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Atmospheric Mercury Measurements

and Modeling at the Grand Bay NERR

Mark Cohen, Winston

Luke, Paul Kelley, Roland

Draxler, Fantine Ngan,

and Richard Artz



NOAA Air Resources Lab,

Silver Spring, Maryland



Gulf of Mexico Alliance

Mercury Forum

May 10-12, 2010

Mote Marine Lab,

Sarasota, FL

http://www.arl.noaa.gov/mercury.php

Gulf of Mexico Alliance Mercury Forum, May 10-12, 2010, Mote Marine Lab, Sarasota, Florida

Four Collaborative Comprehensive

Atmospheric Mercury Measurement Sites



2002 Mercury

Emissions data

from USEPA,

Part of AMNet, Envr. Canada, Allegheny Portage

and CEC (kg/yr) with Canaan Valley Institute

an emerging 5-10

and National Park Service



inter-agency 10-50

50-100

speciated 100–300 Beltsville

mercury 300–500

with USEPA,

Univ. of Maryland,

ambient 500–1000

and MD DNR



concentration 1000–3500 Canaan Valley

measurement Type of Emissions Source

with Canaan Valley Inst.

and Univ. of Maryland

network coal-fired power plants

Appalachian Lab



other fuel combustion Grand Bay

waste incineration with Grand Bay NERR, USEPA,

Mississippi Dept. of Environmental Quality,

metallurgical and Jackson State University

manufacturing & other



Gulf of Mexico Alliance Mercury Forum, May 10-12, 2010, Mote Marine Lab, Sarasota, Florida

Grand Bay NERR site often sees Gulf of Mexico air

masses, but is potentially influenced by several

regional mercury emissions sources

type of source

Monitoring Site coal-fired power plant

Mississippi Alabama

NOAA waste incinerator

manufacturing

SEARCH

Barry

metallurgical

USGS MS 22

other fuel combustion

UWF/FSU paper manuf AL02





MDN Molino

Mobile Pace

Daniel

Pascagoula Holcim Cement

MSW incin OLF Crist

Mobile

Ellyson

AL24 Bay Weeks

Pascagoula Bay

Watson Pensacola

where the wind comes haz waste incin





from that we see at the NOAA Grand Bay

NERR Hg site

Grand Bay site total atmospheric

mercury emissions

(kg/yr, 1999 EPA NEI)

1 – 50



50 - 100

100 - 200



200 - 400

Gulf of Mexico Alliance Mercury Forum, May 10-12, 2010, Mote Marine Lab, Sarasota, Florida

Atmospheric Mercury Monitoring

Station at the Grand Bay NERR



view from top of the tower









mercury and trace gas

monitoring tower

(10 meters)



Gulf of Mexico Alliance Mercury Forum, May 10-12, 2010, Mote Marine Lab, Sarasota, Florida

Some of the instrumentation inside

the trailer at the Grand Bay NERR site









Gulf of Mexico Alliance Mercury Forum, May 10-12, 2010, Mote Marine Lab, Sarasota, Florida

Measurements began in 2006

and the site has evolved over time

Sept 2006: Summer 2010:

Aug 21 – Oct 5, 2008: site Field Intensive

Speciated Hg, shut down due to threat of

SO2, O3, and CO (being planned)

hurricanes

measurements begin at

“inland” site

Jan 2010:

Jan 2008: Black

2005-2006: NO/NOy Carbon

site selection added added

2005









2006









2007









2008









2009









2010

Feb 2007: Meteorological

measurements added





Oct 2007: 2010: MS DEP adds

Move to “coastal” comprehensive suite

site near Pavillion; of wet deposition

2nd Tekran speciated Hg

measurements with

measurement suite added funding from USEPA



Gulf of Mexico Alliance Mercury Forum, May 10-12, 2010, Mote Marine Lab, Sarasota, Florida

Atmospheric mercury measurements

are very challenging







“Hmmm…

maybe

better if

the tower

goes

vertical?”









