globalchange  > 气候变化与战略
DOI: 10.1073/pnas.1922486117
论文题名:
Photochemistry of oxidized Hg(I) and Hg(II) species suggests missing mercury oxidation in the troposphere
作者: Saiz-Lopez A.; Travnikov O.; Sonke J.E.; Thackray C.P.; Jacob D.J.; Carmona-García J.; Francés-Monerris A.; Roca-Sanjuán D.; Ulises Acuña A.; Dávalos J.Z.; Cuevas C.A.; Jiskra M.; Wang F.; Bieser J.; Plane J.M.C.; Francisco J.S.
刊名: Proceedings of the National Academy of Sciences of the United States of America
ISSN: 0027-8424
出版年: 2020
卷: 117, 期:49
起始页码: 30949
结束页码: 30956
语种: 英语
英文关键词: Atmospheric chemistry ; Atmospheric modeling ; Gas-phase mercury reactivity ; Mercury photoreduction ; Tropospheric chemistry
Scopus关键词: bromine ; mercury ; Article ; concentration (parameter) ; geography ; oxidation ; photochemistry ; photolysis ; priority journal ; simulation ; steady state ; troposphere ; wet deposition
英文摘要: Mercury (Hg), a global contaminant, is emitted mainly in its elemental form Hg0to the atmosphere where it is oxidized to reactive HgIIcompounds, which efficiently deposit to surface ecosystems. Therefore, the chemical cycling between the elemental and oxidized Hg forms in the atmosphere determines the scale and geographical pattern of global Hg deposition. Recent advances in the photochemistry of gas-phase oxidized HgIand HgIIspecies postulate their photodissociation back to Hg0as a crucial step in the atmospheric Hg redox cycle. However, the significance of these photodissociation mechanisms on atmospheric Hg chemistry, lifetime, and surface deposition remains uncertain. Here we implement a comprehensive and quantitative mechanism of the photochemical and thermal atmospheric reactions between Hg0, HgI, and HgIIspecies in a global model and evaluate the results against atmospheric Hg observations. We find that the photochemistry of HgIand HgIIleads to insufficient Hg oxidation globally. The combined efficient photoreduction of HgIand HgIIto Hg0competes with thermal oxidation of Hg0, resulting in a large model overestimation of 99% of measured Hg0and underestimation of 51% of oxidized Hg and ∼66% of HgIIwet deposition. This in turn leads to a significant increase in the calculated global atmospheric Hg lifetime of 20 mo, which is unrealistically longer than the 3-6-mo range based on observed atmospheric Hg variability. These results show that the HgIand HgIIphotoreduction processes largely offset the efficiency of bromine-initiated Hg0oxidation and reveal missing Hg oxidation processes in the troposphere. © 2020 National Academy of Sciences. All rights reserved.
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资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/163912
Appears in Collections:气候变化与战略

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作者单位: Saiz-Lopez, A., Department of Atmospheric Chemistry and Climate, Institute of Physical Chemistry Rocasolano, Spanish National Research Council (CSIC), Madrid, 28006, Spain; Travnikov, O., Meteorological Synthesizing Centre-East of EMEP, Moscow, 115419, Russian Federation; Sonke, J.E., Geosciences Environnement Toulouse, CNRS/Observatoire Midi-Pyrenees (OMP), Universite de Toulouse, Toulouse, 31400, France; Thackray, C.P., Harvard John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138, United States; Jacob, D.J., Harvard John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138, United States; Carmona-García, J., Institut de Ciencia Molecular, Universitat de Valencia, Valencia, 46071, Spain; Francés-Monerris, A., Departamento de Quimica Fisica, Universitat de Valencia, Valencia, 46100, Spain, Universite de Lorraine, CNRS, Laboratoire de Physique et Chimie Theoriques (LPCT), Nancy, F-54000, France; Roca-Sanjuán, D., Institut de Ciencia Molecular, Universitat de Valencia, Valencia, 46071, Spain; Ulises Acuña, A., Department of Atmospheric Chemistry and Climate, Institute of Physical Chemistry Rocasolano, Spanish National Research Council (CSIC), Madrid, 28006, Spain; Dávalos, J.Z., Department of Atmospheric Chemistry and Climate, Institute of Physical Chemistry Rocasolano, Spanish National Research Council (CSIC), Madrid, 28006, Spain; Cuevas, C.A., Department of Atmospheric Chemistry and Climate, Institute of Physical Chemistry Rocasolano, Spanish National Research Council (CSIC), Madrid, 28006, Spain; Jiskra, M., Geosciences Environnement Toulouse, CNRS/Observatoire Midi-Pyrenees (OMP), Universite de Toulouse, Toulouse, 31400, France, Department of Environmental Sciences, University of Basel, Basel, 4056, Switzerland; Wang, F., Department of Environment and Geography, Centre for Earth Observation Science, University of Manitoba, Winnipeg, MB R3T 2N2, Canada; Bieser, J., Helmholtz-Zentrum Geethacht, Institute of Coastal Research, Geesthacht, 21502, Germany; Plane, J.M.C., School of Chemistry, University of Leeds, Leeds, LS2 9TJ, United Kingdom; Francisco, J.S., Department of Earth and Environmental Science, University of Pennsylvania, Philadelphia, PA 19104, United States, Department of Chemistry, University of Pennsylvania, Philadelphia, PA 19104, United States

Recommended Citation:
Saiz-Lopez A.,Travnikov O.,Sonke J.E.,et al. Photochemistry of oxidized Hg(I) and Hg(II) species suggests missing mercury oxidation in the troposphere[J]. Proceedings of the National Academy of Sciences of the United States of America,2020-01-01,117(49)
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