Effect of temperature and air movement on the flux of elemental mercury from substrate to the atmosphere

The flux of elemental mercury vapor from intact mill tailings (36 to 1270 μg Hg/g), soil (7 μg Hg/g), and cinnabar ore (934 μg Hg/g) was measured as a function of temperature (20°–60°C) and wind velocity (0.2–0.8 m/s) using a controlled environment, open gas-exchange system. Continuous air movement over core surfaces in the gas-exchange chamber resulted in a logarithmic decline in mercury flux with time. Measurement of the effect of environmental parameters on mercury flux was done after attainment of a quasi steady state of flux. Prior to attainment of this state the activation energy for mercury flux was less than the molar heat of vaporization of element mercury (14 kcal/mol). At steady state the substrate-to-air flux of mercury vapor increased logarithmically with temperature, mimicking the element's vapor pressure curve; and activation energies (16.4 to 25.7 kcal/mol) for mercury flux were higher than the molar heat of vaporization of elemental mercury due to physicochemical properties of the soil (e.g., porosity, organic matter, clay content) that affect gas-phase mercury transport and fate. A change in wind velocity from 0.2 to 0.8 m/s resulted in an increase in mercury flux by a factor of 2 for a core with >150 μg Hg/g and no significant response from two cores with <150 μg Hg/g. Using data from gas-exchange experiments, equations were derived for predicting the response of mercury flux to a range of temperatures and wind velocities for a variety of substrate mercury concentrations. The equations and the results of this study are used to predict the flux of mercury to the atmosphere from substrate enriched in mercury.

[1]  N. J. Rosenberg,et al.  Microclimate: The Biological Environment. , 1976 .

[2]  Lars Håkanson,et al.  Mercury in the Swedish environment — Recent research on causes, consequences and corrective methods , 1991 .

[3]  R. Mason,et al.  Cycling of volatile mercury in temperate lakes , 1991 .

[4]  S. Lindberg,et al.  Design and initial tests of a dynamic enclosure chamber for measurements of vapor-phase mercury fluxes over soils , 1995 .

[5]  P. Liss Processes of gas exchange across an air-water interface☆ , 1973 .

[6]  Jerry R. Miller,et al.  Mercury mobility at the Carson River Superfund Site, west-central Nevada, USA: Interpretation of mercury speciation data in mill tailings, soils, and sediments , 1997 .

[7]  William F. Fitzgerald,et al.  The biogeochemical cycling of elemental mercury: Anthropogenic influences☆ , 1994 .

[8]  B. Kimball,et al.  Air Turbulence Effects upon Soil Gas Exchange1 , 1971 .

[9]  William F. Fitzgerald,et al.  Is mercury increasing in the atmosphere? The need for an atmospheric mercury network (AMNET) , 1995 .

[10]  T. Meyers,et al.  Micrometeorological gradient approach for quantifying air/surface exchange of mercury vapor: tests over contaminated soils. , 1995, Environmental science & technology.

[11]  R. Turner,et al.  Mercury emissions from chlorine-production solid waste deposits , 1977, Nature.

[12]  P. Hanson,et al.  NO2 deposition to elements representative of a forest landscape , 1989 .

[13]  M. Gustin,et al.  Atmospheric mercury concentrations above mercury contaminated mill tailings in the Carson River Drainage Basin, NV , 1995 .

[14]  J. Benoit,et al.  Mercury cycling and effects in freshwater wetland ecosystems , 1993 .

[15]  S. McLaughlin,et al.  The flux of sulfur-containing gases to vegetation , 1983 .

[16]  S. Siegel,et al.  Temperature determinants of plant-soil-air mercury relationships , 1988, Water, Air, and Soil Pollution.

[17]  Ki‐Hyun Kim,et al.  High-precision measurements of mercury vapor in air : design of a six-port-manifold mass flow controller system and evaluation of mass flow errors at atmospheric pressure , 1994 .

[18]  O. Lindqvist,et al.  Vertical fluxes of volatile mercury over forest soil and lake surfaces in Sweden: VERTICAL FLUXES OF VOLATILE MERCURY , 1991 .

[19]  Jerry R. Miller,et al.  Dispersal of mercury-contaminated sediments by geomorphic processes, sixmile canyon, Nevada, USA: Implications to site characterization and remediation of fluvial environments , 1996 .

[20]  T. Meyers,et al.  Micrometeorological measurements of mercury vapor fluxes over background forest soils in eastern Tennessee , 1995 .

[21]  O. Lindqvist,et al.  Cycling of mercury between water, air, and soil compartments of the environment , 1989 .

[22]  Ki‐Hyun Kim,et al.  Foliar exchange of mercury vapor: Evidence for a compensation point , 1995 .

[23]  N. Bloom,et al.  Determination of volatile mercury species at the picogram level by low-temperature gas chromatography with cold-vapour atomic fluorescence detection , 1988 .

[24]  O. Lindqvist,et al.  Vertical fluxes of volatile mercury over forest soil and lake surfaces in Sweden , 1991 .

[25]  E. Landa The retention of metallic mercury vapor by soils , 1978 .

[26]  Evaluation of volatilization of hazardous constituents at hazardous-waste land-treatment sites. Final report , 1986 .

[27]  P. Liss,et al.  Flux of Gases across the Air-Sea Interface , 1974, Nature.

[28]  D. R. Jackson,et al.  Atmospheric Emission and Plant Uptake of Mercury from Agricultural Soils near the Almadén Mercury Mine , 1979 .

[29]  R. R. Turner,et al.  Atmosphere-surface exchange of mercury in a forest: Results of modeling and gradient approaches , 1992 .

[30]  J. Hoste,et al.  The accuracy of the vapour-injection calibration method for the determination of mercury by amalgamation/cold-vapour atomic absorption spectrometry , 1985 .

[31]  S. Fang Sorption and transformation of mercury vapor by dry soil , 1978 .

[32]  R. Keislar,et al.  Atmospheric Mercury Concentrations Associated with Geologically and Anthropogenically Enriched Sites in Central Western Nevada , 1996 .

[33]  E. Greacen,et al.  VAPOR TRANSFER IN SOIL DUE TO AIR TURBULENCE , 1966 .

[34]  R. Klusman,et al.  Environmental influences upon mercury, radon and helium concentrations in soil gases at a site near Denver, Colorado , 1987 .

[35]  G. Taylor,et al.  High levels of mercury contamination in multiple media of the Carson River drainage basin of Nevada: implications for risk assessment. , 1994, Environmental health perspectives.