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Wastewater is a major reservoir for chemical contaminants, both anthropogenic and biogenic. Recent chemical and toxicological analysis reveals the abundance and impact of these compounds, often termed contaminants of emerging concern (CECs). Concurrently, incomplete removal of these compounds in wastewater treatment plants sets a precedent for detailed characterisation and monitoring of such substances. Although liquid chromatography (LC) is frequently used for analysis of CECs in wastewater, gas chromatography (GC) maintains its significance for non-polar to mid-polar analytes. GC offers advantages such as increased separation efficiency, fewer matrix effects, and greater availability and reliability of reference mass spectra compared to LC. Comprehensive two-dimensional gas chromatography (GC × GC) delivers unmatched peak capacity and separational capabilities, critical in the resolution of diverse compound groups present within wastewater. When coupled with high resolution mass spectrometry, it provides a powerful identification tool with spectral databases and both 1st and 2nd dimensional retention indices, and has allowed for the separation, reliable annotation and characterisation of diverse CECs within wastewater in recent years. Herein, on the basis of recent studies from the last fifteen years, we outline cutting-edge methodologies and strategies for wastewater analysis using GC × GC. This includes sample preparation, derivatization of polar analytes, instrumental setup, and data analysis, ultimately providing the reader a framework for future non-targeted analysis of wastewater and other complex environmental matrices., Competing Interests: Declaration of competing interest The authors declare the following financial interests/personal relationships which may be considered as potential competing interests:Jason Devers reports financial support was provided by Innovation Fund Denmark. Jason Devers reports financial support was provided by Horizon Europe. Jan H Christensen reports financial support was provided by Innovation Fund Denmark. Jan H Christensen reports financial support was provided by Horizon Europe. If there are other authors, they declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 The Authors. Published by Elsevier B.V. All rights reserved.)

Due to the decoupling of the first ( 1 D) and second ( 2 D) dimension in pulsed elution-LC × LC (PE-LC × LC), method development is more flexible and straightforward compared to fast comprehensive LC × LC where the dependencies of key parameters between the two dimensions limits its flexibility. In this study we present a method for pulse generation, which is based on a switching valve alternating between one pump that delivers the gradient and a second pump that delivers low eluotrophic strength for the pause state. Consequently, the dwell volume of the system was circumvented and 7.5, and 3.75 times shorter pulse widths could be generated at flow rates of 0.2, and 0.4 mL/min with satisfactory accuracies between programmed and observed mobile phase composition (relative deviation of 6.0 %). We investigated how key parameters including pulse width and step height, 2 D gradient time and flow rate affected the peak capacity in PE-LC × LC. The conditions yielding the highest peak capacity for the PE-LC × LC- high-resolution mass spectrometry (HRMS) system were applied to a wastewater effluent sample. The results were compared to a one dimensional (1D)-LC-HRMS chromatogram. The peak capacity increased with a factor 34 from 112 for the 1D-LC run to 3770 for PE-LC × LC-HRMS after correction for undersampling. The analysis time for PE-LC × LC-HRMS was 12.1 h compared to 67.5 min for the 1D-LC-HRMS run. The purity of the mass spectra improved for PE-LC × LC-HRMS by a factor 2.6 (p-value 3.3 × 10 -6 ) and 2.0 (p-value 2.5 × 10 -3 ) for the low and high collision energy trace compared to the 1D-LC-HRMS analysis. Furthermore, the signal-to-noise ratio (S/N) was 4.2 times higher (range: 0.06-56.7, p-value 3.8 × 10 -2 ) compared to the 1D-LC-HRMS separation based on 42 identified compounds. The improvements in S/N were explained by the lower peak volume obtained in the PE-LC × LC-HRMS., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024. Published by Elsevier B.V.)

Matrix effects can affect detection limits, precision, and accuracy and lead to signal enhancement or suppression effects in gas chromatography analysis. Analyte protectants, such as shikimic acid and gluconolactone, can imitate the effect of matrix components and reduce the differences in matrix effect between samples. This study aimed to investigate the ability of analyte protectants to enhance gas chromatography detector signals of different oxygenated-polycyclic aromatic hydrocarbons. Addition of 100 μg L -1 shikimic acid and 200 μg L -1 gluconolactone effectively enhanced detector response of the investigated target compounds. Addition of a higher content of analyte protectants did not result in any further enhancement. It was found that between four and eleven consecutive injections of a standard solution with analyte protectants were required to obtain a stable compound response. The long-term signal stability was then maintained with subsequent injections, though an overall negative drift of the system was observed over the sequence of 200 investigated injections. Analysis of the actual sample matrix instead of standards in pure solvent, as presented in this study, could also be a way to minimize the required number of injections. Shikimic acid and gluconolactone were first and foremost able to enhance signals of oxygenated-polycyclic aromatic hydrocarbons with similar functional groups (hydroxyl) in their molecular structure. It can be relevant to consider alternative analyte protectants with different functional groups according to the type of target compounds investigated., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 The Authors. Published by Elsevier B.V. All rights reserved.)

Affected by both future anthropogenic emissions and climate change, future prediction of PM 2.5 and its Oxidative Potential (OP) distribution is a significant challenge, especially in developing countries like China. To overcome this challenge, we estimated historical and future PM 2.5 concentrations and associated OP using the Danish Eulerian Hemispheric Model (DEHM) system with meteorological input from WRF weather forecast model. Considering different future socio-economic pathways and emission scenario assumptions, we quantified how the contribution from various anthropogenic emission sectors will change under these scenarios. Results show that compared to the CESM_SSP2-4.5_CLE scenario (based on moderate radiative forcing and Current Legislation Emission), the CESM_SSP1-2.6_MFR scenario (based on sustainability development and Maximum Feasible Reductions) is projected to yield greater environmental and health benefits in the future. Under the CESM_SSP1-2.6_MFR scenario, annual average PM 2.5 concentrations (OP) are expected to decrease to 30 (0.8 nmolmin -1 m -3 ) in almost all regions by 2030, which will be 65 % (67 %) lower than that in 2010. From a long-term perspective, it is anticipated that OP in the Fen-Wei Plain region will experience the maximum reduction (82.6 %) from 2010 to 2049. Largely benefiting from the effective control of PM 2.5 in the region, it has decreased by 82.1 %. Crucially, once emission reduction measures reach a certain level (in 2040), further reductions become less significant. This study also emphasized the significant role of secondary aerosol formation and biomass-burning sources in influencing OP during both historical and future periods. In different scenarios, the reduction range of OP from 2010 to 2049 is estimated to be between 71 % and 85 % by controlling precursor emissions involved in secondary aerosol formation and emissions from biomass burning. Results indicate that strengthening the control of anthropogenic emissions in various regions are key to achieving air quality targets and safeguarding human health in the future., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier B.V. All rights reserved.)

Detailed spatial models of monthly air pollution levels at a very fine spatial resolution (25 m) can help facilitate studies to explore critical time-windows of exposure at intermediate term. Seasonal changes in air pollution may affect both levels and spatial patterns of air pollution across Europe. We built Europe-wide land-use regression (LUR) models to estimate monthly concentrations of regulated air pollutants (NO 2 , O 3 , PM 10 and PM 2.5 ) between 2000 and 2019. Monthly average concentrations were collected from routine monitoring stations. Including both monthly-fixed and -varying spatial variables, we used supervised linear regression (SLR) to select predictors and geographically weighted regression (GWR) to estimate spatially-varying regression coefficients for each month. Model performance was assessed with 5-fold cross-validation (CV). We also compared the performance of the monthly LUR models with monthly adjusted concentrations. Results revealed significant monthly variations in both estimates and model structure, particularly for O 3 , PM 10 , and PM 2.5 . The 5-fold CV showed generally good performance of the monthly GWR models across months and years (5-fold CV R 2 : 0.31-0.66 for NO 2 , 0.4-0.79 for O 3 , 0.4-0.78 for PM 10 , 0.46-0.87 for PM 2.5 ). Monthly GWR models slightly outperformed monthly-adjusted models. Correlations between monthly GWR model were generally moderate to high (Pearson correlation >0.6). In conclusion, we are the first to develop robust monthly LUR models for air pollution in Europe. These monthly LUR models, at a 25 m spatial resolution, enhance epidemiologists to better characterize Europe-wide intermediate-term health effects related to air pollution, facilitating investigations into critical exposure time windows in birth cohort studies., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 The Authors. Published by Elsevier B.V. All rights reserved.)

Objectives: The association between air pollution and risk of respiratory tract infection (RTI) in adults needs to be clarified in settings with low to moderate levels of air pollution. We investigated this in the Danish population between 2004 and 2016., Methods: We included 3 653 490 persons aged 18-64 years in a nested case-control study. Exposure was defined as the average daily concentration at the individual's residential address of CO, NO X , NO 2 , O 3 , SO 2 , NH 3 , PPM 2.5 , black carbon, organic carbon, mineral dust, sea salt, secondary inorganic aerosols, SO 4 2- , NO 3 - , NH 4 + , secondary organic aerosols, PM 2.5 , and PM 10 during a 3-month exposure window. RTIs were defined by hospitalization for RTIs. Incidence rate ratios (IRRs) and 95% CIs were estimated comparing highest with lowest decile of exposure using conditional logistic regression models., Results: In total, 188 439 incident cases of RTI were identified. Exposure to most air pollutants was positively associated with risk of RTI. For example, NO 2 showed an IRR of 1.52 (CI: 1.48-1.55), and PM 2.5 showed an IRR of 1.45 (CI: 1.40-1.50). In contrast, exposure to sea salt, PM 10 , NH 3 , and O 3 was negatively associated with a risk of RTIs., Discussion: In this nationwide study comprising adults, exposure to air pollution was associated with risk of RTIs and subgroups hereof. Sea salt, PM 10 , NH 3 , and O 3 may be proxies for rural areas, as the levels of these species in Denmark are higher near the western coastlines and/or in rural areas with fewer combustion sources., (Copyright © 2023 The Authors. Published by Elsevier Ltd.. All rights reserved.)

