Understanding and quantifying motor vehicle emissions with vehicle specific power and TILDAS remote sensing

Motor vehicles are one of the largest sources of air pollutants worldwide. Despite their importance, motor vehicle emissions are inadequately understood and quantified. This is due in part to large variations in individual vehicle emissions with changing operating conditions, and to significant differences between vehicles. To better relate emissions with operating conditions, a new parameter termed "specific power" (SP) is presented. SP is the instantaneous tractive power per unit vehicle mass. This parameter has three main advantages: it can be calculated from roadside measurements, it captures most of the dependence of light-duty vehicle emissions on driving conditions, and it is directly specified in emissions certification cycles. The dependence of CO, HC, and NOx emissions on SP is better than on several other commonly used parameters, such as speed, acceleration, power, or fuel rate. Using SP as the basic metric allows meaningful comparisons to be made between data from different remote sensing sites, dynamometer driving cycles, and emission models. Modem U.S. vehicles are likely to operate under commanded enrichment when SP exceeds the maximum value on the Federal Test Procedure (-22 kW/Metric Ton). This may allow transient high emissions to be screened out during future remote sensing campaigns. Remote sensing can address the problem of inter-vehicle differences by quickly and cheaply measuring the emissions of large numbers of vehicles. Here, a tunable infrared laser differential absorption spectrometer (TILDAS) remote sensor was used to gather the first on-road measurements of N20 and N02, and the first high precision measurements of NO. NO was detected with a sensitivity of 5 ppm, which allowed even Ultra Low Emission Vehicles to be measured. On-road accuracy was demonstrated by comparing the TILDAS results with the on-board measurements of a heavy-duty diesel truck (HDDT). The remote sensor could operate with an optical path length of 88 meters, more than five times that of competing instruments. The NO and N20 emission distributions of passenger cars (PCs) and light-duty trucks (LDTs) were found to be highly skewed, while the NO emission distribution for HDDTs was not. N20 emissions from PCs and LDTs are estimated to contribute between 0.5% and 0.9% to U.S. greenhouse gas emissions. Thesis supervisor: Gregory J. McRae Title: Bayer Professor of Chemical Engineering

[1]  Matsuo Odaka,et al.  Deterioration Effect of Three-way Catalyst on Nitrous Oxide Emission , 1998 .

[2]  Jana B. Milford,et al.  Air Quality Implications of Methanol Fuel Utilization , 1988 .

[3]  Robert M. Reuter,et al.  Fuel Effects in Auto/Oil High Emitting Vehicles , 1993 .

[4]  G. Bishop,et al.  On-road carbon monoxide emission measurement comparisons for the 1988-1989 Colorado oxy-fuels program , 1990 .

[5]  J. Seinfeld,et al.  Atmospheric Chemistry and Physics: From Air Pollution to Climate Change , 1998 .

[6]  Craig T. Bowman,et al.  Control of combustion-generated nitrogen oxide emissions: Technology driven by regulation , 1992 .

[7]  Michael D. Jack,et al.  Remote and On-Board Instrumentation for Automotive Emissions Monitoring , 1995 .

[8]  Edward S. Yeung,et al.  Pressure‐broadened linewidths of nitric oxide , 1976 .

[9]  Grigorios C. Koltsakis,et al.  CATALYTIC AUTOMOTIVE EXHAUST AFTERTREATMENT , 1997 .

[10]  Matthew P. Fraser,et al.  Detection of Excess Ammonia Emissions from In-Use Vehicles and the Implications for Fine Particle Control , 1998 .

[11]  Edward L. Glover,et al.  Identifying Excess Emitters with a Remote Sensing Device: A Preliminary Analysis , 1991 .

[12]  Gary A. Bishop,et al.  A cost-effectiveness study of carbon monoxide emissions reduction utilizing remote sensing , 1993 .

[13]  Barbara Zielinska,et al.  Real-world emissions and calculated reactivities of organic species from motor vehicles , 1996 .

[14]  A Sjödin,et al.  Estimations of real-world N2O emissions from road vehicles by means of measurements in a traffic tunnel. , 1995, Journal of the Air & Waste Management Association.

[15]  Lawrence R. Smith,et al.  Characterization of Exhaust Emissions from High Mileage Catalyst-Equipped Automobiles , 1982 .

[16]  G. Bishop,et al.  Enhancement of Remote Sensing for Mobile Source Nitric Oxide. , 1996, Journal of the Air & Waste Management Association.

[17]  R. Stephens,et al.  Remote Sensing Measurements of Carbon Monoxide Emissions from On-Road Vehicles , 1991 .

[18]  G. Bishop,et al.  Emission Characteristics of Mexico City Vehicles , 1992 .

