Reactivity of oleic acid in organic particles: changes in oxidant uptake and reaction stoichiometry with particle oxidation

Literature Information

Publication Date 2009-07-07
DOI 10.1039/B904285G
Impact Factor 3.676
Authors

Amy M. Sage, Emily A. Weitkamp, Allen L. Robinson, Neil M. Donahue


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Abstract

The heterogeneous reaction of ozone with oleic acid has been studied extensively as a simple model system for investigating the oxidation of organic compounds in atmospheric particles. In this work, we simultaneously quantify oleic acid and ozone decay during three stepwise oxidation events, allowing us to quantify reactivity of oleic acid throughout the oxidative lifetime of initially pure particles. Throughout their lifetime, uptake in these particles is driven by reaction, as evidenced by similar timescales for ozone and oleic acid decay. The oleic acid decay rate slows with increasing particle oxidation, most likely due to the continued dilution of the particles with oxidation products. However, the initial stoichiometry is as high as 3.75 oleic acid molecules destroyed per ozone molecule lost. This significantly exceeds the 2 : 1 ratio that can be explained by an initial ozonolysis reaction and known secondary chemistry between the Criegee intermediate and the organic acid moiety. It implies that there is additional, previously unrecognized secondary chemistry that likely involves the carbon backbone. Our understanding of reactivity, even in this simple system, remains incomplete.

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Source Journal

Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
Self-citation Rate: 10.3%
Articles per Year: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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