Response of biogenic secondary organic aerosol formation to anthropogenic NOx emission mitigation

Zhizhao Wang; Florian Couvidat; Karine Sartelet

doi:10.1016/j.scitotenv.2024.172142

Response of biogenic secondary organic aerosol formation to anthropogenic NOx emission mitigation

Sci Total Environ. 2024 Jun 1:927:172142. doi: 10.1016/j.scitotenv.2024.172142. Epub 2024 Apr 6.

Authors

Zhizhao Wang¹, Florian Couvidat², Karine Sartelet³

Affiliations

¹ Centre d'Enseignement et de Recherche en Environnement Atmosphérique (CEREA), Ecole des Ponts ParisTech, EdF R&D, IPSL, Marne-la-Vallée 77455, Île-de-France, France; Institut National de l'Environnement Industriel et des Risques (INERIS), Verneuil-en-Halatte, 60550 Oise, France; Now at University of California, Riverside (UCR), Riverside 92521, CA, USA; Now at National Center for Atmospheric Research (NCAR), Boulder 80301, CO, USA. Electronic address: zhizhaow@ucr.edu.
² Institut National de l'Environnement Industriel et des Risques (INERIS), Verneuil-en-Halatte, 60550 Oise, France.
³ Centre d'Enseignement et de Recherche en Environnement Atmosphérique (CEREA), Ecole des Ponts ParisTech, EdF R&D, IPSL, Marne-la-Vallée 77455, Île-de-France, France.

PMID: 38583610
DOI: 10.1016/j.scitotenv.2024.172142

Abstract

This study investigates the effects of anthropogenic nitrogen oxide (NOx) mitigation reduction on secondary organic aerosol (SOA) formation from monoterpene and sesquiterpene precursors across Europe, using the three-dimensional (3-D) Chemical Transport Model (CTM) CHIMERE. Two SOA mechanisms of varying complexity are employed: the GENOA-generated Biogenic Mechanism (GBM) and the Hydrophobic/Hydrophilic Organic mechanism (H²O). GBM is a condensed SOA mechanism generated by automatic reduction from near-explicit chemical mechanisms (i.e., the Master Chemical Mechanism - MCM and the peroxy radical autoxidation mechanism - PRAM) using the GENerator of Reduced Organic Aerosol Mechanisms version 2.0 (GENOA v2.0). Conversely, the H²O mechanism is developed primarily based on experimental data, with simplified chemical pathways and SOA formation yields reflecting those from chamber experiments. In the 3-D simulations conducted for the summer of 2018 over Europe, the implementation of GBM significantly improved the model's performance in comparison to simulations using the H²O mechanism, yielding results more consistent with measured aerosol concentrations extracted from the EBAS database. In response to NOx emission mitigation, simulated SOA concentrations increase with GBM but decrease when using the H²O mechanism, unless a highly oxygenated molecules (HOMs) formation scheme is incorporated. The SOA composition becomes more oxidized and concentrations elevate after NOx reduction, particularly in simulations using GBM. These higher concentrations are likely due to enhanced reaction rates of organic peroxy radicals (RO₂) with HO₂, resulting in more oxidized products from monoterpene degradation that favors HOM formation. The results suggest that detailed SOA mechanisms including autoxidation are necessary for accurate predictions of SOA concentrations in 3-D modeling.

Keywords: Aerosol mechanism; Chemical transport modeling; Monoterpene SOA mechanism; NOx emission reduction; Sesquiterpene SOA mechanism.