{"title":"Rheological Properties and Gelation Behavior of Chitosan in a Weakly Alkaline NaHCO3/Urea Aqueous Solution","authors":"Haoyu Xin, Xuejie Yu, Yiwen Lu and Jie Cai*, ","doi":"10.1021/acs.macromol.4c0167310.1021/acs.macromol.4c01673","DOIUrl":null,"url":null,"abstract":"<p >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 NaHCO<sub>3</sub>/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 NaHCO<sub>3</sub>/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.</p>","PeriodicalId":51,"journal":{"name":"Macromolecules","volume":"58 10","pages":"5283–5295 5283–5295"},"PeriodicalIF":5.1000,"publicationDate":"2025-05-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Macromolecules","FirstCategoryId":"92","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.macromol.4c01673","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"POLYMER SCIENCE","Score":null,"Total":0}
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.
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.