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Background
Hazard and risk assessment of nanomaterials (NMs) face challenges due to, among others, the numerous existing nanoforms, discordant data and conflicting results found in the literature, and specific challenges in the application of strategies such as grouping and read-across, emphasizing the need for New Approach Methodologies (NAMs) to support Next Generation Risk Assessment (NGRA). Here these challenges are addressed in a study that couples physico-chemical characterization with in vitro investigations and in silico similarity analyses for nine nanoforms, having different chemical composition, sizes, aggregation states and shapes. For cytotoxicity assessment, three methods (Alamar Blue, Colony Forming Efficiency, and Electric Cell-Substrate Impedance Sensing) are applied in a cross-validation approach to support NAMs implementation into NGRA.
Results
The results highlight the role of physico-chemical properties in eliciting biological responses. Uptake studies reveal distinct cellular morphological changes. The cytotoxicity assessment shows varying responses among NMs, consistent among the three methods used, while only one nanoform gave a positive response in the genotoxicity assessment performed by comet assay.
Conclusions
The study highlights the potential of in silico models to effectively identify biologically active nanoforms based on their physico-chemical properties, reinforcing previous knowledge on the relevance of certain properties, such as aspect ratio. The potential of implementing in vitro methods into NGRA is underlined, cross-validating three cytotoxicity assessment methods, and showcasing their strength in terms of sensitivity and suitability for the testing of NMs.
2024
2024
Holocene black carbon in New Zealand lake sediment records
Black carbon emitted from incomplete combustion of biomass and fossil fuel burning is an important aerosol; however, available long-term black carbon data are limited to remote polar and high-alpine ice cores from few geographic regions. Black carbon records from lake sediments fill geographic gaps but such records are still scarce, particularly in the Southern Hemisphere. We applied a new incandescence-based methodology to develop Holocene refractory black carbon (rBC) records from four lake-sediment archives in New Zealand and compare these with macroscopic charcoal records. Our rBC records suggest periods with substantial rBC deposition during the Holocene before human arrival in the 13th century reflecting long-range transport and possibly local wetland fires. With Polynesian settlement, rBC deposition increased on the South Island in agreement with macroscopic charcoal records, and it is this period of burning that is proposed as the source of rBC increases evident in Antarctic ice cores. However, sites on the North Island show no contemporaneous rBC increase suggesting regional differences in biomass burning patterns between the North and South islands. None of the New Zealand records show an increase in rBC from fossil fuel sources during the Industrial Era post-1850 CE.
2024
Comparison of observation- and inventory-based methane emissions for eight large global emitters
Monitoring 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).
2024
The Modeled Seasonal Cycles of Surface N2O Fluxes and Atmospheric N2O
Nitrous oxide (N2O) is a greenhouse gas and stratospheric ozone-depleting substance with large and growing anthropogenic emissions. Previous studies identified the influx of N2O-depleted air from the stratosphere to partly cause the seasonality in tropospheric N2O (aN2O), but other contributions remain unclear. Here, we combine surface fluxes from eight land and four ocean models from phase 2 of the Nitrogen/N2O Model Intercomparison Project with tropospheric transport modeling to simulate aN2O at eight remote air sampling sites for modern and pre-industrial periods. Models show general agreement on the seasonal phasing of zonal-average N2O fluxes for most sites, but seasonal peak-to-peak amplitudes differ several-fold across models. The modeled seasonal amplitude of surface aN2O ranges from 0.25 to 0.80 ppb (interquartile ranges 21%–52% of median) for land, 0.14–0.25 ppb (17%–68%) for ocean, and 0.28–0.77 ppb (23%–52%) for combined flux contributions. The observed seasonal amplitude ranges from 0.34 to 1.08 ppb for these sites. The stratospheric contributions to aN2O, inferred by the difference between the surface-troposphere model and observations, show 16%–126% larger amplitudes and minima delayed by ∼1 month compared to Northern Hemisphere site observations. Land fluxes and their seasonal amplitude have increased since the pre-industrial era and are projected to grow further under anthropogenic activities. Our results demonstrate the increasing importance of land fluxes for aN2O seasonality. Considering the large model spread, in situ aN2O observations and atmospheric transport-chemistry models will provide opportunities for constraining terrestrial and oceanic biosphere models, critical for projecting carbon-nitrogen cycles under ongoing global warming.
