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HBr emissions from volcanoes lead rapidly to the formation of BrO within volcanic plumes and have an impact on tropospheric chemistry, at least at the local and regional scales. The motivation of this paper is to prepare a framework for further 3D modelling of volcanic halogen emissions in order to determine their fate within the volcanic plume and then in the atmosphere at the regional and global scales. The main aim is to evaluate the ability of the model to produce a realistic partitioning of bromine species within a grid box size typical of MOCAGE (Model Of atmospheric Chemistry At larGE scale) 3D (0.5∘ × 0.5∘). This work is based on a 1D single-column configuration of the global chemistry-transport model MOCAGE that has low enough computational cost to allow us to perform a large set of sensitivity simulations. This paper uses the emissions from the Mount Etna eruption on 10 May 2008. Several reactions are added to MOCAGE to represent the volcanic plume halogen chemistry. A simple plume parameterisation is also implemented and tested. The use of this parameterisation tends to only slightly limit the efficiency of BrO net production. Both simulations with and without the parameterisation give results for the partitioning of the bromine species, of ozone depletion and of the ratio that are consistent with previous studies.
A series of test experiments were performed to evaluate the sensitivity of the results to the composition of the emissions (primary sulfate aerosols, Br radical and NO) and to the effective radius assumed for the volcanic sulfate aerosols. Simulations show that the plume chemistry is sensitive to all these parameters. We also find that the maximum altitude of the eruption changes the BrO production, which is linked to the vertical variability of the concentrations of oxidants in the background air. These sensitivity tests display changes in the bromine chemistry cycles that are generally at least as important as the plume parameterisation. Overall, the version of the MOCAGE chemistry developed for this study is suitable to produce the expected halogen chemistry in volcanic plumes during daytime and night-time.
2023
For the next-generation risk assessment (NGRA) of chemicals and nanomaterials, new approach methodologies (NAMs) are needed for hazard assessment in compliance with the 3R’s to reduce, replace and refine animal experiments. This study aimed to establish and characterize an advanced respiratory model consisting of human epithelial bronchial BEAS-2B cells cultivated at the air–liquid interface (ALI), both as monocultures and in cocultures with human endothelial EA.hy926 cells. The performance of the bronchial models was compared to a commonly used alveolar model consisting of A549 in monoculture and in coculture with EA.hy926 cells. The cells were exposed at the ALI to nanosilver (NM-300K) in the VITROCELL® Cloud. After 24 h, cellular viability (alamarBlue assay), inflammatory response (enzyme-linked immunosorbent assay), DNA damage (enzyme-modified comet assay), and chromosomal damage (cytokinesis-block micronucleus assay) were measured. Cytotoxicity and genotoxicity induced by NM-300K were dependent on both the cell types and model, where BEAS-2B in monocultures had the highest sensitivity in terms of cell viability and DNA strand breaks. This study indicates that the four ALI lung models have different sensitivities to NM-300K exposure and brings important knowledge for the further development of advanced 3D respiratory in vitro models for the most reliable human hazard assessment based on NAMs.
2023
Titanium dioxide nanoparticles (TiO2 NPs) are used in a wide range of applications. Although inhalation of NPs is one of the most important toxicologically relevant routes, experimental studies on potential harmful effects of TiO2 NPs using a whole-body inhalation chamber model are rare. In this study, the profile of lymphocyte markers, functional immunoassays, and antioxidant defense markers were analyzed to evaluate the potential adverse effects of seven-week inhalation exposure to two different concentrations of TiO2 NPs (0.00167 and 0.1308 mg TiO2/m3) in mice. A dose-dependent effect of TiO2 NPs on innate immunity was evident in the form of stimulated phagocytic activity of monocytes in low-dose mice and suppressed secretory function of monocytes (IL-18) in high-dose animals. The effect of TiO2 NPs on adaptive immunity, manifested in the spleen by a decrease in the percentage of T-cells, a reduction in T-helper cells, and a dose-dependent decrease in lymphocyte cytokine production, may indicate immunosuppression in exposed mice. The dose-dependent increase in GSH concentration and GSH/GSSG ratio in whole blood demonstrated stimulated antioxidant defense against oxidative stress induced by TiO2 NP exposure.
