School of Energy & Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea.
Division of Environmental Science and Engineering, Pohang University of Science and Technology (POSTECH), Pohang, Gyeongsangbuk-do 37673, Republic of Korea; R&D Center, ANPOLY INC., Pohang, Gyeongsangbuk-do 37666, Republic of Korea; Institute for Convergence Research and Education in Advanced Technology, Yonsei University International Campus I-CREATE, Incheon 21983, South Korea.
Carbohydr Polym. 2024 Jan 15;324:121504. doi: 10.1016/j.carbpol.2023.121504. Epub 2023 Oct 16.
Low-molecular-weight chitosan (LMW chitosan, <10 kDa) have a significant potential for biomedical applications (e.g., antimicrobial and gene/drug delivery) because of their higher water solubility at pH values ranging from 3.0 to 8.5, compared to that of the high-molecular-weight (>100 kDa) chitosan. A comprehensive understanding of the LMW interaction mechanism with specific functional groups is necessary to predict their binding efficiency to other molecules for effectively utilizing their potential within biological systems. In this study, we used a surface forces apparatus (SFA) to investigate molecular interactions between LMW chitosan and four different functionalized self-assembled monolayers (SAMs) in aqueous solutions at pH values of 3.0, 6.5, and 8.5. Chitosan exhibited the strongest interaction energy with methyl-terminated SAM (CH-SAM), indicating the significance of hydrophobic interaction. Many chitin/chitosan fibers in nature bind polyphenols (e.g., eumelanin) to form robust composites, which can be attributed to the strong attraction between chitosan and phenyl-SAM, presumably caused by cation-π interactions. These findings demonstrate the potential of modulating the magnitude of the interaction energy by controlling the solution pH and types of targeted functional groups to realize the optimal design of chitosan-based hybrid composites with other biomolecules or synthetic materials.
低分子量壳聚糖（LMW 壳聚糖，<10 kDa）由于其在 pH 值为 3.0 至 8.5 的范围内具有更高的水溶性，相对于高分子量 (>100 kDa）壳聚糖，具有显著的生物医学应用潜力（例如，抗菌和基因/药物输送）。为了有效地利用其在生物系统中的潜力，需要全面了解 LMW 与特定官能团的相互作用机制，以预测其与其他分子的结合效率。在这项研究中，我们使用表面力仪（SFA）在 pH 值为 3.0、6.5 和 8.5 的水溶液中研究了 LMW 壳聚糖与四种不同功能化自组装单层（SAM）之间的分子相互作用。壳聚糖与甲基封端的 SAM（CH-SAM）表现出最强的相互作用能，表明疏水相互作用的重要性。自然界中的许多壳聚糖纤维与多酚（如真黑素）结合形成坚固的复合材料，这可能归因于壳聚糖与苯基-SAM 之间的强吸引力，可能是由于阳离子-π 相互作用。这些发现表明通过控制溶液 pH 值和靶向官能团的类型来调节相互作用能的大小，从而实现与其他生物分子或合成材料的壳聚糖基杂化复合材料的最佳设计具有潜力。
