WPI-Nano Life Science Institute (WPI-NanoLSI), Kanazawa University, Kakuma-machi, Kanazawa, Ishikawa 920-1192, Japan.
RIKEN Center for Biosystems Dynamics Research, 1-7-22 Suehiro-cho, Tsurumi-ku, Yokohama 230-0045, Japan.
J Colloid Interface Sci. 2025 Feb;679(Pt B):435-445. doi: 10.1016/j.jcis.2024.10.119. Epub 2024 Oct 22.
Molecular recognition, involving the binding of two or more molecules, is widely found in multiple disciplines. It plays a crucial role in driving specific molecular functionalization or biological activities such as antigen-antibody interactions. Recently, the molecular recognition of single peptides self-assembly at interfaces has been widely investigated since their broad applications in biosensors and bioelectronics. However, the recognition characteristics of peptide-peptide co-assembly on solids have not been investigated yet, which provides a basis for potential multi-probes biosensing or structure-intermingled functionalized bioelectronic applications. Here, we explored the molecular recognition characteristics of co-assembled peptides on two-dimensional (2D) layered nanomaterials, specifically graphite. Our findings showed distinct surface characteristics of peptide co-assembly in comparison to the independent peptide self-assembly. Peptide co-assembly exhibited the nucleation and growth heterogeneities with reduced nucleation and growth rates, dominated by a diffusion-limited step as confirmed via carrying out the sequential assembly experiments. Moreover, molecular dynamics simulation reveals a slowdown binding process of co-assembled peptides to graphite. Furthermore, the misattachment of one peptide to arrays of another type of peptide with distinct structural ordering orientations severely postponed peptide elongation. Therefore, our work provides valuable insight into the fundamental surface characteristics of two co-assembled peptides as they specifically recognize graphite surface via undergoing continuous surface behaviors from binding to diffusion until final ordering process. The formation of co-assembled peptide patterns on 2D layered nanomaterials incorporates multiple functions, enabling to provide potential applications in intermingled peptide-based biosensing or bioelectronic nanodevices.
分子识别，涉及两个或多个分子的结合，广泛存在于多个学科中。它在驱动特定的分子功能化或生物活性方面起着至关重要的作用，例如抗原-抗体相互作用。最近，由于其在生物传感器和生物电子学中的广泛应用，单肽自组装在界面上的分子识别受到了广泛的研究。然而，肽-肽共组装在固体上的识别特性尚未被研究，这为潜在的多探针生物传感或结构交织功能化生物电子应用提供了基础。在这里，我们探索了共组装肽在二维（2D）层状纳米材料，特别是石墨上的分子识别特性。我们的研究结果表明，与独立的肽自组装相比，共组装肽具有明显不同的表面特性。肽共组装表现出成核和生长的非均质性，成核和生长速率降低，这由扩散限制步骤主导，通过进行顺序组装实验得到证实。此外，分子动力学模拟揭示了共组装肽与石墨结合的过程较慢。此外，一个肽错误地附着在具有不同结构有序取向的另一种肽的阵列上，严重推迟了肽的延伸。因此，我们的工作为两种共组装肽在通过连续的表面行为从结合到扩散到最终的有序过程中特异性识别石墨表面的基本表面特性提供了有价值的见解。共组装肽图案在二维层状纳米材料上的形成包含多种功能，可用于交织肽基生物传感或生物电子纳米器件的潜在应用。