2023
Persistent organic pollutants (POPs) are synthetic compounds that were intentionally produced in large quantities and have been distributed in the global environment, originating a threat due to their persistence, bioaccumulative potential, and toxicity. POPs reach the Antarctic continent through long-range atmospheric transport (LRAT). In these areas, low temperatures play a significant role in the environmental fate of POPs, retaining them for a long time due to cold trapping by diffusion and wet deposition, acting as a net sink for many POPs. However, in the current context of climate change, the remobilization of POPs that were trapped in water, ice, and soil for decades is happening. Therefore, continuous monitoring of POPs in polar air is necessary to assess whether there is a recent re-release of historical pollutants back to the environment. We reviewed the scientific literature on atmospheric levels of several POP families (polychlorinated biphenyls – PCBs, hexachlorobenzene – HCB, hexachlorocyclohexanes – HCHs, and dichlorodiphenyltrichloroethane – DDT) from 1980 to 2021. We estimated the atmospheric half-life using characteristic decreasing times (TD). We observed that HCB levels in the Antarctic atmosphere were higher than the other target organochlorine pesticides (OCPs), but HCB also displayed higher fluctuations and did not show a significant decrease over time. Conversely, the atmospheric levels of HCHs, some DDTs, and PCBs have decreased significantly. The estimated atmospheric half-lives for POPs decreased in the following order: 4,4' DDE (13.5 years) > 4,4' DDD (12.8 years) > 4,4' DDT (7.4 years) > 2,4' DDE (6.4 years) > 2,4' DDT (6.3 years) > α-HCH (6 years) > HCB (6 years) > γ-HCH (4.2 years). For PCB congeners, they decreased in the following order: PCB 153 (7.6 years) > PCB 138 (6.5 years) > PCB 101 (4.7 years) > PCB 180 (4.6 years) > PCB 28 (4 years) > PCB 52 (3.7 years) > PCB 118 (3.6 years). For HCH isomers and PCBs, the Stockholm Convention (SC) ban on POPs did have an impact on decreasing their levels during the last decades. Nevertheless, their ubiquity in the Antarctic atmosphere shows the problematic issues related to highly persistent synthetic chemicals.
2023
Leaching of chemicals and DOC from tire particles under simulated marine conditions
Tire wear particles (TWPs) represent one of the major anthropogenic pools of particles ending up in the environment. They contain a large variety of chemicals, a part of which may be released into the environment through leaching, although the influence of sunlight and other environmental factors during this process is still unclear. This laboratory study compares the leaching of organic compounds from TWP in seawater in the dark and under artificial sunlight for 1) cryo-milled tire tread (CMTT), 2) ‘virgin’ crumb rubber (VCR) and 3) crumb rubber immersed in the sea for ≥12 months prior to the experiments (WCR). Leachates were analyzed for dissolved organic carbon (DOC) and 19 tire-derived chemicals, benzothiazoles and phenylguanidines as well as phenylendiamines by liquid chromatography-high resolution-mass spectrometry. For DOC and most chemicals, the amounts released decreased in the order CMTT > VCR > WCR and increased when leaching occurred under artificial sunlight. sunlight also led to the formation of 23 transformation processes related to 1,3-diphenylguanidine (DPG). In contrast, 4-hydroxydiphenylamine (4-HDPA) and N-(1,3-dimethylbutyl)-N′-phenyl-p-phenylenediamine quinone (6-PPDQ) were found in lower amounts upon sunlight exposure. The 19 quantified chemicals, however, did only account for 6%–55% of the DOC in the leachates; most of the DOC, thus, remained unexplained. This study highlights that the amount of chemicals leached from tire particles depends upon their aging history and may be modulated by environmental conditions.
