A National Survey of Total Gaseous Mercury Stable Isotope Composition and Concentration across the US

David Krabbenhoft1, Michael Tate2, Sarah Janssen3, John DeWild4, Jacob Ogorek5 and Ryan Lepak6

With the 2011 promulgation of the Mercury and Air Toxics Standards by the U.S. Environmental Protection Agency, and the successful negotiation by United Nations Environment Programme of the Minamata Convention, global emissions of mercury (Hg) to the atmosphere from anthropogenic sources are expected to decline.  Recent reports suggest regional gaseous Hg declines have already begun well before they were anticipated; however, providing independent evidence for the drivers of such declines is difficult.  To address this challenge, the U.S. Geological Survey and the National Atmospheric Deposition program (NADP) initiated a national-scale effort to establish a baseline of total gaseous mercury (TGM) and Hg stable isotopic compositions using bulk-air sampling at 31 sites distributed across North America over a two-year period (March 2016 – May 2018). To facilitate this effort, the USGS Mercury Research Laboratory developed a simple, small sampling device for TGM that is easily deployed in most any environmental setting using AC or DC power. A priority of our device was that it would allow accurate measurement of TGM, but also allow for measurement of stable Hg isotopes – the first known such effort at a continental scale. Because the isotope measurements require about 5 ng of Hg, the sampling interval for this effort was typically 5-14 days, and as such the measurements represent a time-integrated sample. Approximately two thirds of our TGM samplers were operated at MDN or AMNet sites. The other selected sites were chosen to fill geographic gaps in coverage that were principally in the western US.  The network includes a highly diverse set of sites ranging from remote (e.g., Denali National Park, Alaska, Mauna Loa, Hawaii, and Nova Scotia) to highly urbanized locations (e.g., Bronx, New York and Boston, Massachusetts). Measured mass-dependent fractionation (MDF, d202Hg) at urban sites were consistently lighter in d202Hg compared to remote background sites, suggesting the influence of near-field Hg emission sources that based on previous studies supports the notion that the isotopes are reliable indicators of nearby sources.  The site at Oak Ridge National Lab, near the contaminated Y12 plant, had also showed a depleted Hg isotope source signature - mean d202Hg of -0.04±0.36‰. Overall, our study results suggest Hg concentration and isotope enrichments in regional settings.  The most prominent example of this is from the northeastern United States: from the Ohio River Valley to remote sites in northern Maine and Nova Scotia. The long-term goal of this effort is to provide baseline assessments of atmospheric Hg concentrations and isotope abundances that will play a key role in helping to conduct the Minamata effectiveness evaluation.

 

1USGS, dpkrabbe@usgs.gov
2USGS, mttate@usgs.gov
3USGS, sjanssen@usgs.gov
4USGS, jfdewild@usgs.gov
5USGS, jmogorek@usgs.gov
6University of Wisconsin-Madison, rlepak@wisc.edu