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A multi-pollutant and multi-sectorial approach to screening the consistency of emission inventories

Thunis, Philippe; Clappier, Alain; Pisoni, Enrico; Bessagnet, Bertrand; Kuenen, Jeroen; Guevara, Marc; Lopez-Aparicio, Susana

Some studies show that significant uncertainties affect emission inventories, which may impeach conclusions based on air-quality model results. These uncertainties result from the need to compile a wide variety of information to estimate an emission inventory. In this work, we propose and discuss a screening method to compare two emission inventories, with the overall goal of improving the quality of emission inventories by feeding back the results of the screening to inventory compilers who can check the inconsistencies found and, where applicable, resolve errors. The method targets three different aspects: (1) the total emissions assigned to a series of large geographical areas, countries in our application; (2) the way these country total emissions are shared in terms of sector of activity; and (3) the way inventories spatially distribute emissions from countries to smaller areas, cities in our application. The first step of the screening approach consists of sorting the data and keeping only emission contributions that are relevant enough. In a second step, the method identifies, among those significant differences, the most important ones that provide evidence of methodological divergence and/or errors that can be found and resolved in at least one of the inventories. The approach has been used to compare two versions of the CAMS-REG European-scale inventory over 150 cities in Europe for selected activity sectors. Among the 4500 screened pollutant sectors, about 450 were kept as relevant, among which 46 showed inconsistencies. The analysis indicated that these inconsistencies arose almost equally from large-scale reporting and spatial distribution differences. They mostly affect SO2 and PM coarse emissions from the industrial and residential sectors. The screening approach is general and can be used for other types of applications related to emission inventories.

2022

Rainwater Chemistry and Total Deposition of Acidity from the Northern Savanna to the Southern Coastal Fynbos of South Africa

Mompati, Mpho K.; Piketh, Stuart J.; Aas, Wenche; van Zyl, Pieter Gideon; Pienaar, Jacobus J.; Curtis, Christopher J.

South Africa is the largest national source of industrial atmospheric pollutants in Africa, and the emission of acid-forming pollutants occurs mainly in the eastern Highveld region of the country. However, spatial information on deposition is very sparse beyond the primary emissions zone. Here we quantify wet and dry deposition at four sites from the far northern savanna (Vaalwater) through the grasslands of the interior coal-producing belt of Mpumalanga (Elandsfontein) and the remote KwaZulu Natal Drakensberg mountains (Cathedral Peak) to the fynbos of the southern coast of the country (Knysna), a distance of over 1200 km. Rainwater samples were collected using automated wet-only samplers and analysed for mineral ions and water-soluble organic acids. Wet deposition fluxes were driven largely by rainfall amount rather than differences in chemical composition for three inland sites, with the highest wet deposited sulphur (S) (5.1 kgS/ha/year) and nitrogen (N) (6.9 kgN/ha/year) found in the Drakensberg mountains, greatly expanding the potentially harmful deposition footprint beyond the industrialised Highveld zone. Furthermore, the study period covered the extreme drought years of 2015–2016; hence, wet deposition fluxes could be significantly underestimated relative to more average rainfall years. Dry deposition fluxes, estimated using passive samplers and inferential methods, were far higher at the industrial Highveld site. Overall, total (wet + dry) deposition of S was greatest at the Highveld site (12.0 kgS/ha/year), but the greatest total N deposition (7.0 kgN/ha/year) was found at the remote Drakensberg site. Measured levels of both S and N deposition are well within the ranges found to cause acidification of soils and surface waters in northern hemisphere studies, or changes in vegetation species composition, and could be much higher in more typical, wetter years.

