Helical foldamers replicating membrane-spanning gramicidin a with pH responsiveness and ultrafast potassium permeability

IF 7.6 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Jun Tian, Lei Zhang, Ze Lin, Shizhong Mao, Zeyuan Dong
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引用次数: 0

Abstract

Structural simulation of natural ion channels remains a challenging topic. To fabricate artificial ion channels structurally resembling natural gramicidin A (gA), we prepared a type of precise hollow helical molecular channel by means of a modular synthesis strategy. Helical molecules are able to form 2.9 nm membrane-spanning channels through dimeric π-stacking assembly and efficiently accelerate ion transmembrane transport, with ultrahigh transport activity of up to 28 nM. Among these molecular channels with transmembrane structures similar to gA, one of them significantly exceeds natural gA for potassium ion transport, while another one exhibits the same proton transport activity as natural gA under identical conditions. Moreover, we found that the positive charges near the entrance of the channel reduce the potassium transport rate of the channel but significantly promote proton transport. In addition, a molecular channel with terminal amine groups shows pH-regulated ion transport function. This is the first example of structural replication of natural gA, in which helically folded molecules with assembled dimeric structure yield fantastic ion transport properties.

Abstract Image

具有pH响应性和超快钾渗透性的螺旋折叠体复制跨膜gramicidin a
天然离子通道的结构模拟仍然是一个具有挑战性的课题。为了制备结构类似天然革兰杀菌素A (gA)的人工离子通道,我们采用模块化合成策略制备了一种精确的空心螺旋分子通道。螺旋分子可通过二聚体π堆积组装形成2.9 nm的跨膜通道,有效加速离子跨膜运输,其转运活性可达28 nm。在这些与gA具有相似跨膜结构的分子通道中,其中一条通道的钾离子转运能力明显超过天然gA,另一条通道在相同条件下表现出与天然gA相同的质子转运活性。此外,我们发现通道入口附近的正电荷降低了通道的钾转运速率,但显著促进了质子的转运。此外,具有末端胺基的分子通道具有ph调节的离子运输功能。这是天然gA结构复制的第一个例子,其中具有组装二聚体结构的螺旋折叠分子产生了奇妙的离子传输特性。
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来源期刊
Chemical Science
Chemical Science CHEMISTRY, MULTIDISCIPLINARY-
CiteScore
14.40
自引率
4.80%
发文量
1352
审稿时长
2.1 months
期刊介绍: Chemical Science is a journal that encompasses various disciplines within the chemical sciences. Its scope includes publishing ground-breaking research with significant implications for its respective field, as well as appealing to a wider audience in related areas. To be considered for publication, articles must showcase innovative and original advances in their field of study and be presented in a manner that is understandable to scientists from diverse backgrounds. However, the journal generally does not publish highly specialized research.
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