在空气/水界面的新机械路径
Chongqin Zhu1,2, Manoj Kumar1, Jie Zhong1
1Department of Chemistry, University of Nebraska-Lincoln , Lincoln, Nebraska 68588, United States.
Journal of the American Chemical Society
|August 11, 2016
概括
最小的Criegee中间体 (CH2OO) 与水的反应在空气/水界面比气相要快得多. 这项研究揭示了新的反应途径,
科学领域:
- 大气化学
- 化学动力学
- 计算化学
背景情况:
- 克里吉中间体在热层化学中至关重要.
- 它们与水群的反应是关键的,但气溶/云效应的研究不足.
研究的目的:
- 研究气相和空气/水界面上的CH2OO与水的反应.
- 在接口上阐明反应机制和动力学.
主要方法:
- 一开始的量子化学计算.
- 适应性缓冲力量子力学/分子力学 (QM/MM) 动力学模拟.
主要成果:
- 在接口处,CH2OO与水的反应比气相快2-3次.
- 在接口上确定循环结构介导和阶段性机制.
- 阶段性机制不需要循环结构,形成HOCH2OOH.
结论:
- 水界面极大地加快了克里吉的中间反应.
- 在空气/水界面上对CH2OO反应的新机理见解.
- 这些发现鼓励对云中的克里奇化学进行实验研究.
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