水面作为液态水中气体NO2反应的有效过渡停止
Marilia T C Martins-Costa1, Josep M Anglada2, Joseph S Francisco3
1Laboratoire de Physique et Chimie Théoriques, UMR CNRS 7019, University of Lorraine, CNRS, BP 70239, 54506 Vandoeuvre-lès-Nancy, France.
Journal of the American Chemical Society
|December 4, 2020
概括
在云中,二氧化 (NO2) 与水的反应形成酸 (HONO) 尚未完全理解. 模拟显示水上的NO2二极管寿命过短,这表明大气HONO生产需要催化剂.
科学领域:
- 大气化学
- 表面科学
- 计算化学
背景情况:
- 二氧化 (NO2) 与水的异质反应在黑暗条件下是大气酸 (HONO) 的潜在来源.
- 在各种表面上控制这种反应的精确机制仍然不完全理解.
研究的目的:
- 通过第一原理模拟,对纯水滴表面的NO2水解机制进行研究.
- 在大气HONO形成中确定NO2二极管路径的可行性.
主要方法:
- 第一个原则是电子结构计算.
- 量子化学模拟的NO2-水相互作用.
- 反应途径和中间寿命的分析.
主要成果:
- 在纯水面上反应性NO2二极管的计算寿命不足以解释观察到的HONO形成率.
- 纯水上的直接水解途径在动力学上是有限的.
结论:
- 大气中NO2在云层中的水解形成可能需要在水滴上吸附的催化物种.
- 表面吸附的有机或无机化合物在催化NO2水解中起着至关重要的作用.
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