Particulate matter and groundlevel ozone are responsible for over 4 thousands premature deaths in the EU (traffic accidents for only 39 thousands) Voj
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1 2 th ETH Conference on Combustion Generated Nanoparticles Zurich, Switzerland, June 13-16, 16, 216 FTIR-PEMS, Mini-PEMS & Micro-PEMS: Extending portable on-board emissions monitoring systems to non-regulated pollutants and small engines Michal Vojtisek-Lom Lom, Vít t Beránek Faculty of Mechanical Engineering,, Czech Technical University in Prague michal.vojtisek@fs.cvut.cz (+42) Martin Pechout, Luboš Dittrich,, Michael Fenkl Faculty of Mechanical Engineering, Technical University of Liberec, CZC EU LIFE+ program, project MEDETOX - Innovative Methods of Monitoring of Diesel Engine Exhaust Toxicity in Real Urban Traffic (LIFE1 ENV/CZ/651) Vojtisek-Lom, 2th ETH Conference on Combustion Generated Nanoparticles, June 14, 216 1
2 Particulate matter and groundlevel ozone are responsible for over 4 thousands premature deaths in the EU (traffic accidents for only 39 thousands) Vojtisek-Lom, 2th ETH Conference on Combustion Generated Nanoparticles, June 14, 216 2
3 Problematic pollutants in engine exhaust Particles + secondary aerosol NO x + tropospheric ozone CO, benzene, lead no longer a problem New and emerging problems: NO 2 - formation in oxidation catalysts NH 3 - formation in reduction catalysts - formation in three-way catalysts when run rich Aldehydes oxygenated fuels (ethanol) Greenhouse gases N 2 O - NO x reduction catalysts (SCR, LNT) CH 4 - natural gas engines, LNT catalyst Vojtisek-Lom, 2th ETH Conference on Combustion Generated Nanoparticles, June 14, 216 3
4 Real-world emissions could be higher than during standardized tests (i.e., type approval) Optimization for type-approval conditions No EGR at full load Catalyst sized for low flow and too small for high loads Technology limits - low SCR temperature cold start, creep Malfunction & deterioration No one is watching Switching off EGR, LNT fuel / SCR urea injection Cycle beating strategy DPF removal, SCR deactivation, etc. Vojtisek-Lom, 2th ETH Conference on Combustion Generated Nanoparticles, June 14, 216 4
5 Problem compounded by downsizing & turbocharging: Relatively low torque at idle. Challenges of EU automobile diesel engines Euro 4 Skoda Fabia chassis dynamometer runs NEDC vs. full-power loaded accelerations Problem compounded by cold DOC during accelerations after long idle Maintaining adequate excess air competes with desire for additional torque NOx: Use of EGR competes with the desire for additional torque NOx PM Long idle / low load: DOC cooldown, combustion deterioration, high fraction of OC in PM NOx reduced by EGR? Vojtisek-Lom, 2th ETH Conference on Combustion Generated Nanoparticles, June 14, 216 5
6 Challenges of EU automobile gasoline engines Euro 4 Skoda Fabia engine dynamometer runs BMEP [MPa] 1,2 1,8,6,4 Air excess ratio (λ) Characteristic of λ ratio for gasoline,95,91,88 1,2 1,3,9 1,2 1,2,91 BMEP [MPa] 1,2 1,8 Reducing exhaust gas temperatures (catalyst protection) by fuel-rich operation at high rpm and at high loads Concentration of THC [ppm] for gasoline HC ,2 1,2 1 1,2 1,3 2 1,2 3 4,93 5 rpm 6,6,4, Stoichiometric operation rpm 6 Vojtisek-Lom, 2th ETH Conference on Combustion Generated Nanoparticles, June 14, 216 6
7 Role of on-board, real-world emissions measurement ON-BOARD INSTRUMENTATION OR CHASE VEHICLE Measurement of individual vehicles during real-world oepration Low to intermediate number of vehicles Wide variety of operating conditions HC HC [g/mile] [g/mile] REMOTE SENSING I/M PROGRAMS Inspection & maintenance Screening High number of vehicles Low cost Low precision LABORATORY EMISSIONS Research Engineering Type Approval High quality, high cost, Small number of vehicles test mileage test mileage HOURS / KM DRIVEN With PEMS, it is always necessary to match the instrumentation and test designs to what we want to find out. (Low-cost high-throughput vs. detailed high-accuracy measurement) Vojtisek-Lom, 2th ETH Conference on Combustion Generated Nanoparticles, June 14, 216 7
