Hydrogels are extracellular-matrix-like biomimetic materials that have wide biomedical applications in tissue engineering and drug delivery. However, most hydrogels cannot simultaneously fulfill the mechanical and cell compatibility requirements. In the present study, we prepared a semi-interpenetrating network composite gel (CG) by incorporating short chain chitosan (CS) into a covalent tetra-armed poly(ethylene glycol) network. In addition to satisfying physicochemical, mechanics, biocompatibility, and cell affinity requirements, this CG easily encapsulated acetylsalicylic acid (ASA) via electrostatic interactions and chain entanglement, achieving sustained release for over 14 days and thus promoting periodontal ligament stem cell (PDLSC) proliferation and osteogenic differentiation. In vivo studies corroborated the capacity of PDLSCs and ASA-laden CG to enhance new bone regeneration in situ using a mouse calvarial bone defect model. This might be attributed to PDLSCs and host mesenchymal stem cells expressing monocyte chemoattractant protein-1, which upregulated M2 macrophage recruitment and polarization in situ , indicating its appealing potential in bone tissue engineering.
Development of artificial biomaterials by mimicking extracellular matrix of bone tissue is a promising strategy for bone regeneration. Hydrogel has emerged as a type of viable substitute, but its inhomogeneous networks and weak mechanics greatly impede clinical applications. Here, a dual crosslinked gelling system is developed with tunable architectures and mechanics to promote osteogenic capacity. Polyhedral oligomeric silsesquioxane (POSS) is designated as a rigid core surrounded by six disulfide‐linked PEG shells and two 2‐ureido‐4[1H]‐pyrimidinone (UPy) groups. Thiol‐disulfide exchange is employed to fabricate chemical network because of the pH‐responsive “on/off” function. While self‐complementary UPy motif is capable of optimizing local microstructure to enhance mechanical properties. Taking the merits of biocompatibility and high‐mechanics in periodontal ligament stem cells (PDLSCs) proliferation, attachment, and osteogenesis, hybrid hydrogel exhibits outstanding osteogenic potential both in vitro and in vivo. Importantly, it is the first time that a key epigenetic regulator of ten‐eleven translocation 2 (Tet2) is discovered to significantly elevate the continuously active the WNT/β‐catenin through Tet2/HDAC1/E‐cadherin/β‐catenin signaling cascade, thereby promoting PDLSCs osteogenesis. This work represents a general strategy to design the hydrogels with customized networks and biomimetic mechanics, and illustrates underlying osteogenic mechanisms that will extend the design rationales for high‐functional biomaterials in tissue engineering.
A novel surface modification technique was developed to provide a copper nickel alloy (M) surface with bactericidal and anticorrosion properties for inhibiting biocorrosion. 4-(chloromethyl)-phenyl tricholorosilane (CTS) was first coupled to the hydroxylated alloy surface to form a compact silane layer, as well as to confer the surface with chloromethyl functional groups. The latter allowed the coupling of 4-vinylpyridine (4VP) to generate the M-CTS-4VP surface with biocidal functionality. Subsequent surface graft polymerization of 4VP, in the presence of benzoyl peroxide (BPO) initiator, from the M-CTS-4VP surface produced the poly(4-vinylpyridine) (P(4VP)) grafted surface, or the M-CTS-P(4VP) surface. The pyridine nitrogen moieties on the M-CTS-P(4VP) surface were quaternized with hexylbromide to produce a high concentration of quaternary ammonium groups. Each surface functionalization step was ascertained by X-ray photoelectron spectroscopy (XPS) and static water contact angle measurements. The alloy with surface-quaternized pyridinium cation groups (N+) exhibited good bactericidal efficiency in a Desulfovibrio desulfuricans-inoculated seawater-based modified Barr's medium, as indicated by viable cell counts and fluorescence microscopy (FM) images of the surface. The anticorrosion capability of the organic layers was verified by the polarization curve and electrochemical impedance spectroscopy (EIS) measurements. In comparison, the pristine (surface hydroxylated) Cu-Ni alloy was found to be readily susceptible to biocorrosion under the same environment.
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