论文标题
使用Angstrom尺度毛细血管对离子的空间选择性超出空间选择性
Beyond steric selectivity of ions using angstrom-scale capillaries
论文作者
论文摘要
离子选择通道在生理过程中起关键作用,并在许多技术中使用。虽然生物通道可以用相似的水合壳有效地将相同的离子分开,但使用人工固态通道模仿这种精致的选择性仍然是一个挑战。虽然,有几种纳米多孔膜相对于某些离子表现出很高的选择性,但潜在的机制基于水合离子尺寸和/或电荷。需要合理化人工通道的设计,以使它们能够在相似大小的相同带离子之间进行选择,这反过来又需要了解这种选择性以及如何发生这种选择性。为了解决这个问题,我们研究了由范德华组装制成的埃恒级人造通道,该通道的大小与典型的离子相当,并且在通道壁上几乎没有剩余电荷。这使我们可以排除基于空间和基于库仑的排除的一阶效应。我们表明,所研究的二维Angstrom尺度毛细血管可以区分具有相似水合直径的相同荷兰离子。选择性归因于离子在纳米结合水的分层结构中所占据的不同位置,该位置取决于离子核的大小,而在阴离子和阳离子上也有所不同。揭示的机制指向离子分离的可能性,超出了简单的空间筛分。
Ion-selective channels play a key role in physiological processes and are used in many technologies. While biological channels can efficiently separate same-charge ions with similar hydration shells, it remains a challenge to mimic such exquisite selectivity using artificial solid-state channels. Although, there are several nanoporous membranes that show high selectivity with respect to certain ions, the underlying mechanisms are based on the hydrated ion size and/or charge. There is a need to rationalize the design of artificial channels to make them capable of selecting between similar-size same-charge ions, which in turn requires understanding of why and how such selectivity can occur. To address this issue, we study angstrom-scale artificial channels made by van der Waals assembly, which are comparable in size with typical ions and carry little residual charge on channel walls. This allows us to exclude the first-order effects of steric and Coulomb-based exclusion. We show that the studied two-dimensional angstrom-scale capillaries can distinguish between same-charge ions with similar hydrated diameters. The selectivity is attributed to different positions occupied by ions within the layered structure of nanoconfined water, which depend on the ion-core size and differ for anions and cations. The revealed mechanism points at possibilities of ion separation beyond the simple steric sieving.