激光解吸电离技术在线测量苯水相二次有机气溶胶
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摘要
利用气溶胶激光飞行时间质谱仪激光解吸电离技术开展了苯水相二次有机气溶胶在线测量研究。实验结果表明,苯水相光氧化反应形成的二次有机气溶胶粒子粒径小于1.0μm,激光解吸电离质谱中存在醛类m/z 29(CHO~+)、57(CHOCO~+),羧酸m/z 44(COO~+),苯环m/z 77(C_6H~+_5)、65(C_5H~+_5)和酚类化合物m/z 93(C_6H_5O~+)特征裂解碎片峰。醛类、羧酸和酚类化合物是苯水相SOA粒子的化学组分,各类型组分含量大小关系为:醛类化合>羧酸>酚类化合物。气溶胶激光飞行时间质谱仪激光解吸电离技术能够用于水相SOA粒子化学组分的在线测量,可用于水相SOA形成机理和过程的研究。
The on-line measurement of secondary organic aerosol formed from aqueous photooxidation of benzene with the laser desorption ionization technology of aerosol laser time-of-flight mass spectrometer was carried out. The experimental results indicated that the diameter of secondary organic aerosol particles formed from the aqueous photooxidation of benzene is less than 1.0 μm. Characteristic fragmentation peaks of aldehydes of m/z 29(CHO~+), 57(CHOCO~+), carboxylic acid of m/z 44(COO~+), benzene ring of m/z 77(C_6H~+_5), 65(C_5H~+_5) and phenolic compounds of m/z 93(C_6H_5O~+)were found in laser desorption mass spectra of secondary organic aerosol particles. Experimental results demonstrate that aldehydes, carboxylic acids and phenolic compounds are the chemical components of secondary organic aerosol particles, and the contents of various components were: aldehydes > carboxylic acids > phenolic compounds. These were shown that the laser desorption ionization technology of aerosol laser time-of-flight mass spectrometer can be used for on-line measurement of chemical composition of aqueous secondary organic aerosol particles, is a useful tool to reveal the formation mechanism and process of aqueous secondary organic aerosol particles.
The on-line measurement of secondary organic aerosol formed from aqueous photooxidation of benzene with the laser desorption ionization technology of aerosol laser time-of-flight mass spectrometer was carried out. The experimental results indicated that the diameter of secondary organic aerosol particles formed from the aqueous photooxidation of benzene is less than 1.0 μm. Characteristic fragmentation peaks of aldehydes of m/z 29(CHO~+), 57(CHOCO~+), carboxylic acid of m/z 44(COO~+), benzene ring of m/z 77(C_6H~+_5), 65(C_5H~+_5) and phenolic compounds of m/z 93(C_6H_5O~+)were found in laser desorption mass spectra of secondary organic aerosol particles. Experimental results demonstrate that aldehydes, carboxylic acids and phenolic compounds are the chemical components of secondary organic aerosol particles, and the contents of various components were: aldehydes > carboxylic acids > phenolic compounds. These were shown that the laser desorption ionization technology of aerosol laser time-of-flight mass spectrometer can be used for on-line measurement of chemical composition of aqueous secondary organic aerosol particles, is a useful tool to reveal the formation mechanism and process of aqueous secondary organic aerosol particles.
引文
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[22] 王光辉,熊少祥.有机质谱解析[M].北京:化学化工出版社,2005:89—107.Wang Guanghui,Xiong Shaoxiang.Analysis of organic mass spectrometry[M].Beijing:Chemical Industry Press,2005:89—107.
[23] Sato K,Takami A,Isozaki T,et al.Mass spectrometric study of secondary organic aerosol formed from the photo-oxidation of aromatic hydrocarbons[J].Atmospheric Environment,2010,44(8):1080—1087.
