Receptor Modeling Source Apportionment for Air Quality Management John G. Watson (john.watson@dri.edu) Judith C. Chow Desert Research Institute Reno, Nevada, USA Presented at: The Workshop on Air Quality Management, Measurement, Modeling, and Health Effects University of Zagreb, Zagreb, Croatia 24 May 2007 Objectives • Review receptor models and data requirements • Summarize prior uses of receptor models in air quality management • Describe strategies for separating primary and secondary source contributions The First Receptor Model What you can see or smell Black Carbon (BC) Remains at Mesa Verde National Park, Colorado, USA • Not all BC is from diesel and other vehicular emissions • “Marker” is a better term than “tracer” • There’s something of everything in everything Source and Receptor Models The source model uses source emissions as inputs and calculates ambient concentrations. The receptor model uses ambient concentrations as inputs and calculates source contributions. (From Watson, 1979.) Lagrangian Source Model Cikl = ΣjΣmΣn TijklmnDklnFijQjkmn CALCULATED AT RECEPTOR CALCULATED BY CHEMICAL MODEL CALCULATED BY MET MODEL MEASURED AT SOURCE (INVENTORY) CMB Receptor Model Cikl = ΣjTijklFijΣmΣn DklnQjkmn MEASURED AT RECEPTOR MEASURED AT SOURCE (T=1 OR ESTIMATED BY OTHER METHOD Sijkl, SOURCE CONTRIBUTION ESTIMATE Chemical Mass Balance Equation: Ci Input: J F j1 ij Sj for i 1 to N • Ambient concentrations (Ci) and uncertainties (sCj), source profiles (Fij), and uncertainties (sFij). Output: • Source contributions (Sj) and uncertainties (sSj). Measurements: • Size-classified mass, elements, ions, and carbon concentrations on both ambient and source samples. CMB Solutions Minimize differences between calculated and measured values for overdetermined set of equations ϰ2 = minΣi [(Ci-Ci)2/ϭCi2] + ΣiΣi [(Fij-Fij)2/ϭFij2 ] Britt and Luecke, (1973), single sample, bold=true value ϰ2 =minΣi [(Ci-ΣjFijSj)2/(ϭCi2+ΣjϭFij2Sj2)] Effective Variance, Watson et al., (1984), single sample ϰ2 =minΣi [(Ci-ΣjFijSj)2/ϭCi2)] Ordinary Weighted Least Squares, Friedlander (1973), single sample Other CMB Solutions Sj=Ci/Fij Tracer solution, Hidy and Friedlander (1971), Winchester and Nifong (1971), single sample ϰ2 =minΣk [(Massk-ΣiCik/Fii)2] Multiple Linear Regression, Kleinman et al (1980), multiple samples ϰ2 =minΣi Σk [(Cik-ΣjFijSjk)2/ϭCik2)] Positive Matrix Factorization, Paatero (1997), multiple samples Receptor Models are Not Statistical • They don’t test hypotheses or determine statistical significance • Receptor models should be physically based with statements of simplifying assumptions and evaluation of deviations from assumptions • They infer mechanisms and interactions rather than explicitly calculate them • Receptor models recognize and elucidate patterns in measured components, space and time that bound the types, quantities, and locations of source contributions • Some of them explicitly use input data uncertainties to weight influence of inputs and estimate uncertainties of outputs Types of “Modern” Receptor Models • Chemical Mass Balance CMB with various solutions including marker (trace method, effective variance (EV), principal component analysis (PCA), UNMIX, abd positive matrix factorization (PMF) solutions • Aerosol Evolution and Equilibrium Estimates