氨老化苯二次有机气溶胶棕碳组分的表征

IF 3 4区 地球科学 Q2 ENVIRONMENTAL SCIENCES Journal of Atmospheric Chemistry Pub Date : 2017-10-29 DOI:10.1007/s10874-017-9372-x
Mingqiang Huang, Jun Xu, Shunyou Cai, Xingqiang Liu, Weixiong Zhao, Changjin Hu, Xuejun Gu, Li Fang, Weijun Zhang
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引用次数: 19

摘要

含氮有机化合物(NOC)是一类重要的棕碳化合物,由二次有机气溶胶(SOA)与还原态氮反应生成。本研究通过在自制雾霾室中辐照苯/CH3ONO/NO/NH3混合空气,研究了苯SOA中氨(NH3)气老化产生的NOC化合物。采用紫外-可见分光光度计、衰减全反射-傅里叶变换红外光谱仪(ATR-FTIR)和气溶胶激光飞行时间质谱仪(ALTOFMS)结合模糊c均值(FCM)聚类算法,分别测定了NH3存在下老化苯SOA颗粒NOC产物。实验结果表明,NH3对苯的SOA形成有显著的促进作用。NH3与气态有机酸反应生成的有机铵盐,如乙醛酸铵、6-氧-2,4-己二烯酸铵是NH3老化苯SOA颗粒NOC的主要产物。h -咪唑、h -咪唑-2-乙醛等咪唑类产物通过NH3与苯双醛的非均相反应,成功地检测到它们是重要的棕碳成分。咪唑产物的形成表明,一些含有有机氮化合物的环境颗粒可能来自这一机制。本研究结果可能为探讨NH3沉积和SOA老化机制提供有价值的信息。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

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Characterization of brown carbon constituents of benzene secondary organic aerosol aged with ammonia

Nitrogen-containing organic compounds (NOC) formed from secondary organic aerosols (SOA) age via reaction with reduced nitrogen species are a vital class of brown carbon compounds. NOC compounds from ammonia (NH3) gas-aging of benzene SOA were investigated in present study, and the experiments were performed by irradiating benzene/CH3ONO/NO/NH3 air mixtures in a home-made smog chamber. The particulate NOC products of aged benzene SOA in the presence of NH3 were measured by UV-Vis spectrophotometer, attenuated total reflectance-Fourier transform infrared (ATR-FTIR), and aerosol laser time-of-flight mass spectrometer (ALTOFMS) coupled with Fuzzy C-Means (FCM) clustering algorithm, respectively. Experimental results demonstrated that NH3 has significant promotion effect on benzene SOA formation. Organic ammonium salts, such as ammonium glyoxylate, ammonium 6-oxo-2,4-hexadienoiclate, which are formed from NH3 reactions with gaseous organic acids were detected as the major particulate NOC products of NH3-aged benzene SOA. 1H–imidazole, 1H–imidazole-2-carbaldehyde and other imidazole products via the heterogeneous reactions between NH3 and dialdehydes of benzene SOA were successfully detected as important brown carbon constituents. The formation of imidazole products suggests that some ambient particles contained organonitrogen compounds may be come from this mechanism. The results of this study may provide valuable information for discussing NH3 deposition and SOA aging mechanisms.

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来源期刊
Journal of Atmospheric Chemistry
Journal of Atmospheric Chemistry 地学-环境科学
CiteScore
4.60
自引率
5.00%
发文量
16
审稿时长
7.5 months
期刊介绍: The Journal of Atmospheric Chemistry is devoted to the study of the chemistry of the Earth''s atmosphere, the emphasis being laid on the region below about 100 km. The strongly interdisciplinary nature of atmospheric chemistry means that it embraces a great variety of sciences, but the journal concentrates on the following topics: Observational, interpretative and modelling studies of the composition of air and precipitation and the physiochemical processes in the Earth''s atmosphere, excluding air pollution problems of local importance only. The role of the atmosphere in biogeochemical cycles; the chemical interaction of the oceans, land surface and biosphere with the atmosphere. Laboratory studies of the mechanics in homogeneous and heterogeneous transformation processes in the atmosphere. Descriptions of major advances in instrumentation developed for the measurement of atmospheric composition and chemical properties.
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