2024
PFAS Exposure is Associated with a Lower Spermatic Quality in an Arctic Seabird
Several studies have reported an increasing occurrence of poly- and perfluorinated alkyl substances (PFASs) in Arctic wildlife tissues, raising concerns due to their resistance to degradation. While some research has explored PFAS’s physiological effects on birds, their impact on reproductive functions, particularly sperm quality, remains underexplored. This study aims to assess (1) potential association between PFAS concentrations in blood and sperm quality in black-legged kittiwakes (Rissa tridactyla), focusing on the percentage of abnormal spermatozoa, sperm velocity, percentage of sperm motility, and morphology; and (2) examine the association of plasma levels of testosterone, corticosterone, and luteinizing hormone with both PFAS concentrations and sperm quality parameters to assess possible endocrine disrupting pathways. Our findings reveal a positive correlation between the concentration of longer-chain perfluoroalkyl carboxylates (PFCA; C11–C14) in blood and the percentage of abnormal sperm in kittiwakes. Additionally, we observed that two other PFAS (i.e., PFOSlin and PFNA), distinct from those associated with sperm abnormalities, were positively correlated with the stress hormone corticosterone. These findings emphasize the potentially harmful substance-specific effects of long-chain PFCAs on seabirds and the need for further research into the impact of pollutants on sperm quality as a potential additional detrimental effect on birds.
2024
Hydrofluorocarbons (HFCs) are powerful anthropogenic greenhouse gases (GHGs) with high global-warming potentials (GWPs). They have been widely used as refrigerants, insulation foam-blowing agents, aerosol propellants, and fire suppression agents. Since the mid-1990s, emissions of HFCs have been increasing rapidly as they are used in many applications to replace ozone-depleting chlorofluorocarbons (CFCs) and hydrochlorofluorocarbons (HCFCs) whose consumption and production have been phased out under the Montreal Protocol (MP). Due to the high GWP of HFCs, the Kigali Amendment to the MP requires the phasedown of production and consumption of HFCs to gradually achieve an 80 %–85 % reduction by 2047, starting in 2019 for non-Article 5 (developed) countries with a 10 % reduction against each defined baseline and later schedules for Article 5 (developing) countries. In this study, we have examined long-term high-precision measurements of atmospheric abundances of five major HFCs (HFC-134a, HFC-143a, HFC-32, HFC-125, and HFC-152a) at Gosan station, Jeju Island, South Korea, from 2008 to 2020. Background abundances of HFCs gradually increased, and the inflow of polluted air masses with elevated abundances from surrounding source regions were detected over the entire period. From these pollution events, we inferred regional and country-specific HFC emission estimates using two independent Lagrangian particle dispersion models and Bayesian inversion frameworks (FLEXPART-FLEXINVERT+ and NAME-InTEM). The spatial distribution of the derived “top-down” (measurement based) emissions for all HFCs shows large fluxes from megacities and industrial areas in the region. Our most important finding is that HFC emissions in eastern China and Japan have sharply increased from 2016 to 2018. The contribution of East Asian HFC emissions to the global total increased from 9 % (2008–2014) to 13 % (2016–2020). In particular, HFC emissions in Japan (Annex I country) rose rapidly from 2016 onward, with accumulated total inferred HFC emissions being ∼ 114 Gg yr−1, which is ∼ 76 Gg yr−1 higher for 2016–2020 than the “bottom-up” (i.e., based on activity data and emission factors) emissions of ∼ 38 Gg yr−1 reported to the United Nations Framework Convention on Climate Change (UNFCCC). This is likely related to the increase in domestic demand in Japan for refrigerants and air-conditioning-system-related products and incomplete accounting. A downward trend of HFC emissions that started in 2019 reflects the effectiveness of the F-gas policy in Japan. Eastern China and South Korea, though not obligated to report to the UNFCCC, voluntarily reported emissions, which also show differences between top-down and bottom-up emission estimates, demonstrating the need for atmospheric measurements, comprehensive data analysis, and accurate reporting for precise emission management. Further, the proportional contribution of each country's CO2-equivalent HFC emissions has changed over time, with HFC-134a decreasing and HFC-125 increasing. This demonstrates the transition in the predominant HFC substances contributing to global warming in each country.