how reduction in one precursor will affect PM end-products • Back Trajectory estimates source areas for different pollutants or source contributions Chemical Mass Balance Equation: Ci Input: J F j1 ij Sj for i 1 to N • Ambient concentrations (Ci) and uncertainties (sCj), source profiles (Fij), and uncertainties (sFij). Output: • Source contributions (Sj) and uncertainties (sSj). Measurements: • Size-classified mass, elements, ions, and carbon concentrations on both ambient and source samples. Receptor Measurements from Ambient Samplers Airmetrics portable MiniVol sampler BGI FRM Omni PM2.5 and PM10 PM1, PM2.5, and PM10 Source profiles from source testing Many contributors not inventoried Real-World Cooking Simulated Cooking More source profiles could be obtained from certification tests Roadside compliance test in India Material balance says much about sources (Mexico City, Feb/Mar 1997) (Chow et al., 2002) Commonly measured elements, ions, and carbon (Zielinska et al., 1998) 10 1 0.1 0.01 Percent of PM2.5 Mass 10 1 0.1 0.01 Percent of PM2.5 Mass a) Fugitive Dust c) Gas Veh. Exhaust Average Abundance Average Abundance Ions, Carbon Fractions, Elements, and Inorganic Gases C hl o So N rid lu A S itra e b O le mm ulfate rg P o o t a t n e Bl nic assium a c C iu k ar m C bo a M S rbon ag od n Al nesium u m iu Ph inum os Sili m ph c o or n C S us Po hl ulfu ta orin r C ssiu e a T lc m Va itanium C na iu M hro dium an m m g a iu ne m se N Iron i C ck op el pe Ar Zin r Se se c l n B eni ic R romum u St bid ine Zi ron ium rc tiu C on m O arb Me ium xi on de m rcu s o L ry Su of no ead lfu nitr xid r d og e io en xi de C hl o So N rid lu A S itra e bl m u t O e m lfa e rg P o o t a t n e Bl nic assium a c C iu k ar m C bo a M S rbon ag od n n Al esium u m iu Ph inum os Sili m ph c o or n C Sul us Po hl fu ta orin r C ssiu e a T lc m Va itanium C na iu M hro dium an m m g a iu ne m se N Iro C i ck n op el pe A Z r Se rseinc l n B eni ic R romum u St bid ine Zi ron ium rc tiu C on m O arb Me ium xi on de m rcu s o L ry Su of no ead lfu nitr xid r d og e io en xi de Percent of PM2.5 Mass 1000 100 1000 100 C hl o So N rid lu A S itra e bl m u t O e m lfa e rg P o o t a t n e Bl nic assium ac C iu k ar m C bo a M S rbon ag od n n Al esium um iu Ph inum os Sili m ph c o or n C Sul us Po hl fu ta orin r C ssiu e a T lc m Va itanium C na iu M hro dium an m m ga iu ne m se N Iro C ick n op el pe A Z r Se rseinc l n B eni ic R romum u St bid ine Zi ron ium rc tiu C on m O arb Me ium xi on de m rcu s o L ry Su of no ead lfu nitr xid r d og e io en xi de C hl o So N rid lu A S itra e b O le mm ulfate rg P o o t a t n e Bl nic assium ac C iu k ar m C bo a M S rbon ag od n Al nesium um iu Ph inum os Sili m ph c o or n C S us Po hl ulfu ta orin r C ssiu e a T lc m Va itanium C na iu M hro dium an m m ga iu ne m se N Iron i C ck op el pe Ar Zin r Se se c l n B eni ic R romum u St bid ine Zi ron ium rc tiu C on m O arb Me ium xi on de m rcu s o L ry Su of no ead lfu nitr xid r d og e io en xi de Percent of PM2.5 Mass More specificity obtained with source profiles Variability 1000 100 b) Coal-Fired Boiler 0.001 0.001 0.0001 0.0001 Ions, Carbon Fractions, Elements, and Inorganic Gases Variability d) Hardwood Burning 0.001 0.001 0.0001 0.0001 Average Abundance Average