[19]  James N. Braddock,et al.  IMPACT OF LOW AMBIENT TEMPERATURE ON 3-WAY CATALYST CAR EMISSIONS , 1981 .

[20]  Greg Yarwood,et al.  Revision of light-duty vehicle emission inventories using real-world measurements-auto/oil program, phase II , 1998 .

[21]  Jeanine Bonamy,et al.  Air broadened NO linewidths in a temperature range of atmospheric interest , 1983 .

[22]  Ronald K. Hanson,et al.  Laser diode wavelength-modulation spectroscopy for simultaneous measurement of temperature, pressure, and velocity in shock-heated oxygen flows. , 1993, Applied optics.

[23]  R. Hanson,et al.  Design of a diode-laser sensor to monitor water vapor in high-pressure combustion gases. , 1997, Applied optics.

[24]  U. Epa,et al.  Development of Speed Correction Cycles , 1997 .

[25]  A. Denny Ellerman,et al.  Analysis of post-Kyoto CO₂ emissions trading using marginal abatement curves , 1998 .

[26]  W. Hucho,et al.  Aerodynamics of Road Vehicles , 1987 .

[27]  William J. Kessler,et al.  Simultaneous water vapor concentration and temperature measurements using 1.31-micron diode lasers , 1996 .

[28]  M. Zahniser,et al.  A tunable diode laser system for the remote sensing of on-road vehicle emissions , 1998 .

[29]  Steven H Cadle,et al.  Real-World Vehicle Emissions: A Summary of the Seventh Coordinating Research Council On-Road Vehicle Emissions Workshop. , 1998, Journal of the Air & Waste Management Association.

[30]  Suresh T. Gulati,et al.  Catalytic Air Pollution Control: Commercial Technology , 1994 .

[31]  Harry C. Watson,et al.  Predicting Fuel Consumption and Emissions-Transferring Chassis Dynamometer Results to Real Driving Conditions , 1983 .

[32]  G. G. De Soete,et al.  The Effect of Aging on Nitrous Oxide N2O Formation by Automotive Three-Way Catalysts , 1991 .

[33]  J. Lennard-jones,et al.  Molecular Spectra and Molecular Structure , 1929, Nature.

[34]  J. E. Peterson,et al.  On-Road Hydrocarbon Remote Sensing in the Denver Area , 1993 .

[35]  G I Mackay,et al.  Measurement of NO2 and HNO3 in diesel exhaust gas by tunable diode laser absorption spectrometry. , 1987, Environmental science & technology.

[36]  Feng An,et al.  A Simple Physical Model for High Power Enrichment Emissions. , 1996, Journal of the Air & Waste Management Association.

[37]  John B. Heywood,et al.  Internal combustion engine fundamentals , 1988 .

[38]  J. Houghton Climate change 1994 : radiative forcing of climate change and an evaluation of the IPCC IS92 emission scenarios , 1995 .

[39]  B. Everitt,et al.  Statistical methods for rates and proportions , 1973 .

[40]  J. W. C. Johns,et al.  Absolute intensities in CO2: the 4.3- and 2.7-μm regions revisited , 1989 .

[41]  Laurence S. Rothman,et al.  The HITRAN molecular spectroscopic database and HAWKS (HITRAN atmospheric workstation) , 1998, Defense, Security, and Sensing.

[42]  Paul J. Crutzen,et al.  Nitrous oxide emissions from motor vehicles in tunnels and their global extrapolation , 1993 .

[43]  W. B. Petersen,et al.  Turbulent diffusion behind vehicles: Effect of traffic speed on pollutant concentrations , 1991 .

[44]  Gary A. Bishop,et al.  Infrared emission and remote sensing , 1992 .

[45]  Werner A. Stahel,et al.  Emission factors from road traffic from a tunnel study (Gubrist tunnel, Switzerland). Part I: concept and first results , 1995 .

[46]  J. W. C. Johns,et al.  Absolute intensity and pressure broadening measurements of CO2 in the 4.3-μm region , 1987 .

[47]  Markus W. Sigrist,et al.  Emission factors for ethene and ammonia from a tunnel study with a photoacoustic trace gas detection system , 1996 .

[48]  David D. Nelson,et al.  Infrared tunable diode laser measurements of nitrogen oxide species in an aircraft engine exhaust , 1995, Optics & Photonics.

[49]  Douglas R. Lawson,et al.  Comparison of Emission Inventory and Ambient Concentration Ratios of CO, NMOG, and NOx in California's South Coast Air Basin , 1992 .