8 Early portable on-board emissions monitoring systems Vojtisek-Lom and Cobb 1997 Univ. of Pittsburgh, Exhaust flow inferred from engine data Leo Breton, US EPA, mid 9 s (US patent 6,148,656 filed 1999) Measured exhaust flow Vojtisek-Lom 1999 First commercially sold PEMS Vojtisek-Lom, 2th ETH Conference on Combustion Generated Nanoparticles, June 14, 216 8
9 PEMS acronym started to be used around 1998 by Matt Spears (US EPA), Chris Frey (NC State University), and others, o as a generic term for on-board monitoring system that is portable or at least transportable and can be easily fitted on a vehicle What is or should be PEMS now? Those on-board monitoring system that are portable? Only PEMS meeting type-approval legislation requirements, or also PEMS used for research, engineering and other purposes? On-board monitoring & sampling system (transportable) Dr. Jesse Tu, California Air Resources Board, PEMS workshop, UC Riverside, 211 Vojtisek-Lom, 2th ETH Conference on Combustion Generated Nanoparticles, June 14, 216 9
10 On-board monitoring & sampling system (not road-legal) Southwest Research Institute, Reno, NV, USA Foto by author, Pennsylvania Transportation Institute, 23 Vojtisek-Lom, 2th ETH Conference on Combustion Generated Nanoparticles, June 14, 216 1
11 On-board emissions monitoring system (high precision, low detection limit, more transportable than portable ) System VOEM Flemisch Technology Institute (VITO), Belgium Lenaers G., Pelkmans L. and Debal P. (23): The Realisation of an On-board Emission Measuring System Serving as a R&D Tool for Ultra Low Emitting Vehicles. Int. J. Veh. Design, Vol.31, No. 3, pp Vojtisek-Lom, 2th ETH Conference on Combustion Generated Nanoparticles, June 14,
12 Downsizing PEMS: Transport as carry-on luggage on airplane (Vojtisek-Lom and Allsop, SAE ) Compact design used for non-road engine tests (Lanni and Vojtisek-Lom, ETH 27) Vojtisek-Lom, 2th ETH Conference on Combustion Generated Nanoparticles, June 14,
13 Online real-world measurements qualitative PM on SI SAE SAE Installs on motorcycles to locomotives This example from a Euro 4 diesel car NOx [mg/s], PM*1 [mg/s], CO2 [g/s], speed [km/h] Miniature portable on-board emissions monitoring system (MiniPEMS( MiniPEMS) HC, CO, NO, NO 2, PM mass, PM length heated ionization fire detector undiluted raw exhaust (multiplied by intake air flow for comparison measurements) ~.1 mg/m3 sensitivity cheap (1 EUR) poor man s PEMS concept length length mean mobility diameter 1 1.E+4 1.E+5 1.E+6 1.E+7 14:13: 14:15: 14:17: 14:19: 14:21: Vojtisek-Lom, 2th ETH Conference on Combustion Generated Nanoparticles, June 14, ionization chamber length concentration [mm/cm3] Rapeseed oil no DPF Rapeseed oil with DPF Diesel fuel no DPF Diesel fuel with DPF Length vs. PN>23 nm with volatiles EEPS total number concentration > 23 nm [#/cm3] CO2 NOx PM*1 rpm km/h
14 Low-cost on-board system overview (Vojtisek-Lom and Cobb, CRC On-road vehicle emissions workshop, 1998) Engine ECU Measured concentrations HC, CO, CO2, NO, particulates Direct measurement Mass air flow, intake air pressure and temperature, engine rpm, vehicle speed, engine temperatures Diagnostic interface GPS position. Speed, altitude Time signal Aftertreatmemt Aftertreatmemt Time shift (delay) Determined experimentally η vol * M air * p intake * ω * displacement Q vzd = R * T intake Synchronization of data Harmonization of sample interval to 1 s 1. Exhaust gas flow calculations 2. Mass emissions = const. x concentration x exhaust flow 3. Fuel consumption = C emissions (PM, HC, CO, CO2) / C in fuel Integrating: Emissions per test, distance, kg of fuel Data recording Vojtisek-Lom, 2th ETH Conference on Combustion Generated Nanoparticles, June 14,
