scholarly journals A 2-year record of atmospheric mercury species at a background Southern Hemisphere station on Amsterdam Island

2014 ◽  
Vol 14 (20) ◽  
pp. 11461-11473 ◽  
Author(s):  
H. Angot ◽  
M. Barret ◽  
O. Magand ◽  
M. Ramonet ◽  
A. Dommergue

Abstract. Although essential to fully understand the cycling of mercury at the global scale, mercury species records in the Southern Hemisphere are scarce. Under the framework of the Global Mercury Observation System (GMOS) project, a monitoring station has been set up on Amsterdam Island (37°48´ S, 77°34´ E) in the remote southern Indian Ocean. For the first time in the Southern Hemisphere, a 2-year record of gaseous elemental mercury (GEM), reactive gaseous mercury (RGM) and particle-bound mercury (PBM) is presented. GEM concentrations were remarkably steady (1.03 ± 0.08 ng m−3) while RGM and PBM concentrations were very low and exhibited a strong variability (mean: 0.34 pg m−3, range: < detection limit–4.07 pg m−3; and mean: 0.67 pg m−3, range: < detection limit–12.67 pg m−3, respectively). Despite the remoteness of the island, wind sector analysis, air mass back trajectories and the observation of radonic storms highlighted a long-range contribution from the southern African continent to the GEM and PBM budgets from July to September during the biomass burning season. Low concentrations of GEM were associated with southerly polar and marine air masses from the remote southern Indian Ocean. This unique data set provides new baseline GEM concentrations in the Southern Hemisphere midlatitudes while mercury speciation along with upcoming wet deposition data will help to improve our understanding of the mercury cycle in the marine boundary layer.

2014 ◽  
Vol 14 (10) ◽  
pp. 14439-14470
Author(s):  
H. Angot ◽  
M. Barret ◽  
O. Magand ◽  
M. Ramonet ◽  
A. Dommergue

Abstract. Scarcity of mercury species records in the Southern Hemisphere is a critical weak point for the development of appropriate modeling and regulation scenarios. Under the framework of the "Global Mercury Observation System" (GMOS) project, a monitoring station has been set up on Amsterdam Island (37°48' S, 77°34' E) in the remote southern Indian Ocean. For the first time in the Southern Hemisphere, a 2 year record of gaseous elemental mercury (GEM), reactive gaseous mercury (RGM) and particle-bound mercury (PBM) is presented. GEM concentrations were remarkably steady (1.03 ± 0.08 pg m−3) while RGM and PBM concentrations were very low and exhibited a strong variability (mean: 0.34 pg m−3 [range: 0.28–4.07 pg m−3] and mean: 0.67 pg m−3 [range: 0.28–12.67 pg m−3], respectively). Despite the remoteness of the island, wind sector analysis, air mass back trajectories and the observation of radonic storms highlighted a long-range contribution from the southern African continent to the GEM and PBM budgets in winter during the biomass burning season. Lowest concentrations of GEM were associated with southerly polar and marine air masses from the remote southern Indian Ocean. This unique dataset provides new baseline GEM concentrations in the Southern Hemisphere mid-latitudes for further modeling studies, while mercury speciation along with upcoming wet deposition data will help improving our understanding of mercury cycle in the marine boundary layer.


2010 ◽  
Vol 10 (8) ◽  
pp. 3985-3997 ◽  
Author(s):  
F. Sprovieri ◽  
I. M. Hedgecock ◽  
N. Pirrone

Abstract. Atmospheric mercury species concentrations were measured during two oceanographic cruise campaigns covering the Adriatic Sea, the first during the autumn in 2004 and the second in the summer of 2005. The inclement weather during the autumn campaign meant that no clear in-situ production of oxidised gas phase mercury was seen. Events where high values of HgII(g) and/or Hg associated with particulates (HgP) were observed, could be linked to probable anthropogenic emission source areas. During the summer campaign however, the by now rather familiar diurnal variation of HgII(g) concentration, with maxima around midday, was observed. Again there were events when high HgII(g) and particulates (HgP) concentrations were seen which did not fit with the pattern of daily in-situ HgII(g) production. These events were traceable, with the help of back trajectory calculations, to areas of anthropogenic emissions. The back trajectories for all the events during which high Hg species concentrations were encountered showed that the airmass being sampled had passed near port areas in the previous 24 h. Not all these ports are associated with major industrial installations, it is possible therefore (bearing in mind the uncertainty associated with the back trajectory calculations) that either shipping or port activities are a Hg source. Box modelling studies of the summer 2005 campaign show that although the in-situ production of HgII(g) occurs in the MBL, the exact chemical mechanism responsible is difficult to determine. However given the high O3 concentrations encountered during this campaign it seems clear that if Hg0 does react with O3, it does not produce gas phase HgII. Equally, the reaction between Hg0 and OH if it occurs, does not contribute appreciably to HgII(g) production.


