and the mean value of the particle number size distribution measured by ELPI are presented. 20

21 1.6E E+04 DC, wet SMPS, wet CPC, dry ELPI, dry 5.6E E E km/h 4.2E+14 DC [cm 2 /km] 1.0E E E E E E E E+14 CPC, SMPS, ELPI [1/km] 2.0E E E E+04 DC, wet +23, -20, -20 C 120 km/h SMPS, wet +23, -20, -20 C CPC, dry ELPI, dry +23, -20, -20 C +23, -20, E E E+14 DC [cm 2 /km] 2.0E E E E E E E+14 CPC, SMPS, ELPI [1/km] 5.0E E E+13 Figure 11. Total particle concentration for vehicle 3. 21

22 2.5E-02 CVS, 50 km/h DGI, +23, C 2.0E-02 gravimetric mass [g/km] 1.5E E E-03 gravimetric mass [g/km] 9.0E E E E E E E E-02 CVS, DGI, +23, C 120 km/h 1.0E-02 Figure 12. Gravimetric mass at CVS with conventional filter holder and wet branch with DGI filter holder for vehicle 3. At both speeds the particle emissions showed at +23 C chamber temperature the highest particle concentration for most instruments. This surprising result might be explained by different exhaust gas recirculation rates (EGR) at the different temperatures during the steady state tests. The level and the variation of the NO x and CO 2 concentration is depicted in Figure 13 at +23 and 20 C chamber temperature. While the EGR was stable at +23 C, the EGR was on a lower level at -20 C indicated by 22

23 lower CO 2 and higher NO X concentrations. The lower EGR at the subzero temperatures is most probably the explanation for the lower particle emissions. The effect of the EGR seemed to have a much larger effect on the particle emission than the effect of the combustion air temperature vehicle 3, 120 km/h, +23 C NOx CO NOx [ppm] CO2 [%] time [ms] 9.8 vehicle 3, 120 km/h, -20 C time [s]*0.1 NOx CO2 9.6 turn on EGR 300 turn off EGR 9.4 NOx [ppm] CO2 [%] time [s]*0.1 Figure 13. Varying of the NO x and CO 2 concentrations in the raw exhaust as a consequence of the EGR. 23

24 3.1.4 Vehicle 4 (Diesel, DI, 2.0, with particle trap) The SMPS measurements revealed no distinct size distributions for both speeds of 50 and 120 km/h and all three investigated temperatures due to very low particle concentration close to the noise level. As an example a typical particle distribution is shown in Figure 14. The values for DC, CPC, total ELPI, and total SMPS concentration are presented in Figure 15. The results of the gravimetric measurements from the CVS-tunnel with the conventional filter holder and with the DGI filter holder at the wet branch are shown in Figure 16. Due to the low particle concentration no clear trend of the temperature can be seen. 1.0E E E E+10 dn/dlogdp [1/km] 6.0E E E E E E particle diametre dp [nm] Figure 14. Number size distribution for the vehicle 4 at 120 km/h steady state and +23 C. Three SMPS scans and the mean value of the particle number size distribution measured by ELPI are presented. 24

25 DC, wet 50 km/h SMPS, wet CPC, dry ELPI, dry 4.8E E E+10 DC [cm 2 /km] E E E E+10 CPC, SMPS, ELPI [1/km] 2 6.0E DC, wet 120 km/h SMPS, wet CPC, dry ELPI, dry 4.8E E E+10 DC [cm 2 /km] E E E E+10 CPC, SMPS, ELPI [1/km] 2 6.0E+09 0 Figure 15. Total particle concentration for steady state tests for vehicle 4. 25

26 1.2E-02 CVS, DGI, +23, C gravimetric mass [g/km] 1.0E E E E km/h 2.0E-03 gravimetric mass [g/km] 5.0E E E E E E E E-03 CVS, 120 km/h DGI, +23, C 1.0E E-04 Figure 16. Gravimetric mass at CVS with conventional filter holder and wet branch with DGI filter holder for vehicle Vehicle 5 (Gasoline, DI, 2.0) For the DISI vehicle, wide particle distributions with weak accumulation mode at about 80 to 100 nm were detected for both speeds and all temperatures. The number size distributions as measured with SMPS and ELPI at 50 and 120 km/h and a chamber temperature of 20 C are shown in Figure 17. The 26

