Improved Mechanistic Model of the Atmospheric Redox Chemistry of Mercury

Research output: Journal Publications and Reviews (RGC: 21, 22, 62)21_Publication in refereed journalpeer-review

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Author(s)

  • Viral Shah
  • Daniel J. Jacob
  • Colin P. Thackray
  • Elsie M. Sunderland
  • Theodore S. Dibble
  • Alfonso Saiz-Lopez
  • Ivan Černušák
  • Vladimir Kellö
  • Pedro J. Castro
  • Rongrong Wu
  • Chuji Wang

Related Research Unit(s)

Detail(s)

Original languageEnglish
Number of pages12
Journal / PublicationEnvironmental Science & Technology
Online published17 Aug 2021
Publication statusOnline published - 17 Aug 2021

Link(s)

Abstract

We present a new chemical mechanism for Hg0/HgI/HgII atmospheric cycling, including recent laboratory and computational data, and implement it in the GEOS-Chem global atmospheric chemistry model for comparison to observations. Our mechanism includes the oxidation of Hg0 by Br and OH, subsequent oxidation of HgI by ozone and radicals, respeciation of HgII in aerosols and cloud droplets, and speciated HgII photolysis in the gas and aqueous phases. The tropospheric Hg lifetime against deposition in the model is 5.5 months, consistent with observational constraints. The model reproduces the observed global surface Hg0 concentrations and HgII wet deposition fluxes. Br and OH make comparable contributions to global net oxidation of Hg0 to HgII. Ozone is the principal HgI oxidant, enabling the efficient oxidation of Hg0 to HgII by OH. BrHgIIOH and HgII(OH)2, the initial HgII products of Hg0 oxidation, respeciate in aerosols and clouds to organic and inorganic complexes, and volatilize to photostable forms. Reduction of HgII to Hg0 takes place largely through photolysis of aqueous HgII–organic complexes. 71% of model HgII deposition is to the oceans. Major uncertainties for atmospheric Hg chemistry modeling include Br concentrations, stability and reactions of HgI, and speciation and photoreduction of HgII in aerosols and clouds.

Research Area(s)

  • mercury modeling, chemical mechanism, mercury oxidation, mercury photoreduction, atmospheric lifetime, mercury deposition

Citation Format(s)

Improved Mechanistic Model of the Atmospheric Redox Chemistry of Mercury. / Shah, Viral; Jacob, Daniel J.; Thackray, Colin P.; Wang, Xuan; Sunderland, Elsie M.; Dibble, Theodore S.; Saiz-Lopez, Alfonso; Černušák, Ivan; Kellö, Vladimir; Castro, Pedro J.; Wu, Rongrong; Wang, Chuji.

In: Environmental Science & Technology, 17.08.2021.

Research output: Journal Publications and Reviews (RGC: 21, 22, 62)21_Publication in refereed journalpeer-review