Sea salt emission, transport and influence on size-segregated nitrate simulation: A case study in northwestern Europe by WRF-Chem

Sea salt aerosol (SSA) is one of the major components of primary aerosols and has significant impact on the formation of secondary inorganic particles mass on a global scale. In this study, the fully online coupled WRF-Chem model was utilized to evaluate the SSA emission scheme and its influence on the nitrate simulation in a case study in Europe during 10–20 September 2013. Meteorological conditions near the surface, wind pattern and thermal stratification structure were well reproduced by the model. Nonetheless, the coarse-mode (PM1 − 10) particle mass concentration was substantially overestimated due to the overestimation of SSA and nitrate. Compared to filter measurements at four EMEP stations (coastal stations: Bilthoven, Kollumerwaard and Vredepeel; inland station: Melpitz), the model overestimated SSA concentrations by a factor of 8–20. We found that this overestimation was mainly caused by overestimated SSA emissions over the North Sea during 16–20 September. Over the coastal regions, SSA was injected into the continental free troposphere through an “aloft bridge” (about 500 to 1000 m above the ground), a result of the different thermodynamic properties and planetary boundary layer (PBL) structure between continental and marine regions. The injected SSA was further transported inland and mixed downward to the surface through downdraft and PBL turbulence. This process extended the influence of SSA to a larger downwind region, leading, for example, to an overestimation of SSA at Melpitz, Germany, by a factor of  ∼  20. As a result, the nitrate partitioning fraction (ratio between particulate nitrate and the summation of particulate nitrate and gas-phase nitric acid) increased by about 20 % for the coarse-mode nitrate due to the overestimation of SSA at Melpitz. However, no significant difference in the partitioning fraction for the fine-mode nitrate was found. About 140 % overestimation of the coarse-mode nitrate resulted from the influence of SSA at Melpitz. In contrast, the overestimation of SSA inhibited the nitrate particle formation in the fine mode by about 20 % because of the increased consumption of precursor by coarse-mode nitrate formation

Atmospheric Methane : Comparison Between Methane's Record in 2006–2022 and During Glacial Terminations

Atmospheric methane's rapid growth from late 2006 is unprecedented in the observational record. Assessment of atmospheric methane data attributes a large fraction of this atmospheric growth to increased natural emissions over the tropics, which appear to be responding to changes in anthropogenic climate forcing. Isotopically lighter measurements of (Figure presented.) are consistent with the recent atmospheric methane growth being mainly driven by an increase in emissions from microbial sources, particularly wetlands. The global methane budget is currently in disequilibrium and new inputs are as yet poorly quantified. Although microbial emissions from agriculture and waste sources have increased between 2006 and 2022 by perhaps 35 Tg/yr, with wide uncertainty, approximately another 35–45 Tg/yr of the recent net growth in methane emissions may have been driven by natural biogenic processes, especially wetland feedbacks to climate change. A model comparison shows that recent changes may be comparable or greater in scale and speed than methane's growth and isotopic shift during past glacial/interglacial termination events. It remains possible that methane's current growth is within the range of Holocene variability, but it is also possible that methane's recent growth and isotopic shift may indicate a large-scale reorganization of the natural climate and biosphere is under way

The consolidated European synthesis of CO2 emissions and removals for the European Union and United Kingdom:1990-2020

