Reactive uptake of N<sub>2</sub>O<sub>5</sub> by atmospheric aerosol is dominated by interfacial processes

doi:10.1126/science.abd7716

GSTDTAP > 气候变化

DOI	10.1126/science.abd7716
	Reactive uptake of N₂O₅ by atmospheric aerosol is dominated by interfacial processes
	Mirza Galib; David T. Limmer
	2021-02-26
发表期刊	Science
出版年	2021
英文摘要	The uptake and hydrolysis of N2O5 from the atmosphere by aqueous aerosols was long thought to occur by solvation and subsequent hydrolysis in the bulk of the aerosol. However, this mechanistic hypothesis was unverifiable because of the fast reaction kinetics. Galib et al. used molecular simulations to show instead that the mechanism is the inverse: Interfacial hydrolysis is followed by solvation into the interior. Their reactive uptake model is consistent with some existing experimental observations. Science , this issue p. [921][1] Nitrogen oxides are removed from the troposphere through the reactive uptake of N2O5 into aqueous aerosol. This process is thought to occur within the bulk of an aerosol, through solvation and subsequent hydrolysis. However, this perspective is difficult to reconcile with field measurements and cannot be verified directly because of the fast reaction kinetics of N2O5. Here, we use molecular simulations, including reactive potentials and importance sampling, to study the uptake of N2O5 into an aqueous aerosol. Rather than being mediated by the bulk, uptake is dominated by interfacial processes due to facile hydrolysis at the liquid-vapor interface and competitive reevaporation. With this molecular information, we propose an alternative interfacial reactive uptake model consistent with existing experimental observations. [1]: /lookup/doi/10.1126/science.abd7716
领域	气候变化 ; 资源环境
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文献类型	期刊论文
条目标识符	http://119.78.100.173/C666/handle/2XK7JSWQ/315938
专题	气候变化资源环境科学
推荐引用方式 GB/T 7714	Mirza Galib,David T. Limmer. Reactive uptake of N₂O₅ by atmospheric aerosol is dominated by interfacial processes[J]. Science,2021.
APA	Mirza Galib,&David T. Limmer.(2021).Reactive uptake of N₂O₅ by atmospheric aerosol is dominated by interfacial processes.Science.
MLA	Mirza Galib,et al."Reactive uptake of N₂O₅ by atmospheric aerosol is dominated by interfacial processes".Science (2021).