15 On-board system versatility: Motorcycle to locomotive Truck Battery 5 Hz GPS receiver Speed, position, altitude Intake air manifold absolute pressure Raw exhaust sampling point (no dilution) 29 Coliber Fartt scooter.49 liter carbureted engine Locomotive 163 liter diesel Special adapter fabricated and inserted before muffler (outside air penetrates well into tailpipe) Engine speed measured with optical tachometer Vojtisek-Lom, 2th ETH Conference on Combustion Generated Nanoparticles, June 14,
16 Motorcycle (scooter) test summary per km Emissions per km HC [g] Route length: approx. 13 km Start point altitude: 41 m Peak altitude: 66 m CO [g] Lowest point altitude: 38 m NOx [g] PM laser [mg] PM ion1 [km] PM ion2 [km] CO2 [g] Urban Rural Vojtisek-Lom, 2th ETH Conference on Combustion Generated Nanoparticles, June 14,
17 These ~2 mg of particles are not from a diesel engine, but from garden machinery! Full-flow dilution tunnel MiniPEMS Raw or diluted GPS Full-flow PM sampling Transfer line Vojtisek-Lom, 2th ETH Conference on Combustion Generated Nanoparticles, June 14,
18 Extending PEMS to small non-road engines: Off-board emissions monitoring system Full-flow dilution tunnel with particle sampling Device under test Transfer line Full-flow dilution tunnel Batteries Flow meter PM sampling MiniPEMS Raw or diluted Vojtisek-Lom, 2th ETH Conference on Combustion Generated Nanoparticles, June 14,
19 Lawnmower and weed-eater eater test summary Wolfgarden 4-cycle Briggs&Stratton US EPA Stage II Stiga 4-cycle Briggs&Stratton US EPA Phase 1 Mid-9's 4-cycle mower Weed-eater Stihl FS35 2-cycle PM [g/h] Pall TX4 filters 2-44 mg/filter Quartz fiber filters hundreds mg/filter PM [g/h] (mass deposited on filter) Vojtisek-Lom, 2th ETH Conference on Combustion Generated Nanoparticles, June 14,
20 FTIR (Fourier Transform Infra Red) Spectrometer - measures large portion of infrared spectra - quantification of compounds absorbing in IR through deconvolution of spectra - greenhouse gases CO2, CH4, N2O - reactive nitrogen compounds NO, NO2, NH3, HCN, HCNO - various heterogeneous molecules present in concentrations that can be detected and discerned from other compounds Moving mirror Beamsplitter x -x Fixed mirror Sample IR Source He-Ne laser Laser diode Detector H 2 O CH 4 CO 2 CO Different HC NO 2 NO H 2 O CO 2 NH 3 Diagram: Nicolet Vojtisek-Lom, 2th ETH Conference on Combustion Generated Nanoparticles, June 14, 216 2
21 There is a range of FTIR: Smaller and lighter but less resolution (i.e. Daham 25 Univ. Leeds Gasmet) and higher resolution, more sensitive, but less portable (i.e., Jetter 2, Nicolet / Honda) Daham B., Andrews G.E., Li H., Bellesteros R., Bell M., Tate J. and Ropkins K.; Application of a Portable FTIR for Measuring on road Emissions. SAE technical paper Jetter, J., Maeshiro, S., Hatcho, S., and Klebba, R., "Development of an On-Board Analyzer for Use on Advanced Low Emission Vehicles," SAE Technical Paper , 2, doi:1.4271/ Vojtisek-Lom, 2th ETH Conference on Combustion Generated Nanoparticles, June 14,
22 On-board FTIR tests, Euro 6 truck, 12 tons gross weight Portable FTIR: ~35 ~ kg, ~3 W,.5 cm - 1, 5 m cell, 13 C, t mobile FTIR: ~, 5 m cell, 13 C, t 1 FTIR: ~9 kg, ~6 W,.5 cm - 1, 6 m cell, 13 C, t ~3s 9 ~3s Batteries Charger Inverter Particle counter Portable FTIR project MEDETOX TU Liberec 3 tons of weights (total payload 3,5 t = 58%) 12 tons gross weight 9.5 tons actual weight Mobile FTIR (laboratory grade Nicolet Antaris IGS) Czech Techical Univ Prague Vojtisek-Lom, 2th ETH Conference on Combustion Generated Nanoparticles, June 14,
