IVL Swedish Environmental Research Institute

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  • 1.
    Ferm, Martin
    IVL Swedish Environmental Research Institute.
    Impacts of air pollution and climate on materials in Athens, Greece2017In: Atmospheric Chemistry And Physics, ISSN 1680-7316, E-ISSN 1680-7324, Vol. 17, p. 439–448-Article in journal (Refereed)
    Abstract [en]

    For more than 10 years now the National and Kapodistrian University of Athens, Greece, has contributed to the UNECE (United Nations Economic Commission for Europe) ICP Materials (International Co-operative Programme on Effects on Materials including Historic and Cultural Monuments) programme for monitoring the corrosion/soiling levels of different kinds of materials due to environmental air-quality parameters. In this paper we present the results obtained from the analysis of observational data that were collected in Athens during the period 2003–2012.

    According to these results, the corrosion/soiling of the particular exposed materials tends to decrease over the years, except for the case of copper. Based on this long experimental database that is applicable to the multi-pollutant situation in the Athens basin, we present dose–response functions (DRFs) considering that “dose” stands for the air pollutant concentration, “response” for the material mass loss (normally per annum) and “function”, the relationship derived by the best statistical fit to the data.

  • 2.
    Fridell, Erik
    et al.
    IVL Swedish Environmental Research Institute.
    Karl, Matthias
    Bieser, Johannes
    Geyer, Beate
    Matthias, Volker
    Jalkanen, Jukka-Pekka
    Johansson, Lasse
    Impact of a nitrogen emission control area (NECA) on the future air quality and nitrogen deposition to seawater in the Baltic Sea region2019In: Atmospheric Chemistry And Physics, ISSN 1680-7316, E-ISSN 1680-7324, Vol. 19, no 1Article in journal (Refereed)
    Abstract [sv]

    Emissions och spridningsberäkningar för emissioner från sjöfart

  • 3.
    Hageström, Ulla
    et al.
    IVL Swedish Environmental Research Institute.
    Hansson, Katarina
    IVL Swedish Environmental Research Institute.
    Spandow, Pia
    IVL Swedish Environmental Research Institute.
    Munthe, John
    IVL Swedish Environmental Research Institute.
    Wängberg, Ingvar
    IVL Swedish Environmental Research Institute.
    Five-year records of mercury wet deposition flux at GMOS sites in the Northern and Southern hemispheres2017In: Atmospheric Chemistry And Physics, ISSN 1680-7316, E-ISSN 1680-7324, Vol. 17, p. 2689-2708Article in journal (Refereed)
    Abstract [en]

    The atmospheric deposition of mercury (Hg) occurs via several mechanisms, including dry and wet scavenging by precipitation events. In an effort to understand the atmospheric cycling and seasonal depositional characteristics of Hg, wet deposition samples were collected for approximately 5 years at 17 selected GMOS monitoring sites located in the Northern and Southern hemispheres in the framework of the Global Mercury Observation System (GMOS) project.

    Total mercury (THg) exhibited annual and seasonal patterns in Hg wet deposition samples. Interannual differences in total wet deposition are mostly linked with precipitation volume, with the greatest deposition flux occurring in the wettest years. This data set provides a new insight into baseline concentrations of THg concentrations in precipitation worldwide, particularly in regions such as the Southern Hemisphere and tropical areas where wet deposition as well as atmospheric Hg species were not investigated before, opening the way for future and additional simultaneous measurements across the GMOS network as well as new findings in future modeling studies.

