GSTDTAP  > 地球科学
DOI10.5194/acp-18-14539-2018
Heterogeneous OH oxidation of secondary brown carbon aerosol
Schnitzler, Elijah G.; Abbatt, Jonathan P. D.
2018-10-11
发表期刊ATMOSPHERIC CHEMISTRY AND PHYSICS
ISSN1680-7316
EISSN1680-7324
出版年2018
卷号18期号:19页码:14539-14553
文章类型Article
语种英语
国家Canada
英文摘要

Light-absorbing organic aerosol, or brown carbon (BrC), has significant but poorly constrained effects on climate; for example, oxidation in the atmosphere may alter its optical properties, leading to absorption enhancement or bleaching. Here, we investigate for the first time the effects of heterogeneous OH oxidation on the optical properties of a laboratory surrogate of aqueous, secondary BrC in a series of photo-oxidation chamber experiments. The BrC surrogate was generated from aqueous resorcinol, or 1,3-dihydroxybenzene, and H2O2 exposed to > 300 nm radiation that is atomized, passed through trace gas denuders, and injected into the chamber, which was conditioned to either 15 % or 60 % relative humidity (RH). Aerosol absorption and scattering coefficients and single scattering albedo (SSA) at 405 nm were measured using a photoacoustic spectrometer. At 60 % RH, upon OH exposure, absorption first increased, and the SSA decreased sharply. Subsequently, absorption decreased faster than scattering, and SSA increased gradually. Comparisons to the modelled trend in SSA, based on Mie theory calculations, confirm that the observed trend is due to chemical evolution, rather than slight changes in particle size. The initial absorption enhancement is likely due to molecular functionalization and/or oligomerization and the bleaching to fragmentation. By contrast, at 15 % RH, slow absorption enhancement was observed without appreciable bleaching. A multi-layer kinetics model, consisting of two surface reactions in series, was constructed to provide further insights regarding the RH dependence of the optical evolution. Candidate parameters suggest that the oxidation is efficient, with uptake coefficients on the order of unity. The parameters also suggest that, as RH decreases, reactivity decreases and aerosol viscosity increases, such that particles are well-mixed at 60 % RH but not at 15 % RH. These results further the current understanding of the complex processing of BrC that may occur in the atmosphere.


领域地球科学
收录类别SCI-E
WOS记录号WOS:000447008300001
WOS关键词GAS-PARTICLE INTERACTIONS ; BIOMASS BURNING PARTICLES ; CHARGE-TRANSFER COMPLEXES ; KINETIC-MODEL FRAMEWORK ; CLOUD SURFACE-CHEMISTRY ; AQUEOUS-PHASE REACTIONS ; AIR-WATER-INTERFACE ; DOUBLE-LAYER MODEL ; LIGHT-ABSORPTION ; ORGANIC AEROSOL
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/30672
专题地球科学
作者单位Univ Toronto, Dept Chem, Toronto, ON M5S 3H6, Canada
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GB/T 7714
Schnitzler, Elijah G.,Abbatt, Jonathan P. D.. Heterogeneous OH oxidation of secondary brown carbon aerosol[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2018,18(19):14539-14553.
APA Schnitzler, Elijah G.,&Abbatt, Jonathan P. D..(2018).Heterogeneous OH oxidation of secondary brown carbon aerosol.ATMOSPHERIC CHEMISTRY AND PHYSICS,18(19),14539-14553.
MLA Schnitzler, Elijah G.,et al."Heterogeneous OH oxidation of secondary brown carbon aerosol".ATMOSPHERIC CHEMISTRY AND PHYSICS 18.19(2018):14539-14553.
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