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Urban and Rural Sources of Particulate Matter

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Presentation given by Prof John Wenger at the 2015 Clean Air Conference, 28/09/15, Dublin

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Urban and Rural Sources of Particulate Matter

  1. 1. Urban and Rural Sources of Particulate Matter John Wenger Centre for Research into Atmospheric Chemistry Environmental Research Institute University College Cork Ireland Email: j.wenger@ucc.ie web: http://www.ucc.ie/en/crac/
  2. 2. Outline • Properties of Particulate Matter (PM) • Linking chemical composition and sources of PM • Case Studies - Cork City - Killarney • Summary and Perspectives
  3. 3. Particulate Matter PM10 - Particulate Matter with diameter less than 10 microns PM2.5 - Particulate Matter with diameter less than 2.5 microns
  4. 4. All Shapes and Sizes • Large number of particles < 0.1 microns • Majority of mass in range 0.1-10 microns
  5. 5. Natural Anthropogenic Primary Sources
  6. 6. • Formation and growth of particles in the atmosphere • Ammonium, sulfate, nitrate, secondary organic aerosol Gas + scavenging Particle Particle Particle Particle+ coagulation Particle Gas Gas+ nucleation Particle Gas condensation Particle Secondary Sources
  7. 7. Fine fraction (PM2.5) Coarse fraction (PM2.5-PM10) • Approximate composition of PM in Ireland determined by off-line analysis of filter samples Chemical Composition Elemental and Organic Carbon Sulphate Nitrate Ammonium Chloride Insoluble minerals Na, K, Mg, Ca
  8. 8. Chemical species Sources Elemental/Black Carbon (EC or BC) Fuel combustion (automobiles, industry, coal/wood burning) Organic Carbon Fuel combustion, secondary organic aerosols from VOC oxidation processes Nitrate / Sulfate Gas-particle conversion of NO2 / SO2 produced from combustion processes Ammonium Gas-particle conversion of NH3 produced from agriculture Chloride Sea spray Minerals (Oxides of Ca, Mg, Si, Al, Fe) Resuspension of dust/soil Metals (K, V and Ni, Pb, Zn, Cd, Hg etc.) Industry, combustion, often specific sources Linking Composition and Sources of PM
  9. 9. Reducing PM levels We need to know AND quantify the sources • How much PM is from traffic? • How much PM is from solid fuel burning? • How much PM is from other sources? • How do the emissions from these sources vary during the day and by season? Detailed measurements of the PM are required • Size, concentration and chemical composition at a HIGH-TIME resolution • Source Apportionment Modelling
  10. 10. Case Study: Cork Harbour • Long-term (1 year) monitoring campaigns • Intensive (1 month) measurement campaigns
  11. 11. X B B B Tivoli Docks August 2008 and February 2009 Intensive Measurement Campaign Healy et al., Atmospheric Chemistry and Physics 2010
  12. 12. Tivoli Docks August 2008 and February 2009 Intensive Measurement Campaign A range of state-of-the-art instruments deployed for On-line monitoring of particle mass, size, number and chemical composition in real-time
  13. 13. Aerosol Time-of-Flight Mass Spectrometer • Detects elemental carbon, organic carbon, metals, inorganic ions in single particles • Provides size-resolved chemical composition (0.1-3.0 micron) • Operates in real-time → big advantage over filter collection and off- line analysis approach
  14. 14. Sea-Salt Particle Mass Spectrum (Na and Cl are markers of interest) Biomass Burning Particle Mass Spectrum (K is major marker for biomass) Single Particle Mass Spectra
  15. 15. Sources in Cork Harbour: 3 Vehicular Traffic 0 500 1000 1500 2000 2500 ATOFMScounts(h-1) Time Ca-traffic EC-traffic EC-phos Sources in Cork Harbour: Vehicular Traffic Healy et al., Atmospheric Chemistry and Physics 2010
  16. 16. 0 50 100 150 200 250 0 100 200 300 400 500 600 700 800 ATOFMScounts(h-1) ATOFMScounts(h-1) Time coal peat wood Sources in Cork Harbour: Solid Fuel Combustion Healy et al., Atmospheric Chemistry and Physics 2010
  17. 17. • State-of-the-art analytical techniques used to apportion PM mass Source Apportionment of PM Healy et al., Atmospheric Chemistry and Physics, 2010 PM2.5 average (µg/m3) Solid Fuel Burning % Traffic % Other Local Sources % Regional Sources % August 2008 9.7 5 23 24 26 February 2009 16.2 50 19 21 10 Kourtchev et al., Science of the Total Environment, 2011 Dall’Osto et al., Atmospheric Chemistry and Physics, 2013
  18. 18. Extent of Bituminous Coal Ban 2015
  19. 19. • What is the contribution of residential solid fuel burning to PM levels in towns where the Ban on Bituminous Coal is not in place? The Burning Question
  20. 20. What is the contribution of each fuel type? Sod Peat (Turf) “Smokeless” Coal Wood Bituminous (Smoky) Coal Peat Briquettes
  21. 21. Source Apportionment of Particulate Matter in Urban and Rural Residential Areas of Ireland (SAPPHIRE) 1 April 2014 – 31 March 2016 http://www.ucc.ie/en/crac/research/sapphire/
  22. 22. • Outside the Smoky Coal Ban Area (pop. < 15,000) • No natural gas supply • High usage of solid fuels (coal, peat/turf & wood) Monitoring Locations • Killarney, Co. Kerry (Nov & Dec 2014) • Enniscorthy, Co. Wexford (Jan & Feb 2015) K E
