| 1. |
- Song, S., et al.
(författare)
-
Top-down constraints on atmospheric mercury emissions and implications for global biogeochemical cycling
- 2015
-
Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 15:12, s. 7103-7125
-
Tidskriftsartikel (refereegranskat)abstract
- We perform global-scale inverse modeling to constrain present-day atmospheric mercury emissions and relevant physiochemical parameters in the GEOS-Chem chemical transport model. We use Bayesian inversion methods combining simulations with GEOS-Chem and ground-based Hg-0 observations from regional monitoring networks and individual sites in recent years. Using optimized emissions/parameters, GEOS-Chem better reproduces these ground-based observations and also matches regional over-water Hg-0 and wet deposition measurements. The optimized global mercury emission to the atmosphere is 5.8 Gg yr(-1). The ocean accounts for 3.2 Gg yr(-1) (55 % of the total), and the terrestrial ecosystem is neither a net source nor a net sink of Hg-0. The optimized Asian anthropogenic emission of Hg-0 (gas elemental mercury) is 650-1770 Mg yr(-1), higher than its bottom-up estimates (550-800 Mg yr(-1)). The ocean parameter inversions suggest that dark oxidation of aqueous elemental mercury is faster, and less mercury is removed from the mixed layer through particle sinking, when compared with current simulations. Parameter changes affect the simulated global ocean mercury budget, particularly mass exchange between the mixed layer and subsurface waters. Based on our inversion results, we re-evaluate the long-term global biogeochemical cycle of mercury, and show that legacy mercury becomes more likely to reside in the terrestrial ecosystem than in the ocean. We estimate that primary anthropogenic mercury contributes up to 23 % of present-day atmospheric deposition.
|
|
| 2. |
- Brenninkmeijer, C. A. M., et al.
(författare)
-
Civil Aircraft for the regular investigation of the atmosphere based on an instrumented container: The new CARIBIC system
- 2007
-
Ingår i: Atmospheric Chemistry and Physics. - 1680-7324. ; 7:18, s. 4953-4976
-
Tidskriftsartikel (refereegranskat)abstract
- An airfreight container with automated instruments for measurement of atmospheric gases and trace compounds was operated on a monthly basis onboard a Boeing 767-300 ER of LTU International Airways during long-distance flights from 1997 to 2002 (CARIBIC, Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container, http://www.caribic-atmospheric.com). Subsequently a more advanced system has been developed, using a larger capacity container with additional equipment and an improved inlet system. CARIBIC phase #2 was implemented on a new long-range aircraft type Airbus A340-600 of the Lufthansa German Airlines (Star Alliance) in December 2004, creating a powerful flying observatory. The instrument package comprises detectors for the measurement of O-3, total and gaseous H2O, NO and NOy, CO, CO2, O-2, Hg, and number concentrations of sub-micrometer particles (>4 nm, >12 nm, and >18 nm diameter). Furthermore, an optical particle counter (OPC) and a proton transfer mass spectrometer (PTR-MS) are incorporated. Aerosol samples are collected for analysis of elemental composition and particle morphology after flight. Air samples are taken in glass containers for laboratory analyses of hydrocarbons, halocarbons and greenhouse gases (including isotopic composition of CO2) in several laboratories. Absorption tubes collect oxygenated volatile organic compounds. Three differential optical absorption spectrometers (DOAS) with their telescopes mounted in the inlet system measure atmospheric trace gases such as BrO, HONO, and NO2. A video camera mounted in the inlet provides information about clouds along the flight track. The flying observatory, its equipment and examples of measurement results are reported.
|
|
| 3. |
- Sprovieri, F., et al.
(författare)
-
Atmospheric mercury concentrations observed at ground-based monitoring sites globally distributed in the framework of the GMOS network
- 2016
-
Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 16:18, s. 11915-11935
-
Tidskriftsartikel (refereegranskat)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.
|
|
| 4. |
- Ahrens, L., et al.
