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Critical Insights into Untargeted GC-HRMS Analysis: Exploring Volatile Organic Compounds in Italian Ambient Air
Full text linkThis study critically examines the workflow for untargeted analysis of volatile organic compounds (VOCs) in ambient air, from sampling strategies to data interpretation by using GC-HRMS. While untargeted approaches are well-established in liquid chromatography (LC) due to advanced-deconvolution tools and extensive metabolomic libraries, their application in gas chromatography (GC) remains less developed, particularly for VOCs. The high structural isomerism of VOCs and the relative novelty of GC-based untargeted methodologies present unique challenges, including limited software tools and reference libraries. Air samples from suburban and rural sites in central Italy were analyzed to explore chemical diversity and address methodological gaps. This study evaluates critical decisions, such as sampling strategies, extraction techniques, and data-processing workflows, highlighting the limitations of automated deconvolution tools and the need for manual validation. Results revealed distinct source contributions, with suburban areas showing higher levels of anthropogenic compounds and rural areas dominated by biogenic emissions. This work underscores the potential of GC-HRMS untargeted analysis to advance environmental chemistry, while addressing key pitfalls and providing practical recommendations for reliable application. By bridging methodological gaps, it offers a roadmap for future studies aiming to integrate untargeted and targeted approaches in air quality research.publishedVersio
A scalable framework for harmonizing, standardization, and correcting crowd-sourced low-cost sensor PM2.5 data across Europe
Full text linkCitizen-operated low-cost air quality sensors (LCSs) have expanded air quality monitoring through community engagement. However, still challenges related to lack of semantic standards, data quality, and interoperability hinder their integration into official air quality assessments, management, and research. Here, we introduce FILTER, a geospatially scalable framework designed to unify, correct, and enhance the reliability of crowd-sourced PM2.5 data across various LCS networks. FILTER assesses data quality through five steps: range check, constant value detection, outlier detection, spatial correlation, and spatial similarity. Using official data, we modeled PM2.5 spatial correlation and similarity (Euclidean distance) as functions of geographic distance as benchmarks for evaluating whether LCS measurements are sufficiently correlated/consistent with neighbors. Our study suggests a −10 to 10 Median Absolute Deviation threshold for outlier flagging (360 h). We find higher PM2.5 spatial correlation in DJF compared to JJA across Europe while lower PM2.5 similarity in DJF compared to JJA. We observe seasonal variability in the maximum possible distance between sensors and reference stations for in-situ (remote) PM2.5 data correction, with optimal thresholds of ∼11.5 km (DJF), ∼12.7 km (MAM), ∼20 km (JJA), and ∼17 km (SON). The values implicitly reflect the spatial representativeness of stations. ±15 km relaxation for each season remains feasible when data loss is a concern. We demonstrate and validate FILTER's effectiveness using European-scale data originating from the two community-based monitoring networks, sensor.community and PurpleAir with QC-ed/corrected output including 37,085 locations and 521,115,762 hourly timestamps. Results facilitate uptake and adoption of crowd-sourced LCS data in regulatory applications.publishedVersio
Sovereignty-Aware Intrusion Detection on Streaming Data: Automatic Machine Learning Pipeline and Semantic Reasoning
Full text linkIntrusion Detection Systems (IDS) are critical in safeguarding network infrastructures against malicious attacks. Traditional IDSs often struggle with knowledge representation, real-time detection, and accuracy, especially when dealing with high-throughput data. This paper proposes a novel IDS framework that leverages machine learning models, streaming data, and semantic knowledge representation to enhance intrusion detection accuracy and scalability. Additionally, the study incorporates the concept of Digital Sovereignty, ensuring that data control, security, and privacy are maintained according to national and regional regulations. The proposed system integrates Apache Kafka for real-time data processing, an automatic machine learning pipeline (e.g., Tree-based Pipeline Optimization Tool (TPOT)) for classifying network traffic, and OWL-based semantic reasoning for advanced threat detection. The proposed system, evaluated on NSL-KDD and CIC-IDS-2017 datasets, demonstrated qualitative outcomes such as local compliance, reduced data storage needs due to real-time processing, and improved adaptability to local data laws. Experimental results reveal significant improvements in detection accuracy, processing efficiency, and Sovereignty alignment.publishedVersio
Sources of ultrafine particles at a rural midland site in Switzerland