[50]  R. Hanson,et al.  Rapid tuning cw laser technique for measurements of gas velocity, temperature, pressure, density, and mass flux using NO. , 1991, Applied optics.

[51]  James A. Miller,et al.  Mechanism and modeling of nitrogen chemistry in combustion , 1989 .

[52]  Peter Werle,et al.  A review of recent advances in semiconductor laser based gas monitors , 1998 .

[53]  H. Michaels,et al.  EMISSIONS OF NITROUS OXIDE FROM HIGHWAY MOBILE SOURCES: COMMENTS ON THE DRAFT "INVENTORY OF U.S. GREENHOUSE GAS EMISSIONS AND SINKS, 1990-1996" (MARCH 1998) , 1998 .

[54]  Ronald K. Hanson,et al.  Scanned- and fixed-wavelength absorption diagnostics for combustion measurements using multiplexed diode lasers , 1996 .

[55]  John Aurie Dean,et al.  Instrumental methods of analysis , 1951 .

[56]  Gudmund Smedler,et al.  Nitrous Oxide Formation Over Three-Way Catalyst , 1994 .

[57]  Steven H Cadle,et al.  Real-World Vehicle Emissions: A Summary of the Sixth Coordinating Research Council On-Road Vehicle Emissions Workshop. , 1997, Journal of the Air & Waste Management Association.

[58]  G. Bishop,et al.  Worldwide on-road vehicle exhaust emissions study by remote sensing. , 1995, Environmental science & technology.

[59]  Robert A. Harley,et al.  A Fuel-Based Inventory for Heavy-Duty Diesel Truck Emissions , 1998 .

[60]  D. D. Nelson,et al.  Air-Broadened Linewidth Measurements in the ν2 Vibrational Band of the Hydroperoxyl Radical , 1994 .

[61]  Tayfun E. Tezduyar,et al.  PARALLEL COMPUTATION OF INCOMPRESSIBLE FLOWS WITH COMPLEX GEOMETRIES , 1997 .

[62]  R. Hanson,et al.  Multiplexed diode-laser sensor system for simultaneous H2O, O2, and temperature measurements. , 1994, Optics letters.

[63]  Charles M. Urban,et al.  Exhaust Emissions from Malfunctioning Three-Way Catalyst-Equipped Automobiles , 1980 .

[64]  Robert F. Sawyer,et al.  MOBILE SOURCES CRITICAL REVIEW 1998 NARSTO ASSESSMENT , 2000 .

[65]  R. H. Barnard,et al.  Road Vehicle Aerodynamic Design: An Introduction , 1996 .

[66]  利久 亀井,et al.  California Institute of Technology , 1958, Nature.

[67]  G. Bishop,et al.  On-Road Evaluation of Inspection/Maintenance Effectiveness , 1996 .

[68]  John H. Seinfeld,et al.  Fundamentals of Air Pollution Engineering , 1988 .

[69]  Marc Ross,et al.  Real-World Emissions from Conventional Passenger Cars. , 1998, Journal of the Air & Waste Management Association.

[70]  G. Herzberg,et al.  Infrared and Raman spectra of polyatomic molecules , 1946 .

[71]  P. L. Kelley,et al.  Detection of Air Pollutants with Tunable Diode Lasers , 1971, Science.

[72]  S. Rogak,et al.  Gaseous emissions from vehicles in a traffic tunnel in Vancouver, British Columbia. , 1998, Journal of the Air & Waste Management Association.

[73]  Laurence S. Rothman,et al.  Intensities and collision-broadening parameters from infrared spectra: an update. , 1992 .

[74]  Alan W. Gertler,et al.  Comparison of MOBILE4.1 and MOBILE5 predictions with measurements of vehicle emission factors in Fort McHenry and Tuscarora mountain tunnels , 1996 .

[75]  J. A. Cole,et al.  Errors in grab sample measurements of N2O from combustion sources , 1989 .

[76]  Marc Ross,et al.  A Fuel Rate Based Catalyst Pass Fraction Model for Predicting Tailpipe NOx Emissions from a Composite Car , 1999 .

[77]  Philip L. Varghese,et al.  Tunable diode laser measurements on nitric oxide in a hypersonic wind tunnel , 1995 .

[78]  Toshio Kobayashi,et al.  A Review of CFD Methods and Their Application to Automobile Aerodynamics , 1992 .

[79]  Ilene Grabel,et al.  University of Denver , 1939 .

[80]  John C. Hilliard,et al.  Nitrogen Dioxide in Engine Exhaust , 1979 .

[81]  Howard Levinsky,et al.  4th International Conference on Technologies and combustion for a clean environment , 1997 .

