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Intercorrelations of Chlorinated Paraffins, Dechloranes, and Legacy Persistent Organic Pollutants in 10 Species of Marine Mammals from Norway, in Light of Dietary Niche
Get PDFShort-, medium-, and long-chain chlorinated paraffins (CPs) (SCCPs, MCCPs, and LCCPs) and dechloranes are chemicals of emerging concern; however, little is known of their bioaccumulative potential compared to legacy contaminants in marine mammals. Here, we analyzed SCCPs, MCCPs, LCCPs, 7 dechloranes, 4 emerging brominated flame retardants, and 64 legacy contaminants, including polychlorinated biphenyls (PCBs), in the blubber of 46 individual marine mammals, representing 10 species, from Norway. Dietary niche was modeled based on stable isotopes of nitrogen and carbon in the skin/muscle to assess the contaminant accumulation in relation to diet. SCCPs and dechlorane-602 were strongly positively correlated with legacy contaminants and highest in killer (Orcinus orca) and sperm (Physeter macrocephalus) whales (median SCCPs: 160 ng/g lw; 230 ng/g lw and median dechlorane-602: 3.8 ng/g lw; 2.0 ng/g lw, respectively). In contrast, MCCPs and LCCPs were only weakly correlated to recalcitrant legacy contaminants and were highest in common minke whales (Balaenoptera acutorostrata; median MCCPs: 480 ng/g lw and LCCPs: 240 ng/g lw). The total contaminant load in all species was dominated by PCBs and legacy chlorinated pesticides (63–98%), and MCCPs dominated the total CP load (42–68%, except 11% in the long-finned pilot whale Globicephala melas). Surprisingly, we found no relation between contaminant concentrations and dietary niche, suggesting that other large species differences may be masking effects of diet such as lifespan or biotransformation and elimination capacities. CP and dechlorane concentrations were higher than in other marine mammals from the (sub)Arctic, and they were present in a killer whale neonate, indicating bioaccumulative properties and a potential for maternal transfer in these predominantly unregulated chemicals.publishedVersio
Combined Contaminant Levels from Local Harvested Food Items in the Norwegian–Finnish–Russian Border Region
Get PDFThis paper presents the results of a multidisciplinary study with the aim of assessing the potential combined risk from consuming locally harvested food products in the Euro-Arctic region of Norway, Finland, and Russia. The three important contaminant groups—radioactive substances, heavy metals, and persistent organic pollutants (POPs)—were measured in food samples such as berries, mushrooms, fish, birds, reindeer, and moose; they were sampled in 2013–2015. To assess the combined pollution levels and investigate the trends, similarities, and variations between different contaminant groups, subsequent multivariate statistical analysis was performed. The results showed that, in general, the levels of radioactive substances, toxic elements, and POPs were below the permitted EU maximum content in food products. However, statistical analysis revealed some correlations, similarities, and peculiarities between the accumulation of different contaminants in various species, which allowed for a better understanding of the mechanisms of accumulation and interaction between different contaminant groups. It also gave a better insight into the possible added risks and helped pinpoint species that could serve as reference markers for the accumulation of different contaminants in food. Mushrooms, fish, and reindeer were found to be important markers in the combined risk assessments for the contents of metals and radioactive substances. Further research, as well as the development of methodologies for combined assessments, are recommended.publishedVersio
Ammonia emission estimates using CrIS satellite observations over Europe
Get PDFOver the past century, ammonia (NH3) emissions have increased with the growth of livestock and fertilizer usage. The abundant NH3 emissions lead to secondary fine particulate matter (PM2.5) pollution, climate change, and a reduction in biodiversity, and they affect human health. Up-to-date and spatially and temporally resolved information on NH3 emissions is essential to better quantify their impact. In this study we applied the existing Daily Emissions Constrained by Satellite Observations (DECSO) algorithm to NH3 observations from the Cross-track Infrared Sounder (CrIS) to estimate NH3 emissions. Because NH3 in the atmosphere is influenced by nitrogen oxides (NOx), we implemented DECSO to estimate NOx and NH3 emissions simultaneously. The emissions are derived over Europe for 2020 on a spatial resolution of 0.2°×0.2° using daily observations from both CrIS and the TROPOspheric Monitoring Instrument (TROPOMI; on the Sentinel-5 Precursor (S5P) satellite). Due to the limited number of daily satellite observations of NH3, monthly emissions of NH3 are reported. The total NH3 emissions derived from observations are about 8 Tg yr−1, with a precision of about 5 %–17 % per grid cell per year over the European domain (35–55° N, 10° W–30° E). The comparison of the satellite-derived NH3 emissions from DECSO with independent bottom-up inventories and in situ observations indicates a consistency in terms of magnitude on the country totals, with the results also being comparable regarding the temporal and spatial distributions. The validation of DECSO over Europe implies that we can use DECSO to quickly derive fairly accurate monthly emissions of NH3 over regions with limited local information on NH3 emissions.publishedVersio
Estimating stratospheric polar vortex strength using ambient ocean-generated infrasound and stochastics-based machine learning
Get PDFThere are sparse opportunities for direct measurement of upper stratospheric winds, yet improving their representation in subseasonal-to-seasonal prediction models can have significant benefits. There is solid evidence from previous research that global atmospheric infrasound waves are sensitive to stratospheric dynamics. However, there is a lack of results providing a direct mapping between infrasound recordings and polar-cap upper stratospheric winds. The global International Monitoring System (IMS), which monitors compliance with the Comprehensive Nuclear-Test-Ban Treaty, includes ground-based stations that can be used to characterize the infrasound soundscape continuously. In this study, multi-station IMS infrasound data were utilized along with a machine-learning supported stochastic model, Delay-SDE-net, to demonstrate how a near-real-time estimate of the polar-cap averaged zonal wind at 1-hPa pressure level can be found from infrasound data. The infrasound was filtered to a temporal low-frequency regime dominated by microbaroms, which are ambient-noise infrasonic waves continuously radiated into the atmosphere from nonlinear interaction between counter-propagating ocean surface waves. Delay-SDE-net was trained on 5 years (2014–2018) of infrasound data from three stations and the ERA5 reanalysis 1-hPa polar-cap averaged zonal wind. Using infrasound in 2019–2020 for validation, we demonstrate a prediction of the polar-cap averaged zonal wind, with an error standard deviation of around 12 m·s compared with ERA5. These findings highlight the potential of using infrasound data for near-real-time measurements of upper stratospheric dynamics. A long-term goal is to improve high-top atmospheric model accuracy, which can have significant implications for weather and climate prediction.publishedVersio
Zürich II Statement on Per- and Polyfluoroalkyl Substances (PFASs): Scientific and Regulatory Needs
No full textPer- and polyfluoroalkyl substances (PFASs) are a class of synthetic organic chemicals of global concern. A group of 36 scientists and regulators from 18 countries held a hybrid workshop in 2022 in Zürich, Switzerland. The workshop, a sequel to a previous Zürich workshop held in 2017, deliberated on progress in the last five years and discussed further needs for cooperative scientific research and regulatory action on PFASs. This review reflects discussion and insights gained during and after this workshop and summarizes key signs of progress in science and policy, ongoing critical issues to be addressed, and possible ways forward. Some key take home messages include: 1) understanding of human health effects continues to develop dramatically, 2) regulatory guidelines continue to drop, 3) better understanding of emissions and contamination levels is needed in more parts of the world, 4) analytical methods, while improving, still only cover around 50 PFASs, and 5) discussions of how to group PFASs for regulation (including subgroupings) have gathered momentum with several jurisdictions proposing restricting a large proportion of PFAS uses. It was concluded that more multi-group exchanges are needed in the future and that there should be a greater diversity of participants at future workshops.publishedVersio
The Greenhouse Gas Budget of Terrestrial Ecosystems in East Asia Since 2000