2023
Response of Total Column Ozone at High Latitudes to Sudden Stratospheric Warmings
The total column ozone (TCO) at northern high latitudes is increased over a course of 1–2 months after a major sudden stratospheric warming as a consequence of enhanced ozone eddy transport and diffusive ozone fluxes. We analyzed ground-based measurements of TCO from Oslo, Andøya and Ny Ålesund from 2000 to 2020. During this time interval, 15 major sudden stratospheric warmings (SSWs) occurred. The observed TCO variations are in a good agreement with those of ECMWF Reanalysis v5 (ERA5), showing that TCO from ERA5 is reliable, even during dynamically active periods. ERA5 has the advantage that it has no data gaps during the polar night. We found that TCO was increased by up to 190 DU after the SSW of February 2010, over one month. The composite analysis of the 15 SSWs provided the result that TCO is increased on average by about 50 DU over one month after the central date of the SSW.
2023
There is concern over possible effects on ecosystems and humans from exposure to persistent organic pollutants (POPs) and chemicals with similar properties. The main objective of this study was to develop, evaluate, and apply the Nested Exposure Model (NEM) designed to simulate the link between global emissions and resulting ecosystem exposure while accounting for variation in time and space. NEM, using environmental and biological data, global emissions, and physicochemical properties as input, was used to estimate PCB-153 concentrations in seawater and biota of the Norwegian marine environment from 1930 to 2020. These concentrations were compared to measured concentrations in (i) seawater, (ii) an Arctic marine food web comprising zooplankton, fish and marine mammals, and (iii) Atlantic herring (Clupea harengus) and Atlantic cod (Gadus morhua) from large baseline studies and monitoring programs. NEM reproduced PCB-153 concentrations in seawater, the Arctic food web, and Norwegian fish within a factor of 0.1–31, 0.14–3.1, and 0.09–21, respectively. The model also successfully reproduced measured trophic magnification factors for PCB-153 at Svalbard as well as geographical variations in PCB-153 burden in Atlantic cod between the Skagerrak, North Sea, Norwegian Sea, and Barents Sea, but estimated a steeper decline in PCB-153 concentration in herring and cod during the last decades than observed. Using the evaluated model with various emission scenarios showed the important contribution of European and global primary emissions for the PCB-153 load in fish from Norwegian marine offshore areas.
2023
The tropospheric NO2 column from Sentinel-5P/TROPOMI (2018–2020) and Aura/OMI (2010–2020) over Poland, notably for 7 major Polish cities, was used to assess the annual variability and the COVID-19 lockdown effect. On a national scale, during lockdown (March–June 2020), strong sources of pollution were found in Katowice and Warszawa, as well as at the power plant in Bełchatów. A gradual drop in OMI NO2 values between March and June was found for all cities and the entire domain of Poland, this being a part of the annual NO2 cycle derived for every year from 2010 to 2020. In fact, the gradual drop of NO2 in the lockdown year was within the typical monthly and annual variability. In March 2020, Kraków showed the highest NO2 reduction rate. A reduction of NO2 was observed in Gdańsk, Wrocław, and Warszawa during every month of the lock-down period. Several factors, including wind speed and direction, temperature, and increased emission sources, can limit the dispersion and removal of NO2. Although meteorological conditions have a significant impact on the annual cycle of NO2 in Poland, it is important to note that anthropogenic emissions remain the primary driver of NO2 concentrations. Therefore, the study concludes that the effect of COVID-19 restrictions on NO2 pollution was negligible and clarifies the current understanding of the COVID-19 effect over Poland, with an emphasis on hotspots in the major Polish cities and their vicinity. This is consistent with our understanding that the reduction of NO2 pollution is seen in cities due to reduced traffic (domestic, municipal, and airborne).
