Diffuse anthropogenic and naturally mercury‐enriched areas represent long‐lived sources of elemental mercury to the atmosphere. The Nevada Study and Tests of the Release of Mercury From Soils (STORMS) project focused on the measurement of mercury emissions from a naturally enriched area. During the project, concurrent measurements of mercury fluxes from naturally mercury‐enriched substrate were made September 1–4, 1997, using four micrometeorological methods and seven field flux chambers. Ambient air mercury concentrations ranged from 2 to nearly 200 ng m−3 indicating that the field site is a source of atmospheric mercury. The mean daytime mercury fluxes, during conditions of no precipitation, measured with field chambers were 50 to 360 ng m−2 h−1, and with the micrometeorological methods were 230 to 600 ng m−2 h−1. This wide range in mercury emission rates reflects differences in method experimental designs and local source strengths. Mercury fluxes measured by many field chambers were significantly different (p<0.05) but linearly correlated. This indicates that field chambers responded similarly to environmental conditions, but differences in experimental design and site heterogeneity had a significant influence on the magnitude of mercury fluxes. Data developed during the field study demonstrated that field flux chambers are ideal for assessment of the physicochemical processes driving mercury flux and development of an understanding of the magnitude of the influence of individual factors on flux. In general, mean mercury fluxes measured with micrometeorological methods during daytime periods were nearly 3 times higher than mean fluxes measured with field flux chambers. Micrometeorological methods allow for derivation of a representative mercury flux occurring from an unconstrained system and provide an assessment of the actual magnitude and variability of fluxes occurring from an area.
As part of an international Hg flux intercomparison at the Steamboat Springs, Nevada, geothermal area, several dynamic soil flux chambers and micrometeorological gradient systems were operated over desert soils in early September 1997. A series of unanticipated convective rain cells impacted the site with the first rainfall in ∼90 days, and the initial 4‐cm rainfall increased soil moisture from ∼0.01 to 0.06% (vol/vol). Several chambers were operating prior to the events, and two were deployed over wet soils following rainfall. Rainfall resulted in an immediate and steep rise in ambient air Hg concentrations and soil Hg emissions which persisted for 12–24 hours. Fluxes increased most quickly and to a greater degree over the wettest soils, and the rate of increase was related to chamber design and flushing rate. The flux response was also apparent in the micrometeorological data. In general, soil emissions increased by an order of magnitude following the rain, and reached levels ∼6 times above those at the same time the previous day. These fluxes were significantly correlated with temperature, radiation, humidity, wind speed, and soil moisture. After drying for ∼40 hours, selected soil plots were manually irrigated with low‐Hg‐distilled water. Mercury emissions responded similarly across the three treated sites, uniformly increasing from ∼60 ng m−2 h−1 pretreatment to ∼650 ng m−2 h−1 posttreatment, which was a factor of ∼6 higher than adjacent control soils. Possible causes of the increases in flux include soil gas displacement, desorption of Hg° by water molecules, and desorption of Hg(II) and subsequent reduction in solution. The kinetics of the flux response, combined with local soil and climatic conditions, suggest that Hg emissions were responding primarily to soil moisture and solar radiation. These data have interesting implications for the role of changing regional climates on biogeochemical cycling of Hg.
7 February 2013 in Atmospheric Chemistry and Physics
Global emissions of mercury continue to change at the same time as the Arctic is experiencing ongoing climatic changes. Continuous monitoring of atmospheric mercury provides important information about long-term trends in the balance between transport, chemistry, and deposition of this pollutant in the Arctic atmosphere. Ten-year records of total gaseous mercury (TGM) from 2000 to 2009 were analyzed from two high Arctic sites at Alert (Nunavut, Canada) and Zeppelin Station (Svalbard, Norway); one sub-Arctic site at Kuujjuarapik (Nunavik, Québec, Canada); and three temperate Canadian sites at St. Anicet (Québec), Kejimkujik (Nova Scotia) and Egbert (Ontario). Five of the six sites examined showed a decreasing trend over this time period. Overall trend estimates at high latitude sites were: −0.9% yr−1 (95% confidence limits: −1.4, 0) at Alert and no trend (−0.5, +0.7) at Zeppelin Station. Faster decreases were observed at the remainder of the sites: −2.1% yr−1 (−3.1, −1.1) at Kuujjuarapik, −1.9% yr−1 (−2.1, −1.8) at St. Anicet, −1.6% yr−1 (−2.4, −1.0) at Kejimkujik and −2.2% yr−1 (−2.8, −1.7) at Egbert. Trends at the sub-Arctic and mid-latitude sites agree with reported decreases in background TGM concentration since 1996 at Mace Head, Ireland, and Cape Point, South Africa, but conflict with estimates showing an increase in global anthropogenic emissions over a similar period. Trends in TGM at the two high Arctic sites were not only less negative (or neutral) overall but much more variable by season. Possible reasons for differences in seasonal and overall trends at the Arctic sites compared to those at lower latitudes are discussed, as well as implications for the Arctic mercury cycle. The first calculations of multi-year trends in reactive gaseous mercury (RGM) and total particulate mercury (TPM) at Alert were also performed, indicating increases from 2002 to 2009 in both RGM and TPM in the spring when concentrations are highest.
21 June 2000 in Environmental Science & Technology