  • 4.
    Hallquist, Åsa
    IVL Swedish Environmental Research Institute.
    Online gas- and particle-phase measurements of organosulfates, organosulfonates and nitrooxy organosulfates in Beijing utilizing a FIGAERO ToF-CIMS2018In: Atmospheric Chemistry And Physics, ISSN 1680-7316, E-ISSN 1680-7324, no 18, p. 10355-10371Article in journal (Refereed)
    Abstract [en]

    A time-of-flight chemical ionization mass spectrometer (CIMS) utilizing the Filter Inlet for Gas and Aerosol (FIGAERO) was deployed at a regional site 40km north-west of Beijing and successfully identified and measured 17 sulfur-containing organics (SCOs are organo/nitrooxy organosulfates and sulfonates) with biogenic and anthropogenic precursors. The SCOs were quantified using laboratory-synthesized standards of lactic acid sulfate and nitrophenol organosulfate (NP OS). The variation in field observations was confirmed by comparison to offline measurement techniques (orbitrap and high-performance liquid chromatography, HPLC) using daily averages. The mean total (of the 17 identified by CIMS) SCO particle mass concentration was 210±110ngm−3 and had a maximum of 540ngm−3, although it contributed to only 2±1% of the organic aerosol (OA). The CIMS identified a persistent gas-phase presence of SCOs in the ambient air, which was further supported by separate vapour-pressure measurements of NP OS by a Knudsen Effusion Mass Spectrometer (KEMS). An increase in relative humidity (RH) promoted partitioning of SCO to the particle phase, whereas higher temperatures favoured higher gas-phase concentrations.

    Biogenic emissions contributed to only 19% of total SCOs measured in this study. Here, C10H16NSO7, a monoterpene-derived SCO, represented the highest fraction (10%) followed by an isoprene-derived SCO. The anthropogenic SCOs with polycyclic aromatic hydrocarbon (PAH) and aromatic precursors dominated the SCO mass loading (51%) with C11H11SO7, derived from methyl naphthalene oxidation, contributing to 40ngm−3 and 0.3% of the OA mass. Anthropogenic-related SCOs correlated well with benzene, although their abundance depended highly on the photochemical age of the air mass, tracked using the ratio between pinonic acid and its oxidation product, acting as a qualitative photochemical clock. In addition to typical anthropogenic and biogenic precursors the biomass-burning precursor nitrophenol (NP) provided a significant level of NP OS. It must be noted that the contribution analysis here is only representative of the detected SCOs. There are likely to be many more SCOs present which the CIMS has not identified.

    Gas- and particle-phase measurements of glycolic acid suggest that partitioning towards the particle phase promotes glycolic acid sulfate production, contrary to the current formation mechanism suggested in the literature. Furthermore, the HSO4 ⋅ H2SO4− cluster measured by the CIMS was utilized as a qualitative marker for acidity and indicates that the production of total SCOs is efficient in highly acidic aerosols with high SO42− and organic content. This dependency becomes more complex when observing individual SCOs due to variability of specific VOC precursors.

  • 5.
    Hallquist, Åsa
    et al.
    IVL Swedish Environmental Research Institute.
    Garmash, Olga
    P. Rissanen, Matti
    Pullinen, Iida
    Schmitt, Sebastian
    Kausiala, Oskari
    Tillmann, Ralf
    Zhao, Defeng
    Percival, Carl
    J. Bannan, Thomas
    Priestley, Michael
    Kleist, Einhard
    Kiendler-Scharr, Astrid
    Hallquist, Mattias
    Berndt, Torsten
    McFiggans, Gordon
    Wildt, Jürgen
    F. Mentel, Thomas
    Ehn, Mikael
    Multi-generation OH oxidation as a source for highly oxygenated organic molecules from aromatics2019In: Atmospheric Chemistry And Physics, ISSN 1680-7316, E-ISSN 1680-7324Article in journal (Refereed)
  • 6.
    Jutterström, Sara
    et al.
    IVL Swedish Environmental Research Institute.
    Moldan, Filip
    Moldanová, Jana
    Karl, Matthias
    Matthias, Volker
    Posch, Maximilian
    The impact of nitrogen and sulfur emissions from shipping on the exceedance of critical loads in the Baltic Sea region2021In: Atmospheric Chemistry And Physics, ISSN 1680-7316, E-ISSN 1680-7324, Vol. 21, no 20, p. 15827-15845Article in journal (Refereed)
    Abstract [en]

    The emissions of nitrogen (N) and sulfur (S)species to the atmosphere from shipping significantly contribute to S and N deposition near the coast and to acidification and/or eutrophication of soils and freshwater.

