Photoreduction of gaseous oxidized mercury changes global atmospheric mercury speciation, transport and deposition

Saiz-Lopez, Alfonso; Sitkiewicz, Sebastian P.; Roca-Sanjuán, Daniel; Oliva-Enrich, Josep M.; Dávalos, Juan Z.; Notario, Rafael; Jiskra, Martin; Xu, Yang; Wang, Feiyue; Thackray, Colin P.; Sunderland, Elsie M.; Jacob, Daniel J.; Travnikov, Oleg; Cuevas, Carlos A.; Acuña, A. Ulises; Rivero, Daniel; Plane, John M.  C.; Kinnison, Douglas E.; Sonke, Jeroen E.

doi:10.1038/s41467-018-07075-3

Photoreduction of gaseous oxidized mercury changes global atmospheric mercury speciation, transport and deposition

Journal Article · Thu Nov 15 00:00:00 EST 2018 · Nature Communications

DOI:https://doi.org/10.1038/s41467-018-07075-3· OSTI ID:1624123

^[1]; Sitkiewicz, Sebastian P. ^[2]; Roca-Sanjuán, Daniel ^[3]; Oliva-Enrich, Josep M. ^[4]; Dávalos, Juan Z. ^[4]; Notario, Rafael ^[4]; ^[5]; Xu, Yang ^[5]; ^[6]; ^[7]; Sunderland, Elsie M. ^[7]; Jacob, Daniel J. ^[7]; Travnikov, Oleg ^[8]; Cuevas, Carlos A. ^[4]; Acuña, A. Ulises ^[4]; Rivero, Daniel ^[4]; Plane, John M. C. ^[9]; Kinnison, Douglas E. ^[10]; Sonke, Jeroen E. ^[5]

Consejo Superior de Investigaciones Cientificas (CSIC), Madrid (Spain). Inst. of Physical Chemistry Rocasolano. Dept. of Atmospheric Chemistry and Climate; DOE/OSTI
Euskal Herriko Unibertsitatea, Donostia (Spain). Kimika Fakultatea. Donostia International Physics Center (DIPC); Univ. of Valencia (Spain). Inst. de Ciencia Molecular
Univ. of Valencia (Spain). Inst. de Ciencia Molecular
Consejo Superior de Investigaciones Cientificas (CSIC), Madrid (Spain). Inst. of Physical Chemistry Rocasolano. Dept. of Atmospheric Chemistry and Climate
Univ. de Toulouse (France). Geosciences Environment Toulouse
Univ. of Manitoba, Winnepeg, MB (Canada). Centre for Earth Observation Science. Dept. of Environment and Geography
Harvard Univ., Cambridge, MA (United States). Harvard John A. Paulson School of Engineering and Applied Sciences
Meteorological Synthesizing Centre, Moscow (Russia)
Univ. of Leeds, Leeds (United Kingdom). School of Chemistry
National Center for Atmospheric Research, Boulder, CO (United States). Atmospheric Chemistry Observations and Modelling

Anthropogenic mercury (Hg(0)) emissions oxidize to gaseous Hg(II) compounds, before deposition to Earth surface ecosystems. Atmospheric reduction of Hg(II) competes with deposition, thereby modifying the magnitude and pattern of Hg deposition. Global Hg models have postulated that Hg(II) reduction in the atmosphere occurs through aqueous-phase photoreduction that may take place in clouds. Here we report that experimental rainfall Hg(II) photoreduction rates are much slower than modelled rates. We compute absorption cross sections of Hg(II) compounds and show that fast gas-phase Hg(II) photolysis can dominate atmospheric mercury reduction and lead to a substantial increase in the modelled, global atmospheric Hg lifetime by a factor two. Models with Hg(II) photolysis show enhanced Hg (0) deposition to land, which may prolong recovery of aquatic ecosystems long after Hg emissions are lowered, due to the longer residence time of Hg in soils compared with the ocean. Fast Hg(II) photolysis substantially changes atmospheric Hg dynamics and requires further assessment at regional and local scales.

View Accepted Manuscript (DOE)

Research Organization:: Harvard Univ., Cambridge, MA (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: SC0010687

OSTI ID:: 1624123

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 9; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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