SO3与HONO2的反应以及对大气中的硫分区的影响
Bo Long1, Yu Xia1, Junwei Lucas Bao2
1College of Materials Science and Engineering, Guizhou Minzu University, 550025 Guiyang, China.
Journal of the American Chemical Society
|May 16, 2022
概括
硫三氧化物 (SO3) 与平流层中的酸 (HONO2) 反应,为硫的去除提供了新的途径. 这种反应也可能形成影响平流层硫分离的新产物.
科学领域:
- 大气化学
- 环境科学
- 化学动力学
背景情况:
- 三氧化硫 (SO3) 是硫循环中的关键大气中间体.
- 传统的通过水蒸气去除SO3在较高的海拔上效果较差.
- 层层 SO3 积累对大气化学有影响.
研究的目的:
- 研究三氧化硫与酸 (SO3 + HONO2) 的反应动力学.
- 确定这种反应在平流层中的大气意义.
- 探索潜在的新反应产物及其影响.
主要方法:
- 使用一个双层理论策略,结合过渡状态理论 (W2X//DF-CCSD(T) -F12b/jun'-cc-pVDZ) 和变化过渡状态理论 (M08-HX/MG3S).
- 使用系统特定的量子赖斯-拉姆斯珀格-卡塞尔 (SS-QRRK) 理论计算了压力依赖的速率常数.
- 对低于1 bar的SO3+HONO2反应进行了分析.
主要成果:
- SO3 + HONO2反应在1 bar以下具有显著的落差效应.
- 这种反应是平流层中SO3的潜在去除途径,与SO3+2H2O竞争.
- 反应也可能在热层中去除HONO2,与OH + HONO2竞争.
- 发现了一种意想不到的短寿命产物,影响了硫的分离和有机硫酸盐的形成.
结论:
- SO3 + HONO2反应是一个重要的大气过程,特别是在平流层.
- 这种反应为平流层中硫的去除提供了一种新的机制.
- 新产品的形成对了解硫循环和有机硫酸盐的产生有影响.
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