Quantification of land surface-atmosphere fluxes of carbon dioxide (CO2) and their trends and uncertainties is essential for monitoring progress of the EU27+UK bloc as it strives to meet ambitious targets determined by both international agreements and internal regulation. This study provides a consolidated synthesis of fossil sources (CO2 fossil) and natural (including formally managed ecosystems) sources and sinks over land (CO2 land) using bottom-up (BU) and top-down (TD) approaches for the European Union and United Kingdom (EU27+UK), updating earlier syntheses (Petrescu et al., 2020, 2021). Given the wide scope of the work and the variety of approaches involved, this study aims to answer essential questions identified in the previous syntheses and understand the differences between datasets, particularly for poorly characterized fluxes from managed and unmanaged ecosystems. The work integrates updated emission inventory data, process-based model results, data-driven categorical model results, and inverse modeling estimates, extending the previous period 1990-2018 to the year 2020 to the extent possible. BU and TD products are compared with the European national greenhouse gas inventory (NGHGI) reported by parties including the year 2019 under the United Nations Framework Convention on Climate Change (UNFCCC). The uncertainties of the EU27+UK NGHGI were evaluated using the standard deviation reported by the EU member states following the guidelines of the Intergovernmental Panel on Climate Change (IPCC) and harmonized by gap-filling procedures. Variation in estimates produced with other methods, such as atmospheric inversion models (TD) or spatially disaggregated inventory datasets (BU), originate from within-model uncertainty related to parameterization as well as structural differences between models. By comparing the NGHGI with other approaches, key sources of differences between estimates arise primarily in activities. System boundaries and emission categories create differences in CO2 fossil datasets, while different land use definitions for reporting emissions from land use, land use change, and forestry (LULUCF) activities result in differences for CO2 land. The latter has important consequences for atmospheric inversions, leading to inversions reporting stronger sinks in vegetation and soils than are reported by the NGHGI. For CO2 fossil emissions, after harmonizing estimates based on common activities and selecting the most recent year available for all datasets, the UNFCCC NGHGI for the EU27+UK accounts for 926g±g13gTggCgyr-1, while eight other BU sources report a mean value of 948 [937,961]gTggCgyr-1 (25th, 75th percentiles). The sole top-down inversion of fossil emissions currently available accounts for 875gTggC in this same year, a value outside the uncertainty of both the NGHGI and bottom-up ensemble estimates and for which uncertainty estimates are not currently available. For the net CO2 land fluxes, during the most recent 5-year period including the NGHGI estimates, the NGHGI accounted for -91g±g32gTggCgyr-1, while six other BU approaches reported a mean sink of -62 [-117,-49]gTggCgyr-1, and a 15-member ensemble of dynamic global vegetation models (DGVMs) reported -69 [-152,-5]gTggCgyr-1. The 5-year mean of three TD regional ensembles combined with one non-ensemble inversion of -73gTggCgyr-1 has a slightly smaller spread (0th-100th percentiles of [-135,+45]gTggCgyr-1), and it was calculated after removing net land-atmosphere CO2 fluxes caused by lateral transport of carbon (crop trade, wood trade, river transport, and net uptake from inland water bodies), resulting in increased agreement with the NGHGI and bottom-up approaches. Results at the category level (Forest Land, Cropland, Grassland) generally show good agreement between the NGHGI and category-specific models, but results for DGVMs are mixed. Overall, for both CO2 fossil and net CO2 land fluxes, we find that current independent approaches are consistent with the NGHGI at the scale of the EU27+UK. We conclude that CO2 emissions from fossil sources have decreased over the past 30 years in the EU27+UK, while land fluxes are relatively stable: positive or negative trends larger (smaller) than 0.07 (-0.61)gTggCgyr-2 can be ruled out for the NGHGI. In addition, a gap on the order of 1000gTggCgyr-1 between CO2 fossil emissions and net CO2 uptake by the land exists regardless of the type of approach (NGHGI, TD, BU), falling well outside all available estimates of uncertainties. However, uncertainties in top-down approaches to estimate CO2 fossil emissions remain uncharacterized and are likely substantial, in addition to known uncertainties in top-down estimates of the land fluxes. The data used to plot the figures are available at 10.5281/zenodo.8148461 (McGrath et al., 2023).</p

Spatial distribution of residential wood combustion emissions in the Nordic countries : How well national inventories represent local emissions?

Highlights • New high-resolution emission inventory for Nordic residential wood combustion. • Country level methods can produce similar spatial distributions as local level. • Difference between urban and rural RWC is important for the spatial distribution. • National characteristics are essential for spatial representation of RWC emissions.Residential wood combustion (RWC) is a major source of air pollutants in the Nordic and many other countries. The emissions of the pollutants have been estimated with inventories on several scopes, e.g. local and national. An important aspect of the inventories is the spatial distribution of the emissions, as it has an effect on health impact assessments. In this study, we present a novel residential wood combustion emission inventory for the Nordic countries based on national inventories and new gridding of the emissions. We compare the emissions of the Nordic inventory, and especially their spatial distribution, to local assessments and European level TNO-newRWC-inventory to assess the spatial proxies used. Common proxies used in the national inventories in the Nordic countries were building data on locations and primary heating methods and questionnaire-based wood use estimates for appliances or primary heating methods. Chimney sweeper register data was identified as good proxy data, but such data may not be available in an applicable format. Comparisons of national inventories to local assessments showed the possibility to achieve similar spatial distributions through nation-wide methods as local ones. However, this won't guarantee that the emissions are similar. Comparison to the TNO-newRWC-inventory revealed the importance of how differences between urban and rural residential wood combustion are handled. The comparison also highlighted the importance of local characteristics of residential wood combustion in the spatial distribution of emissions

Decadal Variabilities in Tropospheric Nitrogen Oxides Over United States, Europe, and China

