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氮氧化物和相对湿度对甲苯光氧化生成二次有机气溶胶的影响。

Effect of NOx and RH on the secondary organic aerosol formation from toluene photooxidation.

作者信息

Liu Shijie, Liu Xiaodi, Wang Yiqian, Zhang Si, Wu Can, Du Wei, Wang Gehui

机构信息

Key Lab of Geographic Information Science of the Ministry of Education, School of Geographic Sciences, East China Normal University, Shanghai 210062, China.

Key Lab of Geographic Information Science of the Ministry of Education, School of Geographic Sciences, East China Normal University, Shanghai 210062, China; Institute of Eco-Chongming, 3663 North Zhongshan Road, Shanghai 200062, China.

出版信息

J Environ Sci (China). 2022 Apr;114:1-9. doi: 10.1016/j.jes.2021.06.017. Epub 2022 Jan 16.

Abstract

The secondary organic aerosol (SOA) formation mechanism and physicochemical properties can highly be influenced by relative humidity (RH) and NOx concentration. In this study, we performed a laboratory investigation of the SOA formation from toluene/OH photooxidation system in the presence or absence of NOx in dry and wet conditions. The chemical composition of toluene-derived SOA was measured using Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). It was found that the mass concentration of toluene decreased with increasing RH and NOx concentration. However, the change of SOA chemistry composition (f, O/C) with increased RH was not consistent in the condition with or without NOx. The light absorption and mass absorption coefficient (MAC) of the toluene-derived SOA only increased with RH in the presence of NOx. In contrast, MAC is invariant with RH in the absence of NOx. HR-ToF-AMS results showed that, in the presence of NOx, the increased nitro-aromatic compounds and N/C ratio concurrently caused the increase of SOA light absorption and O/C in wet conditions, respectively. The relative intensity of CHON and CHON family to the total nitrogen-containing organic compounds (NOCs) increased with the increasing RH, and be the major components of NOCs in wet condition. This work revealed a synergy effect of NOx and RH on SOA formation from toluene photooxidation.

摘要

二次有机气溶胶(SOA)的形成机制和物理化学性质会受到相对湿度(RH)和氮氧化物(NOx)浓度的显著影响。在本研究中,我们在干燥和潮湿条件下,对有无NOx存在时甲苯/OH光氧化体系中SOA的形成进行了实验室研究。使用Aerodyne高分辨率飞行时间气溶胶质谱仪(HR-ToF-AMS)测量了甲苯衍生的SOA的化学成分。结果发现,甲苯的质量浓度随RH和NOx浓度的增加而降低。然而,在有或无NOx的条件下,SOA化学成分(f,O/C)随RH增加的变化并不一致。仅在有NOx存在时,甲苯衍生的SOA的光吸收和质量吸收系数(MAC)才随RH增加。相反,在无NOx时,MAC随RH不变。HR-ToF-AMS结果表明,在有NOx存在时,硝基芳烃化合物的增加和N/C比的增加分别导致潮湿条件下SOA光吸收和O/C的增加。CHON和CHON家族相对于总含氮有机化合物(NOCs)的相对强度随RH增加而增加,并且是潮湿条件下NOCs的主要成分。这项工作揭示了NOx和RH对甲苯光氧化形成SOA的协同作用。

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