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  • 1.
    Castro, Mafalda
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Chlorinated Paraffins: improved understanding of their bioaccumulation and toxicity in Daphnia magna2020Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    Chlorinated paraffins (CPs) are industrial chemicals, mainly used as flame retardants, plasticizers and metal cutting fluids. Their production has reached historically high levels in the last decade, with an annual production exceeding one million tonnes. In 2017, short chain chlorinated paraffins (SCCPs) were regulated due to their Persistent, Bioaccumulative and Toxic (PBT) properties, while medium and long chain chlorinated paraffins (MC and LCCPs) were suggested as alternatives. The high hydrophobicity of CPs, which complicates bioaccumulation and aquatic toxicity testing, has hindered proper hazard identification by regulatory authorities. This project was initiated in response to the insufficient understanding of bioaccumulative and toxicological properties of these chemicals, which have even surpassed the environmental levels of legacy Persistent Organic Pollutants (POPs) in certain regions.

    The research presented in this thesis, contributes to filling these knowledge gaps by adapting methods for reliable bioaccumulation and aquatic toxicity assessment. In Paper I, passive dosing, traditionally used for other highly hydrophobic compounds, was adapted and validated for CPs. SC, MC and LCCPs partitioned from silicone into water and, when the crustacean Daphnia magna was introduced into the test system, the CPs were observed to be effectively taken up by the test organism. This passive-dosing approach was further used in Paper II, to investigate the bioconcentration and bioaccumulation potential in D. magna. All tested CPs were found to bioaccumulate in daphnids, including highly hydrophobic, long chained CP congeners. The two most bioaccumulative CPs in Paper II (CP-52 and Huels70C) were thereafter used in a chronic toxicity study (Paper III) and significantly decreased population growth and disrupted fatty acid metabolism of D. magna. Finally, in Paper IV, liposome-mediated delivery of chemicals to aquatic biota was adapted for the first time for organic contaminants, including CPs. This approach yielded stable body burdens of the tested chemicals in D. magna and allowed for kinetic and toxicity assessments.

    Overall, two alternative bioaccumulation and aquatic toxicity testing methods were successfully adapted for technically challenging (industrial) chemicals. These methods allowed the determination of endpoints of scientific and regulatory interest, such as the high bioaccumulation and toxicity potential of CPs, but were also used to demonstrate their metabolic disruption potential in small crustaceans. 

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  • 2.
    Castro, Mafalda
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Gorokhova, Elena
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Yuan, Bo
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Lücke-Johansson, Sandra
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Sobek, Anna
    Breitholtz, Magnus
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Chlorinated paraffins alter fatty acid metabolism and life histories in DaphniaManuscript (preprint) (Other academic)
  • 3.
    Castro, Mafalda
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Lindqvist, Dennis
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Liposome-mediated delivery of challenging chemicals to aid environmental assessment of Bioaccumulative (B) and Toxic (T) propertiesManuscript (preprint) (Other academic)
  • 4.
    Coll Mora, Claudia
    Stockholm University, Faculty of Science, Department of Environmental Science.
    How to estimate environmental persistence: Understanding persistence of organic micropollutants in rivers from a multidisciplinary perspective2020Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    Organic micropollutants such as food additives, pharmaceuticals and personal care products are found in rivers worldwide. Persistence is a key criteria in chemical risk assessment as micropollutants that are persistent pose an exposure hazard to humans and the environment. As biodegradation is the most relevant removal process for many micropollutants in rivers, persistence assessment relies on the estimation of the biodegradation half-life.  This thesis presents new approaches to understand the biodegradation of organic pollutants in rivers.

    The application of Junge relationships (previously established for atmospheric pollutants), to river systems, was investigated in paper I to assess if biodegradation half-lives in the Danube river are correlated with variability in measured concentrations. Model scenarios show Junge relationships could potentially be found in measurements performed near the mouth of the river, but Junge relationships were not found in currently available monitoring data. In paper II an experimental design and response surface model were developed to study the effect of hyporheic exchange (induced by flowing water) and bacterial diversity in sediment on dissipation half-lives of two micropollutants in flumes. Faster dissipation was observed in flumes with high bacterial diversity and higher hyporheic exchange, and thus both variables are relevant to study dissipation processes in rivers. The influence of biological factors beyond bacteria diversity is explored in papers III and IV, by characterizing the bacteria community composition of sediment in OECD 308 bottle incubations (a standard test that is often recommended in risk assessment guidelines). In paper III, higher variation in half-lives (e.g. relative standard deviations > 50%) were found for micropollutants with longer half-lives (e.g. from 40 to more than 120 days). Higher variation in half-lives also corresponded to differences in bacteria community composition and specifically to increased or decreased abundance of certain bacteria genera. Although the exact bacteria genera involved in the biodegradation of the micropollutants cannot be determined in papers II or III, our results suggest bacteria community composition and diversity should be considered in the interpretation of biodegradation half-lives since they are related to variability in biodegradation and to understand extrapolation from laboratory to the field. Finally in paper IV, it is investigated if the bacteria communities are affected by the OECD 308 test conditions. Changes in the bacteria communities in the sediment between the initial river community, the beginning and the end of the incubation, at high and a low concentrations are reported. Overall, 8% of bacteria genera increased or decreased in relative abundance in all comparisons, and it is unclear if these small changes in bacteria communities could have had an effect on the observed half-lives in paper III.

