Atmospheric mercury speciation dynamics at the high-altitude Pic du Midi Observatory, southern France

Continuous measurements of atmospheric gaseous elemental mercury (GEM), particulate bound mercury (PBM) and gaseous oxidized mercury (GOM) at the high-altitude Pic du Midi Observatory (PDM Observatory, 2877 m a.s.l.) in southern France were made from November 2011 to November 2012. The mean GEM,...

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Main Authors: X. Fu, N. Marusczak, L.-E. Heimbürger, B. Sauvage, F. Gheusi, E. M. Prestbo, J. E. Sonke
Format: Article
Language:English
Published: Copernicus Publications 2016-05-01
Series:Atmospheric Chemistry and Physics
Online Access:https://www.atmos-chem-phys.net/16/5623/2016/acp-16-5623-2016.pdf
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author X. Fu
X. Fu
N. Marusczak
L.-E. Heimbürger
L.-E. Heimbürger
B. Sauvage
F. Gheusi
E. M. Prestbo
J. E. Sonke
author_facet X. Fu
X. Fu
N. Marusczak
L.-E. Heimbürger
L.-E. Heimbürger
B. Sauvage
F. Gheusi
E. M. Prestbo
J. E. Sonke
author_sort X. Fu
collection DOAJ
description Continuous measurements of atmospheric gaseous elemental mercury (GEM), particulate bound mercury (PBM) and gaseous oxidized mercury (GOM) at the high-altitude Pic du Midi Observatory (PDM Observatory, 2877 m a.s.l.) in southern France were made from November 2011 to November 2012. The mean GEM, PBM and GOM concentrations were 1.86 ng m<sup>−3</sup>, 14 pg m<sup>−3</sup> and 27 pg m<sup>−3</sup>, respectively and we observed 44 high PBM (peak PBM values of 33–98 pg m<sup>−3</sup>) and 61 high GOM (peak GOM values of 91–295 pg m<sup>−3</sup>) events. The high PBM events occurred mainly in cold seasons (winter and spring) whereas high GOM events were mainly observed in the warm seasons (summer and autumn). In cold seasons the maximum air mass residence times (ARTs) associated with high PBM events were observed in the upper troposphere over North America. The ratios of high PBM ARTs to total ARTs over North America, Europe, the Arctic region and Atlantic Ocean were all elevated in the cold season compared to the warm season, indicating that the middle and upper free troposphere of the Northern Hemisphere may be more enriched in PBM in cold seasons. PBM concentrations and PBM ∕ GOM ratios during the high PBM events were significantly anti-correlated with atmospheric aerosol concentrations, air temperature and solar radiation, suggesting in situ formation of PBM in the middle and upper troposphere. We identified two distinct types of high GOM events with the GOM concentrations positively and negatively correlated with atmospheric ozone concentrations, respectively. High GOM events positively correlated with ozone were mainly related to air masses from the upper troposphere over the Arctic region and middle troposphere over the temperate North Atlantic Ocean, whereas high GOM events anti-correlated with ozone were mainly related to air masses from the lower free troposphere over the subtropical North Atlantic Ocean. The ARTs analysis demonstrates that the lower and middle free troposphere over the North Atlantic Ocean was the largest source region of atmospheric GOM at the PDM Observatory. The ratios of high GOM ARTs to total ARTs over the subtropical North Atlantic Ocean in summer were significantly higher than those over the temperate and sub-arctic North Atlantic Ocean as well as that over the North Atlantic Ocean in other seasons, indicating abundant in situ oxidation of GEM to GOM in the lower free troposphere over the subtropical North Atlantic Ocean in summer.