    In thecountries around the Baltic Sea, the shipping volume and itsrelative importance as a source of emissions are expected toincrease if no efficient regulations are implemented.

    To assess the extent of environmental damage due to ship emissions for the Baltic Sea area, the exceedance of critical loads(CLs) for N and S has been calculated for the years 2012 and2040.

    The paper evaluates the effects of several future scenarios, including the implementation of NECA and SECA(Nitrogen And Sulfur Emission Control Areas).

    The implementation of NECA and SECA caused a significant decreasein the exceedance of CLs for N as a nutrient while the impact on the – already much lower – exceedance of CLs foracidification was less pronounced.

    The relative contributionfrom Baltic shipping to the total deposition decreased from2012 in the 2040 scenario for both S and N. In contrastto exceedances of CLs for acidification, shipping still hasan impact on exceedances for eutrophication in 2040.

    Geographically, the impact of shipping emissions is unevenlydistributed even within each country. This is illustrated bycalculating CL exceedances for 21 Swedish counties.

    Theimpact, on a national level, is driven by a few coastal counties, where the impact of shipping is much higher than thenational summary suggests.

  • 7.
    Karlsson, Per Erik
    IVL Swedish Environmental Research Institute.
    Reanalysis of and attribution to near-surface ozone concentrations in Sweden during 1990-20132018In: Atmospheric Chemistry And Physics, ISSN 1680-7316, E-ISSN 1680-7324, no 17, p. 13869-13890Article in journal (Refereed)
    Abstract [en]

    We have constructed two data sets of hourly resolution reanalyzed near-surface ozone (O3) concentrations for the period 1990–2013 for Sweden. Long-term simulations from a chemistry-transport model (CTM) covering Europe were combined with hourly ozone concentration observations at Swedish and Norwegian background measurement sites using retrospective variational data analysis. The reanalysis data sets show improved performance over the original CTM when compared to independent observations.

    In one of the reanalyses, we included all available hourly near-surface O3 observations, whilst in the other we carefully selected time-consistent observations. Based on the second reanalysis we investigated statistical aspects of the distribution of the near-surface O3 concentrations, focusing on the linear trend over the 24-year period. We show that high near-surface O3 concentrations are decreasing and low O3 concentrations are increasing, which is reflected in observed improvement of many health and vegetation indices (apart from those with a low threshold).

    Using the CTM we also conducted sensitivity simulations to quantify the causes of the observed change, focusing on three factors: change in hemispheric background concentrations, meteorology and anthropogenic emissions. The rising low concentrations of near-surface O3 in Sweden are caused by a combination of all three factors, whilst the decrease in the highest O3 concentrations is caused by European O3 precursor emissions reductions.

    While studying the impact of anthropogenic emissions changes, we identified systematic differences in the modeled trend compared to observations that must be caused by incorrect trends in the utilized emissions inventory or by too high sensitivity of our model to emissions changes.

  • 8.
    Langer, Sarka
    IVL Swedish Environmental Research Institute.
    Chemical cycling and deposition of atmospheric mercury in polar regions: review of recent measurements and comparison with models.2016In: Atmospheric Chemistry And Physics, ISSN 1680-7316, E-ISSN 1680-7324, Vol. 16, p. 10735–10763-Article in journal (Refereed)
    Abstract [en]

    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.

  • 9.
    Moldanova, Jana
    et al.
    IVL Swedish Environmental Research Institute.
    Fallgren, Henrik
    IVL Swedish Environmental Research Institute.
    Passig, J.
    Schade, J.
    I. Rosewig, E.
    Irsig, R.
    Kröger-Badge, T.
    Czech, H.
    Sklorz, M.
    Streibel, T.
    Li, L.
    Li, X.
    Zhou, Z.
    Zimmermann, R.
    Resonance-Enhanced Detection of Metals in Aerosols using Single Particle Mass Spectrometry2020In: Atmospheric Chemistry And Physics, ISSN 1680-7316, E-ISSN 1680-7324, Vol. 20, no 12, p. 7139-7152Article in journal (Refereed)
    Abstract [en]

