分子限制狭缝几何中亚稳态电荷调节途径的实时可视化
Real-time visualization of metastable charge regulation pathways in molecularly confined slit geometries
摘要：
离子在分子尺度的有限空间中的传输是生活和技术各个方面的核心：进入裂缝，它可能在几天内打破钢铁;通过膜分离器，它决定了电化学能量转换设备的效率;或者通过脂质膜，它引导神经通信。然而，在亚纳米限制中直接观察离子迁移率和结构是实验上具有挑战性的，并且到目前为止，只能通过分子模拟来实现。在这里，我们展示了定量的，3D分子分辨离子运输的水性离子液体和S-块金属离子溶液，局限于电化学调制，分子大小的狭缝。我们的原子分辨固/液界面的分析揭示了一般的规则，如何确定的电荷调节机制的离子-离子和离子-表面相互作用和熵约束效应。改变我们的一般理解，受限的电荷调节可能会通过快速，动力学上有利的，亚稳态的途径，其次是缓慢的扩散热力学离子重组，这对所有的电荷调节系统具有重要意义。
英文摘要：
Transport of ions in molecular-scale confined spaces is central to all aspects of life and technology: into a crack, it may break steel within days; through a membrane separator, it determines the efficiency of electrochemical energy conversion devices; or through lipid membranes, it steers neural communication. Yet, the direct observation of ion mobility and structuring in sub-nanometer confinement is experimentally challenging and, so far, solely accessible to molecular simulations. Here, we show quantitative, 3D molecularly-resolved ion transportation of aqueous ionic liquid and s-block metal ion solutions, confined to electrochemically-modulated, molecular-sized slits. Our analysis of atomically resolved solid/liquid interface unveils generic rules of how enthalpic ion-ion and ion-surface interactions and entropic confinement effects determine the charge regulation mechanism. Altering our general understanding, the confined charge regulation may proceed via fast, kinetically favoured, metastable pathways, followed by slow diffusive thermodynamic ion reorganization, which has important implications for all charge-regulated systems.
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