Quantifying the Role of the Relative Humidity-Dependent Physical State of Organic Particulate Matter in the Uptake of Semivolatile Organic Molecules | |
Han, Yuemei1,3; Gong, Zhaoheng1; Ye, Jianhuai1; Liu, Pengfei1; McKinney, Karena A.1,4; Martin, Scot T.1,2 | |
通讯作者 | Han, Yuemei(yuemei.han@ieecas.cn) ; Martin, Scot T.(scot_martin@harvard.edu) |
2019-11-19 | |
发表期刊 | ENVIRONMENTAL SCIENCE & TECHNOLOGY |
ISSN | 0013-936X |
卷号 | 53期号:22页码:13209-13218 |
摘要 | The uptake of gas-phase dicarboxylic acids to organic particulate matter (PM) was investigated to probe the role of the PM physical state in exchange processes between gas-phase semivolatile organic molecules and organic PM. A homologous series of probe molecules, specifically isotopically labeled C-13-dicarboxylic acids, was used in conjunction with aerosol mass spectrometry to obtain a quantitative characterization of the uptake to organic PM for different relative humidities (RHs). The PM was produced by the dark ozonolysis of unlabeled alpha-pinene. The uptake of C-13-labeled oxalic, malonic, and alpha-ketoglutaric acids increased stepwise by 5 to 15 times with increases in RH from 15 to 80%. The enhanced uptake with increasing RH was explained primarily by the higher molecular diffusivity in the particle phase, as associated with changes in the physical state of the organic PM from a nonliquid state to a progressively less-viscous liquid state. At high RH, the partitioning of the probe molecules to the particle phase was more associated with physicochemical interactions with the organic PM than that with the co-absorbed liquid water. Uptake of the probe molecules also increased with a decrease in volatility along the homologous series. This study quantitatively shows the key roles of the particle physical state in governing the interactions of organic PM with semivolatile organic molecules. |
DOI | 10.1021/acs.est.9b05354 |
关键词[WOS] | ALPHA-PINENE ; ATMOSPHERIC AEROSOLS ; DICARBOXYLIC-ACIDS ; ELEMENTAL ANALYSIS ; SOLID-STATE ; GAS UPTAKE ; PHASE ; VISCOSITY ; ISOPRENE ; SULFATE |
收录类别 | SCI ; SCI |
语种 | 英语 |
资助项目 | Office of Science of the U.S. Department of Energy[DE-SC0012792] ; Division of Atmospheric and Geospace Sciences of the U.S. National Science Foundation[1640378] |
WOS研究方向 | Engineering ; Environmental Sciences & Ecology |
项目资助者 | Office of Science of the U.S. Department of Energy ; Division of Atmospheric and Geospace Sciences of the U.S. National Science Foundation |
WOS类目 | Engineering, Environmental ; Environmental Sciences |
WOS记录号 | WOS:000498279400025 |
出版者 | AMER CHEMICAL SOC |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://ir.ieecas.cn/handle/361006/13009 |
专题 | 粉尘与环境研究室 |
通讯作者 | Han, Yuemei; Martin, Scot T. |
作者单位 | 1.Harvard Univ, Sch Engn & Appl Sci, Cambridge, MA 02138 USA 2.Harvard Univ, Dept Earth & Planetary Sci, Cambridge, MA 02138 USA 3.Chinese Acad Sci, Inst Earth Environm, Key Lab Aerosol Chem & Phys, State Key Lab Loess & Quaternary Geol, Xian 710061, Shaanxi, Peoples R China 4.Colby Coll, Dept Chem, Waterville, ME 04901 USA |
推荐引用方式 GB/T 7714 | Han, Yuemei,Gong, Zhaoheng,Ye, Jianhuai,et al. Quantifying the Role of the Relative Humidity-Dependent Physical State of Organic Particulate Matter in the Uptake of Semivolatile Organic Molecules[J]. ENVIRONMENTAL SCIENCE & TECHNOLOGY,2019,53(22):13209-13218. |
APA | Han, Yuemei,Gong, Zhaoheng,Ye, Jianhuai,Liu, Pengfei,McKinney, Karena A.,&Martin, Scot T..(2019).Quantifying the Role of the Relative Humidity-Dependent Physical State of Organic Particulate Matter in the Uptake of Semivolatile Organic Molecules.ENVIRONMENTAL SCIENCE & TECHNOLOGY,53(22),13209-13218. |
MLA | Han, Yuemei,et al."Quantifying the Role of the Relative Humidity-Dependent Physical State of Organic Particulate Matter in the Uptake of Semivolatile Organic Molecules".ENVIRONMENTAL SCIENCE & TECHNOLOGY 53.22(2019):13209-13218. |
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