Physical state of 2-methylbutane-1,2,3,4-tetraol in pure and internally mixed aerosols

Lessmeier J, Dette HP, Godt A, Koop T (2018)
Atmospheric Chemistry and Physics 18(21): 15841-15857.

Zeitschriftenaufsatz | Veröffentlicht | Englisch
 
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Abstract / Bemerkung
2-Methylbutane-1,2,3,4-tetraol (hereafter named tetraol) is an important oxidation product of isoprene and can be considered as a marker compound for isoprene-derived secondary organic aerosols (SOAs). Little is known about this compound's physical phase state, although some field observations indicate that isoprene-derived secondary organic aerosols in the tropics tend to be in a liquid rather than a solid state. To gain more knowledge about the possible phase states of tetraol and of tetraol-containing SOA particles, we synthesized tetraol as racemates as well as enantiomerically enriched materials. Subsequently the obtained highly viscous dry liquids were investigated calorimetrically by differential scanning calorimetry revealing subambient glass transition temperatures Tg. We also show that only the diastereomeric isomers differ in their Tg values, albeit only by a few kelvin. We derive the phase diagram of water–tetraol mixtures over the whole tropospheric temperature and humidity range from determining glass transition temperatures and ice melting temperatures of aqueous tetraol mixtures. We also investigated how water diffuses into a sample of dry tetraol. We show that upon water uptake two homogeneous liquid domains form that are separated by a sharp, locally constrained concentration gradient. Finally, we measured the glass transition temperatures of mixtures of tetraol and an important oxidation product of α-pinene-derived SOA: 3-methylbutane-1,2,3-tricarboxylic acid (3-MBTCA). Overall, our results imply a liquid-like state of isoprene-derived SOA particles in the lower troposphere at moderate to high relative humidity (RH), but presumably a semisolid or even glassy state at upper tropospheric conditions, particularly at low relative humidity, thus providing experimental support for recent modeling calculations.
Erscheinungsjahr
2018
Zeitschriftentitel
Atmospheric Chemistry and Physics
Band
18
Ausgabe
21
Seite(n)
15841-15857
eISSN
1680-7324
Page URI
https://pub.uni-bielefeld.de/record/2932049

Zitieren

Lessmeier J, Dette HP, Godt A, Koop T. Physical state of 2-methylbutane-1,2,3,4-tetraol in pure and internally mixed aerosols. Atmospheric Chemistry and Physics. 2018;18(21):15841-15857.
Lessmeier, J., Dette, H. P., Godt, A., & Koop, T. (2018). Physical state of 2-methylbutane-1,2,3,4-tetraol in pure and internally mixed aerosols. Atmospheric Chemistry and Physics, 18(21), 15841-15857. doi:10.5194/acp-18-15841-2018
Lessmeier, J., Dette, H. P., Godt, A., and Koop, T. (2018). Physical state of 2-methylbutane-1,2,3,4-tetraol in pure and internally mixed aerosols. Atmospheric Chemistry and Physics 18, 15841-15857.
Lessmeier, J., et al., 2018. Physical state of 2-methylbutane-1,2,3,4-tetraol in pure and internally mixed aerosols. Atmospheric Chemistry and Physics, 18(21), p 15841-15857.
J. Lessmeier, et al., “Physical state of 2-methylbutane-1,2,3,4-tetraol in pure and internally mixed aerosols”, Atmospheric Chemistry and Physics, vol. 18, 2018, pp. 15841-15857.
Lessmeier, J., Dette, H.P., Godt, A., Koop, T.: Physical state of 2-methylbutane-1,2,3,4-tetraol in pure and internally mixed aerosols. Atmospheric Chemistry and Physics. 18, 15841-15857 (2018).
Lessmeier, Jörn, Dette, Hans Peter, Godt, Adelheid, and Koop, Thomas. “Physical state of 2-methylbutane-1,2,3,4-tetraol in pure and internally mixed aerosols”. Atmospheric Chemistry and Physics 18.21 (2018): 15841-15857.
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