27 values for DC, CPC and total ELPI and SMPS concentration are shown in Figure 18. The results of gravimetric measurements from the CVS-tunnel with the conventional filter holder and at the wet branch with the DGI filter holder are shown in Figure 19. A clear increase of particle emission with decreasing chamber temperature was observed at 50 km/h. No temperature dependence was found at 120 km/h. 27

28 6.0E km/h 5.0E+13 dn/dlogdp [1/km] 4.0E E E E E particle diametre dp [nm] 120 km/h 5.0E+13 dn/dlogdp [1/km] 4.0E E E E particle diametre dp [nm] Figure 17. Number size distribution for the vehicle 5 at 50 and 120 km/h steady state and -20 C. Three SMPS scans and the mean value of the particle number size distribution measured by ELPI are presented. 28

29 1.0E+03 DC, wet SMPS, wet CPC, dry ELPI, dry 1.5E E km/h 1.2E+13 DC [cm 2 /km] 6.0E E E E+12 CPC, SMPS, ELPI [1/km] 2.0E E E+03 DC, wet SMPS, wet CPC, dry ELPI, dry 4.0E E E+13 DC [cm 2 /km] 1.2E E km/h 2.4E E+13 CPC, SMPS, ELPI [1/km] 4.0E E+12 Figure 18. Total particle concentration for vehicle 5. 29

30 7.0E-03 CVS, DGI, +23, C gravimetric mass [g/km] 6.0E E E E E km/h 1.0E-03 gravimetric mass [g/km] 1.8E E E E E E E E E-03 CVS, 120 km/h DGI, +23, C Figure 19. Gravimetric mass at CVS with conventional filter holder and wet branch with DGI filter holder for vehicle CADC (warm start) In contrast to the steady state tests and the ACU cycle, volatile nanoparticles were observed for the CADC cycle. Volatile nanoparticles emission mainly occurred in the high-speed part after acceleration. In Figure 20 the representative sequences of the CADC cycle are marked. Volatile particles were observed for all vehicles and at all three chamber temperatures. 30

31 particle concentratio [1/cm3] 1.7E E E E E E E+07 bag 1 bag 2 bag 3 vehicle 1, +23 C CPC, wet branch volatile nanoparticles speed [km/h] 2.1E Time [s] CPC, dry branch 1.2E+09 bag 1 bag 2 bag E+09 vehicle 2, +23 C volatile nanoparticles 140 particle concentration [1/cm3] 9.0E E E E E+08 CPC, wet branch speed [km/h] 1.5E Time [s] CPC, dry branch Figure 20. Occurrence of volatile nanoparticles within the CADC cycle for vehicle 1 and 2 at chamber temperature +23 C. 31

32 3.2.1 Gasoline vehicles The results of the whole CADC cycle are shown in Figure 21 and Figure 22. The results of the ELPI and CPC in the dry branch do not show a significant influence on the chamber temperature for any tested vehicles. In the wet branch the particulate number highly fluctuated from test to test measured by the DC and CPC. No clear effect on the chamber temperature could be observed. The mass concentration for the vehicle 1 was so low that no consistent results could be obtained as presented in Figure 22. For the other two vehicles the variations were smaller, but no chamber temperature dependence could be identified. Vehicle 1 had the lowest particle emissions of all vehicles. The mass concentration was about one order of magnitude lower than for vehicle 2 and vehicle 5. Also the particle number emissions in the wet and dry branch were about one order of magnitude lower than for vehicle 2 and 5. In good agreement to the steady state tests at 120 km/h the conventional gasoline vehicle 2 had particle emission comparable with DISI (vehicle 5). While vehicle 5 had especially higher number of volatile nanoparticles the particle number in the dry branch were general more than double as much for vehicle 2 as for vehicle 5. Since no chamber temperature dependence could be found for the warm start measurements of the CADC test cycle no separate temperature splitting of the urban, road and motorway part were carried out. In Figure 23 the mean values and standard deviations of all investigated CADC over all temperatures are presented for all gasoline vehicles. The high deviations from the mean value were caused by the occurrence of volatile nanoparticles in the wet branch. Therefore, low deviations were found in the dry branch. 32

