Final Report: Improved Treatment of Atmospheric Organic Particulate Matter Concentrations from Biomass Combustion Emissions

EPA Grant Number: R833747
Title: Improved Treatment of Atmospheric Organic Particulate Matter Concentrations from Biomass Combustion Emissions
Investigators: Kreidenweis, Sonia M. , Collett Jr., Jeffrey L. , Hao, Wei Min , Heald, Colette L. , Jimenez, Jose-Luis , Kroll, Jesse H. , Onasch, T. , Trimborn, Achim , Worsnop, Douglas R.
Institution: Colorado State University , Aerodyne Research Inc. , Fire Sciences Laboratory, Rocky Mountain Research Station
EPA Project Officer: Hunt, Sherri
Project Period: September 1, 2007 through December 31, 2010 (Extended to December 31, 2012)
Project Amount: $598,645
RFA: Sources and Atmospheric Formation of Organic Particulate Matter (2007) RFA Text |  Recipients Lists
Research Category: Air Quality and Air Toxics , Particulate Matter , Air

Objective:

We proposed to measure volatility distributions, for the first time via both isothermal dilution and thermal processing, of open biomass burning emissions for a variety of fuel types relevant to U.S. air quality. We proposed to interpret our data using semivolatile partitioning models, and to develop new biomass-burning emissions maps and partitioning models for use in large-scale model runs.

Summary/Accomplishments (Outputs/Outcomes):

We completed a series of experiments in which we generated open biomass burning emissions and subjected them to controlled dilution and thermal processing. The isothermal dilution scheme represents a new way of obtaining partitioning data that, to our knowledge, has not been previously attempted for biomass burning smoke. We measured the response of the aerosol mass concentrations and speciation to this processing in order to develop a database that can be used to characterize the volatility of the combustion emissions shown in Figure 1. We found differences in the gas/particulate partitioning behavior observed in isothermal dilution vs. thermal processing, with more evaporation at low aerosol concentrations observed under heating. We concluded that these differences most likely point to long timescales (minutes to hours) for gas-aerosol equilibration of some semivolatile components. Our analyses further revealed a wide variation in the emissions of OA from different fuels. However, when normalized to fractional emissions as a function of the absolute organic aerosol concentration, all smokes displayed surprisingly similar volatility behavior, with less than half of the initial emissions remaining in the particle phase at dilutions typical of the troposphere several hours downwind of the emissions source. Our findings show that organic particulate emissions from open biomass burning should be modeled as semivolatile, and the subsequent atmospheric fates of the evaporated organic species must be studied further so they can be accurately simulated. As demonstrated in piggyback studies carried out in tandem with our studies, these fates are likely to involve not only photochemical production of ozone, but also further oxidation of organic gases to form condensable species that contribute to atmospheric loadings of secondary organic aerosol.

The data from our studies will help improve models of biomass burning primary particulate emissions, including understanding how emissions vary during different burn phases. Improved representation of the role of biomass combustion in affecting ambient PM2.5 levels is expected to be a key contribution to improved understanding of the sources of atmospheric organic particulate matter, including secondary organic aerosol, and its impacts on air quality and health.

 

Figure 1: The fraction of condensable organic emissions measured in the particulate phase (Xp), for smoke produced in the combustion of the indicated fuels. The particulate-phase fraction is shown as a function of the absolute organic aerosol (OA) concentrations, which were adjusted via isothermal dilution in these experiments. The solid line is a fit through the data shown, whereas the dotted lines indicate best-fit (upper curve) and lower bound estimates of volatility from thermal processing of the smokes. Both methods clearly indicate that emitted organic aerosol mass is lost upon dilution; relative mass losses were similar among fuels tested, allowing one fit equation to be derived for all the biomass burning smokes. In general, more than half of the organic species initially emitted as particulate-phase material will evaporate to the gas phase by the time the plume is diluted to typical remote ambient concentrations. These gases are then available to participate in atmospheric chemical reactions, including photochemistry leading to ozone formation and oxidation reactions leading to formation of secondary organic aerosol. The emission factors (kg organic aerosol/kg dry fuel) at organic aerosol loadings of 104 µg m-3 are shown in the legend, demonstrating the wide range of total organic emissions from these different fuels. The findings will be used in air quality modeling to adjust total emission factors (“potential organic aerosol”) from burning of these fuels, and to predict the organic species mass concentrations remaining in the aerosol phase upon dilution of the smoke plumes.