    This thesis contributes to the understanding of physical and biological factors influencing biodegradation and potential implications for risk assessment of organic micropollutants in rivers.

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  • 5. Du, Xinyu
    et al.
    Yuan, Bo
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Zhou, Yihui
    de Wit, Cynthia A.
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Zheng, Ziye
    Yin, Ge
    Chlorinated Paraffins in Two Snake Species from the Yangtze River Delta: Tissue Distribution and Biomagnification2020In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 54, no 5, p. 2753-2762Article in journal (Refereed)
    Abstract [en]

    Very-short, short-, medium-, and long-chain chlorinated paraffins (vSCCPs, SCCPs, MCCPs, and LCCPs, respectively) were analyzed in different tissues of the terrestrial short-tailed mamushi (Gloydius brevicaudus) and the semi-aquatic red-backed rat snake (Elaphe rufodorsata) from the Yangtze River Delta, China. The total CP concentrations in liver, muscle, and adipose tissues in the two snake species were in the range of 2500-24 000, 4900-48 000, and 12-630 ng/g lw, respectively. Tissue burdens indicated that vSCCPs (C6-9) and SCCPs (C10-3) preferentially distributed to snake liver, while adipose was an important storage site and sink of MCCPs (C14-17) and LCCPs (C->18). On a lipid weight basis, vSCCPs and SCCPs were found in highest concentrations in red-backed rat snake liver and MCCPs and LCCPs in muscle, whereas for short-tailed mamushi, all CP groups were predominant in muscle, probably reflecting ecosystem/food web differences. Moreover, vSCCPs, SCCPs, MCCPs, and LCCPs were found to be biomagnified from black-spotted frogs to red-backed rat snakes with mean (maximum) biomagnification factors of 2.2 (3.4), 1.9 (3.7), 1.8 (2.8), and 1.7 (4.5), respectively. This is the first field study of biomagnification potential involving vSCCPs and LCCPs and highlights the need to include all CPs in studies.

  • 6. Li, Li
    et al.
    Qiu, Yanling
    Gustafsson, Asa
    Krais, Annette M.
    Weiss, Jana M.
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Lundh, Thomas
    Bergman, Åke
    Stockholm University, Faculty of Science, Department of Environmental Science. Tongji University, China; Örebro University, Sweden.
    Characterization of residential household dust from Shanghai by particle size and analysis of organophosphorus flame retardants and metals2019In: Environmental Sciences Europe, ISSN 2190-4707, E-ISSN 2190-4715, Vol. 31, no 1, article id 94Article in journal (Refereed)
    Abstract [en]

    Background Physical and biological properties of dust particles might affect the availability and distribution of chemicals associated to indoor dust; however it has not been adequately examined. In this study, household dust from Shanghai was fractionated into five particle sizes and size distribution, morphology, surface area, organic matter, microorganisms, elemental composition, metals and organophosphorus flame retardants (OPFRs) compositions were characterized. Also, household dust samples from Stockholm that has previously been characterized were included in the analysis of OPFRs for comparison. Results The respirable fraction had a yield of 3.3% in mass percentage, with a particle size of 2.22 +/- 2.04 mu m. As expected, both metals and OPFRs concentrations increased with decreased particle size. Al and Fe dominated (66-87%) followed by the concentrations of Zn (5-14%) and Ga (1.8-5%) of the sum of 16 metals in the dust. The concentrations of OPFRs in Shanghai dust ranged from 5.34 to 13.7 mu g/g (median: 7.21 mu g/g), compared to household dust from Stockholm that ranged from 16.0 to 28.3 mu g/g (median: 26.6 mu g/g). Tris(2-chloroisopropyl) phosphate (TCIPP) and tris(2-chloroethyl) phosphate (TCEP) dominated in Shanghai dust samples while tris(2-butoxyethyl) phosphate (TBOEP) dominated in dust from Stockholm homes. Conclusion The results showed that mass percentage for each particle size fraction was not evenly distributed. Furthermore, the particle-bound microorganisms and OPFRs increased with decreased particle size, whereas metals had the highest concentrations at specific dust sizes. Therefore, it is essential to select the proper particle size in order to assess any specific human exposure study to indoor pollutants.