33 1.2E+02 DC, wet +23, -7, -7, -20, -20 C CPC, wet +23, -7,-7, C CPC, dry +23, -7,-7, C ELPI, dry +23, -7,-7, C 1.2E+13 DC [cm 2 /km] 1.0E E E E+01 vehicle 1 gasoline 1.0E E E E+12 CPC, ELPI [1/km] 2.0E E E E E+03 DC, wet +23, +23, -7,-7, C CPC, wet +23, +23, -7,-7, C CPC, dry +23, +23, -7,-7, C ELPI, dry +23, +23, -7,-7, C vehicle 2 gasoline 1.4E E E+14 DC [cm 2 /km] 2.4E E E E E E+13 CPC, ELPI [1/km] 6.0E E E E E+04 DC, wet +23, +23, -7,-7, C CPC, wet +23, +23, -7,-7, C CPC, dry +23, +23, -7,-7, C ELPI, dry +23, +23, -7,-7, C vehicle 5 gasoline 4.0E E E+14 DC [cm 2 /km] 2.0E E E E E E E+14 CPC, ELPI [1/km] 5.0E E+13 Figure 21. Particle emission over the whole CADC cycle for the gasoline vehicles. 33

34 1.8E E E-03 CVS, +23, -7, -7, -20, -20 C vehicle 1 gasoline DGI, +23, -7, -7, -20, -20 C gravimetric mass [g/km] 1.2E E E E E E E-02 CVS, +23, +23, -7, -7, -20, -20 C DGI, +23, +23, -7, -7, -20, -20 C gravimetric mass [g/km] 1.0E E E E-03 vehicle 2 gasoline 2.0E E-02 CVS, +23, +23, -7, -7, -20, -20 C DGI, +23, +23, -7, -7, -20, -20 C gravimetric mass [g/km] 1.2E E E E E-03 vehicle 5 gasoline mass distribution [%] 2.0E-03 Figure 22. Gravimetric mass over the whole CADC cycle for the gasoline vehicles. The mass size distribution of the DGI is the mean value over all tests. 34

35 3.6E E E+02 DC, wet urban, road, motorway CPC, wet urban, road, motorway CPC, dry urban, road, motorway ELPI, dry urban, road, motorway vehicle 1 gasoline 5.4E E E E E+13 DC [cm 2 /km] 2.0E E E E E E+13 CPC, ELPI [1/km] 8.0E E E E E E E+03 DC, wet urban, road, motorway CPC, wet urban, road, motorway CPC, dry urban, road, motorway ELPI, dry urban, road, motorway vehicle 2 gasoline 2.0E E E E E+14 DC [cm 2 /km] 3.0E E E E E E E E+13 CPC, ELPI [1/km] 1.0E E E E E E E+04 DC, wet urban, road, motorway CPC, wet urban, road, motorway CPC, dry urban, road, motorway ELPI, dry urban, road, motorway vehicle 5 gasoline 6.0E E E E E+14 DC [cm 2 /km] 1.5E E E E E E E E+14 CPC, ELPI [1/km] 5.0E E E E+13 Figure 23. Mean values over all measured CADC cycles of the urban, road and motorway part. The values from the CPC in the dry branch have not been calculated yet. 35

36 3.2.2 Diesel vehicles The results of the whole CADC cycle are shown in Figure 24 and Figure 25. Similar to the gasoline vehicles no chamber temperature dependence on the particle emissions could be detected. Fluctuations were mainly seen for the volatile nanoparticles and were more pronounced for the vehicle 4 with particle trap than for vehicle 3. While in the urban part no volatile particles were observed, the particle concentration in the wet branch were found to be two and four order of magnitude higher compared to the dry branch for the road and motorway part, respectively. However, the total nanoparticle emissions, obviously dominated by volatile ones, were still lower than for vehicle 3. The particle number emissions were about two to three orders of magnitude lower than for vehicle 3 and about one to two order of magnitude lower than for the gasoline vehicles in the dry branch. The diesel vehicle with trap showed a clear temperature dependence on the mass emissions resulting to about six times higher mass concentration for 20 C compared to +23 C. Nevertheless, the mass concentration emitted by vehicle 4 was comparable low with a gasoline vehicle and thus, at least two orders of magnitude lower than for vehicle 3. In Figure 26 the mean values of all CADC cycles and their standard deviations are presented for each vehicle. Due to the low emission of vehicle 4 the deviations are especially high in the wet branch. In the regeneration phase of the motorway part the particle emissions were strongly increased. The main contribution came from volatile nanoparticles. 36

