Influence of climate change on Persistent Organic Pollutants and Chemicals of Emerging Concern in the Arctic: State of knowledge and recommendations for future research.

de Wit, C.A.; Vorkamp, K.; Muir, D.
2022 | Environ. Sci.: Processes Impacts

Airborne and marine microplastics from an oceanographic survey at the Baltic Sea: an emerging role of air-sea interaction?

Luca Ferrero; Lorenzo Scibetta; Piotr Markuszewski; Mikolaj Mazurkiewic; Violetta Drozdowska; Przemyslaw Makuch; Patrycja Jutzenka-Trzbiatowska; Adriana Zaleska-Medynska; Sergio Ando; Franscesco Seliu; ; E. Douglas Nilsson; Ezio Bolzacchini
2022 | Sci. Total Environ. | 824 (153709) (1-16)
air-sea interaction , atmosphere , baltic salmon , Microplastic , sea

Microplastics (MPs) pollution is one of the most important problems of the Earth. They have been found in all the natural
environments, including oceans and the atmosphere. In this study, the concentrations of both atmospheric and
marine MPs were measured over the Baltic along a research cruise that started in the Gdansk harbour, till the Gotland
island, and the way back. A deposition box (based on a combination of active/passive sampling) was used to collect
airborne MPs while, marine MPs concentrations were investigated during the cruise using a dedicated net. Ancillary
data were obtained using a combination of particle counters (OPC, LAS and CPC), Aethalometer (AE33 Magee Scientific),
spectrofluorometer (sea surface samples, Varian Cary Eclipse), and meteorological sensors. Results showed airborne
microplastics average concentrations higher in the Gdansk harbour (161 ± 75 m−3) compared to the open
Baltic Sea and to the Gotland island (24± 9 and 45 ±20 m−3). These latter values are closer to the ones measured
in the sea (79±18m−3). The MPs composition was investigated using μ-Raman (for the airborne ones) and FTIR (for marine ones); similar results (e.g. polyethylene, polyethylene terephthalates, polyurethane) were found in the two environmental

<compartments. The concentrations and sd<dimilar composition in air and sea suggested a linkag e between
the two compartments. For this purpose, the atmospheric MPs' equivalent aerodynamic diameter was calculated (28
±3μm) first showing the capability of atmospheric MPs to remain suspended in the air. At the same time, the computed
turnover times (0.3–90 h; depending on MPs size) limited the transport distance range. The estimated M-^Ps sea emission fluxes (4–18 ∗ 10^-6 μm^3 m−2 s−1 range) finally showed the contemporary presence of atmospheric transport
together with a continuous emission fromthe sea surface enabling a grasshopper long-range transport ofmicroplastics
across the sea.

Sediment Remediation Using Activated Carbon: Effects of Sorbent Particle Size and Resuspension on Sequestration of Metals and Organic Contaminants

Rämö, Robert; Bonaglia, Stefano; Nybom, Inna; Kreutzer, Anne; Witt, Gesine; Sobek, Anna; Gunnarsson, Jonas, S.
2022 | Environ. Toxicol. Chem. (1-15)

Outside the safe operating space of the planetary boundary for novel entities.

Persson, L.; Carney Almroth, B.; Collins, C.; Cornell, S.E.; de Wit, C.A.; Diamond, M.L.; Fantke, P.; Hassellöv, M.; MacLeod, M.; Ryberg, M.; Søgaard Jørgensen, P.; Villarrubia-Gómez, P.; Wang, Z.; Hauschild, M.Z.
2022 | Environ. Sci. Technol. | 56 (1510-1521)

Combined Use of Total Fluorine and Oxidative Fingerprinting for Quantitative Determination of Side-Chain Fluorinated Polymers in Textiles

Liagkouridis, I.; Awad, R.; Schellenberger, S.; Plassmann, M.M.; Cousins, I.T.; Benskin, J.P.
2022 | Environ. Sci. Technol. Lett. | 9 (1) (30-36)

Detection of Benzo[a]pyrene Diol Epoxide Adducts to Histidine and Lysine in Serum Albumin In Vivo by High-Resolution-Tandem Mass Spectrometry

