Secondary Organic Aerosol (SOA) from Photo-Oxidation of Toluene: 1 Influence of Reactive Nitrogen, Acidity and Water Vapours on Optical Properties

oleh: Kalyan Mitra, Harsh Raj Mishra, Xiangyu Pei, Ravi Kant Pathak

Format: Article
Diterbitkan: MDPI AG 2022-07-01

Deskripsi

Many climate models treat the light-absorbing SOA component called “brown carbon” (BrC) as non-light absorbing because its formation and transformations are poorly understood. We therefore investigated the influence of reactive nitrogen (NO<sub>x</sub>, NH<sub>3</sub>)-, acidity (H<sub>2</sub>SO<sub>4</sub>)-, and water-mediated chemistry on SOA formed by the photo-oxidation of toluene, the subsequent formation and transformation of BrC, and its optical properties. We discovered that nitrogen-poor (NP) SOA is formed when the molar ratio of NO<sub>x</sub> to reacted toluene (henceforth, [NO<sub>x</sub>/ΔHC]) is 0.15 or less, whereas nitrogen-rich (NR) SOA is formed when [NO<sub>x</sub>/ΔHC] > 0.15. NR and NP SOA have markedly different characteristics. The light absorption coefficient (B<sub>abs</sub>) and mass absorption cross-section (MAC) of the SOA increased with [NO<sub>x</sub>/ΔHC] under both the NP and NR regimes. For NP SOA, the MAC increased with [NO<sub>x</sub>/ΔHC] independently of the relative humidity (RH). However, the MAC of NR SOA was RH-dependent. Under both NP and NR regimes, acidity promoted SOA browning while NH<sub>3</sub> increased B<sub>abs</sub> and MAC at 80% RH. The highest MAC was observed at the lowest RH (20%) for acidic NR SOA, and it was postulated that the MAC of SOA depends mainly on the pH and the [H<sup>+</sup>]<sub>free</sub>/[SOA mass] ratio of the aqueous SOA phase.