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  • Copernicus  (11)
  • 1
    Publication Date: 2017-04-24
    Description: Current understanding of mercury (Hg) behavior in the atmosphere contains significant gaps. Some key characteristics of Hg processes, including anthropogenic and geogenic emissions, atmospheric chemistry, and air–surface exchange, are still poorly known. This study provides a complex analysis of processes governing Hg fate in the atmosphere involving both measured data from ground-based sites and simulation results from chemical transport models. A variety of long-term measurements of gaseous elemental Hg (GEM) and reactive Hg (RM) concentration as well as Hg wet deposition flux have been compiled from different global and regional monitoring networks. Four contemporary global-scale transport models for Hg were used, both in their state-of-the-art configurations and for a number of numerical experiments to evaluate particular processes. Results of the model simulations were evaluated against measurements. As follows from the analysis, the interhemispheric GEM gradient is largely formed by the prevailing spatial distribution of anthropogenic emissions in the Northern Hemisphere. The contributions of natural and secondary emissions enhance the south-to-north gradient, but their effect is less significant. Atmospheric chemistry has a limited effect on the spatial distribution and temporal variation of GEM concentration in surface air. In contrast, RM air concentration and wet deposition are largely defined by oxidation chemistry. The Br oxidation mechanism can reproduce successfully the observed seasonal variation of the RM ∕ GEM ratio in the near-surface layer, but it predicts a wet deposition maximum in spring instead of in summer as observed at monitoring sites in North America and Europe. Model runs with OH chemistry correctly simulate both the periods of maximum and minimum values and the amplitude of observed seasonal variation but shift the maximum RM ∕ GEM ratios from spring to summer. O3 chemistry does not predict significant seasonal variation of Hg oxidation. Hence, the performance of the Hg oxidation mechanisms under study differs in the extent to which they can reproduce the various observed parameters. This variation implies possibility of more complex chemistry and multiple Hg oxidation pathways occurring concurrently in various parts of the atmosphere.
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 2
    Publication Date: 2017-02-08
    Description: 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.
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 3
    Publication Date: 2017-01-13
    Description: Atmospheric deposition is the most important pathway by which Hg reaches marine ecosystems, where it can be methylated and enter the base of food chain. The deposition, transport and chemical interactions of atmospheric Hg have been simulated over Europe for the year 2013 in the framework of the Global Mercury Observation System (GMOS) project, performing 14 different model sensitivity tests using two high-resolution three-dimensional chemical transport models (CTMs), varying the anthropogenic emission datasets, atmospheric Br input fields, Hg oxidation schemes and modelling domain boundary condition input. Sensitivity simulation results were compared with observations from 28 monitoring sites in Europe to assess model performance and particularly to analyse the influence of anthropogenic emission speciation and the Hg0(g) atmospheric oxidation mechanism. The contribution of anthropogenic Hg emissions, their speciation and vertical distribution are crucial to the simulated concentration and deposition fields, as is also the choice of Hg0(g) oxidation pathway. The areas most sensitive to changes in Hg emission speciation and the emission vertical distribution are those near major sources, but also the Aegean and the Black seas, the English Channel, the Skagerrak Strait and the northern German coast. Considerable influence was found also evident over the Mediterranean, the North Sea and Baltic Sea and some influence is seen over continental Europe, while this difference is least over the north-western part of the modelling domain, which includes the Norwegian Sea and Iceland. The Br oxidation pathway produces more HgII(g) in the lower model levels, but overall wet deposition is lower in comparison to the simulations which employ an O3 ∕ OH oxidation mechanism. The necessity to perform continuous measurements of speciated Hg and to investigate the local impacts of Hg emissions and deposition, as well as interactions dependent on land use and vegetation, forests, peat bogs, etc., is highlighted in this study.
