Wang Mingzhan, Sadhukhan Tumpa, Lewis Nicholas H C, Wang Maoyu, He Xiang, Yan Gangbin, Ying Dongchen, Hoenig Eli, Han Yu, Peng Guiming, Lee One-Sun, Shi Fengyuan, Tiede David M, Zhou Hua, Tokmakoff Andrei, Schatz George C, Liu Chong
Pritzker School of Molecular Engineering, University of Chicago, Chicago, IL 60637.
Department of Chemistry, Northwestern University, Evanston, IL 60208.
Proc Natl Acad Sci U S A. 2024 Jan 9;121(2):e2313616121. doi: 10.1073/pnas.2313616121. Epub 2024 Jan 2.
Emulating angstrom-scale dynamics of the highly selective biological ion channels is a challenging task. Recent work on angstrom-scale artificial channels has expanded our understanding of ion transport and uptake mechanisms under confinement. However, the role of chemical environment in such channels is still not well understood. Here, we report the anomalously enhanced transport and uptake of ions under confined MoS-based channels that are ~five angstroms in size. The ion uptake preference in the MoS-based channels can be changed by the selection of surface functional groups and ion uptake sequence due to the interplay between kinetic and thermodynamic factors that depend on whether the ions are mixed or not prior to uptake. Our work offers a holistic picture of ion transport in 2D confinement and highlights ion interplay in this regime.
模拟高选择性生物离子通道的埃级动力学是一项具有挑战性的任务。近期关于埃级人工通道的研究拓展了我们对受限环境下离子传输和摄取机制的理解。然而,化学环境在这类通道中的作用仍未得到充分理解。在此,我们报告了在尺寸约为五埃的基于二硫化钼的受限通道中离子传输和摄取异常增强的现象。基于二硫化钼的通道中的离子摄取偏好可通过表面官能团的选择和离子摄取顺序来改变,这是由于动力学和热力学因素之间的相互作用,而这些因素取决于离子在摄取前是否混合。我们的工作提供了二维受限环境中离子传输的整体图景,并突出了该体系中的离子相互作用。