Abundance Variability 7200±1400 10 1 0.1 0.01 Ions, Carbon Fractions, Elements, and Inorganic Gases 1000 100 Variability 10 1 0.1 0.01 Ions, Carbon Fractions, Elements, and Inorganic Gases PM2.5 Mass Fraction PM2.5 Mass Fraction PM2.5 Mass Fraction PM2.5 Mass Fraction 0.1 10 1 10 1 10 1 1 0.1 ClNO3SO4= NH4+ Na+ K+ OC1 OC2 OC3 OC4 OP OC EC1 EC2 EC3 EC TC Al Si P S Cl K Ca Ti Mn Fe Cu Zn As Se Br Rb Sr Pb Retene Indeno[123Benzo(ghi)p Coronene ster35 ster45 ster48 ster49 hop17 hop19 hop24 hop26 4_allyl_guaia levoglucosan palmitoleic palmitic acid oleic acid stearic acid cholesterol phthalic acid Norfarnesan Farnesane Norpristane Pristane Phytane (Chow et al. 2006) PM2.5 Mass Fraction Many toxic elements have been removed from emissions. Organic markers take their place 1 PVRD UNC 0.01 0.001 0.0001 GAS UNC 0.1 0.01 0.001 0.0001 DIESEL UNC 0.1 0.01 0.001 0.0001 COOK UNC 0.1 0.01 0.001 0.0001 10 BURNING UNC 0.01 0.0001 0.001 Carbon fractions have been found useful and can be obtained from existing samples (Watson et al., 1994) Gasoline-fueled vehicles Diesel-fueled vehicles Thermally-evolved material can be separated by chromatography and mass spectrometry Challenge is to extract information that separates sources Gasoline Coal power plant Diesel Roadside dust Examples of U.S. CMB Model Air Quality Findings and Results • Oregon wood stove emissions standard (Watson, 1979) • Midwest contributions to east coast sulfate and ozone (Wolff et al., 1977, Lioy et al., 1980, Mueller et al., 1983, Rahn and Lowenthal, 1984) • Washoe County, Nevada, stove changeout, burning ban, and “squealer” number (Chow et al., 1989) • California EMFAC emissions model revisions (Fujita et al., 1992, 1994) • SCAQMD (Los Angeles) grilling emission standard (Rogge, 1993) • SCAQMD (Los Angeles) street sweeper specification (Chow et al., 1990) Examples of U.S. CMB Model Air Quality Findings and Results (continued) • SCAQMD (Los Angeles) Chino dairy reduction (NH3) regulation (SCAQMD, 1996) • PM10 SIP implementation of wood burning, road dust, and industrial emission reductions (Davis and Maughan, 1984, Houck et al., 1981, 1982, Cooper et al., 1988, 1989) • Navajo Generating Station SO2 scrubbers (Malm et al., 1989) • Hayden Generating Station SO2 scrubbers (Watson et al., 1996) • Mohave Generating Station shutdown (Pitchford et al., 1999) • Denver Colorado urban visibility standard (Watson et al., 1988) 0% 0% 11% 19% Czech Republic PM2.5, winter '93 Worldwide PM Source Contribution Estimates by Chianjen, Taiwan, PM2.5, Feb/Mar '99 10% 23% 19% 3% 3% 0% 0% 3% 0% 0% 4% 18% Chemical Mass Balance (Chow and Watson, 2002) 0% 0% 24% 22% Toronto PM2.5, Summer '98 0%0% 19% 0% 0% 40% 11% Industry Transportation Vegetative Burning (RWC) Geological Marine aerosol/Sea salt Sulfate/Secondary ammonium sulfate Secondary ammonium nitrate Secondary organics Other/Unidentified 4% 63% 17% Sulfate/Secondary ammonium sulfate Secondary ammonium nitrate Secondary organics Other/Unidentified 2.5 Sihwa, Korea, PM , 1998-99 Measured PM2.5 mass = 12.4 µg/m3 17% PM2.5 mass = 48.2 µg/m3 3 PM2.5 mass = 51.1±2.8 µg/m Industry Transportation Vegetative burning (RWC) Geological Marine aerosol/Sea salt Sulfate/Secondary ammonium sulfate Secondary ammonium nitrate Industry Transportation Secondary organics Vegetative Burning (RWC) Geological Other/Unidentified Marine aerosol/Sea salt 6% 9% 29% 11% 3% 0% 0% 4% Industry Transportation Vegetative burning (RWC) Geological Marine aerosol/Sea salt Sulfate/Secondary ammonium sulfate Secondary ammonium nitrate Secondary organics Other/Unidentified 0% 6% 1% 16% 22% 63% PM2.5 mass = 35.6±2.7 µg/m3 PM2.5 mass = 12.4 µg/m3 Downtown Los Angeles PM10, 1995 Mexico City PM2.5, 1989-90 5% 0%0% 8% 0% 4% 10% 13% 0% 20% 36% 4% PM10 mass = 48.1±3.1 µg/m3 0%3% 10%1% 1% 0% 15% 19% 0% 14% 0% 0% 0% 24% 11% Antarctica PM10, 1995-97 South Africa PM2.5, winter '97 Industry Transportation Vegetative burning (RWC) Geological Marine aerosol/Sea salt Sulfate/Secondary ammonium sulfate Secondary ammonium nitrate Secondary organics Other/Unidentified 0% 1% 6% 0% 1% Industry Transportation Vegetative burning (RWC) Geological Marine aerosol/Sea salt Sulfate/Secondary ammonium sulfate Secondary ammonium nitrate Secondary organics Other/Unidentified Industry Transportation Vegetative Burning (RWC) Geological Marine aerosol/Sea salt Sulfate/Secondary ammonium sulfate Secondary ammonium nitrate Secondary organics Other/Unidentified 72% 50% PM2.5 mass = 118.9 µg/m3 15% PM2.5 mass = 126 µg/m3 57% PM10 mass = 3.4±0.2 µg/m3 Receptor Model Results Need to be Challenged CMB Sensitivity Test c c c Case PVRD GAS DIES 1a 2b 3a 4b 5a 6b 7a 8b 0 0 0 0.04±0.3 0 0 0 0 1.9±1.3 0 2.2±1.4 0 1.0±0.9 0 2.4±1.4 30±7 6.6±2.2 7.1±2.3 7.6±2.2 8.5±2.2 3.0±1.6 3.2±1.6 8.2±2.4 0 Source Contribution Estimates (µg/m3) by Source Type BURN-Hc BURN-Sc COOKc MARINEc AMSULc 16±3 15±3 18±2 17±2 19±3 18±2 5.8±6.2 7.0±6.4 37±3 36±3 10±6 0 20±5 23±6 21±6 25±6 23±5 24±6 - 0 0 0 0 0.49±0.12 0.49±0.12 0 0.05±0.20 1.1±0.4 1.3±0.3 1.1±0.4 1.3±0.4 1.3±0.3 1.4±0.3 1.0±0.4 0 AMNITc PMASSd R2e CHIf 18±2 18±2 18±2 18±2 18±2 18±2 18±2 17±2 92 94 89 91 110 109 77 85 0.96 0.98 0.96 0.97 0.88 0.91 0.92 0.97 0.6 0.7 0.6 0.7 3.0 4.1 1.2 0.4 a With organics. Without organics. c Source Types. d Percent mass explained by the model run e R-square f Chi-Square b (Chow et al. 2006) CMB Pseudo-Inverse Normalized (MPIN) (Chow et al. 2006) Matrix Species Code/Nameb NO3SO4= NH4+ Na+ K+ OC3 OC4 OC EC2 EC3 EC Al Si Cl K Fe Se Br Pb Indeno[123-cd]pyrene (INCDPY) Benzo(ghi)perylene (BGHIPE) Coronene (CORONE) 17α(H), 21β(H)-29-Hopane (HOP19) Levoglucosan (LEVGU) Syringaldehyde (SYRALD) Palmitoleic acid (PALOL) Oleic acid (OLAC) Cholesterol (CHOL) Norfarnesane (NORFAR) Farnesane (FARNES) Norpristane (NORPRI) Pristane (PRIST) Phytane (PHYTAN) GAS 0.00 0.00 0.00 -0.07 -0.04 -0.04 0.00 -0.07 0.06 0.01 -0.23 -0.09 0.55 0.03 -0.09 -0.19 0.00 0.13 0.03 0.54 0.93 1.00 0.57 0.05 0.08 -0.06 -0.02 -0.03 0.11 0.04 0.04 -0.02 -0.02 DIES 0.00 0.00 0.00 -0.06 0.00 0.02 0.04 -0.03 1.00 0.00 0.22 -0.07 -0.17 0.02 -0.07 -0.12 0.01 0.15 -0.01 -0.14 -0.16 -0.14 -0.02 0.06 0.10 0.00 -0.01 -0.02 0.07 0.11 0.23 0.01 0.18 BURN-H 0.01 0.00 -0.01 0.04 1.00 0.10 0.12 -0.01 0.37 -0.03 -0.51 -0.20 -0.27 0.21 0.58 -0.59 0.01 0.12 -0.01 0.00 0.09 0.13 0.09 0.50 0.73 -0.06 0.00 -0.05 0.06 0.06 0.10 -0.03 0.08 Source Code BURN-S COOK -0.01 0.00 0.00 0.00 0.01 0.00 0.09 0.10 0.00 -0.30 -0.20 0.52 0.00 0.14 -0.10 1.00 -0.64 -0.15 0.03 0.03 0.80 -0.17 0.43 -0.10 0.44 -0.10 -0.12 0.01 0.23 -0.24 1.00 -0.14 -0.01 0.00 -0.16 -0.03 -0.03 0.09 0.06 -0.05 -0.16 -0.03 -0.23 -0.06 -0.15 -0.07 -0.25 -0.08 -0.38 -0.11 -0.19 0.49 -0.08 0.20 -0.07 0.22 -0.09 -0.02 -0.09 -0.02 -0.20 0.02 -0.06 0.16 -0.13 -0.02 AMSUL -0.10 1.00 0.10 0.01 -0.06 0.00 -0.02 0.00 -0.16 0.00 -0.01 0.01 -0.08 -0.02 -0.03 0.03 0.00 -0.05 0.00 -0.08 -0.14 -0.15 -0.10 -0.04 -0.06 0.02 0.01 0.01 -0.03 -0.02 -0.04 0.01 -0.02 AMNIT 1.00 -0.18 0.92 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 -0.01 0.00 0.00 0.00 0.00 0.00 0.00 -0.01 -0.01 -0.01 -0.01 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 One Atmosphere (Gases and Particles) Also Works for Receptor Models (Gertler et al., 1996) Light Duty Emission Rates Heavy Duty Emission Rates Hourly (VOC) data provide temporal corroboration of emissions and reveal unknown sources Unknown event Morning traffic 200 150 100 50 Exhaust Liq. Gasoline Gasoline Vapor Industrial Biogenic CNG 18 12 6 8/21- 0 18 12 6 8/20- 0 CDT 18 12 6 8/19- 0 18 12 6 8/18- 0 18 12 6 0 8/17- 0 Contributions (mg/m3) (Houston, TX, 1993) (Lu, 1996) Unexpl. High Time Resolution is Desired Spikes indicate local sources (Watson and Chow, 2001) MER BC PED BC MER WS MER WD 360 15 270 10 180 5 90 0 0 0 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 Hour (CST) Wind Direction (WD) (deg from N) Black Carbon (BC) (µg/m3) & Wind Speed (WS) (m/s) b) Monday 3/10/97 20 Wind Direction is Suggestive for Local Sources Conditional Probability Function (CPF) for a Selenium Factor at the Pittsburg Supersite (Pekney et al., 2006) These must be associated with measured source profiles (Chen et al., 2006) 3 Source factors derived from ambient data by UNMIX and PMF High PM2.5 Period Average Contribution (g/m ) 10 1 0.1 0.01 1E-3 10 1 0.1 0.01 1E-3 10 1 0.1 0.01 1E-3 10 1 0.1 0.01 1E-3 10 1 0.1 0.01 1E-3 10 1 0.1 0.01 1E-3 10 1 0.1 0.01 1E-3 10 1 0.1 0.01 1E-3 Marine Zinc Resuspended Dust Agriculture Vegetative Burning Secondary Aerosol Motor Vehicle RWC Pb Cd Sr Br Se As Zn Ni Fe Mn Cr Va Ca K Si Al TC EC EC3 EC2 EC1 OC POC OC4 OC3 OC2 OC1 K+ Na+ T-NH3 NH4+ SO4= NO3ClPM2.5 Markers for Biogenic SOA (Pandis, 2001) • Pinic acid, pinonic acid, norpinic acid, and norpinonic acid are products of the oxidation of most monoterpenes • There are some (apparently) unique tracers: • Hydropinonaldehydes for α-pinene • Nopinone for β-pinene • 3-caric acid for carene • Sabinic acid for sabenene • Several of these compounds measured in field studies in forests (usually a few nanograms per cubic meter, sometimes as much as 0.1 µg m-3) SO4=/SO2 Ratio changes during Aerosol Aging (and should be Reflected in Source Profiles) (Watson et al., 2002) Back trajectories indicate source regions (Xu et al., 2006) Regression parameters for Grand Canyon National Park (2000–2002). Percent of time the parcel is in a horizontal grid cell based on back trajectories starting at 500 m. Receptor Models Can Estimate the Future in Some Circumstances 200% 200% 180% 180% Fractional Change in Particle Nitrate Concentration Fractional Change in Particle Nitrate Concentration (Denver, CO, 1997) (Watson et al., 1998) 160% 140% 120% 100% 80% 60% 40% 20% 0% 160% 140% 120% 100% 80% 60% 40% 20% 0% 0% 20% 40% 60% 80% 100% 120% 140% 160% 180% Fractional Change of Particle Plus Gas Ammonia Concentrations Effect of ammonia reductions on ammonium nitrate particles 200% 0% 20% 