[82]  David D. Nelson,et al.  Infrared tunable diode laser diagnostics for aircraft exhaust emissions characterization , 1994, Photonics West - Lasers and Applications in Science and Engineering.

[83]  Gary A Bishop,et al.  Motor Vehicle Emissions Variability. , 1996, Journal of the Air & Waste Management Association.

[84]  Matsuo Odaka,et al.  Methane and Nitrous Oxide (N20) Emission Characteristics from Automobiles , 1996 .

[85]  V. M. Devi,et al.  THE HITRAN MOLECULAR DATABASE: EDITIONS OF 1991 AND 1992 , 1992 .

[86]  M. J. Heimrich,et al.  Diesel NOx Catalytic Converter Development: A Review , 1996 .

[87]  H. Riveros,et al.  Carbon monoxide trend, meteorology, and three-way catalysts in Mexico City. , 1998, Journal of the Air & Waste Management Association.

[88]  Harold I. Schiff,et al.  Application of tunable diode laser spectroscopy to the real-time analysis of engine oil economy , 1992 .

[89]  Harold I. Schiff,et al.  The use of tunable diode laser absorption spectroscopy for atmospheric measurements , 1994 .

[90]  Remote Sensing OF VEHICLE EXHAUST EMISSIONS. , 1994, Environmental Science and Technology.

[91]  Roger Westerholm,et al.  Multivariate analysis of exhaust emissions from heavy-duty diesel fuels , 1996 .

[92]  David D. Nelson,et al.  Air-broadened linewidth measurements in the ν2 vibrational band of HOCl , 1997 .

[93]  Robert M Heavenrich,et al.  LIGHT-DUTY AUTOMOTIVE TECHNOLOGY AND FUEL ECONOMY TRENDS THROUGH 1996. , 1988 .

[94]  D Wehinger,et al.  SCHADSTOFFEMISSIONEN VON OTTOMOTOREN MIT GEREGELTEM DREIWEGEKATALYSATOR. MESSUNG UNTER BERUECKSICHTIGUNG DER SEKUNDAEREMISSION DISTICKSTOFFOXID , 1994 .

[95]  Michel Prigent,et al.  Nitrous Oxide N 2 O in Engines Exhaust Gases-A First Appraisal of Catalyst Impact , 1989 .

[96]  Robert M. Reuter,et al.  Effects of Gasoline Properties (T50, T90, and Sulfur) on Exhaust Hydrocarbon Emissions of Current and Future Vehicles: Speciation Analysis - The Auto/Oil Air Quality Improvement Research Program , 1995 .

[97]  G. Bishop,et al.  Method comparisons of vehicle emissions measurements in the fort mchenry and Tuscarora mountain tunnels , 1996 .

[98]  R. Rasmussen,et al.  Combustion as a source of nitrous oxide in the atmosphere , 1976 .

[99]  Bo Galle,et al.  ON-ROAD EMISSION FACTORS DERIVED FROM MEASUREMENTS IN A TRAFFIC TUNNEL , 1998 .

[100]  Michael P. Walsh Global trends in motor vehicle pollution control: a 1997 update , 1997 .

[101]  Craig A. Harvey,et al.  Assessment of Unregulated Emissions from Gasoline Oxygenated Blends , 1990 .

[102]  W. J. Koehl,et al.  Effects of Gasoline Composition on Vehicle Engine-Out and Tailpipe Hydrocarbon Emissions - The Auto/Oil Air Quality Improvement Research Program , 1992 .

[103]  R. Harley,et al.  Impact of Oxygenated Gasoline Use on California Light-Duty Vehicle Emissions , 1996 .

[104]  J C Chow,et al.  Validation of the chemical mass balance receptor model applied to hydrocarbon source apportionment in the southern california air quality study. , 1994, Environmental science & technology.

[105]  Juhani Laurikko,et al.  The Effect of Ambient Temperature on the Emissions of Some Nitrogen Compounds:A Comparative Study on Low-, Medium- and High-Mileage Three-Way Catalyst Vehicles , 1995 .

[106]  Steven H Cadle,et al.  Analysis of Remote Sensing Errors of Omission and Commission Under FTP Conditions. , 1996, Journal of the Air & Waste Management Association.

[107]  Gary A. Bishop,et al.  ON-ROAD REMOTE SENSING OF AUTOMOBILE EMISSIONS IN THE CHICAGO AREA, YEAR 1. , 1998 .

[108]  R. Moss,et al.  Climate change 1995 - impacts, adaptations and mitigation of climate change : scientific-technical analyses , 1997 .

[109]  A. Bouwman,et al.  Uncertainties in the global source distribution of nitrous oxide , 1995 .

