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• W4386770151 abstract "<strong class=journal-contentHeaderColor>Abstract.</strong> Siloxanes are composed of silicon, oxygen, and alkyl groups and are emitted from consumer chemicals. Despite being entirely anthropogenic, siloxanes are being detected in remote regions and are ubiquitous in indoor and urban environments. Decamethylcyclopentasiloxane (D₅) is one of the most common cyclic congeners, and smog chamber and oxidation flow reactor (OFR) experiments have found D₅ + OH to form secondary organosiloxane aerosol (SOSiA). However, there is uncertainty about the reaction products, and the reported SOSiA mass yields (<em>Y</em>_SOSiA) appear inconsistent. To quantify small volatile oxidation products (VOP) and to consolidate the <em>Y</em>_SOSiA in the literature, we performed experiments using a Potential Aerosol Mass OFR while varying D₅ concentration, humidity, and OH exposure (OH_exp). We use a proton transfer reaction time-of-flight mass spectrometer to quantify D₅, HCHO, and HCOOH, and detect other VOP, which we tentatively identify as siloxanols and siloxanyl formates. We determine molar yields of HCHO and HCOOH between 52 – 211 % and 45 – 127 %, respectively. With particle size distributions measured with a scanning mobility particle sizer, we find <em>Y</em>_SOSiA to be < 10 % at OH_exp < 1.3 × 10¹¹ s cm^-3 and ~20 % at OH_exp corresponding to that of the lifetime of D₅ at atmospheric OH concentrations. We also find that <em>Y</em>_SOSiA is dependent on both organic aerosol mass loading and OH_exp. We use a kinetic box model of SOSiA formation and aging (aging-VBS model) to reconcile the <em>Y</em>_SOSiA values found in this study and the literature. The model uses a volatility basis set (VBS) of the primary oxidation products as well as an aging rate coefficient in the gas phase, <em>k</em>_age,gas, of 2.17 × 10^-11 cm³ s^-1, and an aging rate coefficient in the particle phase, <em>k</em>_age,particle, which is ten times smaller. The combination of primary VBS and OH-dependent oxidative aging predicts SOSiA formation much better than a standard-VBS parameterization that does not consider aging (R² = 0.970 vs. 0.847). The need for an ageing-dependent parameterization to accurately model SOSiA formation shows that concepts developed for secondary organic aerosol precursors, which are able to form low-volatile products at low OH_exp, do not necessarily apply to D₅ + OH. The resulting yields of HCHO and HCOOH and the parameterization of <em>Y</em>_SOSiA may be used in larger scale models to assess the implications of siloxanes on air quality." @default.
• W4386770151 created "2023-09-16" @default.
• W4386770151 creator A5092877954 @default.
• W4386770151 date "2023-09-15" @default.
• W4386770151 modified "2023-09-26" @default.
• W4386770151 title "Reply on RC2" @default.
• W4386770151 doi "https://doi.org/10.5194/egusphere-2023-1033-ac2" @default.
• W4386770151 hasPublicationYear "2023" @default.
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