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1.
  • Assefa, Anteneh Taye, et al. (författare)
  • Assessment of PCDD/F Source Contributions in Baltic Sea Sediment Core Records
  • 2014
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851 .- 1086-931X .- 1520-6912. ; 48:16, s. 9531-9539
  • Tidskriftsartikel (refereegranskat)abstract
    • Spatial and temporal trends of sources of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) in the Baltic Sea were evaluated by positive matrix factorization (PMF) and principal component analysis (PCA). Sediment cores were sampled at eight coastal, one coastal reference, and six offshore sites covering the northern to the southern Baltic Sea. The cores, which covered the period 1919-2010, were sliced into 2-3 cm disks among which 8-11 disks per core (in total 141 disks) were analyzed for all tetra- through octa-CDD/Fs. Identification and apportionment of PCDD/F sources was carried out using PMF. Five stable model PCDD/F congener patterns were identified, which could be associated with six historically important source types: (i) atmospheric background deposition (ABD), (ii) use and production of pentachlorophenol (PCP), (iii) use and production of tetra-chlorophenol (TeCP), (iv) high temperature processes (Thermal), (v) hexa-CDD-related sources (HxCDD), and (vi) chlorine-related sources (Chi), all of which were still represented in the surface layers. Overall, the last four decades of the period 1920-2010 have had a substantial influence on the Baltic Sea PCDD/F pollution, with 88 +/- 7% of the total amount accumulated during this time. The 1990s was the peak decade for all source types except TeCP, which peaked in the 1980s in the northern Baltic Sea and has still not peaked in the southern part. The combined impact of atmospheric-related emissions (ABD and Thermal) was dominant in the open sea system throughout the study period (1919-2010) and showed a decreasing south to north trend (always >80% in the south and >50% in the north). Accordingly, to further reduce levels of PCDD/Fs in the open Baltic Sea ecosystem, future actions should focus on reducing atmospheric emissions.
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2.
  • Bidleman, Terry F., et al. (författare)
  • Atmospheric transport and deposition of bromoanisoles along a temperate to arctic gradient
  • 2017
  • Ingår i: Environmental Science and Technology. - Washington : American Chemical Society (ACS). - 1086-931X .- 1520-6912 .- 0013-936X .- 1520-5851. ; 51:19, s. 10974-10982
  • Tidskriftsartikel (refereegranskat)abstract
    • Bromoanisoles (BAs) arise from O-methylation of bromophenols, produced by marine algae and invertebrates. BAs undergo sea-air exchange and are transported over the oceans. Here we report 2,4-DiBA and 2,4,6-TriBA in air and deposition on the Swedish west coast (Råö) and the interior of arctic Finland (Pallas). Results are discussed in perspective with previous measurements in the northern Baltic region in 2011−2013. BAs in air decreased from south to north in the order Råö > northern Baltic > Pallas. Geometric mean concentrations at Pallas increased significantly (p < 0.05) between 2002 and 2015 for 2,4-DiBA but not for 2,4,6-TriBA. The logarithm of BA partial pressures correlated significantly to reciprocal air temperature at the coastal station Råö and over the Baltic, but only weakly (2,4-DiBA) or not significantly (2,4,6-TriBA) at inland Pallas. Deposition fluxes of BAs were similar at both sites despite lower air concentrations at Pallas, due to greater precipitation scavenging at lower temperatures. Proportions of the two BAs in air and deposition were related to Henry’s law partitioning and source regions. Precipitation concentrations were 10−40% of those in surface water of Bothnian Bay, northern Baltic Sea. BAs deposited in the bay catchment likely enter rivers and provide an unexpected source to northern estuaries. BAs may be precursors to higher molecular weight compounds identified by others in Swedish inland lakes.
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3.
  • Brandsma, Sicco H., et al. (författare)
  • Two organophosphorus flame retardants, resorcinol bis (diphenylphosphate)(PBDPP) and bisphenol A bis (diphenylphosphate) (BPA-BDPP) used as alternatives for BDE209 detected in dust
  • 2013
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 1086-931X .- 1520-6912 .- 0013-936X .- 1520-5851. ; 47:24, s. 14434-14441
  • Tidskriftsartikel (refereegranskat)abstract
    • Resorcinol bis(diphenylphosphate) (RBDPP) and bisphenol A bis(diphenylphosphate) (BPA-BDPP) are two halogen-free organophosphorus flame retardant (PFRs) that are used as an alternative for the decabromodiphenyl ether (Deca-BDE) technical mixture in TV/flatscreen housing and other electronic consumer products.' In this study, dust samples were collected from various microenvironments in The Netherlands (houses, cars), Greece.(houses), and Sweden (apartments, cars, furniture stores, electronics stores) and analyzed for RBDPP and BPA-BDPP. Additionally, the dust samples from The Netherlands were analyzed for decabromodiphenyl ether (BDE-209) for comparison and for TPHP, which is a byproduct in the RBDPP and BPA-BDPP technical products. BPA-BDPP was detected in almost all dust samples from The Netherlands, Greece, and Sweden. Highest concentrations were found in dust samples collected on electronic equipment from all three countries with BPA-BDPP levels ranging from <0.1 to 1300 mu g/g and RBDPP levels from <0.04 to 520 mu g/g. RBDPP and BPA-BDPP levels in dust collected further away from the electronics (source) were usually lower. BDE-209 levels in The Netherlands dust samples collected on and around the electronics were similar and much lower than the BPA-BDPP/RBDPP levels, indicating that the electronics were not the source of BDE-209. Strong positive correlations were found between TPHP concentrations and those of RBDPP (r = 0.805) and BPA-BDPP (r = 0.924), probably due to TPHP being a byproduct in commercial RBDPP and BPA-BDPP mixtures in electronics. To our knowledge, this is the first time that RBDPP and BPA-BDPP were detected in dust samples from Europe.
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4.
  • Börjesson, Gunnar, et al. (författare)
  • Methane fluxes from a Swedish landfill determined by geostatistical treatment of static chamber measurements
  • 2000
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 1086-931X .- 1520-6912 .- 0013-936X .- 1520-5851. ; 34:18, s. 4044-4050
  • Tidskriftsartikel (refereegranskat)abstract
    • Methane emissions from a Swedish landfill were measured with a static chamber technique on three occasions during 1997. Methane flux rates ranged from -15.2 x 10-3 to 40 g of CH4 m-2 h-1, and the spatial variability was high (CV = 343-386%). The spatial distribution of the emissions was estimated with the help of ordinary kriging, which is a spatial interpolation method. Three different approaches to estimate the total amounts were used: kriging on logarithm-transformed data, kriging with extremes excluded, and linear interpolation of measurements. These were compared between themselves and with the flux rates measured with a tracer gas technique. While the latter gave an estimate of 41 kg of CH4 h-1 from the landfill (with small variations), the highest possible estimate obtained with static chambers and geostatistical methods was 9.7 kg of CH4 h-1. The conclusion is that static chambers can hardly be trusted for making more than small-scale estimates of landfill gas emissions.Methane emissions from a Swedish landfill were measured with a static chamber technique on three occasions during 1997. Methane flux rates ranged from -15.2 ╫ 10-3 to 40 g of CH4 m-2 h-1, and the spatial variability was high (CV = 343-386%). The spatial distribution of the emissions was estimated with the help of ordinary kriging, which is a spatial interpolation method. Three different approaches to estimate the total amounts were used: kriging on logarithm-transformed data, kriging with extremes excluded, and linear interpolation of measurements. These were compared between themselves and with the flux rates measured with a tracer gas technique. While the latter gave an estimate of 41 kg of CH4 h-1 from the landfill (with small variations), the highest possible estimate obtained with static chambers and geostatistical methods was 9.7 kg of CH4 h-1. The conclusion is that static chambers can hardly be trusted for making more than small-scale estimates of landfill gas emissions.
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5.
  • Destouni, G., et al. (författare)
  • General quantification of catchment-scale nutrient and pollutant transport through the subsurface to surface and coastal waters
  • 2010
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 1086-931X .- 1520-6912 .- 0013-936X .- 1520-5851. ; 44:6, s. 2048-2055
  • Tidskriftsartikel (refereegranskat)abstract
    • This study develops a general quantification framework for consistent intermodel and intercatchment comparison of the nutrient and pollutant mass loading from multiple sources in a catchment area to downstream surface and coastal waters. The framework accounts for the wide spectrum of different transport pathways and travel times through the subsurface (soil, groundwater, sediment) and the linked surface (streams, lakes, wetlands) water systems of a catchment. The account is based on key flow partitioning and mass delivery fractions, which can be quantified differently by different flow and transport and reaction models. The framework application is exemplified for two Swedish catchment cases with regard to the transport of phosphorus and of a generic attenuating solute. The results show essential differences in model quantifications of transport pathways and temporal spreading, with important implications for our understanding of cause and effect in the catchment-scale nutrient and pollutant loading to downstream waters.
