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AbstractAir pollution from fine particulate matter (PM2.5) has been associated with various health implications that can lead to increased morbidity and excess mortality. Epidemiological and toxicological studies have shown that carbonaceous particles (black carbon and organic aerosols) may be more hazardous to human health than inorganic ones. Health impact studies and emission reduction policies are based on total PM2.5 concentration without differentiating the more harmful components. In such assessments, PM2.5 and their sub-component concentrations are usually modeled with air quality models. Organic aerosols have been shown to be consistently underestimated, which may affect excess mortality estimates. Here, we use the WRF-Chem model to simulate PM2.5 (including carbonaceous particles) over the wider European domain and assess some of the main factors that contribute to uncertainty. In particular, we explore the impact of anthropogenic emissions and meteorological modeling on carbonaceous aerosol concentrations. We further assess their effects on excess mortality estimates by using the Global Exposure Mortality Model (GEMM). We find that meteorological grid nudging is essential for accurately representing both PM2.5 and carbonaceous aerosols and that, for this application, results improve more significantly compared to spectral nudging. Our results indicate that the explicit account of organic precursors (semi-volatile and intermediate-volatile organic carbons—SVOCs/IVOCs) in emission inventories would improve the accuracy of organic aerosols modeling. We conclude that uncertainties related to PM2.5 modeling in Europe lead to a ∼15% deviation in excess mortality, which is comparable to the risk model uncertainty. This estimate is relevant when all PM2.5 sub-components are assumed to be equally toxic but can be higher by considering their specific toxicity.

The changing composition of the atmosphere, driven by anthropogenic emissions, is the cause of anthropogenic climate change as well as deteriorating air quality. Emission inventories are essential to understand the contribution of various human activities, model and predict the changing atmospheric composition, and design cost-effective mitigation measures. At present, national emission inventories in South America (SA) focus on Greenhouse Gases (GHG) as part of their obligation to the United Nations Framework Convention for Climate Change (UNFCC) within the framework of their national communications. Emission inventories other than GHG in SA focus mainly on growing urban areas and megacities. Therefore, studies examining air quality at national, regional or continental scales in SA depend on (down-scaled) global emission inventories. This paper examines the emission estimates of air pollutants from various global inventories for five SA countries, namely Argentina, Brazil, Chile, Colombia and Peru. A more detailed analysis is conducted for the EDGAR and ECLIPSE emission inventories, in particular comparing local city-scale inventories of a major city in each country. Although total emissions between down-scaled global inventories and local city inventories are often comparable, large discrepancies exist between the sectoral contributions. This is critical, as the mitigation of poor air quality will depend on addressing the right sources. Potential sources of discrepancies between global and local inventories include the spatial distribution proxies, difference in emission factors used and/or the use of generic statistical country data when estimating emissions. This highlights the importance of using local information when generating national emission inventories, especially for air quality modeling and development of effective mitigation measures. This study represents the first step towards an increased understanding of the strengths and weaknesses of emissions information in SA. ; FONDECYT Project of International Networking 150043 Comisión Nacional de Investigación Cientifica y Tecnológica (CONICYT) CONICYT FONDECYT 1150873 1181139 Center for Climate Research and Resilience (CR2) ANID/FONDAP 15110009 European Union (EU) GA 777544 870301 project ANID-PIA-Anillo INACH ACT192057 MAP-AQ ANID/FONDAP 15110009 Fondo para la Investigación Cientifica y Tecnológica PICT 2016-3590 Universidad Nacional Tecnológica de Lima Sur-UNTELS 032-2019-UNTELS project METROCLIMA FAPESP 2016/18438-0 ANPCyT PICT-O 2016-4802

Reliable quantification of the sources and sinks of atmospheric carbon dioxide (CO2), including that of their trends and uncertainties, is essential to monitoring the progress in mitigating anthropogenic emissions under the Kyoto Protocol and the Paris Agreement. This study provides a consolidated synthesis of estimates for all anthropogenic and natural sources and sinks of CO2 for the European Union and UK (EU27 + UK), derived from a combination of state-of-the-art bottom-up (BU) and top-down (TD) data sources and models. Given the wide scope of the work and the variety of datasets involved, this study focuses on identifying essential questions which need to be answered to properly understand the differences between various datasets, in particular with regards to the less-well-characterized fluxes from managed ecosystems. The work integrates recent emission inventory data, process-based ecosystem model results, data-driven sector model results and inverse modeling estimates over the period 1990-2018. BU and TD products are compared with European national greenhouse gas inventories (NGHGIs) reported under the UNFCCC in 2019, aiming to assess and understand the differences between approaches. For the uncertainties in NGHGIs, we used the standard deviation obtained by varying parameters of inventory calculations, reported by the member states following the IPCC Guidelines. Variation in estimates produced with other methods, like atmospheric inversion models (TD) or spatially disaggregated inventory datasets (BU), arises from diverse sources including within-model uncertainty related to parameterization as well as structural differences between models. In comparing NGHGIs with other approaches, a key source of uncertainty is that related to different system boundaries and emission categories (CO2 fossil) and the use of different land use definitions for reporting emissions from land use, land use change and forestry (LULUCF) activities (CO2 land). At the EU27 + UK level, the NGHGI (2019) fossil CO2 emissions ...