Aqueous phase oligomerization of α,β-unsaturated carbonyls and acids investigated using ion mobility spectrometry coupled to mass spectrometry (IMS-MS)

作者: Pascal Renard , Sabrine Tlili , Sylvain Ravier , Etienne Quivet , Anne Monod

DOI: 10.1016/J.ATMOSENV.2015.10.060

关键词: Ion-mobility spectrometryMonomerComputational chemistryMass spectrometryMoleculeAqueous two-phase systemChemistryElectrosprayOrganic chemistryOligomerDegree of unsaturation

摘要: Abstract One of the current essential issues to unravel our ability forecast future climate change and air quality, implies a better understanding natural processes leading secondary organic aerosol (SOA) formation, in particular formation fate oligomers. The difficulty characterizing macromolecules is discern between large oxygenated molecules from series oligomers containing repeated small monomers diverse structures. In present study, taking advantage previously established radical vinyl oligomerization methyl vinylketone (MVK) aqueous phase, where relatively simple up 14 were observed, we have investigated same reactivity on several other unsaturated water soluble compounds (UWSOCs) few mixtures these precursor compounds. technique used characterize formed was traveling wave ion mobility spectrometry coupled hybrid quadrupole - time flight mass spectrometer (IMS-MS) fitted with an electrospray source ultra-high performance liquid chromatography (UPLC). allows for additional separation, especially ions, long carbon chains. We shown efficiency IMS-mass detect derived MVK photooxidation phase. results then compared oligomers, ten individual biogenic UWSOCs. allowed distinguishing different arising precursors. It also clearly showed that bearing non-conjugated unsaturation did not provide oligomerization. Finally, it technique, applied conjugated precursors, exhibited precursors co-oligomerize, i.e. forming only one complex oligomer system are discussed terms atmospheric implications detection chamber and/or field samples.

参考文章(66)
I. Kourtchev, S. J. Fuller, C. Giorio, R. M. Healy, E. Wilson, I. O'Connor, J. C. Wenger, M. McLeod, J. Aalto, T. M. Ruuskanen, W. Maenhaut, R. Jones, D. S. Venables, J. R. Sodeau, M. Kulmala, M. Kalberer, Molecular composition of biogenic secondary organic aerosols using ultrahigh resolution mass spectrometry: comparing laboratory and field studies Atmospheric Chemistry and Physics. ,vol. 14, pp. 2155- 2167 ,(2014) , 10.5194/ACP-14-2155-2014
NC Bouvier-Brown, AH Goldstein, DR Worton, DM Matross, JB Gilman, WC Kuster, D Welsh-Bon, C Warneke, JA De Gouw, TM Cahill, R Holzinger, None, Methyl chavicol: characterization of its biogenic emission rate, abundance, and oxidation products in the atmosphere Atmospheric Chemistry and Physics. ,vol. 9, pp. 2061- 2074 ,(2009) , 10.5194/ACP-9-2061-2009
D. V. Spracklen, J. L. Jimenez, K. S. Carslaw, D. R. Worsnop, M. J. Evans, G. W. Mann, Q. Zhang, M. R. Canagaratna, J. Allan, H. Coe, G. McFiggans, A. Rap, P. Forster, Aerosol mass spectrometer constraint on the global secondary organic aerosol budget Atmospheric Chemistry and Physics. ,vol. 11, pp. 12109- 12136 ,(2011) , 10.5194/ACP-11-12109-2011
Lynn R. Mazzoleni, Parichehr Saranjampour, Megan M. Dalbec, Vera Samburova, A. Gannet Hallar, Barbara Zielinska, Douglas H. Lowenthal, Steve Kohl, Identification of water-soluble organic carbon in non-urban aerosols using ultrahigh-resolution FT-ICR mass spectrometry: organic anions Environmental Chemistry. ,vol. 9, pp. 285- 297 ,(2012) , 10.1071/EN11167
Magda Claeys, Wu Wang, Alina C Ion, Ivan Kourtchev, András Gelencsér, Willy Maenhaut, Formation of secondary organic aerosols from isoprene and its gas-phase oxidation products through reaction with hydrogen peroxide Atmospheric Environment. ,vol. 38, pp. 4093- 4098 ,(2004) , 10.1016/J.ATMOSENV.2004.06.001
Nicole C. Bouvier-Brown, Rupert Holzinger, Katrin Palitzsch, Allen H. Goldstein, Large emissions of sesquiterpenes and methyl chavicol quantified from branch enclosure measurements Atmospheric Environment. ,vol. 43, pp. 389- 401 ,(2009) , 10.1016/J.ATMOSENV.2008.08.039
Hartmut Herrmann, Thomas Schaefer, Andreas Tilgner, Sarah A. Styler, Christian Weller, Monique Teich, Tobias Otto, Tropospheric aqueous-phase chemistry: kinetics, mechanisms, and its coupling to a changing gas phase. Chemical Reviews. ,vol. 115, pp. 4259- 4334 ,(2015) , 10.1021/CR500447K
Pascal Renard, Allison E Reed Harris, Rebecca J Rapf, Sylvain Ravier, Carine Demelas, Bruno Coulomb, Etienne Quivet, Veronica Vaida, Anne Monod, Aqueous Phase Oligomerization of Methyl Vinyl Ketone by Atmospheric Radical Reactions Journal of Physical Chemistry C. ,vol. 118, pp. 29421- 29430 ,(2014) , 10.1021/JP5065598