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6.
  • Drake, Henrik, 1979-, et al. (författare)
  • Incorporation of Metals into Calcite in a Deep Anoxic Granite Aquifer
  • 2018
  • Ingår i: Environmental Science & Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851 .- 1086-931X .- 1520-6912. ; 52:2, s. 493-502
  • Tidskriftsartikel (refereegranskat)abstract
    • Understanding metal scavenging by calcite in deep aquifers in granite is of importance for deciphering and modeling hydrochemical fluctuations and water rock interaction in the upper crust and for retention mechanisms associated With underground, repositories for toxic wastes. Metal scavenging into calcite has generally been established in the laboratory or in natural environments that cannot be unreservedly applied to conditions in deep crystalline rocks, an environment of broad interest, for nuclear waste repositories. Here, we report a microanalytical study: of calcite precipitated over a period of 17 years from anoxic, low-temperature (14 degrees C), neutral (pH: 7.4-7.7), and brackish (Cl: 1700-7100 mg/L) groundwater flowing in fractures at >400 m depth in granite rock. This enabled assessment of the trace metal uptake by calcite under these deep-seated conditions. Aquatic speciation modeling was carried out to assess influence of metal complexation on the partitioning into calcite. The resulting environment-specific partition coefficients were for several divalent ions in line with values obtained in controlled laboratory experiments, whereas for several other ions they differed substantially. High absolute uptake of rare earth elements and U(IV) suggests that coprecipitation into calcite can be an important sink for these metals and analogousactinides in the vicinity of geological repositories.
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7.
  • Ejlertsson, Jörgen, et al. (författare)
  • Anaerobic Degradation of Nonylphenol Mono- and Diethoxylates in Digestor Sludge, Landfilled Municipal Solid Waste, and Landfilled Sludge
  • 1999
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 1086-931X .- 1520-6912 .- 0013-936X .- 1520-5851. ; 33:2, s. 301-306
  • Tidskriftsartikel (refereegranskat)abstract
    • The aim of this study was to investigate the extent to which anaerobic digestor sludge, landfilled sludge, and landfilled municipal solid waste (MSW) degrade NPEOs under methanogenic conditions. NPEO1 and NPEO2 (NPEO1-2), used in a mixture, were chosen as model compounds. Anaerobic experimental bottles were amended with 100% digestor sludge at three different concentrations of NPEO1-2:  2, 60, and 308 mg L-1. [U-14C]-NPEO1-2 was used to detect any possible decomposition of the aromatic moiety of the NPEO1-2. All inoculates used degraded NPEO1-2 at 2 mg L-1, with nonylphenol (NP) forming the ultimate degradation product. The NP formed was not further degraded, and the incubations with labeled NPEO showed that the aromatic structure remained intact. Both landfill inoculates also transformed NPEO1-2 at 60 mg L-1. CH4 production was temporarily hampered in bottles with MSW landfill inoculum at 60 and 308 mg L-1. With 2 mg L-1 of NPEO, CH4 production closely followed that in the controls. Both NP and NPEO1-2 interacted with the organic matter which resulted in sorption to the solid phase.        
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8.
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9.
  • Kim, Jihee, et al. (författare)
  • Mass Budget of Methylmercury in the East Siberian Sea: The Importance of Sediment Sources
  • 2020
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 1086-931X .- 1520-6912 .- 0013-936X .- 1520-5851.
  • Tidskriftsartikel (refereegranskat)abstract
    • Biological concentrations of methylmercury(MeHg) are elevated throughout the Arctic Ocean; however, to date, the major sources and the spatial variability of MeHg are not well quantified. To identify the major inputs and outputs of MeHg to the Arctic shelf water column, we measured MeHg concentrations in the seawater and sediment samples from the East Siberian Sea collected from August to September 2018. We found that the MeHg concentrations in seawater and pore water were higher on the slope than on the shelf, while the MeHg concentrations in the sediment were higher on the shelf than on the slope. We created a mass budget for MeHg and found that the benthic diffusion and resuspension largely exceed other sources, such as atmospheric deposition and river water input. The major sinks of MeHg in the water column were dark demethylation and evasion. When we extrapolated our findings on benthic diffusion to the entire Arctic shelf system, the annual MeHg diffusion from the shelf sediments was estimated to be 23,065 ± 939 mol yr−1, about 2 times higher than previously proposed river discharges. Our study suggests that the MeHg input from shelf sediments in the Arctic Ocean is significant and has been previously underestimated.
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10.
  • Lemieux, Christine L, et al. (författare)
  • Cancer Risk Assessment of Polycyclic Aromatic Hydrocarbon Contaminated Soils Determined Using Bioassay-Derived Levels of Benzo[a]pyrene Equivalents
  • 2015
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 1086-931X .- 1520-6912 .- 0013-936X .- 1520-5851. ; 49:3, s. 1797-1805
  • Tidskriftsartikel (refereegranskat)abstract
    • Here we evaluate the excess lifetime cancer risk (ELCR) posed by 10 PAH-contaminated soils using (i) the currently advocated, targeted chemical-specific approach that assumes dose additivity for carcinogenic PAHs and (ii) a bioassay-based approach that employs the in vitro mutagenic activity of the soil fractions to determine levels of benzo[a]pyrene equivalents and, by extension, ELCR. Mutagenic activity results are presented in our companion paper.1 The results show that ELCR values for the PAH-containing fractions, determined using the chemical-specific approach, are generally (i.e., 8 out of 10) greater than those calculated using the bioassay-based approach; most are less than 5-fold greater. Only two chemical-specific ELCR estimates are less than their corresponding bioassay-derived values; differences are less than 10%. The bioassay-based approach, which permits estimation of ELCR without a priori knowledge of mixture composition, proved to be a useful tool to evaluate the chemical-specific approach. The results suggest that ELCR estimates for complex PAH mixtures determined using a targeted, chemical-specific approach are reasonable, albeit conservative. Calculated risk estimates still depend on contentious PEFs and cancer slope factors. Follow-up in vivo mutagenicity assessments will be required to validate the results and their relevance for human health risk assessment of PAH-contaminated soils
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11.
  • Lindström, David, et al. (författare)
  • Chromium(III) and Chromium(VI) Surface Treated Galvanized Steel for Outdoor Constructions : Environmental Aspects
  • 2010
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 1086-931X .- 1520-6912 .- 0013-936X .- 1520-5851. ; 44:11, s. 4322-4327
  • Tidskriftsartikel (refereegranskat)abstract
    • The long-term degradation of chromium(III) (Zn-Cr(III)) and chromium(VI)-based (Zn-Cr(VI)) surface treatments on galvanized steel and their capacities to hinder the release of zinc induced by atmospheric corrosion at non-sheltered urban and marine exposure conditions for two years are investigated. Compared to bare zinc sheet, both surface treatments revealed high corrosion protection abilities and capacities to hinder the release of zinc, still evident after two years of exposure. The zinc barrier properties of the thinner Zn-Cr(VI) (10 nm) treatment were during the first 100 days of urban exposure slightly improved compared with Zn-Cr(III) (35 nm). However, their long-term protection capacities were inversed.  Released concentrations of total chromium correspond to annual release rates less than 0.000032 (Zn-Cr(III)) and 0.00014 g Cr m-2yr-1 (Zn-Cr(VI)) after one year of urban exposure. Ageing by indoor storage of the surface treatments prior to outdoor exposure reduced the released Cr concentrations from the surface treatments. No Cr(VI) was released from the aged surfaces but from the freshly exposed Zn-Cr(VI).   Marine exposure conditions resulted in a faster reduction of chromate to chromium(III)oxide compared with urban conditions, and a significantly lower amount of both chromium(III) and chromium(VI) released from Zn-Cr(VI) at the marine site compared with the urban site.
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12.
  • Plassmann, Merle M., et al. (författare)
  • Theoretical and Experimental Simulation of the Fate of Semifluorinated n-Alkanes during Snowmelt
  • 2010
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 1086-931X .- 1520-6912 .- 0013-936X .- 1520-5851. ; 44:17, s. 6692-6697
  • Tidskriftsartikel (refereegranskat)abstract
    • Semifluorinated n-alkanes (SFAs) are highly fluorinated anthropogenic chemicals that are released into the environment through their use in ski waxes. Nothing is known about their environmental partitioning in general and their fate during snowmelt in particular. Properties were estimated for a range of SFAs with different chain lengths and degrees of fluorination using the SPARC calculator and poly parameter linear free energy relationships (ppLFERs). The calculations resulted in very low water solubility and vapor pressures and, consequently, high log KOW and log KOA values. Artificially produced snow in a cold room was spiked with a range of SFAs and subsequently melted with infrared lamps. Melt water, particles, and air samples taken during melting were analyzed. Both calculations and experiments showed that SFAs used in ski waxes will bind to particles or snow grain surfaces during snowmelt and thus are predicted to end up on the soil surface in skiing areas.
