Hydrogels
are important for stretchable and wearable multifunctional
sensors, but their application is limited by their low mechanical
strength and poor long-term stability. Herein, a conductive organohydrogel
with a 3D honeycomb structure was prepared by integrating carbon nanotubes
(CNTs) and carbon black (CB) into a poly(vinyl alcohol)/glycerol (PVA/Gly)
organohydrogel. Such a nanocomposite organohydrogel is built on a
physical cross-linking network formed by the hydrogen bonds among
PVA, glycerol, and water. CNTs and CB had an add-in synergistic impact
on the mechanical and electrical performances of the PVA/Gly organohydrogel
because of the distinct aspect ratios and geometric shapes. The prepared
organohydrogel integrated with a tensile strength of 4.8 MPa, a toughness
of 15.93 MJ m–3, and flexibility with an elongation
at break up to 640%. The organohydrogels also showed good antifreezing
feature, long-term moisture retention, self-healing, and thermoplasticity.
Sensors designed from these organohydrogels displayed high stretching
sensitivity to tensile strain and temperature, with a gauge factor
of 2.1 within a relatively broad strain range (up to ∼600%
strain), a temperature coefficient of resistance of −0.935%·°C–1, and long-term durability. The sensors could detect
full-range human physiological signals and respond to the change in
temperature, which are highly desired for multifunctional wearable
electronic devices.
Engineering a proper immune response following biomaterial implantation is essential to bone tissue regeneration. Herein, a biomimetically hierarchical scaffold composed of deferoxamine@poly(ε‐caprolactone) nanoparticles (DFO@PCL NPs), manganese carbonyl (MnCO) nanosheets, gelatin methacryloyl hydrogel, and a polylactide/hydroxyapatite (HA) matrix is fabricated to augment bone repair by facilitating the balance of the immune system and bone metabolism. First, a 3D printed stiff scaffold with a well‐organized gradient structure mimics the cortical and cancellous bone tissues; meanwhile, an inside infusion of a soft hydrogel further endows the scaffold with characteristics of the extracellular matrix. A Fenton‐like reaction between MnCO and endogenous hydrogen peroxide generated at the implant‐tissue site triggers continuous release of carbon monoxide and Mn2+, thus significantly lessening inflammatory response by upregulating the M2 phenotype of macrophages, which also secretes vascular endothelial growth factor to induce vascular formation. Through activating the hypoxia‐inducible factor‐1α pathway, Mn2+ and DFO@PCL NP further promote angiogenesis. Moreover, DFO inhibits osteoclast differentiation and synergistically collaborates with the osteoinductive activity of HA. Based on amounts of data in vitro and in vivo, strong immunomodulatory, intensive angiogenic, weak osteoclastogenic, and superior osteogenic abilities of such an osteoimmunity‐regulating scaffold present a profound effect on improving bone regeneration, which puts forward a worthy base and positive enlightenment for large‐scale bone defect repair.
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