23 Student projects: Unregulated emissions - E85, n-butanol, isobutanol in unmodified gasoline engines in Škoda cars Nitrogen compounds speciation NO, NO 2, NH 3 Greenhouse gases N 2 O, CH 4, CO 2 Formaldehyde, acetaldehyde, other compounds or functional groups SAE SAE SAE On-board FTIR 6 m cell.5 cm-1 optical resolution ~ 3 kg, ~ 3-4 W 7-8 hours on ~6 kg of batteries Vojtisek-Lom, 2th ETH Conference on Combustion Generated Nanoparticles, June 14,
24 Euro 5 diesel car, LNT speed [km/h] NO [ppm], CH4 [ppm] CH4 [ppm] NOx [ppm] N2O [ppm] CO2 [%] LNT regenerations no LNT regeneration = higher NOx 13:4 13:45 13:5 13:55 14: 14:5 14:1 14:15 14:2 14:25 14:3 14:35 14: acceleration [m/s2] CO2 [%], N2O [ppm] LNT regeneration: spikes in CO 2 (> 14%) and CO Spikes in CH 4, N 2 O (otherwise negligible) No regeneration = saved fuel, high NO x Vojtisek-Lom, 2th ETH Conference on Combustion Generated Nanoparticles, June 14,
25 Škoda Octavia Euro 5 diesel, LNT FTIR-PEMS examination of RDE emissions of nitrogen species: NO, NO 2, NH 3, N 2 O TU Liberec to EC Joint Research Center (Ispra, Italy) About 8 hours of instrument run time (6:45 sampling time) (limited by battery and liquid nitrogen capacity) Germany (high speed) & Switzerland (hills and high altitude) Germany: km, 4: mg/km N 2 O 687 mg/km NO x 158 g/km CO 2 Switzerland: km, 1: mg/km NO x 14 g/km CO 2 Why is the car NO x -compliant in Switzerland but not in Germany??? Vojtisek-Lom, 2th ETH Conference on Combustion Generated Nanoparticles, June 14,
26 Škoda Octavia Euro 5 diesel, LNT speed [km/h] (1 m avg) Speed [km/h] NOx [g/km] per. Mov. Avg. (NOx 2.8 [g/km]) 2.4 elapsed distance [km] speed [km/h] (1 km avg) elapsed distance [km] NOx [g/km] 3.6 Speed [km/h] NOx [g/km] per. Mov. Avg. (NOx 2.8 [g/km]) NOx [g/km] (1 km avg) Vojtisek-Lom, 2th ETH Conference on Combustion Generated Nanoparticles, June 14,
27 Škoda Octavia Euro 5 diesel, LNT > 5 km of data, 1 point = 1 m average NO x vs. CO 2 NO x vs. speed NOx [g/km] Nox/CO2 1 segment average NOx [g/km] NOx [g/km] Nox/CO segment avg mg NOx / g CO2 segment average NOx [g/km] segment avg mg NOx / g CO segment average CO2 [g/km] segment average speed [km/h].1 NOx both absolute and per CO2 (per kg fuel) Exponentially increase with speed and with fuel consumption (g/km m CO2) Vojtisek-Lom, 2th ETH Conference on Combustion Generated Nanoparticles, June 14,
28 Škoda Octavia Euro 5 diesel, LNT > 5 km of data, 1 point = 1 m average 35 NOx [g/km] 35 Nox/CO2 segment CO2 [g/km] segment CO2 [g/km] segment average speed [km/h] segment average speed [km/h] NOx both absolute and per CO2 (per kg fuel) Exponentially increase with speed and with fuel consumption (g/km m CO2) Vojtisek-Lom, 2th ETH Conference on Combustion Generated Nanoparticles, June 14,
29 SOR CN12 Euro 6 diesel bus Hradčany any military airport Average emissions - Braunschweig cycle: 195 mg/km NO x. At 37 liters / 1 km, 22 g/kwh: 162 mg/kwh (Euro 6: 46 mg/kwh) Diesel car NOx limit: 18 mg/km Euro 5, 8 mg/km Euro 6 Diesel car real driving NOx: Euro 3-5: 1 mg/km One Euro 5 car = 1 mg/km = 5 buses!!! But 5 buses can transport 1x more people. Vojtisek-Lom, 2th ETH Conference on Combustion Generated Nanoparticles, June 14,
30 speed [km/h], fuel [dm3/h] SOR CN12 Euro 6 diesel bus Hradčany any military airport NO, NO2, N2O, NH3,..., CO, CO2, PM diesel: N2O > (NO+NO2) fuel-from-ecu [dm3/h] actual speed [km/h] NO [mg/s] N2O [mg/s] fuel-from-co2 [dm3/h] prescribed speed NO2 [mg/s] 14:14: 14:19: 14:24: 14:29: 14:34: 14:39: 14:44: 14:49: N2O, NO, NO2 [mg/s] CH4 (ppm) NO (ppm) NH3 (ppm) CNG: CH4, NO, NH3! Vojtisek-Lom, 2th ETH Conference on Combustion Generated Nanoparticles, June 14, 216 3
