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Quantitative assessment of organosulfates in size-segregated rural fine aerosol

机译:大小隔离的农村精细气溶胶中有机硫酸盐的定量评估

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Organosulfates have recently come into the focus of organic aerosol researchas potentially important components of water-soluble secondary organicaerosol (SOA) which now dominate tropospheric fine aerosol. Their presencehas been confirmed by the identification of sulfate esters of abundantbiogenic carbonyl compounds in both smog chamber and continental aerosol.However, none of the studies have been able to determine the masscontribution of organosulfates to SOA.In this paper, as possibly the very first attempt to quantify organosulfatesin ambient aerosol, we inferred the mass concentrations of organosulfates byconcurrently determining mass concentrations of total sulfur, sulfate andmethanesulfonate in rural fine aerosol using two highly sensitive analyticaltechniques. Although uncertainties were relatively large, we found that massconcentrations of organosulfates in water-soluble fine aerosol ranged from0.02 μgS m−3 to 0.09 μgS m−3 yielding a masscontribution of 6–12% to bulk sulfur concentrations (or 6–14% tosulfate concentrations). The inferred size distribution of organosulfatessuggested that they possibly form in heterogeneous reactions fromsemi-volatile carbonyl compounds with subsequent or concurrent condensationof gaseous sulfuric acid producing a refractory organic film on particlesurfaces.
机译:有机硫酸盐最近已成为有机气溶胶研究的重点,因为它是水溶性次要有机气溶胶(SOA)的潜在重要成分,而SOA目前在对流层精细气溶胶中占主导地位。通过在烟雾室和大陆气溶胶中都鉴定了丰富的生物羰基化合物的硫酸酯,证实了它们的存在。然而,没有任何研究能够确定有机硫酸盐对SOA的质量贡献。 作为量化环境气溶胶中有机硫酸盐的首次尝试,我们通过使用两种高度灵敏的分析技术同时测定了农村精细气溶胶中总硫,硫酸盐和甲磺酸盐的质量浓度,从而推断了有机硫酸盐的质量浓度。尽管不确定性相对较大,但我们发现水溶性细气溶胶中有机硫酸盐的质量浓度范围为0.02μgSm -3 至0.09μgSm -3 ,产生的质量贡献为总硫浓度的6-12%(或硫酸盐浓度的6-14%)。推断的有机硫酸盐的粒度分布表明它们可能在半挥发性羰基化合物的异相反应中形成,随后气态硫酸随后或同时缩合,在颗粒表面形成难熔的有机膜。

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