Evaluation of modelled versus observed NMVOC compounds at EMEP sites in Europe

•Atmospheric volatile organic compounds (VOC) constitute a wide range of species, acting as precursors to ozone and aerosol formation. Atmospheric chemistry and transport models (CTMs) are crucial to understanding the emissions, distribution, and impacts of VOCs. Given the uncertainties in VOC emissions, lack of evaluation studies, and recent changes in emissions, this work adapts the European Monitoring and Evaluation Programme Meteorological Synthesizing Centre – West (EMEP MSC-W) CTM to evaluate emission inventories in Europe. Here we undertake the first intensive model-measurement comparison of VOCs in two decades. The modelled surface concentrations are evaluated both spatially and temporally, using measurements from the regular EMEP monitoring network in 2018 and 2019, and a 2022 campaign. To achieve this, we utilised the UK National Atmospheric Emission Inventory to derive explicit emission profiles for individual species and employed a `tracer' method to produce pure concentrations that are directly comparable to observations. Model simulations for 2018 compare the use of two European inventories, CAMS and CEIP, and of two chemical mechanisms, CRIv2R5Em and EmChem19rc; those for 2019 and 2022 use CAMS and CRIv2R5Em only. •The degree to which the modelled and measured VOCs agree varies depending on the specific species. The model successfully captures the overall spatial and temporal variations of major alkanes (e.g., ethane, n-butane) and unsaturated species (e.g., ethene, benzene), but less though for propane, i-butane, and ethyne. This discrepancy underscores potential issues in the boundary conditions for these latter species and in their primary emissions from in particular the solvent and road transport sectors. Specifically, potential missing propane emissions and issues with its boundary conditions are highlighted by large model underestimations and smaller propane to ethane ratios compared to the measurement. Meanwhile, both the model and measurement show strong linear correlations among butane isomers and among pentane isomers, indicating common sources for these pairs of isomers. However, modelled ratios of i- to n-butane and i- to n-pentane are approximately one-third of the measured ratios, which is largely driven by significant emissions of n-butane and n-pentane from the solvent sector. This suggests issues with the speciation profile of the solvent sector, or underrepresented contributions from transport and fuel evaporation sectors in current inventories, or both. Furthermore, the modelled ethene-to-ethyne and benzene-to-ethyne ratios differ significantly from measured ratios. The different model performance strongly points to shortcomings in the spatial and temporal patterns and magnitudes of ethyne emissions, especially during winter. For OVOCs, modelled and measured methanal and methylglyoxal display a good agreement, which demonstrates that the model captures the overall photo-oxidation processes reasonably well. However, the insufficiency of suitable measurements limits the evaluation of other OVOCs. Finally, the model exhibits very similar performance across simulations using different inventories, which suggests that the emission profiles are likely to exert a more significant impact on the agreement between modelled and measured data than the total emissions reported for each sector. Therefore, the future focus may need to shift towards refining these speciation profiles through for example new emission measurement campaigns to improve the model accuracy

Variability of ambient air ammonia in urban Europe (Finland, France, Italy, Spain, and the UK)

This study addressed the scarcity of NH3 measurements in urban Europe and the diverse monitoring protocols, hindering direct data comparison. Sixty-nine datasets from Finland, France, Italy, Spain, and the UK across various site types, including industrial (IND, 8), traffic (TR, 12), urban (UB, 22), suburban (SUB, 12), and regional background (RB, 15), are analyzed to this study. Among these, 26 sites provided 5, or more, years of data for time series analysis. Despite varied protocols, necessitating future harmonization, the average NH3 concentration across sites reached 8.0 ± 8.9 μg/m3. Excluding farming/agricultural hotspots (FAHs), IND and TR sites had the highest concentrations (4.7 ± 3.2 and 4.5 ± 1.0 μg/m3), followed by UB, SUB, and RB sites (3.3 ± 1.5, 2.7 ± 1.3, and 1.0 ± 0.3 μg/m3, respectively) indicating that industrial, traffic, and other urban sources were primary contributors to NH3 outside FAH regions. When referring exclusively to the FAHs, concentrations ranged from 10.0 ± 2.3 to 15.6 ± 17.2 μg/m3, with the highest concentrations being reached in RB sites close to the farming and agricultural sources, and that, on average for FAHs there is a decreasing NH3 concentration gradient towards the city. Time trends showed that over half of the sites (18/26) observed statistically significant trends. Approximately 50 % of UB and TR sites showed a decreasing trend, while 30 % an increasing one. Meta-analysis revealed a small insignificant decreasing trend for non-FAH RB sites. In FAHs, there was a significant upward trend at a rate of 3.51[0.45,6.57]%/yr. Seasonal patterns of NH3 concentrations varied, with urban areas experiencing fluctuations influenced by surrounding emissions, particularly in FAHs. Diel variation showed differing patterns at urban monitoring sites, all with higher daytime concentrations, but with variations in peak times depending on major emission sources and meteorological patterns. These results offer valuable insights into the spatio-temporal patterns of gas-phase NH3 concentrations in urban Europe, contributing to future efforts in benchmarking NH3 pollution control in urban areas.</p