2009 ◽  
Vol 6 (1) ◽  
pp. 70 ◽  
Author(s):  
Aurélie Colomb ◽  
Valérie Gros ◽  
Séverine Alvain ◽  
Roland Sarda-Esteve ◽  
Bernard Bonsang ◽  
...  

Environmental context. Oceans represent 70% of the blue planet, and surprisingly, ocean emission in term of volatile organic compounds is poorly understood. The potential climate impacts on a global scale of various trace organic gases have been established, and the terrestrial inputs are well studied, but little is known about which of these can be emitted from oceanic sources. In the present study, atmospheric samples were taken over the Southern Indian Ocean, while crossing some oceanic fronts and different phytoplankton species. Such a study should aid in understanding oceanic emission, especially from phytoplankton, and will help modellers to determine concentrations of organic traces in the remote marine troposphere. Abstract. Considering its size and potential importance, the ocean is poorly characterised in terms of volatile organic compounds (VOC) that play important roles in global atmospheric chemistry. In order to better understand their potential sources and sinks over the Southern Indian Austral Ocean, shipborne measurements of selected species were made during the MANCHOT campaign during December 2004, on board the research vessel Marion Dufresne. Along the transect La Réunion to Kerguelen Island, air measurements of selected VOC (including dimethylsulfide (DMS) isoprene, carbonyls and organohalogens), carbon monoxide and ozone were performed, crossing subtropical, temperate and sub-Antarctic waters as well as pronounced subtropical and sub-Antarctic oceanic fronts. The remote marine boundary layer was characterised at latitudes 45–50°S. Oceanic fronts were associated with enhanced chlorophyll and biological activity in the seawater and elevated DMS and organohalogens in the atmosphere. These were compared with a satellite-derived phytoplankton distribution (PHYSAT). Diurnal variation for isoprene, terpenes, acetone and acetaldehyde was observed, analogously to recent results observed in mesocosm experiments.


2016 ◽  
Vol 16 (3) ◽  
pp. 1511-1530 ◽  
Author(s):  
V. Shah ◽  
L. Jaeglé ◽  
L. E. Gratz ◽  
J. L. Ambrose ◽  
D. A. Jaffe ◽  
...  

Abstract. We collected mercury observations as part of the Nitrogen, Oxidants, Mercury, and Aerosol Distributions, Sources, and Sinks (NOMADSS) aircraft campaign over the southeastern US between 1 June and 15 July 2013. We use the GEOS-Chem chemical transport model to interpret these observations and place new constraints on bromine radical initiated mercury oxidation chemistry in the free troposphere. We find that the model reproduces the observed mean concentration of total atmospheric mercury (THg) (observations: 1.49 ± 0.16 ng m−3, model: 1.51 ± 0.08 ng m−3), as well as the vertical profile of THg. The majority (65 %) of observations of oxidized mercury (Hg(II)) were below the instrument's detection limit (detection limit per flight: 58–228 pg m−3), consistent with model-calculated Hg(II) concentrations of 0–196 pg m−3. However, for observations above the detection limit we find that modeled Hg(II) concentrations are a factor of 3 too low (observations: 212 ± 112 pg m−3, model: 67 ± 44 pg m−3). The highest Hg(II) concentrations, 300–680 pg m−3, were observed in dry (RH  <  35 %) and clean air masses during two flights over Texas at 5–7 km altitude and off the North Carolina coast at 1–3 km. The GEOS-Chem model, back trajectories and observed chemical tracers for these air masses indicate subsidence and transport from the upper and middle troposphere of the subtropical anticyclones, where fast oxidation of elemental mercury (Hg(0)) to Hg(II) and lack of Hg(II) removal lead to efficient accumulation of Hg(II). We hypothesize that the most likely explanation for the model bias is a systematic underestimate of the Hg(0) + Br reaction rate. We find that sensitivity simulations with tripled bromine radical concentrations or a faster oxidation rate constant for Hg(0) + Br, result in 1.5–2 times higher modeled Hg(II) concentrations and improved agreement with the observations. The modeled tropospheric lifetime of Hg(0) against oxidation to Hg(II) decreases from 5 months in the base simulation to 2.8–1.2 months in our sensitivity simulations. In order to maintain the modeled global burden of THg, we need to increase the in-cloud reduction of Hg(II), thus leading to faster chemical cycling between Hg(0) and Hg(II). Observations and model results for the NOMADSS campaign suggest that the subtropical anticyclones are significant global sources of Hg(II).