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13.
  • Sun, Jiachen, et al. (författare)
  • Hepatic Fatty Acid Profiles Associated with Exposure to Emerging and Legacy Halogenated Contaminants in Two Harbor Seal Populations across the North Atlantic
  • 2022
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 1086-931X .- 1520-6912 .- 0013-936X .- 1520-5851. ; 56:3, s. 1830-1840
  • Tidskriftsartikel (refereegranskat)abstract
    • Fatty acids (FAs) have been extensively used as indicators of foraging ecology in marine mammals, yet their association with exposure to contaminants has rarely been investigated. The present study provided the first characterization of the relationship between hepatic FA profiles and exposure to a suite of contaminants in a sentinel species─the harbor seal (Phoca vitulina)─from the Gulf of Maine and the south coast of Sweden. FA profiles differed in the two seal populations, and the levels of legacy and alternative brominated flame retardants and polyhalogenated carbazoles were significantly elevated in Maine seals. Correlations between individual FAs and multiple flame retardants (FRs) and poly- and perfluoroalkyl substances (PFASs) were found in seals from both populations. Moreover, several FR and PFAS chemicals were significantly associated with the estimated desaturating enzyme activity inferred from the FA profiles. The ratios of poly to monounsaturated FAs (∑PUFAs/∑MUFAs) and those of unsaturated to saturated FAs (∑UFAs/∑SFAs) were significantly associated with HBBZ, PFHxS, or BDE 47 in seals from Maine and Sweden, whereas ∑n – 6/∑n – 3 PUFAs was significantly associated with BDE 154 and 36-CCZ in Swedish and Maine seals, respectively. Our results suggest the lipid metabolism-disrupting potential of these contaminants in marine mammals and warrant continuous biomonitoring and risk assessment, considering the critical role of PUFAs in vital biological processes.
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14.
  • Undeman, Emma, et al. (författare)
  • The susceptibility of human populations to environmental exposure to organic contaminants
  • 2010
  • Ingår i: Environmental Science and Technology. - Washington, D.C. : American Chemical Society. - 1086-931X .- 1520-6912 .- 0013-936X .- 1520-5851. ; 44:16, s. 6249-6255
  • Tidskriftsartikel (refereegranskat)abstract
    • Environmental exposure to organic contaminants is a complex function of environmental conditions, food chain characteristics, and chemical properties. In this study the susceptibility of various human populations to environmental exposure to neutral organic contaminants was compared. An environmental fate model and a linked bioaccumulation model were parameterized to describe ecosystems in different climatic regions (temperate, arctic, tropical and steppe). The human body burden resulting from constant emissions of hypothetical chemicals was estimated for each region. An exposure susceptibility index was defined as the body burden in the region of interest normalized to the burden of the same chemical in a reference human from the temperate region eating an average diet. For most persistent chemicals emitted to air, the Arctic had the highest susceptibility index (max 520). Susceptibility to exposure was largely determined by the food web properties. The properties of the physical environment only had a marked effect when air or water, not food, was the dominant source of human exposure. Shifting the mode of emission markedly changed the relative susceptibility of the ecosystems in some cases. The exposure arising from chemical use clearly varies between ecosystems, which makes an understanding of ecosystem susceptibility to exposure important for chemicals management.
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15.
  • Achermann, Stefan, et al. (författare)
  • Trends in Micropollutant Biotransformation along a Solids Retention Time Gradient
  • 2018
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 52:20, s. 11601-11611
  • Tidskriftsartikel (refereegranskat)abstract
    • For many polar organic micropollutants, biotransformation by activated sludge microorganisms is a major removal process during wastewater treatment. However, our current understanding of how wastewater treatment operations influence microbial communities and their micropollutant biotransformation potential is limited, leaving major parts of observed variability in biotransformation rates across treatment facilities unexplained. Here, we present biotransformation rate constants for 42 micropollutants belonging to different chemical classes along a gradient of solids retention time (SRT). The geometric mean of biomass-normalized first-order rate constants shows a clear increase between 3 and 15 d SRT by 160% and 87%, respectively, in two experiments. However, individual micropollutants show a variety of trends. Rate constants of oxidative biotransformation reactions mostly increased with SRT. Yet, nitrifying activity could be excluded as primary driver. For substances undergoing other than oxidative reactions, i.e., mostly substitution-type reactions, more diverse dependencies on SRT were observed. Most remarkably, characteristic trends were observed for groups of substances undergoing similar types of initial transformation reaction, suggesting that shared enzymes or enzyme systems that are conjointly regulated catalyze biotransformation reactions within such groups. These findings open up opportunities for correlating rate constants with measures of enzyme abundance such as genes or gene products, which in turn should help to identify enzymes associated with the respective biotransformation reactions.
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16.
  • Adediran, Gbotemi A., et al. (författare)
  • Microbial Biosynthesis of Thiol Compounds : Implications for Speciation, Cellular Uptake, and Methylation of Hg(II)
  • 2019
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 53:14, s. 8187-8196
  • Tidskriftsartikel (refereegranskat)abstract
    • Cellular uptake of inorganic divalent mercury (Hg(II)) is a key step in microbial formation of neurotoxic methylmercury (MeHg), but the mechanisms remain largely unidentified. We show that the iron reducing bacterium Geobacter sulfurreducens produces and exports appreciable amounts of low molecular mass thiol (LMM-RSH) compounds reaching concentrations of about 100 nM in the assay medium. These compounds largely control the chemical speciation and bioavailability of Hg(II) by the formation of Hg(LMM-RS)2 complexes (primarily with cysteine) in assays without added thiols. By characterizing these effects, we show that the thermodynamic stability of Hg(II)-complexes is a principal controlling factor for Hg(II) methylation by this bacterium such that less stable complexes with mixed ligation involving LMM-RSH, OH-, and Cl- are methylated at higher rates than the more stable Hg(LMM-RS)2 complexes. The Hg(II) methylation rate across different Hg(LMM-RS)2 compounds is also influenced by the chemical structure of the complexes. In contrast to the current perception of microbial uptake of Hg, our results adhere to generalized theories for metal biouptake based on metal complexation with cell surface ligands and refine the mechanistic understanding of Hg(II) availability for microbial methylation.
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17.
  • Adolfsson-Erici, Margaretha, et al. (författare)
  • Internal Benchmarking Improves Precision and Reduces Animal Requirements for Determination of Fish Bioconcentration Factors
  • 2012
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 46:15, s. 8205-8211
  • Tidskriftsartikel (refereegranskat)abstract
    • The enactment of new chemical regulations has generated a large need for the measurement of the fish bioconcentration factor (BCF). Past experience shows that the BCF determination lacks precision, requires large numbers of fish, and is costly. A new protocol was tested that shortens the experiment from up to 12 weeks for existing protocols to 2 weeks and reduces the number of fish by a factor of 5, while introducing internal benchmarking for the BCF determination. Rainbow trout were simultaneously exposed to 11 chemicals. The BCFs were quantified using one of the test chemicals, musk xylene, as a benchmark. These were compared with BCFs measured in a parallel experiment based on the OECD 305 guideline. The agreement was <20% for five chemicals and between 20%-25% for two further, while two chemicals lay outside the BCF operating window of the experiment and one was lost due to analytical difficulties. This agreement is better than that observed in a BCF Gold Standard Database. Internal benchmarking allows the improvement of the precision of BCF determination in parallel to large reduction in costs and fish requirements.
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18.
  • Aeppli, Christoph, et al. (författare)
  • Chlorine Isotope Effects and Composition of Naturally Produced Organochlorines from Chloroperoxidases, Flavin-Dependent Halogenases, and in Forest Soil
  • 2013
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 47:13, s. 6864-6871
  • Tidskriftsartikel (refereegranskat)abstract
    • The use of stable chlorine isotopic signatures (delta Cl-37) of organochlorine compounds has been suggested as a tool to determine both their origins and transformations in the environment. Here we investigated the delta Cl-37 fractionation of two important pathways for enzymatic natural halogenation: chlorination by chloroperoxidase (CPO) and flavin-dependent halogenases (FDH). Phenolic products of CPO were highly Cl-37 depleted (delta Cl-37 = -12.6 +/- 0.9 parts per thousand); significantly more depleted than all known industrially produced organochlorine compounds (delta Cl-37 = -7 to +6 parts per thousand). In contrast, four FDH products did not exhibit any observable isotopic shifts (delta Cl-37 = -0.3 +/- 0.6 parts per thousand). We attributed the different isotopic effect to the distinctly different chlorination mechanisms employed by the two enzymes. Furthermore, the delta Cl-37 in bulk organochlorines extracted from boreal forest soils were only slightly depleted in Cl-37 relative to inorganic Cl. In contrast to previous suggestions that CPO plays a key role in production of soil organochlorines, this observation points to the additional involvement of either other chlorination pathways, or that dechlorination of naturally produced organochlorines can neutralize delta Cl-37 shifts caused by CPO chlorination. Overall, this study demonstrates that chlorine isotopic signatures are highly useful to understand sources and cycling of organochlorines in nature. Furthermore, this study presents delta Cl-37 values of FDH products as well of bulk organochlorines extracted from pristine forest soil for the first time.
