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Preprints
https://doi.org/10.5194/acp-2020-461
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2020-461
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.

  02 Jun 2020

02 Jun 2020

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This preprint is currently under review for the journal ACP.

Influence of aromatics on tropospheric gas-phase composition

Domenico Taraborrelli1, David Cabrera-Perez2, Sara Bacer2,a, Sergey Gromov2, Jos Lelieveld2, Rolf Sander2, and Andrea Pozzer2,3 Domenico Taraborrelli et al.
  • 1Institute of Energy and Climate Research (IEK-8), Forschungszentrum Jülich GmbH, 52425 Jülich, Germany
  • 2Atmospheric Chemistry Department, Max-Planck Institute of Chemistry, Hahn-Meitner-Weg 1, 55128 Mainz, Germany
  • 3International Centre for Theoretical Physics, 34100 Trieste, Italy
  • anow at: Université Grenoble Alpes, CNRS, Grenoble INP, LEGI, 38000 Grenoble, France

Abstract. Aromatics contribute a significant fraction to organic compounds in the troposphere and are mainly emitted by anthropogenic activities and biomass burning. Their oxidation in lab experiments is known to lead to the formation of ozone and aerosol precursors. However, their overall impact on tropospheric composition is uncertain as it depends on transport, multiphase chemistry, and removal processes of the oxidation intermediates. Representation of aromatics in global atmospheric models has been either neglected or highly simplified. Here, we present an assessment of their impact on the gas-phase chemistry, using the general circulation model EMAC (ECHAM5/MESSy Atmospheric Chemistry). We employ a comprehensive kinetic model to represent the oxidation of the following monocyclic aromatics: benzene, toluene, xylenes, phenol, styrene, ethylbenzene, trimethylbenzenes, benzaldehyde, and lumped higher aromatics that contain more than 9 C atoms.

Significant regional changes are identified for several species. For instance, glyoxal increases by 130 % in Europe and 260 % in East Asia, respectively. Large increases in HCHO are also predicted in these regions. In general, the influence of aromatics is particularly evident in areas with high concentrations of NOx, with increases up to 12 % in O3 and 17 % in OH.

On a global scale, the estimated net changes are minor when aromatic compounds are included in our model. For instance, the tropospheric burden of CO increases by about 6 %, while the burdens of OH, O3, and NOx (NO + NO2) decrease between 3 % and 9 %. The global mean changes are small, partially because of compensating effects between high- and low-NOx regions. The largest change is predicted for the important aerosol precursor glyoxal, which increases globally by 36 %. In contrast to other studies, the net change in tropospheric ozone is predicted to be negative, −3 % globally. This change is larger in the northern hemisphere where global models usually show positive biases. We find that the reaction with phenoxy radicals is a significant loss for ozone, of the order of 200–300 Tg/yr, which is similar to the estimated ozone loss due to bromine chemistry.

Although the net global impact of aromatics is limited, our results indicate that aromatics can strongly influence tropospheric chemistry on a regional scale, most significantly in East Asia. An analysis of the main model uncertainties related to oxidation and emissions suggests that the impact of aromatics may even be significantly larger.

Domenico Taraborrelli et al.

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Domenico Taraborrelli et al.

Domenico Taraborrelli et al.

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Latest update: 11 Aug 2020
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Short summary
Atmospheric pollutants from anthropogenic activities and biomass burning are usually regarded as ozone precursors. Monocyclic aromatics are no exception. Calculations with a comprehensive atmospheric model are consistent with this view but only for air masses close to pollution source regions. However, the same model predicts that aromatics, when transported to remote areas, may effectively destroy ozone. This loss of tropospheric ozone rivals the one attributed to bromine.
Atmospheric pollutants from anthropogenic activities and biomass burning are usually regarded as...
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