2016 ◽  
Vol 16 (13) ◽  
pp. 8249-8264 ◽  
Author(s):  
Hélène Angot ◽  
Olivier Magand ◽  
Detlev Helmig ◽  
Philippe Ricaud ◽  
Boris Quennehen ◽  
...  

Abstract. Under the framework of the GMOS project (Global Mercury Observation System) atmospheric mercury monitoring has been implemented at Concordia Station on the high-altitude Antarctic plateau (75°06′ S, 123°20′ E, 3220 m above sea level). We report here the first year-round measurements of gaseous elemental mercury (Hg(0)) in the atmosphere and in snowpack interstitial air on the East Antarctic ice sheet. This unique data set shows evidence of an intense oxidation of atmospheric Hg(0) in summer (24-hour daylight) due to the high oxidative capacity of the Antarctic plateau atmosphere in this period of the year. Summertime Hg(0) concentrations exhibited a pronounced daily cycle in ambient air with maximal concentrations around midday. Photochemical reactions and chemical exchange at the air–snow interface were prominent, highlighting the role of the snowpack on the atmospheric mercury cycle. Our observations reveal a 20 to 30 % decrease of atmospheric Hg(0) concentrations from May to mid-August (winter, 24 h darkness). This phenomenon has not been reported elsewhere and possibly results from the dry deposition of Hg(0) onto the snowpack. We also reveal the occurrence of multi-day to weeklong atmospheric Hg(0) depletion events in summer, not associated with depletions of ozone, and likely due to a stagnation of air masses above the plateau triggering an accumulation of oxidants within the shallow boundary layer. Our observations suggest that the inland atmospheric reservoir is depleted in Hg(0) in summer. Due to katabatic winds flowing out from the Antarctic plateau down the steep vertical drops along the coast and according to observations at coastal Antarctic stations, the striking reactivity observed on the plateau most likely influences the cycle of atmospheric mercury on a continental scale.


1975 ◽  
Vol 5 (2) ◽  
pp. 237-250 ◽  
Author(s):  
Douglas F. Williams ◽  
William C. Johnson

Planktonic foraminiferal assemblages have been examined in 25 trigger core top samples and 51 piston core top samples collected between latitudes 28° S and 55° S and longitudes 79° E and 120° E from the southern Indian Ocean during cruises of the U.S.N.S. Eltanin. Samples taken from water depths exceeding 4000 m and/or showing evidence of calcium carbonate dissolution were eliminated from further analysis. The final piston core data set consists of 34 samples; the trigger core data set containing 21 samples. A close relationship exists between changes in the planktonic foraminiferal assemblages in the surface sediments and surface water temperatures. Species diversity values were computed for each of the core top assemblages using the Shannon-Wiener Index and the Brillouin Index, each of which takes into consideration the number of species and the proportionment of individuals among the species. The Shannon and Brillouin diversity values for all samples are positively correlated (correlation coefficient (r) = +.999). Regression analysis of latitude versus Shannon diversity values in the trigger core samples clearly shows a decrease in diversity with increasing latitude (r = −.979). Furthermore, a strong correlation (r = +.977) exists between decreasing species diversity (Shannon) and decreasing average summer-winter temperature of the overlying surface waters. A paleotemperature equation derived from the relationship of diversity in trigger core samples and surface water temperature was used to generate paleotemperature curves for five trigger cores and a 6 m piston core of Late Pleistocene age, located beneath the present position of the Subtropical Convergence. A 7–8° C temperature range is suggested between the interglacial and glacial episodes in this Late Pleistocene sequence, and probably reflects latitudinal shifts of the Subtropical Convergence and Australasian Front during the Late Pleistocene.