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19.
  • Aeppli, Christoph, et al. (författare)
  • Use of Cl and C Isotopic Fractionation to Identify Degradation and Sources of Polychlorinated Phenols : Mechanistic Study and Field Application
  • 2013
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 47:2, s. 790-797
  • Tidskriftsartikel (refereegranskat)abstract
    • The widespread use of chlorinated phenols (CPs) as a wood preservative has led to numerous contaminated sawmill sites. However, it remains challenging to assess the extent of in situ degradation of CPs. We evaluated the use of compound-specific chlorine and carbon isotope analysis (Cl- and C-CSLA) to assess CP biotransformation. In a laboratory system, we measured isotopic fractionation during oxidative 2,4,6-trichlorophenol dechlorination by representative soil enzymes (C. fumago chloroperoxidase, horseradish peroxidase, and laccase from T. versicolor). Using a mathematical model, the validity of the Rayleigh approach to evaluate apparent kinetic isotope effects (AKIE) was confirmed. A small but significant Cl-AKIE of 1.0022 +/- 0.0006 was observed for all three enzymes, consistent with a reaction pathway via a cationic radical species. For carbon, a slight inverse isotope effect was observed (C-AKIE = 0.9945 +/- 0.0019). This fractionation behavior is clearly distinguishable from reported reductive dechlorination mechanisms. Based on these results we then assessed degradation and apportioned different types of technical CP mixtures used at two former sawmill sites. To our knowledge, this is the first study that makes use of two-element CSIA to study sources and transformation of CPs in the environment.
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20.
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21.
  • Agrell, Cecilia, et al. (författare)
  • Evidence of Latitudinal Fractionation of Polychlorinated Biphenyl Congeners along the Baltic Sea Region
  • 1999
  • Ingår i: Environmental Science & Technology. - : American Chemical Society (ACS). - 1520-5851 .- 0013-936X. ; 33:8, s. 1149-1156
  • Tidskriftsartikel (refereegranskat)abstract
    • Annual cycles of the atmospheric concentrations of PCBs were determined at 16 (mostly rural) stations around the Baltic Sea between 1990 and 1993. The concentration levels of individual congeners were found to be influenced by their physical-chemical properties, ambient temperature, and geographical location. Median levels of PCBs were similar at all stations except at one urban site near Riga. A latitudinal gradient with higher levels in the south was found for the sum of PCB as well as for individual congeners, and the gradient was more pronounced for the low volatility congeners. As a result, the high volatility congeners increased in relative importance with latitude. Generally, PCB concentrations increased with temperature, but slopes of the partial pressure in air versus reciprocal temperature were different between congeners and between stations. In general, the low volatility congeners were more temperature dependent than the high volatility PCB congeners. Steep slopes at a sampling location indicate that the concentration in air is largely determined by diffusive exchange with soils. Lack of a temperature dependence may be due to the influence of long-range transported air masses at remote sites and due to the episodic or random nature of PCB sources at urban sites.
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22.
  • Ahlgren, Joakim, et al. (författare)
  • Sediment Depth Attenuation of Biogenic Phosphorus Compounds Measured by 31P NMR
  • 2005
  • Ingår i: Environmental Science and Technology. - Univ Uppsala, Dept Analyt Chem, SE-75124 Uppsala, Sweden. Univ Uppsala, Dept Ecol & Evolut, Uppsala, Sweden. Univ Uppsala, Dept Organ Chem, SE-75124 Uppsala, Sweden. : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 39:3, s. 867-872
  • Tidskriftsartikel (refereegranskat)abstract
    • Being a major cause of eutrophication and subsequent loss of water quality, the turnover of phosphorus (P) in lake sediments is in need of deeper understanding. A major part of the flux of P to eutrophic lake sediments is organically bound or of biogenic origin. This P is incorporated in a poorly described mixture of autochthonous and allochthonous sediment and forms the primary storage of P available for recycling to the water column, thus regulating lake trophic status. To identify and quantify biogenic sediment P and assess its lability, we analyzed sediment cores from Lake Erken, Sweden, using traditional P fractionation, and in parallel, NaOH extracts were analyzed using 31P NMR. The surface sediments contain orthophosphates (ortho-P) and pyrophosphates (pyro-P), as well as phosphate mono- and diesters. The first group of compounds to disappear with increased sediment depth is pyrophosphate, followed by a steady decline of the different ester compounds. Estimated half-life times of these compound groups are about 10 yr for pyrophosphate and 2 decades for mono- and diesters. Probably, these compounds will be mineralized to ortho-P and is thus potentially available for recycling to the water column, supporting further growth of phytoplankton. In conclusion, 31P NMR is a useful tool to asses the bioavailability of certain P compound groups, and the combination with traditional fractionation techniques makes quantification possible.
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23.
  • Ahrens, Lutz (författare)
  • Characterization of Two Passive Air Samplers for Per- and Polyfluoroalkyl Substances
  • 2013
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 47, s. 14024-14033
  • Tidskriftsartikel (refereegranskat)abstract
    • Two passive air sampler (PAS) media were characterized under field conditions for the measurement of per- and polyfluoroalkyl substances (PFASs) in the atmosphere. The PASs, consisting of polyurethane foam (PUF) and sorbent-impregnated PUF (SIP) disks, were deployed for over one year in parallel with high volume active air samplers (HV-AAS) and low volume active air samplers (LV-AAS). Samples were analyzed for perfluoroalkyl carboxylic acids (PFCAs), perfluoroalkane sulfonic acids (PFSAs), fluorotelomer alcohols (FTOHs), fluorotelomer methacrylates (FTMACs), fluorotelomer acrylates (FTACs), perfluorooctane sulfonamides (FOSAs), and perfluorooctane sulfonamidoethanols (FOSEs). Sampling rates and the passive sampler medium (PSM)-air partition coefficient (KPSM-A) were calculated for individual PFASs. Sampling rates were similar for PFASs present in the gas phase and particle phase, and the linear sampling rate of 4 m(-3) d(-1) is recommended for calculating effective air sample volumes in the SIP-PAS and PUF-PAS for PFASs except for the FOSAs and FOSEs in the PUF-PAS. SIP disks showed very good performance for all tested PFASs while PUF disks were suitable only for the PFSAs and their precursors. Experiments evaluating the suitability of different isotopically labeled fluorinated depuration compounds (DCs) revealed that C-13(8)-perfluorooctanoic acid (PFOA) was suitable for the calculation of site-specific sampling rates. Ambient temperature was the dominant factor influencing the seasonal trend of PFASs.
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24.
  • Ahrens, Lutz (författare)
  • Occurrence and Gas–Particle Partitioning of Organic UV-Filters in Urban Air
  • 2020
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 54, s. 12881-12889
  • Tidskriftsartikel (refereegranskat)abstract
    • A retrospective analysis of a comprehensive series of high-volume air samples (n = 70) collected during 2010-2011 in Toronto (Canada) was performed. Seven UV compounds were analyzed by gas chromatography-tandem mass spectrometry (GC-MS/MS) with sum of concentrations (gas + particle phase) ranging from 80 to 2030 pg/m(3). Homosalate (HMS) was the most prevalent organic UV-filter in air (47% of the total concentration), followed by 2-ethylhexyl salicylate (EHS, similar to 29%), E- and Z-2-ethylhexyl 4-methoxycinnamate (EHMC, similar to 17%). Ambient air (gas + particle phase) concentrations of organic UV-filters showed a strong seasonality, with peak levels during the summer. An analysis of Clausius-Clapeyron slopes indicated that much of the ambient burden of organic UV-filters are explained by volatilization from terrestrial and aquatic surfaces and supplemented with human activities and use of lotions and sunscreens, containing organic UV-filters, in addition to its use in plastics, textiles, paints, and pesticides. The results showed that organic UV-filters exist mainly in the gas phase with some exceptions, for instance, octocrylene (OCR), which was associated with both gas and particle phases, and avobenzone (AVB), which was predominantly in the particle phase. Lastly, this study revealed the need for basic physical chemical property data for organic UV-filters, including information on transformation rates and products, for better evaluating their environmental fate and effects.
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25.
