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在空气-水界面的Criegee中间体与酸的反应
Manoj Kumar1, Jie Zhong1, Xiao Cheng Zeng1,2,3
1Department of Chemistry , University of Nebraska-Lincoln , Lincoln , Nebraska 68588 , United States.
Journal of the American Chemical Society
|March 23, 2018
概括
在空气-水界面的Criegee中间体的大气化学质量至关重要. 通过酸介导的CH3CHOO水化比直接反应具有主导作用,对污染的城市环境产生影响.
科学领域:
- 大气化学
- 环境科学
- 物理化学
背景情况:
- 水面在大气化学中起着重要作用.
- 克里基介质在水面上的双分子反应不太清楚.
- 克里奇介质会影响主要大气物种的热层预算.
研究的目的:
- 调查反CH3CHOO与酸 (HNO3) 在空气-水界面上的反应机制和光谱信号.
- 阐明受污染的城市环境中的主要反应途径.
- 确定反应产品的潜在光谱标记物.
主要方法:
- 使用波恩-奥本海默分子动力学模拟.
- 使用电子嵌入式的双层ONIOM (QM:MM).
- 在皮秒时间尺度上研究了反应动态.
主要成果:
- 在空气-水界面上,HNO3介导的抗CH3CHOO水化是主要的途径.
- 直接反应形成氧乙是一种次要道.
- 这两种途径都通过一个阶段性机制进行.
结论:
- 在雾,污染的城市大气中,HNO3介导的水化途径很重要.
- 光谱标记 (NO拉伸,NO2曲) 可以区分反应产物.
- 类似的机制也可能适用于有机酸,
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