Full text linkUltrafine particles (UFPs; i.e., atmospheric aerosol particles smaller than 100 nm in diameter) are known to be responsible for a series of adverse health effects as they can deposit in humans' bodies. So far, most field campaigns studying the sources of UFPs have focused on urban environments. This study investigates the outdoor sources of UFPs at the atmospheric monitoring station in Payerne, which represents a typical rural location in Switzerland. We aim to quantify the primary and secondary fractions of UFPs based on specific measurements between July 2020 and July 2021 complementing a series of operational meteorological, trace gas and in situ aerosol observations. To distinguish between primary and secondary contributions, we use a method that relies on measuring the fraction of non-volatile particles as a proxy for primary particles. We further compare our measurement results to previously established methods. We find that primary particles resulting from traffic and residential wood burning (direct emissions – mostly non-volatile BC-rich) contribute less than 40 % to the total number of UFPs, mostly in the Aitken mode. On the other hand, we observe local new particle formation (NPF) events (observed from ∼ 1 nm) evident from the increase in cluster ions (1.5–3 nm) and nucleation-mode particle (2.5–25 nm) concentrations, especially in spring and summer. These events, mediated by sulfuric acid, contribute to increasing the UFP number concentration, especially in the nucleation mode. Besides NPF, the chemical processing of particles emitted from multiple sources (including traffic and residential wood burning) contributes substantially to the nucleation-mode particle concentration. Under the present conditions investigated here, we find that secondary processes mediate the increase in UFP concentration to levels equivalent to those in urban locations, affecting both air quality and human health.publishedVersio
New Approach Methods (NAMs) for genotoxicity assessment of nano- and advanced materials; Advantages and challenges
Full text linkGenotoxicity assessment is essential for ensuring chemical safety and mitigating risks to human health and the environment. Traditional methods, reliant on animal models, are time-consuming, costly, and raise ethical concerns. New Approach Methods (NAMs) offer innovative, cost-effective, and ethical alternatives, playing a pivotal role in both traditional and next-generation risk assessment (NGRA) by minimizing the need for animal testing, particularly in genotoxicity evaluations. However, the development of NAMs often overlooks the particular physicochemical properties of nanomaterials (NMs), which significantly influence their toxicological behaviour and can interfere with genotoxicity evaluation. This underscores an urgent need for the standardization and adaptation of NAMs to address nano- and advanced material-specific genotoxicity challenges. In this review, we summarize the challenges associated with genotoxicity testing of NMs and highlight the suitability of existing in vitro and in silico NAMs for NMs and advanced materials, enabling genotoxicity testing across various exposure routes and organ systems. Despite considerable progress, regulatory validation remains constrained by the absence of approved test guidelines and standardized protocols. To achieve regulatory acceptance, it is crucial to adapt NAMs to NM-specific exposure scenarios, refine test systems to better mimic human biology, develop tailored in vitro protocols, and ensure thorough characterisation of NMs both in pristine form and dispersed in culture medium. Collaborative efforts among scientists, regulators, industry, and advocacy groups are vital to improving the reliability and regulatory acceptance of NAMs. By addressing these challenges, NAMs have the potential to revolutionize genotoxicity risk assessment, advancing it towards a more sustainable, efficient and ethical framework.publishedVersio
HTAP3 Fires: towards a multi-model, multi-pollutant study of fire impacts
Full text linkOpen biomass burning has major impacts globally and regionally on atmospheric composition. Fire emissions include particulate matter, tropospheric ozone precursors, and greenhouse gases, as well as persistent organic pollutants, mercury, and other metals. Fire frequency, intensity, duration, and location are changing as the climate warms, and modelling these fires and their impacts is becoming more and more critical to inform climate adaptation and mitigation, as well as land management. Indeed, the air pollution from fires can reverse the progress made by emission controls on industry and transportation. At the same time, nearly all aspects of fire modelling – such as emissions, plume injection height, long-range transport, and plume chemistry – are highly uncertain. This paper outlines a multi-model, multi-pollutant, multi-regional study to improve the understanding of the uncertainties and variability in fire atmospheric science, models, and fires' impacts, in addition to providing quantitative estimates of the air pollution and radiative impacts of biomass burning. Coordinated under the auspices of the Task Force on Hemispheric Transport of Air Pollution, the international atmospheric modelling and fire science communities are working towards the common goal of improving global fire modelling and using this multi-model experiment to provide estimates of fire pollution for impact studies. This paper outlines the research needs, opportunities, and options for the fire-focused multi-model experiments and provides guidance for these modelling experiments, outputs, and analyses that are to be pursued over the next 3 to 5 years. The paper proposes a plan for delivering specific products at key points over this period to meet important milestones relevant to science and policy audiences.publishedVersio
Hazard characterization of the mycotoxins enniatins and beauvericin to identify data gaps and improve risk assessment for human health