(författare)
-
Determination of polyfluoroalkyl compounds in water and suspended particulate matter in the river Elbe and North Sea, Germany
- 2009
-
Ingår i: Frontiers of Environmental Science & Engineering in China. - : Springer Science and Business Media LLC. - 1673-7520 .- 1673-7415. ; 3:2, s. 152-170
-
Tidskriftsartikel (refereegranskat)abstract
- The distribution of polyfluoroalkyl compounds (PFCs) in the dissolved and particulate phase and their discharge from the river Elbe into the North Sea were studied. The PFCs quantified included C-4-C-8 perfluorinated sulfonates (PFSAs), 6:2 fluorotelomer sulfonate (6:2 FTS), C-6 and C-8 perfluorinated sulfonates (PFSiAs), C-4-C-12 perfluorinated carboxylic acids (PFCAs), perfluoro-3,7-dimethyl-octanoic acid (3,7m(2)-PFOA), perfluorooctane sulfonamide (FOSA), and n-ethyl perfluroctane sulfonamidoethanol (EtFOSE). PFCs were mostly distributed in the dissolved phase, where perfluorooctanoic acid (PFOA) dominated with 2.9-12.5 ng/L. In the suspended particulate matter FOSA and perfluorooctane sulfonate (PFOS) showed the highest concentrations (4.0 ng/L and 2.3 ng/L, respectively). The total flux of Sigma PFCs from the river Elbe was estimated to be 802 kg/year for the dissolved phase and 152 kg/year for the particulate phase. This indicates that the river Elbe acts as a source of PFCs into the North Sea. However, the concentrations of perfluorobutane sulfonate (PFBS) and perfluorobutanoic acid (PFBA) in the North Sea were higher than that in the river Elbe, thus an alternative source must exist for these compounds
|
|
| 5. |
- Heue, K-P, et al.
(författare)
-
SO2 and BrO observation in the plume of the Eyjafjallajokull volcano 2010: CARIBIC and GOME-2 retrievals
- 2011
-
Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7324. ; 11:6, s. 2973-2989
-
Tidskriftsartikel (refereegranskat)abstract
- The ash cloud of the Eyjafjallajokull (also referred to as: Eyjafjalla (e.g. Schumann et al., 2011), Eyjafjoll or Eyjafjoll (e.g. Ansmann et al., 2010)) volcano on Iceland caused closure of large parts of European airspace in April and May 2010. For the validation and improvement of the European volcanic ash forecast models several research flights were performed. Also the CARIBIC (Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container) flying laboratory, which routinely measures at cruise altitude (approximate to 11 km) performed three dedicated measurements flights through sections of the ash plume. Although the focus of these flights was on the detection and quantification of the volcanic ash, we report here on sulphur dioxide (SO2) and bromine monoxide (BrO) measurements with the CARIBIC DOAS (Differential Optical Absorption Spectroscopy) instrument during the second of these special flights on 16 May 2010. As the BrO and the SO2 observations coincide, we assume the BrO to have been formed inside the volcanic plume. Average SO2 and BrO mixing ratios of approximate to 40 ppb and approximate to 5 ppt respectively are retrieved inside the plume. The BrO to SO2 ratio retrieved from the CARIBIC observation is approximate to 1.3x10(-4). Both SO2 and BrO observations agree well with simultaneous satellite (GOME-2) observations. SO2 column densities retrieved from satellite observations are often used as an indicator for volcanic ash. As the CARIBIC O-4 column densities changed rapidly during the plume observation, we conclude that the aerosol and the SO2 plume are collocated. For SO2 some additional information on the local distribution can be derived from a comparison of forward and back scan GOME-2 data. More details on the local plume size and position are retrieved by combining CARIBIC and GOME-2 data.
|
|
| 6. |
|
|
| 7. |
|
|
| 8. |
|
|
| 9. |
- Martinsson, B., et al.
(författare)
-
Analyzing atmospheric trace gases and aerosols using passenger aircraft
- 2005
-
Ingår i: Eos. - 0096-3941. ; 86:8, s. 77-77
-
Forskningsöversikt (refereegranskat)abstract
- CARIBIC (Civil Aircraft for the Regular Investigation of the Atmosphere Based on an Instrument Container) resumed regular measurement flights with an extended scientific payload in December 2004. After an automated measurement container was successfully deployed on intercontinental flights using a Boeing 767 from 1997 to 2002, a far more powerful package now is deployed using a new Airbus A340‐600 made available by Lufthansa German Airlines (Star Alliance). The new CARIBIC system will help address a range of current atmospheric science questions during its projected lifetime of 10 years.European and Japanese scientists are developing a variety of atmospheric chemistry research and monitoring projects based on the use of passenger aircraft. This is a logical approach with a main advantage being that near‐global coverage is obtained, in contrast to limited coverage through research aircraftbased expeditions. Moreover, highly detailed and consistent data sets can be acquired, as compared to satellite observations in general. In addition, even compared to land‐based observatories, operational costs are moderate.
|
|
| 10. |
- Munthe, John, et al.
