DOI: 10.1016/j.atmosenv.2018.02.009
Scopus记录号: 2-s2.0-85041852074
论文题名: Temperature effects on multiphase reactions of organic molecular markers: A modeling study
作者: Pratap V ; , Chen Y ; , Yao G ; , Nakao S
刊名: Atmospheric Environment
ISSN: 0168-2563
EISSN: 1573-515X
出版年: 2018
卷: 179 起始页码: 40
结束页码: 48
语种: 英语
英文关键词: Biomass burning
; Diffusion coefficient
; Diffusivity
; Levoglucosan
; Low-temperature
; Markers
; Saturation concentration
; Winter
Scopus关键词: Atmospheric humidity
; Diffusion
; Humidity control
; Biomass-burning
; Levoglucosan
; Low temperatures
; Markers
; Saturation concentration
; Winter
; Temperature
; levoglucosan
; aerosol
; atmospheric modeling
; biomarker
; biomass burning
; concentration (composition)
; gas phase reaction
; heating
; low temperature
; oxidation
; partitioning
; relative humidity
; saturation
; source apportionment
; temperature effect
; winter
; Article
; biomass
; combustion
; heating
; humidity
; oxidation
; particle size
; priority journal
; temperature sensitivity
; vapor pressure
; wettability
; winter
; wood
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: Various molecular markers are used in source apportionment studies. In early studies, molecular markers were assumed to be inert. However, recent studies suggest that molecular markers can decay rapidly through multiphase reactions, which makes interpretation of marker measurements challenging. This study presents a simplified model to account for the effects of temperature and relative humidity on the lifetime of molecular markers through a shift in gas-particle partitioning as well as a change in viscosity of the condensed phase. As a model case, this study examines the stability of levoglucosan, a key marker species of biomass burning, over a wide temperature range relevant to summertime and wintertime. Despite the importance of wood combustion for space heating in winter, the lifetime of levoglucosan in wintertime is not well understood. The model predicts that in low-temperature conditions, levoglucosan predominantly remains in the particle phase, and therefore its loss due to gas-phase oxidation reactions is significantly reduced. Furthermore, the movement of the levoglucosan from the bulk of the particle to the particle surface is reduced due to low diffusivity in the semi-solid state. The simplified model developed in this study reasonably reproduces upper and lower bounds of the lifetime of levoglucosan investigated in previous studies. The model results show that the levoglucosan depletion after seven days reduces significantly from ∼98% at 25 °C to <1% at 0 °C under dry conditions. The depletion of levoglucosan increases at higher relative humidities. However, at temperatures below 0 °C, levoglucosan appears to be a useful marker (lifetime > 1 week) even at 60% relative humidity irrespective of the assumed fragility parameter D that controls estimated diffusivity. The model shows that lifetime of an organic molecular marker strongly depends on assumed D especially when a semi-volatile marker is in semi-solid organic aerosol. © 2018 Citation statistics:
资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/83001
Appears in Collections: 气候变化事实与影响
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作者单位: Department of Chemical and Biomolecular Engineering, Clarkson University, Potsdam, NY, United States; Department of Mathematics, Clarkson University, Potsdam, NY, United States
Recommended Citation:
Pratap V,, Chen Y,, Yao G,et al. Temperature effects on multiphase reactions of organic molecular markers: A modeling study[J]. Atmospheric Environment,2018-01-01,179