College of Chemistry, Fuzhou University, Fuzhou, Fujian, 350116, China.
Department of Chemistry & Biochemistry, Rowan University, 201 Mullica Hill Road, Glassboro, NJ 08028, USA.
Angew Chem Int Ed Engl. 2022 Jul 11;61(28):e202200259. doi: 10.1002/anie.202200259. Epub 2022 May 12.
Currently, completely abiotic channel systems that concurrently reproduce the high selectivity and high permeation rate of natural protein channels are rare. Here, we provide one such biomimetic channel system, i.e., a novel family of helically folded hybrid amide foldamers that can serve as powerful artificial proton channels to mimic key transport features of the exceptionally selective Matrix-2 (M2) proton channels. Possessing an angstrom-scale tubular pore 3 Å in diameter, these low water permeability artificial channels transport protons at a rate 1.22 and 11 times as fast as gramicidin A and M2 channels, respectively, with exceptionally high selectivity factors of 167.6, 122.7, and 81.5 over Cl , Na , and K ions. Based on the experimental and computational findings, we propose a novel proton transport mechanism where a proton may create a channel-spanning water chain from two or more short water chains to facilitate its own transmembrane flux via the Grotthuss mechanism.
目前，能够同时复制天然蛋白质通道高选择性和高通透率的完全非生物通道系统还很少见。在这里，我们提供了这样一个仿生通道系统，即一种新型的螺旋折叠混合酰胺折叠物家族，它们可以作为强大的人工质子通道，模拟具有极高选择性的基质-2 (M2) 质子通道的关键传输特性。这些具有埃米级管状孔的人工通道直径为 3Å，水透过率低，质子传输速度分别比革兰氏菌素 A 和 M2 通道快 1.22 和 11 倍，对 Cl 、Na 和 K 离子的选择性因子分别高达 167.6、122.7 和 81.5。基于实验和计算结果，我们提出了一种新的质子传输机制，质子可能通过两个或更多短水链从两个或更多短水链中创建一个贯穿通道的水链，通过质子扩散机制促进自身跨膜通量。