    We describe resonance effects in laser desorption–ionization (LDI) of particles that substantially increase the sensitivity and selectivity to metals in single-particle mass spectrometry (SPMS). Within the proposed scenario, resonant light absorption by ablated metal atoms increases their ionization rate within a single laser pulse. By choosing the appropriate laser wavelength, the key micronutrients Fe, Zn and Mn can be detected on individual aerosol particles with considerably improved efficiency. These ionization enhancements for metals apply to natural dust and anthropogenic aerosols, both important sources of bioavailable metals to marine environments. Transferring the results into applications, we show that the spectrum of our KrF-excimer laser is in resonance with a major absorption line of iron atoms. To estimate the impact of resonant LDI on the metal detection efficiency in SPMS applications, we performed a field experiment on ambient air with two alternately firing excimer lasers of different wavelengths. Herein, resonant LDI with the KrF-excimer laser (248.3 nm) revealed iron signatures for many more particles of the same aerosol ensemble compared to the more common ArF-excimer laser line of 193.3 nm (nonresonant LDI of iron). Many of the particles that showed iron contents upon resonant LDI were mixtures of sea salt and organic carbon. For nonresonant ionization, iron was exclusively detected in particles with a soot contribution. This suggests that resonant LDI allows a more universal and secure metal detection in SPMS. Moreover, our field study indicates relevant atmospheric iron transport by mixed organic particles, a pathway that might be underestimated in SPMS measurements based on nonresonant LDI. Our findings show a way to improve the detection and source attribution capabilities of SPMS for particle-bound metals, a health-relevant aerosol component and an important source of micronutrients to the surface oceans affecting marine primary productivity.

  • 10.
    Moldanova, Jana
    et al.
    IVL Swedish Environmental Research Institute.
    Fridell, Erik
    IVL Swedish Environmental Research Institute.
    O. P. Ramacher, M.
    Tang, L.
    Matthias, V.
    Karl, M.
    Johansson, L.
    The impact of ship emissions on air quality and human health in the Gothenburg area – Part II: Scenarios for 20402020In: Atmospheric Chemistry And Physics, ISSN 1680-7316, E-ISSN 1680-7324, Vol. 20, no 10, p. 667-10686Article in journal (Refereed)
    Abstract [en]

    Shipping is an important source of air pollutants, from the global to the local scale. Ships emit substantial amounts of sulfur dioxides, nitrogen dioxides, and particulate matter in the vicinity of coasts, threatening the health of the coastal population, especially in harbour cities. Reductions in emissions due to shipping have been targeted by several regulations. Nevertheless, effects of these regulations come into force with temporal delays, global ship traffic is expected to grow in the future, and other land-based anthropogenic emissions might decrease. Thus, it is necessary to investigate combined impacts to identify the impact of shipping activities on air quality, population exposure, and health effects in the future. We investigated the future effect of shipping emissions on air quality and related health effects considering different scenarios of the development of shipping under current regional trends of economic growth and already decided regulations in the Gothenburg urban area in 2040. Additionally, we investigated the impact of a large-scale implementation of shore electricity in the Port of Gothenburg. For this purpose, we established a one-way nested chemistry transport modelling (CTM) system from the global to the urban scale, to calculate pollutant concentrations, population-weighted concentrations, and health effects related to NO2, PM2.5, and O3. The simulated concentrations of NO2 and PM2.5 in future scenarios for the year 2040 are in general very low with up to 4 ppb for NO2 and up to 3.5 µg m−3 PM2.5 in the urban areas which are not close to the port area. From 2012 the simulated overall exposure to PM2.5 decreased by approximately 30 % in simulated future scenarios; for NO2 the decrease was over 60 %. The simulated concentrations of O3 increased from the year 2012 to 2040 by about 20 %. In general, the contributions of local shipping emissions in 2040 focus on the harbour area but to some extent also influence the rest of the city domain. The simulated impact of onshore electricity implementation for shipping in 2040 shows reductions for NO2 in the port of up to 30 %, while increasing O3 of up to 3 %. Implementation of onshore electricity for ships at berth leads to additional local reduction potentials of up to 3 % for PM2.5 and 12 % for SO2 in the port area. All future scenarios show substantial decreases in population-weighted exposure and health-effect impacts.

