Li Hailong, Mars Julian, Lohstroh Wiebke, Koza Michael Marek, Butt Hans-Jürgen, Mezger Markus
Department of Physics at Interfaces, Max Planck Institute for Polymer Research, Ackermannweg 10, 55128, Mainz, Germany.
Heinz Maier-Leibnitz Zentrum (MLZ), Technische Universität München, Lichtenbergstrasse 1, 85748, Garching, Germany.
Angew Chem Int Ed Engl. 2021 Mar 29;60(14):7697-7702. doi: 10.1002/anie.202013125. Epub 2021 Feb 25.
At solid/ice interfaces, a premelting layer is formed at temperatures below the melting point of bulk water. However, the structural and dynamic properties within the premelting layer have been a topic of intense debate. Herein, we determined the translational diffusion coefficient D of water in ice/clay nanocomposites serving as model systems for permafrost by quasi-elastic neutron scattering. Below the bulk melting point, a rapid decrease of D is found for charged hydrophilic vermiculite, uncharged hydrophilic kaolin, and more hydrophobic talc, reaching plateau values below -4 °C. At this temperature, D in the premelting layer is reduced up to a factor of two compared to supercooled bulk water. Adjacent to charged vermiculite the lowest water mobility was observed, followed by kaolin and the more hydrophobic talc. Results are explained by the intermolecular water interactions with different clay surfaces and interfacial segregation of the low-density liquid water (LDL) component.
在固体/冰界面处,低于大块水熔点的温度下会形成一个预熔层。然而,预熔层内的结构和动力学性质一直是激烈争论的话题。在此,我们通过准弹性中子散射确定了作为永久冻土模型系统的冰/粘土纳米复合材料中水的平移扩散系数D。在大块熔点以下,对于带电亲水性蛭石、不带电亲水性高岭土和疏水性更强的滑石,发现D迅速降低,在-4°C以下达到平稳值。在此温度下,与过冷大块水相比,预熔层中的D降低了多达两倍。在带电蛭石附近观察到最低的水迁移率,其次是高岭土和疏水性更强的滑石。结果通过水分子与不同粘土表面的相互作用以及低密度液态水(LDL)成分的界面偏析来解释。