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 4
    Publication Date: 2016-08-01
    Description: Mercury (Hg) emissions from Biomass Burning (BB) are an important source of atmospheric Hg and is a major factor driving the inter-annual variation of Hg concentrations in the troposphere. 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 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 Hg0g availability to the global atmospheric pool. This reduces Hg deposition from BB to the world's oceans from 71 % to 62 %. The impact locally is however significant, northern boreal and tropical forests where fires are frequent and uncontrolled leads to notable Hg inputs to local ecosystems. Under water-stressed conditions in tropical forests and warming temperatures in northern forests this effect may be exacerbated in the future.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 5
    Publication Date: 2016-05-25
    Description: An assessment of current and future emissions, air concentrations and atmospheric deposition of mercury world-wide are presented on the basis of results obtained during the performance of the EU GMOS (Global Mercury Observation System) project. Emission estimates for mercury were prepared with the main goal of applying them in models to assess current (2013) and future (2035) air concentrations and atmospheric deposition of this contaminant. The artisanal and small- scale gold mining, as well as combustion of fossil fuels (mainly coal) for energy and heat production in power plants and in industrial and residential boilers are the major anthropogenic sources of Hg emissions to the atmosphere at present. These sources account for about 37 % and 25 % of the total anthropogenic Hg emissions globally, estimated to be about 2000 tonnes. The emissions in Asian countries, particularly in China and India dominate the total emissions of Hg. The current estimate of mercury emissions from natural processes (primary mercury emissions and re-emissions), including mercury depletion events, were estimated to be 5207 tonnes per year which represent nearly 70 % of the global mercury emission budget. Oceans are the most important sources (36 %) followed by biomass burning (9 %). A comparison of the 2035 anthropogenic emissions estimated for 3 different scenarios with current anthriopogenic emissions indicates a reduction of these emissions in 2035 up to 85 % for the best case scenario. Two global chemical transport models (GLEMOS and ECHMERIT) have been used for the evaluation of future Hg pollution levels considering future emission scenarios. Projections of future changes in Hg deposition on a global scale simulated by these models for three anthropogenic emissions scenarios of 2035 indicate a decrease of up to 50 % deposition in the Northern Hemisphere and up to 35 % in Southern Hemisphere for the best case scenario. The EU GMOS project has proved to be a very important research instrument for supporting, first the scientific justification for the Minamata Convention, and then monitoring of the implementation of targets of this Convention, as well as, the EU Mercury Strategy. This project provided the state-of-the art with regard to the development of the latest emission inventories for mercury, future emission scenarios, dispersion modelling of atmospheric Hg on global and regional scale, and source – receptor techniques for Hg emission apportionment on a global scale.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 6
    Publication Date: 2016-08-05
    Description: Atmospheric deposition is the most important pathway by which Hg reaches marine ecosystems, where it can be methylated and enter the base of food chain. The deposition, the transport and chemical interactions of atmospheric Hg has been simulated over Europe for the year 2013 in the framework of the Global Mercury Observation System (GMOS) project, performing 14 different model sensitivity tests using two high resolution three-dimensional Chemical Transport Models (CTMs), varying the anthropogenic emissions data sets, atmospheric Br input fields, the Hg oxidation schemes and the modelling domain boundary condition input. Sensitivity simulation results were compared with observations from 28 monitoring sites in Europe, to assess model performance and particularly to analyse the influence of anthropogenic emission speciation and the Hg0(g) atmospheric oxidation mechanism. The contribution of anthropogenic Hg emissions, their speciation and vertical distribution is crucial to the simulated concentration and deposition fields, as is also the choice of Hg0(g) oxidation pathway. The areas most sensitive to changes in Hg emission speciation and the emission vertical distribution are those near major sources, but also the Aegean and the Black Seas, the English Channel, the Skagerrak Strait and the North German coast. Considerable influence was found also evident over the Mediterranean, the North and Baltic Sea, some influence is seen over continental Europe, while this difference is least over the north-western part of the modelling domain, which includes the Norwegian Sea and Iceland. The Br oxidation pathway produces more HgII(g) in the lower model levels, but overall wet deposition is lower in comparison to the simulations which employ an O3/OH oxidation mechanism. The necessity to perform continuous measurements of speciated Hg, to investigate the local impacts of Hg emissions and deposition, as well as interactions dependent on land use and vegetation, forests, peat bogs etc. is highlighted in this study