Zurita, J; Motwani, HV; Ilag, LL; Souliotis, VL; Kyrtopoulos, SA; Nilsson, U; Törnqvist, M
2022 | Toxics | 10 (1)

Correction to Fate of Springtime Atmospheric Reactive Mercury: Concentrations and Deposition at Zeppelin, Svalbard

Stefan Osterwalder; Sarrah M. Dunham-Cheatham; Beatriz Ferreira Araujo; Olivier Magand; Jennie L. Thomas; Foteini Baladima; Katrine Aspmo Pfaffhuber; Torunn Berg; Lei Zhang; Jiaoyan Huang; Paul Zieger; Aurélien Dommergue; Jeroen E. Sonke; Mae Sexauer Gustin

Development, validation, and application of a new method for the quantitative determination of monohydrogen-substituted perfluoroalkyl carboxylic acids (H-PFCAs) in surface water

Awchi, M; Gebbink, WA; Berendsen, BJA; Benskin, JP; van Leeuwen, SPJ
2022 | Chemosphere | 287
h-pfcas , lc-ms , line , ms , pfas , pfcas , samples , substances , surface water , suspect
Per- and polyfluoroalkyl substances (PFASs) are a large and diverse class of chemicals. While some have been phased out internationally due to concerns over their human and environmental health risks, novel alternative PFASs continue to be manufactured and detected in environmental samples. The occurrence and fate of these alternatives remain poorly understood. The present study investigated the occurrence of an emerging class of PFAS alternative, the monohydrogen-substituted perfluoroalkyl carboxylic acids (H-PFCAs), in conjunction with the more well-known PFCAs. A weak anion exchange solid phase extraction-liquid chromatography tandem mass spectrometry method for quantitative determination of H-PFCAs in surface water was developed, validated, and applied on samples collected from the Netherlands. To improve chromatography, especially for short-chain (H-) PFCAs, an ion-pairing agent, tetrabutylammonium hydrogen sulphate, was used. The method was validated for linearity (R2 > 0.99), instrumental detection limits (0.01-0.09 ng/mL), method detection limits (0.03-0.75 ng/ mL), matrix effects (<20%), percent absolute- and relative recovery (57-121%), trueness (130-80%), repeatability (<20%), and within-lab reproducibility (<20%). Eleven out of fourteen PFASs showed acceptable results. Application of the newly validated method to surface water throughout the Netherlands revealed trace levels of H-PFCAs (including two new H-PFCAs) and high concentrations of PFCAs.

Highly time-resolved chemical speciation and source apportionment of organic aerosol components in Delhi, India, using extractive electrospray ionization mass spectrometry

