Chemical ageing and transformation of diffusivity in semi-solid multi-component organic aerosol particles

Recent experimental evidence underlines the importance of reduced diffusivity in amorphous semi-solid or glassy atmospheric aerosols. This paper investigates the impact of diffusivity on the ageing of multi-component reactive organic particles approximating atmospheric cooking aerosols. We apply and...

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Main Authors: C. Pfrang, M. Shiraiwa, U. Pöschl
Format: Article
Language:English
Published: Copernicus Publications 2011-07-01
Series:Atmospheric Chemistry and Physics
Online Access:http://www.atmos-chem-phys.net/11/7343/2011/acp-11-7343-2011.pdf
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author C. Pfrang
M. Shiraiwa
U. Pöschl
author_facet C. Pfrang
M. Shiraiwa
U. Pöschl
author_sort C. Pfrang
collection DOAJ
description Recent experimental evidence underlines the importance of reduced diffusivity in amorphous semi-solid or glassy atmospheric aerosols. This paper investigates the impact of diffusivity on the ageing of multi-component reactive organic particles approximating atmospheric cooking aerosols. We apply and extend the recently developed KM-SUB model in a study of a 12-component mixture containing oleic and palmitoleic acids. We demonstrate that changes in the diffusivity may explain the evolution of chemical loss rates in ageing semi-solid particles, and we resolve surface and bulk processes under transient reaction conditions considering diffusivities altered by oligomerisation. This new model treatment allows prediction of the ageing of mixed organic multi-component aerosols over atmospherically relevant timescales and conditions. We illustrate the impact of changing diffusivity on the chemical half-life of reactive components in semi-solid particles, and we demonstrate how solidification and crust formation at the particle surface can affect the chemical transformation of organic aerosols.
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spelling doaj.art-7bf5178db03c4e82a6269cebca69fcf42022-12-21T17:44:50ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242011-07-0111147343735410.5194/acp-11-7343-2011Chemical ageing and transformation of diffusivity in semi-solid multi-component organic aerosol particlesC. PfrangM. ShiraiwaU. PöschlRecent experimental evidence underlines the importance of reduced diffusivity in amorphous semi-solid or glassy atmospheric aerosols. This paper investigates the impact of diffusivity on the ageing of multi-component reactive organic particles approximating atmospheric cooking aerosols. We apply and extend the recently developed KM-SUB model in a study of a 12-component mixture containing oleic and palmitoleic acids. We demonstrate that changes in the diffusivity may explain the evolution of chemical loss rates in ageing semi-solid particles, and we resolve surface and bulk processes under transient reaction conditions considering diffusivities altered by oligomerisation. This new model treatment allows prediction of the ageing of mixed organic multi-component aerosols over atmospherically relevant timescales and conditions. We illustrate the impact of changing diffusivity on the chemical half-life of reactive components in semi-solid particles, and we demonstrate how solidification and crust formation at the particle surface can affect the chemical transformation of organic aerosols.http://www.atmos-chem-phys.net/11/7343/2011/acp-11-7343-2011.pdf
spellingShingle C. Pfrang
M. Shiraiwa
U. Pöschl
Chemical ageing and transformation of diffusivity in semi-solid multi-component organic aerosol particles
Atmospheric Chemistry and Physics
title Chemical ageing and transformation of diffusivity in semi-solid multi-component organic aerosol particles
title_full Chemical ageing and transformation of diffusivity in semi-solid multi-component organic aerosol particles
title_fullStr Chemical ageing and transformation of diffusivity in semi-solid multi-component organic aerosol particles
title_full_unstemmed Chemical ageing and transformation of diffusivity in semi-solid multi-component organic aerosol particles
title_short Chemical ageing and transformation of diffusivity in semi-solid multi-component organic aerosol particles
title_sort chemical ageing and transformation of diffusivity in semi solid multi component organic aerosol particles
url http://www.atmos-chem-phys.net/11/7343/2011/acp-11-7343-2011.pdf
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AT uposchl chemicalageingandtransformationofdiffusivityinsemisolidmulticomponentorganicaerosolparticles