Elemental and water-insoluble organic carbon in Svalbard snow: a synthesis of observations during 2007-2018

Zdanowicz, C; Gallet, JC; Bjorkman, MP; Larose, C; Schuler, T; Luks, B; Koziol, K; Spolaor, A; Barbaro, E; Martma, T; van Pelt, W; Wideqvist, U; Strom, J
2021 | Atmos. Chem. Phys. | 21 (4) (3035-3057)
Light-absorbing carbonaceous aerosols emitted by biomass or fossil fuel combustion can contribute to amplifying Arctic climate warming by lowering the albedo of snow. The Svalbard archipelago, being near to Europe and Russia, is particularly affected by these pollutants, and improved knowledge of their distribution in snow is needed to assess their impact. Here we present and synthesize new data obtained on Svalbard between 2007 and 2018, comprising measurements of elemental (EC) and water-insoluble organic carbon (WIOC) in snow from 37 separate sites. We used these data, combined with meteorological data and snowpack modeling, to investigate the variability of EC and WIOC deposition in Svalbard snow across latitude, longitude, elevation and time. Overall, EC concentrations (C-snow(EC)) ranged from < 1.0 to 266.6 ng g(-1), while WIOC concentrations (C-snow(WIOC)) ranged from < 1 to 9426 ng g(-1), with the highest values observed near Ny-Alesund. Calculated snowpack loadings (L-snow(EC), L-snow(WIOC)) on glaciers surveyed in spring 2016 were 0.1 to 2.6 mg m(-2) and 2 to 173 mg m(-2), respectively. The median C-snow(EC) and the L-snow(EC) on those glaciers were close to or lower than those found in earlier (2007- 2009), comparable surveys. Both L-snow(EC) and L(snow)(WIOC )increased with elevation and snow accumulation, with dry deposition likely playing a minor role. Estimated area-averaged snowpack loads across Svalbard were 1.1 mg EC m(-2) and 38.3 mg WIOC m(-2) for the 2015-2016 winter. An similar to 11-year long dataset of spring surface snow measurements from the central BrOgger Peninsula was used to quantify the interannual variability of EC and WIOC deposition in snow. In most years, C-snow(EC) and C-snow(WIOC) at Ny-Alesund (50 m a.s.l.) were 2-5 times higher than on the nearby Austre Brogger-breen glacier (456 m a.s.l.), and the median EC/WIOC in Ny-Alesund was 6 times higher, suggesting a possible influence of local EC emission from Ny-Alesund. While no long-term trends between 2011 and 2018 were found, C-snow(EC) and C-snow(WIOC) showed synchronous variations at Ny-Alesund and Austre Broggerbreen. When compared with data from other circum-Arctic sites obtained by comparable methods, the median C(snow)(EC)on Svalbard falls between that found in central Greenland (lowest) and those in continental sectors of European Arctic (northern Scandinavia, Russia and Siberia; highest), which is consistent with large-scale patterns of BC in snow reported by surveys based on other methods.

Rapid in-plate screening of biotransformation products in single zebrafish embryos

Ribbenstedt, A; Benskin, JP
2021 | RSC Adv | 11 (45) (27812-27819)
chemicals , danio-rerio , dog , fate , ms/ms , pharmaceuticals , propranolol metabolism , toxicokinetics , urine , water treatment plants
A procedure was developed for rapid screening of xenobiotic biotransformation products (bioTPs) in single zebrafish (ZF; Danio rerio) embryos. Exposure was carried out from 0-120 hours post fertilization (hpf) to 6 different concentrations of the model compound propranolol (PPL). Following in-plate extraction and non-target instrumental analysis by high resolution mass spectrometry, suspected bioTPs were identified using custom data filtration scripts and matching to in silico structural predictions. A total of eight PPL bioTPs were identified (five at a level 1 confidence and one at a level 2-3 confidence). These findings supplement previously generated toxicometabolomic models derived from the same dataset, and were obtained without conducting additional exposure experiments. In addition to facilitating assessments of inter-individual variability in bioTP production in ZF embryos, we demonstrate that bioTPs can be elucidated using extremely small quantities of biomass (i.e. similar to 200 mu g). To the best of our knowledge, this is the first time bioTP elucidation has been carried out in single ZF embryos.