Air pollution is a significant contributor to the global burden of disease with a plethora of associated health effects such as pulmonary and systemic inflammation. C-reactive protein (CRP) is associated with a wide range of diseases and is associated with several exposures. Studies on the effect of air pollution exposure on CRP levels in low to moderate pollution settings have shown inconsistent results. In this cross-sectional study high sensitivity CRP measurements on 18,463 Danish blood donors were linked to modelled air pollution data for NO x , NO 2 , O 3 , CO, SO 2 , NH 3 , mineral dust, black carbon, organic carbon, sea salt, secondary inorganic aerosols and its components, primary PM 2.5 , secondary organic aerosols, total PM 2.5 , and total PM 10 at their residential address over the previous month. Associations were analysed using ordered logistic regression with CRP quartile as individuals outcome and air pollution exposure as scaled deciles. Analyses were adjusted for health related and socioeconomic covariates using health questionnaires and Danish register data. Exposure to different air pollution components was generally associated with higher CRP (odds ratio estimates ranging from 1.11 to 1.67), while exposure to a few air pollution components was associated with lower CRP. For example, exposure to NO 2 increased the odds of high CRP 1.32-fold (95%CI 1.16-1.49), while exposure to NH3 decreased the odds of high CRP 0.81-fold (95%CI 0.73-0.89). This large study among healthy individuals found air pollution exposure to be associated with increased levels of CRP even in a setting with low to moderate air pollution levels., Competing Interests: Declaration of competing interest The authors declare the following financial interests/personal relationships which may be considered as potential competing interests:Co-author is chairman of Zealand Regional Committee on Health Research Ethics - Ole Birger Pedersen., (Copyright © 2023 The Authors. Published by Elsevier Inc. All rights reserved.)

Air pollution is associated with increased risk of myocardial infarction (MI), but it is unresolved to what extent the association is modified by factors such as socioeconomic status, comorbidities, financial stress, residential green space, or road traffic noise. We formed a cohort of all (n = 1,964,702) Danes, aged 50-85 years, with 65,311 cases of MI during the followed-up period 2005-2017. For all participants we established residential five-year running average exposure to particulate matter <2.5 μm (PM 2.5 ), ultrafine particles (UFP, <0.1 μm), elemental carbon (EC) and nitrogen dioxide (NO 2 ). We evaluated risk in population strata, using Aalen additive hazards models to estimate absolute risk and Cox proportional hazards models to estimate relative risk of MI with 95% confidence intervals (CI). PM 2.5 and the other pollutant were associated with MI. Lower education and lower income were associated with higher absolute risks of MI from air pollution, whereas no clear effect modification was apparent for relative risk estimates. For example, 5 μg/m 3 higher PM 2.5 was associated with HR for MI of 1.16 (95% CI: 1.10-1.22) among those with only mandatory education and 1.13 (95% CI: 1.03-1.24) among those with long education. The corresponding rate differences per 100,000 person years were 243 (95% CI: 216-271) and 358 (95% CI: 338-379), respectively. Higher level of comorbidity was consistently across all four pollutants associated with both higher absolute and relative risk of MI. In conclusion, people with comorbid conditions or of lower SES appeared more vulnerable to long-term exposure to air pollution and more cases of MI may be prevented by focused interventions in these groups., Competing Interests: Declaration of competing interest The authors declare the following financial interests/personal relationships which may be considered as potential competing interests: Ole Raaschou-Nielsen reports financial support was provided by Health Effects Institute., (Copyright © 2023 Elsevier Inc. All rights reserved.)

Background Colon cancer incidence is rising globally, and factors pertaining to urbanization have been proposed involved in this development. Traffic noise may increase colon cancer risk by causing sleep disturbance and stress, thereby inducing known colon cancer risk-factors, e.g. obesity, diabetes, physical inactivity, and alcohol consumption, but few studies have examined this. Objectives The objective of this study was to investigate the association between traffic noise and colon cancer (all, proximal, distal) in a pooled population of 11 Nordic cohorts, totaling 155,203 persons. Methods We identified residential address history and estimated road, railway, and aircraft noise, as well as air pollution, for all addresses, using similar exposure models across cohorts. Colon cancer cases were identified through national registries. We analyzed data using Cox Proportional Hazards Models, adjusting main models for harmonized sociodemographic and lifestyle data. Results During follow-up (median 18.8 years), 2757 colon cancer cases developed. We found a hazard ratio (HR) of 1.05 (95% confidence interval (CI): 0.99-1.10) per 10-dB higher 5-year mean time-weighted road traffic noise. In sub-type analyses, the association seemed confined to distal colon cancer: HR 1.06 (95% CI: 0.98-1.14). Railway and aircraft noise was not associated with colon cancer, albeit there was some indication in sub-type analyses that railway noise may also be associated with distal colon cancer. In interaction-analyses, the association between road traffic noise and colon cancer was strongest among obese persons and those with high NO 2 -exposure. Discussion A prominent study strength is the large population with harmonized data across eleven cohorts, and the complete address-history during follow-up. However, each cohort estimated noise independently, and only at the most exposed façade, which may introduce exposure misclassification. Despite this, the results of this pooled study suggest that traffic noise may be a risk factor for colon cancer, especially of distal origin., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier Inc. All rights reserved.)

Oil spill attenuation in Arctic marine environments depends on oil-degrading bacteria. However, the seasonally harsh conditions in the Arctic such as nutrient limitations and sub-zero temperatures limit the activity even for bacteria capable of hydrocarbon metabolism at low temperatures. Here, we investigated whether the variance between epipelagic (seasonal temperature and inorganic nutrient variations) and mesopelagic zone (stable environmental conditions) could limit the growth of oil-degrading bacteria and lead to lower oil biodegradation rates in the epipelagic than in the mesopelagic zone. Therefore, we deployed absorbents coated with three oil types in a SW-Greenland fjord system at 10-20 m (epipelagic) and 615-650 m (mesopelagic) water depth for one year. During this period we monitored the development and succession of the bacterial biofilms colonizing the oil films by 16S rRNA gene amplicon quantification and sequencing, and the progression of oil biodegradation by gas chromatography - mass spectrometry oil fingerprinting analysis. The removal of hydrocarbons was significantly different, with several polycyclic aromatic hydrocarbons showing longer half-life times in the epipelagic than in the mesopelagic zone. Bacterial community composition and density (16S rRNA genes/ cm 2 ) significantly differed between the two zones, with total bacteria reaching to log-fold higher densities (16S rRNA genes/cm 2 ) in the mesopelagic than epipelagic oil-coated absorbents. Consequently, the environmental conditions in the epipelagic zone limited oil biodegradation performance by limiting bacterial growth., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier B.V. All rights reserved.)

Background: Air pollution is a well-recognized risk factor for cardiovascular disease. However, the mechanistic pathways underlying the association are not completely understood. Hence, further studies are required to shed light on potential mechanisms, through which air pollution may affect the development from subclinical to clinical cardiovascular disease., Objectives: To investigate associations between short-term exposure to air pollution and high-density lipoprotein (HDL), non-high density lipoprotein (non-HDL), systolic and diastolic blood pressure., Methods: The study was conducted among 32,851 Danes from the Diet, Cancer and Health - Next Generations cohort, who had a blood sample taken and blood pressure measured. We measured HDL and non-HDL in the blood samples. We modelled exposure to fine particulate matter (PM 2.5 ), ultrafine particles (UFP), elemental carbon (EC) and nitrogen dioxide (NO 2 ) in time-windows from 24 h up to 90 days before blood sampling. Pollutants were modelled as total air pollution from all sources, and apportioned into contributions from non-traffic and traffic sources. We analyzed data using linear and logistic regression, with adjustment for socio-economic and lifestyle factors., Results: Air pollution exposure over 24 h to 30 days was generally adversely associated with lipid profile and blood pressure, e.g. for 30-day UFP-exposure, adjusted β-estimates were: -0.025 (-0.043; -0.006) for HDL, 0.086 (0.042; 0.130) for non-HDL, 2.45 (1.70; 3.11) for systolic and 1.56 (1.07; 20.4) for diastolic blood pressure, per 10,000 particles/cm 3 . The strongest associations were found for the non-traffic components of air pollution, and among those who were overweight/obese., Discussion: In this large study of air pollution and lipid levels and blood pressure, we found that 24-h to 30-day PM 2.5 , UFP, EC and NO 2 concentrations were generally adversely associated with lipid profile and blood pressure, two important cardiovascular risk factors. The study suggests potential pathways, through which air pollution could affect the development of cardiovascular disease., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier Inc. All rights reserved.)

Air pollution with particulate matter is an established lung carcinogen. Studies have suggested an association with breast cancer, but the evidence is inconsistent., Methods: From nationwide registers, we identified all breast cancer cases (n = 55 745) in Denmark between 2000 and 2014. We matched one control for each case on age and year of birth. We used a multi-scale dispersion model to estimate outdoor concentrations of particulate matter <2.5 μm (PM 2.5 ), elemental carbon (EC) and nitrogen dioxide (NO 2 ) as time-weighted average over all addresses up to 20 years prior to diagnosis. We calculated odds ratios (OR) and 95% confidence intervals (CI) by conditional logistic regression with adjustment for marital status, educational level, occupational status, personal income, region of origin, medication and area-level socio-economic indicators., Results: A 10 μg/m 3 higher PM 2.5 was associated with an OR for breast cancer of 1.21 (95% CI: 1.11-1.33). The corresponding ORs for EC (per 1 μg/m 3 ) and NO 2 (per 10 μg/m 3 ) were 1.03 (95% CI: 1.00-1.07) and 1.03 (95% CI: 1.01-1.06), respectively. In multi-pollutant models, the OR for PM 2.5 changed only little, whereas ORs for EC or NO 2 approached the null. In an analysis of persons below 55 years, PM 2.5 was associated with an OR of 1.32 (95% CI: 1.09-1.60) per 10 μg/m 3 increase., Conclusion: We found evidence of an association between the investigated air pollutants and breast cancer, especially PM 2.5 . There were indications that the association differed by age at diagnosis. We were not able to include all potential confounders and thus, results should be interpreted with caution., Competing Interests: Declaration of competing interest The authors declare the following financial interests/personal relationships which may be considered as potential competing interests: Joergen Brandt reports financial support was provided by NordForsk., (Copyright © 2022 Elsevier Inc. All rights reserved.)