  • 7.
    McGivney, Eric
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Cederholm, Linnea
    Barth, Andreas
    Stockholm University, Faculty of Science, Department of Biochemistry and Biophysics.
    Hakkarainen, Minna
    Hamacher-Barth, Evelyne
    Stockholm University, Faculty of Science, Department of Biochemistry and Biophysics.
    Ogonowski, Martin
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Gorokhova, Elena
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Rapid Physicochemical Changes in Microplastic Induced by Biofilm Formation2020In: Frontiers in Bioengineering and Biotechnology, E-ISSN 2296-4185, Vol. 8, article id 205Article in journal (Refereed)
    Abstract [en]

    Risk assessment of microplastic (MP) pollution requires understanding biodegradation processes and related changes in polymer properties. In the environment, there are two-way interactions between the MP properties and biofilm communities: (i) microorganisms may prefer some surfaces, and (ii) MP surface properties change during the colonization and weathering. In a 2-week experiment, we studied these interactions using three model plastic beads (polyethylene [PE], polypropylene [PP], and polystyrene [PS]) exposed to ambient bacterioplankton assemblage from the Baltic Sea; the control beads were exposed to bacteria-free water. For each polymer, the physicochemical properties (compression, crystallinity, surface chemistry, hydrophobicity, and surface topography) were compared before and after exposure under controlled laboratory conditions. Furthermore, we characterized the bacterial communities on the MP surfaces using 16S rRNA gene sequencing and correlated community diversity to the physicochemical properties of the MP. Significant changes in PE crystallinity, PP stiffness, and PS maximum compression were observed as a result of exposure to bacteria. Moreover, there were significant correlations between bacterial diversity and some physicochemical characteristics (crystallinity, stiffness, and surface roughness). These changes coincided with variation in the relative abundance of unique OTUs, mostly related to the PE samples having significantly higher contribution of Sphingobium, Novosphingobium, and uncultured Planctomycetaceae compared to the other test materials, whereas PP and PS samples had significantly higher abundance of Sphingobacteriales and Alphaproteobacteria, indicating possible involvement of these taxa in the initial biodegradation steps. Our findings demonstrate measurable signs of MP weathering under short-term exposure to environmentally relevant microbial communities at conditions resembling those in the water column. A systematic approach for the characterization of the biodegrading capacity in different systems will improve the risk assessment of plastic litter in aquatic environments.

  • 8. Pospisilova, V
    et al.
    Lopez-Hilfiker, F. D.
    Bell, D. M.
    El Haddad, I
    Mohr, Claudia
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Huang, W.
    Heikkinen, L.
    Xiao, M.
    Dommen, J.
    Prevot, A. S. H.
    Baltensperger, U.
    Slowik, J. G.
    On the fate of oxygenated organic molecules in atmospheric aerosol particles2020In: Science Advances, E-ISSN 2375-2548, Vol. 6, no 11, article id eaax8922Article in journal (Refereed)
    Abstract [en]

    Highly oxygenated organic molecules (HOMs) are formed from the oxidation of biogenic and anthropogenic gases and affect Earth's climate and air quality by their key role in particle formation and growth. While the formation of these molecules in the gas phase has been extensively studied, the complexity of organic aerosol (OA) and lack of suitable measurement techniques have hindered the investigation of their fate post-condensation, although further reactions have been proposed. We report here novel real-time measurements of these species in the particle phase, achieved using our recently developed extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF). Our results reveal that condensed-phase reactions rapidly alter OA composition and the contribution of HOMs to the particle mass. In consequence, the atmospheric fate of HOMs cannot be described solely in terms of volatility, but particle-phase reactions must be considered to describe HOM effects on the overall particle life cycle and global carbon budget.

  • 9.
    Posselt, Malte
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Transformation of Micropollutants in the Hyporheic Zone2020Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    Hyporheic zones (HZs) are reactive transition regions between rivers and aquifers which are thought to play an important role in the attenuation of micropollutants. Micropollutants are chemical substances such as pharmaceuticals, industrial chemicals or personal care products that are found in trace concentrations in the environment and that can be harmful to organisms. This thesis aimed to narrow the knowledge gap on the environmental fate of wastewater-derived polar organic micropollutants in the aquatic environment, with a specific emphasis on the hyporheic zone.

