Auflistung nach Autor:in "Huthwelker, Thomas"

Gerade angezeigt 1 - 2 von 2

Aging induced changes on NEXAFS fingerprints in individual combustion particles
(Copernicus, 24.11.2011) Zelenay, Veronika; Mooser, René; Tritscher, Torsten; Křepelová, Adela; Heringa, Maarten F.; Chirico, Roberto; Prévôt, André SH.; Weingartner, Ernest; Baltensperger, Urs; Dommen, Josef; Watts, B.; Raabe, Jörg; Huthwelker, Thomas; Ammann, Markus
Abstract. Soot particles can significantly influence the Earth's climate by absorbing and scattering solar radiation as well as by acting as cloud condensation nuclei. However, despite their environmental (as well as economic and political) importance, the way these properties are affected by atmospheric processing of the combustion exhaust gases is still a subject of discussion. In this work, individual soot particles emitted from two different vehicles, a EURO 2 transporter, a EURO 3 passenger car, and a wood stove were investigated on a single-particle basis. The emitted exhaust, including the particulate and the gas phase, was processed in a smog chamber with artificial solar radiation. Single particle specimens of both unprocessed and aged soot were characterized using near edge X-ray absorption fine structure spectroscopy (NEXAFS) and scanning electron microscopy. Comparison of NEXAFS spectra from the unprocessed particles and those resulting from exhaust photooxidation in the chamber revealed changes in the carbon functional group content. For the wood stove emissions, these changes were minor, related to the relatively mild oxidation conditions. For the EURO 2 transporter emissions, the most apparent change was that of carboxylic carbon from oxidized organic compounds condensing on the primary soot particles. For the EURO 3 car emissions oxidation of primary soot particles upon photochemical aging has likely contributed as well. Overall, the changes in the NEXAFS fingerprints were in qualitative agreement with data from an aerosol mass spectrometer. Furthermore, by taking full advantage of our in situ microreactor concept, we show that the soot particles from all three combustion sources changed their ability to take up water under humid conditions upon photochemical aging of the exhaust. Due to the selectivity and sensitivity of the NEXAFS technique for the water mass, also small amounts of water taken up into the internal voids of agglomerated particles could be detected. Because such small amounts of water uptake do not lead to measurable changes in particle diameter, it may remain beyond the limits of volume growth measurements, especially for larger agglomerated particles.
01A - Beitrag in wissenschaftlicher Zeitschrift
Deposition uniformity and particle size distribution of ambient aerosol collected with a rotating drum impactor
(Taylor & Francis, 30.06.2009) Bukowiecki, Nicolas; Richard, Agnes; Furger, Markus; Weingartner, Ernest; Aguirre, Myriam; Huthwelker, Thomas; Lienemann, Peter; Gehrig, Robert; Baltensperger, Urs
Rotating drum impactors (RDI) are cascade type impactors used for size and time resolved aerosol sampling, mostly followed by spectrometric analysis of the deposited material. They are characterized by one rectangular nozzle per stage and are equipped with an automated stepping mechanism for the impaction wheels. An existing three-stage rotating drum impactor was modified, to obtain new midpoint cutoff diameters at 2.5 μm, 1 μm, and 0.1 μm, respectively. For RDI samples collected under ambient air conditions, information on the size-segregation and the spatial uniformity of the deposited particles are key factors for a reliable spectrometric analysis of the RDI deposits. Two aerodynamic particle sizers (APS) were used for the determination of the RDI size fractionation characteristics, using polydisperse laboratory room air as quasi-stable proxy for urban ambient air. This experimental approach was suitable for the scope of this study, but was subject to numerous boundary conditions that limit a general use. Aerodynamic stage penetration midpoint diameters were estimated to be 2.4 and 1.0 μm for the first two RDI stages. Additionally, the spatial uniformity and geometrical size distribution of the deposited aerosol were investigated using micro-focus synchrotron radiation X-ray fluorescence spectrometry (micro-SR-XRF) and transmission electron microscopy (TEM), respectively. The size distribution of the particles found on the TEM samples agreed well with the results from the APS experiments. The RDI deposits showed sufficient uniformity for subsequent spectrometric analysis, but in the 2.5–10 μm size range the particle area density was very low. All of the applied methods confirmed the theoretical cutoff values of the modified RDI and showed that compared to other cascade impactors, the determined stage penetration sharpness was rather broad for the individual impactor stages.
01A - Beitrag in wissenschaftlicher Zeitschrift