2007 Progress Report: Emissions Inventory and Process Reconciliation Using Molecular Markers and Hybrid/Inverse Photochemical Modeling with Direct Sensitivity Analysis

EPA Grant Number: R831076
Title: Emissions Inventory and Process Reconciliation Using Molecular Markers and Hybrid/Inverse Photochemical Modeling with Direct Sensitivity Analysis
Investigators: Russell, Armistead G. , Odman, Mehmet Talat , Zheng, M.
Institution: Georgia Institute of Technology
EPA Project Officer: Chung, Serena
Project Period: November 1, 2003 through October 30, 2006 (Extended to September 30, 2008)
Project Period Covered by this Report: November 1, 2006 through October 30, 2007
Project Amount: $449,899
RFA: Measurement, Modeling, and Analysis Methods for Airborne Carbonaceous Fine Particulate Matter (PM2.5) (2003) RFA Text |  Recipients Lists
Research Category: Air , Air Quality and Air Toxics , Particulate Matter

Objective:

The objectives of the study are to:

  • Source apportionment of fine PM using an air quality model  and a receptor model
  • Identify the reasons of the discrepancy of sources of PM2.5 apportioned from the air quality model with those from the receptor model.
  • To assess and improve the emissions inventory for primary organic particulate matter in the eastern United States
  • To identify and quantify primary and secondary organic tracers in fine particulate matter (PM2.5) with optimal GC/MS (gas chromatography/mass spectroscopy) methodology
  • To study spatial and temporal variations of organic tracers in Atlanta, GA
  • To investigate chemical composition and source profiles of fine particulate matter (PM2.5) in an aged prescribed burning plume in GA.

Progress Summary:

1st Year:    In the 1st year, key information for CMAQ and a CMB model using organic molecular markers (CMB-MM) was prepared. For CMB-MM, the number of molecular markers applied in the model was optimized, silylation to the samples from the EPA eastern speciation sites was applied, and QA/QC analysis by studying the precision, accuracy, and recovery of organic tracer analysis using SRM 1649a was carried out. For air quality modeling, the important PM 2.5 emission sources were identified to select organic carbon tracers, the basic emission inventories were prepared, and source apportionment using CMAQ model was performed. Source apportionment results from CMAQ were further utilized to improve the emission inventories.

2nd Year: Quantitative uncertainty study of CMB-MM modeling using Monte Carlo approach was done. The results of Monte Carlo simulations indicated highest uncertainties in meat cooking: 136%, 116%, and 46% for normal distribution, lognormal distribution, and CMB-MM output, respectively. To reduce difference between TOR and TOT method, conversion factors of OC to EC ratios (OC/EC) were calculated using the Southeastern Aerosol Research and Characterization Study (SEARCH) samples, and CMB-MM was re-applied using improved OC/EC.  Based on CMAQ results, three major changes in emission inventories were made; 1) new point sources in Georgia, 2) new forest fire emissions using 2001 EPA temporal profiles and VISTAS forest fire emissions for 2002, and 3) correcting monthly distribution of area source emissions.

3rd Year:  In the 3rd year, field sampling at highway, urban, and rural sites during winter time and summer time in 2004 and 2005 were collected, and in-depth study on reconciliation between CMAQ and CMB model was performed. CMB modeling with locally optimized source-profiles, regional source apportionment of PM2.5 using CMAQ with the Decoupled Direct Method in 3D (DDM), and receptor-oriented sensitivity analysis using area of influence were performed.

4th Year: Tracers for biogenic secondary organic aerosol were analyzed for 2005 summer and 2006 winter periods. A source profile of prescribed burning was updated and it’s chemical composition was investigated. Scaling factors for PM2.5 emission inventories were estimated using the ridge regression analysis and CMAQ modeling was conducted for June 2005, July 2005 and January 2006 episodes using 36km, 12km and 4km grid sizes.

