Use of Ion Exchange to Regulate the Heterogeneous Ice Nucleation Efficiency of Mica,Journal of the American Chemical Society

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Use of Ion Exchange to Regulate the Heterogeneous Ice Nucleation Efficiency of Mica
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2020-09-27 , DOI: 10.1021/jacs.0c00920
Shenglin Jin ₁ , Yuan Liu _{2,

3} , Malte Deiseroth ₄ , Jie Liu ₁ , Ellen H. G. Backus _{4,

5} , Hui Li ₂ , Han Xue ₁ , Lishan Zhao ₁ , Xiao Cheng Zeng ₃ , Mischa Bonn ₄ , Jianjun Wang _{1,

6}

Affiliation

Heterogeneous ice nucleation (HIN) triggered by mineral surfaces typically exposed to various ions can have a significant impact on the regional atmosphere and climate. However, the dependence of HIN on the nature of the mineral surface ions is still largely unexplored due to the complexity of mineral surfaces. Because the K+ on the atomically flat (001) surface of mica can be readily replaced by different cations through ion exchange, muscovite mica was selected; its simple nature provides a very straightforward system that can serve as the model for investigating the effects of mineral surface ions on HIN. Our experiments show that the surface (001) of H+-exchanged mica displays markedly higher HIN efficiencies than that of Na-/K-mica. Vibrational sum-frequency generation spectroscopy reveals that H-mica induces substantially less orientation ordering than Na-/K-mica within the contact water layer at the interface. Molecular dynamics simulations suggest that the HIN efficiency of mica depends on the positional arrangement and orientation of the interfacial water. The formation of the hexagonal ice Ih basal-type structure in the first water layer atop the mica surface facilitates HIN, which is determined by the size of the protruding ions atop the mica surface and by the surface adsorption energy. The orienta-tional distribution is optimal for HIN when 25% of the water molecules in the first water layer atop the mica surface have one OH group pointing up and 25% have one OH group pointing down, which, in turn, is determined by the surface charge distribution.

中文翻译：

利用离子交换调节云母异质冰成核效率

由通常暴露于各种离子的矿物表面触发的非均质冰核 (HIN) 会对区域大气和气候产生重大影响。然而，由于矿物表面的复杂性，HIN 对矿物表面离子性质的依赖性在很大程度上仍未被探索。由于云母原子平面（001）表面上的K+可以很容易地通过离子交换被不同的阳离子取代，因此选择了白云母；它的简单性质提供了一个非常简单的系统，可以作为研究矿物表面离子对 HIN 影响的模型。我们的实验表明，H+ 交换云母的表面 (001) 显示出明显高于 Na-/K-云母的 HIN 效率。振动和频发生光谱表明，在界面处的接触水层内，H-云母比 Na-/K-云母引起的取向排序要少得多。分子动力学模拟表明，云母的 HIN 效率取决于界面水的位置排列和方向。云母表面第一层水层中六角冰 Ih 基底型结构的形成促进了 HIN，这取决于云母表面突出离子的大小和表面吸附能。当云母表面第一层水层中 25% 的水分子的一个 OH 基团朝上，25% 的一个 OH 基团朝下时，HIN 的方向分布是最佳的，而这又由表面电荷分布。

更新日期：2020-09-27

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