Journal Articles on this Report : 22 Displayed | Download in RIS Format

Other project views: All 29 publications 22 publications in selected types All 22 journal articles
Type Citation Project Document Sources
Journal Article Bian Q, May AA, Kreidenweis SM, Pierce JR. Investigation of particle and vapor wall-loss effects on controlled wood-smoke smog-chamber experiments. Atmospheric Chemistry and Physics 2015;15(19):11027-11045. R833747 (Final)
RD834554 (Final)
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  • Journal Article Cappa CD, Jimenez JL. Quantitative estimates of the volatility of ambient organic aerosol. Atmospheric Chemistry and Physics 2010;10(12):5409-5424. R833747 (2010)
    R833747 (2011)
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  • Journal Article Cubison MJ, Ortega AM, Hayes PL, Farmer DK, Day D, Lechner MJ, Brune WH, Apel E, Diskin GS, Fisher JA, Fuelberg HE, Hecobian A, Knapp DJ, Mikoviny T, Riemer D, Sachse GW, Sessions W, Weber RJ, Weinheimer AJ, Wisthaler A, Jimenez JL. Effects of aging on organic aerosol from open biomass burning smoke in aircraft and laboratory studies. Atmospheric Chemistry and Physics 2011;11(23):12049-12064. R833747 (2010)
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  • Journal Article DeCarlo PF, Ulbrich IM, Crounse J, de Foy B, Dunlea EJ, Aiken AC, Knapp D, Weinheimer AJ, Campos T, Wennberg PO, Jimenez JL. Investigation of the sources and processing of organic aerosol over the Central Mexican Plateau from aircraft measurements during MILAGRO. Atmospheric Chemistry and Physics 2010;10(12):5257-5280. R833747 (2010)
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  • Journal Article Engelhart GJ, Hennigan CJ, Miracolo MA, Robinson AL, Pandis SN. Cloud condensation nuclei activity of fresh primary and aged biomass burning aerosol. Atmospheric Chemistry and Physics 2012;12(15):7285-7293. R833747 (Final)
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  • Journal Article Hennigan CJ, Miracolo MA, Engelhart GJ, May AA, Presto AA, Lee T, Sullivan AP, McMeeking GR, Coe H, Wold CE, Hao W-M, Gilman JB, Kuster WC, de Gouw J, Schichtel BA, Collett Jr. JL, Kreidenweis SM, Robinson AL. Chemical and physical transformations of organic aerosol from the photo-oxidation of open biomass burning emissions in an environmental chamber. Atmospheric Chemistry and Physics 2011;11(15):7669-7686. R833747 (2010)
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  • Journal Article Hennigan CJ, Westervelt DM, Riipinen I, Engelhart GJ, Lee T, Collett Jr JL, Pandis SN, Adams PJ, Robinson AL. New particle formation and growth in biomass burning plumes:An important source of cloud condensation nuclei. Geophysical Research Letter 2012;39(9):L09805 (5 pp.). R833747 (Final)
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  • Journal Article Huffman JA, Ziemann PJ, Jayne JT, Worsnop DR, Jimenez JL. Development and characterization of a fast-stepping/scanning thermodenuder for chemically-resolved aerosol volatility measurements. Aerosol Science & Technology 2008;42(5):395-407. R833747 (Final)
    R831080 (Final)
    R832161 (2007)
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  • Journal Article Huffman JA, Docherty KS, Mohr C, Cubison MJ, Ulbrich IM, Ziemann PJ, Onasch TB, Jimenez JL. Chemically-resolved volatility measurements of organic aerosol from different sources. Environmental Science & Technology 2009;43(14):5351-5357. R833747 (2008)
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  • Journal Article Huffman JA, Docherty KS, Aiken AC, Cubison MJ, Ulbrich IM, DeCarlo PF, Sueper D, Jayne JT, Worsnop DR, Ziemann PJ, Jimenez JL. Chemically-resolved aerosol volatility measurements from two magacity field studies. Atmospheric Chemistry and Physics 2009;9(18):7161-7182. R833747 (2008)
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  • Journal Article Jimenez JL, Canagaratna MR, Donahue NM, Prevot AS, Zhang Q, Kroll JH, DeCarlo PF, Allan JD, Coe H, Ng NL, Aiken AC, Docherty KS, Ulbrich IM, Grieshop AP, Robinson AL, Duplissy J, Smith JD, Wilson KR, Lanz VA, Hueglin C, Sun YL, Tian J, Laaksonen A, Raatikainen T, Rautiainen J, Vaattovaara P, Ehn M, Kulmala M, Tomlinson JM, Collins DR, Cubison MJ, Dunlea EJ, Huffman JA, Onasch TB, Alfarra MR, Williams PI, Bower K, Kondo Y, Schneider J, Drewnick F, Borrmann S, Weimer S, Demerjian K, Salcedo D, Cottrell L, Griffin R, Takami A, Miyoshi T, Hatakeyama S, Shimono A, Sun JY, Zhang YM, Dzepina K, Kimmel JR, Sueper D, Jayne JT, Herndon SC, Trimborn AM, Williams LR, Wood EC, Middlebrook AM, Kolb CE, Baltensperger U, Worsnop DR. Evolution of organic aerosols in the atmosphere. Science 2009;326(5959):1525-1529. R833747 (Final)
