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通过盐诱导相分离和环境共沸蒸发工艺制备的果胶纳米多孔结构。

Pectin Nanoporous Structures Prepared via Salt-Induced Phase Separation and Ambient Azeotropic Evaporation Processes.

机构信息

Department of Chemical Engineering, Department of Intelligent Energy and Industry, Chung-Ang University, Seoul 06974, Republic of Korea.

Department of Material Science and Engineering, Texas A&M University, College Station, Texas 77843, United States.

出版信息

Biomacromolecules. 2024 Mar 11;25(3):1709-1723. doi: 10.1021/acs.biomac.3c01230. Epub 2024 Feb 20.

Abstract

Polysaccharide nanoporous structures are suitable for various applications, ranging from biomedical scaffolds to adsorption materials, owing to their biocompatibility and large surface areas. Pectin, in particular, can create 3D nanoporous structures in aqueous solutions by binding with calcium cations and creating nanopores by phase separation; this process involves forming hydrogen bonds between alcohols and pectin chains in water and alcohol mixtures and the resulting penetration of alcohols into calcium-bound pectin gels. However, owing to the dehydration and condensation of polysaccharide chains during drying, it has proven to be challenging to maintain the 3D nanoporous structure without using a freeze-drying process or supercritical fluid. Herein, we report a facile method for creating polysaccharide-based xerogels, involving the co-evaporation of water with a nonsolvent (e.g., a low-molecular-weight hydrophobic alcohol such as isopropyl or -propyl alcohol) at ambient conditions. Experiments and coarse-grained molecular dynamics simulations confirmed that salt-induced phase separation and hydrogen bonding between hydrophobic alcohols and pectin chains were the dominant processes in mixtures of pectin, water, and hydrophobic alcohols. Furthermore, the azeotropic evaporation of water and alcohol mixed in approximately 1:1 molar ratios was maintained during the natural drying process under ambient conditions, preventing the hydration and aggregation of the hydrophilic pectin chains. These results introduce a simple and convenient process to produce 3D polysaccharide xerogels under ambient conditions.

摘要

多糖纳米多孔结构由于其生物相容性和大的表面积,适用于从生物医学支架到吸附材料等各种应用。特别是果胶可以通过与钙离子结合并通过相分离形成纳米孔来在水溶液中创建 3D 纳米多孔结构;这个过程涉及到在水和醇混合物中醇和果胶链之间形成氢键,以及醇渗透到与钙结合的果胶凝胶中。然而,由于多糖链在干燥过程中的脱水和缩合,在不使用冷冻干燥或超临界流体的情况下,保持 3D 纳米多孔结构一直是一个挑战。在这里,我们报告了一种创建基于多糖的干凝胶的简便方法,涉及在环境条件下共蒸发水和非溶剂(例如,低分子量疏水分子醇,如异丙醇或丙醇)。实验和粗粒度分子动力学模拟证实,盐诱导的相分离和疏水分子醇与果胶链之间的氢键是果胶、水和疏水分子醇混合物中的主要过程。此外,在环境条件下的自然干燥过程中,保持了水和醇以约 1:1 摩尔比混合的共沸蒸发,防止了亲水性果胶链的水合和聚集。这些结果引入了一种在环境条件下生产 3D 多糖干凝胶的简单方便的方法。

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