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AGU: Geophysical Research Letters

 

Index Terms

  • Atmospheric Composition and Structure: Constituent sources and sinks
  • Atmospheric Composition and Structure: Geochemical cycles
  • Atmospheric Composition and Structure: Troposphere: composition and chemistry
  • Geochemistry: Major and trace element geochemistry
  • Geochemistry: Geochemical cycles

Abstract

GEOPHYSICAL RESEARCH LETTERS, VOL. 33, L20808, 5 PP., 2006
doi:10.1029/2006GL027176

Global lifetime of elemental mercury against oxidation by atomic bromine in the free troposphere

Christopher D. Holmes

Department of Earth and Planetary Sciences and Division of Engineering and Applied Sciences, Harvard University, Cambridge, Massachusetts, USA

Daniel J. Jacob

Department of Earth and Planetary Sciences and Division of Engineering and Applied Sciences, Harvard University, Cambridge, Massachusetts, USA

Xin Yang

Centre for Atmospheric Science, University of Cambridge, Cambridge, UK

We calculate the global mean atmospheric lifetime of elemental mercury (Hg0) against oxidation by atomic bromine (Br) in the troposphere by combining recent kinetic data for the Hg-Br system with modeled global concentrations of tropospheric Br. We obtain a lifetime of 0.5–1.7 years based on the range of kinetic data, implying that oxidation of Hg0 by Br is a major, and possibly dominant, global sink for Hg0. Most of the oxidation takes place in the middle and upper troposphere, where Br concentrations are high and where cold temperatures suppress thermal decomposition of the HgBr intermediate. This oxidation mechanism is consistent with mercury observations, including in particular high gaseous Hg(II) concentrations in Antarctic summer. Better free-tropospheric measurements of bromine radicals and further kinetic study of the Hg-Br system are essential to more accurately assess the global importance of Br as an oxidant of atmospheric Hg0.

Received 9 June 2006; accepted 31 August 2006; published 21 October 2006.

Citation: Holmes, C. D., D. J. Jacob, and X. Yang (2006), Global lifetime of elemental mercury against oxidation by atomic bromine in the free troposphere, Geophys. Res. Lett., 33, L20808, doi:10.1029/2006GL027176.

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