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  • Journal Article Jolleys, MD, Coe H, McFiggans G, McMeeking GR, Lee T, Kreidenweis SM, Collett Jr. JL, Sullivan AP. Organic aerosol emission ratios from the laboratory combustion of biomass fuels. Journal of Geophysical Research-Atmospheres 2014;119(22):12850-12871. R833747 (Final)
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  • Journal Article Kimmel JR, Farmer DK, Cubison MJ, Sueper D, Tanner C, Nemitz E, Worsnop DR, Gonin M, Jimenez JL. Real-time aerosol mass spectrometry with millisecond resolution. International Journal of Mass Spectrometry 2011;303(1):15-26. R833747 (2010)
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  • Journal Article Lee T, Sullivan AP, Mack L, Jimenez JL, Kreidenweis SM, Onasch TB, Worsnop DR, Malm W, Wold CE, Hao WM, Collett Jr. JL. Chemical smoke marker emissions during flaming and smoldering phases of laboratory open burning of wildland fuels. Aerosol Science and Technology 2010;44(9):i-v. R833747 (2009)
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  • Journal Article Lewis KA, Arnott WP, Moosmüller H, Chakrabarty RK, Carrico CM, Kreidenweis SM, Day DE, Malm WC, Laskin A, Jimenez JL, Ulbrich IM, Huffman JA, Onasch TB, Trimborn A, Liu L, Mishchenko MI. Reduction in biomass burning aerosol light absorption upon humidification:roles of inorganically-induced hygroscopicity, particle collapse, and photoacoustic heat and mass transfer. Atmospheric Chemistry and Physics 2009;9(22):8949-8966. R833747 (Final)
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  • Journal Article May AA, Levin EJT, Hennigan CJ, Riipinen I, Lee T, Collett Jr. JL, Jimenez JL, Kreidenweis SM, Robinson AL. Gas-particle partitioning of primary organic aerosol emissions: 3. Biomass burning. Journal of Geophysical Research–Atmospheres 2013;118(19):11327-11338. R833747 (Final)
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  • Journal Article McMeeking GR, Fortner E, Onasch TB, Taylor JW, Flynn M, Coe H, Kreidenweis SM. Impacts of nonrefractory material on light absorption by aerosols emitted from biomass burning. Journal of Geophysical Research-Atmospheres 2014;119(21):12272-12286. R833747 (Final)
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  • Journal Article Ng NL, Canagaratna MR, Jimenez JL, Zhang Q, Ulbrich IM, Worsnop DR. Real-time methods for estimating organic component mass concentrations from aerosol mass spectrometer data. Environmental Science & Technology 2011;45(3):910-916. R833747 (Final)
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  • Journal Article Onasch TB, Fortner EC, Trimborn AM, Lambe AT, Tiwari AJ, Marr LC, Corbin JC, Mensah AA, Williams LR, Davidovits P, Worsnop DR. Investigations of SP-AMS carbon ion distributions as a function of refractory black carbon particle type. Aerosol Science and Technology 2015;49(6):409-422. R833747 (Final)
    R835033 (2014)
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  • Journal Article Robinson CB, Kimmel JR, David DE, Jayne JT, Trimborn A, Worsnop DR, Jimenez JL. Thermal desorption metastable atom bombardment ionization aerosol mass spectrometer. International Journal of Mass Spectrometry 2011;303(2-3):164-172. R833747 (2010)
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  • Journal Article Saleh R, Hennigan CJ, McMeeking GR, Chuang WK, Robinson ES, Coe H, Donahue NM, Robinson AL. Absorptivity of brown carbon in fresh and photo-chemically aged biomass-burning emissions. Atmospheric Chemistry and Physics 2013;13(15):7683-7693. R833747 (Final)
    R835035 (2013)
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  • Journal Article Spracklen DV, Jimenez JL, Carslaw KS, Worsnop DR, Evans MJ, Mann GW, Zhang Q, Canagaratna MR, Allan J, Coe H, McFiggans G, Rap A, Forster P. Aerosol mass spectrometer constraint on the global secondary organic aerosol budget. Atmospheric Chemistry and Physics 2011;11(23):12109-12136. R833747 (2010)
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  • Supplemental Keywords:

    Primary organic aerosol, semivolatile organics, volatile organic carbon (VOC), organic gas-aerosol partitioning, modeling, volatility distribution, thermal denuder, levoglucosan, source profiles, fire emissions, fire maps

    Progress and Final Reports:

    Original Abstract
    2008 Progress Report
    2009 Progress Report
    2010 Progress Report
    2011 Progress Report