    In Paper I an efficient workflow was developed for the in-situ characterization of polar organic micropollutants and their transformation products (TPs) in the hyporheic zone at high spatial and temporal resolution and with minimal disturbance of natural flow paths. A low volume sampling device was combined with a newly developed high throughput-direct injection-UHPLC-MS/MS method. Application in the field revealed significant differences in micropollutant concentrations that varied over small time- and spatial scales. In Paper II the results of a comprehensive field study performed in the urban lowland river Erpe in Berlin, Germany, are presented. The work provided data on in-situ attenuation behavior of 24 micropollutants and TPs, along with novel insights into the spatially- and temporally varying environmental factors which play a major role in controlling in-stream attenuation of micropollutants. Paper III describes a novel, multi-flume experiment designed to investigate the influence of hyporheic exchange flow and sediment bacterial diversity on dissipation half-lives of 31 micropollutants and associated TPs. Attenuation and transformation of most substances increased significantly with bacterial diversity; fewer compounds responded to both bacterial diversity and hyporheic exchange flow. In addition to the discovery of several novel TPs, a number of bacterial strains were identified that might be associated with micropollutant degradation. In Paper IV the fate of metformin in the hyporheic zone was examined using large-scale (100m) recirculating flumes to perform realistic yet well-controlled experiments. In addition to determining dissipation half-lives in surface and pore water, the formation of novel TPs was investigated via suspect screening and bacterial communities were characterized using microbiological analyses. Data from these experiments indicate that dunes and macrophytes promote hyporheic exchange flow and create reactive environments with steep and varying biogeochemical gradients, which enhanced the degradation of metformin.

    Collectively, the fate of 33 parent compounds and 37 transformation products was assessed in field and mesocosm experiments described in this thesis. Additionally, 29 suspected TPs were tentatively identified. Higher bacterial diversity in the hyporheic zone and more intense hyporheic exchange flows significantly enhanced biodegradation of organic micropollutants. A number of known and novel TPs were discovered under diverse conditions, many of which showed signs of environmental persistence, providing further evidence for inclusion of TPs in contaminant risk assessments and regulatory frameworks. This work highlights the importance of considering both small- and reach-scale temporal and spatial variability for a mechanistic understanding of attenuation in in-stream studies.

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  • 10.
    Posselt, Malte
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Mechelke, Jonas
    Rutere, Cyrus
    Coll, Claudia
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Jaeger, Anna
    Raza, Muhammad
    Meinikmann, Karin
    Krause, Stefan
    Sobek, Anna
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Lewandowski, Jörg
    Horn, Marcus
    Hollender, Juliane
    Benskin, Jonathan P.
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Bacterial Diversity Controls Transformation of Wastewater-Derived Organic Contaminants in River-Simulating FlumesManuscript (preprint) (Other academic)
  • 11.
    Posselt, Malte
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Schaper, Jonas L.
    Jaeger, Anna
    Rutere, Cyrus
    Mechelke, Jonas
    Kusebauch, Björn
    Gergs, René
    Portman, Andrea
    Herzog, Skuyler
    Galloway, Jason
    Lewandowski, Jörg
    Hollender, Juliane
    Horn, Marcus
    Benskin, Jonathan P.
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Metformin Transformation in a Large-Scale Flume StudyManuscript (preprint) (Other academic)
  • 12. Stafoggia, Massimo
    et al.
    Johansson, Christer
    Stockholm University, Faculty of Science, Department of Environmental Science. Environment and Health Administration, Sweden.
    Glantz, Paul
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Renzi, Matteo
    Shtein, Alexandra
    de Hoogh, Kees
    Kloog, Itai
    Davoli, Marina
    Michelozzi, Paola
    Bellander, Tom
    A Random Forest Approach to Estimate Daily Particulate Matter, Nitrogen Dioxide, and Ozone at Fine Spatial Resolution in Sweden2020In: Atmosphere, ISSN 2073-4433, E-ISSN 2073-4433, Vol. 11, no 3, article id 239Article in journal (Refereed)
    Abstract [en]