  • Ahrens, Lutz, et al. (författare)
  • Partitioning Behavior of Per- and Polyfluoroalkyl Compounds between Pore Water and Sediment in Two Sediment Cores from Tokyo Bay, Japan
  • 2009
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 43:18, s. 6969-6975
  • Tidskriftsartikel (refereegranskat)abstract
    • The partitioning behavior of per- and polyfluoroalkyl compounds (PFCs) between pore water and sediment in two sediment cores collected from Tokyo Bay, Japan, was investigated. In addition, the fluxes and temporal trends in one dated sediment core were studied. Short-chain perfluoroalkyl carboxylic acids (PFCAs) (C ≤ 7) were found exclusively in pore water, while long-chain PFCAs (C ≥ 11) were found only in sediment. The perfluoroalkyl sulfonates (PFSAs), n-ethylperfluoro-1-octanesulfonamidoacetic acid (N-EtFOSAA), and perfluorooctane sulfonamide (PFOSA) seemed to bind more strongly to sediment than PFCAs. The enrichment of PFCs on sediment increased with increasing organic matter and decreasing pH. The perfluorocarbon chain length and functional group were identified as the dominating parameters that had an influence on the partitioning behavior of the PFCs in sediment. The maximum ΣPFC contamination in sediment was observed in 2001-2002 to be a flux of 197 pg cm-2 yr-1. Statistically significant increased concentrations in Tokyo Bay were found for perfluorooctanesulfonate (PFOS) (1956-2008), perfluorononanoic acid (PFNA) (1990-2008), and perfluoroundecanoic acid (PFUnDA) (1990-2008). Concentrations of PFOSA and N-EtFOSAA increased between 1985 and 2001, but after 2001, the concentration decreased significantly, which corresponded with the phase out of perfluorooctyl sulfonyl fluoride-based compounds by the 3M Company in 2000.
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26.
  • Ahrens, Lutz (författare)
  • Passive Sampling in Regulatory Chemical Monitoring of Nonpolar Organic Compounds in the Aquatic Environment
  • 2016
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 50, s. 3-17
  • Forskningsöversikt (refereegranskat)abstract
    • We reviewed compliance monitoring requirements in the European Union, the United States, and the Oslo-Paris Convention for the protection of the marine environment of the North-East Atlantic, and evaluated if these are met by passive sampling methods for nonpolar compounds. The strengths and shortcomings of passive sampling are assessed for water, sediments, and biota. Passive water sampling is a suitable technique for measuring concentrations of freely dissolved compounds. This method yields results that are incompatible with the EU's quality standard definition in terms of total concentrations in water, but this definition has little scientific basis. Insufficient quality control is a present weakness of passive sampling in water. Laboratory performance studies and the development of standardized methods are needed to improve data quality and to encourage the use of passive sampling by commercial laboratories and monitoring agencies. Successful prediction of bioaccumulation based on passive sampling is well documented for organisms at the lower trophic levels, but requires more research for higher levels. Despite the existence of several knowledge gaps, passive sampling presently is the best available technology for chemical monitoring of nonpolar organic compounds. Key issues to be addressed by scientists and environmental managers are outlined.
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27.
  • Ahrens, Lutz (författare)
  • Temporal Variations of Cyclic and Linear Volatile Methylsiloxanes in the Atmosphere Using Passive Samplers and High-Volume Air Samplers
  • 2014
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 48, s. 9374-9381
  • Tidskriftsartikel (refereegranskat)abstract
    • Cyclic and linear volatile methylsiloxanes (cVMSs and IVMSs, respectively) were measured in ambient air over a period of over one year in Toronto, Canada. Air samples were collected using passive air samplers (PAS) consisting of sorbent-impregnated polyurethane foam (SIP) disks in parallel with high volume active air samplers (HV-AAS). The average difference between the SIP-PAS derived concentrations in air for the individual VMSs and those measured using HV-AAS was within a factor of 2. The air concentrations (HV-AAS) ranged 22-351 ng m(-3) and 1.3-15 ng m(-3) for Sigma cVMSs (D-3, D-4, D-5, D-6) and Sigma lVMSs (L-3, L-4, L-5), respectively, with decamethylcyclopentasiloxane (D-5) as the dominant compound (similar to 75% of the Sigma VMSs). Air masses arriving from north to northwest (i.e., less populated areas) were significantly less contaminated with VMSs compared to air arriving from the south that are impacted by major urban and industrial areas in Canada and the U.S. (p < 0.05). In addition, air concentrations of Sigma cVMSs were lower during major snowfall events (on average, 73 ng m(-3)) in comparison to the other sampling periods (121 ng m(-3)). Ambient temperature had a small influence on the seasonal trend of VMS concentrations in air, except for dodecamethylcyclohexasiloxane (D-6), which was positively correlated with the ambient temperature (p < 0.001).
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28.
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29.
  • Aldén, Louise, et al. (författare)
  • No long-term persistence of bacterial pollution-induced community tolerance in tylosin-polluted soil
  • 2008
  • Ingår i: Environmental Science & Technology. - : American Chemical Society (ACS). - 1520-5851 .- 0013-936X. ; 42:18, s. 6917-6921
  • Tidskriftsartikel (refereegranskat)abstract
    • Pollution-induced community tolerance (PICT) of soil bacteria to the antibiotic tylosin was studied over 95 days. Tylosin was added at increasing concentrations, together with different amounts of alfalfa to study the effects of substrate addition on PICT and bacterial growth in soil. The leucine incorporation technique was used to estimate bacterial growth and as a detection method in the PICT concept. Direct inhibition of the bacterial growth rates, resulting in a dose-response curve, was found above 50 mg of tylosin kg(-1) of soil two days after tylosin addition (IC50 value of 960 mg tylosin kg(-1)). After 10 days of exposure to at least 50 mg of tylosin kg(-1), the PICT was observed and correlated to inhibition of bacterial growth by tylosin. A return of the PICT to control levels was found over time, and after 95 days at 1500 mg of tylosin kg(-1), essentially no PICT was found, as compared to the unpolluted control soil. The return of PICT to pre-exposure levels was not totally reflected in the recovery of bacterial growth. Alfalfa addition did not affect the inhibitory effect of tylosin on bacterial growth rates; neither did it alter the PICT. Since tylosin is relatively rapidly degraded in soil, our results indicate that the PICT will return to prepollution levels when the selective pressure of the toxicant is removed and will thus be a useful technique for monitoring remediation measures.
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30.
  • Alejandre, Elizabeth M., et al. (författare)
  • Characterization Factors to Assess Land Use Impacts on Pollinator Abundance in Life Cycle Assessment
  • 2023
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 57:8, s. 3445-3454
  • Tidskriftsartikel (refereegranskat)abstract
    • While wild pollinators play a key role in global food production, their assessment is currently missing from the most commonly used environmental impact assessment method, Life Cycle Assessment (LCA). This is mainly due to constraints in data availability and compatibility with LCA inventories. To target this gap, relative pollinator abundance estimates were obtained with the use of a Delphi assessment, during which 25 experts, covering 16 nationalities and 45 countries of expertise, provided scores for low, typical, and high expected abundance associated with 24 land use categories. Based on these estimates, this study presents a set of globally generic characterization factors (CFs) that allows translating land use into relative impacts to wild pollinator abundance. The associated uncertainty of the CFs is presented along with an illustrative case to demonstrate the applicability in LCA studies. The CFs based on estimates that reached consensus during the Delphi assessment are recommended as readily applicable and allow key differences among land use types to be distinguished. The resulting CFs are proposed as the first step for incorporating pollinator impacts in LCA studies, exemplifying the use of expert elicitation methods as a useful tool to fill data gaps that constrain the characterization of key environmental impacts.
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31.
  • Álvarez-Ruiz, Rodrigo, et al. (författare)
  • Postflood Monitoring in a Subtropical Estuary and Benchmarking with PFASs Allows Measurement of Chemical Persistence on the Scale of Months
  • 2021
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 55:21, s. 14607-14616
  • Tidskriftsartikel (refereegranskat)abstract
    • Measurements of chemical persistence in natural environments can provide insight into behavior not easily replicated in laboratory studies. However, it is difficult to find environmental situations suitable for such measurements, particularly for substances with half-lives exceeding several weeks. The objective of this study was to demonstrate that a strategic postflood monitoring campaign can be used to quantify transformation half-lives on the scale of months in a real aquatic system. Water samples were collected in the upper Brisbane River estuary on 36 occasions over 37 weeks and analyzed for 127 pharmaceuticals and personal care products (PPCPs), pesticides, and perfluoroalkyl substances (PFASs). High quality time trend data were obtained for 41 substances. For many of these, data on the input of a wastewater treatment plant to the upper estuary were also obtained. A mass balance model of the estuary stretch was formulated and parametrized using PFASs as persistent benchmarking chemicals. Transformation half-life estimates were obtained for 10 PPCPs and 7 pesticides ranging from 18 to 260 days. Furthermore, insight was obtained into dominant transformation processes as well as the magnitude of chemical inputs to the estuary and their sources. The approach developed shows that under certain conditions, estuaries can be used to quantify the persistence of organic contaminants with half-lives of the order of several months.
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32.