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 7
    Publication Date: 2016-06-16
    Description: 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 reemission). 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 reemission 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 inter-annual variability are appropriately represented in the models, and identifies research gaps in our understanding of the atmospheric Hg cycling in high latitudes.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 8
    Publication Date: 2016-10-31
    Description: Current understanding of mercury (Hg) behaviour in the atmosphere contains significant gaps. Some key characteristics of Hg processes including anthropogenic and geogenic emissions, atmospheric chemistry, and air-surface exchange are still poorly known. This study provides a complex analysis of processes governing Hg fate in the atmosphere involving both measurement data from ground-based sites and simulation results of chemical transport models. A variety of long-term measurements of gaseous elemental Hg (GEM) and reactive Hg (RM) concentration as well as Hg wet deposition flux has been compiled from different global and regional monitoring networks. Four contemporary global-scale transport models for Hg were applied both in their state-of-the-art configurations and for a number of numerical experiments aimed at evaluation of particular processes. Results of the model simulation were evaluated against measurements. As it follows from the analysis the inter-hemispheric gradient of GEM is largely formed by the spatial distribution of anthropogenic emissions which prevail in the Northern Hemisphere. Contribution of natural and secondary emissions enhances the south-to-north gradient but their effect is less significant. The atmospheric chemistry does not affect considerably both spatial distribution and temporal variation of GEM concentration in the surface air. On the other hand, RM air concentration and wet deposition are largely defined by oxidation chemistry. The Br oxidation mechanism allows successfully reproducing observed seasonal variation of the RM / GEM ratio in the near-surface layer, whereas it predicts maximum in wet deposition in spring instead of summer as observed at monitoring sites located in North America and Europe. Model runs with the OH chemistry correctly simulate both the periods of maximum and minimum values and the amplitude of observed seasonal variation but lead to shifting the maximum RM / GEM ratios from spring to summer. The O3 chemistry does not provide significant seasonal variation of Hg oxidation. Thus, performance of the considered Hg oxidation mechanisms differs in reproduction of different observed parameters that can imply possibility of more complex chemistry and multiple pathways of Hg oxidation occurring concurrently in various parts of the atmosphere.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 9
    Publication Date: 2016-12-07
    Description: High-resolution Earth system model simulations generate enormous data volumes, and retaining the data from these simulations often strains institutional storage resources. Further, these exceedingly large storage requirements negatively impact science objectives, for example, by forcing reductions in data output frequency, simulation length, or ensemble size. To lessen data volumes from the Community Earth System Model (CESM), we advocate the use of lossy data compression techniques. While lossy data compression does not exactly preserve the original data (as lossless compression does), lossy techniques have an advantage in terms of smaller storage requirements. To preserve the integrity of the scientific simulation data, the effects of lossy data compression on the original data should, at a minimum, not be statistically distinguishable from the natural variability of the climate system, and previous preliminary work with data from CESM has shown this goal to be attainable. However, to ultimately convince climate scientists that it is acceptable to use lossy data compression, we provide climate scientists with access to publicly available climate data that have undergone lossy data compression. In particular, we report on the results of a lossy data compression experiment with output from the CESM Large Ensemble (CESM-LE) Community Project, in which we challenge climate scientists to examine features of the data relevant to their interests, and attempt to identify which of the ensemble members have been compressed and reconstructed. We find that while detecting distinguishing features is certainly possible, the compression effects noticeable in these features are often unimportant or disappear in post-processing analyses. In addition, we perform several analyses that directly compare the original data to the reconstructed data to investigate the preservation, or lack thereof, of specific features critical to climate science. Overall, we conclude that applying lossy data compression to climate simulation data is both advantageous in terms of data reduction and generally acceptable in terms of effects on scientific results.
    Print ISSN: 1991-959X
    Electronic ISSN: 1991-9603
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 10
    Publication Date: 2016-08-30
    Description: 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.
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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