酚羰基水相反应形成aqSOA的过程：硫酸铵与硝酸铵溶液的比较,Environmental Science & Technology

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酚羰基水相反应形成aqSOA的过程：硫酸铵与硝酸铵溶液的比较
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2018-08-03 , DOI: 10.1021/acs.est.8b03441
Dan Dan Huang _{1,

2} , Qi Zhang ₃ , Heidi H. Y. Cheung ₄ , Lu Yu ₃ , Shan Zhou ₃ , Cort Anastasio ₅ , Jeremy D. Smith ₅ , Chak K. Chan ₁

Affiliation

我们调查了硫酸盐和硝酸盐对木材燃烧产生的两种酚羰基的光氧化作用对水相（aqSOA）中形成的次级有机气溶胶形成和演化的影响。丁香醛（C ₉ H ₁₀ O ₄）和乙酰丁香酮（C ₁₀ H ₁₂ O ₄）的光氧化可有效形成AqSOA。）在硫酸铵和硝酸铵溶液中的溶液，质量产率为30％至120％。通过气溶胶质谱仪获得的有机质谱图上的正矩阵分解显示出aqSOA的化学演化过程中功能化，低聚化和碎片化过程的结合。在反应的最初4小时内，官能化和低聚反应占主导，酚醛低聚物及其衍生物显着促进了aqSOA的形成；第一代产品的氧化导致大量的氧化开环产物。硝酸盐溶液中丁香醛和乙酰丁香酮的降解速度分别是硫酸盐溶液中的1.5和3.5倍，硝酸盐实验中的aqSOA产率是硫酸盐实验中的两倍。

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Formation and Evolution of aqSOA from Aqueous-Phase Reactions of Phenolic Carbonyls: Comparison between Ammonium Sulfate and Ammonium Nitrate Solutions

We investigate the effects of sulfate and nitrate on the formation and evolution of secondary organic aerosol formed in the aqueous phase (aqSOA) from photooxidation of two phenolic carbonyls emitted from wood burning. AqSOA was formed efficiently from the photooxidation of both syringaldehyde (C₉H₁₀O₄) and acetosyringone (C₁₀H₁₂O₄) in ammonium sulfate and ammonium nitrate solutions, with mass yields ranging from 30% to 120%. Positive matrix factorization on the organic mass spectra acquired by an Aerosol Mass Spectrometer revealed a combination of functionalization, oligomerization, and fragmentation processes in the chemical evolution of aqSOA. Functionalization and oligomerization dominated in the first 4 h of reaction, with phenolic oligomers and their derivatives significantly contributing to aqSOA formation; and oxidation of the first-generation products led to an abundance of oxygenated ring-opening products. Degradation rates of syringaldehyde and acetosyringone in nitrate solutions were 1.5 and 3.5 times faster than rates in sulfate solutions, and aqSOA yields in nitrate experiments are twice as high as in sulfate experiments. Nitrate likely promoted the reactions because it is a photolytic source of OH radicals, while sulfate is not, highlighting the importance of aerosol-phase nitrate in the formation of aqSOA by facilitating the photooxidation of organic precursors.

更新日期：2018-08-03

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