  • Alves, Andreia, et al. (författare)
  • Case Study on Screening Emerging Pollutants in Urine and Nails
  • 2017
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 51:7, s. 4046-4053
  • Tidskriftsartikel (refereegranskat)abstract
    • Alternative plasticizers and flame retardants (FRs) have been introduced as replacements for banned or restricted chemicals, but much is still unknown about their metabolism and occurrence in humans. We identified the metabolites formed in vitro for four alternative plasticizers (acetyltributyl citrate (ATBC), bis(2-propylheptyl) phthalate (DPHP), bis(2-ethylhexyl) terephthalate (DEHTP), bis(2ethylhexyl) adipate (DEHA)), and one FR (2,2-bis (chloromethyl)-propane-1,3-diyltetrakis(2-chloroethyl) bisphosphate (V6)). Further, these compounds and their metabolites were investigated by LC/ESI-Orbitrap-MS in urine and finger nails collected from a Norwegian cohort. Primary and secondary ATBC metabolites had detection frequencies (% DF) in finger nails ranging from 46 to 95%. V6 was identified for the first time in finger nails, suggesting that this matrix may also indicate past exposure to FRs as well as alternative plasticizers. Two isomeric forms of DEHTP primary metabolite were highly detected in urine (97% DF) and identified in finger nails, while no DPHP metabolites were detected in vivo. Primary and secondary DEHA metabolites were identified in both matrices, and the relative proportion of the secondary metabolites was higher in urine than in finger nails; the opposite was observed for the primary metabolites. As many of the metabolites present in in vitro extracts were further identified in vivo in urine and finger nail samples, this suggests that in vitro assays can reliably mimic the in vivo processes. Finger nails may be a useful noninvasive matrix for human biomonitoring of specific organic contaminants, but further validation is needed.
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33.
  • Amin, H., et al. (författare)
  • Indoor Airborne Microbiome and Endotoxin: Meteorological Events and Occupant Characteristics Are Important Determinants
  • 2023
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 57:32, s. 11750-11766
  • Tidskriftsartikel (refereegranskat)abstract
    • Minimal research exists onthe factors influencing the indoorbacterial community. Despite their proposed importance for health,here we report environmental factors influencing the composition ofthe indoor bacterial communities. Airborne bacteria and endotoxin may affect asthma andallergies.However, there is limited understanding of the environmental determinantsthat influence them. This study investigated the airborne microbiomesin the homes of 1038 participants from five cities in Northern Europe:Aarhus, Bergen, Reykjavik, Tartu, and Uppsala. Airborne dust particleswere sampled with electrostatic dust fall collectors (EDCs) from theparticipants' bedrooms. The dust washed from the EDCs'clothes was used to extract DNA and endotoxin. The DNA extracts wereused for quantitative polymerase chain (qPCR) measurement and 16SrRNA gene sequencing, while endotoxin was measured using the kineticchromogenic limulus amoebocyte lysate (LAL) assay. The results showedthat households in Tartu and Aarhus had a higher bacterial load anddiversity than those in Bergen and Reykjavik, possibly due to elevatedconcentrations of outdoor bacterial taxa associated with low precipitationand high wind speeds. Bergen-Tartu had the highest difference (ANOSIM R = 0.203) in & beta; diversity. Multivariate regressionmodels showed that & alpha; diversity indices and bacterial and endotoxinloads were positively associated with the occupants' age, numberof occupants, cleaning frequency, presence of dogs, and age of thehouse. Further studies are needed to understand how meteorologicalfactors influence the indoor bacterial community in light of climatechange.
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34.
  • Andersen, Christina, et al. (författare)
  • Inhalation and Dermal Uptake of Particle and Gas-phase Phthalates - A Human Exposure Study
  • 2018
  • Ingår i: Environmental Science & Technology. - : American Chemical Society (ACS). - 1520-5851 .- 0013-936X. ; 52:21, s. 12792-12800
  • Tidskriftsartikel (refereegranskat)abstract
    • Phthalates are ubiquitous in indoor environments, which raises concern about their endocrine disrupting properties. However, studies of human uptake from airborne exposure are limited. We studied the inhalation uptake and dermal uptake by air-to-skin transfer with clean clothing as a barrier of two deuterium-labelled airborne phthalates: particle-phase D4-DEHP (di-(2-ethylhexyl)phthalate) and gas-phase D4-DEP (diethyl phthalate). Sixteen participants, wearing trousers and long-sleeved shirts, were under controlled conditions exposed to airborne phthalates in four exposure scenarios: dermal uptake alone, and combined inhalation+dermal uptake of both phthalates. The results showed an average uptake of D4-DEHP by inhalation of 0.0014±0.00088 (µg kg-1 bw)/(µg m-3)/h. No dermal uptake of D4-DEHP was observed during the 3 hour exposure with clean clothing. The deposited dose of D4-DEHP accounted for 26% of the total inhaled D4-DEHP mass. For D4-DEP, the average uptake by inhalation+dermal was 0.0067±0.0045 and 0.00073±0.00051 (µg kg-1 bw)/(µg m-3)/h for dermal uptake. Urinary excretion factors of metabolites after inhalation were estimated to 0.69 for D4-DEHP and 0.50 for D4-DEP. Under the described settings, the main uptake of both phthalates was through inhalation. The results demonstrate the differences in uptake of gas and particles, and highlights the importance of considering the deposited dose in particle uptake studies.
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35.
  • Andersen, M. H. G., et al. (författare)
  • Exposure to Air Pollution inside Electric and Diesel-Powered Passenger Trains
  • 2019
  • Ingår i: Environmental Science & Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 53:8, s. 4579-4587
  • Tidskriftsartikel (refereegranskat)abstract
    • Diesel-powered trains are used worldwide for passenger transport. The present study aimed to assess air pollution concentrations in passenger cars from diesel and electric trains. Personal exposure monitoring (6-7 h per day) was carried out for 49 days on diesel and 22 days on electric trains. Diesel trains had higher concentrations of all the assessed air pollution components. Average increases (and fold differences) in passenger cars of diesel trains compared with electric trains were for ultrafine particles 212 000 particles/cm(3) (35-fold), black carbon 8.3 mu g/m(3) (6-fold), NOx 316 mu g/m(3) (8-fold), NO2 38 mu g/m(3) (3-fold), PM2.5 34 mu g/m(3) (2-fold), and benzo(a)pyrene 0.14 mu g/m(3) (6-fold). From time-series data, the pull and push movement modes, the engine in use, and the distance to the locomotive influenced the concentrations inside the diesel trains. In conclusion, concentrations of all air pollutants were significantly elevated in passenger cars in diesel trains compared to electric trains.
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36.
  • Anderson, Craig, 1976, et al. (författare)
  • Influence of in situ biofilm coverage on the radionuclide adsorption capacity of subsurface granite
  • 2007
  • Ingår i: Environmental Science & Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 41:3, s. 830-836
  • Tidskriftsartikel (refereegranskat)abstract
    • Any migration of radionuclides from nuclear waste repositories is expected to be mitigated by adsorption to the host rocks surrounding hydraulically conductive fractures. Fluid rock interfaces are considered to be important barriers for nuclear waste disposal schemes but their adsorptive capacity can be affected by the growth of microbial biofilms. This study indicates that biofilms growing on fracture surfaces decrease the rocks adsorption capacity for migrating radionuclides except for trivalent species. Potential suppression of adsorption by biofilms should, therefore, be accounted for in performance safety assessment models. In this study, the adsorptive capacity of in situ anaerobic biofilms grown 450 m underground on either glass or granite slides was compared to the capacity of the same surfaces without biofilms. Surfaces were exposed to the radiotracers Co-60(II), Pm-147(III), Am-241(III), Th-234(IV), and Np-237(V) for a period of 660 h in a pH neutral anaerobic synthetic groundwater. Adsorption was investigated at multiple time points over the 660 h using liquid scintillation and ICP-MS. Results indicate that these surfaces adsorb between 0 and 85% of the added tracers under the conditions of the specific experiments. After 660 h, the distribution coefficients, R (ratio between what is sorbed and what is left in the aqueous phase), approached 3 x 10(4) m for Co-60, 3 x 10(5) m for Pm-147 and 24 'Am, I x 106 m for 234Th, and 1 x 103 m for 237Np. The highest rate of adsorption was during the first 200 h of the adsorption experiments and started to approach equilibrium after 500 h. Adsorption to colloids and precipitates contributed to decreases of up to 20% in the available Co-60, Pm-147, Am-241, and Np-237 in the adsorption systems. In the 234Th system 95% of the aqueous 234Th was removed by adsorbing to colloids. Although the range of R values for each surface tested generally overlapped, the biofilms consistently demonstrated lower R values except for the trivalant Pm-147 and Am-241 adsorption systems.
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37.
