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DOI | 10.5194/acp-19-15247-2019 |
Sources of organic aerosols in Europe: A modeling study using CAMx with modified volatility basis set scheme | |
Jiang J.; Aksoyoglu S.; El-Haddad I.; Ciarelli G.; Denier Van Der Gon H.A.C.; Canonaco F.; Gilardoni S.; Paglione M.; Minguillón M.C.; Favez O.; Zhang Y.; Marchand N.; Hao L.; Virtanen A.; Florou K.; O'Dowd C.; Ovadnevaite J.; Baltensperger U.; Prévôt A.S.H. | |
发表日期 | 2019 |
ISSN | 16807316 |
起始页码 | 15247 |
结束页码 | 15270 |
卷号 | 19期号:24 |
英文摘要 | Source apportionment of organic aerosols (OAs) is of great importance to better understand the health impact and climate effects of particulate matter air pollution. Air quality models are used as potential tools to identify OA components and sources at high spatial and temporal resolution; however, they generally underestimate OA concentrations, and comparisons of their outputs with an extended set of measurements are still rare due to the lack of long-term experimental data. In this study, we addressed such challenges at the European level. Using the regional Comprehensive Air Quality Model with Extensions (CAMx) and a volatility basis set (VBS) scheme which was optimized based on recent chamber experiments with wood burning and diesel vehicle emissions, and which contains more source-specific sets compared to previous studies, we calculated the contribution of OA components and defined their sources over a wholeyear period (2011). We modeled separately the primary and secondary OA contributions from old and new diesel and gasoline vehicles, biomass burning (mostly residential wood burning and agricultural waste burning excluding wildfires), other anthropogenic sources (mainly shipping, industry and energy production) and biogenic sources. An important feature of this study is that we evaluated the model results with measurements over a longer period than in previous studies, which strengthens our confidence in our modeled source apportionment results. Comparison against positive matrix factorization (PMF) analyses of aerosol mass spectrometric measurements at nine European sites suggested that the modified VBS scheme improved the model performance for total OA as well as the OA components, including hydrocarbonlike (HOA), biomass burning (BBOA) and oxygenated components (OOA). By using the modified VBS scheme, the mean bias of OOA was reduced from-1:3 to-0:4 μgm-3 corresponding to a reduction of mean fractional bias from-45% to-20 %. The winter OOA simulation, which was largely underestimated in previous studies, was improved by 29% to 42% among the evaluated sites compared to the default parameterization. Wood burning was the dominant OA source in winter (61 %), while biogenic emissions contributed ∼55% to OA during summer in Europe on average. In both seasons, other anthropogenic sources comprised the second largest component (9% in winter and 19% in summer as domain average), while the average contributions of diesel and gasoline vehicles were rather small (∼5 %) except for the metropolitan areas where the highest contribution reached 31 %. The results indicate the need to improve the emission inventory to include currently missing and highly uncertain local emissions, as well as further improvement of VBS parameterization for winter biomass burning. Although this study focused on Europe, it can be applied in any other part of the globe. This study highlights the ability of long-term measurements and source apportionment modeling to validate and improve emission inventories, and identify sources not yet properly included in existing inventories. © Author(s) 2019. |
语种 | 英语 |
scopus关键词 | aerosol; air quality; atmospheric modeling; biomass burning; concentration (composition); emission inventory; organic matter; source apportionment; traffic emission; Europe |
来源期刊 | Atmospheric Chemistry and Physics
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文献类型 | 期刊论文 |
条目标识符 | http://gcip.llas.ac.cn/handle/2XKMVOVA/143967 |
作者单位 | Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen PSI, 5232, Switzerland; Department of Chemical Engineering, Carnegie Mellon University, Pittsburgh, United States; TNO, Department of Climate, Air and Sustainability, Utrecht, Netherlands; Italian National Research Council, Institute of Atmospheric Sciences and Climate, Bologna, Italy; Institute of Environmental Assessment and Water Research (IDAEA), CSIC, Barcelona, 08034, Spain; Institut National de l'Environnement Industriel et des Risques (INERIS), Verneuil-en-Halatte, France; Laboratoire des Sciences du Climat et de l'Environnement (LSCE), Gif-sur-Yvette, France; Aix-Marseille Univ, CNRS, LCE, Marseille, France; Department of Applied Physics, University of Eastern Finland, P.O. Box 1627, Kuopio, 70211, Finland; Department of Chemical Engineering, University of Patras, Patras, 26500, Greece; School of Physics, Ryan Institute's Centre for Climate and Air Pollution Studies, and Marine Renewable Energy Ireland, National University of ... |
推荐引用方式 GB/T 7714 | Jiang J.,Aksoyoglu S.,El-Haddad I.,et al. Sources of organic aerosols in Europe: A modeling study using CAMx with modified volatility basis set scheme[J],2019,19(24). |
APA | Jiang J..,Aksoyoglu S..,El-Haddad I..,Ciarelli G..,Denier Van Der Gon H.A.C..,...&Prévôt A.S.H..(2019).Sources of organic aerosols in Europe: A modeling study using CAMx with modified volatility basis set scheme.Atmospheric Chemistry and Physics,19(24). |
MLA | Jiang J.,et al."Sources of organic aerosols in Europe: A modeling study using CAMx with modified volatility basis set scheme".Atmospheric Chemistry and Physics 19.24(2019). |
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