2023
Car tire rubber constitutes one of the largest fractions of microplastics emissions to the environment. The two main emission sources are tire wear particles (TWPs) formed through abrasion during driving and runoff of crumb rubber (CR) granulate produced from end-of-life tires that is used as infill on artificial sports fields. Both tire wear particles and crumb rubber contain a complex mixture of metal and organic chemical additives, and exposure to both the particulate forms and their leachates can cause adverse effects in aquatic species. An understanding of the exposure pathways and mechanisms of toxicity are, however, scarce. While the most abundant metals and organic chemicals in car tire rubber have multiple other applications, para-phenylenediamines (PDs) are primarily used as rubber antioxidants and were recently shown to cause negative effects in aquatic organisms. The present study investigated the responses of the marine lumpfish (Cyclopterus lumpus) to crumb rubber exposure in a controlled feeding experiment. Juvenile fish were offered crumb rubber particles with their feed for 1 week, followed by 2 weeks of depuration. Crumb rubber particle ingestion occurred in >75% of exposed individuals, with a maximum of 84 particles observed in one specimen. Gastrointestinal tract retention times varied, with some organisms having no crumb rubber particles and others still containing up to 33 crumb rubber particles at the end of the experiment. Blood samples were analyzed for metals and organic chemicals, with ICP-MS analysis revealing there was no uptake of metals by the exposed fish. Interestingly, high resolution GC-MS analysis indicated that uptake of PDs into lumpfish blood was proportionate to the number of ingested CR particles. Three of the PDs found in blood were the same as those identified in the additive mixture Vulkanox3100. N-(1,3-dimethylbutyl)-N′-phenyl-p-phenylenediamine (6PPD) was the most concentrated PD in both the crumb rubber and lumpfish blood. The transformation product 6PPD-quinone was detected in the rubber material, but not in the blood. This study demonstrates that PDs are specific and bioavailable chemicals in car tire rubber that have the potential to serve as biomarkers of recent exposure to tire chemicals, where simple blood samples could be used to assess recent tire chemical exposure in vertebrates, including humans.
2023
Volcanoes are known to be important emitters of atmospheric gases and aerosols, which for certain volcanoes can include halogen gases and in particular HBr. HBr emitted in this way can undergo rapid atmospheric oxidation chemistry (known as the bromine explosion) within the volcanic emission plume, leading to the production of bromine oxide (BrO) and ozone depletion. In this work, we present the results of a modelling study of a volcanic eruption from Mt Etna that occurred around Christmas 2018 and lasted 6 d. The aims of this study are to demonstrate and evaluate the ability of the regional 3D chemistry transport model Modèle de Chimie Atmosphérique de Grande Echelle (MOCAGE) to simulate the volcanic halogen chemistry in this case study, to analyse the variability of the chemical processes during the plume transport, and to quantify its impact on the composition of the troposphere at a regional scale over the Mediterranean basin.
The comparison of the tropospheric SO2 and BrO columns from 25 to 30 December 2018 from the MOCAGE simulation with the columns derived from the TROPOspheric Monitoring Instrument (TROPOMI) satellite measurements shows a very good agreement for the transport of the plume and a good consistency for the concentrations if considering the uncertainties in the flux estimates and the TROPOMI columns. The analysis of the bromine species' partitioning and of the associated chemical reaction rates provides a detailed picture of the simulated bromine chemistry throughout the diurnal cycle and at different stages of the volcanic plume's evolution. The partitioning of the bromine species is modulated by the time evolution of the emissions during the 6 d of the eruption; by the meteorological conditions; and by the distance of the plume from the vent, which is equivalent to the time since the emission. As the plume travels further from the vent, the halogen source gas HBr becomes depleted, BrO production in the plume becomes less efficient, and ozone depletion (proceeding via the Br+O3 reaction followed by the BrO self-reaction) decreases. The depletion of HBr relative to the other prevalent hydracid HCl leads to a shift in the relative concentrations of the Br− and Cl− ions, which in turn leads to reduced production of Br2 relative to BrCl.
The MOCAGE simulations show a regional impact of the volcanic eruption on the oxidants OH and O3 with a reduced burden of both gases that is caused by the chemistry in the volcanic plume. This reduction in atmospheric oxidation capacity results in a reduced CH4 burden. Finally, sensitivity tests on the composition of the emissions carried out in this work show that the production of BrO is higher when the volcanic emissions of sulfate aerosols are increased but occurs very slowly when no sulfate and Br radicals are assumed to be in the emissions. Both sensitivity tests highlight a significant impact on the oxidants in the troposphere at the regional scale of these assumptions.
All the results of this modelling study, in particular the rapid formation of BrO, which leads to a significant loss of tropospheric ozone, are consistent with previous studies carried out on the modelling of volcanic halogens.
2023