| Abstrakt: |
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. [ABSTRACT FROM AUTHOR] |
