Abstract

Abstract. There exists observational evidence that gaseous elemental mercury (GEM) can be readily removed from the atmosphere via chemical oxidation followed by deposition in the polar and sub-polar regions, free troposphere, lower stratosphere, and marine boundary layer under specific environmental conditions. Here we report GEM depletions in a temperate mixed forest at Mt. Changbai, Northeast China. The strong depletions occurred predominantly at night during the leaf-growing season and in the absence of gaseous oxidized mercury (GOM) enrichment (GOM < 3 pg m−3). Vertical gradients of decreasing GEM concentrations from layers above to under forest canopy suggest in situ loss of GEM to forest canopy at Mt. Changbai. Foliar GEM flux measurements showed that the foliage of two predominant tree species is a net sink of GEM at night, with a mean flux of −1.8 ± 0.3 ng m2 h−1 over Fraxinus mandshurica (deciduous tree species) and −0.1 ± 0.2 ng m2 h−1 over Pinus Koraiensis (evergreen tree species). Daily integrated GEM δ202Hg, Δ199Hg, and Δ200Hg at Mt. Changbai during 8–18 July 2013 ranged from −0.34 to 0.91 ‰, from −0.11 to −0.04 ‰ and from −0.06 to 0.01 ‰, respectively. A large positive shift in GEM δ202Hg occurred during the strong GEM depletion events, whereas Δ199Hg and Δ200Hg remained essentially unchanged. The observational findings and box model results show that uptake of GEM by forest canopy plays a predominant role in the GEM depletion at Mt. Changbai forest. Such depletion events of GEM are likely to be a widespread phenomenon, suggesting that the forest ecosystem represents one of the largest sinks ( ∼ 1930 Mg) of atmospheric Hg on a global scale.

Highlights

  • Mercury (Hg) is a persistent toxic air pollutant that is ubiquitously distributed in the atmosphere

  • The sum of gaseous elemental mercury (GEM) and gaseous oxidized mercury (GOM) is known as total gaseous mercury (TGM)

  • The discovery of atmospheric mercury depletion events (AMDEs) in polar and sub-polar regions demonstrated that atmospheric GEM can be readily removed from the atmosphere via reactive

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Summary

Introduction

Mercury (Hg) is a persistent toxic air pollutant that is ubiquitously distributed in the atmosphere. The lower GEM concentrations observed in the leafgrowing season at many forest sites across the Atmospheric Mercury Network (AMNet) in USA (Lan et al, 2012) suggest forest to be a net GEM sink. It is still unclear whether the loss of GEM over forest is caused by direct dry deposition to canopy or chemical conversions of GEM to GOM (Mao et al, 2008). Atmospheric Hg speciation, vertical gradient of GEM, foliage–air and soil–air exchange flux of GEM and isotope signatures of GEM samples have been observed in an intensive campaign to explore the possible mechanisms responsible for the observed GEM depletion

Site description
Atmospheric Hg measurements
Foliar GEM exchange
Isotopic composition of atmospheric GEM
Results and discussion
Foliage–air exchange flux of GEM
Mechanisms for the observed GEM depletion
Conclusions and implications for the global atmospheric Hg cycling
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