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Single-chain heteropolymers transport protons selectively and rapidly
Nature ( IF 50.5 ) Pub Date : 2020-01-08 , DOI: 10.1038/s41586-019-1881-0
Tao Jiang 1, 2 , Aaron Hall 1 , Marco Eres 1, 3 , Zahra Hemmatian 4, 5 , Baofu Qiao 6 , Yun Zhou 7 , Zhiyuan Ruan 1 , Andrew D Couse 1, 8 , William T Heller 9 , Haiyan Huang 10 , Monica Olvera de la Cruz 6, 11 , Marco Rolandi 4 , Ting Xu 1, 3, 12, 13
Affiliation  

Precise protein sequencing and folding are believed to generate the structure and chemical diversity of natural channels1,2, both of which are essential to synthetically achieve proton transport performance comparable to that seen in natural systems. Geometrically defined channels have been fabricated using peptides, DNAs, carbon nanotubes, sequence-defined polymers and organic frameworks3,4,5,6,7,8,9,10,11,12,13. However, none of these channels rivals the performance observed in their natural counterparts. Here we show that without forming an atomically structured channel, four-monomer-based random heteropolymers (RHPs)14 can mimic membrane proteins and exhibit selective proton transport across lipid bilayers at a rate similar to those of natural proton channels. Statistical control over the monomer distribution in an RHP leads to segmental heterogeneity in hydrophobicity, which facilitates the insertion of single RHPs into the lipid bilayers. It also results in bilayer-spanning segments containing polar monomers that promote the formation of hydrogen-bonded chains15,16 for proton transport. Our study demonstrates the importance of the adaptability that is enabled by statistical similarity among RHP chains and of the modularity provided by the chemical diversity of monomers, to achieve uniform behaviour in heterogeneous systems. Our results also validate statistical randomness as an unexplored approach to realize protein-like behaviour at the single-polymer-chain level in a predictable manner.



中文翻译:

单链杂聚物选择性和快速地传输质子

精确的蛋白质测序和折叠被认为会产生自然通道1,2的结构和化学多样性,这两者对于综合实现与自然系统中所见的质子传输性能相当的关键。几何定义的通道已使用肽、DNA、碳纳米管、序列定义的聚合物和有机框架3、4、5、6、7、8、9、10、11、12、13制造。然而,这些渠道中没有一个可以与在其自然对应物中观察到的表现相媲美。在这里,我们展示了在不形成原子结构通道的情况下,基于四单体的无规杂聚物 (RHP) 14可以模拟膜蛋白,并以与天然质子通道相似的速率在脂质双层中表现出选择性质子转运。对 RHP 中单体分布的统计控制导致疏水性的节段异质性,这有助于将单个 RHP 插入脂质双层。它还导致含有极性单体的双层跨链段,促进氢键链的形成15,16用于质子运输。我们的研究证明了通过 RHP 链之间的统计相似性实现的适应性以及单体化学多样性提供的模块化对于在异质系统中实现统一行为的重要性。我们的结果还验证了统计随机性是一种未经探索的方法,可以以可预测的方式在单聚合物链水平上实现蛋白质样行为。

更新日期:2020-01-08
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