The continuous change in observed key indicators such as increasing nitrogen deposition, temperatures and precipitation will have marked but uncertain consequences for the ecosystem carbon (C) sink-source functioning of the Arctic. Here, we use multiple in-situ data streams measured by the Greenland Ecosystem Monitoring programme in tight connection with the Soil-Plant-Atmosphere model and climate projections from the high-resolution HIRHAM5 regional model. We apply this modelling framework with focus on two climatically different tundra sites in Greenland (Zackenberg and Kobbefjord) to assess how sensitive the net C uptake will expectedly be under warmer and wetter conditions across the 21st century and pin down the relative contribution to the overall C sink strength from climate versus plant trait variability. Our results suggest that temperatures (5-7.7 °C), total precipitation (19-110 %) and vapour pressure deficit will increase (32-36 %), while shortwave radiation will decline (6-9 %) at both sites by 2100 under the RCP8.5 scenario. Such a combined effect will, on average, intensify the net C uptake by 9-10 g C m -2 year -1 at both sites towards the end of 2100, but Zackenberg is expected to have more than twice the C sink strength capacity of Kobbefjord. Our sensitivity analysis not only reveals that plant traits are the most sensitive parameters controlling the net C exchange in both sites at the beginning and end of the century, but also that the projected increase in the net C uptake will likely be similarly influenced by future changes in climate and existing local nutrient conditions. A series of experiments forcing realistic changes in plant nitrogen status at both sites corroborates this hypothesis. This work proves the unique synergy between monitoring data and numerical models to assist robust model calibration/validation and narrow uncertainty ranges and ultimately produce more reliable C cycle projections in understudied regions such as Greenland., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 The Authors. Published by Elsevier B.V. All rights reserved.)

This work builds upon recent developments in the field of second dimensional (2D) retention indices (RI) for use in comprehensive two-dimensional gas chromatography (GC×GC), expanding application to the most commonly used "normal" orthogonality column configuration, where 2D RI are rarely employed. Initially, one dimensional retention indices for 80 wastewater pollutants were determined by GC-MS on a mid-polar ZB-50 column. In order to determine the 2D RIs for peaks detected in wastewater extracts separated by GC×GC -MS, a single injection of a ten-compound standard mix allowed the construction of model-generated isovolatility curves. These curves were used for the determination of 2D RIs of compounds initially identified on the basis of the mass spectral match factor and 1D RIs. Good agreements (average deviation of 1.7%) were observed between the calculated 2D RIs and the measured reference RIs for these compounds. These results show that this approach provides an additional level of confidence for the identification of compounds detected in GC×GC-MS and demonstrates the potential of this approach for improved compound identification in non-targeted analysis., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022. Published by Elsevier B.V.)

A major challenge in processing of complex data obtained from chromatography hyphenated to mass spectrometry is to resolve chromatographically co-eluting compounds. In this study, we present a workflow for the resolution of ultra-high pressure liquid chromatography high-resolution mass spectrometry data obtained by the broadband data-independent acquisition MS E operation (UHPLCHRMS E ). The workflow is based on a recently introduced algorithm for Parallel Factor Analysis 2 (PARAFAC2) that allows to enforce non-negativity on all the model coefficients. The workflow was tested on three sets of UHPLC-HRMS E measurements from a Lupinus angustifolius L. crop field study, which included plant tissue samples, soil samples and samples from drainage water as well as stream water close to the field. The three datasets included 93, 59, and 75 chromatographic runs in total for the plant, soil and water batches, respectively. Nonnegative-PARAFAC2 models were fitted on the summed high and low energy (HE and LE) traces on chromatographic intervals corresponding to spiked standard for the three sample sets independently. In soil and plant samples, 13 out of 14 spiked standards were resolved by NN-PARAFAC2 even in presence of chromatographic co-elution, and their mass spectral loadings could be matched to a reference spectrum. In contrast, only seven spiked standards were correctly resolved and matched for the water samples because a higher chromatographic baseline rendered the data noisier. The results show that the workflow we present can provide improved mass spectral selectivity for data-independent acquisition compared to using the raw mass spectra and can be used to match fragment ions from the HE trace, and precursor and adduct ions from the LE trace even in presence of co-eluting compounds., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper. The authors declare the following financial interests/personal relationships which may be considered as potential competing interests:, (Copyright © 2022 The Author(s). Published by Elsevier B.V. All rights reserved.)

Global anthropogenic and legacy mercury (Hg) emissions are the main sources of Arctic Hg contamination, primarily transported there via the atmosphere. This review summarizes the state of knowledge of the global anthropogenic sources of Hg emissions, and examines recent changes and source attribution of Hg transport and deposition to the Arctic using models. Estimated global anthropogenic Hg emissions to the atmosphere for 2015 were ~2220 Mg, ~20% higher than 2010. Global anthropogenic, legacy and geogenic Hg emissions were, respectively, responsible for 32%, 64% (wildfires: 6-10%) and 4% of the annual Arctic Hg deposition. Relative contributions to Arctic deposition of anthropogenic origin was dominated by sources in East Asia (32%), Commonwealth of Independent States (12%), and Africa (12%). Model results exhibit significant spatiotemporal variations in Arctic anthropogenic Hg deposition fluxes, driven by regional differences in Hg air transport routes, surface and precipitation uptake rates, and inter-seasonal differences in atmospheric circulation and deposition pathways. Model simulations reveal that changes in meteorology are having a profound impact on contemporary atmospheric Hg in the Arctic. Reversal of North Atlantic Oscillation phase from strongly negative in 2010 to positive in 2015, associated with lower temperature and more sea ice in the Canadian Arctic, Greenland and surrounding ocean, resulted in enhanced production of bromine species and Hg(0) oxidation and lower evasion of Hg(0) from ocean waters in 2015. This led to increased Hg(II) (and its deposition) and reduced Hg(0) air concentrations in these regions in line with High Arctic observations. However, combined changes in meteorology and anthropogenic emissions led to overall elevated modeled Arctic air Hg(0) levels in 2015 compared to 2010 contrary to observed declines at most monitoring sites, likely due to uncertainties in anthropogenic emission speciation, wildfire emissions and model representations of air-surface Hg fluxes., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Crown Copyright © 2022. Published by Elsevier B.V. All rights reserved.)

This study aimed to investigate the ability of analyte protectants to enhance GC-MS signals and compensate matrix effects for a range of micropollutants in pure standard, effluent, and influent wastewater samples during analysis and detection. Wastewater samples were prepared for analysis using multilayer solid phase extraction for the purpose of extracting sample components with a broad range of physical-chemical properties. The sample extracts were either spiked or not spiked with target compounds and four analyte protectants: 3-ethoxy-1,2-propanediol, D-sorbitol, gluconolactone, and shikimic acid. In this way, it was possible to evaluate the matrix effects of wastewater samples and compare the use of analyte protectants with the conventional correction method of allocating a best matching internal standard to each target compound. A relation was observed between level of wastewater treatment and matrix effects, with the largest effects observed for influent samples and the smallest effects for effluent samples. Compensation of matrix effects with analyte protectants gave comparable results with the conventional correction method of allocating a best matching internal standard to each of the 13 investigated micropollutants. The best overall compensation was observed using analyte protectants and the internal standard correction method in combination., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 The Author(s). Published by Elsevier B.V. All rights reserved.)

Background: Transportation noise increases the risk of ischemic heart disease (IHD), but few studies have investigated subtypes of IHD, such as myocardial infarction (MI), angina pectoris, or heart failure. We aimed to study whether exposure to road, railway and aircraft noise increased risk for ischemic heart disease (IHD), IHD subtypes, and heart failure in the entire adult Danish population, investigating exposures at both maximum exposed and silent façades of each residence., Methods: We modelled road, railway, and aircraft noise at the most and least exposed façades for the period 1995-2017 for all addresses in Denmark and calculated 10-year time-weighted running means for 2.5 million individuals age ≥50 years, of whom 122,523 developed IHD and 79,358 developed heart failure during follow-up (2005-2017). Data were analyzed using Cox proportional hazards models, adjusted for individual and area-level sociodemographic covariates and air pollution., Results: We found road traffic noise at the most exposed façade (L den ) to be associated with higher risk of IHD, myocardial infarction (MI), angina pectoris, and heart failure, with hazard ratios (HRs) (95% confidence intervals (CI)) of 1.052 (1.044-1.059), 1.041 (1.032-1.051), 1.095 (1.071-1.119), and 1.039 (1.033-1.045) per 10 dB higher 10-year mean exposure, respectively. These associations followed a near-linear exposure-response relationship and were robust to adjustment for air pollution with PM 2.5 . Railway noise at the least exposed façade was associated with heart failure (HR 1.28; 95% CI: 1.004-1.053), but not the other outcomes. Exposure to aircraft noise (>45 dB) seemed associated with increased risk for MI and heart failure., Conclusions: We found road traffic noise and potentially railway and aircraft noise to increase risk of various major cardiovascular outcomes, highlighting the importance of preventive actions towards transportation noise., (Copyright © 2022 Elsevier Inc. All rights reserved.)

