Exploring the influence of particle phase in the ozonolysis of oleic and elaidic acid

Kohli, Ravleen Kaur; Reynolds, Ryan S.; Wilson, Kevin R.; Davies, James F.

doi:10.1080/02786826.2023.2226183

Cited by 10 publications

(6 citation statements)

References 83 publications

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“…1B, outlining the major components of the assembly. A number of studies utilizing a similar design have been recently published for liquid droplet and particle capture, 30,[35][36][37][38][39][40] and thus, we briey review the general construction of the OPSI and provide details on the specic components used. The OPSI design consists of a PEEK 3-way tee connected to a stainless 1/8 ′′ tube on the top port.…”

Section: Open-port Sampling Interface (Opsi) Mass Spectrometrymentioning

confidence: 99%

Iodide oxidation by ozone at the surface of aqueous microdroplets

Prophet,

Polley,

Van Berkel

et al. 2024

Chem. Sci.

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Section: Open-port Sampling Interface (Opsi) Mass Spectrometrymentioning

confidence: 99%

Iodide oxidation by ozone at the surface of aqueous microdroplets

Prophet,

Polley,

Van Berkel

et al. 2024

Chem. Sci.

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“…1B, outlining the major components of the assembly. A number of studies utilizing a similar design have been recently published for liquid droplet and particle capture, 28,[33][34][35][36][37][38] and thus, we briefly review the general construction of the OPSI and provide details on the specific components used.…”

Section: B Open-port Sampling Interface (Opsi) Mass Spectrometrymentioning

confidence: 99%

Iodide Ozonolysis at the Surface of Aqueous Microdroplets

Prophet,

Polley,

Van Berkel

et al. 2023

Preprint

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The ozonolysis of iodide occurs at the sea-surface and within sea-spray aerosol, influencing the overall ozone budget in the marine boundary layer and leading to the emission of reactive halogen gases. A detailed account of the surface mechanism has proven elusive, however, due to the difficulty in quantifying multiphase kinetics. To obtain a clearer understanding of this reaction mechanism at the air-water interface, we report pH-dependent ozonolysis kinetics of I- in single levitated microdroplets as a function of [O3] using a quadrupole electrodynamic trap and an open port sampling interface for mass spectrometry. A kinetic model, constrained by molecular simulations of O3 dynamics at the air-water interface, is used to understand the coupled diffusive, reactive, and evaporative pathways at the microdroplet surface, which exhibit a strong dependence on bulk solution pH. Under acidic conditions, the surface reaction is limited by O3 diffusion in the gas phase, whereas under basic conditions the reaction becomes rate limited on the surface. The pH dependence also suggests the existence of a reactive intermediate IOOO- as has previously been observed in the ozonolysis of Br-. Expressions for steady-state surface concentrations of reactants are derived and utilized to directly compute uptake coefficients for this system, allowing for an exploration of uptake dependence on reactant concentration. In the present experiments, reactive uptake coefficients of O3 scale weakly with bulk solution pH, increasing from 4×10-4 to 2×10-3 with decreasing solution pH from pH 13 to pH 3.

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“…The discrepancy in the atmospheric chemical lifetimes of COA/corresponding marker compounds and estimations of the corresponding values by laboratory experiments have been discussed for a few decades (Robinson et al, 2006;Rudich et al, 2007;Weitkamp et al, 2008;Wang and Yu, 2021). Atmospheric chemical lifetimes of oleic and linoleic acids estimated by laboratory experiments are typically in the order of minutes (Morris et al, 2002;Knopf et al, 2005;Hung and Tang, 2010;Liu et al, 2023). On the other hand, a field observation in Los Angeles, USA suggested that the atmospheric chemical lifetime of oleic acid was much longer than the time scale (Rogge et al, 1991;Zahardis and Petrucci, 2007).…”

mentioning

confidence: 99%

“…The discrepancy among the field and laboratory chemical lifetimes of COA markers has typically been associated with chemical composition of COA (Rudich et al, 2007). Namely, mixing of saturated fatty acids from cooking such as stearic and palmitic acids makes COA to be highly viscous or solid at room temperature, reducing chemical reactivity (Knopf et al, 2005).…”

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confidence: 99%

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Suppressed atmospheric chemical aging of cooking organic aerosol particles in wintertime conditions

Liu,

He,

Liu

et al. 2023

Preprint

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Abstract. Cooking organic aerosol (COA) is one of the major constituents of particulate matter in urban areas. COA is oxidized by atmospheric oxidants such as ozone, changing its physical, chemical and toxicological properties. However, atmospheric chemical lifetimes of COA and its tracers such as oleic acid are typically longer than that have been estimated by laboratory studies. We tackled the issue by considering temperature. Namely, we hypothesize that increased viscosity of COA at ambient temperature accounts for its prolonged atmospheric chemical lifetimes in wintertime. Laboratory generated COA particles from cooking oil were exposed to ozone in an aerosol flow tube reactor for the temperature range of -20 °C ~ 35 °C. The pseudo-second order chemical reaction rate constants (k2) decreased by orders of magnitude for lower temperatures. The temperature dependence of k2 was fit well by considering diffusion-limited chemical reaction mechanism, suggesting that reduced viscosity was responsible for the decrease in chemical reactivity. In combination with the observed global surface temperature, the atmospheric chemical lifetimes of COA were estimated to be much longer in wintertime (>1 hour) than that in summertime (a few minutes) for temperate and boreal regions. Our present study demonstrates that the oxidation lifetimes of COA particles will need to be parameterized as a function of temperature in the future for estimating environmental impacts and fates of this category of particulate matter.

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Exploring the influence of particle phase in the ozonolysis of oleic and elaidic acid

Cited by 10 publications

References 83 publications

Iodide oxidation by ozone at the surface of aqueous microdroplets

Iodide oxidation by ozone at the surface of aqueous microdroplets

Iodide Ozonolysis at the Surface of Aqueous Microdroplets

Suppressed atmospheric chemical aging of cooking organic aerosol particles in wintertime conditions

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