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ARL Mercury Measurements in the mid-Atlantic and Gulf of Mexico Regions: Status and Update

ARL Mercury Measurements in the mid-Atlantic and Gulf of Mexico Regions: Status and Update. Winston Luke, Paul Kelley, Mark Cohen NOAA/Air Resources Laboratory Prepared for EPA/NOAA Meeting Silver Spring, June 24, 2009. Measurements at Beltsville, MD CASTNet Site. Monitoring sites.

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ARL Mercury Measurements in the mid-Atlantic and Gulf of Mexico Regions: Status and Update

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  1. ARL Mercury Measurements in the mid-Atlantic and Gulf of Mexico Regions: Status and Update Winston Luke, Paul Kelley, Mark Cohen NOAA/Air Resources Laboratory Prepared for EPA/NOAA Meeting Silver Spring, June 24, 2009

  2. Measurements at Beltsville, MD CASTNet Site

  3. Monitoring sites rural AQS other AQS NADP/MDN CASTNet Symbol color indicates type of mercury source Hg site IMPROVE coal incinerator metals manuf/other Symbol size and shape indicates 1999 mercury emissions, kg/yr 1 - 50 50 - 100 100 - 200 200 – 400 400 - 700 700 – 1000 > 1000 Beltsville, MD CASTNet Site Harford County MSW Incin Brandon Shores and H.A. Wagner 100 miles from DC Montgomery County MSW Incin Eddystone Dickerson Arlington - Pentagon MSW Incin Possum Point Beltsville monitoring site Chalk Point Morgantown Bremo

  4. Site is impacted by a variety of local-regional sources with unique emissions characteristics. Coupled chemical-meteorological analysis will yield important insights into mercury emissions, transport, transformation, and removal at the site.

  5. As at Grand Bay, higher RGM is typically associated with high O3 concentrations and chemically aged air masses, suggesting that reactive gaseous mercury concentrations at the site reflect the influence of regional continental emissions.

  6. Multi-Day RGM Event, April 16-19, 2008

  7. size/shape of symbol denotes amount of mercury emitted (kg/yr) color of symbol denotes type of mercury source Back-trajectories starting at the indicated fraction of the mixed layer height. Circles on the trajectories mark the hourly positions 0.1 coal-fired power plants 10 - 50 0.3 other fuel combustion 50 - 100 0.5 waste incineration 100 – 200 0.7 metallurgical 200 - 400 manufacturing & other 0.9 400 - 600 Large Point Sources of Reactive Gaseous Mercury (RGM) Emissions Based on the 2002 U.S EPA National Emissions Inventory (NEI) All back trajectories run at 12 km resolution

  8. size/shape of symbol denotes amount of mercury emitted (kg/yr) color of symbol denotes type of mercury source Back-trajectories starting at the indicated fraction of the mixed layer height. Circles on the trajectories mark the hourly positions 0.1 coal-fired power plants 10 - 50 0.3 other fuel combustion 50 - 100 0.5 waste incineration 100 – 200 0.7 metallurgical 200 - 400 manufacturing & other 0.9 400 - 600 Large Point Sources of Reactive Gaseous Mercury (RGM) Emissions Based on the 2002 U.S EPA National Emissions Inventory (NEI)

  9. The next day…

  10. size/shape of symbol denotes amount of mercury emitted (kg/yr) color of symbol denotes type of mercury source Back-trajectories starting at the indicated fraction of the mixed layer height. Circles on the trajectories mark the hourly positions 0.1 coal-fired power plants 10 - 50 0.3 other fuel combustion 50 - 100 0.5 waste incineration 100 – 200 0.7 metallurgical 200 - 400 manufacturing & other 0.9 400 - 600 Large Point Sources of Reactive Gaseous Mercury (RGM) Emissions Based on the 2002 U.S EPA National Emissions Inventory (NEI)

  11. size/shape of symbol denotes amount of mercury emitted (kg/yr) color of symbol denotes type of mercury source Back-trajectories starting at the indicated fraction of the mixed layer height. Circles on the trajectories mark the hourly positions 0.1 coal-fired power plants 10 - 50 0.3 other fuel combustion 50 - 100 0.5 waste incineration 100 – 200 0.7 metallurgical 200 - 400 manufacturing & other 0.9 400 - 600 Large Point Sources of Reactive Gaseous Mercury (RGM) Emissions Based on the 2002 U.S EPA National Emissions Inventory (NEI)