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spelling doaj.art-a9ebe6957b664858bed298140dcc701b2022-12-22T03:48:02ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242016-05-01165623563910.5194/acp-16-5623-2016Atmospheric mercury speciation dynamics at the high-altitude Pic du Midi Observatory, southern FranceX. Fu0X. Fu1N. Marusczak2L.-E. Heimbürger3L.-E. Heimbürger4B. Sauvage5F. Gheusi6E. M. Prestbo7J. E. Sonke8Observatoire Midi-Pyrénées, Laboratoire Géosciences Environnement Toulouse, CNRS/IRD/Université de Toulouse, 14, Avenue Édouard Belin, 31400 Toulouse, FranceState Key Laboratory of Environmental Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, 46 Guanshui Road, 550002 Guiyang, ChinaObservatoire Midi-Pyrénées, Laboratoire Géosciences Environnement Toulouse, CNRS/IRD/Université de Toulouse, 14, Avenue Édouard Belin, 31400 Toulouse, FranceObservatoire Midi-Pyrénées, Laboratoire Géosciences Environnement Toulouse, CNRS/IRD/Université de Toulouse, 14, Avenue Édouard Belin, 31400 Toulouse, FranceMediterranean Institute of Oceanography, Campus de Luminy,13288 Marseille, FranceObservatoire Midi-Pyrénées, Laboratoire d'Aérologie, CNRS/IRD/Université de Toulouse, 14, Avenue Édouard Belin, 31400 Toulouse, FranceObservatoire Midi-Pyrénées, Laboratoire d'Aérologie, CNRS/IRD/Université de Toulouse, 14, Avenue Édouard Belin, 31400 Toulouse, FranceTekran Research and Development, 330 Nantucket Blvd., Toronto, ON, M1P2P4, CanadaObservatoire Midi-Pyrénées, Laboratoire Géosciences Environnement Toulouse, CNRS/IRD/Université de Toulouse, 14, Avenue Édouard Belin, 31400 Toulouse, FranceContinuous measurements of atmospheric gaseous elemental mercury (GEM), particulate bound mercury (PBM) and gaseous oxidized mercury (GOM) at the high-altitude Pic du Midi Observatory (PDM Observatory, 2877 m a.s.l.) in southern France were made from November 2011 to November 2012. The mean GEM, PBM and GOM concentrations were 1.86 ng m<sup>−3</sup>, 14 pg m<sup>−3</sup> and 27 pg m<sup>−3</sup>, respectively and we observed 44 high PBM (peak PBM values of 33–98 pg m<sup>−3</sup>) and 61 high GOM (peak GOM values of 91–295 pg m<sup>−3</sup>) events. The high PBM events occurred mainly in cold seasons (winter and spring) whereas high GOM events were mainly observed in the warm seasons (summer and autumn). In cold seasons the maximum air mass residence times (ARTs) associated with high PBM events were observed in the upper troposphere over North America. The ratios of high PBM ARTs to total ARTs over North America, Europe, the Arctic region and Atlantic Ocean were all elevated in the cold season compared to the warm season, indicating that the middle and upper free troposphere of the Northern Hemisphere may be more enriched in PBM in cold seasons. PBM concentrations and PBM ∕ GOM ratios during the high PBM events were significantly anti-correlated with atmospheric aerosol concentrations, air temperature and solar radiation, suggesting in situ formation of PBM in the middle and upper troposphere. We identified two distinct types of high GOM events with the GOM concentrations positively and negatively correlated with atmospheric ozone concentrations, respectively. High GOM events positively correlated with ozone were mainly related to air masses from the upper troposphere over the Arctic region and middle troposphere over the temperate North Atlantic Ocean, whereas high GOM events anti-correlated with ozone were mainly related to air masses from the lower free troposphere over the subtropical North Atlantic Ocean. The ARTs analysis demonstrates that the lower and middle free troposphere over the North Atlantic Ocean was the largest source region of atmospheric GOM at the PDM Observatory. The ratios of high GOM ARTs to total ARTs over the subtropical North Atlantic Ocean in summer were significantly higher than those over the temperate and sub-arctic North Atlantic Ocean as well as that over the North Atlantic Ocean in other seasons, indicating abundant in situ oxidation of GEM to GOM in the lower free troposphere over the subtropical North Atlantic Ocean in summer.https://www.atmos-chem-phys.net/16/5623/2016/acp-16-5623-2016.pdf
spellingShingle X. Fu
X. Fu
N. Marusczak
L.-E. Heimbürger
L.-E. Heimbürger
B. Sauvage
F. Gheusi
E. M. Prestbo
J. E. Sonke
Atmospheric mercury speciation dynamics at the high-altitude Pic du Midi Observatory, southern France
Atmospheric Chemistry and Physics
title Atmospheric mercury speciation dynamics at the high-altitude Pic du Midi Observatory, southern France
title_full Atmospheric mercury speciation dynamics at the high-altitude Pic du Midi Observatory, southern France
title_fullStr Atmospheric mercury speciation dynamics at the high-altitude Pic du Midi Observatory, southern France
title_full_unstemmed Atmospheric mercury speciation dynamics at the high-altitude Pic du Midi Observatory, southern France
title_short Atmospheric mercury speciation dynamics at the high-altitude Pic du Midi Observatory, southern France
title_sort atmospheric mercury speciation dynamics at the high altitude pic du midi observatory southern france
url https://www.atmos-chem-phys.net/16/5623/2016/acp-16-5623-2016.pdf
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