37 3.0E+04 DC, wet +23, -7,-7, C CPC, wet +23, -7,-7, C CPC, dry +23, -7,-7, C ELPI, dry +23, -7,-7, C 6.0E E+04 vehicle 3 diesel 5.0E+14 DC [cm 2 /km] 2.0E E E E E E+14 CPC, ELPI [1/km] 5.0E E E+02 DC, wet +23, +23, -7,-7, C CPC, wet +23, +23, -7,-7, C CPC, dry +23, +23, -7,-7, C ELPI, dry +23, +23, -7,-7, C 7.0E E E+02 vehicle 4 diesel 6.0E E+13 DC [cm 2 /km] 1.6E E E+01 DC [cm 2 /km] Trap regeneration at +23 C CPC wet 3.60E+03 DC 1.2E E E E E E+03 CPC 6.0E E+03 dry ELPI 4.0E E+02 dry 2.0E+14 0E+00 CPC, ELPI [1/km] 4.0E E E+13 CPC, ELPI [1/km] 4.0E E+13 Figure 24. Particle emission over the whole CADC cycle for the diesel vehicles. 37

38 7.0E-02 CVS, +23, -7, -7, -20, -20 C DGI, +23, -7, -7, -20, -20 C gravimetric mass [g/km] 6.0E E E E E E-02 vehicle 3 diesel 4.5E E E-03 CVS, +23, +23, -7, -7, -20, -20 C vehicle 4 diesel DGI, +23, +23, -7, -7, -20, -20 C gravimetric mass [g/km] 3.0E E E E E E-04 Figure 25. Gravimetric mass over the whole CADC cycle for the diesel vehicles. The mass size distribution of the DGI is the mean value over all tests. 38

39 4.0E E E+04 DC, wet urban, road, motorway CPC, wet urban, road, motorway CPC, dry ELPI, dry urban, road, motorway urban, road, motorway vehicle 3 diesel 7.0E E E E E+14 DC [cm 2 /km] 2.4E E E E E E+14 CPC, ELPI [1/km] 1.2E E E E E E E E E+02 DC, wet urban, road, motorway CPC, wet urban, road, motorway CPC, dry ELPI, dry urban, road, motorway urban, road, motorway vehicle 4 diesel 1.2E E E+13 DC [cm 2 /km] 1.8E E E E E+01 DC [cm 2 /km] 4.5E E E E E E E E+03 DC wet CPC wet CPC dry ELPI dry regeneration 1.8E E E E E E E E+14 CPC, ELPI [1/km] 8.4E E E E E+13 CPC, ELPI [1/km] 5.0E E E E E E+13 Figure 26. Mean values over all measured CADC cycles of the urban, road and motorway part. The values of the CPC in the dry branch have not calculated yet. 39

40 3.3 NEDC (cold and warm start) Emissions at different temperatures (cold start) The NEDC particle emissions for the vehicles at different temperatures are presented in Figure 27 to Figure 33 below. The Honda clearly showed higher emissions at lower temperatures with an increase of about 100 times from +22 C to 7 C for the G1 fuel (Figure 27) and even higher at 15 C. It was expected to find the emissions from the low-sulphur fuel (G3) to be lower than the G1-fuel but this was not seen. Increased particle emission was also found for the DISI at lower temperatures, but the effect was not as pronounced as for the Honda. The cold temperature effect to the particle emissions for the diesel vehicles was much less pronounced as compared to the two gasoline vehicles. However, the logarithmic scale in the figures tends to make the existing differences less obvious. Also an effect of fuel quality could be observed with lower emissions from the D5-fuel as compared to the D2 fuel. 1,0E+14 ELPI stages 1-7 CPC DC 1,0E+05 particle emission (#/km) 1,0E+13 1,0E+12 1,0E+04 1,0E+03 DC (cm2/km) 1,0E tem perature (C ) 1,0E+02 Figure 27. Honda particle emission over NEDC at different test cell temperatures using G1 fuel. 40

