Volatility of mixed atmospheric humic-like substances and ammonium sulfate particles
Volatility of mixed atmospheric humic-like substances and ammonium sulfate particles
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大气类腐殖质物质与硫酸铵颗粒混合的挥发性
DOI：
10.5194/acp-17-3659-2017
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发表时间：
2016-10
影响因子：
6.3
通讯作者：
Kerminen
中科院分区：
文献类型：
--
作者：
Nie Wei;Hong Juan;Hame Silja A. K.;Ding Aijun;Li Yugen;Yan Chao;Hao Liqing;Mikkila Jyri;Zheng Longfei;Xie Yuning;Zhu Caijun;Xu Zheng;Chi Xuguang;Huang Xin;Zhou Yang;Lin Peng;Virtanen Annele;Worsnop Douglas R.;Kulmala Markku;Ehn Mikael;Yu Jianzhen;Kerminen
摘要。由于物种形成和多相过程的复杂性，有机气溶胶的挥发性仍然知之甚少。本研究从南京SORPES站采集的4个大气气溶胶样品中提取腐殖质样物质（HULIS），并利用挥发性串联差分迁移率分析仪（VTDMA）研究了不同粒径颗粒的挥发性行为。尽管4个样品中提取的HULIS颗粒质量浓度差异较大，但均表现出非常高的氧化态（O ： C > 0.95），表明次生形成是长三角地区HULIS的主要来源。在280 °C的温度下，提取的HULIS整体挥发性较低，所有再生的HULIS颗粒的剩余体积分数（VFR）均大于55 %。应用动力学传质模型对热熔盐（TD）数据进行了解析，得到了半挥发性组分（SVOC）、低挥发性组分（LVOC）和极低挥发性组分（ELVOC）的质量分数。结果表明，LVOC和ELVOC占HULIS总体积的80%以上（ %）。雾化过程导致再生HULIS颗粒的大小依赖蒸发，并导致更小颗粒中的ELVOC更多。为了了解无机盐与大气有机混合物之间的相互作用对有机气溶胶挥发性的影响，对硫酸铵和HULIS混合样品的蒸发进行了测量。结果表明，硫酸铵对HULIS的挥发性有显著的非线性影响。的估计分数ELVOC有机部分最大的粒子(145 海里)从26 %,增加纯湖里样本,93 % 1 : 3(质量比的湖里 : 作为)混合样本,到45 % 2 : 2混合样本,和70 % 3 : 1混合样本,这表明与硫酸铵倾向于减少大气有机化合物的波动。我们的研究结果表明，HULIS是有机气溶胶相中重要的低挥发性，甚至是极低挥发性的化合物。氧化、低聚、聚合和与无机盐的相互作用等多相过程是大气HULIS的重要形成途径，是低挥发性和极低挥发性有机气溶胶的重要来源。
Abstract. The volatility of organic aerosols remains poorly understood due to the complexity of speciation and multiphase processes. In this study, we extracted humic-like substances (HULIS) from four atmospheric aerosol samples collected at the SORPES station in Nanjing, eastern China, and investigated the volatility behavior of particles at different sizes using a Volatility Tandem Differential Mobility Analyzer (VTDMA). In spite of the large differences in particle mass concentrations, the extracted HULIS from the four samples all revealed very high-oxidation states (O : C > 0.95), indicating secondary formation as the major source of HULIS in Yangtze River Delta (YRD). An overall low volatility was identified for the extracted HULIS, with the volume fraction remaining (VFR) higher than 55 % for all the regenerated HULIS particles at the temperature of 280 °C. A kinetic mass transfer model was applied to the thermodenuder (TD) data to interpret the observed evaporation pattern of HULIS, and to derive the mass fractions of semi-volatile (SVOC), low-volatility (LVOC) and extremely low-volatility components (ELVOC). The results showed that LVOC and ELVOC dominated (more than 80 %) the total volume of HULIS. Atomizing processes led to a size-dependent evaporation of regenerated HULIS particles, and resulted in more ELVOC in smaller particles. In order to understand the role of interaction between inorganic salts and atmospheric organic mixtures in the volatility of an organic aerosol, the evaporation of mixed samples of ammonium sulfate (AS) and HULIS was measured. The results showed a significant but nonlinear influence of ammonium sulfate on the volatility of HULIS. The estimated fraction of ELVOC in the organic part of the largest particles (145 nm) increased from 26 %, in pure HULIS samples, to 93 % in 1 : 3 (mass ratio of HULIS : AS) mixed samples, to 45 % in 2 : 2 mixed samples, and to 70 % in 3 : 1 mixed samples, suggesting that the interaction with ammonium sulfate tends to decrease the volatility of atmospheric organic compounds. Our results demonstrate that HULIS are important low-volatility, or even extremely low-volatility, compounds in the organic-aerosol phase. As important formation pathways of atmospheric HULIS, multiphase processes, including oxidation, oligomerization, polymerization and interaction with inorganic salts, are indicated to be important sources of low-volatility and extremely low-volatility species of organic aerosols.
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DOI：
10.1002/chin.201528326
发表时间：
2015-07
期刊：
ChemInform
影响因子：
--
作者：
M. Bilde;K. Barsanti;Murray Booth;C. Cappa;N. Donahue;E. Emanuelsson;G. Mcfiggans;U. Krieger;C. Marcolli;D. Topping
通讯作者：
M. Bilde;K. Barsanti;Murray Booth;C. Cappa;N. Donahue;E. Emanuelsson;G. Mcfiggans;U. Krieger;C. Marcolli;D. Topping
影响因子：
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作者：
T. Kristensen;H. Wex;Bettina Nekat;J. Nøjgaard;D. Pinxteren;D. Lowenthal;L. Mazzoleni;K. Dieckmann;C. Koch;T. Mentel;H. Herrmann;A. Hallar;F. Stratmann;M. Bilde
通讯作者：
T. Kristensen;H. Wex;Bettina Nekat;J. Nøjgaard;D. Pinxteren;D. Lowenthal;L. Mazzoleni;K. Dieckmann;C. Koch;T. Mentel;H. Herrmann;A. Hallar;F. Stratmann;M. Bilde
影响因子：
6.3
作者：
B. Murphy;N. Donahue;A. Robinson;S. Pandis
通讯作者：
B. Murphy;N. Donahue;A. Robinson;S. Pandis
DOI：
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发表时间：
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期刊：
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影响因子：
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作者：
通讯作者：
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影响因子：
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作者：
H. Lukács;A. Gelencser;S. Hammer;H. Puxbaum;C. Pio;M. Legrand;A. Kasper-Giebl;M. Handler;A. L
通讯作者：
H. Lukács;A. Gelencser;S. Hammer;H. Puxbaum;C. Pio;M. Legrand;A. Kasper-Giebl;M. Handler;A. L