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SEARCH & VISTAS Special Studies

SEARCH & VISTAS Special Studies. RPO National Technical Meeting St. Louis, MO November 5, 2003. Outline. SEARCH Overview Data Quality for Continuous PM Carbon Collaboration NH 3 Measurements Biomass Emissions In-Plume Oxidation Rates SO 4 Neutralization Other. SEARCH. SEARCH

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SEARCH & VISTAS Special Studies

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  1. SEARCH & VISTAS Special Studies RPO National Technical Meeting St. Louis, MO November 5, 2003

  2. Outline SEARCH Overview Data Quality for Continuous PM Carbon Collaboration NH3 Measurements Biomass Emissions In-Plume Oxidation Rates SO4 Neutralization Other

  3. SEARCH SEARCH SouthEastern Aerosol Research and CHaracterization Study Jefferson Street Site (JST) Atlanta, GA Yorkville Site (YRK) Yorkville, GA SEARCH

  4. SEARCH Network SEARCH rural suburban urban Yorkville North Birmingham Jefferson Street Centreville Oak Grove OLF #8 Gulfport Pensacola

  5. SEARCH SEARCH Measurements - Continuous

  6. SEARCH Measurements - Discrete SEARCH Note: all measurements blank corrected

  7. Comparisons of Continuous and Discrete PM Measurements in SEARCH

  8. SEARCH TEOM Configuration • Nafion drier • 30C • Heavy insulation (thermal shock) • Filter change every 3 days

  9. Yorkville TEOM vs. FRM 2002 Median absolute difference = 0.84 ug/m3 Median absolute % difference = 6.8 No seasonality

  10. ARA Continuous SO4 • Harvard SO4 analyzer • Denuders to remove SO2 (carbonate) and reduced S gases (C monolith) • Reduction of SO4 to SO2 on hot SS (850+C) • Automated zeroing every 90 minutes • 1-minute data acquisition • Mean and s.d. each averaging interval

  11. ARA Continuous NO3/NH4 • 3-channel analyzer for NH4 and NO3 • NH4 via oxidation to NO on hot Pt • NO3 via reduction to NO on Mo • Remove gas phase species with acid/base denuders and C monolith • Detection via NO-ozone CL • 1-minute data acquisition

  12. 14 Filter SO4 PILS SO4 ARA SO4 12 10 8 6 4 2 0 8/2/2002 8/3/2002 8/4/2002 8/5/2002 8/6/2002 8/7/2002 8/8/2002 8/9/2002 9/1/2002 9/2/2002 9/3/2002 9/4/2002 9/5/2002 9/6/2002 9/7/2002 9/8/2002 8/10/2002 8/11/2002 8/12/2002 8/13/2002 8/14/2002 8/15/2002 8/16/2002 8/17/2002 8/18/2002 8/19/2002 8/20/2002 8/21/2002 8/22/2002 8/23/2002 8/24/2002 8/25/2002 8/26/2002 8/27/2002 8/28/2002 8/29/2002 8/30/2002 8/31/2002 Time Series of 24-Hr SO42- SO4 (ug/m3)

  13. 25 ARA SO4 PILS SO4 20 15 10 5 0 9/1/02 0:00 9/2/02 0:00 9/3/02 0:00 9/4/02 0:00 9/5/02 0:00 9/6/02 0:00 9/7/02 0:00 9/8/02 0:00 8/23/02 0:00 8/24/02 0:00 8/25/02 0:00 8/26/02 0:00 8/27/02 0:00 8/28/02 0:00 8/29/02 0:00 8/30/02 0:00 8/31/02 0:00 9/1/02 12:00 9/2/02 12:00 9/3/02 12:00 9/4/02 12:00 9/5/02 12:00 9/6/02 12:00 9/7/02 12:00 8/23/02 12:00 8/24/02 12:00 8/25/02 12:00 8/26/02 12:00 8/27/02 12:00 8/28/02 12:00 8/29/02 12:00 8/30/02 12:00 8/31/02 12:00 Time Series of Hourly SO42- SO4 (ug/m3)

  14. SEARCH Continuous vs. Filter SO42- at Yorkville(using CE = 0.82)

  15. 25 PILS = 1.003*ARA+ 0.027 2 R = 0.9214 20 15 PILS SO4 10 5 0 0 5 10 15 20 25 ARA SO4 SEARCH Hourly SO42- PILS vs. ARA ContinuousAtlanta, GA - August 2002(using CE = 0.86)

