Composition and origin of PM2.5 aerosol particles in the upper Rhine valley in summer

• Verfasst von: Shen, Xiaoli [VerfasserIn]
• Verfasst von: Vogel, Heike [VerfasserIn]
• Verfasst von: Leisner, Thomas [VerfasserIn]
• Titel: Composition and origin of PM2.5 aerosol particles in the upper Rhine valley in summer
• Verf.angabe: Xiaoli Shen, Heike Vogel, Bernhard Vogel, Wei Huang, Claudia Mohr, Ramakrishna Ramisetty, Thomas Leisner, André S. H. Prévôt, Harald Saathoff
• E-Jahr: 2019
• Jahr: 25 October 2019
• Umfang: 20 S.
• Fussnoten: Im Titel ist "2.5." tiefer gestellt ; Gesehen am 11.12.2019
• Titel Quelle: Enthalten in: Atmospheric chemistry and physics
• Ort Quelle: Katlenburg-Lindau : EGU, 2001
• Jahr Quelle: 2019
• Band/Heft Quelle: 19(2019), 20, Seite 13189-13208
• ISSN Quelle: 1680-7324
• DOI: doi:10.5194/acp-19-13189-2019
• Datenträger: Online-Ressource
• Sprache: eng
• K10plus-PPN: 168511766X

Abstract

<p><strong>Abstract.</strong> We conducted a 6-week measurement campaign in summer 2016 at a rural site about 11&thinsp;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&thinsp;<span class="inline-formula">µ</span>m. For the entire measurement period, the total aerosol particle mass was dominated by sodium salts, contributing on average (<span class="inline-formula">36±27</span>)&thinsp;% to the total single particles measured by the LAAPTOF. The total particulate organic compounds, sulfate, nitrate, and ammonium contributed on average (<span class="inline-formula">58±12</span>)&thinsp;%, (<span class="inline-formula">22±7</span>)&thinsp;%, (<span class="inline-formula">10±1</span>)&thinsp;%, and (<span class="inline-formula">9±3</span>)&thinsp;% 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 (<span class="inline-formula">9±7</span>)&thinsp;% hydrocarbon-like OA (HOA), (<span class="inline-formula">16±11</span>)&thinsp;% semi-volatile oxygenated OA (SV-OOA), and (<span class="inline-formula">75±15</span>)&thinsp;% low-volatility 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 <span class="inline-formula">SO₂</span> 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 (<span class="inline-formula">70±24</span>)&thinsp;% of the total single particles and organic compounds accounting for (<span class="inline-formula">77±6</span>)&thinsp;% 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&thinsp;km away. These particles showed markers like <span class="inline-formula"><i>m</i>∕<i>z</i></span> 129 <span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M16" display="inline" overflow="scroll" dspmath="mathml"><mrow class="chem"><msub><mi mathvariant="normal">C</mi><mn mathvariant="normal">5</mn></msub><msub><mi mathvariant="normal">H</mi><mn mathvariant="normal">7</mn></msub><msubsup><mi mathvariant="normal">NO</mi><mn mathvariant="normal">3</mn><mo>+</mo></msubsup></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="50pt" height="15pt" class="svg-formula" dspmath="mathimg" md5hash="d4ff83f068ed31521ae4740043c64a93"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-19-13189-2019-ie00001.svg" width="50pt" height="15pt" src="acp-19-13189-2019-ie00001.png"/></svg:svg></span></span>, indicating the influence of anthropogenic emissions modifying their composition, e.g. from chloride to nitrate salts during the long-range transport. For a 3&thinsp;d episode including high organic mass concentrations, model simulations show that on average (<span class="inline-formula">74±7</span>)&thinsp;% 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 (<span class="inline-formula">∼64</span>&thinsp;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<span id="page13190"/> 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. <span class="inline-formula">O₃</span>, <span class="inline-formula">NO₂</span>, and <span class="inline-formula">SO₂</span>) 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.</p>