Dialkylsulfate formation in sulfuric acid-seeded secondary organic aerosol produced using an outdoor chamber under natural sunlight

作者: Jiaying Li , Myoseon Jang , Ross L. Beardsley

DOI: 10.1071/EN15129

关键词: IsopreneSulfateFluorescence spectrometryAerosolOzoneSulfuric acidNOxEnvironmental chemistryOrganosulfateChemistry

摘要: Environmental context Laboratory and field studies have both provided evidence for organosulfate formation by esterification of H2SO4 with organic compounds in aerosols. Using an outdoor chamber, the production dialkylsufate was measured aerosols produced photooxidation various hydrocarbons presence aerosol NOx. The organosulfates influences decrease acidity hygroscopicity. Abstract Secondary (SOA) were volatile (VOCs) isoprene, α-pinene toluene, excess amounts sulfuric acid seed varying NOx concentrations using a large, smog chamber. Aerosol ([H+], μmol m–3) colorimetry integrated reflectance UV-visible spectrometer (C-RUV). C-RUV technique measures changes through neutralisation ammonia dialkylsulfate, diester acid. concentration (μmol dialkylsulfate estimated difference [H+] obtained from particle-into-liquid-sampler ion chromatography (PILS-IC). yield (YdiOS) defined as normalised ammonium-free sulfate ([SO42–]free=[SO42–] – 0.5 [NH4+]) carbon. highest YdiOS appeared isoprene SOA lowest SOA. Under our experimental conditions, more than 50% total sulfates acid-seeded dialkylsulfates. For all SOA, higher observed under conditions (VOC (ppb C)/NO (ppb)<15). Among major functional groups (–COOH, –CO–H, –CHO –ONO2) predicted to be present simple absorptive partitioning model products multiphase system (gas, inorganic aerosol), –ONO2 found correlated YdiOS. In particular, strong correlation between alcohol groups.

参考文章(65)
Allan F. M. Barton, CRC Handbook of Solubility Parameters and Other Cohesion Parameters Barton, A.F.M. <https://researchrepository.murdoch.edu.au/view/author/Barton, Allan.html> (2017) CRC Handbook of Solubility Parameters and Other Cohesion Parameters. Routledge as part of the Taylor and Francis group, New York.. ,(1983)
Barbara Nozière, Sanna Ekström, Tomas Alsberg, Sara Holmström, None, Radical‐initiated formation of organosulfates and surfactants in atmospheric aerosols Geophysical Research Letters. ,vol. 37, ,(2010) , 10.1029/2009GL041683
Raymond Eller Kirk, Donald Frederick Othmer, Encyclopedia of Chemical Technology ,(1998)
Myoseon Jang, Nadine M Czoschke, Sangdon Lee, Richard M Kamens, Heterogeneous Atmospheric Aerosol Production by Acid-Catalyzed Particle-Phase Reactions Science. ,vol. 298, pp. 814- 817 ,(2002) , 10.1126/SCIENCE.1075798
Yadian Gómez-González, Jason D. Surratt, Filip Cuyckens, Rafal Szmigielski, Reinhilde Vermeylen, Mohammed Jaoui, Michael Lewandowski, John H. Offenberg, Tadeusz E. Kleindienst, Edward O. Edney, Frank Blockhuys, Christian Van Alsenoy, Willy Maenhaut, Magda Claeys, Characterization of organosulfates from the photooxidation of isoprene and unsaturated fatty acids in ambient aerosol using liquid chromatography/(-) electrospray ionization mass spectrometry Journal of Mass Spectrometry. ,vol. 43, pp. 371- 382 ,(2008) , 10.1002/JMS.1329
J. D. Surratt, A. W. H. Chan, N. C. Eddingsaas, M. Chan, C. L. Loza, A. J. Kwan, S. P. Hersey, R. C. Flagan, P. O. Wennberg, J. H. Seinfeld, Reactive intermediates revealed in secondary organic aerosol formation from isoprene Proceedings of the National Academy of Sciences of the United States of America. ,vol. 107, pp. 6640- 6645 ,(2010) , 10.1073/PNAS.0911114107
Nataša Šegatin, Cveto Klofutar, Salting-Out of Some Alkyl Acetates in Aqueous Sodium Chloride Solutions Monatshefte fuer Chemie/Chemical Monthly. ,vol. 131, pp. 0131- 0144 ,(2000) , 10.1007/S007060050014
C. Bloss, V. Wagner, M. E. Jenkin, R. Volkamer, W. J. Bloss, J. D. Lee, D. E. Heard, K. Wirtz, M. Martin-Reviejo, G. Rea, J. C. Wenger, M. J. Pilling, Development of a detailed chemical mechanism (MCMv3.1) for the atmospheric oxidation of aromatic hydrocarbons Atmospheric Chemistry and Physics. ,vol. 5, pp. 641- 664 ,(2004) , 10.5194/ACP-5-641-2005
Elizabeth A. Stone, Liming Yang, Liya E. Yu, Maheswar Rupakheti, Characterization of organosulfates in atmospheric aerosols at Four Asian locations Atmospheric Environment. ,vol. 47, pp. 323- 329 ,(2012) , 10.1016/J.ATMOSENV.2011.10.058
Simon L. Clegg, Peter Brimblecombe, Anthony S. Wexler, Thermodynamic Model of the System H+−NH4+−SO42-−NO3-−H2O at Tropospheric Temperatures Journal of Physical Chemistry A. ,vol. 102, pp. 2137- 2154 ,(1998) , 10.1021/JP973042R