Temporal variability of mercury speciation in urban air

Semi-continuous measurements of ambient mercury (Hg) species were performed in Detroit, MI, USA for the calendar year 2003. The mean (±standard deviation) concentrations for gaseous elemental mercury (GEM), particulate mercury (HgP), and reactive gaseous mercury (RGM) were 2.2±1.3 ng m−3, 20.8±30.0, and 17.7±28.9 pg m−3, respectively. A clear seasonality in Hg speciation was observed with GEM and RGM concentrations significantly (p<0.001) greater in warm seasons, while HgP concentrations were greater in cold seasons. The three measured Hg species also exhibited clear diurnal trends which were particularly evident during the summer months. Higher RGM concentrations were observed during the day than at night. Hourly HgP and GEM concentrations exhibited a similar diurnal pattern with both being inversely correlated with RGM. Multivariate analysis coupled with conditional probability function analysis revealed the conditions associated with high Hg concentration episodes, and identified the inter-correlations between speciated Hg concentrations, three common urban air pollutants (sulfur dioxide, ozone, and nitric oxides), and meteorological parameters. This analysis suggests that both local and regional sources were major factors contributing to the observed temporal variations in Hg speciation. Boundary layer dynamics and the seasonal meteorological conditions, including temperature and moisture content, were also important factors affecting Hg variability.

[1]  L. Poissant Field observations of total gaseous mercury behaviour: Interactions with ozone concentration and water vapour mixing ratio in air at a rural site , 1997 .

[2]  R. Stevens,et al.  Use of Elemental Tracers to Source Apportion Mercury in South Florida Precipitation , 1999 .

[3]  M. Landis,et al.  Gaseous elemental mercury in the marine boundary layer: evidence for rapid removal in anthropogenic pollution. , 2003, Environmental science & technology.

[4]  John Munthe,et al.  Atmospheric mercury—An overview , 1998 .

[5]  G. Keeler,et al.  Automated speciated mercury measurements in Michigan. , 2005, Environmental science & technology.

[6]  R. Stevens,et al.  Development and characterization of an annular denuder methodology for the measurement of divalent inorganic reactive gaseous mercury in ambient air. , 2002, Environmental science & technology.

[7]  S. Pehkonen,et al.  The chemistry of atmospheric mercury: a review , 1999 .

[8]  S. E. Lindberg,et al.  Atmospheric Mercury Speciation: Concentrations and Behavior of Reactive Gaseous Mercury in Ambient Air , 1998 .

[9]  G. Keeler,et al.  Source–receptor relationships for atmospheric mercury in urban Detroit, Michigan , 2006 .

[10]  R. Stevens,et al.  An investigation of source–receptor relationships for mercury in south Florida using event precipitation data , 1998 .

[11]  S. Lindberg,et al.  Atmospheric speciation of mercury in two contrasting Southeastern US airsheds , 2005 .

[12]  M. Landis,et al.  The effects of the coastal environment on the atmospheric mercury cycle , 2003 .

[13]  Nicola Pirrone,et al.  Dynamics of mercury pollution on regional and global scales , 2005 .

[14]  R. Stevens,et al.  Divalent inorganic reactive gaseous mercury emissions from a mercury cell chlor-alkali plant and its impact on near-field atmospheric dry deposition , 2004 .

[15]  P. Constant,et al.  A year of continuous measurements of three atmospheric mercury species (GEM, RGM and Hgp) in southern Québec, Canada , 2005 .

[16]  Christopher M. Andolina,et al.  Atmospheric gaseous mercury concentrations in New York State: relationships with meteorological data and other pollutants , 2004 .

[17]  Min Young Kim,et al.  Some insights into short-term variability of total gaseous mercury in urban air , 2001 .

[18]  G. Keeler,et al.  Artifacts associated with the measurement of particulate mercury in an urban environment: The influence of elevated ozone concentrations , 2005 .

[19]  Brian Everitt,et al.  Cluster analysis , 1974 .

[20]  R. Draxler An Overview of the HYSPLIT_4 Modelling System for Trajectories, Dispersion, and Deposition , 1998 .

[21]  G. Keeler,et al.  Characterization of complex mixtures in urban atmospheres for inhalation exposure studies. , 2005, Experimental and toxicologic pathology : official journal of the Gesellschaft fur Toxikologische Pathologie.

[22]  M. Pilote,et al.  Mercury concentrations in single event precipitation in southern Québec , 1998 .

[23]  Philip K. Hopke,et al.  Comparison between Conditional Probability Function and Nonparametric Regression for Fine Particle Source Directions , 2004 .

[24]  A. Richter,et al.  Dynamic oxidation of gaseous mercury in the Arctic troposphere at polar sunrise. , 2002, Environmental science & technology.

[25]  I. Olmez,et al.  Atmospheric mercury in the vapor phase, and in fine and coarse particulate matter at Perch River, New York , 1998 .

[26]  Source proximity reflected in spatial and temporal variability in particle and vapor phase Hg concentrations in Detroit, MI , 2005 .

[27]  David S Lee,et al.  Gas-phase mercury in the atmosphere of the United Kingdom , 1998 .

[28]  A. Vette,et al.  Atmospheric mercury in the Lake Michigan basin: influence of the Chicago/Gary urban area. , 2002, Environmental science & technology.

[29]  M. Pilote,et al.  Atmospheric mercury speciation and deposition in the Bay St. François wetlands , 2004 .

[30]  G. Keeler,et al.  Comparison of methods for particulate phase mercury analysis: sampling and analysis , 2002, Analytical and bioanalytical chemistry.