Eight years of sub-micrometre organic aerosol composition data from the boreal forest characterized using a machine-learning approach

Heikkinen, L; Aijala, M; Daellenbach, KR; Chen, G; Garmash, O; Aliaga, D; Graeffe, F; Raty, M; Luoma, K; Aalto, P; Kulmala, M; Petaja, T; Worsnop, D; Ehn, M
2021 | Atmos. Chem. Phys. | 21 (13) (10081-10109)
chemistry , components , data sets , emissions , model , pollution , positive matrix factorization , secondary , source apportionment , uncertainty
The Station for Measuring Ecosystem-Atmosphere Relations (SMEAR) II, located within the boreal forest of Finland, is a unique station in the world due to the wide range of long-term measurements tracking the Earth-atmosphere interface. In this study, we characterize the composition of organic aerosol (OA) at SMEAR II by quantifying its driving constituents. We utilize a multi-year data set of OA mass spectra measured in situ with an Aerosol Chemical Speciation Monitor (ACSM) at the station. To our knowledge, this mass spectral time series is the longest of its kind published to date. Similarly to other previously reported efforts in OA source apportionment from multi-seasonal or multi-annual data sets, we approached the OA characterization challenge through positive matrix factorization (PMF) using a rolling window approach. However, the existing methods for extracting minor OA components were found to be insufficient for our rather remote site. To overcome this issue, we tested a new statistical analysis framework. This included unsupervised feature extraction and classification stages to explore a large number of unconstrained PMF runs conducted on the measured OA mass spectra. Anchored by these results, we finally constructed a relaxed chemical mass balance (CMB) run that resolved different OA components from our observations. The presented combination of statistical tools provided a data-driven analysis methodology, which in our case achieved robust solutions with minimal subjectivity. Following the extensive statistical analyses, we were able to divide the 2012-2019 SMEAR II OA data (mass concentration interquartile range (IQR): 0.7, 1.3, and 2.6 mu gm(-3)) into three sub-categories - low-volatility oxygenated OA (LV-OOA), semi-volatile oxygenated OA (SV-OOA), and primary OA (POA) - proving that the tested methodology was able to provide results consistent with literature. LV-OOA was the most dominant OA type (organic mass fraction IQR: 49 %, 62 %, and 73 %). The seasonal cycle of LV-OOA was bimodal, with peaks both in summer and in February. We associated the wintertime LV-OOA with anthropogenic sources and assumed biogenic influence in LV-OOA formation in summer. Through a brief trajectory analysis, we estimated summertime natural LV-OOA formation of tens of ngm 3 h 1 over the boreal forest. SV-OOA was the second highest contributor to OA mass (organic mass fraction IQR: 19 %, 31 %, and 43 %). Due to SV-OOA's clear peak in summer, we estimate biogenic processes as the main drivers in its formation. Unlike for LV-OOA, the highest SV-OOA concentrations were detected in stable summertime nocturnal surface layers. Two nearby sawmills also played a significant role in SV-OOA production as also exemplified by previous studies at SMEAR II. POA, taken as a mix of two different OA types reported previously, hydrocarbon-like OA (HOA) and biomass burning OA (BBOA), made up a minimal OA mass fraction (IQR: 2 %, 6 %, and 13 %). Notably, the quantification of POA at SMEAR II using ACSM data was not possible following existing rolling PMF methodologies. Both POA organic mass fraction and mass concentration peaked in winter. Its appearance at SMEAR II was linked to strong southerly winds. Similar wind direction and speed dependence was not observed among other OA types. The high wind speeds probably enabled the POA transport to SMEAR II from faraway sources in a relatively fresh state. In the event of slower wind speeds, POA likely evaporated and/or aged into oxidized organic aerosol before detection. The POA organic mass fraction was significantly lower than reported by aerosol mass spectrometer (AMS) measurements 2 to 4 years prior to the ACSM measurements. While the co-located long-term measurements of black carbon supported the hypothesis of higher POA loadings prior to year 2012, it is also possible that short-term (POA) pollution plumes were averaged out due to the slow time resolution of the ACSM combined with the further 3 h data averaging needed to ensure good signal-to-noise ratios (SNRs). Despite the length of the ACSM data set, we did not focus on quantifying long-term trends of POA (nor other components) due to the high sensitivity of OA composition to meteorological anomalies, the occurrence of which is likely not normally distributed over the 8-year measurement period. Due to the unique and realistic seasonal cycles and meteorology dependences of the independent OA subtypes complemented by the reasonably low degree of unexplained OA variability, we believe that the presented data analysis approach performs well. Therefore, we hope that these results encourage also other researchers possessing several-yearlong time series of similar data to tackle the data analysis via similar semi- or unsupervised machine-learning approaches. This way the presented method could be further optimized and its usability explored and evaluated also in other environments.

