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F. De Simone, P. Artaxo, M. Bencardino, S. Cinnirella, F. Carbone, F. D'Amore, A. Dommergue, X. B. Feng, C. N. Gencarelli, I. M. Hedgecock, M. S. Landis, F. Sprovieri, N. Suzuki, I. Wängberg, N. Pirrone |
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Title |
Particulate-phase mercury emissions from biomass burning and impact on resulting deposition: a modelling assessment |
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Journal |
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Year |
2017 |
Publication |
Atmos. chem. phys. |
Abbreviated Journal |
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Volume |
17 |
Issue |
3 |
Pages |
1881-1899 |
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Mercury (Hg) emissions from biomass burning (BB) are an important source of atmospheric Hg and a major factor driving the interannual variation of Hg concentrations in the troposphere. The greatest fraction of Hg from BB is released in the form of elemental Hg (Hg0(g)). However, little is known about the fraction of Hg bound to particulate matter (HgP) released from BB, and the factors controlling this fraction are also uncertain. In light of the aims of the Minamata Convention to reduce intentional Hg use and emissions from anthropogenic activities, the relative importance of Hg emissions from BB will have an increasing impact on Hg deposition fluxes. Hg speciation is one of the most important factors determining the redistribution of Hg in the atmosphere and the geographical distribution of Hg deposition. Using the latest version of the Global Fire Emissions Database (GFEDv4.1s) and the global Hg chemistry transport model, ECHMERIT, the impact of Hg speciation in BB emissions, and the factors which influence speciation, on Hg deposition have been investigated for the year 2013. The role of other uncertainties related to physical and chemical atmospheric processes involving Hg and the influence of model parametrisations were also investigated, since their interactions with Hg speciation are complex. The comparison with atmospheric HgP concentrations observed at two remote sites, Amsterdam Island (AMD) and Manaus (MAN), in the Amazon showed a significant improvement when considering a fraction of HgP from BB. The set of sensitivity runs also showed how the quantity and geographical distribution of HgP emitted from BB has a limited impact on a global scale, although the inclusion of increasing fractions HgP does limit Hg0(g) availability to the global atmospheric pool. This reduces the fraction of Hg from BB which deposits to the world's oceans from 71 to 62 %. The impact locally is, however, significant on northern boreal and tropical forests, where fires are frequent, uncontrolled and lead to notable Hg inputs to local ecosystems. In the light of ongoing climatic changes this effect could be potentially be exacerbated in the future. |
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1680-7324 |
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1680-7324 |
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6590 |
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H. Angot, O. Magand, D. Helmig, P. Ricaud, B. Quennehen, H. Gallée, M. Del Guasta, F. Sprovieri, N. Pirrone, J. Savarino, A. Dommergue |
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Title |
New insights into the atmospheric mercury cycling in central Antarctica and implications on a continental scale |
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Year |
2016 |
Publication |
Atmos. chem. phys. |
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Volume |
16 |
Issue |
13 |
Pages |
8249-8264 |
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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. |
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1680-7324 |
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1680-7324 |
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6591 |
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H. Angot, A. Dastoor, F. De Simone, K. Gårdfeldt, C. N. Gencarelli, I. M. Hedgecock, S. Langer, O. Magand, M. N. Mastromonaco, C. Nordstrøm, K. A. Pfaffhuber, N. Pirrone, A. Ryjkov, N. E. Selin, H. Skov, S. Song, F. Sprovieri, A. Steffen, K. Toyota, O. Travnikov, X. Yang, A. Dommergue |
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Title |
Chemical cycling and deposition of atmospheric mercury in polar regions: review of recent measurements and comparison with models |
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Year |
2016 |
Publication |
Atmos. chem. phys. |
Abbreviated Journal |
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Volume |
16 |
Issue |
16 |
Pages |
10735-10763 |
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Abstract |