  12. size/shape of symbol denotes amount of mercury emitted (kg/yr) color of symbol denotes type of mercury source Back-trajectories starting at the indicated fraction of the mixed layer height. Circles on the trajectories mark the hourly positions 0.1 coal-fired power plants 10 - 50 0.3 other fuel combustion 50 - 100 0.5 waste incineration 100 – 200 0.7 metallurgical 200 - 400 manufacturing & other 0.9 400 - 600 Large Point Sources of Reactive Gaseous Mercury (RGM) Emissions Based on the 2002 U.S EPA National Emissions Inventory (NEI)

  13. size/shape of symbol denotes amount of mercury emitted (kg/yr) color of symbol denotes type of mercury source Back-trajectories starting at the indicated fraction of the mixed layer height. Circles on the trajectories mark the hourly positions 0.1 coal-fired power plants 10 - 50 0.3 other fuel combustion 50 - 100 0.5 waste incineration 100 – 200 0.7 metallurgical 200 - 400 manufacturing & other 0.9 400 - 600 Large Point Sources of Reactive Gaseous Mercury (RGM) Emissions Based on the 2002 U.S EPA National Emissions Inventory (NEI)

  14. size/shape of symbol denotes amount of mercury emitted (kg/yr) color of symbol denotes type of mercury source Back-trajectories starting at the indicated fraction of the mixed layer height. Circles on the trajectories mark the hourly positions 0.1 coal-fired power plants 10 - 50 0.3 other fuel combustion 50 - 100 0.5 waste incineration 100 – 200 0.7 metallurgical 200 - 400 manufacturing & other 0.9 400 - 600 Large Point Sources of Reactive Gaseous Mercury (RGM) Emissions Based on the 2002 U.S EPA National Emissions Inventory (NEI)

  15. size/shape of symbol denotes amount of mercury emitted (kg/yr) color of symbol denotes type of mercury source Back-trajectories starting at the indicated fraction of the mixed layer height. Circles on the trajectories mark the hourly positions 0.1 coal-fired power plants 10 - 50 0.3 other fuel combustion 50 - 100 0.5 waste incineration 100 – 200 0.7 metallurgical 200 - 400 manufacturing & other 0.9 400 - 600 Large Point Sources of Reactive Gaseous Mercury (RGM) Emissions Based on the 2002 U.S EPA National Emissions Inventory (NEI)

  16. The next day…

  17. size/shape of symbol denotes amount of mercury emitted (kg/yr) color of symbol denotes type of mercury source Back-trajectories starting at the indicated fraction of the mixed layer height. Circles on the trajectories mark the hourly positions 0.1 coal-fired power plants 10 - 50 0.3 other fuel combustion 50 - 100 0.5 waste incineration 100 – 200 0.7 metallurgical 200 - 400 manufacturing & other 0.9 400 - 600 Large Point Sources of Reactive Gaseous Mercury (RGM) Emissions Based on the 2002 U.S EPA National Emissions Inventory (NEI)

  18. size/shape of symbol denotes amount of mercury emitted (kg/yr) color of symbol denotes type of mercury source Back-trajectories starting at the indicated fraction of the mixed layer height. Circles on the trajectories mark the hourly positions 0.1 coal-fired power plants 10 - 50 0.3 other fuel combustion 50 - 100 0.5 waste incineration 100 – 200 0.7 metallurgical 200 - 400 manufacturing & other 0.9 400 - 600 Large Point Sources of Reactive Gaseous Mercury (RGM) Emissions Based on the 2002 U.S EPA National Emissions Inventory (NEI)

  19. size/shape of symbol denotes amount of mercury emitted (kg/yr) color of symbol denotes type of mercury source Back-trajectories starting at the indicated fraction of the mixed layer height. Circles on the trajectories mark the hourly positions 0.1 coal-fired power plants 10 - 50 0.3 other fuel combustion 50 - 100 0.5 waste incineration 100 – 200 0.7 metallurgical 200 - 400 manufacturing & other 0.9 400 - 600 Large Point Sources of Reactive Gaseous Mercury (RGM) Emissions Based on the 2002 U.S EPA National Emissions Inventory (NEI)