Hyporheic exchange in recirculating flumes under heterogeneous bacterial and morphological conditions

Betterle, A; Jaeger, A; Posselt, M; Coll, C; Benskin, JP; Schirmer, M
2021 | Environ. Earth Sci. | 80 (6)
biodegradation , hyporheic exchange , hyporheic zone , modelling , pollutants , surface water porewater interaction
Hyporheic exchange (HE) contributes to the biogeochemical turnover of macro- and micro-pollutants in rivers. However, the spatiotemporal complexity and variability of HE hinder understanding of its role in the overall functioning of riverine ecosystems. The present study focuses on investigating the role of bacterial diversity and sediment morphology on HE using a multi-flume experiment. A fully coupled surface-subsurface numerical model was used to highlight complex exchange patterns between surface water and the underlying flow field in the sediments. Under the experimental conditions, the surface water flow induced by bedforms has a prominent effect on both local trajectories and residence time distributions of hyporheic flow paths, whereas mean hyporheic retention times are mainly modulated by average surface flowrates. In case of complex bedform morphologies, the numerical model successfully reproduces the HE estimated by means of salt dilution tests. However, the 2D numerical representation of the system falls short in predicting HE in absence of bedforms, highlighting the intrinsic complexity of water circulation patterns in real scenarios. Finally, results show that higher bacterial diversities in the stream sediments can significantly reduce hyporheic fluxes. This work provides a framework to interpret micropollutants turnover in light of the underlying physical transport processes in the hyporheic zone. The study emphasizes the importance of better understanding the tradeoff between physically driven transport processes and bacterial dynamics in the hyporheic zone to quantify the fate of pollutants in streams and rivers.

When science and politics come together: From depletion to recovery of the stratospheric ozone hole This article belongs to Ambio’s 50th Anniversary Collection. Theme: Ozone Layer

2021 | Ambio | 50 (1) (31-34)

Adult female European perch (Perca fluviatilis) from the Baltic Sea show no evidence of thiamine deficiency

Gustafsson, J; Strom, K; Arvstrand, L; Forlin, L; Asplund, L; Balk, L
2021 | J. Sea Res. | 174
apoenzyme , fish , fluviatilis , health , polybrominated diphenyl ethers , seasonal variation , transketolase , vitamin b-1
Deficiency of thiamine (vitamin B1) has been demonstrated in several species in the northern hemisphere and is suggested as a cause for declining populations. European perch from the Baltic Sea show negative temporal trends for several health biomarkers and poor recruitment of unknown cause. In this study, thiamine status of perch liver from the Baltic Sea was studied with emphasis on seasonal variation. During spring the thiamine concentration increased, reached a higher level during the summer and then decreased again during autumn. Despite this variation the thiamine concentration was always sufficient in the perch liver. These results indicate that direct thiamine deficiency is an unlikely explanation for the health effects observed in adult female perch from the Baltic Sea.

Risk-based prioritization of suspects detected in riverine water using complementary chromatographic techniques

Been, F; Kruve, A; Vughs, D; Meekel, N; Reus, A; Zwartsen, A; Wessel, A; Fischer, A; Ter Laak, T; Brunner, AM
2021 | Water Res. | 204
chemical water quality , chemicals , chromatography , data science , drinking water , hrms , ionization efficiency , non-target screening , organic micropollutants , surface water
Surface waters are widely used as drinking water sources and hence their quality needs to be continuously monitored. However, current routine monitoring programs are not comprehensive as they generally cover only a limited number of known pollutants and emerging contaminants. This study presents a risk-based approach combining suspect and non-target screening (NTS) to help extend the coverage of current monitoring schemes. In particular, the coverage of NTS was widened by combining three complementary separations modes: Reverse phase (RP), Hydrophilic interaction liquid chromatography (HILIC) and Mixed-mode chromatography (MMC). Suspect lists used were compiled from databases of relevant substances of very high concern (e.g., SVHCs) and the concentration of detected suspects was evaluated based on ionization efficiency prediction. Results show that suspect candidates can be prioritized based on their potential risk (i.e., hazard and exposure) by combining ionization efficiency-based concentration estimation, in vitro toxicity data or, if not available, structural alerts and QSAR.based toxicity predictions. The acquired information shows that NTS analyses have the potential to complement target analyses, allowing to update and adapt current monitoring programs, ultimately leading to improved monitoring of drinking water sources.

