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Ezra Wood, Scott Herndon, Luwi Oluwole , Simon Albo

6/21/2011 FLAIR workshop, Austin TX. Acknowledgments: TCEQ. Characterization of gas and particle emissions in the greater Houston area using the Aerodyne mobile laboratory. Ezra Wood, Scott Herndon, Luwi Oluwole , Simon Albo

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Ezra Wood, Scott Herndon, Luwi Oluwole , Simon Albo

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  1. 6/21/2011 FLAIR workshop, Austin TX Acknowledgments: TCEQ Characterization of gas and particle emissions in the greater Houston area using the Aerodyne mobile laboratory Ezra Wood, Scott Herndon, LuwiOluwole, Simon Albo T. Onasch1, E. Fortner1, J. Jayne1, J. Wormhoudt1, P. Massoli1, C. Kolb1, H. B. Lee2, M. Zavala3, L. T. Molina3, and W. B. Knighton4 Aerodyne Research, Inc., Harvard University, Molina Center for Energy & Environment, Montana State University

  2. CO, NO2, C2H4, HCHO (QC-TILDAS) aromatic VOCs, 1,3-butadiene, OVOCs (PTR-MS/NO+MS) O3, NO, CO2, SO2 PAN (GC), VOCs (canisters) (UH) Instrumentation Size and chemically-speciated PM (Aerosol Mass Spectrometer) Particle number (CPC) Black Carbon (MAAP), extinction PM size distribution (SMPS) Wind speed/direction Actinic flux GPS position

  3. Goal: Conduct measurements that support emissions characterization • quantification (pounds/hr) • location identification Mobile sampling: Texas City, Mont Belvieu, Ship Channel Stationary sites: Texas City Mont Belvieu U. Houston

  4. C2H4 and HCHO mapping in Mont Belvieu WIND

  5. Quantification of emissions from “traditional” combustion source: fuel-based emission factors Ship Channel May 28, 2009

  6. Carbon balance method 18 ppb NOx / ppm CO2 x total fuel consumption Emission Inventory 58 g NOx/kg fuel

  7. Ship emission factors HONO/NOx: 0.7 to 1.4% (similar to on-road diesel vehicles) -based on comparison with UCLA iDOAS HONO/NO2 ratios

  8. • Destruction Removal Efficiency (DRE) vs. fuel-based emission factors• Assumption that most C ends up as CO, CO2 not valid Flares: use carbon balance method … …with a few complications TCEQ’s Comprehensive Flare Study September 2010:

  9. Emissions observed with ARI mobile laboratory during FLAIR 2009: 1) Useful correlations between combustion tracers (CO, CO2) and VOCs 2) Obvious fugitive emissions 3) Unclear – no obvious correlation between combustion tracers and VOCs, but can’t rule it out

  10. 1. (Useful VOC-COx correlations) Flare Emission Capture from Mobile Laboratory Mobile Lab Maneuvered Here Prevailing Wind Known Plant Flare P-200

  11. Flare Emission Capture from Mobile Laboratory Prevailing Wind Known Plant Flare P-200

  12. Flare Emission Capture from Mobile Laboratory Prevailing Wind Known Plant Flare P-200 Carbon balance methods with a guess about vent gas composition: DRE = 94% (88% - 96%)

  13. Large ethene leak, Winfree Rd 2) obvious fugitive emissions / non-combustion source ·Localized (<10 m) · no CO/CO2/NOx

  14. Unlit flare 2) obvious fugitive emissions / non-combustion source (5/19/2009, Mt. Belvieu)

  15. 3) No obvious correlation between combustion tracers and VOCs, but can’t rule out low DRE flare vs. leak

  16. 3) No obvious correlation between VOCs and COx – low DRE flares?

  17. Driver • Obs. Data • (MET, Sensors) SCIPUFF SCIPUFF TL/Adjoint Minimization algorithm The Aerodyne Inverse Modeling System (AIMS) • Given knowledge of the wind history, determine emission source parameters that when applied in atmospheric dispersion model yield pollutant concentration profiles that are most consistent with observed profiles # of sources, Emission rates, Locations, Start and End times. Aerodyne Research, Inc.

  18. Inversion model results 15 pounds/hr benzene source identified by inversion model WIND

  19. Stationary data: SO2 “upwind” from courthouse site (TC)

  20. HCHO: same spatial signature filtered day/night

  21. Consistent HCHO/SO2 ratio

  22. HCHO: Primary vs. secondary? C2H4 + OH → → 1.43 HCHO photochemical age (OH exposure):

  23. Primary HCHO in Texas City? slope implies [OH] = 2 ×107 to 4 × 107 molecules/cm3 → evidence for primary HCHO

  24. Primary HCHO from Chevron? Slope = 0.02 HCHO (ppb) C2H4 (ppb) Slope and transit time imply [OH] = 1.33 × 106 molecules cm-3 at 07:20 CST 5/21/2009→no evidence for primary HCHO

  25. 1,3-butadiene mapping (Ship Channel) WIND

  26. 1,3-butadiene, styrene

  27. Summary • Mobile measurements useful for locating and quantifying emission sources • Rich dataset: Marathon flare DRE Ship emission factors Winfree road Ethylene leak Primary HCHO emissions from Texas City facililty Ethylene, propylene emission from Chevron (Mont Belvieu) 1,3-butadiene, styrene from Goodyear

  28. back-up slides

  29. Photochemistry

  30. P(OH) = L(OH) Total OH loss rate = 47.3 s-1, and is dominated by reaction with C2H4. This yields an OH concentation of 1.6 × 105 molecules/cm3. Since the HO2 + NO term is obviously not zero, this number should be considered a lower limit to the true OH concentration. This value is likely higher than the [OH] in non alkene plume air considering the time of day (06:12 local time). Further analysis will address the likely range of values for the HO2 + NO term.

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