Background: Exposure to outdoor air pollution is associated with adverse health effects. Previous studies have indicated higher levels of air pollution in socially deprived areas., Aim: To investigate associations between air pollution and socio-demographic variables, comorbidity, stress, and green space at the residence in Denmark., Methods: We included 2,237,346 persons living in Denmark, aged 35 years or older in 2017. We used the high resolution, multi-scale DEHM/UBM/AirGIS air pollution modelling system to calculate mean concentrations of air pollution with PM 2.5 , elemental carbon, ultrafine particles and NO 2 at residences held the preceding five years. We used nationwide registries to retrieve information about socio-demographic indicators at the individual and neighborhood levels. We used general linear regression models to analyze associations between socio-demographic indicators and air pollution at the residence., Results: Individuals with high SES (income, higher white-collar worker and high educational level) and of non-Danish origin were exposed to higher levels of air pollution than individuals of low SES and of Danish origin, respectively. We found comparable levels of air pollution according to sex, stress events and morbidity. For neighborhood level SES indicators, we found high air pollution levels in neighborhoods with low SES measured as proportion of social housing, sole providers, low income and unemployment. In contrast, we found higher air pollution levels in neighborhoods with higher educational level and a low proportion of manual labor. People living in an apartment and/or with little green space had higher air pollution levels., Conclusion: In Denmark, high levels of residential air pollution were associated with higher individual SES and non-Danish origin. For neighborhood-level indicators of SES, no consistent pattern was observed. These results highlight the need for analyzing many different socio-demographic indicators to understand the complex associations between SES and exposure to air pollution., (Copyright © 2022 Elsevier Inc. All rights reserved.)

Background: Many studies investigated the relationship between outdoor fine particulate matter (PM 2.5 ) and cancer. While they generally indicated positive associations, results have not been fully consistent, possibly because of the diversity of methods used to assess exposure., Objectives: To investigate how using different PM 2.5 exposure assessment methods influences risk estimates in the large French general population-based Gazel cohort (20,625 participants at enrollment) with a 26-year follow-up with complete residential histories., Methods: We focused on two cancer incidence outcomes: all-sites combined and lung. We used two distinct exposure assessment methods: a western European land use regression (LUR), and a chemistry-dispersion model (Gazel-Air) for France, each with a time series ≥20-years annual concentrations. Spearman correlation coefficient between the two estimates of PM 2.5 was 0.71 across all person-years; the LUR tended to provide higher exposures. We used extended Cox models with attained age as time-scale and time-dependent cumulative exposures, adjusting for a set of confounders including sex and smoking, to derive hazard ratios (HRs) and their 95% confidence interval, implementing a 10-year lag between exposure and incidence/censoring., Results: We obtained similar two-piece linear associations for all-sites cancer (3711 cases), with a first slope of HRs of 1.53 (1.24-1.88) and 1.43 (1.19-1.73) for one IQR increase of cumulative PM 2.5 exposure for the LUR and the Gazel-Air models respectively, followed by a plateau at around 1.5 for both exposure assessments. For lung cancer (349 cases), the HRs from the two exposure models were less similar, with largely overlapping confidence limits., Conclusion: Our findings using long-term exposure estimates from two distinct exposure assessment methods corroborate the association between air pollution and cancer risk., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 Elsevier B.V. All rights reserved.)

Reusable plastic sports bottles are used extensively worldwide, and little is known about the migration of chemicals from the bottles into drinking water. In this study, we investigated the chemical migration into drinking water stored for 24 h in new bottles, used bottles and bottles washed in the dishwasher. Non-target screening (NTS) by liquid-chromatography - high-resolution mass spectrometry (LC-HRMS) was performed to identify these compounds. We detected > 3500 dishwasher related compounds, with 430 showing migration even after subsequent flushing of the bottles. In addition, more than 400 plastic related compounds were detected, with high peaks for oligomers suspected to originate from the biodegradable polyester polycaprolactone, and aromatic amines, which may have been introduced as slip agents or antioxidants. These compounds have never been reported before in bottled water. Most of the identified compounds migrating out of the used bottles were plasticizers, antioxidants or photoinitiators. The presence of photoinitiators are of particular concern, due to possible endocrine disrupting effects. Furthermore, diethyltoluamide (DEET) was detected, which may have been formed from the plasticizer laurolactam. Typically, the dishwashing process enhanced the leaching of plastic related compounds, and even after additional water flushing, the average peak intensity of these compounds was only reduced by half., (Copyright © 2022 The Authors. Published by Elsevier B.V. All rights reserved.)

Background: For patients with peripheral T-cell lymphoma (PTCL), outcomes using frontline treatment with cyclophosphamide, doxorubicin, vincristine, and prednisone (CHOP) or CHOP-like therapy are typically poor. The ECHELON-2 study demonstrated that brentuximab vedotin plus cyclophosphamide, doxorubicin, and prednisone (A+CHP) exhibited statistically superior progression-free survival (PFS) per independent central review and improvements in overall survival versus CHOP for the frontline treatment of patients with systemic anaplastic large cell lymphoma or other CD30-positive PTCL., Patients and Methods: ECHELON-2 is a double-blind, double-dummy, randomized, placebo-controlled, active-comparator phase III study. We present an exploratory update of the ECHELON-2 study, including an analysis of 5-year PFS per investigator in the intent-to-treat analysis group., Results: A total of 452 patients were randomized (1 : 1) to six or eight cycles of A+CHP (N = 226) or CHOP (N = 226). At median follow-up of 47.6 months, 5-year PFS rates were 51.4% [95% confidence interval (CI): 42.8% to 59.4%] with A+CHP versus 43.0% (95% CI: 35.8% to 50.0%) with CHOP (hazard ratio = 0.70; 95% CI: 0.53-0.91), and 5-year overall survival (OS) rates were 70.1% (95% CI: 63.3% to 75.9%) with A+CHP versus 61.0% (95% CI: 54.0% to 67.3%) with CHOP (hazard ratio = 0.72; 95% CI: 0.53-0.99). Both PFS and OS were generally consistent across key subgroups. Peripheral neuropathy was resolved or improved in 72% (84/117) of patients in the A+CHP arm and 78% (97/124) in the CHOP arm. Among patients who relapsed and subsequently received brentuximab vedotin, the objective response rate was 59% with brentuximab vedotin retreatment after A+CHP and 50% with subsequent brentuximab vedotin after CHOP., Conclusions: In this 5-year update of ECHELON-2, frontline treatment of patients with PTCL with A+CHP continues to provide clinically meaningful improvement in PFS and OS versus CHOP, with a manageable safety profile, including continued resolution or improvement of peripheral neuropathy., Competing Interests: Disclosure SH reports receiving research support from ADC Therapeutics, Affimed, Aileron, Celgene, Daiichi Sankyo, Forty Seven, Kyowa Hakko Kirin, Millennium/Takeda, Seagen, Trillium Therapeutics, and Verastem/Secura Bio; and consulting for Acrotech Biopharma, ADC Therapeutics, Astex, C4 Therapeutics, Celgene, Janssen, Kura Oncology, Kyowa Hakko Kirin, Myeloid Therapeutics, ONO Pharmaceuticals, Seagen, Secura Bio, Shoreline Biosciences, Takeda, Trillium Therapeutics, Tubulis, Verastem, and Vividion Therapeutics. OAO reports advisory membership for Mundipharma, Kymera, Dren Bio, Myeloid Therapeutics, NomoCan; corporate board membership for NomoCan; consultancy for Mundipharma, Servier, Ping; employment with TG therapeutics; equity ownership of TG Therapeutics, Myeloid Therapeutics, Kymera, NomoCan, Dren Bio; honoraria from Mundipharma, Servier, and Pint; research funding from Merck, Bristol Myers Squibb (BMS)/Celgene, Astex, Kymera; and travel expenses from Mundipharma, Servier, and TG Therapeutics. BP reports consultancy, honoraria, research funding, and travel expenses for Seagen; and honoraria and travel expenses for Takeda. LT reports consultancy for Janssen, Nordic Nanovector, and Takeda Europe; and research funding from Mundipharma, Roche, Seagen, and Takeda Europe. SI reports receiving research funding from Seagen, Merck, CRISPRx, Innate, Affimed, Rhizen, Spectrum, Trillium, and Cellectis; and honoraria from Targeted Oncology and Curio Science. RA reports consultancy for AstraZeneca, Bayer Healthcare Pharmaceuticals, Celgene, Cell Medica, Genentech/Roche, Gilead, Kite Pharma, Kyowa, Portola Pharmaceuticals, Sanofi, Seagen, and Takeda; and research funding from Celgene, Forty Seven, Genentech/Roche, Janssen Pharma, Kura, Merck, Millenium, Pharmacyclics, Regeneron, and Seagen. NLB reports advisory boards for ADC Therapeutics, Roche/Genentech, and Seagen; and research funding from ADC Therapeutics, Affimed, Autolus, BMS, Celgene, Forty Seven, Janssen, Kite Pharma, Merck, Millennium, Pharmacyclics, Roche/Genentech, and Seagen. FM reports advisory board membership for AbbVie, Celgene/BMS, Epizyme, Gilead, Roche; consultancy for Gilead, Roche, Servier; and honoraria from Janssen and Roche. ED-D reports advisory board and corporate board membership for Takeda, and travel expenses for BMS, Roche, and Takeda. GR reports advisory board membership for AbbVie, Amgen, Celgene, Gilead, Janssen, Jazz, Pfizer, Roche, Sanofi, Teva; honoraria from BMS, Daiichi, Mundipharma, Novartis, Sandoz; research funding from Seagen; and travel expenses from Alexion, Celgene, and Gilead. WSK reports receiving research funding/grants from Celltrion, Donga, Johnson & Johnson, Kyowa Hakko Kirin, Mundipharma, Pfizer, Roche, Seagen, and Takeda. TF reports advisory board membership for Bayer, BMS, Seagen, consultancy for AstraZeneca, Bayer, BMS, Kyowa Kirin, MorphoSys, Seagen; honoraria for AbbVie, Bayer, BMS, Kite Pharma, Pharmacyclics, Seagen, Takeda; research funding for Amgen, BMS, Celgene, Cell Medica, Corvus, Eisai, Kyowa Hakko Kirin, Pfizer, Portola Pharma, Roche, Seagen, Trillium, Viracta; speaker's bureau for AbbVie, Celgene, Janssen, Kite Pharma, Pharmacyclics, Seagen; and travel expenses for AbbVie, Kite Pharma, Pharmacyclics, Seagen, Takeda. TM reports receiving honoraria from Amgen, Atara, Celgene, Daiichi Sankyo, Janssen, Kite/Gilead, Novartis, Pfizer, Roche, and Takeda; research funding from AstraZeneca, Janssen, and Novartis, and travel expenses from Amgen, Bayer, Celgene, Jazz, Kite/Gilead, Kyowa Kirin, and Pfizer. DB reports advisory board membership for Gilead and Roche; consultancy for Gilead, Janssen, and Roche; research funding from Celgene, Janssen, Roche, and Takeda; and travel expenses from Gilead and Roche. ÁI reports advisory board membership and corporate board membership for Celgene, Janssen, Novartis, Roche, and Takeda; research funding from Seagen and Takeda; and travel expenses from Roche and Takeda. KTo reports consultancy for Celgene, Chugai Pharma, Daiichi Sankyo, HUYA Bioscience International, Kyowa Kirin, Mundipharma, Ono Pharmaceutical, SymBio, Takeda, Yakult, and Zenyaku Kogyo; and honoraria from BMS-Celgene, Chugai Pharma, Daiichi Sankyo, Eisai, HUYA Bioscience International, Kyowa Kirin, Mundipharma, Ono Pharma, Solasia Pharma, Takeda, Yakult, and Zenyaku Kogyo. KTs reports consultancy for Daiichi Sankyo, HUYA, Ono Pharma, Meiji Seika Pharma, and Yakuruto; honoraria from Celgene, Chugai Pharma, Kyowa Hakko Kirin, and Mundy Pharma; research funding from Chugai Pharma, Eisai, HUYA, Seagen, Kyowa Hakko Kirin, Byer, Celgene, and Daiichi-Sankyo. S-PY reports an advisory role for AbbVie, Amgen, Janssen, Astellas, Astex, Novartis, Sanofi, and Takeda. AS reports consulting for Acrotech, BMS-Celgene, Kyowa Hakko Kirin, TG Therapeutics, and Verastem. AH reports receiving research funding from Seagen and travel expenses from Celgene and Roche. KS reports consultancy for AbbVie, AstraZeneca, BMS, Gilead, Merck, Seagen, Servier, Kyowa, Novartis Canada; honoraria from AbbVie, AstraZeneca, BMS, Gilead, Kyowa Kirin, Merck, Novartis, Novartis Canada Pharma, Seagen; research funding from BMS, Roche; and travel expenses from Seagen. SY reports receiving research funding and travel expenses from Seagen. PLZ reports advisory board membership with AbbVie, Gilead, Incyte, Merck, Portola, Roche, Sanofi, Servier, and Takeda; consultancy for BMS, Celgene, Celltron, Eusapharma, Gilead, Immune Design, Janssen-Cilag, Kyowa Kirin, Merck Sharp & Dohme (MSD), Roche, Sandoz, Verastem; honoraria from AbbVie, ADC Therapeutics, BMS, Debiopharm, EUSA Pharma, Gilead, Incyte, Janssen, Kyowa Kirin, Merck, Roche, Servier, Takeda, TG Therapeutics, Verastem; research funding from Portola; and speaker's bureau for AbbVie, ADC Therapeutics, BMS, Celgene, Celltron, EUSA Pharma, Gilead, Immune Design, Incyte, Janssen, Janssen-Cilag, Kyowa Kirin, Merck, MSD, Portola, Roche, Sandoz, Servier, Takeda, TG Therapeutics, and Verastem. HM and VB report employment for Takeda. KF, MF, and MP report being employed by and holding shares in Seagen. TI reports advisory board membership and speaker's bureau for Takeda. All other authors have declared no conflicts of interest., (Copyright © 2021 The Authors. Published by Elsevier Ltd.. All rights reserved.)

