Mingqiang Huang, Jun Xu, Shunyou Cai, Xingqiang Liu, Weixiong Zhao, Changjin Hu, Xuejun Gu, Li Fang, Weijun Zhang
{"title":"氨老化苯二次有机气溶胶棕碳组分的表征","authors":"Mingqiang Huang, Jun Xu, Shunyou Cai, Xingqiang Liu, Weixiong Zhao, Changjin Hu, Xuejun Gu, Li Fang, Weijun Zhang","doi":"10.1007/s10874-017-9372-x","DOIUrl":null,"url":null,"abstract":"<p>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 (NH<sub>3</sub>) gas-aging of benzene SOA were investigated in present study, and the experiments were performed by irradiating benzene/CH<sub>3</sub>ONO/NO/NH<sub>3</sub> air mixtures in a home-made smog chamber. The particulate NOC products of aged benzene SOA in the presence of NH<sub>3</sub> 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 NH<sub>3</sub> 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 NH<sub>3</sub> reactions with gaseous organic acids were detected as the major particulate NOC products of NH<sub>3</sub>-aged benzene SOA. 1H–imidazole, 1H–imidazole-2-carbaldehyde and other imidazole products via the heterogeneous reactions between NH<sub>3</sub> 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 NH<sub>3</sub> deposition and SOA aging mechanisms.</p>","PeriodicalId":611,"journal":{"name":"Journal of Atmospheric Chemistry","volume":"75 2","pages":"205 - 218"},"PeriodicalIF":3.0000,"publicationDate":"2017-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1007/s10874-017-9372-x","citationCount":"19","resultStr":"{\"title\":\"Characterization of brown carbon constituents of benzene secondary organic aerosol aged with ammonia\",\"authors\":\"Mingqiang Huang, Jun Xu, Shunyou Cai, Xingqiang Liu, Weixiong Zhao, Changjin Hu, Xuejun Gu, Li Fang, Weijun Zhang\",\"doi\":\"10.1007/s10874-017-9372-x\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>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 (NH<sub>3</sub>) gas-aging of benzene SOA were investigated in present study, and the experiments were performed by irradiating benzene/CH<sub>3</sub>ONO/NO/NH<sub>3</sub> air mixtures in a home-made smog chamber. The particulate NOC products of aged benzene SOA in the presence of NH<sub>3</sub> 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 NH<sub>3</sub> 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 NH<sub>3</sub> reactions with gaseous organic acids were detected as the major particulate NOC products of NH<sub>3</sub>-aged benzene SOA. 1H–imidazole, 1H–imidazole-2-carbaldehyde and other imidazole products via the heterogeneous reactions between NH<sub>3</sub> 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 NH<sub>3</sub> deposition and SOA aging mechanisms.</p>\",\"PeriodicalId\":611,\"journal\":{\"name\":\"Journal of Atmospheric Chemistry\",\"volume\":\"75 2\",\"pages\":\"205 - 218\"},\"PeriodicalIF\":3.0000,\"publicationDate\":\"2017-10-29\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://sci-hub-pdf.com/10.1007/s10874-017-9372-x\",\"citationCount\":\"19\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Atmospheric Chemistry\",\"FirstCategoryId\":\"89\",\"ListUrlMain\":\"https://link.springer.com/article/10.1007/s10874-017-9372-x\",\"RegionNum\":4,\"RegionCategory\":\"地球科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"ENVIRONMENTAL SCIENCES\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Atmospheric Chemistry","FirstCategoryId":"89","ListUrlMain":"https://link.springer.com/article/10.1007/s10874-017-9372-x","RegionNum":4,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENVIRONMENTAL SCIENCES","Score":null,"Total":0}
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.
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.