Light oxygenated volatile organic compound concentrations in an Eastern Mediterranean urban atmosphere rivalling those in megacities

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Speciation of non-methane hydrocarbons (NMHCs) from anthropogenic sources in Beirut, Lebanon

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Source apportionment vs. emission inventories of non-methane hydrocarbons (NMHC) in an urban area of the Middle East: local and global perspectives

International audienceWe applied the positive matrix factorization model to two large data sets collected during two intensive measurement campaigns (summer 2011 and winter 2012) at a suburban site in Beirut, Lebanon, in order to identify NMHC (non-methane hydrocarbons) sources and quantify their contribution to ambient levels. Six factors were identified in winter and five factors in summer. PMF-resolved source profiles were consistent with source profiles established by near-field measurements. The major sources were traffic-related emissions (combustion and gasoline evaporation) in winter and in summer accounting for 51 and 74 wt %, respectively, in agreement with the national emission inventory. The gasoline evaporation related to traffic source had a significant contribution regardless of the season (22 wt % in winter and 30 wt % in summer). The NMHC emissions from road transport are estimated from observations and PMF results, and compared to local and global emission inventories. The PMF analysis finds reasonable differences on emission rates, of 20-39 % higher than the national road transport inventory. However, global inventories (ACCMIP, EDGAR, MACC-ity) underestimate the emissions up to a factor of 10 for the transportation sector. When combining emission inventory to our results, there is strong evidence that control measures in Lebanon should be targeted on mitigating the NMHC emissions from the traffic-related sources. From a global perspective , an assessment of VOC (volatile organic compounds) an-thropogenic emission inventories for the Middle East region as a whole seems necessary as these emissions could be much higher than expected at least from the road transport sector

Seasonal variation and origins of volatile organic compounds observed during 2 years at a western Mediterranean remote background site (Ersa, Cape Corsica)

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Exploring the seasonal NMHC distribution in an urban area of the Middle East during ECOCEM campaigns: very high loadings dominated by local emissions and dynamics

Non-methane hydrocarbons play an important role in the formation of photochemical oxidants such as ozone. We investigate factors controlling the distribution of non-methane hydrocarbons in an urban area of the Middle East. The study highlights the importance of local emissions and atmospheric dynamics, and the limited effect of photochemistry at the measurement site. Abstract Measurements of over 70 C2-C16 non-methane hydrocarbons (NMHCs) were conducted in suburban Beirut (1.3 million inhabitants) in summer 2011 and winter 2012 during the Emission and Chemistry of Organic Carbon in the East Mediterranean (ECOCEM) field campaign. The levels of NMHCs observed exceeded by a factor of two in total volume the levels found in northern mid-latitude megacities (Paris and Los Angeles), especially for the unburned fossil fuel fraction. Regardless of the season, the major compounds, explaining 50% of the concentrations, were toluene, isopentane, butane, m,p-xylenes, propane and ethylene, emitted by mobile traffic and gasoline evaporation sources. Most NMHCs show a distinct seasonal cycle, with a summer maximum and a winter minimum, unlike seasonal cycles usually observed in the northern mid-latitude urban areas. We show that NMHC distribution is mainly driven by strong local emissions and local atmospheric dynamics, with no clear evidence of photochemical removal in summer or influence from long-range transport

Is Traffic Still an Important Emitter of Monoaromatic Organic Compounds in European Urban Areas?

International audienceTrends of long-term observations and emission inventories suggest that traffic emissions will no longer dominate the concentrations of monoaromatic compounds (i.e., TEX - toluene, xylenes, and ethylbenzene) in European urban areas. But the split limit between traffic and other emission sector contributions such as solvent use remains tenuous. Here long-term observations of an extensive set of hydrocarbons, including TEX, at traffic and urban background sites in London, Paris and Strasbourg were combined to estimate the relative importance of traffic emissions on TEX in every city. When analyzing the urban enhancement emission ratios of TEX-to-benzene on a seasonal basis, two potential source signatures other than traffic could be differentiated in all cities (1) summertime evaporation from fuel and/or solvent and (2) wintertime domestic heating. However, traffic emissions still unambiguously dominate the concentration levels of TEX in every city despite the reduction of their emissions at exhaust pipe over the last two decades. Traffic explains between 60% and 96% (at ±20%) of TEX levels while it is less clear for xylenes at some locations. Our results provide a basis to evaluate regional emission inventories. The method is applicable at any urban area where speciated hydrocarbon monitoring is available