Objective: Recent studies on air pollution and disease have been based on millions of participants within a region or country, relying entirely on register-based confounder adjustment. We aimed to investigate the effects of increasing adjustment for register- and questionnaire-based covariates on the association between air pollution and cardiometabolic diseases., Methods: In a population-based cohort of 246,766 eligible participants randomly selected across Denmark in 2010 and 2013 and followed up until December 31, 2017, we identified 3,247 myocardial infarction (MI) cases, 4,166 stroke cases and 6,366 type 2 diabetes cases. Based on historical address-information, we calculated 5-year time-weighted exposure to PM 2.5 and NO 2 modelled using a validated air pollution model. We used Cox proportional hazards models to calculate hazard ratios (HR) with increasing adjustment for a number of individual- and area-level register-based covariates as well as lifestyle covariates assessed through questionnaires., Results: We found that a 5 μg/m 3 higher PM 2.5 was associated with HRs (95% CI) for MI, stroke and diabetes, of respectively, 1.18 (0.91-1.52), 1.11 (0.88-1.40) and 1.24 (1.03-1.50) in the fully adjusted models. For all three diseases, adjustment for either individual-level, area-level or lifestyle covariates, or combinations of these resulted in higher HRs compared to HRs adjusted only for age, sex and calendar-year, most marked for MI and diabetes. Further adjustment for lifestyle in models with full register-based individual- and area-level adjustment resulted in only minor changes in HRs for all three diseases., Conclusions: Our findings suggest that in studies of air pollution and cardiometabolic disease, which use an adjustment strategy with a broad range of register-based socioeconomic variables, there is no effect on risk estimates from subsequent lifestyle adjustment., (Copyright © 2021 Elsevier Inc. All rights reserved.)

This study investigated the impact of local anthropogenic activity on the marine environment around the remote harbor of Qeqertarsuaq, West Greenland. Blue mussels (Mytilus sp.) were used as a bioindicator, and their physiological condition was found to decrease with increasing proximity to the harbor. Subsequently, the distribution of 19 polycyclic aromatic hydrocarbons (PAHs) and 9 groups of alkylated PAHs were measured in mussel and sediment samples. The highest values were found in a rocky collection area 15 m from a wooden pier frequented by small boats. A PAH source investigation, indicated a mixed source from light fuel oils and creosote used as boat coating. Finally, correlations between the mussels morphological condition and the PAH pollution were found to be significant for 4-, 5-, and 6-ring PAHs. In conclusion, the results indicate that pollution sources in harbors have significant effects on the local environment and should be considered in arctic conservation research., (Copyright © 2021 Elsevier Ltd. All rights reserved.)

Background: Leukemia is one of the most common forms of hematologic malignancy, which can affect people of all ages. We previously showed an association between exposure to ambient particulate matter 2.5 μg (PM 2.5 ) and risk for leukemia in adults. The aim of this study was to investigate which PM 2.5 constituents were responsible for our previous observation., Methods: This is a nationwide register-based case-control study. We identified 14,983 persons diagnosed with leukemia at age 20 or above, 1989-2014, in the Danish Cancer Registry. We selected up to four sex and age-matched controls per case at random from the entire Danish population (n = 51,613). We modelled concentrations of ambient PM 2.5 and its constituents at the addresses of cases and controls for the 10-year period before index date with a state-of-the-art multiscale air pollution modeling system. We used conditional logistic regression to estimate odds ratios (ORs) adjusted for individual and neighborhood level socio-demographic variables., Result: The results showed higher risk for overall leukemia in association with interquartile range exposure to PM 2.5 (OR = 1.09; 95% CI: 1.02, 1.17), black carbon (BC) (OR = 1.02; 95% CI: 1.00, 1.03), secondary inorganic aerosols (SIA) (OR = 1.15; 95% CI: 1.03, 1.29) and its components ammonium (NH 4 ) (OR = 1.08; 95% CI: 1.00, 1.17) and nitrate (NO 3 ) (OR = 1.08; 95% CI: 1.02, 1.14). In leukemia subtype analysis, statistically significant associations were found for AML with PM 2.5 (OR = 1.14; 95% CI: 1.00, 1.29), BC (OR = 1.03; 95% CI: 1.00, 1.07), SIA (OR = 1.23; 95% CI: 1.01, 1.51), NH 4 (OR = 1.16; 95% CI: 1.01, 1.34) and NO 3 (OR = 1.12; 95% CI: 1.01, 1.24). The association between PM 2.5 and leukemia persisted in two pollutants models including sum of primary emitted black and organic carbon (BC + OC), secondary organic aerosols (SOA), or sea-salt. The association between black carbon (BC) and leukemia persisted in two pollutants models including organic carbon (OC). The three pollutant model with sulfate (SO 4 ), NH 4 and NO 3 showed an association with NO 3 but not with SO 4 or NH 4 ., Conclusion: Ambient concentrations of the PM 2.5 components BC, NH 4 and NO 3 at the residence showed associations with risk of incident leukemia in adults., (Copyright © 2020 Elsevier Inc. All rights reserved.)

Phytotoxins are plant secondary metabolites. They have recently been considered as chemicals of emerging concern (CECs) and there is a growing interest in their environmental fate and potential threat to public health. Dedicated target and non-target screening (NTS) analysis of phytotoxins in environmental samples are sparse, meanwhile phytotoxins are rarely detected in NTS-based analysis due to lack of an efficient methodology. Development of new analytical measurement methods is therefore highly needed. In this study, we for the first time investigated key parameters of reversed phase liquid chromatography-high resolution mass spectrometry (RPLC-HRMS) for five major classes of phytotoxins (alkaloids, steroids, terpenoids, flavonoids and aromatic polyketides) in environmental matrices; the investigation included analytical conditions which have not yet been explored by others, e.g. ionization at alkaline pH above 9. As the outcome we established a new analytical method for target/suspect screening and NTS of phytotoxins in the environment, which significantly improved the detection sensitivity with up to 40 times compared to previous methods, and enabled the discovery of over 30 phytotoxins in a NTS-based environmental study. We also observed that the negative ionization of phenols could be facilitated by the number of hydroxyl groups on the ring rather than their position of substitution. This study is of interest for a better fundamental understanding of the behavior of phytotoxins in LC-MS. Dedicated target/suspect screening and NTS methods will facilitate a better risk characterization of phytotoxins in the environment and stimulate implementation of new public regulation on phytotoxins., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2021 Elsevier B.V. All rights reserved.)