2022

Thallium Pollution in Europe Over the Twentieth Century Recorded in Alpine Ice: Contributions From Coal Burning and Cement Production

Legrand, Michel; McConnell, Joseph R.; Preunkert, Susanne; Bergametti, Gilles; Chellman, Nathan J; Desboeufs, Karine; Stohl, Andreas; Eckhardt, Sabine; Plach, Andreas

Emission inventories indicate that thallium, a highly toxic metal, is emitted during coal burning and cement production. These estimates have been established only for the 1980s and 1990s but up to now they have not been compared to long-term observations. Here we used alpine ice cores to document thallium pollution over Europe since ∼1850. Ice-core thallium concentrations increased from 1890 to 1910, and decreased after 1965 to concentrations that were half 1890 levels. Comparison of ice-core trends, estimated past emissions, and state-of-the-art atmospheric aerosol transport modeling suggest that coal burning was responsible for thallium pollution in Europe, particularly from 1920 to 1965 because of high coal consumption at that time. The subsequent decline resulted from decreased coal consumption and reduced emissions following technological improvements. The ice-core data suggest that the rapid growth of cement production that took place in Europe after 1950 had a limited impact on thallium pollution.

American Geophysical Union (AGU)

2022

Health impacts of PM2.5 originating from residential wood combustion in four nordic cities

Orru, Hans; Olstrup, Henrik; Kukkonen, Jaakko; Lopez-Aparicio, Susana; Segersson, David; Geels, Camilla; Tamm, Tanel; Riikonen, Kari; Maragkidou, Androniki; Sigsgaard, Torben; Brandt, Jørgen; Grythe, Henrik; Forsberg, Bertil

Residential wood combustion (RWC) is one of the largest sources of fine particles (PM2.5) in the Nordic cities. The current study aims to calculate the related health effects in four studied city areas in Sweden, Finland, Norway, and Denmark.

BioMed Central (BMC)

2022

Potential environmental impact of bromoform from Asparagopsis farming in Australia

Jia, Yue; Quack, Birgit; Kinley, Robert D.; Pisso, Ignacio; Tegtmeier, Susann

To mitigate the rumen enteric methane (CH4) produced by ruminant livestock, Asparagopsis taxiformis is proposed as an additive to ruminant feed. During the cultivation of Asparagopsis taxiformis in the sea or in terrestrially based systems, this macroalgae, like most seaweeds and phytoplankton, produces a large amount of bromoform (CHBr3), which contributes to ozone depletion once released into the atmosphere. In this study, we focus on the impact of CHBr3 on the stratospheric ozone layer resulting from potential emissions from proposed Asparagopsis cultivation in Australia. The impact is assessed by weighting the emissions of CHBr3 with its ozone depletion potential (ODP), which is traditionally defined for long-lived halocarbons but has also been applied to very short-lived substances (VSLSs). An annual yield of ∼3.5 × 104 Mg dry weight is required to meet the needs of 50 % of the beef feedlot and dairy cattle in Australia. Our study shows that the intensity and impact of CHBr3 emissions vary, depending on location and cultivation scenarios. Of the proposed locations, tropical farms near the Darwin region are associated with the largest CHBr3 ODP values. However, farming of Asparagopsis using either ocean or terrestrial cultivation systems at any of the proposed locations does not have the potential to significantly impact the ozone layer. Even if all Asparagopsis farming were performed in Darwin, the CHBr3 emitted into the atmosphere would amount to less than 0.02 % of the global ODP-weighted emissions. The impact of remaining farming scenarios is also relatively small even if the intended annual yield in Darwin is scaled by a factor of 30 to meet the global requirements, which will increase the global ODP-weighted emissions up to ∼0.5 %.