  20. size/shape of symbol denotes amount of mercury emitted (kg/yr) color of symbol denotes type of mercury source Back-trajectories starting at the indicated fraction of the mixed layer height. Circles on the trajectories mark the hourly positions 0.1 coal-fired power plants 10 - 50 0.3 other fuel combustion 50 - 100 0.5 waste incineration 100 – 200 0.7 metallurgical 200 - 400 manufacturing & other 0.9 400 - 600 Large Point Sources of Reactive Gaseous Mercury (RGM) Emissions Based on the 2002 U.S EPA National Emissions Inventory (NEI)

  21. size/shape of symbol denotes amount of mercury emitted (kg/yr) color of symbol denotes type of mercury source Back-trajectories starting at the indicated fraction of the mixed layer height. Circles on the trajectories mark the hourly positions 0.1 coal-fired power plants 10 - 50 0.3 other fuel combustion 50 - 100 0.5 waste incineration 100 – 200 0.7 metallurgical 200 - 400 manufacturing & other 0.9 400 - 600 Large Point Sources of Reactive Gaseous Mercury (RGM) Emissions Based on the 2002 U.S EPA National Emissions Inventory (NEI)

  22. size/shape of symbol denotes amount of mercury emitted (kg/yr) color of symbol denotes type of mercury source Back-trajectories starting at the indicated fraction of the mixed layer height. Circles on the trajectories mark the hourly positions 0.1 coal-fired power plants 10 - 50 0.3 other fuel combustion 50 - 100 0.5 waste incineration 100 – 200 0.7 metallurgical 200 - 400 manufacturing & other 0.9 400 - 600 Large Point Sources of Reactive Gaseous Mercury (RGM) Emissions Based on the 2002 U.S EPA National Emissions Inventory (NEI)

  23. The next day…

  24. size/shape of symbol denotes amount of mercury emitted (kg/yr) color of symbol denotes type of mercury source Back-trajectories starting at the indicated fraction of the mixed layer height. Circles on the trajectories mark the hourly positions 0.1 coal-fired power plants 10 - 50 0.3 other fuel combustion 50 - 100 0.5 waste incineration 100 – 200 0.7 metallurgical 200 - 400 manufacturing & other 0.9 400 - 600 Large Point Sources of Reactive Gaseous Mercury (RGM) Emissions Based on the 2002 U.S EPA National Emissions Inventory (NEI)

  25. size/shape of symbol denotes amount of mercury emitted (kg/yr) color of symbol denotes type of mercury source Back-trajectories starting at the indicated fraction of the mixed layer height. Circles on the trajectories mark the hourly positions 0.1 coal-fired power plants 10 - 50 0.3 other fuel combustion 50 - 100 0.5 waste incineration 100 – 200 0.7 metallurgical 200 - 400 manufacturing & other 0.9 400 - 600 Large Point Sources of Reactive Gaseous Mercury (RGM) Emissions Based on the 2002 U.S EPA National Emissions Inventory (NEI)

  26. size/shape of symbol denotes amount of mercury emitted (kg/yr) color of symbol denotes type of mercury source Back-trajectories starting at the indicated fraction of the mixed layer height. Circles on the trajectories mark the hourly positions 0.1 coal-fired power plants 10 - 50 0.3 other fuel combustion 50 - 100 0.5 waste incineration 100 – 200 0.7 metallurgical 200 - 400 manufacturing & other 0.9 400 - 600 Large Point Sources of Reactive Gaseous Mercury (RGM) Emissions Based on the 2002 U.S EPA National Emissions Inventory (NEI)

  27. size/shape of symbol denotes amount of mercury emitted (kg/yr) color of symbol denotes type of mercury source Back-trajectories starting at the indicated fraction of the mixed layer height. Circles on the trajectories mark the hourly positions 0.1 coal-fired power plants 10 - 50 0.3 other fuel combustion 50 - 100 0.5 waste incineration 100 – 200 0.7 metallurgical 200 - 400 manufacturing & other 0.9 400 - 600 Large Point Sources of Reactive Gaseous Mercury (RGM) Emissions Based on the 2002 U.S EPA National Emissions Inventory (NEI)