  • Anderson, Maria, 1983, et al. (författare)
  • Particle- and Gaseous Emissions from an LNG Powered Ship
  • 2015
  • Ingår i: Environmental Science & Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 49:20, s. 12568-12575
  • Tidskriftsartikel (refereegranskat)abstract
    • Measurements of particle number and mass concentrations and number size distribution of particles from a ship running on liquefied natural gas (LNG) were made on-board a ship with dual-fuel engines installed. Today there is a large interest in LNG as a marine fuel, as a means to comply with sulfur and NOX regulations. Particles were studied in a wide size range together with measurements of other exhaust gases under different engine loads and different mixtures of LNG and marine gas oil. Results from these measurements show that emissions of particles, NOX, and CO2 are considerably lower for LNG compared to present marine fuel oils. Emitted particles were mainly of volatile character and mainly had diameters below 50 nm. Number size distribution for LNG showed a distinct peak at 9-10 nm and a part of a peak at diameter 6 nm and below. Emissions of total hydrocarbons and carbon monoxide are higher for LNG compared to present marine fuel oils, which points to the importance of considering the methane slip from combustion of LNG.
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38.
  • Andersson, August, et al. (författare)
  • Regionally-Varying Combustion Sources of the January 2013 Severe Haze Events over Eastern China
  • 2015
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 49:4, s. 2038-2043
  • Tidskriftsartikel (refereegranskat)abstract
    • Thick haze plagued northeastern China in January 2013, strongly affecting both regional climate and human respiratory health. Here, we present dual carbon isotope constrained (Delta C-14 and delta C-13) source apportionment for combustion-derived black carbon aerosol (BC) for three key hotspot regions (megacities): North China Plain (NCP, Beijing), the Yangtze River Delta (YRD, Shanghai), and the Pearl River Delta (PRD, Guangzhou) for January 2013. BC, here quantified as elemental carbon (EC), is one of the most health-detrimental components of PM2.5 and a strong climate warming agent. The results show that these severe haze events were equally affected (similar to 30%) by biomass combustion in all three regions, whereas the sources of the dominant fossil fuel component was dramatically different between north and south. In the NCP region, coal combustion accounted for 66% (46-74%, 95% C.I.) of the EC, whereas, in the YRD and PRD regions, liquid fossil fuel combustion (e.g., traffic) stood for 46% (18-66%) and 58% (38-68%), respectively. Taken together, these findings suggest the need for a regionally-specific description of BC sources in climate models and regionally-tailored mitigation to combat severe air pollution events in East Asia.
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39.
  • Andersson, Ronny, et al. (författare)
  • Calculating CO2 Uptake for Existing Concrete Structures during and after Service Life
  • 2013
  • Ingår i: Environmental Science & Technology. - : American Chemical Society (ACS). - 1520-5851 .- 0013-936X. ; 47:20, s. 11625-11633
  • Tidskriftsartikel (refereegranskat)abstract
    • This paper presents a model that can calculate the uptake of CO2 in all existing concrete structures, including its uptake after service life. This is important for the calculation of the total CO2 uptake in the society and its time dependence. The model uses the well-documented cement use and knowledge of how the investments are distributed throughout the building sector to estimate the stock of concrete applications in a country. The depth of carbonation of these applications is estimated using two models, one theoretical and one based on field measurements. The maximum theoretical uptake potential is defined as the amount of CO2 that is emitted during calcination at the production of Portland cement, but the model can also, with some adjustments, be used for the other cement types. The model has been applied on data from Sweden and the results show a CO2 uptake in 2011 in all existing structures of about 300 000 tonnes, which corresponds to about 17% of the total emissions (calcination and fuel) from the production of new cement for use in Sweden in the same year. The study also shows that in the years 2030 and 2050, an increase in the uptake in crushed concrete, from 12 000 tonnes today to 200 000 and 500 000 tonnes of CO2, respectively, could be possible if the waste handling is redesigned.
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40.
  • Andersson, Åse, 1971, et al. (författare)
  • Leaching of concrete admixtures containing thiocyanate and resin acids
  • 2001
  • Ingår i: Environmental Science & Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 35:4, s. 788-793
  • Tidskriftsartikel (refereegranskat)abstract
    • There is an increasing concern about the emission of pollutants during the construction and lifetime of buildings. The leaching of concrete admixtures containing thiocyanate and resin acids was studied using standard leaching tests and chemical analysis. Ecotoxicological risk was assessed for each admixture. Thiocyanate leaching from concrete, with a chlorine-free accelerating admixture, was determined by ion chromatography. Of the total amount of thiocyanate added, 6-8% was emitted within 30 d. The thiocyanate diffusion curve indicates a fast dissolution process from the surface layer, followed by a slower continuous diffusion process. Thiocyanate exhibits both acute and chronic toxicity, which makes it of immediate environmental concern. Resin acid leaching from concrete test specimens containing an admixture of air-entraining agents with tall oil was determined by solid-phase extraction, methylation, and GC/MS. Of added resin acids, 10% was emitted over 143 d. The leaching curves for the resin acids indicate a continuous diffusion that is proportional to the square root of time and follows Fick's first law of diffusion. The chemical composition of the resin acids in the leachate demonstrates degradation and rearrangement of the resin acids during diffusion. Resin acids emitted from concrete are of environmental concern because they are persistent and have the ability to bioaccumulate in aquatic organisms. | There is an increasing concern about the emission of pollutants during the construction and lifetime of buildings. The leaching of concrete admixtures containing thiocyanate and resin acids was studied using standard leaching tests and chemical analysis. Ecotoxicological risk was assessed for each admixture. Thiocyanate leaching from concrete, with a chlorine-free accelerating admixture, was determined by ion chromatography. Of the total amount of thiocyanate added, 6-8% was emitted within 30 d. The thiocyanate diffusion curve indicates a fast dissolution process from the surface layer, followed by a slower continuous diffusion process. Thiocyanate exhibits both acute and chronic toxicity, which makes it of immediate environmental concern. Resin acid leaching from concrete test specimens containing an admixture of air-entraining agents with tall oil was determined by solid-phase extraction, methylation, and GC/MS. Of added resin acids, 10% was emitted over 143 d. The leaching curves for the resin acids indicate a continuous diffusion that is proportional to the square root of time and follows Fick's first law of diffusion. The chemical composition of the resin acids in the leachate demonstrates degradation and rearrangement of the resin acids during diffusion. Resin acids emitted from concrete are of environmental concern because they are persistent and have the ability to bioaccumulate in aquatic organisms.
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41.
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42.
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43.
  • Armitage, James M, et al. (författare)
  • Comparative Assessment of the Global Fate and Transport Pathways of Long-chain Perfluorocarboxylic Acids (PFCAs) and Perfluorocarboxylates (PFCs) Emitted from Direct Sources
  • 2009
  • Ingår i: Environmental Science and Technology. - : American Chemical Society. - 0013-936X .- 1520-5851. ; 43:15, s. 5830-5836
  • Tidskriftsartikel (refereegranskat)abstract
    • A global-scale multispecies mass balance model was used to simulate the long-term fate and transport of perfluorocarboxylic acids (PFCAs) with eight to thirteen carbons (C8−C13) and their conjugate bases, the perfluorocarboxylates (PFCs). The main purpose of this study was to assess the relative long-range transport (LRT) potential of each conjugate pair, collectively termed PFC(A)s, considering emissions from direct sources (i.e., manufacturing and use) only. Overall LRT potential (atmospheric + oceanic) varied as a function of chain length and depended on assumptions regarding pKa and mode of entry. Atmospheric transport makes a relatively higher contribution to overall LRT potential for PFC(A)s with longer chain length, which reflects the increasing trend in the air−water partition coefficient (KAW) of the neutral PFCA species with chain length. Model scenarios using estimated direct emissions of the C8, C9, and C11 PFC(A)s indicate that the mass fluxes to the Arctic marine environment associated with oceanic transport are in excess of mass fluxes from indirect sources (i.e., atmospheric transport of precursor substances such as fluorotelomer alcohols and subsequent degradation to PFCAs). Modeled concentrations of C8 and C9 in the abiotic environment are broadly consistent with available monitoring data in surface ocean waters. Furthermore, the modeled concentration ratios of C8 to C9 are reconcilable with the homologue pattern frequently observed in biota, assuming a positive correlation between bioaccumulation potential and chain length. Modeled concentration ratios of C11 to C10 are more difficult to reconcile with monitoring data in both source and remote regions. Our model results for C11 and C10 therefore imply that either (i) indirect sources are dominant or (ii) estimates of direct emission are not accurate for these homologues.
  •  
44.
  • Armitage, James M, et al. (författare)
  • Modeling the Global Fate and Transport of Perfluorooctane Sulfonate (PFOS) and Precursor Compounds in Relation to Temporal Trends in Wildlife Exposure.