Is Exposure to BMAA a Risk Factor for Neurodegenerative Diseases? A Response to a Critical Review of the BMAA Hypothesis

Dunlop, RA; Banack, SA; Bishop, SL; Metcalf, JS; Murch, SJ; Davis, DA; Stommel, EW; Karlsson, O; Brittebo, EB; Chatziefthimiou, AD; Tan, VX; Guillemin, GG; Cox, PA; Mash, DC; Bradley, WG
2021 | Neurotox Res | 39 (1) (81-106)
als , als/pdc , bmaa , cyanobacteria , neurodegeneration , neurodegenerative diseases
In a literature survey, Chernoff et al. (2017) dismissed the hypothesis that chronic exposure to beta-N-methylamino-L-alanine (BMAA) may be a risk factor for progressive neurodegenerative disease. They question the growing scientific literature that suggests the following: (1) BMAA exposure causes ALS/PDC among the indigenous Chamorro people of Guam; (2) Guamanian ALS/PDC shares clinical and neuropathological features with Alzheimer's disease, Parkinson's disease, and ALS; (3) one possible mechanism for protein misfolds is misincorporation of BMAA into proteins as a substitute for L-serine; and (4) chronic exposure to BMAA through diet or environmental exposures to cyanobacterial blooms can cause neurodegenerative disease. We here identify multiple errors in their critique including the following: (1) their review selectively cites the published literature; (2) the authors reported favorably on HILIC methods of BMAA detection while the literature shows significant matrix effects and peak coelution in HILIC that may prevent detection and quantification of BMAA in cyanobacteria; (3) the authors build alternative arguments to the BMAA hypothesis, rather than explain the published literature which, to date, has been unable to refute the BMAA hypothesis; and (4) the authors erroneously attribute methods to incorrect studies, indicative of a failure to carefully consider all relevant publications. The lack of attention to BMAA research begins with the review's title which incorrectly refers to BMAA as a "non-essential" amino acid. Research regarding chronic exposure to BMAA as a cause of human neurodegenerative diseases is emerging and requires additional resources, validation, and research. Here, we propose strategies for improvement in the execution and reporting of analytical methods and the need for additional and well-executed inter-lab comparisons for BMAA quantitation. We emphasize the need for optimization and validation of analytical methods to ensure that they are fit-for-purpose. Although there remain gaps in the literature, an increasingly large body of data from multiple independent labs using orthogonal methods provides increasing evidence that chronic exposure to BMAA may be a risk factor for neurological illness.

Precursors and Pathways Leading to Enhanced Secondary Organic Aerosol Formation during Severe Haze Episodes

Zheng, Y; Chen, Q; Cheng, X; Mohr, C; Cai, J; Huang, W; Shrivastava, M; Ye, PL; Fu, PQ; Shi, XD; Ge, YL; Liao, KR; Miao, RQ; Qiu, XH; Koenig, TK; Chen, SY
2021 | Environ. Sci. Technol. | 55 (23) (15680-15693)
alpha-dicarbonyls , anthropogenic emissions , aqueous processing , aqueous-phase photooxidation , atmospheric aerosols , chemical composition , dicarboxylic acid , dicarboxylic-acids , fine particulate matter , haze , molecular composition , nitrated phenols , organic nitrates , oxocarboxylic acids , positive matrix factorization , soa
Molecular analyses help to investigate the key precursors and chemical processes of secondary organic aerosol (SOA) formation. We obtained the sources and molecular compositions of organic aerosol in PM2.5 in winter in Beijing by online and offline mass spectrometer measurements. Photochemical and aqueous processing were both involved in producing SOA during the haze events. Aromatics, isoprene, long-chain alkanes or alkenes, and carbonyls such as glyoxal and methylglyoxal were all important precursors. The enhanced SOA formation during the severe haze event was predominantly contributed by aqueous processing that was promoted by elevated amounts of aerosol water for which multifunctional organic nitrates contributed the most followed by organic compounds having four oxygen atoms in their formulae. The latter included dicarboxylic acids and various oxidation products from isoprene and aromatics as well as products or oligomers from methylglyoxal aqueous uptake. Nitrated phenols, organosulfates, and methanesulfonic acid were also important SOA products but their contributions to the elevated SOA mass during the severe haze event were minor. Our results highlight the importance of reducing nitrogen oxides and nitrate for future SOA control. Additionally, the formation of highly oxygenated long-chain molecules with a low degree of unsaturation in polluted urban environments requires further research.