Kumar, V; Giannoukos, S; Haslett, SL; Tong, YD; Singh, A; Bertrand, A; Lee, CP; Wang, DS; Bhattu, D; Stefenelli, G; Dave, JS; Puthussery, JV; Qi, L; Vats, P; Rai, P; Casotto, R; Satish, R; Mishra, S; Pospisilova, V; Mohr, C; Bell, DM; Ganguly, D; Verma, V; Rastogi, N; Baltensperger, U; Tripathi, SN; Prevot, ASH; Slowik, JG
2022 | Atmos. Chem. Phys. | 22 (11) (7739-7761)
air pollution , aromatic-hydrocarbons , eesi-tof-ms , high-resolution , multilinear engine , particle composition , positive matrix factorization , road emission characteristics , urban , volatility
In recent years, the Indian capital city of Delhi has been impacted by very high levels of air pollution, especially during winter. Comprehensive knowledge of the composition and sources of the organic aerosol (OA), which constitutes a substantial fraction of total particulate mass (PM) in Delhi, is central to formulating effective public health policies. Previous source apportionment studies in Delhi identified key sources of primary OA (POA) and showed that secondary OA (SOA) played a major role but were unable to resolve specific SOA sources. We address the latter through the first field deployment of an extractive electrospray ionization timeof-flight mass spectrometer (EESI-TOF) in Delhi, together with a high-resolution aerosol mass spectrometer (AMS). Measurements were conducted during the winter of 2018/19, and positive matrix factorization (PMF) was used separately on AMS and EESI-TOF datasets to apportion the sources of OA. AMS PMF analysis yielded three primary and two secondary factors which were attributed to hydrocarbon-like OA (HOA), biomass burning OA (BBOA-1 and BBOA-2), more oxidized oxygenated OA (M0-00A), and less oxidized oxygenated OA (LO-OOA). On average, 40 % of the total OA mass was apportioned to the secondary factors. The SOA contribution to total OA mass varied greatly between the daytime (76.8 %, 10:00-16:00 local time (LT)) and nighttime (31.0 %, 21:00-04:00 LT). The higher chemical resolution of EESI-TOF data allowed identification of individual SOA sources. The EESI-TOF PMF analysis in total yielded six factors, two of which were primary factors (primary biomass burning and cooking-related OA). The remaining four factors were predominantly of secondary origin: aromatic SOA, biogenic SOA, aged biomass burning SOA, and mixed urban SOA. Due to the uncertainties in the EESI-TOF ion sensitivities, mass concentrations of EESI-TOF SOA-dominated factors were related to the total AMS SOA (i.e. MO-00A + LO-00A) by multiple linear regression (MLR). Aromatic SOA was the major SOA component during the daytime, with a 55.2 % contribution to total SOA mass (42.4 % contribution to total OA). Its contribution to total SOA, however, decreased to 25.4 % (7.9 % of total OA) during the nighttime. This factor was attributed to the oxidation of light aromatic compounds emitted mostly from traffic. Biogenic SOA accounted for 18.4 % of total SOA mass (14.2 % of total OA) during the daytime and 36.1 % of total SOA mass (11.2 % of total OA) during the nighttime. Aged biomass burning and mixed urban SOA accounted for 15.2 % and 11.0 % of total SOA mass (11.7 % and 8.5 % of total OA mass), respectively, during the daytime and 15.4 % and 22.9 % of total SOA mass (4.8 % and 7.1 % of total OA mass), respectively, during the nighttime. A simple dilution-partitioning model was applied on all EESI-TOF factors to estimate the fraction of observed daytime concentrations resulting from local photochemical production (SOA) or emissions (POA). Aromatic SOA, aged biomass burning, and mixed urban SOA were all found to be dominated by local photochemical production, likely from the oxidation of locally emitted volatile organic compounds (VOCs). In contrast, biogenic SOA was related to the oxidation of diffuse regional emissions of isoprene and monoterpenes. The findings of this study show that in Delhi, the nighttime high concentrations are caused by POA emissions led by traffic and biomass burning and the daytime OA is dominated by SOA, with aromatic SOA accounting for the largest fraction. Because aromatic SOA is possibly more toxic than biogenic SOA and primary OA, its dominance during the daytime suggests an increased OA toxicity and health-related consequences for the general public.

Nontarget mass spectrometry and in silico molecular characterization of air pollution from the Indian subcontinent

Papazian, S; D'Agostino, LA; Sadiktsis, I; Froment, J; Bonnefille, B; Sdougkou, K; Xie, HY; Athanassiadis, I; Budhavant, K; Dasari, S; Andersson, A; Gustafsson, O; Martin, JW
2022 | Commun. Earth Environ. | 3 (1)
ambient , brown carbon , chemistry , dark-matter , diversity , evolution , organic aerosol , particulate matter , transport , variability
A combination of high-resolution mass spectrometry and computational molecular characterization techniques can structurally annotate up to 17% of organic compounds in fine particulate matter in highly polluted air sampled in the Maldives. Fine particulate-matter is an important component of air pollution that impacts health and climate, and which delivers anthropogenic contaminants to remote global regions. The complex composition of organic molecules in atmospheric particulates is poorly constrained, but has important implications for understanding pollutant sources, climate-aerosol interactions, and health risks of air pollution exposure. Here, comprehensive nontarget high-resolution mass spectrometry was combined with in silico structural prediction to achieve greater molecular-level insight for fine particulate samples (n = 40) collected at a remote receptor site in the Maldives during January to April 2018. Spectral database matching identified 0.5% of 60,030 molecular features observed, while a conservative computational workflow enabled structural annotation of 17% of organic structures among the remaining molecular dark matter. Compared to clean air from the southern Indian Ocean, molecular structures from highly-polluted regions were dominated by organic nitrogen compounds, many with computed physicochemical properties of high toxicological and climate relevance. We conclude that combining nontarget analysis with computational mass spectrometry can advance molecular-level understanding of the sources and impacts of polluted air.