  28. size/shape of symbol denotes amount of mercury emitted (kg/yr) color of symbol denotes type of mercury source Back-trajectories starting at the indicated fraction of the mixed layer height. Circles on the trajectories mark the hourly positions 0.1 coal-fired power plants 10 - 50 0.3 other fuel combustion 50 - 100 0.5 waste incineration 100 – 200 0.7 metallurgical 200 - 400 manufacturing & other 0.9 400 - 600 Large Point Sources of Reactive Gaseous Mercury (RGM) Emissions Based on the 2002 U.S EPA National Emissions Inventory (NEI)

  29. size/shape of symbol denotes amount of mercury emitted (kg/yr) color of symbol denotes type of mercury source Back-trajectories starting at the indicated fraction of the mixed layer height. Circles on the trajectories mark the hourly positions 0.1 coal-fired power plants 10 - 50 0.3 other fuel combustion 50 - 100 0.5 waste incineration 100 – 200 0.7 metallurgical 200 - 400 manufacturing & other 0.9 400 - 600 Large Point Sources of Reactive Gaseous Mercury (RGM) Emissions Based on the 2002 U.S EPA National Emissions Inventory (NEI)

  30. The next day…

  31. size/shape of symbol denotes amount of mercury emitted (kg/yr) color of symbol denotes type of mercury source Back-trajectories starting at the indicated fraction of the mixed layer height. Circles on the trajectories mark the hourly positions 0.1 coal-fired power plants 10 - 50 0.3 other fuel combustion 50 - 100 0.5 waste incineration 100 – 200 0.7 metallurgical 200 - 400 manufacturing & other 0.9 400 - 600 Large Point Sources of Reactive Gaseous Mercury (RGM) Emissions Based on the 2002 U.S EPA National Emissions Inventory (NEI)

  32. size/shape of symbol denotes amount of mercury emitted (kg/yr) color of symbol denotes type of mercury source Back-trajectories starting at the indicated fraction of the mixed layer height. Circles on the trajectories mark the hourly positions 0.1 coal-fired power plants 10 - 50 0.3 other fuel combustion 50 - 100 0.5 waste incineration 100 – 200 0.7 metallurgical 200 - 400 manufacturing & other 0.9 400 - 600 Large Point Sources of Reactive Gaseous Mercury (RGM) Emissions Based on the 2002 U.S EPA National Emissions Inventory (NEI)

  33. size/shape of symbol denotes amount of mercury emitted (kg/yr) color of symbol denotes type of mercury source Back-trajectories starting at the indicated fraction of the mixed layer height. Circles on the trajectories mark the hourly positions 0.1 coal-fired power plants 10 - 50 0.3 other fuel combustion 50 - 100 0.5 waste incineration 100 – 200 0.7 metallurgical 200 - 400 manufacturing & other 0.9 400 - 600 Large Point Sources of Reactive Gaseous Mercury (RGM) Emissions Based on the 2002 U.S EPA National Emissions Inventory (NEI)

  34. size/shape of symbol denotes amount of mercury emitted (kg/yr) color of symbol denotes type of mercury source Back-trajectories starting at the indicated fraction of the mixed layer height. Circles on the trajectories mark the hourly positions 0.1 coal-fired power plants 10 - 50 0.3 other fuel combustion 50 - 100 0.5 waste incineration 100 – 200 0.7 metallurgical 200 - 400 manufacturing & other 0.9 400 - 600 Large Point Sources of Reactive Gaseous Mercury (RGM) Emissions Based on the 2002 U.S EPA National Emissions Inventory (NEI)

  35. size/shape of symbol denotes amount of mercury emitted (kg/yr) color of symbol denotes type of mercury source Back-trajectories starting at the indicated fraction of the mixed layer height. Circles on the trajectories mark the hourly positions 0.1 coal-fired power plants 10 - 50 0.3 other fuel combustion 50 - 100 0.5 waste incineration 100 – 200 0.7 metallurgical 200 - 400 manufacturing & other 0.9 400 - 600 Large Point Sources of Reactive Gaseous Mercury (RGM) Emissions Based on the 2002 U.S EPA National Emissions Inventory (NEI)