Mercury (Hg) is a worldwide contaminant that can cause adverse health effects to wildlife and humans. While atmospheric modeling traces the link from emissions to deposition of Hg onto environmental surfaces, large uncertainties arise from our incomplete understanding of atmospheric processes (oxidation pathways, deposition, and re-emission). Atmospheric Hg reactivity is exacerbated in high latitudes and there is still much to be learned from polar regions in terms of atmospheric processes. This paper provides a synthesis of the atmospheric Hg monitoring data available in recent years (2011–2015) in the Arctic and in Antarctica along with a comparison of these observations with numerical simulations using four cutting-edge global models. The cycle of atmospheric Hg in the Arctic and in Antarctica presents both similarities and differences. Coastal sites in the two regions are both influenced by springtime atmospheric Hg depletion events and by summertime snowpack re-emission and oceanic evasion of Hg. The cycle of atmospheric Hg differs between the two regions primarily because of their different geography. While Arctic sites are significantly influenced by northern hemispheric Hg emissions especially in winter, coastal Antarctic sites are significantly influenced by the reactivity observed on the East Antarctic ice sheet due to katabatic winds. Based on the comparison of multi-model simulations with observations, this paper discusses whether the processes that affect atmospheric Hg seasonality and interannual variability are appropriately represented in the models and identifies research gaps in our understanding of the atmospheric Hg cycling in high latitudes. |
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1028 |
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1680-7324 |
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1680-7324 |
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yes |
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6592 |
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M. Nerentorp Mastromonaco, K. Gårdfeldt, B. Jourdain, K. Abrahamsson, A. Granfors, M. Ahnoff, A. Dommergue, G. Méjean, H. -W. Jacobi |
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Title |
Antarctic winter mercury and ozone depletion events over sea ice |
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Journal |
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Year |
2016 |
Publication |
Atmospheric environment |
Abbreviated Journal |
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Volume |
129 |
Issue |
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Pages |
125-132 |
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Keywords |
Antarctica Depletion event Mercury Ozone Sea ice |
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Abstract |
During atmospheric mercury and ozone depletion events in the springtime in polar regions gaseous elemental mercury and ozone undergo rapid declines. Mercury is quickly transformed into oxidation products, which are subsequently removed by deposition. Here we show that such events also occur during Antarctic winter over sea ice areas, leading to additional deposition of mercury. Over four months in the Weddell Sea we measured gaseous elemental, oxidized, and particulate-bound mercury, as well as ozone in the troposphere and total and elemental mercury concentrations in snow, demonstrating a series of depletion and deposition events between July and September. The winter depletions in July were characterized by stronger correlations between mercury and ozone and larger formation of particulate-bound mercury in air compared to later spring events. It appears that light at large solar zenith angles is sufficient to initiate the photolytic formation of halogen radicals. We also propose a dark mechanism that could explain observed events in air masses coming from dark regions. Br2 that could be the main actor in dark conditions was possibly formed in high concentrations in the marine boundary layer in the dark. These high concentrations may also have caused the formation of high concentrations of CHBr3 and CH2I2 in the top layers of the Antarctic sea ice observed during winter. These new findings show that the extent of depletion events is larger than previously believed and that winter depletions result in additional deposition of mercury that could be transferred to marine and terrestrial ecosystems. |
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1028 |
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ISSN |
1352-2310 |
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1352-2310 |
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6593 |
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H. Angot, I. Dion, N. Vogel, M. Legrand, O. Magand, A. Dommergue |
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Title |
Multi-year record of atmospheric mercury at Dumont d'Urville, East Antarctic coast: continental outflow and oceanic influences |
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Year |
2016 |
Publication |
Atmos. chem. phys. |
Abbreviated Journal |
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Volume |
16 |
Issue |
13 |
Pages |
8265-8279 |
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Abstract |
