Mechanical Performance of Polyampholyte Hydrogels Influenced by Ionic Bond Strength under Isochoric Conditions

IF 5.1 1区化学 Q1 POLYMER SCIENCE

Macromolecules Pub Date : 2025-03-17 DOI:10.1021/acs.macromol.4c02420

Xueyu Li, Haruna Tsuchibora, Ya Nan Ye, Kunpeng Cui, Takayuki Kurokawa

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Abstract

Hydrogels composed of hierarchical structures are notable for their exceptional strength and toughness. Understanding the toughening mechanisms associated with these hierarchical structures is essential for the application and design of tough soft materials. Using polyampholyte hydrogels as a model system, this study introduces a novel approach that combines electrolyte-induced ionic bond dissociation with PEG-induced osmotic stress to systematically investigate how ionic bond strength and phase separation influence mechanical properties under isochoric conditions. We reveal that increasing electrolyte concentrations induces a structural transition from strong bicontinuous phase-separated networks to a homogeneous structure and eventually to weak bicontinuous phase-separated networks, accompanied by characteristic relaxation times that initially decrease and subsequently increase. This transition leads to abnormal nonmonotonic changes in mechanical properties. We further elucidate that the nonmonotonic behavior in fracture stress and work of extension to fracture, along with self-recovery dynamics, is governed by the phase-separated structural transition, while variations in fracture energy are primarily related to the dynamics of ionic bonds. This work provides valuable insights into the design of tough soft materials through the modulation of the strengths of physical associations.

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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.