Air-soil exchange of mercury from background soils in the United States.

The air-surface exchange of mercury (Hg) was measured, using a dynamic polycarbonate flux chamber, for soils with low or "background" Hg concentrations (<0.1 mg/kg) at eleven locations across the contiguous United States. Sampling locations included agricultural, desert, grassland, mixed and pine forest ecosystems (n=1326 soil flux measurements at 46 individual sites). An overall soil Hg flux of 0.9+/-0.2 ng/m2/h for these background soils was obtained by averaging the means for the different locations. Soil Hg fluxes were significantly lower in dark conditions than in the light for all but the grassland sites. Mean inlet air Hg concentrations were 1.0+/-0.1 ng/m3 in the dark and 1.3+/-0.2 ng/m3 in the light. Soil temperature inside and outside of the chamber, air temperature, relative humidity, and irradiance were measured concurrently with soil Hg flux. Soil-air Hg exchange was weakly predicted by environmental variables (R2 from 0.07 to 0.52). For a single location, flux was better correlated with soil moisture than other measured environmental parameters, suggesting that soil moisture might be an important driver for Hg emissions from background soils. In addition, based on data collected we suggest some quality control measures for use of Tekran 2537A analyzers when measuring low mercury fluxes. Using basic scaling procedures, we roughly estimate that natural emissions from soils in the contiguous U.S. release approximately 100 Mg/yr of Hg to the atmosphere.

Application of controlled mesocosms for understanding mercury air-soil-plant exchange.

Whole system elemental mercury (Hg0) flux was measured for approximately 1.5 years using two large gas exchange mesocosms containing approximately 100 two-year old aspen trees (Populus tremuloides) planted in soil with elevated mercury concentrations (12.3 microg/g). We hypothesized that during leafout, whole mesocosm Hg0 flux would increase due to movement of Hg0 in the transpiration stream from the soil to the air. This hypothesis was not supported; plants were found to assimilate Hg0 from the contaminated air, and whole system Hg0 emissions were reduced as plants leafed-out due to shading of the soil. Surface disturbance, watering, and increases in soil moisture, light, and temperature were all found to increase whole system Hg0 flux, with light being a more significant factor. Although surface soils were maintained at 15-20% moisture, daily watering caused pulses of Hg0 to be released from the soil throughout the experiment. Data developed in this experiment suggested that those processes acting on the soil surface are the primary influence on Hg emissions and that the presence of vegetation, which shields soil surfaces from incident light, reduces Hg emissions from enriched soils.

Foliar exchange of mercury as a function of soil and air mercury concentrations.

Previous research has indicated that foliar mercury (Hg) flux is bi-directional, with influence from both atmospheric and soil Hg. This work investigated the role of soil and air Hg concentrations on foliar Hg exchange using a single-plant gas-exchange system. The exchange of Hg vapor with aspen seedlings grown in soil Hg concentrations of 0.03+/-0.01, 5.8+/-0.5, and 12.3+/-1.3 microg g(-1) and exposed to atmospheric Hg concentrations of 2.4+/-0.5, 11.0+/-0.9, and 30.4+/-2.2 ng m(-3) was measured. At background atmospheric Hg concentrations of 2.4 ng m(-3), foliage released Hg at all three soil Hg concentrations and fluxes ranged from 1.6 to 5.5 ng/m(2)/h. At higher atmospheric Hg concentrations (>11 ng m(-3)), net deposition to foliage ranged from -9 to -47 ng/m(2)/h, exhibiting increase uptake with higher air Hg concentrations. Fluxes associated with aspen showed an immediate response to changes in atmospheric Hg concentrations. Compensation points, the air concentration where no net flux of Hg vapor occurred, were 3-4 ng m(-3) in the light and 2-3 ng m(-3) in the dark for trees grown in soils of 0.03 and 6 microg g(-1) Hg content, and 5-6 ng m(-3) in the light and 2.5-3.5 ng m(-3) in the dark for trees grown in 12 microg g(-1) Hg soils.

Response to louis Henry.

Abstract We have responded to Monsieur Henry's comments in the order in which he presents them.