Issue 8, 2024

Towards automated inclusion of autoxidation chemistry in models: from precursors to atmospheric implications

Abstract

In the last few decades, atmospheric formation of secondary organic aerosols (SOA) has gained increasing attention due to their impact on air quality and climate. However, methods to predict their abundance are mainly empirical and may fail under real atmospheric conditions. In this work, a close-to-mechanistic approach allowing SOA quantification is presented, with a focus on a chain-like chemical reaction called “autoxidation”. A novel framework is employed to (a) describe the gas-phase chemistry, (b) predict the products' molecular structures and (c) explore the contribution of autoxidation chemistry on SOA formation under various conditions. As a proof of concept, the method is applied to benzene, an important anthropogenic SOA precursor. Our results suggest autoxidation to explain up to 100% of the benzene-SOA formed under low-NOx laboratory conditions. Under atmospheric-like day-time conditions, the calculated benzene-aerosol mass continuously forms, as expected based on prior work. Additionally, a prompt increase, driven by the NO3 radical, is predicted by the model at dawn. This increase has not yet been explored experimentally and stresses the potential for atmospheric SOA formation via secondary oxidation of benzene by O3 and NO3.

Graphical abstract: Towards automated inclusion of autoxidation chemistry in models: from precursors to atmospheric implications

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Article information

Article type
Paper
Submitted
29 Apr 2024
Accepted
08 Jul 2024
First published
09 Jul 2024
This article is Open Access
Creative Commons BY license

Environ. Sci.: Atmos., 2024,4, 879-896

Towards automated inclusion of autoxidation chemistry in models: from precursors to atmospheric implications

L. Pichelstorfer, P. Roldin, M. Rissanen, N. Hyttinen, O. Garmash, C. Xavier, P. Zhou, P. Clusius, B. Foreback, T. Golin Almeida, C. Deng, M. Baykara, T. Kurten and M. Boy, Environ. Sci.: Atmos., 2024, 4, 879 DOI: 10.1039/D4EA00054D

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