SEARCH & VISTAS Special Studies. RPO National Technical Meeting St. Louis, MO November 5, 2003
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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 NH 3 Measurements Biomass Emissions In-Plume Oxidation Rates SO 4 Neutralization Other
3 SEARCH SouthEastern Aerosol Research and CHaracterization Study Jefferson Street Site (JST) Atlanta, GA Yorkville Site (YRK) Yorkville, GA
4 SEARCH Network rural urban suburban North Birmingham Yorkville Centreville Jefferson Street Oak Grove Gulfport OLF #8 Pensacola
5 SEARCH Measurements - Continuous Category Trace Gases Fine Particles Mass, BC, B scat SO 4 2-,NO 3, NH 4 + TC Observables O 3, NO, NO 2, HNO 3, NH x, NOy, CO, SO 2, CO 2 Temporal Resolution 1 min. <10 min. or 60 min. Surface Met. Hg (2 sites) T, RH, BP, WS, WD SR, precip. Hg(0), RGM, TPM 1 min. 60 min.
6 SEARCH Measurements - Discrete Category PM 2.5 PM 2.5 Analyte(s) Mass SO 2-4,NO 3, NH + 4 OC, EC Trace Elements Frequency ( ) Daily 1/3 PM coarse Mass 1/3 1/6 PM coarse PM coarse SO 4 2-,NO 3, NH 4 + Trace Elements OC, EC 1/6 (2 sites) 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 TEOM vs FRM y = x R 2 = 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 9/8/ Time Series of 24-Hr SO 4 2- Filter SO4 PILS SO4 ARA SO4 9/7/2002 8/2/2002 8/3/2002 8/4/2002 8/5/2002 8/6/2002 8/7/2002 8/8/2002 8/9/2002 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 9/1/2002 9/2/2002 9/3/2002 9/4/2002 9/5/2002 9/6/2002 SO4 (ug/m3)
13 Time Series of Hourly SO ARA SO4 PILS SO /23/02 0:00 8/23/02 12:00 8/24/02 0:00 8/24/02 12:00 8/25/02 0:00 8/25/02 12:00 8/26/02 0:00 8/26/02 12:00 8/27/02 0:00 8/27/02 12:00 8/28/02 0:00 8/28/02 12:00 8/29/02 0:00 8/29/02 12:00 8/30/02 0:00 8/30/02 12:00 8/31/02 0:00 8/31/02 12:00 9/1/02 0:00 9/1/02 12:00 9/2/02 0:00 9/2/02 12:00 9/3/02 0:00 9/3/02 12:00 9/4/02 0:00 9/4/02 12:00 9/5/02 0:00 9/5/02 12:00 9/6/02 0:00 9/6/02 12:00 9/7/02 0:00 9/7/02 12:00 9/8/02 0:00 0 SO4 (ug/m3)
14 Continuous vs. Filter SO 4 2- at Yorkville (using CE = 0.82) cso4 = 0.988*fSO R 2 = Continuous SO4 (ug/m3) Filter SO4 (ug/m 3)
15 Hourly SO 4 2- PILS vs. ARA Continuous Atlanta, GA - August 2002 (using CE = 0.86) 25 PILS = 1.003*ARA R 2 = PILS SO ARA SO4
16 9/7/2002 9/8/ Time Series of 24-hr NH 4 + Filter NH4 PILS NH4 ARA NMH4 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 9/1/2002 9/2/2002 9/3/2002 9/4/2002 9/5/2002 9/6/2002 NH4 (ug/m3)
17 Time Series of Hourly NH ARA NH4 PILS NH /23/02 0:00 8/23/02 12:00 8/24/02 0:00 8/24/02 12:00 8/25/02 0:00 8/25/02 12:00 8/26/02 0:00 8/26/02 12:00 8/27/02 0:00 8/27/02 12:00 8/28/02 0:00 8/28/02 12:00 8/29/02 0:00 8/29/02 12:00 8/30/02 0:00 8/30/02 12:00 8/31/02 0:00 8/31/02 12:00 9/1/02 0:00 9/1/02 12:00 9/2/02 0:00 9/2/02 12:00 9/3/02 0:00 9/3/02 12:00 9/4/02 0:00 9/4/02 12:00 9/5/02 0:00 9/5/02 12:00 9/6/02 0:00 9/6/02 12:00 9/7/02 0:00 9/7/02 12:00 0 9/8/02 0:00 NH4 (ug/m3)