(författare)
-
Distribution of atmospheric mercury species in Northern Europe: Final results from the MOE-project
- 2003
-
Ingår i: Atmospheric Environment. - 1352-2310 .- 1873-2844. ; 37:Suppl 1
-
Tidskriftsartikel (refereegranskat)abstract
- The mercury species over Europe (MOE) project was aimed at identifying sources, occurrence and atmospheric behaviour of atmospheric Hg species. Within MOE, emission measurements, ambient air measurements, process and regional-scale modelling and laboratory measurements were conducted. In this work, a summary of some of the main results is given. From the emission measurements, information on stack gas concentrations and emission factors for five coal fired power plants and three waste incinerators are presented. Results from field measurements of mercury species in ambient air at five locations in Northern Europe are presented. Examples from regional-scale atmospheric modelling are also given. The results emphasise the importance of information on Hg species for instance in emission inventories and measurement data from background sites. Furthermore, the importance of considering the role of the global cycling of mercury in future control strategies is emphasised
|
|
| 11. |
- Petäjä, Tuukka, et al.
(författare)
-
Overview : Integrative and Comprehensive Understanding on Polar Environments (iCUPE) - concept and initial results
- 2020
-
Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 20:14, s. 8551-8592
-
Tidskriftsartikel (refereegranskat)abstract
- The role of polar regions is increasing in terms of megatrends such as globalization, new transport routes, demography, and the use of natural resources with consequent effects on regional and transported pollutant concentrations. We set up the ERA-PLANET Strand 4 project iCUPE - integrative and Comprehensive Understanding on Polar Environments to provide novel insights and observational data on global grand challenges with an Arctic focus. We utilize an integrated approach combining in situ observations, satellite remote sensing Earth observations (EOs), and multi-scale modeling to synthesize data from comprehensive long-term measurements, intensive campaigns, and satellites to deliver data products, metrics, and indicators to stakeholders concerning the environmental status, availability, and extraction of natural resources in the polar areas. The iCUPE work consists of thematic state-of-the-art research and the provision of novel data in atmospheric pollution, local sources and transboundary transport, the characterization of arctic surfaces and their changes, an assessment of the concentrations and impacts of heavy metals and persistent organic pollutants and their cycling, the quantification of emissions from natural resource extraction, and the validation and optimization of satellite Earth observation (EO) data streams. In this paper we introduce the iCUPE project and summarize initial results arising out of the integration of comprehensive in situ observations, satellite remote sensing, and multi-scale modeling in the Arctic context.
|
|
| 12. |
- Slemr, F., et al.
(författare)
-
CARIBIC observations of gaseous mercury in the upper troposphere and lower stratosphere
- 2013
-
Ingår i: Proceedings of the 16th International Conference on Heavy Metals in the Environment. - : EDP Sciences. - 2100-014X. ; 1
-
Konferensbidrag (refereegranskat)abstract
- A unique set of gaseous mercury measurements in the upper troposphere and lower stratosphere (UT/LS) has been obtained during the monthly CARIBIC (www.caribic-atmospheric.com) flights since May 2005. The passenger Airbus 340-600 of Lufthansa covered routes to the Far East, North America, India, and the southern hemisphere. The accompanying measurements of CO, O3, NOy, H2O, aerosols, halocarbons, hydrocarbons, greenhouse gases, and several other parameters as well as backward trajectories enable a detailed analysis of these measurements. Speciation tests have shown that the CARIBIC measurements represent a good approximation of total gaseous mercury (TGM) concentrations. Above the tropopause TGM always decrease with increasing potential vorticity (PV) and O3 which implies its conversion to particle bound mercury. The observation of the lowest TGM concentrations at the highest particle concentrations in the stratosphere provides further evidence for such conversion. We will show how a seasonally dependent conversion rate could be derived using concomitantly measured SF6 mixing ratios as a timer. Tropospheric mercury data suggest the existence of a decreasing trend in the northern hemisphere whose size is comparable with the trend derived from long-term measurements by ship cruises, at Cape Point (South Africa) and Mace Head (Ireland).
|
|
| 13. |
- Slemr, F., et al.