  36. Recent measurements

  37. Recent measurements

  38. Recent measurements

  39. Issues/Updates/Challenges at Beltsville • The more polluted environment at Beltsville leads to significant trap bias • in Tekran 2537. Cleaning gold traps, even in Aqua Regia, provides only temporary improvement. Traps must really be replaced every 6 months ($1400/pair per instrument). • We will explore the option of making our own gold traps to save considerable expense. • EPA-purchased 2537B detector has been plagued by more persistent problems than any of the 2537A’s fielded by NOAA at Grand Bay or Beltsville. Problems are mostly transient and so far have defied diagnosis at Tekran. It may be necessary to return the instrument for a thorough analysis and repair. • Power stability at Beltsville, for the most part acceptable, deteriorated in Summer 2008. We will monitor stability closely this Summer. • We are collaborating with Mark Engle and Allan Kolker, USGS-Reston, to collect MOUDI and Hi-Vol aerosol samples periodically at the site.

  40. Measurements at Grand Bay NERR, MS

  41. View from top of 10 m tower looking at the southerly (prevailing wind) sampling sector over the U.S. Fish and Wildlife Service Pavilion at Grand Bay NERR

  42. As in 2007, most pronounced correlation was between ozone and RGM, especially during the Spring (March-May). Similar concentrations of RGM and O3 were observed in Springtime 2007 and 2008. Higher RGM in Summer ’08 than Summer ‘07 Spring 2007 Spring 2008

  43. Across all seasons, higher RGM levels were associated with drier air parcels containing aged emissions. Together with the RGM/O3 correlation, this suggests that aged continental emissions, not extremely local sources, are responsible for enhanced RGM at the site. Downward mixing from the middle and upper trop may be involved as well. Lack of increase of FPM at high RH suggests no phase partitioning of RGM to small particles at high RH, but sea salt aerosols may take up RGM.

  44. Two systems were configured identically (pink), then System 2 was fitted with a 10-micron cut point elutriator (blue) over the course of several days. Results suggest that there may be as much mercury in the coarse (sea salt) aerosol fraction as in the fine fraction. Studies will be repeated periodically at the site.

  45. Upgrades to the Site • Under the auspices of the Mississippi Department of Environmental Quality, precipitation collectors will be added at the Grand Bay NERR for the measurement of: • Rainfall amounts • Ott Pluvio gauge • Major ions in precipitation (NTN) • Aerochem collector, upgrade to NCON when approved • Total mercury and trace metals in precipitation (MDN) • Aerochem collector, upgrade to NCON when approved • Siting criteria have been reviewed and approved, and purchase requisitions have been prepared for site improvement and instrument procurement.

  46. Planned Intensive, Spring-Summer 2010 • Collaborative research involving NOAA, GA Tech, Florida State University, and others • Focus is on the role of halogen species in the MBL and their oxidation of • Hg(0) to RGM species, at the surface and aloft. • Components include ongoing speciated mercury and ancillary trace gas measurements at the NERR. A 3-wavelength nephelometer will be added, as will radiosonde/ozonesonde launches from the NERR to determine thermal and chemical structure of the troposphere. • Greg Huey (GA Tech) will measure Br2, BrO, BrCl, and HOBr at the surface via Chemical Ionization Mass Spectrometry. • Tony Hynes (U. Miami) will attempt to measure total and speciated RGM at the surface and aloft using coated and uncoated denuders using the technique of programmable thermal desorption. • Other measurements and participants to be added as work progresses.

  47. Data Reduction Scheme at ARL/HQ • A batch file is executed that first concatenates all the five-minute data files • During review of the raw data, three files (.bGEM, .bRGM, .bFPM) are produced by-hand that contain the JDD start and end times of any period of bad data. The program then reads these files and flags the data • A FORTRAN program is then run in batch mode • All automatic calibrations are parsed out and written to a • separate file • GEM trap bias is calculated for each hour. If it exceeds 10% • then each five-minute period in the GEM cycle and each period in the • desorb cycle is adjusted to increase the low-trap result up to the • proper ratio. • GEM for the hour is just the average of the 12 five-minute results. • FPM for the hour is the sum of the three FPM desorbs minus three • times the pyrolyzer value.

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