41 1,0E+14 ELPI, stages 1-7 CPC DC 1,0E+05 particle emission (#/km) 1,0E+13 1,0E+12 1,0E+04 1,0E+03 DC (cm2/km) 1,0E tem perature (C) 1,0E+02 Figure 28. Honda particle emission over NEDC at different test cell temperatures using G3 fuel. 1,0E+14 ELPI, stages 1-7 CPC DC 1,0E+06 particle emission (#/km) 1,0E+13 1,0E+12 1,0E+05 1,0E+04 DC (cm2/km) 1,0E tem perature (C) 1,0E+03 Figure 29. DISI particle emission over NEDC at different test cell temperatures using G3 fuel. 41

42 1,0E+15 ELPI, stages 1-7 CPC DC 1,0E+05 particle emission (#/km) 1,0E+14 DC (cm2/km) 1,0E tem perature (C) 1,0E+04 Figure 30. Peugeot particle emission over NEDC at different test cell temperatures using D2 fuel. 1,0E+15 E L PI, stages 1-7 CPC DC 1,0E+05 particle emission (#/km) 1,0E+14 DC (cm2/km) 1,0E tem perature (C ) 1,0E+04 Figure 31. Peugeot particle emission over NEDC at different test cell temperatures using D5 fuel. 42

43 1,0E+15 ELPI, stages 1-7 CPC DC 1,0E+06 particle emission (#/km) 1,0E+14 1,0E+05 DC (cm2/km) 1,0E temperature (C) 1,0E+04 Figure 32. VW Golf particle emission over NEDC at different test cell temperatures using D2 fuel. 1,0E+15 ELPI, stages 1-7 CPC DC 1,0E+06 particle emission (#/km) 1,0E+14 1,0E+05 DC (cm2/km) 1,0E tem perature (C) 1,0E+04 Figure 33. VW Golf particle emission over NEDC at different test cell temperatures using D5 fuel Mass measurements (cold start) According to the Particulates protocol particulate mass emissions were measured by two different methods: regulated filter measurements were performed in the CVS tunnel, a five stage gravimetric impactor (DGI) was used in the Particulates system. The results from the duplicate NEDC measurements at three different temperatures are presented in Figure 34 to Figure 37 below. In parallel to the number emissions presented in Figure 27, the Honda showed increasing emissions for lower temperatures. The emissions were very low, 1-2 mg/km, at +22 C but approached the levels of the 43

44 diesel vehicles when operated at -15 C. The other gasoline vehicle, the Mitsubishi, also showed a trend towards increasing emissions at lower ambient temperature. However, since the data only included one measurement at -15 C and the measurements at -7 C were very different from each other, the conclusion is not clear. The most stable vehicle was the Peugeot 406 HDi showing only minor or no effect for the low temperature measurements for the low sulphur fuel (D5) while the D2 fuel showed double the emissions at -15 C as compared to the higher temperatures. The VW Golf showed a similar trend as encountered for the Peugeot, but more pronounced, with increasing emissions at lower temperatures and a larger effect for D2 as compared to D5. Thus, the general conclusions drawn that the emissions from normal gasoline vehicles, such as the Honda, showed a large dependence for ambient temperatures as compared to diesel vehicles holds. Higher emissions were generally encountered for high sulphur fuels as compared to low sulphur fuels. Also the temperature dependence was stronger for the high sulphur fuels. 0,05 DGI_G1 CVS_G1 DGI_G3 CVS_G3 particulate emission (g/km) 0,04 0,03 0,02 0,01 0, temp (C) Figure 34. NEDC particulate emissions for the Honda Accord using two fuels at three temperatures. 44