Under the framework of the Global Mercury Observation System (GMOS) project, a 3.5-year record of atmospheric gaseous elemental mercury (Hg(0)) has been gathered at Dumont d'Urville (DDU, 66°40′ S, 140°01′ E, 43 m above sea level) on the East Antarctic coast. Additionally, surface snow samples were collected in February 2009 during a traverse between Concordia Station located on the East Antarctic plateau and DDU. The record of atmospheric Hg(0) at DDU reveals particularities that are not seen at other coastal sites: a gradual decrease of concentrations over the course of winter, and a daily maximum concentration around midday in summer. Additionally, total mercury concentrations in surface snow samples were particularly elevated near DDU (up to 194.4 ng L−1) as compared to measurements at other coastal Antarctic sites. These differences can be explained by the more frequent arrival of inland air masses at DDU than at other coastal sites. This confirms the influence of processes observed on the Antarctic plateau on the cycle of atmospheric mercury at a continental scale, especially in areas subject to recurrent katabatic winds. DDU is also influenced by oceanic air masses and our data suggest that the ocean plays a dual role on Hg(0) concentrations. The open ocean may represent a source of atmospheric Hg(0) in summer whereas the sea-ice surface may provide reactive halogens in spring that can oxidize Hg(0). This paper also discusses implications for coastal Antarctic ecosystems and for the cycle of atmospheric mercury in high southern latitudes. |
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1028 |
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1680-7324 |
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1680-7324 |
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yes |
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Call Number |
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Serial |
6594 |
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Michelle G. Nerentorp Mastromonaco, Katarina Gårdfeldt, Sarka Langer, Aurélien Dommergue |
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Title |
Seasonal Study of Mercury Species in the Antarctic Sea Ice Environment |
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Journal |
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Year |
2016 |
Publication |
Environmental science & technology |
Abbreviated Journal |
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Volume |
50 |
Issue |
23 |
Pages |
12705-12712 |
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Abstract |
Limited studies have been conducted on mercury concentrations in the polar cryosphere and the factors affecting the distribution of mercury within sea ice and snow are poorly understood. Here we present the first comprehensive seasonal study of elemental and total mercury concentrations in the Antarctic sea ice environment covering data from measurements in air, sea ice, seawater, snow, frost flowers, and brine. The average concentration of total mercury in sea ice decreased from winter (9.7 ng L–1) to spring (4.7 ng L–1) while the average elemental mercury concentration increased from winter (0.07 ng L–1) to summer (0.105 ng L–1). The opposite trends suggest potential photo- or dark oxidation/reduction processes within the ice and an eventual loss of mercury via brine drainage or gas evasion of elemental mercury. Our results indicate a seasonal variation of mercury species in the polar sea ice environment probably due to varying factors such as solar radiation, temperature, brine volume, and atmospheric deposition. This study shows that the sea ice environment is a significant interphase between the polar ocean and the atmosphere and should be accounted for when studying how climate change may affect the mercury cycle in polar regions. |
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1028 |
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0013-936X |
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0013-936X |
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6595 |
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F. Sprovieri, N. Pirrone, M. Bencardino, F. D'Amore, F. Carbone, S. Cinnirella, V. Mannarino, M. Landis, R. Ebinghaus, A. Weigelt, E.-G. Brunke, C. Labuschagne, L. Martin, J. Munthe, I. Wängberg, P. Artaxo, F. Morais, H. D. M. J. Barbosa, J. Brito, W. Cairns, C. Barbante, M. D. C. Diéguez, P. E. Garcia, A. Dommergue, H. Angot, O. Magand, H. Skov, M. Horvat, J. Kotnik, K. A. Read, L. M. Neves, B. M. Gawlik, F. Sena, N. Mashyanov, V. Obolkin, D. Wip, X. B. Feng, H. Zhang, X. Fu, R. Ramachandran, D. Cossa, J. Knoery, N. Marusczak, M. Nerentorp, C. Norstrom |
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Title |
Atmospheric mercury concentrations observed at ground-based monitoring sites globally distributed in the framework of the GMOS network |
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Year |
2016 |
Publication |
Atmos. chem. phys. |
Abbreviated Journal |
