论文标题

蒙脱石相分离是由新兴的界面动力学驱动的

Smectite phase separation is driven by emergent interfacial dynamics

论文作者

Whittaker, Michael L., Lammers, Laura N., Tournassat, Christophe, Gilbert, Benjamin

论文摘要

绿色粘土矿物质对富含粘土的培养基对常见刺激的反应有很大的影响,例如水吸收和离子交换,激发了广泛的努力,以了解这些过程所产生的微观行为,例如肿胀和剥落。尽管如此,关于控制蒙脱石特性的微观力量尚无一般共识,它们是更普遍地理解胶体和界面现象的模型系统。我们发现,控制局部颗粒粒子相互作用的至少四个分子间力及其非线性耦合产生的复杂自由能表面导致动态,不稳定的平衡在不同相之间。弯曲或相互作用界面之间的渗透梯度引起的机械不平衡驱动了通过热波动所维持的雪崩跃迁之间的层和离子的动态交换。我们建议,由晶状体矿物显示出令人惊讶的界面动力学,这是由于水,离子和矿物质的迁移而产生的,使它们与非粘土矿物质的根本不同,因为它们的结构很容易扰动同时脱离化学和机械平衡。

Smectite clay minerals have an outsize impact on the response of clay-rich media to common stimuli, such as water imbibition and ion exchange, motivating extensive effort to understand microscopic behaviors resulting from these processes such as swelling and exfoliation. Nonetheless, there is no general consensus about the microscopic forces that govern smectite properties, which are model systems for understanding colloidal and interfacial phenomena more generally. We find that the complex free energy surface arising from the interplay of at least four intermolecular forces and their nonlinear couplings that control local particle-particle interactions leads to dynamic, unstable equilibria between distinct phases. Mechanical disequilibrium arising from osmotic gradients between curved or interacting interfaces drive the dynamic exchange of layers and ions between dense and dilute phases via avalanche transitions that are sustained by thermal fluctuations. We suggest that the surprising interfacial dynamics displayed by smectite minerals, arising from the vastly different mobilities of water, ions and mineral, makes them fundamentally distinct from non-clay minerals because their structures are easily perturbed away from simultaneous chemical and mechanical equilibrium.

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