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Structure-dependent reactivity of Criegee intermediates studied with spectroscopic methods
Chemical Society Reviews ( IF 46.2 ) Pub Date : 2017-08-25 00:00:00 , DOI: 10.1039/c7cs00336f
Jim Jr-Min Lin,Wen Chao

Criegee intermediates are very reactive carbonyl oxides that are formed in reactions of unsaturated hydrocarbons with ozone (ozonolysis). Recently, Criegee intermediates have gained significant attention since a new preparation method has been reported in 2012, which employs the reaction of iodoalkyl radical with molecular oxygen: for instance, CH2I + O2 → CH2OO + I. This new synthesis route can produce Criegee intermediates with a high number density, which allows direct detection of the Criegee intermediate via various spectroscopic tools, including vacuum UV photoionization mass spectrometry, absorption and action spectroscopy in the UV and IR regions, and microwave spectroscopy. Criegee intermediates have been thought to play important roles in atmospheric chemistry, such as in OH radical formation as well as oxidation of atmospheric gases such as SO2, NO2, volatile organic compounds, organic and inorganic acids, and even water. These reactions are relevant to acid rain and aerosol formation. Kinetics data including rate coefficients, product yields and their temperature and pressure dependences are important for understanding and modeling relevant atmospheric chemistry. In fundamental physical chemistry, Criegee intermediates have unique and interesting features, which have been partially revealed through spectroscopic, kinetic, and dynamic investigations. Although previous review articles have discussed Criegee intermediates, new data and knowledge on Criegee intermediates are still being accumulated. In this tutorial review, we have focused on structure-dependent reactivity of Criegee intermediates and various spectroscopic tools that have been utilized to probe the kinetics of Criegee intermediates.

中文翻译:

分光光度法研究Criegee中间体的结构依赖性反应性

Criegee中间体是非常活泼的羰基氧化物,是在不饱和烃与臭氧(臭氧分解)反应中形成的。最近,自2012年以来报道了一种新的制备方法,该方法利用了碘代烷基自由基与分子氧的反应,例如CH 2 I + O 2 →CH 2 OO + I。Criegee中间体引起了广泛关注。可以产生克里奇中间体具有高数量密度,这允许直接检测克里奇中间体的经由各种光谱工具,包括真空UV光电离质谱,UV和IR区域的吸收和作用光谱以及微波光谱。人们认为Criegee中间体在大气化学中起着重要作用,例如在OH自由基的形成以及诸如SO 2,NO 2的大气中的氧化,挥发性有机化合物,有机和无机酸,甚至水。这些反应与酸雨和气溶胶形成有关。动力学数据,包括速率系数,产物收率以及它们对温度和压力的依赖性,对于理解和建模相关的大气化学非常重要。在基本的物理化学中,Criegee中间体具有独特而有趣的特征,这些特征已通过光谱,动力学和动态研究得到了部分揭示。尽管以前的评论文章讨论了Criegee中间体,但有关Criegee中间体的新数据和知识仍在积累中。在本教程复习中,
更新日期:2017-08-25
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