  • 11.
    Moldanova, Jana
    et al.
    IVL Swedish Environmental Research Institute.
    Yaramenka, Katarina
    IVL Swedish Environmental Research Institute.
    Gustafsson, Malin
    IVL Swedish Environmental Research Institute.
    Tang, L.
    O. P. Ramacher, M.
    Matthias, V.
    Karl, M.
    Johansson, L.
    Jalkanen, J-P.
    Aulinger, A.
    The impact of ship emissions on air quality and human health in the Gothenburg area – Part I: 2012 emissions2020In: Atmospheric Chemistry And Physics, ISSN 1680-7316, E-ISSN 1680-7324, Vol. 20, p. 7509 – 7530-Article in journal (Refereed)
    Abstract [en]

    Ship emissions in and around ports are of interest for urban air quality management in many harbour cities. We investigated the impact of regional and local ship emissions on urban air quality for 2012 conditions in the city of Gothenburg, Sweden, the largest cargo port in Scandinavia. In order to assess the effects of ship emissions, a coupled regional- and local-scale model system has been set up using ship emissions in the Baltic Sea and the North Sea as well as in and around the port of Gothenburg. Ship emissions were calculated with the Ship Traffic Emission Assessment Model (STEAM), taking into account individual vessel characteristics and vessel activity data. The calculated contributions from local and regional shipping to local air pollution in Gothenburg were found to be substantial, especially in areas around the city ports. The relative contribution from local shipping to annual mean NO2 concentrations was 14 % as the model domain average, while the relative contribution from regional shipping in the North Sea and the Baltic Sea was 26 %. In an area close to the city terminals, the contribution of NO2 from local shipping (33 %) was higher than that of road traffic (28 %), which indicates the importance of controlling local shipping emissions. Local shipping emissions of NOx led to a decrease in the summer mean O3 levels in the city by 0.5 ppb (∼2 %) on average. Regional shipping led to a slight increase in O3 concentrations; however, the overall effect of regional and the local shipping together was a small decrease in the summer mean O3 concentrations in the city. In addition, volatile organic compound (VOC) emissions from local shipping compensate up to 4 ppb of the decrease in summer O3 concentrations due to the NO titration effect. For particulate matter with a median aerodynamic diameter less than or equal to 2.5 µm (PM2.5), local ship emissions contributed only 3 % to the annual mean in the model domain, while regional shipping under 2012 conditions was a larger contributor, with an annual mean contribution of 11 % of the city domain average. Based on the modelled local and regional shipping contributions, the health effects of PM2.5, NO2 and ozone were assessed using the ALPHA-RiskPoll (ARP) model. An effect of the shipping-associated PM2.5 exposure in the modelled area was a mean decrease in the life expectancy by 0.015 years per person. The relative contribution of local shipping to the impact of total PM2.5 was 2.2 %, which can be compared to the 5.3 % contribution from local road traffic. The relative contribution of the regional shipping was 10.3 %. The mortalities due to the exposure to NO2 associated with shipping were calculated to be 2.6 premature deaths yr−1. The relative contribution of local and regional shipping to the total exposure to NO2 in the reference simulation was 14 % and 21 %, respectively. The shipping-related ozone exposures were due to the NO titration effect leading to a negative number of premature deaths. Our study shows that overall health impacts of regional shipping can be more significant than those of local shipping, emphasizing that abatement policy options on city-scale air pollution require close cooperation across governance levels. Our findings indicate that the strengthened Sulphur Emission Control Areas (SECAs) fuel sulphur limit from 1 % to 0.1 % in 2015, leading to a strong decrease in the formation of secondary particulate matter on a regional scale was an important step in improving the air quality in the city.