45 0,05 DGI CVS particulate emission (g/km) 0,04 0,03 0,02 0,01 0, temp (C) Figure 35. NEDC particulate emissions for the Mitsubishi Carisma at three temperatures (G3- fuel). particulate emission (g/km) 0,12 0,10 0,08 0,06 0,04 0,02 DGI_D2 CVS_D2 DGI_D5 CVS_D5 0, temp (C) Figure 36. NEDC particulate emissions for the Peugeot 406 HDi using two fuels at three temperatures. 45

46 particulate emission (g/km) 0,12 0,10 0,08 0,06 0,04 0,02 DGI_D2 CVS_D2 DGI_D5 CVS_D5 0, temp (C) Figure 37. NEDC particulate emissions for the VW Golf TDI using two fuels at three temperatures Real time observations (cold and warm start) The real time observation was examined using of ELPI (examples are shown in Figure 38 and Figure 39). Even though the cold start effect was significant for the Honda, the concentrations for the cold and warm ECE were equal during the third and fourth ECE part of the cycle. For the VW Golf there was no observation of a cold start effect and the concentrations for the two tests were equal. These observations validated the assumption that the engine and exhaust system reached its operating temperature during the last two ECE of the cycle, which was further supported by the lubricating oil temperature that was observed to have reached stable values in the last two ECE. Thus, the approach to compare the first two ECE to the last two ECE emissions in order to study cold start effects was regarded as a useful method and was used in section

47 concentration (#/cm3) 1,0E+08 1,0E+07 1,0E+06 1,0E+05 1,0E+04 Cold ECE Warm ECE 1,0E time (s) Figure 38. Total ELPI concentrations during the four ECE for the Honda, G1 fuel at +22 C (the thin line represents the speed of the vehicle with a maximum at 50 km/h). 1,0 E+0 7 Cold ECE Wa rm EC E concentration (#/cm3) 1,0 E+0 6 1,0 E+0 5 1,0 E time (s) Figure 39. Total ELPI concentrations during the four ECE for VW Golf, D2 fuel at +22 C (the thin line represents the speed of the vehicle with a maximum at 50 km/h) Size distributions (cold and warm start) The cold start effect was examined by comparing particle emissions during the first two ECE with the third and fourth ECE at +22 C as measured by ELPI (Figure 40 to Figure 43). Clearly, there was a large difference in cold start effect between the Honda and the other cars. The Honda showed roughly 100 times higher emissions in the first two ECE as compared to the last two ECE while the effect for the other cars was minor or non-existing. This observation was in line with earlier studies showing more pronounced cold start effects for gasoline vehicles as compared to diesel vehicles both in regard to gaseous compounds as for particles. An interesting observation was that the other gasoline vehicle, the Mitsubishi, did not show a clear cold start effect. This may be explained by the more diesel like combustion in the DISI-engine of the Mitsubishi. 47

48 The absolute emissions deserve to be further commented. Even though the Honda showed increased emissions during the cold start, the emissions were more than 100 times lower as compared to what was observed from the diesel vehicles: and particles per km respectively. As the engine and exhaust system of the Honda reached operating temperature, the difference increased to more than a factor of The emission from the DISI was lower by roughly a factor of 10 as compared to the diesels, but considerably higher as compared to the Honda and, again, this may likely be explained by its diesel like characters. Cold UDC1 Warm UDC1 1,0E+12 dn/dlogdp km-1 1,0E+11 1,0E+10 1,0E+09 1,0E particle diameter (nm) Figure 40. Honda particle emissions by ELPI, G3 fuel at +22 C. 48

49 Cold UDC1 Warm UDC1 1,0E+14 dn/dlogdp km-1 1,0E+13 1,0E+12 1,0E+11 1,0E particle diam eter (nm ) Figure 41. Mitsubishi particle emissions by ELPI, G3 fuel at +22 C. Cold UDC1 Warm UDC1 1,0E+15 dn/dlogdp km-1 1,0E+14 1,0E+13 1,0E+12 1,0E particle diam eter (nm ) Figure 42. Peugeot particle emissions by ELPI, D2 fuel at +22 C. 49

