Quantifying the Role of the Relative Humidity-Dependent Physical State of Organic Particulate Matter in the Uptake of Semivolatile Organic Molecules

doi:10.1021/acs.est.9b05354

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	Quantifying the Role of the Relative Humidity-Dependent Physical State of Organic Particulate Matter in the Uptake of Semivolatile Organic Molecules
	Han, Yuemei 3,4; Gong, Zhaoheng 4; Ye, Jianhuai 4; Liu, Pengfei 4; McKinney, Karena A.2,4; Martin, Scot T.1,4
刊名	ENVIRONMENTAL SCIENCE & TECHNOLOGY
	2019-11-19
卷号	53 期号:22 页码:13209-13218
ISSN号	0013-936X
DOI	10.1021/acs.est.9b05354
通讯作者	Han, Yuemei(yuemei.han@ieecas.cn) ; Martin, Scot T.(scot_martin@harvard.edu)
英文摘要	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.
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关键词	ALPHA-PINENE ; ATMOSPHERIC AEROSOLS ; DICARBOXYLIC-ACIDS ; ELEMENTAL ANALYSIS ; SOLID-STATE ; GAS UPTAKE ; PHASE ; VISCOSITY ; ISOPRENE ; SULFATE
WOS研究方向	Engineering ; Environmental Sciences & Ecology
语种	英语
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000498279400025
资助机构	Office of Science of the U.S. Department of Energy ; Division of Atmospheric and Geospace Sciences of the U.S. National Science Foundation
内容类型	期刊论文
源URL	[http://ir.ieecas.cn/handle/361006/13008]
专题	地球环境研究所_粉尘与环境研究室
通讯作者	Han, Yuemei; Martin, Scot T.
作者单位	1.Harvard Univ, Dept Earth & Planetary Sci, Cambridge, MA 02138 USA 2.Colby Coll, Dept Chem, Waterville, ME 04901 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.Harvard Univ, Sch Engn & Appl Sci, Cambridge, MA 02138 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.