海盐气溶胶界面增强的ClNO$_2$生成
Enhanced ClNO$_2$ formation at the interface of sea-salt aerosol
AI总结：
本研究通过分子模拟和理论揭示海盐气溶胶界面因稳定电荷离域过渡态而显著增强ClNO$_2$生成，并建议重新审视气溶胶分支比的现有解释。
摘要：
海盐喷雾气溶胶对$\mathrm{N_2O_5}$的反应性摄取在调节对流层NO$_\mathrm{x}$浓度中起着关键作用。尽管已有大量现场和实验室研究，但其异质反应性的微观理解仍不清楚。在此，我们利用分子模拟和理论来阐明$\mathrm{N_2O_5}$氯化生成ClNO$_2$的过程，这是海盐喷雾气溶胶内的主要反应通道。我们发现，由于电荷离域过渡态在异质环境中的稳定化，ClNO$_2$的生成在空气-水界面处显著增强，这从双分子速率理论在异质环境中的表述中得以体现。我们利用分子反应-扩散方程的数值解及其解析近似，探讨了增强的界面反应性对$\mathrm{N_2O_5}$摄取的影响。我们的结果表明，目前对气溶胶分支比的解释需要重新审视。
英文摘要：
The reactive uptake of $\mathrm{N_2O_5}$ on sea-spray aerosol plays a key role in regulating NO$_\mathrm{x}$ concentration in the troposphere. Despite numerous field and laboratory studies, a microscopic understanding of its heterogeneous reactivity remains unclear. Here, we use molecular simulation and theory to elucidate the chlorination of $\mathrm{N_2O_5}$ to form ClNO$_2$, the primary reactive channel within sea-spray aerosol. We find the formation of ClNO$_2$ is markedly enhanced at the air-water interface due to the stabilization of the charge-delocalized transition state, as evident from the formulation of bimolecular rate theory in heterogeneous environments. We explore the consequences of the enhanced interfacial reactivity in the uptake of $\mathrm{N_2O_5}$ using numerical solutions of molecular reaction-diffusion equations as well as their analytical approximations. Our results suggest that the current interpretation of aerosol branching ratios needs to be revisited.
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