Get PDFEast Asia (China, Japan, Koreas, and Mongolia) has been the world's economic engine over at least the past two decades, exhibiting a rapid increase in fossil fuel emissions of greenhouse gases (GHGs) and has expressed the recent ambition to achieve climate neutrality by mid-century. However, the GHG balance of its terrestrial ecosystems remains poorly constrained. Here, we present a synthesis of the three most important long-lived greenhouse gases (CO2, CH4, and N2O) budgets over East Asia during the decades of 2000s and 2010s, following a dual constraint approach. We estimate that terrestrial ecosystems in East Asia is close to neutrality of GHGs, with a magnitude of between −46.3 ± 505.9 Tg CO2eq yr−1 (the top-down approach) and −36.1 ± 207.1 Tg CO2eq yr−1 (the bottom-up approach) during 2000–2019. This net GHG sink includes a large land CO2 sink (−1229.3 ± 430.9 Tg CO2 yr−1 based on the top-down approach and −1353.8 ± 158.5 Tg CO2 yr−1 based on the bottom-up approach) being offset by biogenic CH4 and N2O emissions, predominantly coming from the agricultural sectors. Emerging data sources and modeling capacities have helped achieve agreement between the top-down and bottom-up approaches, but sizable uncertainties remain in several flux terms. For example, the reported CO2 flux from land use and land cover change varies from a net source of more than 300 Tg CO2 yr−1 to a net sink of ∼−700 Tg CO2 yr−1. Although terrestrial ecosystems over East Asia is close to GHG neutral currently, curbing agricultural GHG emissions and additional afforestation and forest managements have the potential to transform the terrestrial ecosystems into a net GHG sink, which would help in realizing East Asian countries' ambitions to achieve climate neutrality.publishedVersio
Estimating volcanic ash emissions using retrieved satellite ash columns and inverse ash transport modelling using VolcanicAshInversion v1.2.1, within the operational eEMEP volcanic plume forecasting system (version rv4_17)
No full textAccurate modeling of ash clouds from volcanic eruptions requires knowledge about the eruption source parameters including eruption onset, duration, mass eruption rates, particle size distribution, and vertical-emission profiles. However, most of these parameters are unknown and must be estimated somehow. Some are estimated based on observed correlations and known volcano parameters. However, a more accurate estimate is often needed to bring the model into closer agreement with observations. This paper describes the inversion procedure implemented at the Norwegian Meteorological Institute for estimating ash emission rates from retrieved satellite ash column amounts and a priori knowledge. The overall procedure consists of five stages: (1) generate a priori emission estimates, (2) run forward simulations with a set of unit emission profiles, (3) collocate/match observations with emission simulations, (4) build system of linear equations, and (5) solve overdetermined systems. We go through the mathematical foundations for the inversion procedure, performance for synthetic cases, and performance for real-world cases. The novelties of this paper include a memory efficient formulation of the inversion problem, a detailed description and illustrations of the mathematical formulations, evaluation of the inversion method using synthetic known-truth data as well as real data, and inclusion of observations of ash cloud-top height. The source code used in this work is freely available under an open-source license and is able to be used for other similar applications.publishedVersio
Comparison of observation- and inventory-based methane emissions for eight large global emitters
Get PDFMonitoring the spatial distribution and trends in surface greenhouse gas (GHG) fluxes, as well as flux attribution to natural and anthropogenic processes, is essential to track progress under the Paris Agreement and to inform its global stocktake. This study updates earlier syntheses (Petrescu et al., 2020, 2021, 2023), provides a consolidated synthesis of CH4 emissions using bottom-up (BU) and top-down (TD) approaches for the European Union (EU), and is expanded to include seven additional countries with large anthropogenic and/or natural emissions (the USA, Brazil, China, India, Indonesia, Russia, and the Democratic Republic of the Congo (DR Congo)). Our aim is to demonstrate the use of different emission estimates to help improve national GHG emission inventories for a diverse geographical range of stakeholders. We use updated national GHG inventories (NGHGIs) reported by Annex I parties under the United Nations Framework Convention on Climate Change (UNFCCC) in 2023 and the latest available biennial update reports (BURs) reported by non-Annex I parties. Comparing NGHGIs with other approaches highlights that different system boundaries are a key source of divergence. A key system boundary difference is whether anthropogenic and natural fluxes are included and, if they are, how fluxes belonging to these two sources are partitioned. Over the studied period, the total CH4 emission estimates in the EU, the USA, and Russia show a steady decreasing trend since 1990, while for the non-Annex I emitters analyzed