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DOI | 10.5194/acp-19-2433-2019 |
Heterogeneous OH oxidation of isoprene-epoxydiol-derived organosulfates: kinetics, chemistry and formation of inorganic sulfate | |
Lam, Hoi Ki1; Kwong, Kai Chung1; Poon, Hon Yin1; Davies, James F.2; Zhang, Zhenfa3; Gold, Avram3; Surratt, Jason D.3; Chan, Man Nin1,4 | |
2019-02-26 | |
发表期刊 | ATMOSPHERIC CHEMISTRY AND PHYSICS |
ISSN | 1680-7316 |
EISSN | 1680-7324 |
出版年 | 2019 |
卷号 | 19期号:4页码:2433-2440 |
文章类型 | Article |
语种 | 英语 |
国家 | Peoples R China; USA |
英文摘要 | Acid-catalyzed multiphase chemistry of epoxydiols formed from isoprene oxidation yields the most abundant organosulfates (i.e., methyltetrol sulfates) detected in atmospheric fine aerosols in the boundary layer. This potentially determines the physicochemical properties of fine aerosols in isoprene-rich regions. However, chemical stability of these organosulfates remains unclear. As a result, we investigate the heterogeneous oxidation of aerosols consisting of potassium 3-methyltetrol sulfate ester (C5H11SO7K) by gas-phase hydroxyl (OH) radicals at a relative humidity (RH) of 70.8 %. Real-time molecular composition of the aerosols is obtained by using a Direct Analysis in Real Time (DART) ionization source coupled to a high-resolution mass spectrometer. Aerosol mass spectra reveal that 3-methyltetrol sulfate ester can be detected as its anionic form (C5H11SO7-) via direct ionization in the negative ionization mode. Kinetic measurements reveal that the effective heterogeneous OH rate constant is measured to be 4.74 +/- 0.2 x 10(-13) cm(3) molecule(-1) s(-1) with a chemical lifetime against OH oxidation of 16.2 +/- 0.3 days, assuming an OH radical concentration of 1.5 x 10(6) molecules cm(-3). Comparison of this lifetime with those against other aerosol removal processes, such as dry and wet deposition, suggests that 3-methyltetrol sulfate ester is likely to be chemically stable over atmospheric timescales. Aerosol mass spectra only show an increase in the intensity of bisulfate ion (HSO4-) after oxidation, suggesting the importance of fragmentation processes. Overall, potassium 3-methyltetrol sulfate ester likely decomposes to form volatile fragmentation products and aqueous-phase sulfate radial anion (SO4 center dot-). SO4 center dot- subsequently undergoes intermolecular hydrogen abstraction to form HSO4-. These processes appear to explain the compositional evolution of 3-methyltetrol sulfate ester during heterogeneous OH oxidation. |
领域 | 地球科学 |
收录类别 | SCI-E |
WOS记录号 | WOS:000459731300001 |
WOS关键词 | ORGANIC AEROSOL FORMATION ; 2013 SOUTHERN OXIDANT ; SPECTROMETRY DART-MS ; REACTIVE UPTAKE ; MASS-SPECTROMETRY ; RATE CONSTANTS ; PHASE STATE ; RADICALS ; HYDROCARBONS ; PARTICLES |
WOS类目 | Environmental Sciences ; Meteorology & Atmospheric Sciences |
WOS研究方向 | Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://119.78.100.173/C666/handle/2XK7JSWQ/30584 |
专题 | 地球科学 |
作者单位 | 1.Chinese Univ Hong Kong, Fac Sci, Earth Syst Sci Programme, Hong Kong, Peoples R China; 2.UC Riverside, Dept Chem, Riverside, CA USA; 3.Univ N Carolina, Gillings Sch Global Publ Hlth, Dept Environm Sci & Engn, Chapel Hill, NC 27515 USA; 4.Chinese Univ Hong Kong, Inst Environm Energy & Sustainabil, Hong Kong, Peoples R China |
推荐引用方式 GB/T 7714 | Lam, Hoi Ki,Kwong, Kai Chung,Poon, Hon Yin,et al. Heterogeneous OH oxidation of isoprene-epoxydiol-derived organosulfates: kinetics, chemistry and formation of inorganic sulfate[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2019,19(4):2433-2440. |
APA | Lam, Hoi Ki.,Kwong, Kai Chung.,Poon, Hon Yin.,Davies, James F..,Zhang, Zhenfa.,...&Chan, Man Nin.(2019).Heterogeneous OH oxidation of isoprene-epoxydiol-derived organosulfates: kinetics, chemistry and formation of inorganic sulfate.ATMOSPHERIC CHEMISTRY AND PHYSICS,19(4),2433-2440. |
MLA | Lam, Hoi Ki,et al."Heterogeneous OH oxidation of isoprene-epoxydiol-derived organosulfates: kinetics, chemistry and formation of inorganic sulfate".ATMOSPHERIC CHEMISTRY AND PHYSICS 19.4(2019):2433-2440. |
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