18 Scattergram of Hourly NH PILS = 1.048*ARA R 2 = PILS NH ARA NH4
19 9/8/ Time Series of 24-hr NO 3 - Filter NO3 PILS NO3 ARA NO3 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 9/1/2002 9/2/2002 9/3/2002 9/4/2002 9/5/2002 9/6/2002 9/7/2002 NO3 (ug/m3)
20 Time Series of Hourly NO ARA NO3 PILS NO /23/02 0:00 8/23/02 12:00 8/24/02 0:00 8/24/02 12:00 8/25/02 0:00 8/25/02 12:00 8/26/02 0:00 8/26/02 12:00 8/27/02 0:00 8/27/02 12:00 8/28/02 0:00 8/28/02 12:00 8/29/02 0:00 8/29/02 12:00 8/30/02 0:00 8/30/02 12:00 8/31/02 0:00 8/31/02 12:00 9/1/02 0:00 9/1/02 12:00 9/2/02 0:00 9/2/02 12:00 9/3/02 0:00 9/3/02 12:00 9/4/02 0:00 9/4/02 12:00 9/5/02 0:00 9/5/02 12:00 9/6/02 0:00 9/6/02 12:00 9/7/02 0:00 9/7/02 12:00 9/8/02 0: NO3 (ug/m3)
21 Continuous vs. Filter Summary 24-Hr Averages (JST) Filter Mean Mean %E PILS MAE MAPE SO4 (30) NH4 (19) NO3 (23) Filter Mean Mean %E ARA MAE MAPE SO4 (36) NH4 (32) NO3 (35) 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 14 C for Selected Events
24 Primary Carbon Source Attribution Sample Matrix January -December = 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 Sources of Primary OC in PM 2.5 (F) (M) (F) (F) (F/M?) (Secondary F/M?) (M) (M)
26 Simplified Organic Carbon Source Matrix Primary Secondary Total Modern Speciation/CMB Speciation, Models, 14 C Difference Fossil Speciation/CMB Speciation, Models, Difference 14 C Combination of CMB and C-14 data allows calculation of secondary OC by difference.
27 OC Source Matrix Atlanta, GA January Primary* Secondary Total # Modern 64 <5 61 +/-5 Fossil 36 <5 39 +/-5 * 2000 Data: Zheng et al., ES&T, # from 14 Cdata
28 OC Source Matrix Atlanta, GA July 2001 Primary* Secondary Total # Modern <5 > /-5 Fossil 40* <5 41 +/-5 * Zheng et al. Source Apportionment of Fine Particles at Atlanta, GA, AAAR 2002 # from 14 C data
29 SEARCH NH 3 Measurements rural urban suburban 24-hour denuder (1/3 day) all sites N.Birmingham Yorkville Centreville Jefferson St. Continuous at Yorkville (9/15/03) and Oak Grove (1/15/04) Oak Grove OLF Gulfport Pensacola
30 Total Reduced Nitrogen (NH x ) Diagram
31 Continuous NH 3 vs Denuder NH Hour Samples Continuous NH 3, ug/m Continuous NH 3 = 1.12 Denuder NH R2 = Denuder NH 3, ug/m3 Gaseous NH 3 is deduced by subtracting particulate NH 4 from NH x
32 NH 3 Time-Series 9/12/03 9/30/03 Yorkville, GA SEARCH Site 9/16/03 9/17/03 9/18/03 9/19/03 9/20/03 9/21/03 9/22/03 9/23/03 9/24/03 9/25/03 9/26/03 9/27/03 9/28/03 9/29/03 9/30/03 9/14/03 9/15/03 Gaseous NH 3 is deduced by subtracting particulate NH 4 from TRN NH3 9/12/03 9/13/03 [NH3], ppbv
