Diurnal and seasonal variation of mercury species at coastal-suburban, urban, and rural sites in the southeastern United States

Observations for the 2005-2008 time period from three Southeastern Aerosol Research and Characterization (SEARCH) air quality monitoring sites are examined for diurnal and seasonal variation in concentrations of gaseous elemental mercury (GEM), gaseous oxidized mercury (GOM), and particle bound mercury (HgP < 2.5 mu m). The sites are located at 1) a suburban-coastal location near Pensacola, Florida (OLF), 2) an urban location in Birmingham, Alabama (BHM), and 3) a rural location west-northwest of Atlanta, Georgia (YRK). Average concentrations of GEM at both OLF and YRK are 1.35 ng m(-3), whereas at BHM it is 2.12 ng m(-3). All sites show increase in GEM concentration during the morning hours (0.023 and 0.011 ng m(-3) hr(-1) at OLF and YRK between 6 and 10 AM, 0.038 ng m(-3) hr(-1) at BHM between 5 and 10 AM) due to downward mixing of higher concentrations from the residual layer, after which OLF and YRK show negligible variation compared to decrease in concentration at BHM (23-1.9 ng m(-3) from 10 AM to 6 PM). All sites show seasonal variation of GEM with enhanced concentrations found in winter and spring. Average GOM concentrations are 4.26, 8.55, and 78.2 pg m(-3) at OLF, YRK, and BHM, respectively. Seasonally, GOM values are enhanced during fall and spring. All sites undergo a sinusoidal daytime variation of GOM that peaks in the afternoon, while BHM additionally exhibits an early morning enhancement likely caused by vertical mixing. The average HgP concentrations at OLF, YRK, and BHM are 2.49, 4.43, and 39.5 pg m-3, respectively. At OLF, vertical mixing causes an early morning increase in HgP concentration followed by an afternoon decline during all seasons. A daytime increase in HgP is found at YRK for all seasons, while at BHM, nocturnal accumulation followed by a daytime decline is also found for most seasons except winter. In winter, concentrations increase due to vertical mixing in the morning and then decline as the boundary layer grows. Boundary layer processes appear to play an important role in the seasonal and diurnal variation of Hg species and further investigation utilizing a boundary layer process model is warranted. (C) 2011 Elsevier Ltd. All rights reserved.