(författare)
-
Gaseous mercury distribution in the upper troposphere and lower stratosphere observed onboard the CARIBIC passenger aircraft
- 2009
-
Ingår i: Atmospheric Chemistry and Physics. - 1680-7324. ; 9:6, s. 1957-1969
-
Tidskriftsartikel (refereegranskat)abstract
- Total gaseous mercury (TGM) was measured onboard a passenger aircraft during monthly CARIBIC flights (Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrumented Container) made between May 2005 and March 2007 on the routes Frankfurt-Sao Paulo-Santiago de Chile and back and Frankfurt-Guangzhou-Manila and back. The data provide for the first time an insight into the seasonal distributions of TGM in the upper troposphere and lower stratosphere (UT/LS) of both hemispheres and demonstrate the importance of mercury emissions from biomass burning in the Southern Hemisphere. Numerous plumes were observed in the upper troposphere, the larger of which could be characterized in terms of Hg/CO emission ratios and their probable origins. During the flights to China TGM correlated with CO in the upper troposphere with a seasonally dependent slope reflecting the longer lifetime of elemental mercury when compared to that of CO. A pronounced depletion of TGM was always observed in the extratropical lowermost stratosphere. TGM concentrations there were found to decrease with the increasing concentrations of particles. Combined with the large concentrations of particle bond mercury in the stratosphere observed by others, this finding suggests either a direct conversion of TGM to particle bound mercury or an indirect conversion via a semivolatile bivalent mercury compound. Based on concurrent measurements of SF6 during two flights, the rate of this conversion is estimated to 0.4 ng m(-3) yr(-1). A zero TGM concentration was not observed during some 200 flight hours in the lowermost stratosphere suggesting an equilibrium between the gaseous and particulate mercury.
|
|
| 14. |
|
|
| 15. |
- Steffen, A., et al.
(författare)
-
A synthesis of atmospheric mercury depletion event chemistry in the atmosphere and snow
- 2008
-
Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 8:6, s. 1445-1482
-
Tidskriftsartikel (refereegranskat)abstract
- It was discovered in 1995 that, during the spring time, unexpectedly low concentrations of gaseous elemental mercury (GEM) occurred in the Arctic air. This was surprising for a pollutant known to have a long residence time in the atmosphere; however conditions appeared to exist in the Arctic that promoted this depletion of mercury (Hg). This phenomenon is termed atmospheric mercury depletion events (AMDEs) and its discovery has revolutionized our understanding of the cycling of Hg in Polar Regions while stimulating a significant amount of research to understand its impact to this fragile ecosystem. Shortly after the discovery was made in Canada, AMDEs were confirmed to occur throughout the Arctic, sub-Artic and Antarctic coasts. It is now known that, through a series of photochemically initiated reactions involving halogens, GEM is converted to a more reactive species and is subsequently associated to particles in the air and/or deposited to the polar environment. AMDEs are a means by which Hg is transferred from the atmosphere to the environment that was previously unknown. In this article we review Hg research taken place in Polar Regions pertaining to AMDEs, the methods used to collect Hg in different environmental media, research results of the current understanding of AMDEs from field, laboratory and modeling work, how Hg cycles around the environment after AMDEs, gaps in our current knowledge and the future impacts that AMDEs may have on polar environments. The research presented has shown that while considerable improvements in methodology to measure Hg have been made but the main limitation remains knowing the speciation of Hg in the various media. The processes that drive AMDEs and how they occur are discussed. As well, the role that the snow pack and the sea ice play in the cycling of Hg is presented. It has been found that deposition of Hg from AMDEs occurs at marine coasts and not far inland and that a fraction of the deposited Hg does not remain in the same form in the snow. Kinetic studies undertaken have demonstrated that bromine is the major oxidant depleting Hg in the atmosphere. Modeling results demonstrate that there is a significant deposition of Hg to Polar Regions as a result of AMDEs. Models have also shown that Hg is readily transported to the Arctic from source regions, at times during springtime when this environment is actively transforming Hg from the atmosphere to the snow and ice surfaces. The presence of significant amounts of methyl Hg in snow in the Arctic surrounding AMDEs is important because this species is the link between the environment and impacts to wildlife and humans. Further, much work on methylation and demethylation processes has occurred but these processes are not yet fully understood. Recent changes in the climate and sea ice cover in Polar Regions are likely to have strong effects on the cycling of Hg in this environment; however more research is needed to understand Hg processes in order to formulate meaningful predictions of these changes.
|
|