40% 60% 80% 100% 120% 140% 160% 180% Fractional Change of Particle Plus Gas Nitrate Concentrations Effect of nitric acid reductions on ammonium nitrate particles 200% Emission Reduction Effectiveness Long-Term Trends in SO2 Emissions and SO4= Levels (Malm et al., 2002) Murphy’s Law of Reproducibility “If reproducibility is a problem, just use one model” Mohave Generating Station contributions to Meadview sulfate (Pitchford et al., 1999) 1,000 MCMB TMBR HAZEPUFF CALPUFF-Dry 3 Sulfate Concentration (ng/m ) b) 800 DMBR TAGIT ROME CALPUFF-Clouds 600 400 200 0 8/5 8/6 8/7 8/8 8/9 8/10 8/11 8/12 8/13 8/14 8/15 Day in 1992 (Samples begin at 0700 and 1700 MDT) 8/16 Po o rly n- O & R d e e id en hi c oo d le e hi cl lw ve ve cl e hi cl e hi ve ve tia es el ol in di as es ro a tg e ol in so lin ga s ga ex h us t au st ex ha st st ha u ha u ex ex C bu rn oa Fu in l-f g g ire iti ve d po du w st er st at O th io er ns in R es du ta st ur rie an s Se N tc a co oo tu ra nd ki lg ng ar a Se y s am he co m at nd on in ar g iu y m am ni m tr on at iu e m su lfa te of f- ta r in ed FT P ol ds nt a ai C -m Source Contribution (%) Model discrepancies help to improve inventories PM2.5 Inventory/Receptor Model Comparison, Denver, CO (1997) (Watson et al., 2002) 50 Emissions Inventory 40 Receptor Model, %Total Receptor Model, %Primary 30 20 10 0 Source Category SIP Guidance “Weight of Evidence” Approach (EPA, 2001) • Form a conceptual model of the emissions, meteorology, and chemical transformations that are likely to affect exceedances • Develop a modeling/data analysis protocol with stakeholders consistent with available science, measurements, and the conceptual model • Construct and evaluate emission inventory for the domain as indicated by the conceptual model SIP Guidance “Weight of Evidence” Approach (continued) • Assemble and evaluate meteorological measurements for the domain • Apply source and receptor models and to determine contributions • Apply diagnostic tests and justify discarding results that are not physically reasonable SIP Guidance “Weight of Evidence” Approach (continued) • Modify the inventory to reflect different emission reduction strategies in consultation with stakeholders, and evaluate the effects of reductions at receptors • Make models, input data, and results available to others for external review • Judge the weight of evidence supporting or opposing the selected emission reduction strategy prior to implementation Receptor Model Needs: A Summary • Source properties that identify and quantify source contributions at a receptor (Daisey et al., 1986, Gordon et al., 1984) • Better designed networks (Chow et al., 2002, Demerjian, 2000) with respect to • • • • • • • Sampling locations Sampling periods Sample durations Particle sizes Precursor gases Chemical and physical components Meteorology Receptor Model Needs (continued) • Emissions profiles (with cooling and dilution including marker species and gases, (England et al., 2000) • More convenient availability and documentation of source profile and ambient data (U.S. EPA, 1999) • More evaluation, validation, and reconciliation of receptor and source modeling results (Javitz et al., 1988) References Cabada, J.C.; Pandis, S.N.; and Robinson, A.L. 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