Inspired by the highly ordered nanostructure of bone, nanodopant composite biomaterials are gaining special attention for their ability to guide bone tissue regeneration through structural and biological cues. However, bone malformation in orthopedic surgery is a lingering issue, partly due to the high surface energy of traditional nanoparticles contributing to aggregation and inhomogeneity. Recently, carboxyl-functionalized synthetic polymers have been shown to mimic the carboxyl-rich surface motifs of non-collagenous proteins in stabilizing hydroxyapatite and directing intrafibrillar mineralization in-vitro. Based on this biomimetic approach, it is herein demonstrated that carboxyl functionalization of poly(lactic-co-glycolic acid) can achieve great material homogeneity in nanocomposites. This ionic colloidal molding method stabilizes hydroxyapatite precursors to confer even nanodopant packing, improving therapeutic outcomes in bone repair by remarkably improving mechanical properties of nanocomposites and optimizing controlled drug release, resulting in better cell in-growth and osteogenic differentiation. Lastly, better controlled biomaterial degradation significantly improved osteointegration, translating to highly regular bone formation with minimal fibrous tissue and increased bone density in rabbit radial defect models. Ionic colloidal molding is a simple yet effective approach of achieving materials homogeneity and modulating crystal nucleation, serving as an excellent biomimetic scaffolding strategy to rebuild natural bone integrity.
DNA tetrahedron nanostructure (DTNs) has the merits of simple synthesis, high yield, structural stability, and mechanical rigidity, and its three-dimensional structure provides a satisfactory biosensing interface to the improvement of the binding efficiency of antigenic proteins and antibodies. Electrochemiluminescence (ECL) reagent, tris-(4,4′-dicarboxylicacid-2,2′-bipyridyl)ruthenium(II) dichloride (Ru(dcbpy) 3 Cl 2 ), was modified on the electrode through the formation of classical sandwich complex of antibody− antigen−antibody. ECL response of the system increased with the increment of the target (golgi protein 73 (GP73) in this study) with high selectivity. Besides, the composed double-stranded DNA (dsDNA) in each side of DTNs could act as an excellent carrier of methylene blue (MB), thus producing a stable electrochemical internal reference signal on the electrode surface to correct the potential interferences. Therefore, a highly selective and reproductive ratiometric immunosensor was developed on the basis of the ratio of ECL of Ru(dcbpy) 3 Cl 2 and electrochemistry of MB. The ratio value of the ECL/ electrochemistry had a linear relationship with GP73 concentration in the range of 15 pg/mL−0.7 ng/mL, and the limit of detection was 15 pg/mL. The proposed ratiometric ECL immunoassay has been applied to detect GP73 in real serum samples with satisfactory results.
The abnormal expression of pyrophosphatase (PPase) is closely related to many diseases and malignant tumors, so the detection for PPase is of great significance in clinical diagnosis, disease monitoring, and other biomedical aspects. In this study, a sensitive and specific electrochemiluminescence (ECL) biosensor combined highly specific Cu + -catalyzed azide-alkyne cycloaddition (CuAAC) with high efficiency of hybridization chain reaction (HCR) for the purpose of detecting pyrophosphatase has been designed. Highly efficient hybridization chain reaction amplification processed in homogeneous solution and the amplification products were connected to the electrode surface in one step, which solved the problem of low DNA amplification efficiency on the electrode surface because of the steric hindrance. Ru(phen) 3 2+ was embedded into the dsDNA and functioned as ECL probes; the enhanced ECL intensity of the system had a linear relationship with the logarithm of PPase concentration in the range of 0.025−50 mU with a detection limit of 8 μU. The method was proved to be of good specificity, repeatability, and stability that could be used for screening and quantitatively determining pyrophosphatase inhibitor sodium fluoride. The practicability of this method in clinical application has been proved through the detection of serum from the clinical arthritis patients. Moreover, the method can be used to monitor PPase activity of arthritis patients before and after administration to provide reference for the effect of drug treatment.
We present a highly adaptable design platform for multi-responsive, multilayered composite nanoparticles (MC-NPs) with fine-tunable functional layers. A flexible disulfide-linked nanogel template is obtained by a controlled in-situ gelation method, enabling a high degree of control over each successive layer. From this template, we optimize “smart” biomaterials with biofunctional surfaces, tunable drug release kinetics, and magnetic or pH-responsive functionality, fabricated into MC-NPs for targeted drug release and periosteum-mimetic structures for controlled rhBMP-2 release towards bone tissue formation in-vivo. Such a versatile platform for the design of MC-NPs is a powerful tool that shows considerable therapeutic potential in clinical fields such as oncology and orthopedics.
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