2022

Risk-benefit assessment of sunscreen: Opinion of the Panel on Food Additives, Flavourings, Processing Aids, Materials in Contact with Food, and Cosmetics of the Norwegian Scientific Committee for Food and Environment

Bruzell, Ellen Merete; Carlsen, Monica Hauger; Caspersen, Ida Henriette; Denison, Eva Marie-Louise; Devold, Tove Gulbrandsen; Granum, Berit; Mathisen, Gro Haarklou; Rundén-Pran, Elise; Rasinger, Josef; Rohloff, Jens; Svendsen, Camilla; Husøy, Trine

2022

Electrocatalytic performance of oxygen-activated carbon fibre felt anodes mediating degradation mechanism of acetaminophen in aqueous environments

Jakobczyk, Pawel; Skowierzak, Grzegorz; Kaczmarzyk, Iwona; Nadolska, Malgorzata; Wcislo, Anna; Lota, Katarzyna; Bogdanowicz, Robert; Ossowski, Tadeusz; Rostkowski, Pawel; Lota, Gregorz; Ryl, Jacek

Carbon felts are flexible and scalable, have high specific areas, and are highly conductive materials that fit the requirements for both anodes and cathodes in advanced electrocatalytic processes. Advanced oxidative modification processes (thermal, chemical, and plasma-chemical) were applied to carbon felt anodes to enhance their efficiency towards electro-oxidation. The modification of the porous anodes results in increased kinetics of acetaminophen degradation in aqueous environments. The utilised oxidation techniques deliver single-step, straightforward, eco-friendly, and stable physiochemical reformation of carbon felt surfaces. The modifications caused minor changes in both the specific surface area and total pore volume corresponding with the surface morphology.

A pristine carbon felt electrode was capable of decomposing up to 70% of the acetaminophen in a 240 min electrolysis process, while the oxygen-plasma treated electrode achieved a removal yield of 99.9% estimated utilising HPLC-UV-Vis. Here, the electro-induced incineration kinetics of acetaminophen resulted in a rate constant of 1.54 h−1, with the second-best result of 0.59 h−1 after oxidation in 30% H2O2. The kinetics of acetaminophen removal was synergistically studied by spectroscopic and electrochemical techniques, revealing various reaction pathways attributed to the formation of intermediate compounds such as p-aminophenol and others.

The enhancement of the electrochemical oxidation rates towards acetaminophen was attributed to the appearance of surface carbonyl species. Our results indicate that the best-performing plasma-chemical treated CFE follows a heterogeneous mechanism with only approx. 40% removal due to direct electro-oxidation. The degradation mechanism of acetaminophen at the treated carbon felt anodes was proposed based on the detected intermediate products. Estimation of the cost-effectiveness of removal processes, in terms of energy consumption, was also elaborated. Although the study was focussed on acetaminophen, the achieved results could be adapted to also process emerging, hazardous pollutant groups such as anti-inflammatory pharmaceuticals.

Pergamon Press

2022

Thymidine Kinase+/− Mammalian Cell Mutagenicity Assays for Assessment of Nanomaterials

Chen, Tao; Dusinska, Maria; Elespuru, Rosalie K.

The methods outlined here are part of a series of papers designed specifically for genotoxicity assessment of nanomaterials (NM). Common Considerations such as NM characterization, sample preparation and dose selection, relevant to all genotoxicity assays, are found in an accompanying paper. The present paper describes methods for evaluation of mutagenicity in the mammalian (mouse) thymidine kinase (Tk) gene occurring in L5178Y mouse lymphoma (ML) cells and in the designated TK gene in human lymphoblastoid TK6 cells. Mutations change the functional genotype from TK+/− to TK−/−, detectable as cells surviving on media selective for the lack of thymidine kinase (TK) function. Unlike cells with TK enzyme function, the TK−/− cells are unable to integrate the toxic selection agent, allowing these cells to survive as rare mutant colonies. The ML assay has been shown to detect a broad spectrum of genetic damage, including both small scale (point) mutations and chromosomal alterations. This assay is a widely used mammalian cell gene mutation assay for regulatory purposes and is included in the core battery of genotoxicity tests for regulatory decision-making. The TK6 assay is an assay using a human cell line derived similarly via mutagenic manipulations and optimal selection. Details are provided on the materials required, cell culture methods, selection of test chemical concentrations, cytotoxicity, treatment time, mutation expression, cloning, and data calculation and interpretation. The methods describe the microwell plate version of the assays without metabolic activation.