[24] Sun Y L,Zhang Q,Anastasio C,et al.Insights into secondary organic aerosol formed via aqueous-phase reactions of phenolic compounds based on high resolution mass spectrometry[J].Atmospheric Chemical & Physics,2010,10(2):4809—4822.
[25] Grebenkin S Y,Krasnoperov L N.Kinetics and thermochemistry of the hydroxycyclohexadienyl radical reaction with O2:C6H6OH+O2?C6H6(OH)OO[J].Journal of Physical Chemistry A,2004,108(11):1953—1963.
[2] 吴彬青,赵春柳,丁振名.基于PDMS材料的Sagnac干涉光纤挥发性有机物传感器[J].光子学报,2017,46(1):0106003Wu Binqing,Zhao Chunliu,Ding Zhenming.Sagnac interferometer fiber volatile organic compounds sensor based on PDMS [J].Acta Photonica Sinica,2017,46(1):0106003.
[3] 祁骞,周学华,王文兴.二次有机气溶胶的水相形成研究[J].化学进展,2014,26(0203):458—466.Qi Qian,Zhou Xuehua,Wang Wenxing.Studies on formation of aqueous secondary organic aerosols[J].Progress in Chemistry,2014,26(0203):458—466.
[4] 叶招莲,瞿珍秀,马帅帅,等.气溶胶水相反应生成二次有机气溶胶研究进展[J].环境科学,2018,39(8):3954—3964.Ye Zhaolian,Qu Zhenxiu,Ma Shuaishuai,et al.Secondary organic aerosols from aqueous reaction of aerosol water [J].Environmental Science,2018,39(8):3954—3964.
[5] 曹军骥,李建军.二次有机气溶胶的形成及其毒理效应[J].地球环境学报,2016,7(5):431—441.Cao Junji,Li Jianjun.Formation and toxicological effect of secondary organic aerosols[J].Journal of Earth Environment,2016,7(5):431—441.
[6] Haan D O D,Corrigan A L,Tolbert M A,et al.Secondary organic aerosol formation by self-reactions of methylglyoxal and glyoxal in evaporating droplets[J].Environmental Science & Technology,2009,43(21):8184—8190.
[7] 周欢,冯艳丽,姜知明,等.大气中二羰基化合物及其生成的二次有机气溶胶[J].上海大学学报:自然科学版,2016,22(2):159—171.Zhou Huan,Feng Yanli,Jiang Zhiming,et al.Dicarbonyl compounds and formation secondary organic aerosol in atmosphere [J].Journal of Shanghai University:natural Science Edition,2016,22(2):159—171.
[8] Kameel F R,Hoffmann M R,Colussi A J.OH radical-initiated chemistry of isoprene in aqueous media.atmospheric implications [J].Journal of Physical Chemistry A,2013,117(24):5117—5123.
[9] Aljawhary D,Zhao R,Lee A K Y,et al.Kinetics,mechanism,and secondary organic aerosol yield of aqueous phase photo-oxidation of α-pinene oxidation products [J].Journal of Physical Chemistry A,2016,120(9):1395—1407.
[10] Ervens B,Tuppin B J,Weber R J.Secondary organic aerosol formation in cloud droplets and aqueous particles (aqSOA):a review of laboratory,field and model studies[J].Atmospheric Chemistry and Physics,2011,11(21):11069—11102.
[11] Herrmann H,Schaefer T,Tilgener A,et al.Tropospheric aqueous-phase chemistry:kinetics,mechanisms,and its coupling to a changing gas phase[J].Chemical Reviews,2015,115(10):4259—4334.
[12] Pratt K A,Prather K A.Mass spectrometry of atmospheric aerosols-recent developments and applications.part II:On-line mass spectrometry techniques[J].Mass Spectrometry Reviews,2011,31(1):1—16.
[13] 赵文武,黄明强,郝立庆,等.用激光解吸附电离法对三甲苯生成二次有机气溶粒子的分析[J].光学技术,2008,34(4):544—547.Zhao Wenwu,Huang Mingqiang,Hao Liqing,et al.Analysis of secondary organic photooxidation products of trimethylbenzene using laser desorption/ionization method[J].Optical Technique,2008,34(4):544—547.
