Energy Geosciences Division, Lawrence Berkeley National Laboratory, 94720, Berkeley, CA, USA.
Department of Earth and Planetary Science, University of California, 94720, Berkeley, CA, USA.
Nat Commun. 2022 Jun 13;13(1):3382. doi: 10.1038/s41467-022-31004-0.
Visualizing hydrated interfaces is of widespread interest across the physical sciences and is a particularly acute need for layered minerals, whose properties are governed by the structure of the electric double layer (EDL) where mineral and solution meet. Here, we show that cryo electron microscopy and tomography enable direct imaging of the EDL at montmorillonite interfaces in monovalent electrolytes with ångstrom resolution over micron length scales. A learning-based multiple-scattering reconstruction method for cryo electron tomography reveals ions bound asymmetrically on opposite sides of curved, exfoliated layers. We observe conserved ion-density asymmetry across stacks of interacting layers in cryo electron microscopy that is associated with configurations of inner- and outer-sphere ion-water-mineral complexes that we term complexation waves. Coherent X-ray scattering confirms that complexation waves propagate at room-temperature via a competition between ion dehydration and charge interactions that are coupled across opposing sides of a layer, driving dynamic transitions between stacked and aggregated states via layer exfoliation.
可视化水合界面在整个物理科学领域都引起了广泛的关注，对于层状矿物来说，这是一个特别迫切的需求，因为其性质由矿物和溶液相遇的双电层（EDL）结构决定。在这里，我们展示了冷冻电子显微镜和断层摄影术能够在单价电解质中直接成像蒙脱石界面处的EDL，其分辨率在Ångstrom 尺度上超过微米长度尺度。一种基于学习的冷冻电子断层摄影术多次散射重建方法揭示了在弯曲、剥落的层的相对两侧上不对称结合的离子。我们在冷冻电子显微镜中观察到相互作用的层堆栈中存在离子密度的对称性，这与我们称之为配位波的内圈和外圈离子-水-矿物配合物的构型有关。相干 X 射线散射证实，配位波通过离子去水合和电荷相互作用之间的竞争在室温下传播，这些相互作用在层的相对两侧耦合，通过层剥落驱动堆叠和聚集状态之间的动态转变。
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