The removal of biomacromolecules from biofluids decreases the sample complexity and lower electrospray suppression effects. Furthermore, it can increase the analysis sensitivity, precision, and selectivity. Often removal approaches evaluate the model based on a single criterion, like protein removed or response of one of few specific metabolites. In this study, we used a multicriteria approach to test the effect of using the solvents methanol and acetonitrile (organic solvent precipitation), trichloroacetic acid (acidic precipitation) and ammonium sulphate (salting out) to remove biomacromolecules from a downstream recovery process from a bacillus fermentation. The downstream recovery process intermediates were analysed using reversed-phase ultra-high-pressure liquid chromatography with electrospray ionisation and high-resolution time-of-flight mass spectrometry detection. To evaluate the pre-treatment agents the following multicriteria was applied i) practical considerations, ii) total amino acid in the precipitated pellet, iii) putative identification of the molecules removed or created by the different treatments, iv) coherence between high quality extracted ion chromatograms (repeatability of DW-CODA) and v) replicate consistency from principal component analysis score values obtained by using the CHEMometric analysis of sections of Selected Ion Chromatograms (CHEMSIC) method. This study presents a generic workflow to find the best pre-treatment for removing bio-macromolecules from biofluids with a multicriteria approach. In our case, the best protein removal strategy for downstream recovery intermediates was acetonitrile precipitation. This method showed high precision, created few artefact peaks compared to simple sample dilution, and mainly removed small peptides., (Copyright © 2021 Elsevier B.V. All rights reserved.)

Sedimentation ponds have been shown to accumulate several groups of contaminants, most importantly polycyclic aromatic compounds (PACs) and metals. But also, other urban organic pollutants have shown to be present, including polybrominated diphenyl ethers (PBDEs), organophosphate compounds (OPCs) and benzothiazoles (BTs). This investigation aimed at determining the occurrence of these four groups of contaminants in sedimentation ponds and determine their transport from water/sediment to organisms. PACs, including alkylated PACs, PBDEs; OPCs and BTs were determined in water, sediment, plants, dragonfly larvae and fish from two sedimentation ponds and one reference site. Fish were analysed for PAC metabolites. Overall, higher concentrations of all four pollutant groups were detected in water and sediment from sedimentation ponds compared to two natural lakes in rural environments (reference sites). The concentration difference was highest in sediments, and >20 higher concentration was measured in sedimentation ponds (3.6-4.4 ng/g ww) compared to reference (0.2 ng/g ww) for sum BDE6. For PACs and PBDEs a clear transport from water/sediment to organisms were observed. Fish were the highest trophic level organism (3.5-5) in our study, and all four pollutant groups were detected in fish. For PBDEs a trophic biomagnification (TMF) was found both in sedimentation ponds and reference, but higher concentrations in all matrices were measured in sedimentation ponds. TMF was not calculated for PACs since they are metabolised by vertebrates, but a transfer from water/sediment to organisms was seen. For BTs and OPCs, no consistent transfer to plants and dragonfly larvae could be seen. One OPC and two BTs were detected in fish, but only in fish from sedimentation ponds. It is therefore concluded that sedimentation ponds are hotspots for urban and traffic related contaminants, of which especially PACs and PBDEs are transferred to organisms living there., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2020 The Authors. Published by Elsevier B.V. All rights reserved.)

Dechlorane Plus (DP) is a chlorinated flame retardant applied in parallel to or as a replacement product for regulated flame retardants. Detection of DP in environmental media all over the world in recent years necessitates the development of detailed global emission estimates for environmental model studies. Based on production, usage and disposal data two global atmospheric emission scenarios were made with a detailed geographical distribution. The total DP emission is estimated to be 0.02 t/year and 3.2 t/year in a low and high emission scenario, respectively, reflecting the uncertainties in production volumes and emission factors. The emission estimates are tested by implementation in the Danish Eulerian Hemispheric Model, an advanced chemistry-transport model. An evaluation against measurements in the Arctic from the early 2010s, considered to represent background concentrations, shows that the predicted concentration range for the high emission scenario is in line with the measured range, whereas the predicted concentrations for the low emission estimate are more than a factor of 100 lower than the measurements, rendering the high emission estimate most probable., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2020 Elsevier B.V. All rights reserved.)

Background: Particulate matter (PM) air pollution is a complex mixture and the various PM constituents likely affect health differently. The literature on the relationships among specific PM constituents and the risk of cancer is sparse. In this study, we aimed to evaluate the association of PM 2.5 and its constituents with the incidence of non-Hodgkin lymphoma (NHL) and the two main NHL subtypes., Methods: We undertook a nationwide register-based case-control study including 20,847 cases registered in the Danish Cancer Registry with NHL between 1989 and 2014. Among the entire Danish population, we selected 41,749 age and sex-matched controls randomly from the Civil Registration System. We assessed modelled outdoor PM concentrations at addresses of cases and controls with a state-of-the-art multi scale air pollution modelling system and used conditional logistic regression to estimate odds ratios (ORs) adjusted for individual and neighborhood level socio-demographic variables., Results: The 10-year time-weighted average concentrations of PM 2.5 , primary carbonaceous particles (BC/OC), secondary inorganic aerosols (SIA), secondary organic aerosols (SOA) and sea salt were 17.4, 2.3, 7.8, 0.3, and 4.1 μg/m 3 , respectively among controls. The results showed higher risk for NHL in association with exposure to BC/OC (OR = 1.03; 95% CI: 1.00, 1.07, per interquartile range (IQR)) and SOA (OR = 1.54; 95% CI: 1.13, 2.09, per IQR). The results indicated a higher risk for follicular lymphoma in association with several PM components. Including PM 2.5 (OR = 1.16; 95% CI: 0.98-1.38), BC/OC (OR = 1.05; 95% CI: 0.97-1.14), SIA (OR = 1.44; 95% CI: 0.80-1.08), SOA (OR = 4.52; 95% CI: 0.86-23.83) per IQR., Conclusion: This is the first study on PM constituents and the risk of NHL. The results indicated an association with primary carbonaceous and secondary organic PM. The results need replication in other settings before any firm conclusion can be reached., (Copyright © 2020 Elsevier Inc. All rights reserved.)

Background: Fish oil improves cardiometabolic markers in adults, but results in children are inconsistent. Few children meet the recommended fish intake and no randomized trials have investigated how fish intake per se affects children's cardiometabolic profile., Objective: We investigated whether oily fish consumption modulated serum triacylglycerol and diastolic blood pressure (coprimary outcomes) and other cardiometabolic markers in healthy Danish children and whether effects were sex-specific., Methods: In a randomized controlled 12-wk trial, 199 children (aged 8-9 y) received ∼300 g/wk of oily fish or poultry (control). We measured blood pressure, heart rate, and heart rate variability (HRV) via 3-h continuous electrocardiograms and collected fasting blood samples for analysis of erythrocyte EPA [20:5n-3 (ω-3)] + DHA (22:6n-3) and serum triacylglycerol, LDL and HDL cholesterol, glucose, and insulin., Results: One hundred and ninety-seven children (99%) completed the trial. The fish group consumed a median (IQR) of 375 (325-426) g oily fish/wk and the poultry group consumed 400 (359-452) g poultry/wk, which resulted in 2.25 (95% CI: 1.88, 2.62) fatty acid percentage-point higher erythrocyte EPA + DHA in the fish group (P < 0.001). In the fish group, serum triacylglycerol decreased by 0.05 mmol/L (95% CI: 0.00, 0.11 mmol/L) (P = 0.04) and HDL cholesterol increased by 0.07 mmol/L (95% CI: 0.01, 0.13 mmol/L) (P = 0.02); the triacylglycerol effect showed dose-dependency with erythrocyte EPA + DHA (r = -0.15, P = 0.04), whereas HDL showed a tendency for such an association(r = 0.13, P = 0.08). Additional analyses indicated sex-specificity (Pdiet*sex < 0.10), because triacylglycerol was reduced by 0.09 mmol/L (95% CI: 0.02, 0.16 mmol/L) in boys only (girls: -0.00; 95% CI: -0.07, 0.07 mmol/L) and heart rate was reduced by 3.4 bpm (95% CI: 0.2, 6.6 bpm) in girls only (boys: 0.6; 95% CI: -2.6, 3.8 bpm). Blood pressure, HRV, and glucose homeostasis were unaffected., Conclusions: Oily fish intake improved serum triacylglycerol and HDL cholesterol in a dose-dependent manner in 8- to 9-y-old children, but had no effect on blood pressure, HRV, or glucose homeostasis. This supports recommendations for fish intake in children and underlines the importance of initiatives to increase children's intake of oily fish. This trial was registered at clinicaltrials.gov as NCT02809508., (Copyright © American Society for Nutrition 2019.)

Gas-chromatography (GC) analysis of carboxylic acids is limited by the high polarity and low volatility of most of these compounds. Boron trifluoride (BF 3 ) mediated alkylation reactions is one of the most commonly used derivatization methods for making carboxylic acids GC compatible. A semi-automated BF 3 ·EtOH (ethanol) derivatization method was optimized for comprehensive two-dimensional gas chromatography high-resolution mass spectrometry (GC × GC-HR MS) analysis of carboxylic acids in solid phase extraction (SPE) extracts of oil polluted water. The optimal derivatization method were found to be with addition of 300 μL BF 3 ·EtOH per 200 μL sample and reaction at 75 °C for 24 h. Derivatives of eight selected acids (aliphatic, mono- and di-aromatic) were stable over 12 h with relative standard deviations (RSDs) of 2.0-10.7 %, the derivatization method was repeatable (RSDs of 3.2-17.2 %), detection limits (DL) and limit of detections (LODs) was in the range of DL = 0.53-1.63 ppb and LOD = 0.19-2.51 ppb for pure acid standards, and DL = 0.18-3.41 ppb and LOD = 0.28-5.46 ppb for matrix matched acid standards. Finally, the method was validated on the acidic fraction of a mixed anion-exchange SPE of oil polluted water. Thousands of degradation products from parent alkylated polycyclic aromatic hydrocarbons (PAHs) and aliphatic hydrocarbons, such as aliphatic acids and mono-, di- and tri- aromatic acids were analyzed by the applied method and compound groups were tentatively identified., (Copyright © 2019 Elsevier B.V. All rights reserved.)