Future Activities:

  • To analyze PCM samples collected from heavy wildfires for primary and secondary organic tracers with the optimal GC/MS methodology
  • To build a source profile of wildfire emission through comparison of ambient concentrations between smoke events and non-smoke days
  • To analyze the correlations between inorganic tracers and organic tracers for a few major emissions and further study their stability during transports
  • To estimate scaling factors for primary PM2.5 emissions in 2005 summer and 2006 winter episodes
  • To estimate scaling factors for biogenic emissions in 2005 summer and 2006 winter episodes


Journal Articles on this Report : 4 Displayed | Download in RIS Format

Other project views: All 75 publications 40 publications in selected types All 40 journal articles
Type Citation Project Document Sources
Journal Article Marmur A, Unal A, Mulholland JA, Russell AG. Optimization-based source apportionment of PM2.5 incorporating gas-to-particle ratios. Environmental Science & Technology 2005;39(9):3245-3254. R831076 (2004)
R831076 (2007)
R831076 (Final)
R829213 (2006)
R829213 (Final)
R830960 (Final)
R832159 (2005)
R832159 (2006)
R832159 (2007)
R832159 (Final)
  • Abstract from PubMed
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  • Abstract: ES&T-Abstract
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  • Other: ES&T-Full Text PDF
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  • Journal Article Marmur A, Park S-K, Mulholland JA, Tolbert PE, Russell AG. Source apportionment of PM2.5 in the southeastern United States using receptor and emissions-based models:conceptual differences and implications for time-series health studies. Atmospheric Environment 2006;40(14):2533-2551. R831076 (2007)
    R831076 (Final)
    R829213 (Final)
    R830960 (Final)
    R832159 (2005)
    R832159 (2006)
    R832159 (2007)
    R832159 (Final)
  • Full-text: ScienceDirect-Full Text HTML
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  • Abstract: ScienceDirect-Abstract
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  • Other: ScienceDirect-Full Text PDF
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  • Journal Article Weber RJ, Sullivan AP, Peltier RE, Russell A, Yan B, Zheng M, de Gouw J, Warneke C, Brock C, Holloway JS, Atlas EL, Edgerton E. A study of secondary organic aerosol formation in the anthropogenic-influenced southeastern United States. Journal of Geophysical Research 2007;112(D13):D13302 (13 pp.). R831076 (2007)
    R831076 (Final)
    R830960 (Final)
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  • Other: AGU-Full Text PDF
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  • Journal Article Yan B, Zheng M, Hu YT, Lee S, Kim HK, Russell AG. Organic composition of carbonaceous aerosols in an aged prescribed fire plume. Atmospheric Chemistry and Physics 2008;8(21):6381-6394. R831076 (2007)
    R831076 (Final)
    R832159 (2007)
    R832159 (Final)
  • Full-text: ACP-Full Text PDF
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  • Abstract: ACP-Abstract
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  • Supplemental Keywords:

    source apportionment, CMAQ, CMB, organic molecular marker, trace metals,, RFA, Health, Scientific Discipline, Air, Ecosystem Protection/Environmental Exposure & Risk, particulate matter, Air Quality, air toxics, Environmental Chemistry, climate change, Air Pollution Effects, Risk Assessments, Monitoring/Modeling, Environmental Monitoring, Engineering, Chemistry, & Physics, Environmental Engineering, Atmosphere, carbon aerosols, air quality modeling, particle size, atmospheric particulate matter, health effects, aerosol particles, atmospheric particles, mass spectrometry, human health effects, ambient air monitoring, air modeling, air quality models, air sampling, gas chromatography, thermal desorption, carbon particles, air quality model, emissions, molecular markers, direct sensitivity analysis, particulate matter mass, human exposure, ambient particle health effects, particle phase molecular markers, photchemical modeling, aersol particles, particle dispersion, aerosol analyzers

    Progress and Final Reports:

    Original Abstract
  • 2004 Progress Report
  • 2005 Progress Report
  • 2006 Progress Report
  • Final Report