Atmospheric mercury measurements in the Gulf of Mexico and mid-Atlantic regions: Early results from an emerging monitoring network Winston Luke, Mark Cohen,

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Presentation transcript:

Atmospheric mercury measurements in the Gulf of Mexico and mid-Atlantic regions: Early results from an emerging monitoring network Winston Luke, Mark Cohen, Paul Kelley, Steve Brooks NOAA/Air Resources Laboratory, Silver Spring, MD NOAA/Air Resources Laboratory, Silver Spring, MD Jake Walker Grand Bay National Estuarine Research Reserve, Moss Point, MS Prepared for NADP 2007 Technical Committee Meeting Boulder, CO, Sept , 2007

NOAA Mercury Sites Canaan Valley Institute-NOAA Beltsville EPA-NOAA Three sites committed to speciated mercury ambient concentration measurement network Grand Bay NOAA

Barry Holcim Cement NOAA Grand Bay NERR Hg site Weeks Bay OLF Molino Pace Ellyson Jack Watson AL24 AL02 Crist Pascagoula MSW incin haz waste incin paper manuf Victor J. Daniel Mobile Bay Mobile Pascagoula MississippiAlabama NOAA SEARCH USGS UWF/FSU MDN Monitoring Site coal-fired power plant waste incinerator manufacturing metallurgical other fuel combustion type of mercury emissions source total atmospheric mercury emissions (kg/yr, 1999 EPA NEI) – 50 Location of the NOAA Grand Bay NERR Atmospheric Mercury monitoring site, other atmospheric Hg monitoring sites, and major Hg point sources in the region (EPA 1999 NEI emissions inventory) MS 22

Tekran speciation system (Hg 0, RGM,Tekran speciation system (Hg 0, RGM, Hg-p) installed Sept. 29, 2006 Hg-p) installed Sept. 29, 2006 Ancillary measurements (CO, O 3, SO 2 ) added October 20, 2006Ancillary measurements (CO, O 3, SO 2 ) added October 20, 2006 Sampling Height 4 mSampling Height 4 m Meteorological measurements (T, RH, WS, WD, Solar, Precip Rate/Amount) added March 1, 2007; nearby FWS station provided earlier measurementsMeteorological measurements (T, RH, WS, WD, Solar, Precip Rate/Amount) added March 1, 2007; nearby FWS station provided earlier measurements Measurements at Grand Bay NERR, MS

Hourly Averages

As expected, with a few exceptions Hg 0 concentrations show little or no diurnal variation or dependence on wind direction Elemental Mercury (Hg 0 )

Overnight Event Feb. 28-March 1 Strong correlation between Hg 0 and CO, O 3. Suggests combustion (natural sources?) and transport from source regions to West. RGM, Hg-P ca 20 pg m -3 during episode

All Data With the exception of a few well-defined transport events, Hg-P displays no consistent relationship with WD, and exhibits little or no correlation with other trace species Particulate Mercury (Hg-P)

Strongest correlations seen between RGM and O 3, most of which is driven by seasonal dependence – RGM concentrations are highest, relationship with O 3 is strongest in Spring.

Fall Spring Winter Summer

Association of peak RGM with low RH and CO concentrations typical of continental influence suggests highest Spring peaks of RGM are seen in post-frontal activity, with transport from upwind continental sources to the North RGM/RH relationship is tricky, as phase partitioning may also be at issue Spring

All Data Poor correlation with SO 2 suggests: A mix of primary sources with varying emission characteristics A mix of primary and secondary sources of RGM Different chemical processing and removal rates of SO 2 and RGM during transport Lack of correlation –RGM and Hg-P suggests different sources and/or removal rates of these species

Significant diurnal patterns seen in both RGM and Hg-P, but amplitude of diurnal Hg-P profile is much smaller. Highest RGM and Hg-P concentrations seen in Spring

Similarity to O 3 and SO 2 diurnal profiles confirms the importance of downward mixing in the development of the daytime boundary layer, but does not allow us to differentiate between primary and secondary sources of the mercury species.