  • 12.
    Munthe, John
    et al.
    IVL Swedish Environmental Research Institute.
    Kindbom, Karin
    IVL Swedish Environmental Research Institute.
    Current and future levels of mercury atmospheric pollution on a global scale2016In: Atmospheric Chemistry And Physics, ISSN 1680-7316, E-ISSN 1680-7324, Vol. 16, p. 12495-12511Article in journal (Refereed)
    Abstract [en]

    An assessment of current and future emissions, air concentrations, and atmospheric deposition of mercury worldwide is 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 combustion of fossil fuels (mainly coal) for energy and heat production in power plants and in industrial and residential boilers, as well as artisanal and small-scale gold mining, is one of 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 t. Emissions in Asian countries, particularly in China and India, dominate the total emissions of Hg. The current estimates of mercury emissions from natural processes (primary mercury emissions and re-emissions), including mercury depletion events, were estimated to be 5207 t year−1, which represents 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 three different scenarios with current anthropogenic 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 mercury pollution levels considering future emission scenarios. Projections of future changes in mercury deposition on a global scale simulated by these models for three anthropogenic emissions scenarios of 2035 indicate a decrease in 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 the scientific justification for the Minamata Convention and 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 mercury on a global and regional scale, and source–receptor techniques for mercury emission apportionment on a global scale.

  • 13.
    Munthe, John
    et al.
    IVL Swedish Environmental Research Institute.
    Wängberg, Ingvar
    IVL Swedish Environmental Research Institute.
    Atmospheric mercury concentrations observed at ground-based monitoring sites globally distributed in the framework of the GMOS network2016In: Atmospheric Chemistry And Physics, ISSN 1680-7316, E-ISSN 1680-7324, Vol. 16, p. 11915-11935Article in journal (Refereed)
    Abstract [en]

    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.

  • 14.
    Wängberg, Ingvar
    IVL Swedish Environmental Research Institute.
    Multi-model study of mercury dispersion in the atmosphere: Atmospheric processes and model evaluation2017In: Atmospheric Chemistry And Physics, ISSN 1680-7316, E-ISSN 1680-7324, Vol. 17, no 8, p. 5271-5295Article in journal (Refereed)
    Abstract [en]

    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.

  • 15.
    Wängberg, Ingvar
    IVL Swedish Environmental Research Institute.
    Particulate-phase mercury emissions from biomass burning and impact on resulting deposition: a modelling assessment2017In: Atmospheric Chemistry And Physics, ISSN 1680-7316, E-ISSN 1680-7324, Vol. 17, p. 1881–1899-Article in journal (Refereed)
    Abstract [en]

    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 percent. 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.

  • 16.
    Wängberg, Ingvar
    et al.
    IVL Swedish Environmental Research Institute.
    Munthe, John
    IVL Swedish Environmental Research Institute.
    Airborne mercury species at the Råö background monitoring site in Sweden: distribution of mercury as an effect of long-range transport2016In: Atmospheric Chemistry And Physics, ISSN 1680-7316, E-ISSN 1680-7324, Vol. 16, p. 13379–13387-Article in journal (Refereed)
    Abstract [en]

    Within the EU-funded project, Global Mercury Observation System (GMOS) airborne mercury has been monitored at the background Råö measurement site on the western coast of Sweden from mid-May 2012 to the beginning of July 2013 and from the beginning of February 2014 to the end of May 2015. The following mercury species/fractions were measured: gaseous elemental mercury (GEM), particulate bound mercury (PBM) and gaseous oxidised mercury (GOM) using the Tekran measurement system. The mercury concentrations measured at the Råö site were found to be low in comparison to other, comparable, European measurement sites.

    A back-trajectory analysis to study the origin of air masses reaching the Råö site was performed. Due to the remote location of the Råö measurement station it receives background air about 60 % of the time. However, elevated mercury concentrations arriving with air masses coming from the south-east are noticeable. GEM and PBM concentrations show a clear annual variation with the highest values occurring during winter, whereas the highest concentrations of GOM were obtained in spring and summer. An evaluation of the diurnal pattern of GOM, with peak concentrations at midday or in the early afternoon, which often is observed at remote places, shows that it is likely to be driven by local meteorology in a similar way to ozone. Evidence that a significant part of the GOM measured at the Råö site has been formed in free tropospheric air is presented.

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