|
|
|
| Study on the factors affecting the formation of nitrogen-containing organic compounds formed from ammonia and toluene secondary organic aerosol |
| XU Jun1, HUANG Ming-qiang1, FENG Zhuang-zhuang1, CAI Shun-you1, ZHAO Wei-xiong2, HU Chang-jin2, GU Xue-jun2, ZHANG Wei-jun2 |
1. College of Chemistry & Chemical Engineering and Environment, Minnan Normal University, Fujian Provincial Key Laboratory of Modern Analytical Science and Separation Technology, Zhangzhou 363000, China;
2. Laboratory of Atmospheric Physico-Chemistry, Anhui Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Hefei 230031, China |
|
|
|
|
Abstract Ozone was photolyzed to produce OH radicals, and photooxidation of toluene is initiated to generate secondary organic aerosol (SOA) particles in home-made smog chamber, nitrogen-containing organic compounds formed from toluene SOA reaction with ammonia were studied under different experimental conditions. The absorbance at 205 and 270nm of the reaction product solution measured by UV-visible spectrophotometer was used to study the influence of environmental factors such as irradiation time, the concentration of toluene, ammonia, ozone, and relative humidity on the formation of nitrogen-containing organic compounds. The experimental results demonstrated that the concentration of organic acid ammonium and imidazole products gradually increases with the increase of ultraviolet irradiation time and the concentrations of toluene, ammonia and ozone. However, when the concentration of ozone exceeds a certain value, the high concentration of OH radicals generated by photolysis of ozone can oxidize the photooxidation product of toluene into more volatile compounds, which is not conducive to the formation of nitrogen-containing organic compounds. Also, the increase of water molecules would reduce the concentration of OH radicals, resulting in the decrease of the concentration of organic acid ammonium and imidazole products as the relative humidity increases. These would provide the experimental basis for studying the formation of the nitrogen-containing organic brown carbon of anthropogenic SOA particles.
|
|
Received: 08 July 2018
|
|
|
|
|
|
| [1] |
Li L J, Tang P, Nakao S S, et al. Novel approach for evaluating secondary organic aerosol from aromatic hydrocarbons:unified method for predicting aerosol composition and formation[J]. Environmental Science & Technology, 2016,50(12):6249-6256.
|
| [2] |
Gentner D R, Jathar S H, Gordon T D, et al. Review of urban secondary organic aerosol formation from gasoline and diesel motor vehicle emissions[J]. Environmental Science & Technology, 2017, 51(3):1074-1093.
|
| [3] |
Yang B, Ma P, Shu J, et al. Formation mechanism of secondary organic aerosol from ozonolysis of gasoline vehicle exhaust[J]. Environmental Pollution, 2018,234:960-968.
|
| [4] |
Sareen N, Waxman E M, Turpin B J, et al. Potential of aerosol liquid water to facilitate organic aerosol formation:assessing knowledge gaps about precursors and partitioning[J]. Environmental Science & Technology, 2017,51(6):3327-3335.
|
| [5] |
Tang M J, Alexander J M, Kwon D, et al. Optical and physico chemical properties of brown carbon aerosol:light scattering, FTIR extinction spectroscopy, and hygroscopic growth[J]. The Journal of Physical Chemistry A, 2016,120(24):4155-4166.
|
| [6] |
Thurston G D, Ahn J, Cromar K R, et al. Ambient particulate mater air pollution exposure and mortality in the NIH-AARP diet and health cohort[J]. Environmental Health Perspectives, 2016,124(4):484-490.
|
| [7] |
乐满,王式功,谢佳君,等.环境条件对遵义市呼吸系统疾病的影响及预测研究[J]. 中国环境科学, 2018,38(11):4334-4347. Yue M, Wang S G, Xie J J, et al. Study about the impact of environmental conditions on respiratory diseases and prediction in Zunyi City[J]. China Environmental Science, 2018,38(11):4334-4347.
|
| [8] |
董文煊,邢佳,王书肖.1994~2006年中国人为源大气氨排放时空分布[J]. 环境科学, 2010,31(7):1457-1463. Dong W X, Xing J, Wang S X. Temporal and spatial distribution of anthropogenic ammonia emissions in china:1994~2006[J]. Environmental Science, 2010,31(7):1457-1463.
|
| [9] |
Chu B, Zhang X, Liu Y, et al. Synergetic formation of secondary inorganic and organic aerosol:effect of SO2 and NH3on particle formation and growth[J]. Atmospheric Chemistry and Physics, 2016, 16(22):14219-14230.
|
| [10] |
Cheng Y F, Zheng G J, Wei C, et al. Reactive nitrogen chemistry in aerosol water as a source of sulfate during haze events in China[J]. Science Advances, 2016,2(12,e1601530):1-11.
|
| [11] |
Na K, Song C, Switzer C, et al. Effect of ammonia on secondary organic aerosol formation from α-Pinene ozonolysis in dry and humid conditions[J]. Environmental Science & Technology, 2007,41(12):6096-6102.
