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Revealing Atom-Radical Reactivity at Low Temperature Through the N + OH Reaction

机译:通过N + OH反应揭示低温下的原子自由基反应性

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More than 100 reactions between stable molecules and free radicals have been shown to remain rapid at low temperatures. In contrast, reactions between two unstable radicals have received much less attention due to the added complexity of producing and measuring excess radical concentrations. We performed kinetic experiments on the barrierless N(4S) + OH(2π) → H(2S) + NO(2π) reaction in a supersonic flow (Laval nozzle) reactor. We used a microwave-discharge method to generate atomic nitrogen and a relative-rate method to follow the reaction kinetics. The measured rates agreed well with the results of exact and approximate quantum mechanical calculations. These results also provide insight into the gas-phase formation mechanisms of molecular nitrogen in interstellar clouds.
机译:稳定分子与自由基之间的100多种反应已显示在低温下保持快速。相反,由于产生和测量过量自由基浓度增加了复杂性,两个不稳定自由基之间的反应受到的关注较少。我们在超音速流(拉瓦尔喷嘴)反应器中对无障碍N(4S)+ OH(2π)→H(2S)+ NO(2π)反应进行了动力学实验。我们使用微波放电法生成原子氮,并使用相对速率法跟踪反应动力学。测得的速率与精确和近似量子力学计算的结果吻合得很好。这些结果也为星际云中分子氮的气相形成机理提供了见识。

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  • 来源
    《Science》 |2011年第6062期|p.1538-1541|共4页
  • 作者单位

    Universite' de Bordeaux, Institut des Sciences Moleculaires, CNRS UMR 5255, F-33400 Talence, France;

    rnLaboratoire de Catalyse en Chimie Organique, UMR CNRS 6503, Universite de Poitiers, 86022 Poitiers Cedex, France;

    Institute of Theoretical and Computational Chemistry, Key Laboratory of Mesoscopic Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210093, China;

    Universite' de Bordeaux, Institut des Sciences Moleculaires, CNRS UMR 5255, F-33400 Talence, France;

    Universite' de Bordeaux, Institut des Sciences Moleculaires, CNRS UMR 5255, F-33400 Talence, France;

    Universite' de Bordeaux, Institut des Sciences Moleculaires, CNRS UMR 5255, F-33400 Talence, France;

    Institute of Theoretical and Computational Chemistry, Key Laboratory of Mesoscopic Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210093, China;

    Department of Chemistry and Chemical Biology, University of New Mexico, Albuquerque, NM 87131, USA;

    Laboratoire Interdisciplinaire Carnot de Bourgogne, UMR CNRS 5209, Universite de Bourgogne, 21078 Dijon Cedex, France UFR Sciences et Techniques, Universite de Franche-Comte, 25030 Besancon Cedex, France;

    Universite' de Bordeaux, Institut des Sciences Moleculaires, CNRS UMR 5255, F-33400 Talence, France;

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  • 正文语种 eng
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  • 入库时间 2022-08-18 02:54:16

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