50 Cold UDC1 Warm UDC1 1,0E+15 dn/dlogdp km-1 1,0E+14 1,0E+13 1,0E+12 1,0E particle diam eter (nm ) Figure 43. VW Golf particle emissions by ELPI, D2 fuel at +22 C Cold start ratios An useful approach to examine cold start effects is to take the ratio between the first two ECE for the cold and the warm start. This was done for the ELPI, the CPC, and the DC, respectively and then to compare between warm and cold cycle. The results from this comparison are presented in Table 6 to Table 8 representing measurements performed at ambient temperatures of +22 C, -7 C, and 15 C. Table 6. Ratio of ELPI, CPC, and DC mean values of duplicate measurements for cold and warm start of the first two ECE at +22 C (the parenthesis denotes cold emissions). Car Honda Accord Mitsubishi Carisma Peugeot 406 HDi VW Golf TDI ELPI, stages 1-7 Fuel ratio (#/km) G (7.20E+11) G (1.86E+12) G3 2.6 (4.04E+13) D2 1.2 (1.69E+14) D5 0.7 (7.66E+13) D2 1.2 (1.60E+14) D5 0.7 (9.75E+13) CPC ratio (#/km) 13.0 (1.48E+13) 58.1 (9.42E+13) 2.6 (1.25E+14) 1.5 (4.09E+15) 0.8 (1.55E+15) 1.2 (3.45E+15) 0.6 (1.61E+15) DC ratio (cm 2 /km) (1.97E+03) (4.26E+03) 1.4 (5.15E+04) 1.5 (1.41E+05) 0.7 (6.55E+04) 1.3 (1.62E+05) 0.7 (8.63E+04) 50

51 By looking at Table 6, a number of different conclusions may be drawn. For the two diesel cars the ratio was stable at around one, and hence, the conclusion may be drawn that the cold start effect was absent or minor for these vehicles at +22 C as was previously shown. For the Mitsubishi, an ELPI ratio 2.6 was found while the difference for the DC was minor. The observed ratios were larger than one and thus emissions were higher during the cold start as compared to the warm start. The situation was very much different for the Honda showing high ELPI ratios and a pronounced cold start effect, an effect that was even higher for the G3-fuel. At a comparison of the cold start effect at different test cell temperatures, the Honda showed a larger effect for lower temperatures. The trend was not clear for the GDI with a more pronounced cold start effect for successively lower cell temperatures. Finally, the diesel vehicles showed only small or no effects. Table 7. Ratio of ELPI, CPC, and DC mean values of duplicate measurements for cold and warm first of the first two ECE at -7 C (the parenthesis denotes cold emissions). Car Honda Accord Mitsubishi Carisma Peugeot 406 HDi VW Golf TDI ELPI, stages 1-7 Fuel ratio (#/km) G (6.16E+12) G (1.24E+13) G3 2.7 (4.12E+13) D2 1.1 (9.97E+13) D5 1.0 (7.35E+13) D2 0.7 (8.98E+13) D5 0.7 (1.11E+14) CPC ratio (#/km) (4.29E+14) (3.18E+14) 3.3 (1.76E+14) 0.7 (3.46E+15) 0.9 (1.64E+15) 0.7 (1.90E+15) 0.6 (1.86E+15) DC ratio (cm 2 /km) (4.27E+04) (4.10E+04) 3.2 (1.53E+05) 1.2 (9.59E+04) 1.2 (7.28E+04) 0.9 (1.22E+05) 0.8 (1.10E+05) 51