2017 ◽  
Vol 17 (18) ◽  
pp. 11623-11636 ◽  
Author(s):  
Dean Howard ◽  
Peter F. Nelson ◽  
Grant C. Edwards ◽  
Anthony L. Morrison ◽  
Jenny A. Fisher ◽  
...  

Abstract. Mercury is a toxic element of serious concern for human and environmental health. Understanding its natural cycling in the environment is an important goal towards assessing its impacts and the effectiveness of mitigation strategies. Due to the unique chemical and physical properties of mercury, the atmosphere is the dominant transport pathway for this heavy metal, with the consequence that regions far removed from sources can be impacted. However, there exists a dearth of long-term monitoring of atmospheric mercury, particularly in the tropics and Southern Hemisphere. This paper presents the first 2 years of gaseous elemental mercury (GEM) measurements taken at the Australian Tropical Atmospheric Research Station (ATARS) in northern Australia, as part of the Global Mercury Observation System (GMOS). Annual mean GEM concentrations determined at ATARS (0.95 ± 0.12 ng m−3) are consistent with recent observations at other sites in the Southern Hemisphere. Comparison with GEM data from other Australian monitoring sites suggests a concentration gradient that decreases with increasing latitude. Seasonal analysis shows that GEM concentrations at ATARS are significantly lower in the distinct wet monsoon season than in the dry season. This result provides insight into alterations of natural mercury cycling processes as a result of changes in atmospheric humidity, oceanic/terrestrial fetch, and convective mixing, and invites future investigation using wet mercury deposition measurements. Due to its location relative to the atmospheric equator, ATARS intermittently samples air originating from the Northern Hemisphere, allowing an opportunity to gain greater understanding of inter-hemispheric transport of mercury and other atmospheric species. Diurnal cycles of GEM at ATARS show distinct nocturnal depletion events that are attributed to dry deposition under stable boundary layer conditions. These cycles provide strong further evidence supportive of a multi-hop model of GEM cycling, characterised by multiple surface depositions and re-emissions, in addition to long-range transport through the atmosphere.


2013 ◽  
Vol 13 (7) ◽  
pp. 20011-20048
Author(s):  
K. M. Wai ◽  
S. Wu

Abstract. Present-day and future impacts of biomass burning and other sources in the tropics and Southern Hemisphere are studied by global chemical transport model (GCTM), satellites retrievals and surface measurements. The spring CO peaks found at Mahe Island (Western Indian Ocean) are attributed to the burnings in India but not those from Northern Africa. Easter Island (Eastern Pacific Ocean) is impacted indirectly by the hemispheric zonal transport of CO due to the burnings in Southern Africa/Latin America, via the westerlies. An increasing trend for CO by 0.33 ppb yr-1 in the past decade at Ascension Island is attributed to the combined effects of Latin American/Southern Africa burnings and increase of CH4 level. Changes in water vapour and UV over Southern Atlantic Ocean (SAO) in future January have dominated effects on the O3 distribution. More than 55% of O3 concentrations over SAO in both present-day and future September are not directly affected by the emissions (including lightning) over the adjacent two continents but attributable to transport of O3 from outside due to CO and CH4 oxidation and stratospheric intrusion. High NOx emissions in both continents in future increase the PAN concentrations over remote oceans at higher southern latitudes (> 35° S) as far as those near Australia, affecting the O3 budget over there. Future changes of biomass burning and anthropogenic NOx emissions in Southern Africa lead to a new area of O3 maximum near South Africa. The resulted O3 outflow to the Indian Ocean is pronounced due to the effects of the persistent anti-cyclone. A general reduction of future OH radical concentrations is predicted over the remote marine boundary layer in the tropics and Southern Hemisphere, due to the increases in CH4 and CO emissions combined with the low-NOx environment.


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