气候变化领域集成服务门户(CCPortal): Composition and origin of PM2.5 aerosol particles in the upper Rhine valley in summer

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DOI	10.5194/acp-19-13189-2019
	Composition and origin of PM2.5 aerosol particles in the upper Rhine valley in summer
	Shen X.; Vogel H.; Vogel B.; Huang W.; Mohr C.; Ramisetty R.; Leisner T.; Prévôt A.S.H.; Saathoff H.
发表日期	2019
ISSN	16807316
起始页码	13189
结束页码	13208
卷号	19 期号:20
英文摘要	We conducted a 6-week measurement campaign in summer 2016 at a rural site about 11 km north of the city of Karlsruhe in southwest Germany in order to study the chemical composition and origin of aerosols in the upper Rhine valley. In particular, we deployed a single-particle mass spectrometer (LAAPTOF) and an aerosol mass spectrometer (AMS) to provide complementary chemical information on aerosol particles smaller than 2.5 μm. For the entire measurement period, the total aerosol particle mass was dominated by sodium salts, contributing on average (36±27)% to the total single particles measured by the LAAPTOF. The total particulate organic compounds, sulfate, nitrate, and ammonium contributed on average (58±12) %, (22±7) %, (10±1) %, and (9±3)% to the total non-refractory particle mass measured by the AMS. Positive matrix factorization (PMF) analysis for the AMS data suggests that the total organic aerosol (OA) consisted of five components, including (9±7)% hydrocarbon-like OA (HOA), (16±11)% semivolatile oxygenated OA (SV-OOA), and (75±15)% lowvolatility oxygenated OA (LV-OOA). The regional transport model COSMO-ART was applied for source apportionment and to achieve a better understanding of the impact of complex transport patterns on the field observations. Combining field observations and model simulations, we attributed high particle numbers and SO2 concentrations observed at this rural site to industrial emissions from power plants and a refinery in Karlsruhe. In addition, two characteristic episodes with aerosol particle mass dominated by sodium salts particles comprising (70±24)% of the total single particles and organic compounds accounting for (77±6)% of total non-refractory species, respectively, were investigated in detail. For the first episode, we identified relatively fresh and aged sea salt particles originating from the Atlantic Ocean more than 800 km away. These particles showed markers like m=z 129 C5H7NO+3 , indicating the influence of anthropogenic emissions modifying their composition, e.g. from chloride to nitrate salts during the long-range transport. For a 3 d episode including high organic mass concentrations, model simulations show that on average (74±7)% of the particulate organics at this site were of biogenic origin. Detailed model analysis allowed us to find out that three subsequent peaks of high organic mass concentrations originated from different sources, including local emissions from the city and industrial area of Karlsruhe, regional transport from the city of Stuttgart (∼ 64 km away), and potential local night-time formation and growth. Biogenic (forest) and anthropogenic (urban) emissions were mixed during transport and contributed to the formation of organic particles. In addition, topography, temperature inversion, and stagnant meteorological conditions also played a role in the build-up of higher organic particle mass concentrations. Furthermore, the model was evaluated using field observations and corresponding sensitivity tests. The model results show good agreement with trends and concentrations observed for several trace gases (e.g. O3, NO2, and SO2) and aerosol particle compounds (e.g. ammonium and nitrate). However, the model underestimates the number of particles by an order of magnitude and underestimates the mass of organic particles by a factor of 2.3. The discrepancy was expected for particle number since the model does not include all nucleation processes. The missing organic mass indicates either an underestimated regional background or missing sources and/or mechanisms in the model, like night-time chemistry. This study demonstrates the potential of combining comprehensive field observations with dedicated transport modelling to understand the chemical composition and complex origin of aerosols. © Author(s) 2019.
语种	英语
scopus关键词	aerosol composition; ammonium; atmospheric transport; mass spectrometry; nitrate; particulate organic matter; rural atmosphere; sulfate; summer; Baden-Wurttemberg; Germany; Karlsruhe; Rhine Valley; Upper Rhine Valley
来源期刊	Atmospheric Chemistry and Physics
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/144072
作者单位	Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, Hermann-von-Helmholtz-Platz 1, Eggenstein-Leopoldshafen, 76344, Germany; Institute of Geography and Geoecology, Working Group for Environmental Mineralogy and Environmental System Analysis, Karlsruhe Institute of Technology, Kaiserstr. 12, Karlsruhe, 76131, Germany; Department of Environmental Science and Analytical Chemistry, Stockholm University, Stockholm, 11418, Sweden; Institute of Environmental Physics, University Heidelberg, In Neuenheimer Feld 229, Heidelberg, 69120, Germany; Laboratory of Atmospheric Chemistry, Paul Scherrer Institute (PSI), Villigen PSI, 5232, Switzerland; TSI Instruments India Private Limited, Bangalore, 560102, India
推荐引用方式 GB/T 7714	Shen X.,Vogel H.,Vogel B.,et al. Composition and origin of PM2.5 aerosol particles in the upper Rhine valley in summer[J],2019,19(20).
APA	Shen X..,Vogel H..,Vogel B..,Huang W..,Mohr C..,...&Saathoff H..(2019).Composition and origin of PM2.5 aerosol particles in the upper Rhine valley in summer.Atmospheric Chemistry and Physics,19(20).
MLA	Shen X.,et al."Composition and origin of PM2.5 aerosol particles in the upper Rhine valley in summer".Atmospheric Chemistry and Physics 19.20(2019).