Global trends in tropospheric nitrogen dioxide (NO2) have changed dramatically in the past decade. Here, we investigate tropospheric NO2 variabilities over United States, Europe, and E. China in 2005–2018 to explore the mechanisms governing the variation of this critical pollutant. We found large uncertainties in the trends of anthropogenic nitrogen oxides (NOx) emissions, for example, the reductions of NOx emissions, derived with different approaches and data sets, are in the range of 35%–50% over the United States and 15%–45% over Europe in 2005–2018. By contrast, the analysis in this work indicates declines of anthropogenic NOx emissions by about 40% and 25% over the United States and Europe, respectively, in 2005–2018, and about 20% over E. China in 2012–2018. However, the shift of major NOx sources from power generation to industrial and transportation sectors has led to noticeable diminishing effects in emission controls. Furthermore, satellite measurements exhibit the influence of NO2 background levels over the United States and Europe, which offset the impacts of anthropogenic emission declines, resulting in flatter trends of tropospheric NO2 over the United States and Europe. Our analysis further reveals underestimation of background NO2 by chemical transport models, which can lead to inaccurate interpretations of satellite measurements. We use surface in-situ NO2 observations to diagnose the satellite-observed NO2 trends and find top-down NOx emissions over urban grids represent the changes in anthropogenic NOx emissions better. This work highlights the importance of comprehensive applications of different analysis approaches to better characterizing atmospheric composition evolution

Intercomparison of Magnitudes and Trends in Anthropogenic Surface Emissions From Bottom-Up Inventories, Top-Down Estimates, and Emission Scenarios

International audienceThis study compares recent CO, NOx, NMVOC, SO2, BC, and OC anthropogenic emissions from several state-of-the-art top-down estimates to global and regional bottom-up inventories and projections from five Shared Socioeconomic Pathways (SSPs) in several regions. Results show that top-down emissions derived in several recent studies exhibit similar uncertainty as bottom-up inventories in some regions for certain species and even less in the case of Chinese CO emissions. In general, the largest discrepancies are found outside of regions such as the United States, Europe, and Japan where the most accurate and detailed information on emissions is available. In some regions such as China, which has recently undergone dynamical economic growth and changes in air quality regulations, the top-down estimates better capture recent emission trends than global bottom-up inventories. These results show the potential of top-down estimates to complement bottom-up inventories and to aide in the development of emission scenarios, particularly in regions where global inventories lack the necessary up-to-date and accurate information regarding regional activity data and emission factors such as Africa and India. Areas of future work aimed at quantifying and reducing uncertainty are also highlighted. A regional comparison of recent CO and NOx trends in the five SSPs indicate that SSP126, a strong pollution control scenario, best represents the trends from the top-down and regional bottom-up inventories in the United States, Europe, and China, while SSP460, a low-pollution control scenario, lies closest to actual trends in West Africa. This analysis can be useful for air quality forecasting and near-future pollution control/mitigation policy studies

The consolidated European synthesis of CO2 emissions and removals for EU27 and UK: 1990-2018

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 modelling estimates, over the period 1990–2018. BU and TD products are compared with European national GHG inventories (NGHGI) reported under the UNFCCC in 2019, aiming to assess and understand the differences between approaches. For the uncertainties in NGHGI, 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), arise from diverse sources including within-model uncertainty related to parameterization as well as structural differences between models. In comparing NGHGI 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 (including cement production) account for 2624 Tg CO2 in 2014 while all the other seven bottom-up sources are consistent with the NGHGI and report a mean of 2588 (± 463 Tg CO2). The inversion reports 2700 Tg CO2 (± 480 Tg CO2), well in line with the national inventories. Over 2011–2015, the CO2 land sources/sinks from NGHGI estimates report −90 Tg C yr−1 ± 30 Tg C while all other BU approaches report a mean sink of −98 Tg yr−1 (± 362 Tg C from DGVMs only). For the TD model ensemble results, we observe a much larger spread for regional inversions (i.e., mean of 253 Tg C yr−1 ± 400 T g C yr−1). This concludes that a) current independent approaches are consistent with NGHGI b) their uncertainty is too large to allow a "verification" because of model differences and probably also because of the definition of "CO2 flux" obtained from different approache

Transboundary particulate matter, photo-oxidants, acidifying and eutrophying components

This report presents the EMEP activities in 2018 and 2019 in relation to transboundary fluxes of particulate matter, photo-oxidants, acidifying and eutrophying components, with focus on results for 2017. It presents major results of the activities related to emission inventories, observations and modelling. The report also introduces specific relevant research activities addressing EMEP key challenges, as well as technical developments of the observation and modelling capacities