Weingartner, Ernest
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Seasonal and diurnal characteristics of water soluble inorganic compounds in the gas and aerosol phase in the Zurich area
Gas and aerosol samples were taken using a wet effluent diffusion denuder/aerosol collector (WEDD/AC) coupled to ion chromatography (IC) in the city of Zurich, Switzerland from August to September 2002 and in March 2003. Major water soluble inorganic ions; nitrate, sulfate, and nitrite were analyzed online with a time resolution of two hours for the gas and aerosol phase. The fraction of water soluble inorganic anions in PM10 varied from 15% in August to about 38% in March. Seasonal and diurnal variations of nitrate in the gas and aerosol phase were observed with more than 50% of the total nitrate in the gas phase during August and more than 80% of nitrate in the aerosol phase during March exceeding the concentration of sulfate by a factor of 2. Aerosol sulfate, on the other hand, did not show significant variability with season. However, in the gas phase, the SO2 concentration was 6.5 times higher in winter than in summer. Nitrous acid (HONO) also showed a diurnal variation in both the gas and aerosol phase with the lowest concentration (0.2–0.6 µg/m³) in the afternoon. The primary pollutants, NO, CO and SO2 mixing ratios were often at their highest between 04:00–10:00 local time due to the build up of fresh vehicle emission under a nocturnal inversion.
Identification of organic acids in secondary organic aerosol and the corresponding gas phase from chamber experiments
Organic acids in the gas and aerosol phase from photooxidation of 1,3,5-trimethylbenzene in the presence of 300 ppb propene and 300 ppb NOx in smog chamber experiments were determined using a wet effluent diffusion denuder/aerosol collector coupled to ion chromatography (IC) with conductivity detection. Behind the IC, the samples were collected using a fraction collector, for identification of unresolved/unidentified organic acids with IC-mass spectrometry (MS). In total, 20 organic acids were found with MS of which 10 were identified. The organic acids identified offline by IC-MS were then further quantified based on the online IC data. The identification was additionally confirmed with gas chromatography-mass spectrometry. At the maximum aerosol concentration, organic acids comprised 20-45% of the total aerosol mass. The method has a detection limit of 10-100 ng/m3 for the identified carboxylic acids.
Online gas and aerosol measurement of water soluble carboxylic acids in Zurich
We discuss the diurnal and seasonal variability of low molecular weight organic acids in Zurich city on the basis of online quasi‐continuous measurement in the gas and aerosol phase using a wet effluent diffusion denuder/aerosol collector (WEDD/AC) coupled to ion chromatography. The measurements were performed during August–September 2002 and March 2003. Acetic acid exhibited the highest concentration in the gas phase during all the measurement periods, followed by formic acid. Oxalic acid was predominantly found in the aerosol phase and often below the detection limit in the gas phase. In addition, filter samples were analyzed using ion chromatography–mass spectrometry (IC‐MS) to provide more information on organic acids in the aerosol phase. From the offline IC‐MS measurements, 20 monocarboxylic, dicarboxylic, and tricarboxylic acids were determined. In addition, more than 20 different masses were detected with the MS; however, identification of the organic acids was not possible. The sum of the carboxylic acids contributed on average 2% to the water soluble organic carbon (WSOC). The fraction of dicarboxylic acids to the WSOC was higher in summer compared to winter suggesting that dicarboxylic acids are mainly a result of photochemical reactions in summer whereas in winter they mainly result from primary sources.
On the effects of organic matter and sulphur-containing compounds on the CCN activation of combustion particles
The European PartEmis project (Measurement and prediction of emissions of aerosols and gaseous precursors from gas turbine engines) was focussed on the characterisation and quantification of exhaust emissions from a gas turbine engine. The combustion aerosol characterisation included on-line measurements of mass and number concentration, size distribution, mixing state, thermal stability of internally mixed particles, hygroscopicity, cloud condensation nuclei (CCN) activation potential, and off-line analysis of chemical composition. Based on this extensive data set, the role of sulphuric acid coating and of the organic fraction of the combustion particles for the CCN activation was investigated. Modelling of CCN activation was conducted using microphysical and chemical properties obtained from the measurements as input data. Coating the combustion particles with water-soluble sulphuric acid, increases the potential CCN activation, or lowers the activation diameter, respectively. The adaptation of a Köhler model to the experimental data yielded coatings from 0.1 to 3 vol-% of water-soluble matter, which corresponds to an increase in the fraction of CCN-activated combustion particles from ≤10‾⁴ to ≌10‾² at a water vapour saturation ratio Sw=1.006. Additional particle coating by coagulation of combustion particles and aqueous sulphuric acid particles formed by nucleation further reduces the CCN activation diameter. In contrast, particles containing a large fraction of non-volatile organic compounds grow significantly less at high relative humidity than particles with a lower content of non-volatile OC. The resulting reduction in the potential CCN activation with an increasing fraction of non-volatile OC becomes visible as a trend in the experimental data. While a coating of water-soluble sulphuric acid increases the potential CCN activation, or lowers the activation diameter, respectively, the non-volatile organic compounds, mainly found at lower combustion temperatures, can partially compensate this sulphuric acid-related enhancement of CCN activation of carbonaceous combustion aerosol particles.