Frontiers Media S.A.

2022

Common Considerations for Genotoxicity Assessment of Nanomaterials

Elespuru, Rosalie K.; Doak, Shareen H.; Collins, Andrew Richard; Dusinska, Maria; Pfuhler, Stefan; Manjanatha, Mugimane; Cardoso, Renato M.S.; Chen, Connie L.

Genotoxicity testing is performed to determine potential hazard of a chemical or agent for direct or indirect DNA interaction. Testing may be a surrogate for assessment of heritable genetic risk or carcinogenic risk. Testing of nanomaterials (NM) for hazard identification is generally understood to require a departure from normal testing procedures found in international standards and guidelines. A critique of the genotoxicity literature in Elespuru et al., 2018, reinforced evidence of problems with genotoxicity assessment of nanomaterials (NM) noted by many previously. A follow-up to the critique of problems (what is wrong) is a series of methods papers in this journal designed to provide practical information on what is appropriate (right) in the performance of genotoxicity assays altered for NM assessment. In this “Common Considerations” paper, general considerations are addressed, including NM characterization, sample preparation, dosing choice, exposure assessment (uptake) and data analysis that are applicable to any NM genotoxicity assessment. Recommended methods for specific assays are presented in a series of additional papers in this special issue of the journal devoted to toxicology methods for assessment of nanomaterials: the In vitro Micronucleus Assay, TK Mutagenicity assays, and the In vivo Comet Assay. In this context, NM are considered generally as insoluble particles or test articles in the nanometer size range that present difficulties in assessment using techniques described in standards such as OECD guidelines.

Frontiers Media S.A.

2022

Ecosystem specific accumulation of organohalogenated compounds: A comparison between adjacent freshwater and terrestrial avian predators

Bustnes, Jan Ove; Bårdsen, Bård-Jørgen; Herzke, Dorte; Bangjord, Georg; Bourgeon, Sophie; Fritsch, Clémentine; Eulaers, Igor

Insight into processes determining the exposure of organohalogenated contaminants (OHCs) in wildlife might be gained from comparing predators in different ecosystems. This study compared two avian predator species with similar food chain lengths: the goldeneye duck (Bucephala clangula) and the tawny owl (Strix aluco) breeding in adjacent freshwater- and terrestrial ecosystems in central Norway. We measured lipophilic organochlorines (OCs) and protein-bound perfluorinated substances (PFASs) in eggs of the two species over 21 years (1999–2019). Across years, the proportional distribution of OCs (∼90% of the ΣOHC load) relative to PFASs (∼10%) was similar in the two species. Moreover, ΣOC concentrations were similar between the species, but PFAS compounds were 2–12 times higher in the goldeneyes than in tawny owls. OC-pesticides dominated in tawny owls (∼60% of ΣOC), whereas persistent polychlorinated biphenyl (PCBs) congeners were the main OC components in goldeneyes (∼70% of ΣOC). The lipid-normalized concentrations of most OC-pesticides and the less persistent PCB101 declined significantly in both species. Hexachlorobenzene (HCB), p,p’-dichlorodiphenyldichloroethylene (p,p’-DDE), and more persistent PCBs decreased in tawny owls, while they tended to increase in goldeneyes. The increase in HCB was particulary robust. Among the PFASs, contrasted temporal trends were found across the species for four out of 11 compounds: PFOS declined while most perfluorocarboxylic acids (PFCAs) increased in tawny owls. In contrast, most PFASs were stable in goldeneyes. Moreover, there was no annual covariance between the OHC exposure in the two species: i.e., high concentrations in one species in a given year did not translate into high concentrations in the other. Hence, the two avian predators in adjacent ecosystems seem to be subject to different processes determining the OHC exposure, probably related to variation in diet and climate, long-range transport of different contaminants, and emissions of pollution locally.

Elsevier

2022

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