52 Table 8. Ratio of ELPI, CPC, and DC mean values of duplicate measurements for cold and warm of the first two ECE at -15 C (the parenthesis denotes cold UDC1 emissions). Car Honda Accord Mitsubishi Carisma Peugeot 406 HDi VW Golf TDI ELPI, stages 1-7 Fuel ratio (#/km) G (1.88E+13) G (2.25E+13) G3 2.5 (3.12E+13) D2 1.4 (1.26E+14) D5 0.9 (6.97E+13) D2 0.8 (1.44E+14) D5 0.7 (1.17E+14) CPC ratio (#/km) (1.24E+15) (4.91E+14) 2.4 (1.33E+14) 0.7 (2.94E+15) 0.6 (1.54E+15) 0.7 (2.52E+15) 0.7 (2.48E+15) DC ratio (cm 2 /km) (6.70E+04) (4.37E+04) 2.0 (8.43E+04) 1.6 (1.40E+05) 1.2 (7.11E+04) 0.9 (1.67E+05) 0.9 (1.31E+05) 3.4 ACU (cold start) Due to the cold start, particle emissions are expected higher in the starting phase than during the rest of the cycle. Especially, the existence of volatile particles (nucleation mode) was expected in the warming up phase. However, none of the tested vehicles emitted a significantly amount of volatile nanoparticles verified by comparison of the concentrations measured by two CPCs simultaneously running in the wet and dry branch. The integrated particle emission over the ACU cycle is presented in Figure 44. The particle number emissions as measured by a CPC in the wet branch is shown for all investigated temperatures. The two conventional gasoline vehicles (vehicle 1 and vehicle 2) emitted more than 90 % of the total particulate emissions in the first third (bag 1) of the ACU cycle at 7 and 20 C. At +23 C the percentage of the particle emissions differed for the two gasoline vehicle. While vehicle 1 still emitted about 85 % in the first part, vehicle 2 only emitted about 67 % in the first part. However, the total particle emissions over the whole cycle were nearly the same for both gasoline vehicles as shown in Figure 45. The diesel vehicle with the trap (vehicle 4) showed a drastic effect of the cold start. Similar to the conventional gasoline engines 85 % or more of the particles are emitted during the first third of the test cycle. The cold start effect was more pronounced for the subzero temperatures. Almost no influence of the cold start was observed for the conventional diesel vehicle (vehicle 3). The particle emission of the DISI (vehicle 5) showed a significantly lower effect on the cold start and on the temperature than the conventional gasoline vehicles. This demonstrates the more diesel-like particle formation of the DISI-technology. 52

53 % of integrated value C vehicle 1 vehicle 4 vehicle 2 vehicle 5 vehicle bag 1 bag 2 bag 3 % of integrated value Time [s] 100 vehicle 4 90 vehicle C 70 vehicle 2 vehicle vehicle bag 1 bag 2 bag Time [s] % of integrated value vehicle 4 vehicle 2 vehicle 1 vehicle 5 vehicle 3-20 C bag 1 bag 2 bag Time [s] Figure 44. Normalised integrated particle emissions over the ACU test cycle measured by CPC in the wet branch. 53

54 3.4.1 Gasoline vehicles A clear temperature effect could be identified for the three gasoline vehicles. When the temperature was decreased from +23 C to 7 C and 20 C, the particle emissions were clear increased as shown in Figure 45 and Figure 46. Although the two gasoline vehicles differed in the steady state test, the emissions in the ACU cycle were comparable at all three temperatures. The DISI vehicle (vehicle 5) emitted about double as many particles in number and about ten times more in mass as the conventional gasoline vehicles at chamber temperature 23 C. When the temperature was decreased to 7 and 20 C a clear increase of particle emissions could be found for all three gasoline vehicles. The mass size distribution indicated the highest mass in the second stage of the DGI (0.2 to 0.5 µm) for DISI (vehicle 5). While for the two conventional gasoline vehicles the highest mass was found in the first stage (< 0.2 µm). Therefore, the only slight increase in number compared to mass of vehicle 5 can be explained by the higher particle diameter of vehicle 5 compared to the conventional gasoline vehicles Diesel vehicles The results of the two diesel vehicles (vehicle 3 and vehicle 4) are shown in Figure 47 and Figure 48. No clear tendency can be identified of the particle emissions as a function of chamber temperature. The results of vehicle 4 with the particle filter fluctuated stronger than those of the other vehicles, which is probably explained by its very low absolute emission level. The particle mass emission of vehicle 4 was about in the same order as the conventional gasoline vehicle and about one order of magnitude lower than for the conventional diesel. For particle number, the emissions of the vehicle with the trap (vehicle 4) were about one to two orders of magnitude lower compared to the conventional gasoline vehicles and about three orders of magnitude lower compared to the conventional diesel. 54

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