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Volume |
16 |
Issue |
18 |
Pages |
11915-11935 |
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Abstract |
Long-term monitoring of data of ambient mercury (Hg) on a global scale to assess its emission, transport, atmospheric chemistry, and deposition processes is vital to understanding the impact of Hg pollution on the environment. The Global Mercury Observation System (GMOS) project was funded by the European Commission (http://www.gmos.eu) and started in November 2010 with the overall goal to develop a coordinated global observing system to monitor Hg on a global scale, including a large network of ground-based monitoring stations, ad hoc periodic oceanographic cruises and measurement flights in the lower and upper troposphere as well as in the lower stratosphere. To date, more than 40 ground-based monitoring sites constitute the global network covering many regions where little to no observational data were available before GMOS. This work presents atmospheric Hg concentrations recorded worldwide in the framework of the GMOS project (2010–2015), analyzing Hg measurement results in terms of temporal trends, seasonality and comparability within the network. Major findings highlighted in this paper include a clear gradient of Hg concentrations between the Northern and Southern hemispheres, confirming that the gradient observed is mostly driven by local and regional sources, which can be anthropogenic, natural or a combination of both. |
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1028 |
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1680-7324 |
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1680-7324 |
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yes |
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Serial |
6596 |
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F. Carbone, A. G. Bruno, A. Naccarato, F. De Simone, C. N. Gencarelli, F. Sprovieri, I. M. Hedgecock, M. S. Landis, H. Skov, K. A. Pfaffhuber, K. A. Read, L. Martin, H. Angot, A. Dommergue, O. Magand, N. Pirrone |
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Title |
The Superstatistical Nature and Interoccurrence Time of Atmospheric Mercury Concentration Fluctuations |
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Year |
2018 |
Publication |
Journal of Geophysical Research: Atmospheres |
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Volume |
123 |
Issue |
2 |
Pages |
764-774 |
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Keywords |
atmospheric turbulence interoccurrence times mercury superstatistics universal scaling |
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Abstract |
The probability density function (PDF) of the time intervals between subsequent extreme events in atmospheric Hg0 concentration data series from different latitudes has been investigated. The Hg0 dynamic possesses a long-term memory autocorrelation function. Above a fixed threshold Q in the data, the PDFs of the interoccurrence time of the Hg0 data are well described by a Tsallis q-exponential function. This PDF behavior has been explained in the framework of superstatistics, where the competition between multiple mesoscopic processes affects the macroscopic dynamics. An extensive parameter μ, encompassing all possible fluctuations related to mesoscopic phenomena, has been identified. It follows a χ2 distribution, indicative of the superstatistical nature of the overall process. Shuffling the data series destroys the long-term memory, the distributions become independent of Q, and the PDFs collapse on to the same exponential distribution. The possible central role of atmospheric turbulence on extreme events in the Hg0 data is highlighted. |
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1028 |
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ISSN |
2169-8996 |
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2169-8996 |
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yes |
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Serial |
7231 |
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Aurelien Dommergue, Pierre Amato, Romie Tignat-Perrier, Olivier Magand, Alban Thollot, Muriel Joly, Laetitia Bouvier, Karine Sellegri, Timothy Vogel, Jeroen E. Sonke, Jean-Luc Jaffrezo, Marcos Andrade, Isabel Moreno, Casper Labuschagne, Lynwill Martin, Qianggong Zhang, Catherine Larose |
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Title |
Methods to Investigate the Global Atmospheric Microbiome |
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Year |
2019 |
Publication |
Frontiers in Microbiology |
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Volume |
10 |
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Keywords |
aerobiology Aerosols Atmosphere Biodiversity biogeography methods microorganisms Protocols |
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Abstract |