Novel 4-Hydroxybenzyl Adducts in Human Hemoglobin: Structures and Mechanisms of Formation

Rajczewski, AT; Ndreu, L; Pujari, SS; Griffin, TJ; Tornqvist, MA; Karlsson, I; Tretyakova, NY
2021 | Chem. Res. Toxicol. | 34 (7) (1769-1781)
cysteine residues , dna adducts , identification , liver , n-terminal valine , p-cresol , protein cross-linking , quinone methide , serum-albumin , strategy
Humans are exposed to large numbers of electrophiles from their diet, the environment, and endogenous physiological processes. Adducts formed at the N-terminal valine of hemoglobin are often used as biomarkers of human exposure to electrophilic compounds. We previously reported the formation of hemoglobin N-terminal valine adducts (added mass, 106.042 Da) in the blood of human smokers and nonsmokers and identified their structure as 4-hydroxybenzyl-Val. In the present work, mass spectrometry-based proteomics was utilized to identify additional sites for 4-hydroxybenzyl adduct formation at internal nucleophilic amino acid side chains within hemoglobin. Hemoglobin isolated from human blood was treated with para-quinone methide (para-QM) followed by global nanoLC-MS/MS and targeted nanoLC-MS/MS to identify amino acid residues containing the 4-hydroxybenzyl modification. Our experiments revealed the formation of 4-hydroxybenzyl adducts at the alpha His20, alpha Tyr24, alpha Tyr42, alpha His45, beta Ser72, beta Thr84, beta Thr87, beta Ser89, beta His92, beta Cys93, beta Cys112, beta Thr123, and beta His143 residues (in addition to N-terminal valine) through characteristic MS/MS spectra. These amino acid side chains had variable reactivity toward para-QM with alpha His45, alpha Tyr42, beta Cys93, beta His92, and beta Ser72 forming the largest numbers of adducts upon exposure to para-QM. Two additional mechanisms for formation of 4-hydroxybenzyl adducts in humans were investigated: exposure to 4-hydroxybenzaldehyde (4-HBA) followed by reduction and UV-mediated reactions of hemoglobin with tyrosine. Exposure of hemoglobin to a 5-fold molar excess of 4-HBA followed by reduction with sodium cyanoborohydride produced 4-hydroxybenzyl adducts at several amino acid side chains of which alpha His20, alpha Tyr24, alpha Tyr42, alpha His45, beta Ser44, beta Thr84, and beta His92 were verified in targeted mass spectrometry experiments. Similarly, exposure of human blood to ultraviolet radiation produced 4-hydroxybenzyl adducts at alpha His20, alpha Tyr24, alpha Tyr42, alpha His45, beta Ser44, beta Thr84, and beta Ser89. Overall, our results reveal that 4-hydroxybenzyl adducts form at multiple nucleophilic sites of hemoglobin and that para-QM is the most likely source of these adducts in humans.