[14] Huang Mingqiang,Hao Liqing,Gu Xuejun,et al.Effects of inorganic seed aerosols on the growth and chemical composition of secondary organic aerosol formed from OH-initiated oxidation of toluene[J].Journal of Atmospheric Chemistry,2013,70(2):151—164.
[15] Huang Mingqiang,Liu Xingqiang,Hu Changjin,et al.Aerosol laser time-of-flight mass spectrometer for the on-line measurement of secondary organic aerosol in smog chamber[J].Measurement,2014,55:394—401.
[16] 陈天增,葛艳丽,刘永春,等.我国机动车排放VOCs及其大气环境影响[J].环境科学,2018,39(02):478—492.Chen Tianzeng,Ge Yanli,Liu Yongchun,et al.VOCs emission from motor vehicles in China and its impact on the atmospheric environment[J].Environmental Science,2018,39(2):478—492.
[17] 冯状状,黄明强,徐俊,等.羟基启动苯液相光氧化产物的傅里叶变换红外光谱研究[J].红外,2018,39(08):40—45.Feng Zhuangzhuang,Huang Mingqiang,Xu Jun,et al.Study of Fourier transform infrared spectra of OH-Initiated benzene aqueous photooxidation products [J].Infrared,2018,39(08):40—45.
[18] Carlton A G,Turpin B J,Altieri K E,et al.Atmospheric oxalic acid and SOA production from glyoxal:results of aqueous photooxidation experiments[J].Atmospheric Environment,2007,41(35):7588—7602.
[19] 郭晓勇,方黎,蒋兴浩,等.基于模糊聚类算法的气溶胶单粒子飞行时间质谱在线数据分析系统[J].过程工程学报,2006,6(2):138—142.Guo Xiaoyong,Fang Li,Jiang Xinghao,et al.On-line analysis of mass spectra of individual aerosol particles using fuzzy clustering algorithms[J].The Chinese Journal of Process Engineering,2006,6(2):138—142.
[20] 周留柱,顾学军,朱元,等.气溶胶单粒子的检测效率与基质辅助激光解吸电离研究[J].中国激光,2006,33(01):97—101.Zhou Liuzhu,Gu Xuejun,Zhu Yuan,et al.Investigation of individual aerosol particles detection efficiency and matrix assisted laser desorption/ionization[J].Chinese Journal of Lasers,2006,33(01):97—101.
[21] Huang Mingqiang,Hao Liqing,Guo Xiaoyong,et al.Characterization of secondary organic aerosol particles using aerosol laser time-of-flight mass spectrometer coupled with FCM clustering algorithm[J].Atmospheric Environment,2013,64(64):85—94.
[22] 王光辉,熊少祥.有机质谱解析[M].北京:化学化工出版社,2005:89—107.Wang Guanghui,Xiong Shaoxiang.Analysis of organic mass spectrometry[M].Beijing:Chemical Industry Press,2005:89—107.
[23] Sato K,Takami A,Isozaki T,et al.Mass spectrometric study of secondary organic aerosol formed from the photo-oxidation of aromatic hydrocarbons[J].Atmospheric Environment,2010,44(8):1080—1087.
[24] Sun Y L,Zhang Q,Anastasio C,et al.Insights into secondary organic aerosol formed via aqueous-phase reactions of phenolic compounds based on high resolution mass spectrometry[J].Atmospheric Chemical & Physics,2010,10(2):4809—4822.
[25] Grebenkin S Y,Krasnoperov L N.Kinetics and thermochemistry of the hydroxycyclohexadienyl radical reaction with O2:C6H6OH+O2?C6H6(OH)OO[J].Journal of Physical Chemistry A,2004,108(11):1953—1963.