Aging induced changes on NEXAFS fingerprints in individual combustion particles

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

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

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