2024
Per- and polyfluoroalkyl substances (PFAS) are persistent anthropogenic contaminants, some of which are toxic and bioaccumulative. Perfluoroalkyl carboxylic acids (PFCAs) and perfluoroalkyl sulfonic acids (PFSAs) can form during the atmospheric degradation of precursors such as fluorotelomer alcohols (FTOHs), N-alkylated perfluoroalkane sulfonamides (FASAs), and hydrofluorocarbons (HFCs). Since PFCAs and PFSAs will readily undergo wet deposition, snow and ice cores are useful for studying PFAS in the Arctic atmosphere. In this study, 36 PFAS were detected in surface snow around the Arctic island of Spitsbergen during January–August 2019 (i.e., 24 h darkness to 24 h daylight), indicating widespread and chemically diverse contamination, including at remote high elevation sites. Local sources meant some PFAS had concentrations in snow up to 54 times higher in Longyearbyen, compared to remote locations. At a remote high elevation ice cap, where PFAS input was from long-range atmospheric processes, the median deposition fluxes of C2–C11 PFCAs, PFOS and HFPO–DA (GenX) were 7.6–71 times higher during 24 h daylight. These PFAS all positively correlated with solar flux. Together this suggests seasonal light is important to enable photochemistry for their atmospheric formation and subsequent deposition in the Arctic. This study provides the first evidence for the possible atmospheric formation of PFOS and GenX from precursors.
2024
Understanding thermal comfort expectations in older adults: The role of long-term thermal history
Understanding how long-term thermal history affects thermal comfort expectations in older adults (65+) has implications for designing energy-efficient spaces in a changing climate. A growing number of studies focus on thermal sensation/preference votes to represent the current thermal comfort expectations, often overlooking their limitations. This study, however, investigates how factors shaping long-term thermal history link to the current 65+ adults indoor thermal comfort expectations during exposure to heat, by focusing on the upper limit of thermally acceptable temperature range, represented by a self-reported temperature threshold at which 65+ adults believe to feel uncomfortable by indoor heat (Tit). To find Tit, we use answers to “Above what temperature do you start feeling too hot indoors?” by survey respondents in Warsaw (n = 678) and Madrid (n = 527), who lived in their apartment ≥5 years. Statistically, we find indoor factors affecting long-term thermal experiences more significant in explaining 65+ Tit, when compared to outdoor factors such as distance to water, vegetation, or surface thermal radiance. Better-insulated buildings were associated with a lower Tit [...]
2024
To achieve the objectives of COP28 for transitioning away from fossil fuels and phasing these out, both natural and technological solutions are essential, necessitating a step-change in how we implement social innovation. Given the significant CO2 emissions produced by the building sector, there is an urgent need for a transformative shift towards a net-zero building stock by mid-century. This transition to zero-energy and zero-emission buildings is difficult due to complex processes and substantial costs. Building integrated photovoltaics (BIPV) offers a promising solution due to the benefits of enhanced energy efficiency and electricity production. The availability of roof and façade space in offices and other types of buildings, especially in large cities, permits photovoltaic integration in both opaque and transparent surfaces. This study investigates the synergistic relationship between solar conversion technologies and nature-based components. Through a meta-analysis of peer-reviewed literature and critical assessment, effective BIPVs with greenery (BIPVGREEN) combinations suitable for various climatic zones are identified. The results highlight the multi-faceted benefits of this integration across a range of techno-economic and social criteria and underscore the feasibility of up-scaling these solutions for broader deployment. Applying a SWOT analysis approach, the internal strengths and weaknesses, as well as the external opportunities and threats for BIPVGREEN deployment, are investigated. The analysis reveals key drivers of synergistic effects and multi-benefits, while also addressing the challenges associated with optimizing performance and reducing investment costs. The strengths of BIPVGREEN in terms of energy efficiency and sustainable decarbonization, along with its potential to mitigate urban and climate temperature increases, enhance its relevance to the built environment, especially for informal settlements. The significance of prioritizing this BIPVGREEN climate mitigation action in low-income vulnerable regions and informal settlements is crucial through the minimum tax financing worldwide and citizen's engagement in architectural BIPVGREEN co-integration.
2024