盐诱导的 Fmoc-三肽超分子水凝胶：自组装的实验和计算相结合的研究,Nanoscale

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盐诱导的 Fmoc-三肽超分子水凝胶：自组装的实验和计算相结合的研究
Nanoscale ( IF 5.8 ) Pub Date : 2024-04-16 , DOI: 10.1039/d4nr00335g
Miryam Criado-Gonzalez _{1,

2} , Mario Iván Peñas _{1,

2} , Florent Barbault ₃ , Alejandro J. Müller _{2,

4} , Fouzia Boulmedais ₅ , Rebeca Hernández ₁

Affiliation

从自下而上的角度深入研究短序列肽原子水平上的分子相互作用背后的机制，对于开发具有特定结构-性能-功能关系的纳米材料起着关键作用。由于其水溶性差，带有 Fmoc 的肽的自组装通常是通过在有机溶剂中溶解、随后在水中的稀释步骤、pH 变化和/或加热-冷却过程来诱导的。在此，我们报告了一种在 NaCl 溶液中凝胶化 Fmoc-FFpY（F：苯丙氨酸；Y：酪氨酸；p：PO ₄²⁻）（一种带负电荷的三肽）的简单方法。 Fmoc-FFpY 和 Na ⁺离子之间的静电相互作用产生不同的纳米纤维水凝胶，其流变特性和纳米纤维尺寸由纯水介质中的 NaCl 浓度调节。由肽磷酸基团和Na ⁺离子之间的静电相互作用引发，肽自组装由于肽主链之间的氢键以及芳香族Fmoc和苯基单元的π-π堆积而稳定。该水凝胶表现出自愈和热响应特性，可用于潜在的生物医学应用。没有事先训练的系统的分子动力学模拟不仅证实了肽在临界盐浓度下的聚集以及所涉及的不同相互作用，而且还证实了微秒时间尺度的水凝胶的二级结构。值得强调的是使用原子模拟再现水凝胶形态行为的显著成就。据我们所知，这项研究是第一个报告此类通信的研究。

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Salt-induced Fmoc-tripeptide supramolecular hydrogels: a combined experimental and computational study of the self-assembly

Delving into the mechanism behind the molecular interactions at the atomic level of short-sequence peptides plays a key role in the development of nanomaterials with specific structure–property–function relationships from a bottom-up perspective. Due to their poor water solubility, the self-assembly of Fmoc-bearing peptides is usually induced by dissolution in an organic solvent, followed by a dilution step in water, pH changes, and/or a heating–cooling process. Herein, we report a straightforward methodology for the gelation of Fmoc-FFpY (F: phenylalanine; Y: tyrosine; and p: PO₄²⁻), a negatively charged tripeptide, in NaCl solution. The electrostatic interactions between Fmoc-FFpY and Na⁺ ions give rise to different nanofibrillar hydrogels with rheological properties and nanofiber sizes modulated by the NaCl concentration in pure aqueous media. Initiated by the electrostatic interactions between the peptide phosphate groups and the Na⁺ ions, the peptide self-assembly is stabilized thanks to hydrogen bonds between the peptide backbones and the π–π stacking of aromatic Fmoc and phenyl units. The hydrogels showed self-healing and thermo-responsive properties for potential biomedical applications. Molecular dynamics simulations from systems devoid of prior training not only confirm the aggregation of peptides at a critical salt concentration and the different interactions involved, but also corroborate the secondary structure of the hydrogels at the microsecond timescale. It is worth highlighting the remarkable achievement of reproducing the morphological behavior of the hydrogels using atomistic simulations. To our knowledge, this study is the first to report such a correspondence.

更新日期：2024-04-16

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