  • 2009
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 43:24, s. 9274-80
  • Tidskriftsartikel (refereegranskat)abstract
    • A global-scale fate and transport model was applied to investigate the historic and future trends in ambient concentrations of perfluorooctane sulfonate (PFOS) and volatile perfluorooctane sulfonyl fluoride (POSF)-based precursor compounds in the environment. First, a global emission inventory for PFOS and its precursor compounds was estimated for the period 1957-2010. We used this inventory as input to a global-scale contaminant fate model and compared modeled concentrations with field data. The main focus of the simulations was to examine how modeled concentrations of PFOS and volatile precursor compounds respond to the major production phase-out that occurred in 2000-2002. Modeled concentrations of PFOS in surface ocean waters are generally within a factor of 5 of field data and are dominated by direct emissions of this substance. In contrast, modeled concentrations of the precursor compounds considered in this study are lower than measured concentrations both before and after the production phase-out. Modeled surface ocean water concentrations of PFOS in source regions decline slowly in response to the production phase-out while concentrations in remote regions continue to increase until 2030. In contrast, modeled concentrations of precursor compounds in both the atmosphere and surface ocean water compartment in all regions respond rapidly to the production phase-out (i.e., decline quickly to much lower levels). With respect to wildlife biomonitoring data, since precursor compounds are bioavailable and degrade to PFOS in vivo, it is at least plausible that declining trends in PFOS body burdens observed in some marine organisms are attributable to this exposure pathway. The continued increases in PFOS body burdens observed in marine organisms inhabiting other regions may reflect exposure primarily to PFOS itself, present in the environment due to production and use of this compound as well as degradation of precursor compounds.
  •  
45.
  • Armitage, James M, et al. (författare)
  • Modeling the Global Fate and Transport of Perfluorooctanoic Acid (PFOA) and Perfluorooctanoate (PFO) Emitted from Direct Sources Using a Multispecies Mass Balance Model
  • 2009
  • Ingår i: Environmental Science and Technology. - : American Chemical Society. - 0013-936X .- 1520-5851. ; 43:4, s. 1134-1140
  • Tidskriftsartikel (refereegranskat)abstract
    • The global-scale fate and transport processes of perfluorooctanoic acid (PFOA) and perfluorooctanoate (PFO) emitted from direct sources were simulated using a multispecies mass balance model over the period 1950 to 2010. The main goal of this study was to assess the atmospheric and oceanic long-range transport potential of direct source emissions and the implications for the contamination of terrestrial and marine systems worldwide. Consistent with previous modeling studies, ocean transport was found to be the dominant pathway for delivering PFO(A) associated with direct sources to the Arctic marine environment, regardless of model assumptions. The modeled concentrations for surface ocean waters were insensitive to assumptions regarding physical−chemical properties and emission mode of entry and were in reasonable agreement with available monitoring data from the Northern Hemisphere. In contrast, model outputs characterizing atmospheric transport potential were highly sensitive to model assumptions, especially the assumed value of the acid dissociation constant (pKa). However, the complete range of model results for scenarios with different assumptions about partitioning and emissions provide evidence that the atmospheric transport of directly emitted PFO(A) can deliver this substance to terrestrial environments distant from sources. Additional studies in remote or isolated terrestrial systems may provide further insight into the scale of contamination actually attributable to direct sources.
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46.
  •  
47.
  • Arnoldsson, Kristina, et al. (författare)
  • Formation of environmentally relevant brominated dioxins from 2,4,6,-tribromophenol via bromoperoxidase-catalyzed dimerization
  • 2012
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 46:13, s. 7239-7244
  • Tidskriftsartikel (refereegranskat)abstract
    • Polybrominated dibenzo-p-dioxins (PBDD) are emerging environmental pollutants with structural similarities to the highly characterized toxicants polychlorinated dibenzo-p-dioxins. The geographical and temporal variations of PBDD in biota samples from the Baltic Sea do not display features that are normally related to anthropogenic sources such as incineration, and therefore the natural formation of PBDDs has been suggested. This study of the bromoperoxidase mediated oxidative coupling of 2,4,6-tribromophenol (an abundant substance that is naturally formed in marine systems) identified the formation of ppb-level yields of 1,3,6,8-tetrabromodibenzo-p-dioxin (1,3,6,8-TeBDD) through direct condensation. Additional TeBDDs (1,3,7,9-TeBDD, 1,2,4,7-TeBDD and/or 1,2,4,8-TeBDD) and tri-BDDs (1,3,7-TrBDD and 1,3,8-TrBDD) were frequently formed, but at lower yields. The formation of these TeBDDs probably proceeds via bromine shifts or Smiles rearrangements, while the TrBDDs may result from subsequent debromination processes. Since all of the congeners formed by oxidative coupling and subsequent reactions are also found in Baltic Sea biota, the results support the theory that PBDDs are formed from natural precursors.
  •  
48.
  • Arnoldsson, Kristina, et al. (författare)
  • Photochemical formation of polybrominated dibenzo-p-dioxins from environmentally abundant hydroxylated polybrominated diphenyl ethers
  • 2012
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 46:14, s. 7567-7574
  • Tidskriftsartikel (refereegranskat)abstract
    • High levels of polybrominated dibenzo-p-dioxins (PBDDs) have been found in Baltic Sea biota, where the toxic load owing to, for example, polychlorinated dibenzo-p-dioxins and other organic pollutants is already high. The levels and geographic pattern of PBDDs suggest biogenic rather than anthropogenic origin, and both biotic and abiotic formation pathways have been proposed. Photochemical formation from hydroxylated polybrominated diphenyl ethers (OH-PBDE) is a proposed pathway. for PBDDs in marine environments. Ultraviolet radiation-initiated transformations of OH-BDEs 47, 68, 85, 90, 99, and 123, which all are abundant in the environment, were investigated. It was shown that the most abundant PBDDs in the environment (1,3,7-triBDD and 1,3,8-triBDD) can be formed from the most abundant OH-BDEs (OH-BDE 47 and OH-BDE 68) at high rates and with percentage yields. In fact, most of the PBDDs that have been identified in the Baltic Sea environment were formed with high yield from the six studied OH-PBDE, through initial cyclization and subsequent debromination reactions. The high formation yields point to this route as an important source of PBDDs in biota. However, congeners showing relatively high retention in fish, specifically 1,3,6,8- and 1,3,7,9-tetraBDD, were not formed. These are likely formed by enzymatic coupling of brominated phenols.
  •  
49.
  • Arnot, Jon A., et al. (författare)
  • Toward a Consistent Evaluative Framework for POP Risk Characterization
  • 2011
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 45:1, s. 97-103
  • Tidskriftsartikel (refereegranskat)abstract
    • The purpose of Annex E in the Stockholm Convention (SC) on Persistent Organic Pollutants (POPs) is to assess whether a chemical is likely, as a result of its long-range environmental transport, to lead to significant adverse human health or environmental effects, such that global action is warranted. To date, risk profiles for nominated POPs have not consistently selected assessment endpoints or completed mandated risk characterizations. An assessment endpoint hierarchy is proposed to facilitate risk characterization for the implementation of the SC. The framework is illustrated for a nominated POP, hexabromocyclododecane (HBCD), using three risk estimation methods. Based on current monitoring and toxicity data, the screening-level results indicate that humans and ecological receptors in remote regions such as the Arctic are unlikely to experience significant adverse effects (i.e., low risk) due to long-range environmental transport of HBCD. The results for birds are more uncertain than the results for fish and mammals due to the paucity of avian toxicity data. Risk characterization results for HBCD and for some listed POPs are compared to illustrate how the proposed methods can further assist decision-making and chemical management.
  •  
50.
  • Aro, Rudolf, 1992-, et al. (författare)
  • Organofluorine Mass Balance Analysis of Whole Blood Samples in Relation to Gender and Age
  • 2021
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 55:19, s. 13142-13151
  • Tidskriftsartikel (refereegranskat)abstract
    • Studies have highlighted the increasing fraction of unidentified organofluorine (UOF) compounds in human blood, whose health effects are not known. In this study, 130 whole blood samples from the Swedish general population were analyzed for extractable organofluorine (EOF) and selected per- and polyfluoroalkyl substances (PFAS). Organofluorine mass balance analysis revealed that 60% (0-99%) of the EOF in female samples could not be explained by the 63 monitored PFAS; in males, 41% (0-93%) of the EOF was of unidentified origin. Significant differences between both age groups and gender were seen, with the highest fraction of UOF in young females (70% UOF, aged 18-44), which is contrary to what has been reported in the literature for commonly monitored compounds (e.g., perfluorooctane sulfonic acid, PFOS). Increasing the number of monitored PFAS did not lead to a large decrease of the UOF fraction; the seven highest PFAS (C8-C11 PFCAs, C6-C8 PFSAs) accounted for 98% of sum 63 PFAS. The high fraction of UOF in human samples is of concern, as the chemical species of these organofluorine compounds remain unknown and thus their potential health risks cannot be assessed.
  •  
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