in this study, Brazil, China, India, Indonesia, and DR Congo, CH4 emissions have generally increased. Quantitatively, in the EU the mean of 2015–2020 anthropogenic UNFCCC NGHGIs (15±1.8 Tg CH4 yr−1) and the mean of the BU CH4 emissions (17.8 (16–19) Tg CH4 yr−1) generally agree on the magnitude, while inversions show higher emission estimates (medians of 21 (19–22) Tg CH4 yr−1 and 24 (22–25) Tg CH4 yr−1 for the three regional and six global inversions, respectively), as they include natural emissions, which for the EU were quantified at 6.6 Tg CH4 yr−1 (Petrescu et al., 2023). Similarly, for the other Annex I parties in this study (the USA and Russia), the gap between the BU anthropogenic and total TD emissions is partly explained by the natural emissions. For the non-Annex I parties, anthropogenic CH4 estimates from UNFCCC BURs show large differences compared to the other global-inventory-based estimates and even more compared to atmospheric ones. This poses an important potential challenge to monitoring the progress of the global CH4 pledge and the global stocktake. Our analysis provides a useful baseline to prepare for the influx of inventories from non-Annex I parties as regular reporting starts under the enhanced transparency framework of the Paris Agreement. By systematically comparing the BU and TD methods, this study provides recommendations for more robust comparisons of available data sources and hopes to steadily engage more parties in using observational methods to complement their UNFCCC inventories, as well as considering their natural emissions. With anticipated improvements in atmospheric modeling and observations, as well as modeling of natural fluxes, future development needs to resolve knowledge gaps in the BU and TD approaches and to better quantify the remaining uncertainty. TD methods may emerge as a powerful tool to help improve NGHGIs of CH4 emissions, but further confidence is needed in the comparability and robustness of the estimates. The referenced datasets related to figures are available at https://doi.org/10.5281/zenodo.12818506 (Petrescu et al., 2024).publishedVersio
Development of a supramolecular solvent-based extraction method for application to quantitative analyses of a wide range of organic contaminants in indoor dust
Get PDFThis study investigates the efficacy of supramolecular solvent (SUPRAS) in extracting a diverse spectrum of organic contaminants from indoor dust. Initially, seven distinct SUPRAS were assessed across nine categories of contaminants to identify the most effective one. A SUPRAS comprising Milli-Q water, tetrahydrofuran, and hexanol in a 70:20:10 ratio, respectively, demonstrated the best extraction performance and was employed for testing a wider array of organic contaminants. Furthermore, we applied the selected SUPRAS for the extraction of organic compounds from the NIST Standard Reference Material (SRM) 2585. In parallel, we performed the extraction of NIST SRM 2585 with conventional extraction methods using hexane:acetone (1:1) for non-polar contaminants and methanol (100%) extraction for polar contaminants. Analysis from two independent laboratories (in Norway and the Czech Republic) demonstrated the viability of SUPRAS for the simultaneous extraction of twelve groups of organic contaminants with a broad range of physico-chemical properties including plastic additives, pesticides, and combustion by-products. However, caution is advised when employing SUPRAS for highly polar contaminants like current-use pesticides or volatile substances like naphthalene.publishedVersio
Limits to graphite supply in a transition to a post-fossil society
Get PDFTransitioning to electric vehicles (EVs) powered by lithium-ion batteries (LIBs) aims at reducing emissions in the transportation sector, thereby decreasing fuel oil use and crude oil extraction. Yet, synthetic graphite, a crucial anode material for LIBs, is produced from needle coke, a byproduct of oil refining. This dependency could lead to bottlenecks in battery anode production. We found no obvious supply constraints for synthetic graphite in slow electrification scenarios based on different International Energy Agency scenarios. In contrast, net zero scenarios reveal drastic limitations in synthetic graphite supply, due to fast electrification and declining needle coke production. Natural graphite can mitigate supply limitations but faces environmental concerns, long development time and geopolitical concerns. Securing graphite supply while reaching the net zero goals requires comprehensive strategies combining (1) systematic graphite recycling, (2) overcoming current technical challenges, and (3) behavioral shifts towards reduced vehicle ownership and smaller vehicles.publishedVersio