Petroleum-derived fuels are chronically spilled in urbanized areas, affecting the environment and the population's health. Forensic investigations of oil spills aim to find the responsible source of the spills. Weathering processes (dissolution, evaporation, photo-oxidation and biodegradation) change the chemical composition of the spills and hamper the matching of spill-source pairs, especially for light diesel oils (i.e. n-C 9 - n-C 20 ) in which the source diesels can be very similar due to the refining process and only compounds resistant to short- or middle-term weathering are present. In this study, comprehensive two-dimensional gas chromatography - high resolution mass spectrometry (GC × GC - HRMS) and pixel-based analysis were combined for: i) improve the identification of very similar diesel oils, and ii) identify weathering-resistant compounds that can also distinguish samples from different sources. Diesel oils from two sources that have been exposed to different degrees of evaporation, photo-oxidation and biodegradation in a laboratory setup. The study revealed the tentatively identified octanoic acid methyl ester and n-nonaldehyde were more resistance to evaporation than hydrocarbons < n-C 15 . Furthermore, the hydrocarbons > n-C 17 could be used for source-apportionment of all the diesel oils susceptible to evaporation and photo-oxidation, but only pristane and phytane were also more resistant to biodegradation. Naphthenes, bicyclic sesquiterpanes and adamantanes were more resistant to only photo-oxidation and biodegradation. GC × GC - HRMS enhanced the separation of the highly similar naphthenes in the diesel oils; however, the diagnostic power for forensic spill investigations was still similar to 1D GC - HRMS., (Copyright © 2019 Elsevier B.V. All rights reserved.)

Unconventional oil feeds can be rich in oxygenated organic compounds that will negatively affect the fuel properties if they are not removed during refining. In this study, supercritical fluid chromatography (SFC) was utilised for the combined analysis of polycyclic aromatic hydrocarbons (PAHs) and oxygenated polycyclic aromatic compounds (OPACs). One objective was to chromatographically separate PAHs from OPACs; another to reach a high peak capacity, improved peak shapes and high signal-to-noise ratios (S/N) for OPACs. These objectives were set to establish a non-target analysis method for oxygenated compounds in unconventional oils by SFC hyphenated to a UV detector and a quadrupole time-of-flight mass spectrometer (QTOF-MS) with negative electrospray ionisation (ESI - ). Highest peak capacities were observed with a 2-picolylamine column with methanol as modifier, however, a better resolution and S/N were obtained with ethanol and 0.1% formic acid. The elution order for OPACs on all columns followed mainly the polarity of the analytes: furans < aldehydes ≤ ketones < phenols ≤ carboxylic acids. Best separation between PAHs and OPACs was achieved with the ethylene-bridged silica column. The optimised SFC-UV-ESI - -QTOF-MS method was tested on a coal tar middle distillate and a pyrolysis oil where a number of homologous series (e.g. hydroxy-naphthalenes and -benzaldehydes) was tentatively identified., (Copyright © 2019 Elsevier B.V. All rights reserved.)

Background: Based on the encouraging activity and manageable safety profile observed in a phase 1 study, the ECHELON-2 trial was initiated to compare the efficacy and safety of brentuximab vedotin, cyclophosphamide, doxorubicin, and prednisone (A+CHP) versus cyclophosphamide, doxorubicin, vincristine, and prednisone (CHOP) for the treatment of CD30-positive peripheral T-cell lymphomas., Methods: ECHELON-2 is a double-blind, double-dummy, randomised, placebo-controlled, active-comparator phase 3 study. Eligible adults from 132 sites in 17 countries with previously untreated CD30-positive peripheral T-cell lymphomas (targeting 75% with systemic anaplastic large cell lymphoma) were randomly assigned 1:1 to receive either A+CHP or CHOP for six or eight 21-day cycles. Randomisation was stratified by histological subtype according to local pathology assessment and by international prognostic index score. All patients received cyclophosphamide 750 mg/m 2 and doxorubicin 50 mg/m 2 on day 1 of each cycle intravenously and prednisone 100 mg once daily on days 1 to 5 of each cycle orally, followed by either brentuximab vedotin 1·8 mg/kg and a placebo form of vincristine intravenously (A+CHP group) or vincristine 1·4 mg/m 2 and a placebo form of brentuximab vedotin intravenously (CHOP group) on day 1 of each cycle. The primary endpoint, progression-free survival according to blinded independent central review, was analysed by intent-to-treat. This trial is registered with ClinicalTrials.gov, number NCT01777152., Findings: Between Jan 24, 2013, and Nov 7, 2016, 601 patients assessed for eligibility, of whom 452 patients were enrolled and 226 were randomly assigned to both the A+CHP group and the CHOP group. Median progression-free survival was 48·2 months (95% CI 35·2-not evaluable) in the A+CHP group and 20·8 months (12·7-47·6) in the CHOP group (hazard ratio 0·71 [95% CI 0·54-0·93], p=0·0110). Adverse events, including incidence and severity of febrile neutropenia (41 [18%] patients in the A+CHP group and 33 [15%] in the CHOP group) and peripheral neuropathy (117 [52%] in the A+CHP group and 124 [55%] in the CHOP group), were similar between groups. Fatal adverse events occurred in seven (3%) patients in the A+CHP group and nine (4%) in the CHOP group., Interpretation: Front-line treatment with A+CHP is superior to CHOP for patients with CD30-positive peripheral T-cell lymphomas as shown by a significant improvement in progression-free survival and overall survival with a manageable safety profile., Funding: Seattle Genetics Inc, Millennium Pharmaceuticals Inc, a wholly owned subsidiary of Takeda Pharmacuetical Company Limited, and National Institutes of Health National Cancer Institute Cancer Center., (Copyright © 2019 Elsevier Ltd. All rights reserved.)

In this study, we focus on isolation and fractionation strategies by solid phase extraction (SPE) for a broad range of environmentally related organic acids. These emerging potential contaminants are primary degradation products of spilled petrogenic compounds but little attention has been given to their environmental analysis and risk assessment. Three mixed-mode anion exchange sorbents possessing various backbone polarities were compared with respect to the extraction and fractionation efficiency. Quantitative analysis was obtained using an optimized and validated LC-MS method. We demonstrated the importance of reasonable ion source settings for highest sensitivity of individual carboxylic acids. Furthermore, fractionation of carboxylic acids into aliphatic and aromatic fractions by SPE was achieved by step-wise elution. Best performance regarding the isolation of low-concentration acids (sub μg L -1 level) in complex samples was attributed to Strata XA and is caused by high secondary hydrophobic interactions in addition to the ionic interactions. Isolation and fractionation of acid spiked diesel-spilled harbor water (22 μg L -1 spike level) revealed recoveries >80% for all tested carboxylic acids and low carry-overs of neutral petroleum compounds. We conclude that the isolation and fractionation of acidic degradation products by SPE is a powerful tool to investigate this new class of contaminants in relation to identification and ecological risk assessments., (Copyright © 2018 Elsevier B.V. All rights reserved.)

Hydraulic fracturing (HF) has allowed for the utilization of previously unattainable shale oil and gas (O&G) resources. After HF is complete, the waters used to increase the facies' permeability return uphole as wastewaters. When these waters return to the surface, they are characterized by complex organic and inorganic chemistry, and can pose a health risk if not handled correctly. Therefore, these waters must be treated or disposed of properly. However, the variability of these waters' chemical composition over time is poorly understood and likely limits the applicability of their reuse. This study examines the water chemistry of a hydraulically fractured site in the Niobrara formation throughout the flowback period. Samples were collected every other day for the first 18days, then on a regular basis for three months. We identified HF fluid additives, including benzalkonium chlorides (BACs), alkyl ethoxylates (AEOs), and polyethylene glycols (PEGs), as well as geogenic components present in flowback and produced waters, their overall temporal pattern, and variables affecting the reuse of these waters. Observations indicate that alkalinity and iron may limit the reuse of these waters in HF, while chloride and alkalinity may limit the use of these waters for well-casing cement. The presence of numerous surfactant homologs, including biocides, was also observed, with the highest levels at the beginning of the flowback period. Principal component analysis identified three unique groupings in the chemical data that correspond to different stages in the flowback period: (1) the flowback stage (days 1-2); (2) the transition stage (days 6-21); and (3) the produced water stage (days 21-87). Results from this study will be important when designing decision frameworks for assessing water treatment options, particularly if onsite treatment is attempted. Successful reclamation of these waters may alleviate stress on water resources that continues to negatively impact the U. S., (Copyright © 2017 Elsevier B.V. All rights reserved.)

