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Organosulfates in humic-like substance fraction isolated from aerosols at seven locations in East Asia: A study by ultrahigh resolution mass spectrometry.
MedLine Citation:
PMID:  23153227     Owner:  NLM     Status:  Publisher    
Abstract/OtherAbstract:
HUmic-Like substances (HULIS) in ambient aerosols collected at seven locations in East Asia were analyzed using electrospray ionization (ESI) coupled with an ultrahigh resolution mass spectrometer (UHRMS). Locations included a 3-km high mountaintop site in Taiwan, rural, suburban and urban locations in the Pearl River Delta (PRD), South China and in Taiwan. Organosulfates (OS) in the HULIS fraction were tentatively identified through accurate mass measurements and MS/MS spectra interpretation. In the two mountaintop samples collected in regional background atmosphere, little OS were detected while a few hundred OS formulas were identified in the six samples taken in Taiwan and PRD. Many of the OS ions were among the most intense peaks in the negative ESI-UHRMS spectra and their elemental formulas were identical to OS derived from biogenic volatile organic compounds (BVOCs) (e.g. monoterpenes) that have been identified in chamber studies. With OS having less than 6 carbon atoms too hydrophilic to be retained in the HULIS fraction, OS containing 10 carbon atoms were the most abundant, indicating monoterpenes as important precursors of OS in the HULIS fraction. Clear spatial variation in abundance of OS was found among different atmospheric environments, with enhanced coupling of BVOCs with anthropogenic acidic aerosols observed in the PRD samples over the Taiwan samples. The double bond equivalent (DBE) values indicate majority of OS (>90%) in the HULIS fraction are aliphatic. The elemental compositions of OS compounds containing N atoms (defined as CHONS) indicate that they are probably nitrooxy OS. Some insights into OS formation mechanism are also gained through examining the presence/absence of perceived reactant-product formula pairs in the mass spectra. The results suggest the dominant epoxide intermediate pathway for formation of OS compounds without N atoms (defined as CHOS) and confirm the more readily hydrolyzed characteristics of the -ONO2 group than the -OSO3 group while there lacks evidence for the epoxide pathway to account for the formation of OS in the CHONS sub-group.
Authors:
Peng Lin; Jian Zhen Yu; Guenter Engling; Markus Kalberer
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Publication Detail:
Type:  JOURNAL ARTICLE     Date:  2012-11-16
Journal Detail:
Title:  Environmental science & technology     Volume:  -     ISSN:  1520-5851     ISO Abbreviation:  Environ. Sci. Technol.     Publication Date:  2012 Nov 
Date Detail:
Created Date:  2012-11-16     Completed Date:  -     Revised Date:  -    
Medline Journal Info:
Nlm Unique ID:  0213155     Medline TA:  Environ Sci Technol     Country:  -    
Other Details:
Languages:  ENG     Pagination:  -     Citation Subset:  -    
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