  16. 4.0 Filter NH4 PILS NH4 ARA NMH4 3.5 3.0 2.5 2.0 1.5 1.0 0.5 0.0 9/1/2002 9/2/2002 9/3/2002 9/4/2002 9/5/2002 9/6/2002 9/7/2002 9/8/2002 8/17/2002 8/18/2002 8/19/2002 8/20/2002 8/21/2002 8/22/2002 8/23/2002 8/24/2002 8/25/2002 8/26/2002 8/27/2002 8/28/2002 8/29/2002 8/30/2002 8/31/2002 Time Series of 24-hr NH4+ NH4 (ug/m3)

  17. 5 ARA NH4 PILS NH4 4 3 2 1 0 9/1/02 0:00 9/2/02 0:00 9/3/02 0:00 9/4/02 0:00 9/5/02 0:00 9/6/02 0:00 9/7/02 0:00 9/8/02 0:00 8/23/02 0:00 8/24/02 0:00 8/25/02 0:00 8/26/02 0:00 8/27/02 0:00 8/28/02 0:00 8/29/02 0:00 8/30/02 0:00 8/31/02 0:00 9/1/02 12:00 9/2/02 12:00 9/3/02 12:00 9/4/02 12:00 9/5/02 12:00 9/6/02 12:00 9/7/02 12:00 8/23/02 12:00 8/24/02 12:00 8/25/02 12:00 8/26/02 12:00 8/27/02 12:00 8/28/02 12:00 8/29/02 12:00 8/30/02 12:00 8/31/02 12:00 Time Series of Hourly NH4+ NH4 (ug/m3)

  18. 5 PILS = 1.048*ARA- 0.44 2 R = 0.857 4 3 PILS NH4 2 1 0 0 1 2 3 4 5 ARA NH4 Scattergram of Hourly NH4+

  19. 1.0 Filter NO3 PILS NO3 ARA NO3 0.8 NO3 (ug/m3) 0.5 0.3 0.0 9/1/2002 9/2/2002 9/3/2002 9/4/2002 9/5/2002 9/6/2002 9/7/2002 9/8/2002 8/17/2002 8/18/2002 8/19/2002 8/20/2002 8/21/2002 8/22/2002 8/23/2002 8/24/2002 8/25/2002 8/26/2002 8/27/2002 8/28/2002 8/29/2002 8/30/2002 8/31/2002 Time Series of 24-hr NO3-

  20. 3.5 ARA NO3 PILS NO3 3.0 2.5 2.0 1.5 1.0 0.5 0.0 9/1/02 0:00 9/2/02 0:00 9/3/02 0:00 9/4/02 0:00 9/5/02 0:00 9/6/02 0:00 9/7/02 0:00 9/8/02 0:00 8/23/02 0:00 8/24/02 0:00 8/25/02 0:00 8/26/02 0:00 8/27/02 0:00 8/28/02 0:00 8/29/02 0:00 8/30/02 0:00 8/31/02 0:00 9/1/02 12:00 9/2/02 12:00 9/3/02 12:00 9/4/02 12:00 9/5/02 12:00 9/6/02 12:00 9/7/02 12:00 8/23/02 12:00 8/24/02 12:00 8/25/02 12:00 8/26/02 12:00 8/27/02 12:00 8/28/02 12:00 8/29/02 12:00 8/30/02 12:00 8/31/02 12:00 Time Series of Hourly NO3- NO3 (ug/m3)

  21. Continuous vs. Filter Summary24-Hr Averages (JST) MAE = median abs. error; MAPE = median abs. % error

  22. Ongoing Comparison Work in VISTAS • Millbrook Site • R&P 8400S (SO4) vs. HSPH SO4 • R&P 8400N (NO3) vs. ARA NO3 • R&P 5400 (EC) vsAethalometer (BC) • ARA NH4 vs. STN NH4

  23. SEARCH/ARIES Collaboration on Carbonaceous Aerosol • Historical Samples (SEARCH/Improve/STN) • Composite Monthly or Seasonal Quartz Filters • Detailed Speciation (GC/MS) • CMB analysis for major sources • Planned Samples (SEARCH 4 sites/VISTAS 5 • Collect hi-vol samples 4 SEARCH sites, 5 VISTAS sites • Detailed Speciation/CMB and 14C for Selected Events