Bioaccumulation of Per- and polyfluoroalkyl substances (PFASs) in a tropical estuarine food web

Miranda, DA; Benskin, JP; Awad, R; Lepoint, G; Leonel, J; Hatje, V
2021 | Sci. Total Environ. | 754
biomagnification , brazil , os-santos bay , perfluorinated compounds , perfluoroalkyl acids pfaas , perfluorooctane sulfonate , persistent organic pollutants , pfos precursors , pops , sulfluramid use , tissue distribution , todos os santos bay , trace-metal contamination , trophic magnification factors , tropical food web
The biomagnification of per- and polyfluoroalkyl substances (PFASs) was investigated in a tropical mangrove food web from an estuary in Bahia, Brazil. Samples of 44 organisms (21 taxa), along with biofilm, leaves, sediment and suspended particulate matter were analyzed. Sum (Sigma) PFAS concentrations in biota samples were dominated by perfluorooctane sulfonate (PFOS, 93% detection frequency in tissues; 0.05 to 1.97 ng g(-1) ww whole-body (wb)), followed by perfluorotridecanoate (PFTrDA, 57%; 0.01 to 0.28 ng g(-1) ww wb). PFOS precursors such as perfluorooctane sulfonamide (FOSA, 54%; 0.01 to 0.32 ng g(-1) ww wb) and N-ethyl perfluorooctane sulfonamide (EtFOSA; 30%; 0.01 to 0.21 ng g(-1) ww wb) were also detected. PFAS accumulation profiles revealed different routes of exposure among bivalve, crustacean and fish groups. Statistics for left-censored data were used in order to minimize bias on trophic magnification factors (TMFs) calculations. TMFs >1 were observed for PFOS (linear + branched isomers), EtFOSA (linear + branched isomers), and perfluorononanoate (PFNA), and in all cases, dissimilar accumulation patterns were observed among different trophic positions. The apparent biodilution of some long-chain PFCAs through the food chain (TMF < 1) may be due to exposure from multiple PFAS sources. This is the first study investigating bioaccumulation of PFASs in a tropical food web and provides new insight on the behavior of this ubiquitous class of contaminants. (C) 2020 The Authors. Published by Elsevier B.V.

Long-term exposure to particulate air pollution and black carbon in relation to natural and cause-specific mortality: a multicohort study in Sweden

Sommar, JN; Andersson, EM; Andersson, N; Sallsten, G; Stockfelt, L; Ljungman, PLS; Segersson, D; Eneroth, K; Gidhagen, L; Molnar, P; Wennberg, P; Rosengren, A; Rizzuto, D; Leander, K; Lager, A; Magnusson, PKE; Johansson, C; Barregard, L; Bellander, T; Pershagen, G; Forsberg, B
2021 | BMJ Open | 11 (9)
associations , cardiac epidemiology , cardiovascular-disease , cohorts , coupled road dust , emissions , epidemiology , goteborg , lung-cancer , matter , particles , public health , surface moisture model
Objectives To estimate concentration-response relationships for particulate matter (PM) and black carbon (BC) in relation to mortality in cohorts from three Swedish cities with comparatively low pollutant levels. Setting Cohorts from Gothenburg, Stockholm and Umea, Sweden. Design High-resolution dispersion models were used to estimate annual mean concentrations of PM with aerodynamic diameter <= 10 mu m (PM10) and <= 2.5 mu m (PM2.5), and BC, at individual addresses during each year of follow-up, 1990-2011. Moving averages were calculated for the time windows 1-5 years (lag1-5) and 6-10 years (lag6-10) preceding the outcome. Cause-specific mortality data were obtained from the national cause of death registry. Cohort-specific HRs were estimated using Cox regression models and then meta-analysed including a random effect of cohort. Participants During the study period, 7 340 cases of natural mortality, 2 755 cases of cardiovascular disease (CVD) mortality and 817 cases of respiratory and lung cancer mortality were observed among in total 68 679 individuals and 689 813 person-years of follow-up. Results Both PM10 (range: 6.3-41.9 mu g/m(3)) and BC (range: 0.2-6.8 mu g/m(3)) were associated with natural mortality showing 17% (95% CI 6% to 31%) and 9% (95% CI 0% to 18%) increased risks per 10 mu g/m(3) and 1 mu g/m(3) of lag1-5 exposure, respectively. For PM2.5 (range: 4.0-22.4 mu g/m(3)), the estimated increase was 13% per 5 mu g/m(3), but less precise (95% CI -9% to 40%). Estimates for CVD mortality appeared higher for both PM10 and PM2.5. No association was observed with respiratory mortality. Conclusion The results support an effect of long-term air pollution on natural mortality and mortality in CVD with high relative risks also at low exposure levels. These findings are relevant for future decisions concerning air quality policies.

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