The interplay between microbes and atmospheric physical and chemical conditions is an open field of research that can only be fully addressed using multidisciplinary approaches. The lack of coordinated efforts to gather data at representative temporal and spatial scales limits aerobiology to help understand large scale patterns of global microbial biodiversity and its causal relationships with the environmental context. This paper presents the sampling strategy and analytical protocols developed in order to integrate different fields of research such as microbiology, –omics biology, atmospheric chemistry, physics and meteorology to characterize atmospheric microbial life. These include control of chemical and microbial contaminations from sampling to analysis and identification of experimental procedures for characterizing airborne microbial biodiversity and its functioning from the atmospheric samples collected at remote sites from low cell density environments. We used high-volume sampling strategy to address both chemical and microbial composition of the atmosphere, because it can help overcome low aerosol and microbial cell concentrations. To account for contaminations, exposed and unexposed control filters were processed along with the samples. We present a method that allows for the extraction of chemical and biological data from the same quartz filters. We tested different sampling times, extraction kits and methods to optimize DNA yield from filters. Based on our results, we recommend supplementary sterilization steps to reduce filter contamination induced by handling and transport. These include manipulation under laminar flow hoods and UV sterilization. In terms of DNA extraction, we recommend a vortex step and a heating step to reduce binding to the quartz fibers of the filters. These steps have led to a 10-fold increase in DNA yield, allowing for downstream omics analysis of air samples. Based on our results, our method can be integrated into pre-existing long-term monitoring field protocols for the atmosphere both in terms of atmospheric chemistry and biology. We recommend using standardized air volumes and to develop standard operating protocols for field users to better control the operational quality. |
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1664-302X |
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yes |
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Call Number |
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Serial |
7847 |
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Zhiyong Xie, Zhen Wang, Olivier Magand, Alban Thollot, Ralf Ebinghaus, Wenying Mi, Aurelien Dommergue |
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Title |
Occurrence of legacy and emerging organic contaminants in snow at Dome C in the Antarctic |
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Year |
2020 |
Publication |
Science of The Total Environment |
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Volume |
741 |
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140200 |
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Antarctic Organophosphate esters PAH PFAS Snow |
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Concentrations of 9 organophosphate esters (OPEs), 16 perfluoroalkylated substances (PFASs) and 17 polycyclic aromatic hydrocarbons (PAHs) were investigated in surface snow samples collected at Dome C on the Antarctic Plateau in summer 2016. Tris(1-chloro-2-propyl) phosphate (TCPP), tris-(2-chloroethyl) phosphate (TCEP) and tri-n-butylphosphate (TnBP) were the dominant compounds of OPEs, with mean concentrations of 8157 ± 4860, 1128 ± 928 and 1232 ± 1147 pg/L. Perfluorooctanoic acid (PFOA, mean: 358 ± 71 pg/L) was the dominant compound of PFASs, and following by perfluoro-n-hexanoic acid (PFHxA, mean: 222 ± 97 pg/L), perfluoro-n-heptanoic acid (PFHpA, 183 ± 60 pg/L) and perfluoro-n-pentanoic acid (PFPeA, 175 ± 105 pg/L). 2-(Heptafluoropropoxy)propanoic acid (HFPO-DA, mean: 9.2 ± 2.6 pg/L) was determined in the Antarctic for the first time. Significantly positive correlations were observed between HFPO-DA and the short-chain PFASs, implying they have similar emission sources and long-range transport potential. High levels of 2-methylnaphthalene and 1-methylnaphthalene, as well as the ratios of PAH congeners indicated PAHs were attributable mostly to combustion origin. Occurrence and profiles of the indicators of OPEs, PFASs and PAHs, as well as air mass back-trajectory analysis provided direct evidences of human activities on Concordia station and posed obvious impacts on local environments in the Antarctic. Nevertheless, the exchange processes among different environmental matrices may drive the long-range transport and redistribution of the legacy and emerging Organic contaminants from coast to inland in the Antarctic. |
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1028 |
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0048-9697 |
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yes |
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7685 |
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