    Air pollution is one of the leading causes of mortality worldwide. An accurate assessment of its spatial and temporal distribution is mandatory to conduct epidemiological studies able to estimate long-term (e.g., annual) and short-term (e.g., daily) health effects. While spatiotemporal models for particulate matter (PM) have been developed in several countries, estimates of daily nitrogen dioxide (NO2) and ozone (O-3) concentrations at high spatial resolution are lacking, and no such models have been developed in Sweden. We collected data on daily air pollutant concentrations from routine monitoring networks over the period 2005-2016 and matched them with satellite data, dispersion models, meteorological parameters, and land-use variables. We developed a machine-learning approach, the random forest (RF), to estimate daily concentrations of PM10 (PM<10 microns), PM2.5 (PM<2.5 microns), PM2.5-10 (PM between 2.5 and 10 microns), NO2, and O-3 for each squared kilometer of Sweden over the period 2005-2016. Our models were able to describe between 64% (PM10) and 78% (O-3) of air pollutant variability in held-out observations, and between 37% (NO2) and 61% (O-3) in held-out monitors, with no major differences across years and seasons and better performance in larger cities such as Stockholm. These estimates will allow to investigate air pollution effects across the whole of Sweden, including suburban and rural areas, previously neglected by epidemiological investigations.

  • 13.
    Yuan, Bo
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Hui Tay, Joo
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Papadopoulou, Eleni
    Småstuen Haug, Line
    Padilla-Sánchez, Juan Antonio
    de Wit, Cynthia A.
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Complex Mixtures of Chlorinated Paraffins Found in Hand Wipes of a Norwegian Cohort2020In: Environmental Science and Technology Letters, E-ISSN 2328-8930, Vol. 7, no 3, p. 198-205Article in journal (Refereed)
    Abstract [en]

    Up to 18000 ng of total chlorinated paraffins (CPs) was found in hand wipes of individual adult participants in a Norwegian cohort study (n = 60), with a geometric mean (SD) value of 870 (2700) ng. The CPs covered a wide range of alkane chain lengths from C-7 to C-48 with variable chlorine substitution. Complex mixtures of very-short-chain (vSCCPs, C-<10), short-chain (SCCPs, C10-13), medium-chain (MCCPs, C14-17), and long-chain (LCCPs, C->17) CPs were found, contributing on average 0.3%, 20%, 58%, and 22%, respectively, of the total CPs. Significant positive correlations were found between CP levels and factors related to the indoor environment and product use, including living in a house/apartment built before the ban of SCCPs, having a sofa, the number of TVs in the home, and owning a car, which mirrors CP usage as flame retardants and/or plasticizers in consumer products. Compared to previous studies of other organic contaminants in hand wipe samples from the same cohort, CPs were the most abundant flame retardants. This is the first report of CPs in hand wipes, and dermal exposure based on these data suggested that hand contact could be an important human exposure pathway for LCCPs.

  • 14.
    Ågerstrand, Marlene
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Arnold, Kathryn
    Balshine, Sigal
    Brodin, Tomas
    Brooks, Bryan W.
    Maack, Gerd
    McCallum, Erin S.
    Pyle, Greg
    Saaristo, Minna
    Ford, Alex T.
    Emerging investigator series: use of behavioural endpoints in the regulation of chemicals2020In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 22, no 1, p. 49-65Article in journal (Refereed)
    Abstract [en]

    Interest in behavioural ecotoxicology is growing, partly due to technological and computational advances in recording behaviours but also because of improvements of detection capacity facilitating reporting effects at environmentally relevant concentrations. The peer-reviewed literature now contains studies investigating the effects of chemicals, including pesticides and pharmaceuticals, on migration, dispersal, aggression, sociability, reproduction, feeding and anti-predator behaviours in vertebrates and invertebrates. To understand how behavioural studies could be used in regulatory decision-making we: (1) assessed the legal obstacles to using behavioural endpoints in EU chemicals regulation; (2) analysed the known cases of use of behavioural endpoints in EU chemicals regulation; and (3) provided examples of behavioural endpoints of relevance for population level effects. We conclude that the only legal obstacle to the use of behavioural endpoints in EU chemicals regulation is whether an endpoint is considered to be relevant at the population level or not. We also conclude that ecotoxicity studies investigating behavioural endpoints are occasionally used in the EU chemicals regulation, and underscore that behavioural endpoints can be relevant at the population level. To improve the current use of behavioural studies in regulatory decision-making contribution from all relevant stakeholders is required. We have the following recommendations: (1) researchers should conduct robust, well-designed and transparent studies that emphasize the relevance of the study for regulation of chemicals; (2) editors and scientific journals should promote detailed, reliable and clearly reported studies; (3) regulatory agencies and the chemical industry need to embrace new behavioural endpoints of relevance at the population level.

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