Gulf of Mexico Alliance Mercury Forum, May 10-12, 2010, Mote Marine Lab, Sarasota, Florida

The people who are

making the measurements

Winston Luke

Principal Investigator,

NOAA Air Resources Lab

Paul Kelley

Jake Walker Instrument engineer,

Site Operator, data acquisition and

Grand Bay NERR management,

NOAA Air Resources Lab









Gulf of Mexico Alliance Mercury Forum, May 10-12, 2010, Mote Marine Lab, Sarasota, Florida

Current Atmospheric Measurements of Ambient

Air Concentrations and Meteorological Data



Elemental mercury (two instruments)

“Speciated” Atmospheric

Fine particulate mercury (two instruments)

Mercury Concentrations

Reactive gaseous mercury (two instruments)



Sulfur dioxide



Ozone Trace gases and other

measurements to help

Carbon Monoxide

understand and interpret

Nitrogen Oxides (NO, NOy) mercury data

Aerosol Black Carbon



Wind speed, Wind Direction



Temperature, Relative Humidity Meteorological Data

Precipitation Amount



Gulf of Mexico Alliance Mercury Forum, May 10-12, 2010, Mote Marine Lab, Sarasota, Florida

Wet Deposition Measurements added in

2010 by the Mississippi Department

of Environmental Protection

(Henry Folmar, Becky Comyns, others),

with funding from the USEPA





Continuous digital measurement of

Precipitation precipitation amount



Major Ions Weekly measurements of concentrations in

pH, SO4-2, NO3-, PO4-3, Cl-, precipitation (NADP-NTN)

NH4+, Ca+2, Mg+2, K+, Na+



Weekly measurements of concentration in

Total Mercury precipitation (NADP-MDN)



Monthly measurements of concentration in

Methyl Mercury precipitation (composite)



Selected Trace Metals Weekly measurements of concentrations in

As, Cd, Cr, Cu, Pb, Ni, Se, Zn precipitation (MDN Heavy Metal Protocol)



Gulf of Mexico Alliance Mercury Forum, May 10-12, 2010, Mote Marine Lab, Sarasota, Florida

Example of Ambient Concentration

Measurements at the Grand Bay site



The two sets

of speciated

mercury

measurements

generally track

each other

well



Sometimes we

see relatively

pronounced

peaks in one

or more forms

of mercury (in

this example,

RGM)





Gulf of Mexico Alliance Mercury Forum, May 10-12, 2010, Mote Marine Lab, Sarasota, Florida

With two speciation units, can get continuous data

and can also carry out methodological experiments



 PINK data points:

two systems were

configured identically,

to allow only particles

less than 2.5 microns to

be analyzed



 BLUE data points:

System 2 was altered to

allow particles up to 10

microns to be analyzed



 Results suggest that

there may be as much

mercury in the coarse

(sea salt) aerosol

fraction as in the fine

fraction.



Gulf of Mexico Alliance Mercury Forum, May 10-12, 2010, Mote Marine Lab, Sarasota, Florida

Grand Bay Atmospheric Field Intensive

Scheduled for July-Aug 2010

Ground-Based Measurements



• Winston Luke and Paul Kelley (NOAA ARL),

(ongoing) mercury, trace gas, black carbon, met data

• Jake Walker (Grand Bay NERR)



(ongoing) wet deposition: major ions, mercury, methyl-Hg, trace metals • Mississippi State Dept of Env Protection/EPA

Will try to switch to event-based during intensive • Jake Walker (Grand Bay NERR)



ambient concentrations of BrO at the surface

via Chemical Ionization Mass Spectrometry • Greg Huey (Georgia Tech)

(and possibly other Br compounds, e.g., Br2, BrCl, and HOBr





isotopic mercury analysis of event-based precipitation and aerosols • Bill Landing, Flip Froelich (Florida State Univ)



trace metal analysis of size-segregated aerosol

• Mark Engle (USGS)

Spring 2010 and possibly during intensive





Aircraft and Above Surface Measurements



aircraft flights measuring concentrations of Hg0 (Tekran), •Stephen Corda, John Muratore, & colleagues

(Univ. of Tennessee Space Institute – UTSI)

total and “speciated” RGM (coated/uncoated denuders),

• Hynes and Swartzendruber (Univ of Miami)

