Molecular Characterization of Organosulfur Compounds in Biodiesel and Diesel Fuel Secondary Organic Aerosol
Molecular Characterization of Organosulfur Compounds in Biodiesel and Diesel Fuel Secondary Organic Aerosol
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DOI：
10.1021/acs.est.6b03304
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发表时间：
2017-01-03
影响因子：
11.4
通讯作者：
Nizkorodov, Sergey A.
中科院分区：
文献类型：
--
作者：
Blair, Sandra L.;MacMillan, Amanda C.;Nizkorodov, Sergey A.
在高氮氧化物条件下，在有和无二氧化硫（SO2）、氨（NH3）和相对湿度（RH）的条件下，制备了柴油、生物柴油和20%生物柴油/80%柴油混合燃料光氧化过程中形成的二次有机气溶胶（SOA）。SOA中凝聚相有机化合物的组成使用几种互补技术测量，包括气溶胶质谱（AMS）、高分辨率纳喷雾解吸电喷雾电离质谱（nano-DESI/HRMS）和高分辨率和质量精度的21 T傅里叶变换离子回旋共振质谱（21 T FT-ICR MS）。结果表明，SO2光氧化实验中形成的硫酸和缩合的有机硫物种存在于SOA颗粒中。与在干燥条件下进行的实验相比，在RH 90%的高湿度实验中形成的有机硫物种较少。有一个很强的重叠，在这项研究中观察到的有机硫物种与以前的领域和商会的SOA的研究。许多有机硫酸盐（R-OS（O）（2）OH）的MS峰以前被指定为生物源，或在实地研究中来源不明，可能源于人为来源，如柴油和生物柴油燃料中存在的碳氢化合物的光氧化。
Secondary organic aerosol (SOA), formed in the photooxidation of diesel fuel, biodiesel fuel, and 20% biodiesel fuel/80% diesel fuel mixture, are prepared under high-NOx conditions in the presenth and absence of sulfur dioxide (SO2), ammonia (NH3), and relative humidity (RH). The composition of condensed-phase organic compounds in SOA- is measured using several complementary techniques including aerosol mass spectrometry (AMS), high-resolution nanospray desorption electrospray ionization mass spectrometry (nano-DESI/HRMS), arid ultrahigh resolution and mass accuracy 21T Fourier transform ion cyclotron resonance mass spectrometry (21T FT-ICR MS). Results demonstratethat sulfuric acid and condensed organosulfur species formed in photooxidation experiments with SO2 are present in the SOA particle. Fewer organosulfur species are formed in the high humidity experiMents, performed at RH 90%, in comparison with experiments done under dry conditions. There is a strong overlap of organosulfur species observed in this study with previous field and chamber studies of SOA. Many MS peaks of organosulfates (R-OS(O)(2)OH) previously designated as biogenic,or of unknown origin in field studies might have originated from anthropogenic sources, such as photooxidation of hydrocarbons present in diesel and biodiesel fuel.