  24. Primary Carbon Source Attribution Sample Matrix January -December 2002 1= 4 one-month composite; one for each quarter 6= 2 six-month composite; summer & winter 3= 2 three-month composite; summer &winter D= 30 daily samples ; July’01 & Jan’02

  25. SEARCH Sources of Primary OC in PM2.5 (F) (M) (F) (M) (F/M ?) (M) (Secondary F/M?) (F)

  26. Primary Secondary Total S peciation , Modern Speciation/CMB Models, 14C D ifference S peciation , Fossil Speciation/CMB Models, 14C Difference Simplified Organic Carbon Source Matrix Combination of CMB and C-14 data allows calculation of secondary OC by difference. SEARCH

  27. Primary * Secondary Total # Modern 64 <5 61 +/ - 5 Fossil 36 <5 39 +/ - 5 SEARCH OC Source MatrixAtlanta, GA – January * 2000 Data: Zheng et al., ES&T, 2002. # from 14Cdata

  28. Primary* Secondary Total # Modern <5 >50 59 +/ - 5 Fossil 40 * <5 41 +/ - 5 SEARCH OC Source MatrixAtlanta, GA – July 2001 * Zheng et al. Source Apportionment of Fine Particles at Atlanta, GA, AAAR 2002 # from 14C data

  29. SEARCH NH3 Measurements rural suburban urban Yorkville N.Birmingham Jefferson St. Centreville Oak Grove OLF Gulfport Pensacola SEARCH 24-hour denuder (1/3 day) all sites Continuous at Yorkville (9/15/03) and Oak Grove (1/15/04)

  30. SEARCH Total Reduced Nitrogen (NHx) Diagram

  31. SEARCH Continuous NH3 vs Denuder NH324 Hour Samples Gaseous NH3 is deduced by subtracting particulate NH4 from NHx

  32. SEARCH NH3 Time-Series9/12/03 – 9/30/03Yorkville, GA SEARCH Site Gaseous NH3 is deduced by subtracting particulate NH4 from TRN

  33. SEARCH HNO3, NH3, NH4NO3 Event9/24/03 – 9/27/03Yorkville, GA SEARCH Site

  34. SEARCH 1-hour NHx vs. Wind Direction

  35. The Smoking Chicken 4.5 km 2.3 km 1.8 km

  36. Emissions from Biomass Burning HMS Fire and Smoke Summary for 2345 10/21/03 Oak Grove http://www.firedetect.ssd.nesdis.noaa.gov/index.htm

  37. SEARCH WD and Bsp for Oak Grove – 10/21/03 Bsp (m-1)

  38. SEARCH CO and NOy at Oak Grove – 10/21/03

  39. SEARCH NOy vs. CO Oak Grove Event – 10/21/03

  40. SEARCH Comparison of ERs with Literature Values

  41. SEARCH Field Observations of SO2 Oxidation Rates in Coal Fired Power Plant Plumes E. S. Edgerton, B. E. Hartsell, C. J. Waid, ARA, Inc. J. J. Jansen, Southern Company D. Alan Hansen, EPRI AAAR 2003 Anaheim, CA October 22, 2003

  42. SEARCH SO2 and SO4 8/20/02 Event

  43. Daytime Pattern of Observed Oxidation (n = 28) 3 6 3 4 3 1 2 1 4 2 SEARCH

  44. Continuous PM at Jefferson Street August 16, 2001

  45. SO4, xsNH4 and Molar Ratio

  46. Background adjusted Molar Ratio

  47. SEARCH/VISTAS CollaborationonCharacterization of Meteorology and its Relationships to Fine Particle Mass and Visibility in the VISTAS Region

  48. Summary • SEARCH network will provide comprehensive PM/trace gas data through 2005 • Filter data needed to characterize continuous PM technologies • Data adjustments • Data uncertainty • Carbon speciation work underway (primary vs.secondary, Modern vs. Fossil) • NH3 measurements begun in the SE • Primary species: high and variable near sources, expect lower and less variable near sinks • Combination of continuous PM and Gas measurements shows promise • SO4 neutralization variability • Contributions from biomass burning • gas/particle conversion

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