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

Pichelstorfer, Lukas ; Roldin, Pontus LU ; Rissanen, Matti ; Hyttinen, Noora ; Garmash, Olga ; Xavier, Carlton LU ; Zhou, Putian ; Clusius, Petri ; Foreback, Benjamin and Golin Almeida, Thomas , et al. (2024) In Environmental Science: Atmospheres 4(8). p.879-896
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... (More)

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.

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organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Environmental Science: Atmospheres
volume
4
issue
8
pages
18 pages
publisher
Royal Society of Chemistry
external identifiers
  • pmid:39130798
  • scopus:85198941130
ISSN
2634-3606
DOI
10.1039/d4ea00054d
language
English
LU publication?
yes
id
4a0590c5-0277-42b1-b5e9-b524acae87bd
date added to LUP
2024-09-13 15:27:27
date last changed
2024-10-11 20:20:31
@article{4a0590c5-0277-42b1-b5e9-b524acae87bd,
  abstract     = {{<p>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-NO<sub>x</sub> 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 NO<sub>3</sub> radical, is predicted by the model at dawn.</p>}},
  author       = {{Pichelstorfer, Lukas and Roldin, Pontus and Rissanen, Matti and Hyttinen, Noora and Garmash, Olga and Xavier, Carlton and Zhou, Putian and Clusius, Petri and Foreback, Benjamin and Golin Almeida, Thomas and Deng, Chenjuan and Baykara, Metin and Kurten, Theo and Boy, Michael}},
  issn         = {{2634-3606}},
  language     = {{eng}},
  number       = {{8}},
  pages        = {{879--896}},
  publisher    = {{Royal Society of Chemistry}},
  series       = {{Environmental Science: Atmospheres}},
  title        = {{Towards automated inclusion of autoxidation chemistry in models : from precursors to atmospheric implications}},
  url          = {{http://dx.doi.org/10.1039/d4ea00054d}},
  doi          = {{10.1039/d4ea00054d}},
  volume       = {{4}},
  year         = {{2024}},
}