DOI: 10.1016/j.atmosenv.2018.03.021
Scopus记录号: 2-s2.0-85043987608
论文题名: Formation of aqueous-phase secondary organic aerosols from glycolaldehyde and ammonium sulfate/amines: A kinetic and mechanistic study
作者: Yi Y ; , Cao Z ; , Zhou X ; , Xue L ; , Wang W
刊名: Atmospheric Environment
ISSN: 0168-2563
EISSN: 1573-515X
出版年: 2018
卷: 181 起始页码: 117
结束页码: 125
语种: 英语
英文关键词: Amine
; Ammonium sulfate
; Aqueous-phase SOA
; Glycolaldehyde
; Laboratory simulation reaction
Scopus关键词: Aerosols
; Amines
; Amino acids
; Chemical reactions
; Electromagnetic wave absorption
; Ketones
; Light absorption
; Mixtures
; Nitrogen compounds
; Phase interfaces
; Rate constants
; Sulfur compounds
; Ammonium Sulfate
; Aqueous phase
; Atmospheric particles
; First order kinetics
; Glycolaldehydes
; Laboratory simulation
; Reactant concentrations
; Secondary organic aerosols
; Atmospheric aerosols
; aerosol formation
; aldehyde
; aqueous solution
; chemical compound
; concentration (composition)
; kinetics
; laboratory method
; sulfate
Scopus学科分类: Environmental Science: Water Science and Technology
; Earth and Planetary Sciences: Earth-Surface Processes
; Environmental Science: Environmental Chemistry
英文摘要: Atmospheric particles are largely represented by secondary organic aerosols (SOAs) produced by either aqueous- or gas-phase reactions. Recently, the contribution of the former to SOA formation has been shown to substantially increase and even reach that of the latter, which necessitates in-depth mechanistic investigations. For a deeper understanding of aqueous-phase SOA generation, we herein studied the production of these aerosols in the dark from glycolaldehyde (GAld) and ammonium sulfate (AS)/amines (methylamine (MAm) and glycine (Gly)). UV–vis spectroscopy showed that reaction mixtures featured two main absorption bands (at 209–230 and 280–330 nm) that were attributed to the π–π* transitions of Schiff bases and the n–π* transitions of oligomers produced in the above reactions, respectively. Further studies revealed that irrespective of reactant concentration and pH, all the investigated reactions were well fitted by first-order kinetics and were accelerated by increasing AS/MAm concentrations and solution pH under acidic conditions. The reaction rate constants (determined from changes of absorption at 300 nm) followed the order of Gly (kI = 2.39 × 10−6 s−1) > MAm (kI = 1.19 × 10−6 s−1) > AS (kI = 8.33 × 10−7 s−1) at identical low AS/amine concentrations and were in the order of MAm (kI = 2.5 × 10−6 s−1) > AS (kI = 1.39 × 10−6 s−1) at high AS/MAm concentrations. The main reaction pathways corresponded to the aldol self-condensation of GAld and the nucleophilic attack of AS/amines on GAld followed by dehydration, which afforded imines as the major products. The stronger light absorption of (GAld + Gly) mixtures than that of (glyoxal/methylglyoxal + Gly) mixtures was ascribed to the increased amount of imine- and carbonyl group-containing products produced in the former case. © 2018 Elsevier Ltd Citation statistics:
资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/82924
Appears in Collections: 气候变化事实与影响
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作者单位: Environment Research Institute, Shandong University, Jinan, China
Recommended Citation:
Yi Y,, Cao Z,, Zhou X,et al. Formation of aqueous-phase secondary organic aerosols from glycolaldehyde and ammonium sulfate/amines: A kinetic and mechanistic study[J]. Atmospheric Environment,2018-01-01,181