O3, SO2, and particle count • Luke and Kelley (NOAA ARL)



• Luke and Kelley (NOAA ARL)

vertical distribution of O3 and met data above the site (ozonesondes)

• Jake Walker (Grand Bay NERR)



Gulf of Mexico Alliance Mercury Forum, May 10-12, 2010, Mote Marine Lab, Sarasota, Florida

Atmospheric Fate and Transport:

Measurements and Modeling





Hg from

 Model other sources:

evaluation? local, regional

& more distant





 Source

attribution for emissions of

deposition? Hg(0), Hg(II), Hg(p)



Reactive halogens in

marine boundary layer

 Want to Measurement

of ambient air Measurement

provide concentrations of wet

deposition

 Enhanced oxidation of

Hg(0) to RGM?

deposition  Enhanced deposition?

estimates to wet and dry

GOM deposition

to the watershed

wet and dry deposition

ecosystem to the water surface



models



Gulf of Mexico Alliance Mercury Forum, May 10-12, 2010, Mote Marine Lab, Sarasota, Florida

HYSPLIT-Hg -- a specially configured version of

the HYSPLIT atmospheric fate and transport model





 Puffs or particles

emitted from a source



 Chemistry, dispersion

and deposition

simulated



 Puffs grown and split



 Splitting can

overwhelm

computational

resources





Gulf of Mexico Alliance Mercury Forum, May 10-12, 2010, Mote Marine Lab, Sarasota, Florida

HYSPLIT-Hg

now includes an integrated Eulerian grid



 In HYSPLIT (4.9), puffs

are “transferred” to an

Eulerian grid after a

specified time (e.g., 96

hrs)



 the mercury in those

puffs is simulated on

that grid from then on…



 Combines plume

simulation in short-

range with Eulerian

simulation for long-

range transport





Gulf of Mexico Alliance Mercury Forum, May 10-12, 2010, Mote Marine Lab, Sarasota, Florida

Initial Model Evaluation focusing on episodes





 Can the model

reproduce episodes

of high measured

mercury

concentrations?



 Can the model

reproduce high

mercury wet

deposition episodes?







Gulf of Mexico Alliance Mercury Forum, May 10-12, 2010, Mote Marine Lab, Sarasota, Florida

Meteorological data: a critical model input





 During model evaluation exercises,

want to diagnose weaknesses in

model physics and chemistry,

without large influence of met data

errors



 Would like to examine trade-off

between high-resolution and

coarser met data sets, which are

more routinely available



 Dr. Venkata Dodla (JSU) and Dr.

Fantine Ngan (NOAA ARL) are

creating high resolution, ground-

truthed met data sets for episodes

in the region around the site (e.g.,

horizontal resolution of 4 km) Wind speed (shaded) & wind vector (arrows) on

5/6/08, 18 UTC (approx time of episode peak)

Gulf of Mexico Alliance Mercury Forum, May 10-12, 2010, Mote Marine Lab, Sarasota, Florida

Series 3300 CEM - Continuous Speciated Mercury Data

Resolution: 2.5 min Duration: 11 Days





HgT









Emissions data: a critical model input

12

Hg0

Hg2

10







8

Hg - (ug/m )

3









6







4







2







0

25-Aug 26-Aug 27-Aug 28-Aug 29-Aug 30-Aug 31-Aug 01-Sep 02-Sep 03-Sep 04-Sep 05-Sep

Lowman reported dramatic drop in Brewton paper mill :

mercury emissions in 2008 TRI Hg emissions in 2002

NEI , but do not appear

 In model evaluation, want to in 2000-2008 TRI

diagnose weaknesses in model

without large influence of

emissions errors CRIST: New

scrubber

installed

 Need accurate, speciated Dec 2009 will

emissions estimates for all dramatically

sources impacting the site – reduce RGM

for the time period of the emissions

episode

IPSCO Steel:

 Need accurate emissions data significant Hg

for any assessment emissions in

2002 NEI, but

Pascagoula MSW negligible

 We all need accurate emissions Grand Bay

Incinerator shut emissions in

information. How can we NERR site 2008 TRI

down in Jan 2001,

share what we already have,

but still in 2002 NEI

and improve the information

where needed?

