Hydrogels, because of their water-rich nature and soft mechanical characteristics that resemble those of skin tissues, are promising materials for artificial skin. Existing piezoresistive hydrogels combine unique tissue-like and sensory properties, but these materials are often plagued by problems such as poor mechanical properties and the requirement of an external power supply or batteries. Here, a tough and self-powered hydrogel based on a tough polyacrylonitrile hydrogel incorporating ferroelectric poly(vinylidene fluoride) (PAN-PVDF) is reported. The dipolar interactions between the PVDF and PAN chains cause an increase in the best electroactive β-phase PVDF percentage in the composites from 0 to 91.3%; thus, a maximum piezoelectric coefficient d 33 , 30 pC N −1 , was achieved for the hydrogels. Skin-like Young's modulus values (1.33− 4.24 MPa), stretchability (90−175%), and high toughness (1.23 MJ/m 2 ) were achieved simultaneously for the hydrogels. This tough gel is capable of generating an electrical signal output (≈30 mV and ≈2.8 μA) with a rapid response (≈31 ms) due to the stress-induced poling effect. Moreover, the gel can also precisely detect physiological signals (e.g., gesture, pulse, and words). This study provides a simple and efficient method for artificial skin with high toughness, self-power generation capability, fast response, low cost, and tissue-like properties.
Biopolymer based hydrogels are characteristic of their biocompatibility and capability of mimicking extracellular matrix structure to support cellular behavior. However, these hydrogels suffer from low mechanical properties, uncontrolled degradation, and insufficient osteogenic activity, which limits their applications in bone regeneration. In this study, we developed hybrid gelatin (Gel)/oxidized chondroitin sulfate (OCS) hydrogels that incorporated mesoporous bioactive glass nanoparticles (MBGNs) as bioactive fillers for bone regeneration. Gel-OCS hydrogels could be self-crosslinked in situ under physiological conditions in the presence of borax. The incorporation of MBGNs enhanced the crosslinking and accelerated the gelation. The gelation time decreased with increasing the concentration of MBGNs added. Incorporation of MBGNs in the hydrogels significantly improved the mechanical properties in terms of enhanced storage modulus and compressive strength. The injectability of the hydrogels was not significantly affected by the MBGN incorporation. Also, the proliferation and osteogenic differentiation of rat bone marrow mesenchymal stem cells in vitro and rat cranial defect restoration in vivo were significantly promoted by the hydrogels in the presence of MBGNs. The hybrid Gel-OCS/MBGN hydrogels show promising potential as injectable biomaterials or scaffolds for bone regeneration/repair applications given their tunable degradation and gelation behavior as well as favorable mechanical behavior and osteogenic activities.
Imitating the physiological microenvironment of living cell and tissues opens new avenues of research into the application of electricity to medical therapies. In this study, dynamic piezoelectric stimulation is generated in a dynamic culture because of the piezoelectric effect of the poly(vinylidene fluoride)−polypyrrole (PVDF−PPy) electroactive composite. Combined with PPy nanocones, dynamic piezoelectric signals are effectively and continuously provided to cells. In the presence of dynamic piezoelectric stimulation and PPy nanocones, PPy-PVDF NS samples show promoted bone mesenchymal stem cell (BMSCs) adhesion, spreadin, and osteogenic differentiation. On the basis of the results of this study, PPy nanocones and dynamic piezoelectric stimulation can be administered to modulate cell behavior, paving the way for the exploration of cellular responses to dynamic electrical stimulation.
Blood vessels play an important role in bone defect repair and growth, and a critical challenge of bone defect repair is the promotion of blood vessel formation. Most of the current methods promote vascularization by adding specific growth factors, which are costly and easy to inactivate. In this study, we developed a covalently cross‐linked aminated bioactive glass nanoparticle‐chondroitin sulfate methacrylate (ABGN‐CSMA) organic‐inorganic composite hydrogel with angiogenic properties. The amino groups of the ABGNs form covalent bonds with the carboxyl groups on CSMA. Surface amination modification of BGNs not only improved the dispersion of BGNs in CSMA but also significantly improved the mechanical properties of the composite hydrogel. The largest storage modulus (1200 Pa), the largest loss modulus (560 Pa) and the strongest resistance to deformation of the hydrogel are seen at 10% concentration of ABGNs. Simultaneously, the local pH stability and sustained ion release of the composite hydrogel are conducive to cell adhesion, proliferation, and angiogenesis. This work provides evidence for the development of covalently cross‐linked organic‐inorganic composite hydrogels with angiogenic properties.
Multifunctional hydrogel bioadhesives have great prospects in biomedical applications, but their design still faces great challenges, such as multiple and tedious chemical modifications. However, it is difficult to integrate injectable, self‐healing, and stimulus‐responsive properties together. A facile approach based on dynamic metal‐ligand coordination chemistry between chondroitin sulfate (CS) and Fe3+ in the design and synthesis of novel multifunctional metallohydrogel bioadhesives is reported. This CS‐based hydrogel not only has strong tissue adhesion superior to that of commercial fibrin glue, but also exhibits an excellent self‐healing ability and injectability, which are beneficial in the field of bioadhesives. Moreover, the hydrogels undergo a rapid gel–sol transformation in response to multiple external stimuli, including pH, ions, neutral molecules, and chemical redox reactions enabling the rapid removal of the bioadhesive. In addition, metallohydrogels are rapidly formed within 10 s, quick enough to promptly seal the tissue. Importantly, the multifunctional CS‐based bioadhesives are shown to exhibit good biocompatibility, thus allowing the developed materials to meet key requirements for next‐generation tissue adhesives.
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