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Field observation on secondary organic aerosols during Asian dust storm periods: Formation mechanism of oxalic acid and related compounds on dust surface
Abstract Chemical evolution of East Asian dust during transpacific transport has been given much attention for inorganic species such as sulfate, nitrate and ammonium. However, the role of organic species during the transport has almost entirely been ignored. To understand the formation mechanism of secondary organic aerosols (SOA) on dust surfaces, this study investigated the concentrations and compositions of dicarboxylic acids, keto-carboxylic acids, α-dicarbonyls and inorganic ions in size-segregated aerosols (9-stages) collected in Xi'an, central China during the two dust storm episodes in the springs of 2009 and 2011 and compared with those in nondust storm periods. During the events the ambient particulate dicarboxylic acids were 932–2240 ng m−3, which are comparable and even higher than those in nondust periods. Molecular compositions of the above SOA are similar to those in nondust periods with oxalic acid being the leading species. In the presence of the dust storms, all the above mentioned SOA species in Xi'an were predominantly enriched on the coarse particles (>2.1 μm), and oxalic acid well correlated with (R2 = 0.72, p < 0.001) rather than . This phenomenon differs greatly from the SOA in any other nondust period that is usually characterized by an enrichment of oxalic acid in fine mode and a strong correlation of oxalic acid with . We propose a formation pathway to explain these observations, in which nitric acid and/or nitrogen oxides react with dust to produce Ca(NO3)2 and form a liquid phase on the surface of dust aerosols via water vapor-absorption of Ca(NO3)2, followed by a partitioning of the gas-phase water-soluble organic precursors (e.g.,glyoxal and methylglyoxal) into the aqueous-phase and a subsequent oxidation into oxalic acid. To the best of our knowledge, we found for the first time the enrichment of glyoxal and methylglyoxal on dust surface. Our data suggest an important role of nitrate in the heterogeneous formation process of SOA on the surface of dust.
Highlights High concentration of oxalic acid observed during the dust events. Oxalic acid, glyoxal and methylglyoxal dominated in coarse particles. Aqueous-phase formation of oxalic acid on dust surface.
Field observation on secondary organic aerosols during Asian dust storm periods: Formation mechanism of oxalic acid and related compounds on dust surface
Abstract Chemical evolution of East Asian dust during transpacific transport has been given much attention for inorganic species such as sulfate, nitrate and ammonium. However, the role of organic species during the transport has almost entirely been ignored. To understand the formation mechanism of secondary organic aerosols (SOA) on dust surfaces, this study investigated the concentrations and compositions of dicarboxylic acids, keto-carboxylic acids, α-dicarbonyls and inorganic ions in size-segregated aerosols (9-stages) collected in Xi'an, central China during the two dust storm episodes in the springs of 2009 and 2011 and compared with those in nondust storm periods. During the events the ambient particulate dicarboxylic acids were 932–2240 ng m−3, which are comparable and even higher than those in nondust periods. Molecular compositions of the above SOA are similar to those in nondust periods with oxalic acid being the leading species. In the presence of the dust storms, all the above mentioned SOA species in Xi'an were predominantly enriched on the coarse particles (>2.1 μm), and oxalic acid well correlated with (R2 = 0.72, p < 0.001) rather than . This phenomenon differs greatly from the SOA in any other nondust period that is usually characterized by an enrichment of oxalic acid in fine mode and a strong correlation of oxalic acid with . We propose a formation pathway to explain these observations, in which nitric acid and/or nitrogen oxides react with dust to produce Ca(NO3)2 and form a liquid phase on the surface of dust aerosols via water vapor-absorption of Ca(NO3)2, followed by a partitioning of the gas-phase water-soluble organic precursors (e.g.,glyoxal and methylglyoxal) into the aqueous-phase and a subsequent oxidation into oxalic acid. To the best of our knowledge, we found for the first time the enrichment of glyoxal and methylglyoxal on dust surface. Our data suggest an important role of nitrate in the heterogeneous formation process of SOA on the surface of dust.
Highlights High concentration of oxalic acid observed during the dust events. Oxalic acid, glyoxal and methylglyoxal dominated in coarse particles. Aqueous-phase formation of oxalic acid on dust surface.
Field observation on secondary organic aerosols during Asian dust storm periods: Formation mechanism of oxalic acid and related compounds on dust surface
Wang, Gehui (Autor:in) / Cheng, Chunlei (Autor:in) / Meng, Jingjing (Autor:in) / Huang, Yao (Autor:in) / Li, Jianjun (Autor:in) / Ren, Yanqin (Autor:in)
Atmospheric Environment ; 113 ; 169-176
09.05.2015
8 pages
Aufsatz (Zeitschrift)
Elektronische Ressource
Englisch