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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Heterogeneous Ozone Oxidation Reactions of 1-Pentene, Cyclopentene, Cyclohexene, and a Menthenol Derivative Studied by Sum Frequency Generation
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Heterogeneous Ozone Oxidation Reactions of 1-Pentene, Cyclopentene, Cyclohexene, and a Menthenol Derivative Studied by Sum Frequency Generation

机译：通过求和频率生成研究1-戊烯，环戊烯，环己烯和薄荷醇衍生物的异质臭氧氧化反应

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摘要

We report vibrational sum frequency generation (SFG) spectra of glass surfaces functionalized with 1-pentene, 2-hexene, cyclopentene, cyclohexene, and a menthenol derivative. The heterogeneous reactions of ozone with hydrocarbons covalently linked to oxide surfaces serve as models for studying heterogeneous oxidation of biogenic terpenes adsorbed to mineral aerosol surfaces commonly found in the troposphere. Vibrational SFG is also used to track the C=C double bond oxidation reactions initiated by ozone in real time and to characterize the surface-bound product species. Combined with contact angle measurements carried out before and after ozonolysis, the kinetic and spectroscopic studies presented here suggest reaction pathways involving vibrationally hot Criegee intermediates that compete with pathways that involve thermalized surface species. Kinetic measurements suggest that the rate limiting step in the heterogeneous C=C double bond oxidation reactions is likely to be the formation of the primary ozonide. From the determination of the reactive uptake coefficients, we find that ozone molecules undergo between 100 and 10000 unsuccessful collisions with C=C double bonds before the reaction occurs. The magnitude of the reactive uptake coefficients for the cyclic and linear olefins studied here does not follow the corresponding gas-phase reactivities but rather correlates with the accessibility of the C=C double bonds at the surface.
机译：我们报告功能化的1-戊烯，2-己烯，环戊烯，环己烯和薄荷酚的玻璃表面的振动总频率生成（SFG）光谱。臭氧与共价连接到氧化物表面的碳氢化合物的异质反应充当模型，用于研究吸附在对流层中常见的矿物气溶胶表面的生物萜烯的异质氧化。振动SFG还用于实时跟踪由臭氧引发的C = C双键氧化反应，并表征表面结合的产物种类。结合臭氧分解之前和之后进行的接触角测量，此处介绍的动力学和光谱研究表明，反应路径涉及振动热的Criegee中间体，该中间体与涉及热化表面物种的途径竞争。动力学测量结果表明，异质C = C双键氧化反应中的限速步骤很可能是主要的臭氧化物的形成。通过确定反应性吸收系数，我们发现在发生反应之前，臭氧分子会与C = C双键发生100至10000次不成功的碰撞。在此研究的环状和线性烯烃的反应性吸收系数的大小不遵循相应的气相反应性，而是与C = C双键在表面的可及性相关。

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