Higher RGM Associated with N-E trajectories Peak ~ 50 pg m -3 Peak ~ 118 pg m -3 Peak ~ 55 pg m -3 Peak ~ 105 pg m -3 Peak ~ 100 pg m -3 Peak ~ 65 pg m -3

RGM = 105 pg m-3

RGM = 117 pg m-3

RGM = 50.5 pg m-3

RGM = 50.5→12.4 pg m-3

Lower RGM in Maritime trajectories Peak ~ 7 pg m -3 Peak ~ 2 pg m -3 Peak ~ 10 pg m -3

RGM + Hg-P Dry Deposition (ng m -2 day -1 ); assumes V d = 2.5 cm s -1 and 0.3 cm s -1 mid day average FallWinter Spring Summer Dry Dep, Grand Bay ( ) Wet Dep, AL24 ( ) Wet Dep, MS22 ( ) Wet Dep, AL02 ( ) Deposition Estimates

Summary and Conclusions Grand Bay NERR Site typically exhibits rural/remote characteristics with generally low concentrations of all species, but with occasional transport related episodes of higher concentrations.Grand Bay NERR Site typically exhibits rural/remote characteristics with generally low concentrations of all species, but with occasional transport related episodes of higher concentrations. Elemental Hg shows little variation, little or no dependence on WD, and no discernible diurnal pattern, as expected.Elemental Hg shows little variation, little or no dependence on WD, and no discernible diurnal pattern, as expected. Hg-P behaves similarly, but with more transport related episodes and a modest diurnal profile.Hg-P behaves similarly, but with more transport related episodes and a modest diurnal profile. RGM exhibits a more pronounced diurnal profile. Both RGM and Hg-P profiles show increases in daytime, coincident with O 3 and SO 2 peaks, illustrating the importance of downward mixing of an aloft reservoir with the breakup of the nocturnal boundary layer. Photochemical (secondary) production may also be occurring.RGM exhibits a more pronounced diurnal profile. Both RGM and Hg-P profiles show increases in daytime, coincident with O 3 and SO 2 peaks, illustrating the importance of downward mixing of an aloft reservoir with the breakup of the nocturnal boundary layer. Photochemical (secondary) production may also be occurring.

Summary and Conclusions RGM correlates most closely with O 3 in Springtime, and is RGM correlates most closely with O 3 in Springtime, and is associated with dryer air characteristic of continental associated with dryer air characteristic of continental emissions (CO ca 200 ppb). emissions (CO ca 200 ppb). These results suggest RGM is transported from northerly continental sources following cold-frontal penetration in Spring. Reduced frequency of cold frontal passage at the site in Summer leads to lower RGM levels, more sporadic transport to the site from upwind sources.These results suggest RGM is transported from northerly continental sources following cold-frontal penetration in Spring. Reduced frequency of cold frontal passage at the site in Summer leads to lower RGM levels, more sporadic transport to the site from upwind sources. No evidence of strong, substantial RGM production or transport in marine (Gulf) air masses. Hg in coarse aerosols?No evidence of strong, substantial RGM production or transport in marine (Gulf) air masses. Hg in coarse aerosols? Dry deposition estimates, when compared with nearby MDN deposition records, suggest wet deposition dominates the removal of reactive mercury species at the site, especially in Winter. If substantial Hg exists in the coarse aerosol fraction, the reported dry dep fluxes are under reported.Dry deposition estimates, when compared with nearby MDN deposition records, suggest wet deposition dominates the removal of reactive mercury species at the site, especially in Winter. If substantial Hg exists in the coarse aerosol fraction, the reported dry dep fluxes are under reported.

Recent Developments and Future Activities at Grand Bay NERR Migration from old trailer and site to new trailer at permanent site (water’s edge, 2 miles distant)Migration from old trailer and site to new trailer at permanent site (water’s edge, 2 miles distant) Addition of 10m walk-up scaffoldAddition of 10m walk-up scaffold Addition of second Tekran SystemAddition of second Tekran System Synchronous sampling –precision, QA/QC studies, investigation of Hg/aerosol size, etc. Asynchronous sampling for true continuous measurements Addition of NO/NO Y monitorAddition of NO/NO Y monitor

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 Pictures of Permanent Monitoring Site

Acknowledgments We would like to thank Gary Matlock and Russell Callender of NOAA’s National Centers for Coastal Ocean Science for their generous financial support, and to Durwin Carter (Manager, Grand Bay National Wildlife Refuge) and David Ruple (Manager, Grand Bay National Estuarine Research Reserve) for their ongoing support and assistance of this project.