Buckyball-Based Spherical Display of Crown Ethers for De Novo Custom Design of Ion Transport Selectivity,Journal of the American Chemical Society

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Buckyball-Based Spherical Display of Crown Ethers for De Novo Custom Design of Ion Transport Selectivity
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2020-12-04 , DOI: 10.1021/jacs.0c09655
Ning Li ₁ , Feng Chen ₁ , Jie Shen ₁ , Hao Zhang _{2,

3} , Tianxiang Wang ₄ , Ruijuan Ye _{2,

3} , Tianhu Li _{2,

3} , Teck Peng Loh _{2,

3,

4} , Yi Yan Yang ₅ , Huaqiang Zeng _{2,

3}

Affiliation

Searching for membrane-active synthetic analogues that are structurally simple yet functionally comparable to natural channel proteins has been of central research interest in the past four decades, yet custom design of the ion transport selectivity still remains a grand challenge. Here we report on a suite of buckyball-based molecular balls (MBs), enabling transmembrane ion transport selectivity to be custom designable. The modularly tunable MBm-Cn (m = 4-7; n = 6-12) structures consist of a C60-fullerene core, flexible alkyl linkers Cn (i.e., C6 for n-C6H12 group), and peripherally aligned benzo-3m-crown-m ethers (i.e., m = 4 for benzo-12-crown-4) as ion-transporting units. Screening a matrix of 16 such MBs, combinatorially derived from four different crown units and four different Cn linkers, intriguingly revealed that their transport selectivity well resembles the intrinsic ion binding affinity of the respective benzo-crown units present, making custom design of the transport selectivity possible. Specifically, MB4s, containing benzo-12-crown-4 units, all are Li+-selective in transmembrane ion transport, with the most active MB4-C10 exhibiting an EC50(Li+) value of 0.13 μM (corresponding to 0.13 mol % of the lipid present) while excluding all other monovalent alkali-metal ions. Likewise, the most Na+ selective MB5-C8 and K+ selective MB6-C8 demonstrate high Na+/K+ and K+/Na+ selectivity values of 13.7 and 7.8, respectively. For selectivity to Rb+ and Cs+ ions, the most active MB7-C8 displays exceptionally high transport efficiencies, with an EC50(Rb+) value of 105 nM (0.11 mol %) and an EC50(Cs+) value of 77 nM (0.079 mol %).

中文翻译：

基于巴基球的冠醚球形显示，用于离子传输选择性的从头定制设计

在过去的 40 年里，寻找结构简单但功能与天然通道蛋白相当的膜活性合成类似物一直是研究的重点，但离子传输选择性的定制设计仍然是一个巨大的挑战。在这里，我们报告了一套基于巴基球的分子球 (MB)，使跨膜离子传输选择性能够进行定制设计。模块化可调的 MBm-Cn（m = 4-7；n = 6-12）结构由 C60-富勒烯核心、灵活的烷基接头 Cn（即 n-C6H12 基团的 C6）和外围对齐的 benzo-3m-组成冠-m 醚（即，对于苯并-12-冠-4，m = 4）作为离子传输单元。筛选由 16 个这样的 MB 组成的矩阵，这些 MB 组合来自四个不同的冠单元和四个不同的 Cn 接头，有趣的是，它们的传输选择性与存在的各个苯并冠单元的固有离子结合亲和力非常相似，这使得传输选择性的定制设计成为可能。具体来说，MB4s 含有 benzo-12-crown-4 单元，在跨膜离子传输中都是 Li+ 选择性的，最活跃的 MB4-C10 的 EC50(Li+) 值为 0.13 μM（对应于脂质的 0.13 mol%存在）同时排除所有其他单价碱金属离子。同样，Na+ 选择性最强的 MB5-C8 和 K+ 选择性 MB6-C8 分别表现出 13.7 和 7.8 的高 Na+/K+ 和 K+/Na+ 选择性值。对于 Rb+ 和 Cs+ 离子的选择性，最活跃的 MB7-C8 显示出异常高的传输效率，EC50(Rb+) 值为 105 nM (0.11 mol %)，EC50(Cs+) 值为 77 nM (0.079 mol %) .

更新日期：2020-12-04

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