Spatial Patterns and Temporal Changes in Atmospheric-Mercury Deposition for the Midwestern USA, 2001–2016

摘要

Spatial patterns and temporal changes in atmospheric-mercury (Hg) deposition were examined in a five-state study area in the Midwestern USA where 32% of the stationary sources of anthropogenic Hg emissions in the continental USA were located. An extensive monitoring record for wet and dry Hg deposition was compiled for 2001–2016, including 4666 weekly precipitation samples at 13 sites and 27 annual litterfall-Hg samples at 7 sites. This study is the first to examine these Hg data for the Midwestern USA. The median annual precipitation-Hg deposition at the study sites was 10.4 micrograms per square meter per year (μg/m 2 /year) and ranged from 5.8 μg/m 2 /year to 15.0 μg/m 2 /year. The median annual Hg concentration was 9.4 ng/L. Annual litterfall-Hg deposition had a median of 16.1 μg/m 2 /year and ranged from 9.7 to 23.4 μg/m 2 /year. Isopleth maps of annual precipitation-Hg deposition indicated a recurring spatial pattern similar to one revealed by statistical analysis of weekly precipitation-Hg deposition. In that pattern, high Hg deposition in southeastern Indiana was present each year, frequently extending to southern Illinois. Most of central Indiana and central Illinois had similar Hg deposition. Areas with comparatively lower annual Hg deposition were observed in Michigan and Ohio for many years and frequently included part of northern Indiana. The area in southern Indiana where high Hg deposition predominated had the highest number of extreme episodes of weekly Hg deposition delivering up to 15% of the annual Hg load from precipitation in a single week. Modeled 48-h back trajectories indicated air masses for these episodes often arrived from the south and southwest, crossing numerous stationary sources of Hg emissions releasing from 23 to more than 300 kg Hg per year. This analysis suggests that local and regional, rather than exclusively continental or global Hg emissions were likely contributing to the extreme episodes and at least in part, to the spatial patterns of precipitation-Hg deposition in the study area. Statistically significant temporal decreases in weekly precipitation-Hg concentrations in the study area between the periods 2001–2013 and 2014–2016 were observed, coinciding with reported reductions in Hg emissions in the USA required by implementation of national Hg emissions-control rules. These decreases in atmospheric-Hg concentrations are believed to have resulted in the reduced atmospheric-Hg deposition recorded because precipitation depths between the two periods were not significantly different. The Hg-monitoring data for the study area identified an atmospheric deposition response to decreased local and regional Hg emissions.