论文标题
动态粘土微结构通过离子络合波出现
Dynamic clay microstructures emerge via ion complexation waves
论文作者
论文摘要
粘土控制岩石圈中的碳,水和养分传输,促进云层5,并通过水合矿物界面之间的相互作用润滑断层。粘土矿物质特性很难建模,因为它们的结构是无序,弯曲和动态的。因此,使用基于云母的单晶和原子模拟的电动双层模型近似粘土矿物质界面的相互作用。我们发现,在动态弯曲接口处的络合偶极子的波创建了一种新兴的远程力,可驱动在现有模型中未捕获的时间和长度尺度上的去角质和重新打击。曲率以与平面表面不同的方式迁移静电相互作用,从而改变了与凸的凸面和凹面侧的离子之比。低剂量能量过滤的冷冻电子断层扫描的多片段重建能够在水合和弯曲的矿物接口上进行直接成像和电解质分布,并在微米长度尺度上分辨率Ångstrom分辨率。层突然和重复地在很大程度上取决于相反身份的时间尺度上,并反复反复进行,这表明粘土中的弹性,静电和水合力之间的强耦合以前促进了以前被认为是活跃物质的特征的集体重组。
Clays control carbon, water and nutrient transport in the lithosphere, promote cloud formation5 and lubricate fault slip through interactions among hydrated mineral interfaces. Clay mineral properties are difficult to model because their structures are disordered, curved and dynamic. Consequently, interactions at the clay mineral-aqueous interface have been approximated using electric double layer models based on single crystals of mica and atomistic simulations. We discover that waves of complexation dipoles at dynamically curving interfaces create an emergent long-range force that drives exfoliation and restacking over time- and length-scales that are not captured in existing models. Curvature delocalizes electrostatic interactions in ways that fundamentally differ from planar surfaces, altering the ratio of ions bound to the convex and concave sides of a layer. Multiple-scattering reconstruction of low-dose energy-filtered cryo electron tomography enabled direct imaging of ion complexes and electrolyte distributions at hydrated and curved mineral interfaces with ångstrom resolution over micron length scales. Layers exfoliate and restack abruptly and repeatedly over timescales that depend strongly on the counterion identity, demonstrating that the strong coupling between elastic, electrostatic and hydration forces in clays promote collective reorganization previously thought to be a feature only of active matter.