  23. 23. • Site is located on the western side of the town, in the grounds of the Community Hospital in a residential area Monitoring Location: Killarney
  24. 24. • Site is located on the western side of the town, in the grounds of the Community Hospital in a residential area Monitoring Location: Killarney
  25. 25. TEOM PM2.5 mass concentration • PM2.5 up to 10 times higher during evening hours
  26. 26. PM2.5 mass concentration • Strong diurnal pattern
  27. 27. Aerosol Time-of-Flight Mass Spectrometer • Detects elemental carbon, organic carbon, metals, inorganic ions in single particles • Provides size-resolved chemical composition (0.1-3.0 micron) • Operates in real-time → big advantage over filter collection and off- line analysis approach
  28. 28. PEAT PEAT WOOD COAL COAL EC Sulfate Potassium Assigned on the basis of combustion experiments COAL → EC & some potassium, sulfate dominates negative spectra PEAT → EC & OC fragments, some potassium WOOD → Potassium dominates positive spectra EC OC WOOD Mass Spectra: Solid Fuel Combustion
  29. 29. SEA SALT TRAFFIC AMINE/ AMMONIUM Na Cl NaCl2 Na2Cl3 Sea salt characteristics: → sodium & chloride peaks, no EC Traffic characteristics: → calcium & phosphate (lubricating oil), some EC Phosphate Calcium Ammonium/amine characteristics: → ammonium, trimethylamine, OC, large sulfate peak in negative spectra Ammonium Mass Spectra: Other Particle Types
  30. 30. Transported sea salt ATOFMS Particle Number • Low wind speed – local emissions dominate • High wind speed – regional sources dominate
  31. 31. Particles from solid fuel burning 80% of PM2.5 Particle Numbers Particles from solid fuel burning 77% of PM2.5 Particle Mass ATOFMS: Source Contribution to PM2.5 Mass Scaling
  32. 32. • Local sources account for 70-90% of PM2.5 in Cork City. Traffic accounts for ~20%; solid fuel burning 50% in winter. • Residential solid fuel burning contributes 70-80% of PM2.5 in Killarney in winter • Similar results for Enniscorthy: also likely replicated in tens of small towns across Ireland. • Peat, coal and wood all contribute: Extending the smoky coal ban may not be enough to deliver improvements in air quality • No source apportionment study yet performed in Dublin! Summary and Perspectives
  33. 33. Acknowledgements John Sodeau Ian O’Connor Eoin McGillicuddy Jovanna Arndt Paul BuckleyStig Hellebust
  34. 34. Extra Slides
  35. 35. • Missing mass due to regional sources – organic aerosol, ammonium sulfate? ATOFMS Particle Mass vs TEOM
  36. 36. Particles directly emitted from solid fuel combustion = 66% of measured PM2.5 Source contributions (% of TEOM PM2.5)
  37. 37. Killarney: ATOFMS Mass: Diurnal • Particle numbers for entire sampling period averaged to 1 day → clear evening peak shows influence of solid fuel burning on total particle numbers. • Clear evening peak in averaged mass concentration: ‒ peat (16 μg/m3) ‒ wood (12 μg/m3) ‒ coal (10 μg/m3) (combined 38 μg/m3 average per night) 29/09/15 SAPPHIRE Meeting: ATOFMS (Jovanna Arndt) 37
  38. 38. Unidentified 30% Marine and Aged 6% Local Aged 4%Traffic 3%Amines 5% Burning 52% Preliminary Source Apportionment • 5 factors identified • Primary emissions from solid fuel burning = 52% of PM2.5 …….but no separation by fuel type • PMF ME-2 using ATOFMS particle classes, EC-OC, SMPS, OPS, NOx, Aethalometer
  39. 39. Instrument Parameter(s) measured Temporal resolution Aerosol time-of-flight mass spectrometer (TSI model 3800) Single particle chemical composition (100-3000 nm) 1 min Scanning mobility particle sizer (TSI model 3081) Particle number concentration (10-800 nm) 3 min Optical Particle Sizer (TSI model 3330) Particle number concentration (300-10000 nm) 3 min TEOM (Thermo Electron model RP 1400a) PM2.5 mass concentration 30 min Thermal-optical carbon analyser (Sunset Inc. model 3rd generation) Elemental and organic carbon mass concentrations 2 hr 7-Wavelength Aethalometer (Model AE33, Magee Scientific) Black Carbon concentration 1 min High volume sampler (Digitel model DHA 80) Collection of particulate matter (PM2.5) 6 hr Key Instrumentation
  40. 40. TEOM Sunset ECOC Elemental and Organic Carbon (EC/OC) • Majority of PM2.5 during night-time pollution events is carbonaceous aerosol
  41. 41. Low winds – Local sources High winds – Regional sources Influence of Meteorology • Low wind speed – local emissions dominate • High wind speed – regional sources dominate
  42. 42. Enniscorthy: ATOFMS Mass: Diurnal • Averaged ATOFMS mass concentration per day maximum = ~ 60 μg/m3 • Peak averaged daily mass concentrations: − peat (16 μg/m3) − wood (14 μg/m3) − coal (12 μg/m3) − PAH-containing (9 μg/m3) 29/09/15 SAPPHIRE Meeting: ATOFMS (Jovanna Arndt) 42
  43. 43. Enniscorthy: ATOFMS Mass Breakdown 29/09/15 SAPPHIRE Meeting: ATOFMS (Jovanna Arndt) 43 Solid fuel combustion particles = 89% of ATOFMS PM2.5 mass (no comparison with TEOM yet so this % will probably decrease a bit) PAH-containing particles associated with all three fuel types.

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