33 HNO 3, NH 3, NH 4 NO 3 Event 9/24/03 9/27/03 Yorkville, GA SEARCH Site [HNO3] ppbv [NO3] ug/m3,[nh4] ug/m3 9/24/03 0:00 9/24/03 6:00 9/24/03 12:00 9/24/03 18:00 9/25/03 0:00 9/25/03 6:00 9/25/03 12:00 9/25/03 18:00 9/26/03 0:00 9/26/03 6:00 9/26/03 12:00 9/26/03 18:00 9/27/03 0:00 9/27/03 6:00 9/27/03 12:00 9/27/03 18:00 [NH3], ppbv HNO3 NH4 NO3 NH3
34 1-hour NH x vs. Wind Direction [NH3 + NH4], ppbv NH3 + NH Wind Direction, Degrees
35 The Smoking Chicken 2.3 km 4.5 km 1.8 km
36 Emissions from Biomass Burning HMS Fire and Smoke Summary for /21/03 Oak Grove
37 WD and B sp for Oak Grove 10/21/ WDR Bsp 1.0E E-05 WDR (deg.) E E-05 B ( ** 1) Bsp (m -1 ) 0 10/21/03 0:00 10/21/03 4:00 10/21/03 8:00 10/21/03 12:00 10/21/03 16:00 10/21/03 20:00 0.0E+00
38 CO and NOy at Oak Grove 10/21/ CO NOy CO (ppb) NOy (ppb) /21/03 0:00 10/21/03 4:00 10/21/03 8:00 10/21/03 12:00 10/21/03 16:00 10/21/03 20:00 0
39 6.0 NOy vs. CO Oak Grove Event 10/21/03 NOy = *CO R 2 = NOy (ppb) CO (ppb)
40 Comparison of ERs with Literature Values ER (g/kg CO) FUEL NOy (as NO) SO2 PM2.5 TC* BC* Savannah/Grassland Trop. Forest non-trop. Forest Biofuels Ag. Residues This Study (Fires) 28+/ /-2/ / / /- 6.1 This Study (Urban)# 147 +/-10 n.d. 33 +/ /- 2.1 n.d. Andreae and Merlet. Global Geochem Cyclec 15(4): (A&M) * A&M TC and BC based on TSP # Based on Jefferson Street, Atlanta, GA SEARCH data
41 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 SO2 and SO4 8/20/02 Event 70 5 SO2 SO4 ZERO SO2 (ppb) SO4 ( b) /20/2002 0:00 8/20/2002 4:00 8/20/2002 8:00 8/20/ :00 8/20/ :00 8/20/ :00 0
43 3 2.5 Daytime Pattern of Observed Oxidation (n = 28) 3 6 Fall-Winter Spring-Summer Conversion Rate (%) :00 7:00 9:00 11:00 13:00 15:00 17:00 19:00 Midpoint
44 Continuous PM at Jefferson Street August 16, SO4 NO3 NH4 PM SO4, NO3, NH4 (ug/m3) PM2.5 (ug/m3) 0 8/16/01 0:00 8/16/01 2:00 8/16/01 4:00 8/16/01 6:00 8/16/01 8:00 8/16/01 10:00 8/16/01 12:00 8/16/01 14:00 8/16/01 16:00 8/16/01 18:00 8/16/01 20:00 8/16/01 22:00 0
45 SO4, xsnh4 and Molar Ratio SO4 NH4 Ratio 12 Ammonium sulfate 2.0 SO4, NH4 (ug/m3) 9 6 Ammonium bisulfate Molar Ratio /16/01 0:00 8/16/01 2:00 8/16/01 4:00 8/16/01 6:00 8/16/01 8:00 8/16/01 10:00 8/16/01 12:00 8/16/01 14:00 8/16/01 16:00 Sulfuric acid 8/16/01 18:00 8/16/01 20:00 8/16/01 22:00 0.0
46 Background adjusted Molar Ratio SO4 adjratio SO4 (ug/m3) adjratio /16/01 0:00 8/16/01 4:00 8/16/01 8:00 8/16/01 12:00 8/16/01 16:00 8/16/01 20:00 0.0
47 SEARCH/VISTAS Collaboration on Characterization 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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