|
| [12] |
Babar Z B, Park J H, Lim H J. Influence of NH3 on secondary organic aerosols from the ozonolysis and photooxidation of α-pinene in a flow reactor[J]. Atmospheric Environment, 2017,164:71-84.
|
| [13] |
Liu Y, Liggio J, Staebler R, et al. Reactive uptake of ammonia to secondary organic aerosols:kinetics of organonitrogen formation[J]. Atmospheric Chemistry and Physics, 2015,15(23):13569-13584.
|
| [14] |
Huang M Q, Xu J, Cai S Y, et al. Chemical analysis of particulate products of aged 1,3,5-trimethylbenzene secondary organic aerosol in the presence of ammonia[J]. Atmospheric Pollution Research, 2018, 9(1):146-155.
|
| [15] |
Huang M Q, Xu J, Cai S Y, et al. Characterization of brown carbon constituents of benzene secondary organic aerosol aged with ammonia[J]. Journal of Atmospheric Chemistry, 2018,75(2):205-218.
|
| [16] |
Flores J M, Washenfelder R A, Adler G, et al. Complex refractive indices in the near-ultraviolet spectral region of biogenic secondary organic aerosol aged with ammonia[J]. Physical Chemistry Chemical Physics, 2014,16(22):10629-10642.
|
| [17] |
Teich M, van Pinxteren D, Kecorius S, et al. First quantification of imidazoles in ambient aerosol particles:potential photosensitizers, brown carbon constituents, and hazardous components[J]. Environmental Science & Technology, 2016,50(3):1166-1173.
|
| [18] |
Laskin A, Laskin J, Nizkorodov S A. Chemistry of atmospheric brown carbon[J]. Chemical Review, 2015,115(10):4335-4382.
|
| [19] |
Tsui W G, Rao Y, Dai H L, et al. Modeling photosensitized secondary organic aerosol formation in laboratory and ambient aerosols[J]. Environmental Science & Technology, 2017,51(13):7496-7501.
|
| [20] |
Atkinson R. Atmospheric chemistry of VOCs and NOx[J]. Atmospheric Environment, 2000,34(12-14):2063-2101.
|
| [21] |
Romonosky D E, Li Y, Shiraiwa M, et al. aqueous photochemistry of secondary organic aerosol of alpha-Pinene and alpha-Humulene oxidized with ozone, hydroxyl radical, and nitrate radical[J]. The Journal of Physical Chemistry A, 2017,121(6):1298-1309.
|
| [22] |
Lee A K Y, Zhao R, Li R, et al. Formation of light absorbing organo-nitrogen species from evaporation of droplets containing glyoxal and ammonium sulfate[J]. Environmental Science & Technology, 2013,47(22):12819-12826.
|
| [23] |
Pierce J R, Engelhart G J, Hildebrandt L, et al. Constraining particle evolution from wall losses,coagulation, and condensation-evaporation in smog-chamber experiments:optimal estimation based on size distribution measurements[J]. Aerosol Science and Technology, 2008,42(12):1001-1015.
|
| [24] |
郝立庆,王振亚,黄明强,等.羟基自由基浓度对二次有机气溶胶形成的影响[J]. 中国环境科学, 2006,26(S1):65-67. Hao L Q, Wang Z Y, Huang M Q, et al. Influence of hydroxyl radical concentration on the secondary organic aerosol formation[J]. China Environmental Science, 2006,26(S1):65-67.
|
| [25] |
Faust J A, Wong J P S, Lee A K Y, et al. Role of aerosol liquid water in secondary organic aerosol formation from volatile organic compounds[J]. Environmental Science & Technology, 2017,51(3):1405-1413.
|
| [26] |
宋秀瑜,曹念文,赵成,等.南京地区相对湿度对气溶胶含量的影响[J]. 中国环境科学, 2018,38(09):3240-3246. Song X Y, Cao N W, Zhao C, et al. Effect of relative humidity on aerosol content in Nanjing[J]. China Environmental Science, 2011,23(12):2013-2018.
|
| [27] |
张宇飞,朱燕群,王树荣,等.甲苯的光氧化降解试验研究[J]. 环境科学学报, 2015,35(9):2759-2765. Zhang Y F, Zhu Y Q, Wang S R, et al. Experimental study on the degradation of toluene by photo-oxidation[J]. Acta Scientiae Circumstantiae, 2015,35(9):2759-2765.
|
| [28] |
张春洋,马永亮.UV(254nm+185nm)光照降解气态甲苯的实验研究[J]. 中国环境科学, 2011,31(6):898-903. Zhang C Y, Ma Y L. Experimental study on UV(254nm+185nm) phtotodegradation of gaseous toluene[J]. China Environmental Science, 2011,31(6):898-903.
|
| [29] |
Wang Y J, Luo H, Jia L, et al. Effect of particle water on ozone and secondary organic aerosol formation from benzene-NO2-NaCl irradiations[J]. Atmospheric Environment, 2016,140:386-394.
|
| [30] |
Hu G S, Xu Y F, Jia L. Effects of relative humidity on the characterization of a photochemical smog chamber[J]. Journal of Environmental Sciences, 2011,23(12):2013-2018.
|
|
|
|