31 Moving towards biological metrics for PM: PETS (Portable exhaust toxicity samplers) We measure particles and sell fruits by count and mass. But the prices of fruits are not unified, neither per piece, neither per kg. Both volatiles and < 23 nm particles, excluded from EU PMP, can represent a significant share of toxicity I want my RDA of vitamin C of apples. Sorry. We sell fruits by mass. Choices: Sample -> extract -> expose to cells - proportional sampling done for gravimetric PM analysis Expose cells directly (exposure chamber) - no information about this done in a moving vehicle but technically feasible Vojtisek-Lom, 2th ETH Conference on Combustion Generated Nanoparticles, June 14,
32 EURO 3 no aftertreatment 23 Iveco Trakker Proportional exhaust particle sampling On-board measurement & sampling system Assessment of congestion and creep on the road Miniature partialflow dilution tunnel Particulate matter in exhaust [mg/m3] Speed [km/h] :3: 9:45: 1:: 1:15: 1:3: 1:45: congestion congestion Decrease in EGT Increase in PM after congestion EGT/1[C] PM [mg/m3] speed [km/h] congestion speed [km/h] EGT [C] -6 15:: 15:15: 15:3: 15:45: 16:: 16:15: 16:3: 16:45: 17:: Exhaust Gas Temperature at tailpipe [C] speed [km/h], exhaust temp. [C] 17 mg of PM collected on ~11 filters during a week of field measurement Vojtisek-Lom, 2th ETH Conference on Combustion Generated Nanoparticles, June 14,
33 Particle toxicity evaluation DNA adducts test (genotoxicity damage to DNA) Simple test, around 1 mg of particles needed (comparable to PAH analysis) cold idle cold takeoff cold drive city Effects of creep and congestion Euro 3 and 5 heavy diesel trucks cold idle cold takeoff cold drive city city congestion Sum-S9+ post-congestion Sum-S9- freeway Pooled sample Daily DPF all Euro 5 DOC+DPF city congestion post-congestion freeway Sum-S9+ Daily DPF all Pooled sample Sum-S9- Euro 5 DOC+DPF DNA adducts [1^8 per 1 dm3 of exhaust] DNA adducts [1^8 per mg of PM] Sum-S9+ city Sum-S9- congestion post-congestion freeway DNA adducts [1^8 per 1 dm3 of exhaust] Vojtisek-Lom, 2th ETH Conference on Combustion Generated Nanoparticles, June 14,
34 Micro-PEMS concept Inline module fitted at tailpipe NOx and particle concentrations, air-fuel ratio: Sensors used in heavy-duty diesel engines (engine management, OBD - on-board diagnostics,...) Other gaseous pollutants: Inline optical methods (tunable diode laser, NDIR, NDUV, NDvis) Exhaust flow: Pitot tube, ultrasonic, vortex sensors, or calculated from OBD data GPS, GSM or Wifi antenna: vehicle side or roof Power: Thermoelectric cells using exhaust heat, photovoltaics on roof cost: hundreds of EUR/CHF/USD some elements (NOx, flow) already in use TNO, Southwest research institute Vojtisek-Lom, 2th ETH Conference on Combustion Generated Nanoparticles, June 14,
35 (Lab) HiVol sampler Current work: MiniPEMS for small motorcycles (photo from PEMS validation & fuel effects testing) Mini PEMS (Lab) ELPI EEPS on-board FTIR NanoMet Vojtisek-Lom, 2th ETH Conference on Combustion Generated Nanoparticles, June 14,
36 Conclusions On-board emission measurement systems measure in/on a moving vehicle. Portable measurement systems (PEMS) can be readily transported and installed on a vehicle or mobile machinery. PEMS is a concept that can be extended to other metrics, measurement methods, and applications. On-board FTIR might allow for measurement of greenhouse gases (CO2, CH4, N2O), reactive nitrogen (NO, NO2, NH3), and other heterogeneous molecules present in concentrations that can be detected and discerned. MiniPEMS might allow real-world testing of small motorcycles & non-road engines Portable sampling and exposure systems for toxicity assays might allow for more direct assessment of effects of new fuels and technologies on human health. EU LIFE+ program, project MEDETOX - Innovative Methods of Monitoring of Diesel Engine Exhaust Toxicity in Real Urban Traffic (LIFE1 ENV/CZ/651)
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