In conventional polymer materials, mechanical performance is traditionally engineered via material structure, using motifs such as polymer molecular weight, polymer branching, or copolymer-block design1. Here, by means of a model system of 4-arm poly(ethylene glycol) hydrogels crosslinked with multiple, kinetically distinct dynamic metal-ligand coordinate complexes, we show that polymer materials with decoupled spatial structure and mechanical performance can be designed. By tuning the relative concentration of two types of metal-ligand crosslinks, we demonstrate control over the material’s mechanical hierarchy of energy-dissipating modes under dynamic mechanical loading, and therefore the ability to engineer a priori the viscoelastic properties of these materials by controlling the types of crosslinks rather than by modifying the polymer itself. This strategy to decouple material mechanics from structure may inform the design of soft materials for use in complex mechanical environments.

Control of hierarchical polymer mechanics with bioinspired metal-coordination dynamics

Owing to their unique chemical and physical properties, hydrogels are attracting increasing attention in both basic and translational biomedical studies. Although the classical hydrogels with static networks have been widely reported for decades, a growing number of recent studies have shown that structurally dynamic hydrogels can better mimic the dynamics and functions of natural extracellular matrix (ECM) in soft tissues. These synthetic materials with defined compositions can recapitulate key chemical and biophysical properties of living tissues, providing an important means to understanding the mechanisms by which cells sense and remodel their surrounding microenvironments. This review begins with the overall expectation and design principles of dynamic hydrogels. We then highlight recent progress in the fabrication strategies of dynamic hydrogels including both degradation-dependent and degradation-independent approaches, followed by their unique properties and use in biomedical applications such as regenerative medicine, drug delivery, and 3D culture. Finally, challenges and emerging trends in the development and application of dynamic hydrogels are discussed.

Structurally Dynamic Hydrogels for Biomedical Applications: Pursuing a Fine Balance between Macroscopic Stability and Microscopic Dynamics.

Natural biopolymer-based conductive hydrogels, which combine inherent renewable, nontoxic features, biocompatibility and biodegradability of biopolymers, and excellent flexibility and conductivity ...

Recent Progress in Natural Biopolymers Conductive Hydrogels for Flexible Wearable Sensors and Energy Devices: Materials, Structures, and Performance

Recent trends in organic coating based on biopolymers and biomass for controlled and slow release fertilizers.

Herein, a new type of injectable carboxymethyl chitosan (CMCh) hydrogel wound dressing with self-healing properties is constructed. First, CMCh samples are homogeneously synthesized in alkali/urea aqueous solutions. Subsequently, trivalent metal ions of Fe3+ and Al3+ are introduced to form coordination bonds with CMCh, leading to an ultrafast gelation process. A series of hydrogels can be obtained by altering the concentration of CMCh and the relative content of metal ions. Owing to the dynamic and reversible characteristics of the coordination bonds, the hydrogel exhibits self-healing, self-adaption, and thermoresponsive ability. Moreover, due to the interaction between the amino groups on CMCh and SO42-, the hydrogel undergoes phase separation and can be painlessly detached from the skin with little residue. Taking advantage of all these characteristics, the hydrogel is used as a wound dressing and can significantly accelerate skin tissue regeneration and wound closure. This hydrogel has great potential in the application of tissue engineering.

Ultrafast Fabrication of Self-Healing and Injectable Carboxymethyl Chitosan Hydrogel Dressing for Wound Healing.

Ionically Crosslinked chitosan/poly(acrylic Acid) Hydrogels With High Strength, Toughness and Antifreezing Capability

Chitin and chitosan have been extensively used as wound dressings because of their special functions to promote wound healing. However, there was little focus on the effects of the degree of acetyl...

Effect of the Degree of Acetylation of Chitin Nonwoven Fabrics for Promoting Wound Healing

Hydrogel-based multifunctional materials have attracted much attention. In this work, novel mineralized hydrogels were fabricated through physically cross-linked polyvinylpyrrolidone (PVP) and CaCO3. The mineralized hydrogels were prepared by simply mixing CaCl2, Na2CO3, and PVP in aqueous solutions. The CO32- induced the aggregation of the PVP chains and the CaCO3 particles in situ generated in the aqueous solution worked as fillers to strengthen the hydrogels. Based on this method, other kinds of mineralized hydrogels were prepared by replacing the Ca2+ with different metal ions. The mineralized hydrogels displayed shapeable, self-healing and thixotropic properties. Moreover, the mineralized hydrogel-based sensor showed good and stable sensitivity to compressive pressure, and could be used to monitor human actions. This work presents a facile method for preparing mineralized hydrogels, which are promising for various applications due to their outstanding properties.

Self-healing and easy-to-shape mineralized hydrogels for iontronics

Wound healing is a clinical challenge, and nontoxic, nonadherent wound dressings that promote healing are urgently needed. Herein, hydroxybutyl chitosans (HBCSs) with the degree of substitution (DS...

Homogeneously Synthesized Hydroxybutyl Chitosans in Alkali/Urea Aqueous Solutions as Potential Wound Dressings

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