Kinetics, SOA yields, and chemical composition of seconaary organic aerosol from beta-caryophyllene ozonolysis with and without nitrogen oxides between 213 and 313 K

Gao, LY; Song, JW; Mohr, C; Huang, W; Vallon, M; Jiang, F; Leisner, T; Saathoff, H
2022 | Atmos. Chem. Phys. | 22 (9) (6001-6020)
oxidation , sesquiterpene emissions
beta-caryophyllene (BCP) is one of the most important sesquiterpenes (SQTs) in the atmosphere, with a large potential contribution to secondary organic aerosol (SOA) formation mainly from reactions with ozone (O-3) and nitrate radicals (NO3). In this work, we study the temperature dependence of the kinetics of BCP ozonolysis, SOA yields, and SOA chemical composition in the dark and in the absence and presence of nitrogen oxides including nitrate radicals (NO3). We cover a temperature range of 213-313 K, representative of tropospheric conditions. The oxidized components in both gas and particle phases were characterized on a molecular level by a chemical ionization mass spectrometer equipped with a filter inlet for gases and aerosols using iodide as the reagent ion (FIGAERO-iodide-CIMS). The batch mode experiments were conducted in the 84.5 m(3) aluminium simulation chamber AIDA at the Karlsruhe Institute of Technology (KIT). In the absence of nitrogen oxides, the temperature-dependent rate coefficient of the endocyclic double bond in BCP reacting with ozone between 243-313 K is negatively correlated with temperature, corresponding to the following Arrhenius equation: k = (1.6 +/- 0.4) x 10(-15) x exp((559 +/- 97)/ T). The SOA yields increase from 16 +/- 5 % to 37 +/- 11 %, with temperatures decreasing from 313 to 243 K at a total organic particle mass of 10 mu g m(-3). The variation in the ozonolysis temperature leads to a substantial impact on the abundance of individual organic molecules. In the absence of nitrogen oxides, monomers C14-15H22-24O3-7 (37.4 %), dimers C28-30H44-48O5-9 (53.7 %), and timers C41_44H62_6609_11 (8.6 %) are abundant in the particle phase at 213 K. At 313 K, we observed more oxidized monomers (mainly C14-15H22-24O6-9, 67.5 %) and dimers (mainly C27-29H42-44O9-11, 27.6 %), including highly oxidized molecules (HOMs; C14H22O7,9C15H22O7,9C15H24O7,9), which can be formed via hydrogen shift mechanisms, but no significant timers. In the presence of nitrogen oxides, the organonitrate fraction increased from 3 % at 213 K to 12 % and 49 % at 243 and 313 K, respectively. Most of the organonitrates were monomers with Cis skeletons and only one nitrate group. More highly oxygenated organonitrates were observed at higher temperatures, with their signal-weighted O : C atomic ratio increasing from 0.41 to 0.51 from 213 to 313 K. New dimeric and timeric organic species without nitrogen atoms (C-20, C-35) were formed in the presence of nitrogen oxides at 298-313 K, indicating potential new reaction pathways. Overall, our results show that increasing temperatures lead to a relatively small decrease in the rate coefficient of the endocyclic double bond in BCP reacting with ozone but to a strong decrease in SOA yields. In contrast, the formation of HOMs and organonitrates increases significantly with temperature.

Contact information

Visiting addresses:

Geovetenskapens Hus,
Svante Arrhenius väg 8, Stockholm

Arrheniuslaboratoriet, Svante Arrhenius väg 16, Stockholm (Unit for Toxicological Chemistry)

Mailing address:
Department of Environmental Science
Stockholm University
106 91 Stockholm

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Stella Papadopoulou
Science Communicator
Phone +46 (0)8 674 70 11