Rheological Properties and Gelation Behavior of Chitosan in a Weakly Alkaline NaHCO3/Urea Aqueous Solution

IF 5.1 1区化学 Q1 POLYMER SCIENCE

Macromolecules Pub Date : 2025-05-10 DOI:10.1021/acs.macromol.4c01673

Haoyu Xin, Xuejie Yu, Yiwen Lu, Jie Cai

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引用次数: 0

Abstract

Sustainable polymer materials derived from renewable resources have become increasingly important in addressing environmental challenges. Chitosan, a derivative of chitin, offers exceptional potential due to its unique biological and physicochemical properties. However, its practical application has been limited by the harsh conditions typically required for dissolution and processing. Here we demonstrate a novel approach using NaHCO₃/urea aqueous solution as a weakly alkaline solvent system that enables efficient chitosan processing under mild conditions. Through comprehensive rheological analysis, we reveal that the sol–gel transition of chitosan in NaHCO₃/urea aqueous solution is governed by the synergistic interplay of hydrogen bonding, hydrophobic interactions, and chain entanglements. The gelation behavior exhibits strong dependence on chitosan concentration and molecular weight, with higher values promoting robust network formation at lower temperatures. Notably, we discover a reversible sol–gel transition mechanism that enables precise control over material properties through temperature modulation, while maintaining long-term stability despite modest changes in molecular characteristics during storage. These findings advance our understanding of polysaccharide self-assembly in weakly alkaline media and establish a new paradigm for developing controllable chitosan-based materials under environmentally friendly conditions.

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壳聚糖在弱碱性NaHCO3/尿素水溶液中的流变性能及凝胶行为

来源于可再生资源的可持续聚合物材料在解决环境挑战方面变得越来越重要。壳聚糖是甲壳素的衍生物，由于其独特的生物和物理化学性质，具有非凡的潜力。然而，它的实际应用受到溶解和加工通常所需的苛刻条件的限制。在这里，我们展示了一种新的方法，使用NaHCO3/尿素水溶液作为弱碱性溶剂体系，在温和的条件下实现了壳聚糖的高效加工。通过综合流变学分析，我们揭示了壳聚糖在NaHCO3/尿素水溶液中的溶胶-凝胶转变是由氢键、疏水相互作用和链缠结的协同相互作用控制的。壳聚糖的凝胶行为与壳聚糖的浓度和分子量密切相关，分子量越高，在较低温度下形成的网络越稳定。值得注意的是，我们发现了一种可逆的溶胶-凝胶过渡机制，可以通过温度调节精确控制材料性能，同时保持长期稳定性，尽管在储存过程中分子特性发生了适度的变化。这些发现促进了我们对弱碱性介质中多糖自组装的理解，并为在环境友好条件下开发可控壳聚糖基材料建立了新的范例。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Macromolecules 工程技术-高分子科学

CiteScore

9.30

自引率

16.40%

发文量

942

审稿时长

2 months

期刊介绍： Macromolecules publishes original, fundamental, and impactful research on all aspects of polymer science. Topics of interest include synthesis (e.g., controlled polymerizations, polymerization catalysis, post polymerization modification, new monomer structures and polymer architectures, and polymerization mechanisms/kinetics analysis); phase behavior, thermodynamics, dynamic, and ordering/disordering phenomena (e.g., self-assembly, gelation, crystallization, solution/melt/solid-state characteristics); structure and properties (e.g., mechanical and rheological properties, surface/interfacial characteristics, electronic and transport properties); new state of the art characterization (e.g., spectroscopy, scattering, microscopy, rheology), simulation (e.g., Monte Carlo, molecular dynamics, multi-scale/coarse-grained modeling), and theoretical methods. Renewable/sustainable polymers, polymer networks, responsive polymers, electro-, magneto- and opto-active macromolecules, inorganic polymers, charge-transporting polymers (ion-containing, semiconducting, and conducting), nanostructured polymers, and polymer composites are also of interest. Typical papers published in Macromolecules showcase important and innovative concepts, experimental methods/observations, and theoretical/computational approaches that demonstrate a fundamental advance in the understanding of polymers.