Background: The schizophrenia-associated BRD1 gene encodes a transcriptional regulator whose comprehensive chromatin interactome is enriched with schizophrenia risk genes. However, the biology underlying the disease association of BRD1 remains speculative., Methods: This study assessed the transcriptional drive of a schizophrenia-associated BRD1 risk variant in vitro. Accordingly, to examine the effects of reduced Brd1 expression, we generated a genetically modified Brd1 +/- mouse and subjected it to behavioral, electrophysiological, molecular, and integrative genomic analyses with focus on schizophrenia-relevant parameters., Results: Brd1 +/- mice displayed cerebral histone H3K14 hypoacetylation and a broad range of behavioral changes with translational relevance to schizophrenia. These behaviors were accompanied by striatal dopamine/serotonin abnormalities and cortical excitation-inhibition imbalances involving loss of parvalbumin immunoreactive interneurons. RNA-sequencing analyses of cortical and striatal micropunches from Brd1 +/- and wild-type mice revealed differential expression of genes enriched for schizophrenia risk, including several schizophrenia genome-wide association study risk genes (e.g., calcium channel subunits [Cacna1c and Cacnb2], cholinergic muscarinic receptor 4 [Chrm4)], dopamine receptor D 2 [Drd2], and transcription factor 4 [Tcf4]). Integrative analyses further found differentially expressed genes to cluster in functional networks and canonical pathways associated with mental illness and molecular signaling processes (e.g., glutamatergic, monoaminergic, calcium, cyclic adenosine monophosphate [cAMP], dopamine- and cAMP-regulated neuronal phosphoprotein 32 kDa [DARPP-32], and cAMP responsive element binding protein signaling [CREB])., Conclusions: Our study bridges the gap between genetic association and pathogenic effects and yields novel insights into the unfolding molecular changes in the brain of a new schizophrenia model that incorporates genetic risk at three levels: allelic, chromatin interactomic, and brain transcriptomic., (Copyright © 2016 Society of Biological Psychiatry. Published by Elsevier Inc. All rights reserved.)

Autosomal dominant familial neurohypophyseal diabetes insipidus (adFNDI) is caused by variants in the arginine vasopressin (AVP) gene. Here we report the generation of induced pluripotent stem cells (iPSCs) from a 42-year-old man carrying an adFNDI causing variant in exon 1 of the AVP gene using lentivirus-mediated nuclear reprogramming. The iPSCs carried the expected variant in the AVP gene. Furthermore, the iPSCs expressed pluripotency markers; displayed in vitro differentiation potential to the three germ layers and had a normal karyotype consistent with the original fibroblasts. This iPSC line is useful in future studies focusing on the pathogenesis of adFNDI., (Copyright © 2016 The Authors. Published by Elsevier B.V. All rights reserved.)

Road runoff is an important source of pollution to the aquatic environment, and sedimentation ponds have been installed to mitigate effects on the aquatic environment. The purpose of this study was to investigate if a) fish from sedimentation ponds were affected by road pollution and; b) the transfer of PAHs from road runoff material to aquatic organisms was substantial. Minnow from a sedimentation pond (Skullerud) near Oslo (Norway) had higher levels of CYP1A enzyme and DNA stand breaks than minnow from the nearby river, but high concentrations of PAH-metabolites in bile revealed that both populations were highly exposed. Principal component analysis revealed that CYP1A and age of fish were correlated, while levels of PAH-metabolites were not correlated to CYP1A or DNA damage. Minnow from a lake un-affected by traffic had much lower levels of PAH-metabolites than the exposed fish, and also an improved condition. The latter results indicate that fish health was affected by road runoff. A closer investigation of PAH levels of the ecosystems of two sedimentation ponds (Skullerud and Vassum) and nearby environments were conducted. The concentration of the 16 EPA PAHs in sediments of the sedimentation ponds were high (1900-4200ngg(-1)), and even higher levels were observed in plants. Principal component analysis of selected ion chromatograms of PAHs showed a clear separation of plants vs. sediments. The plants preferentially accumulated the high molecular PAHs, both from sedimentation ponds with a petrogenic PAH isomer ratio in sediments; and from a lake with pyrogenic PAH isomer ratio in sediments., (Copyright © 2016 Elsevier B.V. All rights reserved.)

Glyphosate is a commonly applied herbicide in coffee plantations. Because of its non-selective mode of action it can damage the crop exposed through spray drift. Therefore, it is of interest to study glyphosate fate in coffee plants. The aim of this study was to develop an analytical method for accurate and precise quantification of glyphosate and its main metabolite aminomethylphosphonic acid (AMPA) at trace levels in coffee leaves using liquid chromatography with single-quadrupole mass spectrometry detection. The method is based on a two-step solid phase extraction (SPE) with an intermediate derivatization reaction using 9-fluorenylmethylchloroformate (FMOC). An isotope dilution method was used to account for matrix effects and to enhance the confidence in analyte identification. The limit of quantification (LOQ) for glyphosate and AMPA in coffee leaves was 41 and 111 μg kg(-1) dry weight, respectively. For the method optimization a design of experiments (DOE) approach was used. The sample clean-up procedure can be simplified for the analysis of less challenging matrices, for laboratories having a tandem mass spectrometry detector and for cases in which quantification limits above 0.1 mg kg(-1) are acceptable, which is often the case for glyphosate. The method is robust, possesses high identification confidence, while being suitable for most commercial and academic laboratories. All leaf samples from five coffee fields analyzed (n=21) contained glyphosate, while AMPA was absent. The simplified clean-up procedure was successfully validated for coffee leaves, rice, black beans and river water., (Copyright © 2015 Elsevier B.V. All rights reserved.)

Despite increased interest in marine oil exploration in the Arctic, little is known about the fate of Arctic offshore oil pollution. Therefore, in the present study, we examine the oil degradation potential for an Arctic site (Disko Bay, Greenland) and discuss this in relation to a temperate site (North Sea, Denmark). Biodegradation was assessed following exposure to Oseberg Blend crude oil (100 mg L(-1)) in microcosms. Changes in oil hydrocarbon fingerprints of polycyclic aromatic hydrocarbons (PAHs), alkyl-substituted PAHs, dibenzothiophenes, n-alkanes and alkyltoluenes were measured by gas chromatography-mass spectrometry (GC-MS). In the Disko Bay sample, the degradation order was n-alkanes>alkyltoluenes (para->meta->ortho-isomers)>PAHs and dibenzothiophenes, whereas, the degradation order in the North Sea samples was PAHs and dibenzothiophenes>alkyltoluenes>n-alkanes. These differences in degradation patterns significantly affect the environmental risk of oil spills and emphasise the need to consider the specific environmental conditions when conducting risk assessments of Arctic oil pollution., (Copyright © 2015 Elsevier B.V. All rights reserved.)

The development of an appropriate extraction method for untargeted environmental metabolomic analysis of marine polychaetes could promote their use for environmental monitoring purposes. To this end, we compared four extraction methods on the marine polychaete Nereis virens both exposed to crude oil and non-exposed. XCMS was used for feature detection and preprocessing; different normalization and scaling approaches were tested; and principal component analysis (PCA) was used together with basic statistical tests to ascertain common metabolic patterns and determine the most suitable extraction method. We conclude that a two-step extraction procedure with 80:20 (v/v) methanol:water on freeze dried polychaete tissue provides the best trade-off between analysis time, and extraction efficiency and intermediate reproducibility. No definitive conclusions could be drawn about the ability of the method to discriminate controls and crude oils in actual biological replicates because the experiment was carried out by design on analytical replicates only. We show that the normalization to the sum of all the common features, and the use of a weighted least squares criterion to fit the PCA by means of scaling to the median absolute deviation (MAD) of the pooled quality control samples significantly improved the clustering of controls and crude oil exposed samples. The scaling alone led to an increase of 19% in explained variance compared to ordinary PCA., (Copyright © 2015 Elsevier B.V. All rights reserved.)

A method for choosing orthogonal columns for a specific sample set in on-line comprehensive two-dimensional liquid chromatography (LC×LC) was developed on the basis of the hydrophobic subtraction model. The method takes into account the properties of the sample analytes by estimating new F-weights for the prediction of orthogonality. We compared sets of F-weights and used these F-weights to predict orthogonal column combinations: (1) the standard F-weights determined by Gilroy et al. [1], (2) F-weights determined from the retention of sample analytes, and the same procedure of calculation as described by Gilroy et al. [1], (3) F-weights determined from the retention of sample analytes but using principal component analysis (PCA) for the estimation, and (4) the Gilroy F-weights modified by excluding the C-term in the hydrophobic subtraction model, as suggested by Dolan and Snyder [2]. The retention of 13 neutral and 4 acidic oxygenated polycyclic aromatic compounds (PACs) and 3 nitrogen-containing PAC bases was measured isocratically on 12 columns. The isocratic runs were used to determine the hydrophobic subtraction model analyte parameters, and these were used to estimate new F-weights and predict orthogonal column combinations. LC×LC-DAD analysis was then performed on a test mix using these column sets. We found that the column combination predicted from the new F-weights provide a more orthogonal separation of the PACs than those predicted using the standard F-weights and the F-weights modified by excluding the C-term. This emphasizes the necessity of considering the nature of the sample when choosing orthogonal columns., (Copyright © 2013 Elsevier B.V. All rights reserved.)

This study presents the possible regional climate change over South Asia with a focus over India as simulated by three very high resolution regional climate models (RCMs). One of the most striking results is a robust increase in monsoon precipitation by the end of the 21st century but regional differences in strength. First the ability of RCMs to simulate the monsoon climate is analyzed. For this purpose all three RCMs are forced with ECMWF reanalysis data for the period 1989-2008 at a horizontal resolution of ~25 km. The results are compared against independent observations. In order to simulate future climate the models are driven by lateral boundary conditions from two global climate models (GCMs: ECHAM5-MPIOM and HadCM3) using the SRES A1B scenario, except for one RCM, which only used data from one GCM. The results are presented for the full transient simulation period 1970-2099 and also for several time slices. The analysis concentrates on precipitation and temperature over land. All models show a clear signal of gradually wide-spread warming throughout the 21st century. The ensemble-mean warming over India is 1.5°C at the end of 2050, whereas it is 3.9°C at the end of century with respect to 1970-1999. The pattern of projected precipitation changes shows considerable spatial variability, with an increase in precipitation over the peninsular of India and coastal areas and, either no change or decrease further inland. From the analysis of a larger ensemble of global climate models using the A1B scenario a wide spread warming (~3.2°C) and an overall increase (~8.5%) in mean monsoon precipitation by the end of the 21st century is very likely. The influence of the driving GCM on the projected precipitation change simulated with each RCM is as strong as the variability among the RCMs driven with one., (Copyright © 2013 Elsevier B.V. All rights reserved.)