集群的碎片能量与大气新粒子形成有关
Bryan R Bzdek1, Joseph W DePalma, Douglas P Ridge
1Department of Chemistry and Biochemistry, University of Delaware, Newark, Delaware 19716, USA.
Journal of the American Chemical Society
|February 5, 2013
概括
了解小大气集群如何生长是气候建模的关键. 这项研究揭示了氨纳入的激活障碍,表明目前的模型需要修订,以准确地预测新的粒子形成.
科学领域:
- 大气化学 大气化学
- 化学动力学 化学动力学
- 气候科学 气候科学
背景情况:
- 新粒子形成 (NPF) 显著影响云凝结核和全球气候.
- 硫酸对NPF至关重要,但像氨这样的基本物种也很重要.
- 酸合并到小集群中的动力学和热力学尚不清楚.
研究的目的:
- 研究正电荷二硫酸集群的碎片化机制和能量障碍.
- 确定氨和硫酸融入大气集群中的动力学和热力学.
- 提供与NPF相关的大气集群的生长机制的见解.
主要方法:
- 利用里叶变换离子循环子共振质谱与表面诱导解离.
- 进行了对二硫酸盐集群的时间和碰撞能量解析的碎片化分析.
- 综合的赖斯-拉姆斯珀格-卡塞尔-马库斯/准平衡理论建模和量子化学计算.
主要成果:
- 确定了两个碎片化的途径:氨的连续损失,然后硫酸,或氨二硫酸的直接损失.
- 分离的实验性临界能量超过了热力学值,表明激活障碍.
- 与热力学计算相比,观察到较高的氨损失和二硫酸损失的实验临界能量.
结论:
- 集群生长需要激活氨纳入的障碍,挑战扩散有限的生长假设.
- 大气NPF模型必须包含集群生长中的化学步骤的激活障碍.
- 这项研究完善了对大气集群动态及其气候影响的理解.
相关概念视频
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One type of fragmentation pattern is the cleavage of a single bond in the molecular ion. The cleavage leads to a radical and a cation. The cleavage can occur at...
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For example, the fragmentation of...
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