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Characterization of gas and particle emissions in the greater Houston area using the Aerodyne mobile laboratory Ezra Wood, Scott Herndon, Luwi Oluwole,

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Presentation on theme: "Characterization of gas and particle emissions in the greater Houston area using the Aerodyne mobile laboratory Ezra Wood, Scott Herndon, Luwi Oluwole,"— Presentation transcript:

1 Characterization of gas and particle emissions in the greater Houston area using the Aerodyne mobile laboratory Ezra Wood, Scott Herndon, Luwi Oluwole, Simon Albo T. Onasch 1, E. Fortner 1, J. Jayne 1, J. Wormhoudt 1, P. Massoli 1, C. Kolb 1, H. B. Lee 2, M. Zavala 3, L. T. Molina 3, and W. B. Knighton 4 6/21/2011 FLAIR workshop, Austin TX Acknowledgments: TCEQ Aerodyne Research, Inc., Harvard University, Molina Center for Energy & Environment, Montana State University

2 CO, NO 2, C 2 H 4, HCHO (QC-TILDAS) aromatic VOCs, 1,3-butadiene, OVOCs (PTR-MS/NO+MS) O 3, NO, CO 2, SO 2 PAN (GC), VOCs (canisters) (UH) 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 Instrumentation

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 C 2 H 4 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 58 g NO x /kg fuel 18 ppb NO x / ppm CO 2 x total fuel consumption Emission Inventory

7 Ship emission factors Plume time Vessel name/type NO x g/kg fuel dO x / dNO x HCHO g/kg CO g/kg SO 2 g/kg 10:04 Izumo Princess :26 Vega Spring :59 Odfjell Seachem :04 UBC Bremen? :05 Eitzen Chemical :17 Leyte Spirit :24 tug/ferry :36 tug/ferry – :54 Petropavlovsk Williams MSD c Williams SSD b HONO/NO x : 0.7 to 1.4% (similar to on-road diesel vehicles) -based on comparison with UCLA iDOAS HONO/NO 2 ratios

8 Destruction Removal Efficiency (DRE) vs. fuel-based emission factors Assumption that most C ends up as CO, CO 2 not valid Flares: use carbon balance method … …with a few complications TCEQs Comprehensive Flare Study September 2010:

9 Emissions observed with ARI mobile laboratory during FLAIR 2009: 1) Useful correlations between combustion tracers (CO, CO 2 ) and VOCs 2) Obvious fugitive emissions 3) Unclear – no obvious correlation between combustion tracers and VOCs, but cant rule it out

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

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

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

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

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

15 3) No obvious correlation between combustion tracers and VOCs, but cant rule out low DRE flare vs. leak

16 3) No obvious correlation between VOCs and CO x – low DRE flares?

17 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 Driver SCIPUFF SCIPUFF TL/Adjoint Minimization algorithm Obs. Data (MET, Sensors) Aerodyne Research, Inc. # of sources, Emission rates, Locations, Start and End times.

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

19 Stationary data: SO 2 upwind from courthouse site (TC)

20 HCHO: same spatial signature filtered day/night

21 Consistent HCHO/SO 2 ratio

22 HCHO: Primary vs. secondary? C 2 H 4 + OH 1.43 HCHO photochemical age (OH exposure):

23 Primary HCHO in Texas City? slope implies [OH] = 2 ×10 7 to 4 × 10 7 molecules/cm 3 evidence for primary HCHO

24 Primary HCHO from Chevron? Slope and transit time imply [OH] = 1.33 × 10 6 molecules cm -3 at 07:20 CST 5/21/2009 no evidence for primary HCHO C 2 H 4 (ppb) HCHO (ppb) Slope = 0.02

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

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 C 2 H 4. This yields an OH concentation of 1.6 × 10 5 molecules/cm 3. Since the HO 2 + 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 HO 2 + NO term.


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