Full text linkEnniatins (ENNs) and beauvericin (BEA) are cyclic hexadepsipeptide fungal metabolites which have demonstrated antibiotic, antimycotic, and insecticidal activities. The substantial toxic potentials of these mycotoxins are associated with their ionophoric molecular properties and relatively high lipophilicities. ENNs occur extensively in grain and grain-derived products and are considered a food safety issue by the European Food Safety Authority (EFSA). The tolerable daily intake and maximum levels for ENNs in humans and animals remain unestablished due to key toxicological and toxicokinetic data gaps, preventing full risk assessment. Aiming to find critical data gaps impeding hazard characterization and risk evaluation, this review presents a comprehensive summary of the existing information from in vitro and in vivo studies on toxicokinetic characteristics and cytotoxic, genotoxic, immunotoxic, endocrine, reproductive and developmental effects of the most prevalent ENN analogues (ENN A, A1, B, B1) and BEA. The missing information identified showed that additional studies on ENNs and BEA have to be performed before sufficient data for an in-depth hazard characterisation of these mycotoxins become available.publishedVersio
Using a citizen science approach to assess nanoplastics pollution in remote high-altitude glaciers
Full text linkNanoplastics are suspected to pollute every environment on Earth, including very remote areas reached via atmospheric transport. We approached the challenge of measuring environmental nanoplastics by combining high-sensitivity TD-PTR-MS (thermal desorption-proton transfer reaction-mass spectrometry) with trained mountaineers sampling high-altitude glaciers (“citizen science”). Particles < 1 μm were analysed for common polymers (polyethylene, polyethylene terephthalate, polypropylene, polyvinyl chloride, polystyrene and tire wear particles), revealing nanoplastic concentrations ranging 2–80 ng mL− 1 at five of 14 sites. The dominant polymer types found in this study were tire wear, polystyrene and polyethylene particles (41%, 28% and 12%, respectively). Lagrangian dispersion modelling was used to reconstruct possible sources of micro- and nanoplastic emissions for those observations, which appear to lie largely to the west of the Alps. France, Spain and Switzerland have the highest contributions to the modelled emissions. The citizen science approach was found to be feasible providing strict quality control measures are in place, and is an effective way to be able to collect data from remote and inaccessible regions across the world.publishedVersio
Daily high-resolution surface PM2.5 estimation over Europe by ML-based downscaling of the CAMS regional forecast
Full text linkFine particulate matter (PM2.5) is a key air quality indicator due to its adverse health impacts. Accurate PM2.5 assessment requires high-resolution (e.g., atleast 1 km) daily data, yet current methods face challenges in balancing accuracy, coverage, and resolution. Chemical transport models such as those from the Copernicus Atmosphere Monitoring Service (CAMS) offer continuous data but their relatively coarse resolution can introduce uncertainties. Here we present a synergistic Machine Learning (ML)-based approach called S-MESH (Satellite and ML-based Estimation of Surface air quality at High resolution) for estimating daily surface PM2.5 over Europe at 1 km spatial resolution and demonstrate its performance for the years 2021 and 2022. The approach enhances and downscales the CAMS regional ensemble 24 h PM2.5 forecast by training a stacked XGBoost model against station observations, effectively integrating satellite-derived data and modeled meteorological variables. Overall, against station observations, S-MESH (mean absolute error (MAE) of 3.54 μg/m3) shows higher accuracy than the CAMS forecast (MAE of 4.18 μg/m3) and is approaching the accuracy of the CAMS regional interim reanalysis (MAE of 3.21 μg/m3), while exhibiting a significantly reduced mean bias (MB of −0.3 μg/m3 vs. −1.5 μg/m3 for the reanalysis). At the same time, S-MESH requires substantially less computational resources and processing time. At concentrations >20 μg/m3, S-MESH outperforms the reanalysis (MB of −7.3 μg/m3 and -10.3 μg/m3 respectively), and reliably captures high pollution events in both space and time. In the eastern study area, where the reanalysis often underestimates, S-MESH better captures high levels of PM2.5 mostly from residential heating. S-MESH effectively tracks day-to-day variability, with a temporal relative absolute error of 5% (reanalysis 10%). Exhibiting good performance at high pollution events coupled with its high spatial resolution and rapid estimation speed, S-MESH can be highly relevant for air quality assessments where both resolution and timeliness are critical.publishedVersio
Overvåking av langtransportert forurenset luft og nedbør Atmosfæriske tilførsler 2024
No full textThis report presents results from the monitoring of atmospheric composition and deposition of air pollution in 2024, and focuses on main components in air and precipitation, particulate and gaseous phase of inorganic constituents, particulate carbonaceous matter, ground level ozone and particulate matter.Denne rapporten omhandler resultater fra overvåkningsprogrammet for langtransportert forurenset luft og nedbør og atmosfæriske tilførsler i 2024. Rapporten presenterer målinger av uorganiske hovedkomponentene i luft og nedbør, partikulært karbonholdig materiale, partikkelmasse og bakkenært ozon.publishedVersio