Atmospheric photooxidation and ozonolysis of sabinene: reaction rate coefficients, product yields, and chemical budget of radicals

化学 臭氧分解 萨比宁 产量(工程) 激进的 甲醛 丙酮 反应速率常数 臭氧 反应速率 阿累尼乌斯方程 分析化学(期刊) 光化学 物理化学 热力学 有机化学 活化能 动力学 催化作用 物理 色谱法 量子力学 精油 柠檬烯
作者
Jacky Y. S. Pang,Florian Berg,Anna Novelli,Birger Bohn,Michelle Färber,Philip T. M. Carlsson,René Dubus,Georgios I. Gkatzelis,Franz Röhrer,Sergej Wedel,Andreas Wahner,Hendrik Fuchs
出处
期刊:Atmospheric Chemistry and Physics [Copernicus Publications]
卷期号:23 (19): 12631-12649 被引量:1
标识
DOI:10.5194/acp-23-12631-2023
摘要

Abstract. The oxidation of sabinene by the hydroxyl radical (OH) and ozone (O3) was investigated under atmospherically relevant conditions in the atmospheric simulation chamber SAPHIR (Simulation of Atmospheric Photochemistry In a Large Reaction Chamber) at Forschungszentrum Jülich, Germany. The rate coefficients of the reactions of sabinene with OH and with O3 were determined. The temperature dependence between 284 to 340 K of the rate coefficient of the reaction of sabinene with OH, kSAB+OH, was measured for the first time using an OH reactivity instrument, resulting in an Arrhenius expression of (1.67 ± 0.16) × 10−11 × exp((575 ± 30)/T) cm3 s−1. The values agree with those determined in chamber experiments in this work and reported in the literature for ∼ 298 K within the uncertainties of measurements. The ozonolysis reaction rate coefficient of sabinene (kSAB+O3) determined in chamber experiments at a temperature of (278 ± 2) K is (3.4 ± 0.8) × 10−17 cm3 s−1, which is 58 % lower than the value reported in the literature for room temperature. The measurement of products from the oxidation of sabinene by OH resulted in an acetone yield of (21 ± 15) %, a formaldehyde yield of (46 ± 25) %, and a sabinaketone yield of (18 ± 16) %. All yields determined in the chamber experiments agree well with values from previous laboratory studies within their uncertainties. In addition, the formaldehyde yield determined in this study is consistent with that predicted by the sabinene OH-oxidation mechanism which was devised from quantum chemical calculations by Wang and Wang (2018), whereas the acetone yield is about 15 % higher than that predicted by the mechanism. In the ozonolysis experiments, the analysis of product measurements results in an acetone yield of (5 ± 2) %, a formaldehyde yield of (48 ± 15) %, a sabinaketone yield of (31 ± 15) %, and an OH radical yield of (26 ± 29) %. The OH radical yield is lower than expected from the theoretical mechanism in Wang and Wang (2017), but the value still agrees within the uncertainty. An analysis of the chemical budget of OH radicals was performed for the chamber experiments. The analysis reveals that the destruction rate of the OH radical matches the production rate of OH, suggesting that there is no significant missing OH source for example from isomerization reactions of peroxy radicals for the experimental conditions in this work.
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