[110]  Barbara Zielinska,et al.  Real-world automotive emissions—Summary of studies in the Fort McHenry and Tuscarora mountain tunnels , 1995 .

[111]  S. C. Davis,et al.  Transportation Energy Data Book: Edition 14 , 1994 .

[112]  G. Batchelor,et al.  An Introduction to Fluid Dynamics , 1968 .

[113]  M. P. Arroyo,et al.  Diode-laser absorption technique for simultaneous measurements of multiple gasdynamic parameters in high-speed flows containing water vapor. , 1994, Applied optics.

[114]  David T. Mage,et al.  Urban air pollution in megacities of the world , 1996 .

[115]  G. Bishop,et al.  Measuring the Emissions of Passing Cars , 1996 .

[116]  Harold I. Schiff,et al.  Some applications of NIR tunable diodes for remote sensing , 1996 .

[117]  Alan C. Eckbreth,et al.  Recent advances in laser diagnostics for temperature and species concentration in combustion , 1981 .

[118]  Jean M. Dasch,et al.  Nitrous Oxide Emissions from Vehicles , 1992 .

[119]  M. P. Arroyo,et al.  Absorption measurements of water-vapor concentration, temperature, and line-shape parameters using a tunable InGaAsP diode laser. , 1993, Applied optics.

[120]  C.E.I. Byrne,et al.  Aerodynamics of Road Vehicles — 4th edition. Edited by W-H. Hucho. SAE International, Warrendale, PA, USA. Materials Park, OH 44073-0002, USA 1998. 918 pp. Illustrated. £78. , 1999, The Aeronautical Journal (1968).

[121]  G. Bishop,et al.  On-Road Remote Sensing of Vehicle Emissions in Mexico , 1997 .

[122]  K. T. Knapp,et al.  An Experimental Evaluation of Remote Sensing-Based Hydrocarbon Measurements: A Comparison to FID Measurements. , 1996, Journal of the Air & Waste Management Association.

[123]  Brett C Singer,et al.  A Fuel-Based Motor Vehicle Emission Inventory. , 1996, Journal of the Air & Waste Management Association.

[124]  Masaru Hirata,et al.  Effect of Periodic Disturbance on Behavior of Ring Vortices in Axisymmetric Jet. , 1994 .

[125]  J. Seinfeld,et al.  Atmospheric Chemistry and Physics: From Air Pollution to Climate Change , 1997 .

[126]  Robert M. Reuter,et al.  Speciation and Calculated Reactivity of Automotive Exhaust Emissions and Their Relation to Fuel Properties - Auto/Oil Air Quality Improvement Research Program , 1992 .

[127]  Gary A. Bishop,et al.  Enhancements of Remote Sensing for Vehicle Emissions in Tunnels , 1994 .

[128]  J. Seinfeld RETHINKING THE OZONE PROBLEM IN URBAN AND REGIONAL AIR POLLUTION , 1991 .

[129]  Dennys E. Angove,et al.  Nitrous oxide formation during the reaction of simulated exhaust streams over rhodium, platinum and palladium catalysts , 1998 .

[130]  G. Bishop,et al.  Repair Avoidance and Evaluating Inspection and Maintenance Programs , 1998 .

[131]  G. Bishop,et al.  Automobile emissions are statistically gamma distributed. , 1994, Environmental science & technology.

[132]  G. Bishop,et al.  A hydrocarbon detector for the remote sensing of vehicle exhaust emissions , 1995 .

[133]  John D. Spengler,et al.  Particles in our air : concentrations and health effects , 1996 .

[134]  M. Allen,et al.  Diode laser absorption sensors for gas-dynamic and combustion flows. , 1998, Measurement science & technology.

[135]  孝蔵 藤井,et al.  NASA Ames Research Centerにおける数値流体力学研究 , 1985 .

[136]  J. M. Jameson,et al.  Quantitative Chemical Analysis , 1944, Nature.

[137]  G. Bishop,et al.  IR long-path photometry: a remote sensing tool for automobile emissions. , 1989, Analytical chemistry.

[138]  Robert Joumard,et al.  Changes in Pollutant Emissions from Passenger Cars Under Cold Start Conditions , 1996 .

[139]  Ralf Kurtenbach,et al.  Emission of nitrous oxide and methane from aero engines: monitoring by tunable diode laser spectroscopy , 1996 .

[140]  R. L. Hawkins,et al.  Energy levels, intensities, and linewidths of atmospheric carbon dioxide bands , 1992 .

[141]  P. Crutzen,et al.  Methane emission measurements in urban areas in Eastern Germany , 1996 .

[142]  A Goldman,et al.  The HITRAN database: 1986 edition. , 1987, Applied optics.