Large mercury emissions point sources from

May 10-12, 2010, National Lab, Sarasota, Inventory (NEI)

Gulf of Mexico Alliance Mercury Forum,USEPA 2002 Mote Marine EmissionsFlorida

Collaboration with Jackson State University

on atmospheric mercury modeling in the region







 led by Shelton Swanier and Anjaneyulu

Yerramilli, the director of the Trent Lott

Geospatial and Visualization Center



 Manuscript in preparation analyzing the May

5-6 2008 high-RGM episode at the site.



 High-resolution met data (4 km) is being

generated and utilized



 ALSO: JSU Professor Jerzy Leszczynski and

colleagues are carrying out computational

chemistry estimates of atmospherically

relevant reactions of mercury





Gulf of Mexico Alliance Mercury Forum, May 10-12, 2010, Mote Marine Lab, Sarasota, Florida

(Evolving) Atmospheric Chemical

Reaction Scheme for Mercury





 Complete?



 Accurate?



 Concentrations

of Reactants?



 What is RGM?









Gulf of Mexico Alliance Mercury Forum, May 10-12, 2010, Mote Marine Lab, Sarasota, Florida

HYSPLIT Training









http://www.ertcorp.com/HYSPLIT

Gulf of Mexico Alliance Mercury Forum, May 10-12, 2010, Mote Marine Lab, Sarasota, Florida

Acknowledgements





 Jake Walker, Mark Woodrey, Glen Ruple (Grand Bay National Estuarine

Research Reserve)

 Shelton Swanier, Jerzy Lesczcynski, Yerramilli Anjaneyulu, Venkatesh Dodla,

Hari Dasari, & others (Jackson State Univ.)

 Steve Brooks (NOAA ATDD and Canann Valley Institute)

 Glenn Rolph, Barbara Stunder, Ariel Stein, Steve Fine (NOAA Air Resources

Laboratory)

 David Schmeltz, Tim Sharac, Rick Haeuber, Sam Napolitano (US EPA Clean Air

Markets Division)

 Gary Matlock, Russell Callender, Jawed Hameedi (NOAA NOS Nat’l Centers

for Coastal Ocean Science)

 U.S. Fish and Wildlife Service -- Grand Bay National Wildlife Refuge

Gulf of Mexico Alliance Mercury Forum, May 10-12, 2010, Mote Marine Lab, Sarasota, Florida

Summary of NOAA ARL NOAA-led measurement

Mercury Measurement Sites Co-located measurement



Dry

Ambient Air Measurements Precipitation Other

Deposition



Collaborators /









Carbon black









Meteorology

Trace Metals









Throughfall

Major Ions

Speciation

Site









Surrogate

Mercury









Mercury

NO/NOy









Surface

(MDN)

Co-locators









(NTN)

SO2









CO

O3

 PI = Winston Luke (NOAA)

 EPA Clean Air Markets Division

Beltsville

(MD)







Univ of Maryland

Maryland DNR

MACTEC

•••• •• • •

 USGS

 PI = Winston Luke (NOAA)

 Grand Bay NERR

Grand

Bay (MS)







MS Dept Envr Quality

U.S. EPA

U.S. Fish & Wildlife Agency

••••• • • • •

 PI = Steve Brooks(CVI/NOAA

Canaan  Canaan Valley Institute

Valley

(WV)

 Univ Md Frostburg

Appalachian Lab

 USGS

• • •• • • •

 PI = Steve Brooks (CVI/NOAA)

Allegheny

Portage

(PA)







Canaan Valley Institute

Pennsylvania DEP

National Park Service

• ••

Where in the world is Bill Landing?









Gulf of Mexico Alliance Mercury Forum, May 10-12, 2010, Mote Marine Lab, Sarasota, Florida

We may be able to measure

atmospheric impacts at the site from

the BP / DEEPWATER HORIZON oil spill







Wind Rose

estimated for

the Grand Bay

NERR site, for

the months of

May and June,

from 2004-2009









Gulf of Mexico Alliance Mercury Forum, May 10-12, 2010, Mote Marine Lab, Sarasota, Florida


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