Aging induced changes on NEXAFS fingerprints in individual combustion particles

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Autor:innen
Zelenay, Veronika
Mooser, René
Tritscher, Torsten
Křepelová, Adela
Heringa, Maarten F.
Chirico, Roberto
Prévôt, André SH.
Baltensperger, Urs
Dommen, Josef
Autor:in (Körperschaft)
Publikationsdatum
24.11.2011
Typ der Arbeit
Studiengang
Typ
01A - Beitrag in wissenschaftlicher Zeitschrift
Herausgeber:innen
Herausgeber:in (Körperschaft)
Betreuer:in
Übergeordnetes Werk
Atmospheric Chemistry and Physics
Themenheft
Link
Reihe / Serie
Reihennummer
Jahrgang / Band
11
Ausgabe / Nummer
22
Seiten / Dauer
11777–11791
Patentnummer
Verlag / Herausgebende Institution
Copernicus
Verlagsort / Veranstaltungsort
Auflage
Version
Programmiersprache
Abtretungsempfänger:in
Praxispartner:in/Auftraggeber:in
Zusammenfassung
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.
Schlagwörter
Fachgebiet (DDC)
550 - Geowissenschaften
Projekt
Veranstaltung
Startdatum der Ausstellung
Enddatum der Ausstellung
Startdatum der Konferenz
Enddatum der Konferenz
Datum der letzten Prüfung
ISBN
ISSN
1680-7324
1680-7316
Sprache
Englisch
Während FHNW Zugehörigkeit erstellt
Nein
Zukunftsfelder FHNW
Publikationsstatus
Veröffentlicht
Begutachtung
Peer-Review der ganzen Publikation
Open Access-Status
Gold
Lizenz
'https://creativecommons.org/licenses/by/4.0/'
Zitation
ZELENAY, Veronika, René MOOSER, Torsten TRITSCHER, Adela KŘEPELOVÁ, Maarten F. HERINGA, Roberto CHIRICO, André SH. PRÉVÔT, Ernest WEINGARTNER, Urs BALTENSPERGER, Josef DOMMEN, B. WATTS, Jörg RAABE, Thomas HUTHWELKER und Markus AMMANN, 2011. Aging induced changes on NEXAFS fingerprints in individual combustion particles. Atmospheric Chemistry and Physics. 24 November 2011. Bd. 11, Nr. 22, S. 11777–11791. DOI 10.5194/acp-11-11777-2011. Verfügbar unter: https://doi.org/10.26041/fhnw-9376