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Octacalcium phosphate (OCP) is a calcium phosphate compound with a layered structure in which apatite layers, which have a structure similar to hydroxyapatite, and hydrated layers are stacked alternately. OCP can incorporate various carboxylate ions into its interlayers. OCPs with incorporated carboxylate ions, also known as OCP carboxylates (OCPCs), are organically modified at the molecular level. OCPCs are an attractive research target in a wide range of fields, from basic inorganic chemistry to applied materials chemistry. Therefore, it is expected that a comprehensive overview of recent research on OCPCs will be useful in progressing this field. This review focuses on recent advances in OCPCs, namely their synthesis, the identification of new types of carboxylate ions that can be incorporated into OCP interlayers, the steric structure estimation of the interlayer carboxylate ions, and applications of OCPCs as functional materials. OCPC-based functional materials include fluorescent materials, artificial bones, and adsorbents. Furthermore, based on existing studies, challenges in OCPC research and future research directions are described.

Bone is a highly vascularized tissue with a unique and complex structure. Long bone consists of a peripheral cortical shell containing a network of channels for vascular penetration and an inner highly vascularized bone marrow space. Bioprinting is a powerful tool to enable rapid and precise spatial patterning of cells and biomaterials. Here we developed a two-step digital light processing technique to fabricate a bone-mimetic 3D hydrogel construct based on octacalcium phosphate (OCP), spheroids of human umbilical vein endothelial cells (HUVEC), and gelatin methacrylate (GelMA) hydrogels. The bone-mimetic 3D hydrogel construct was designed to consist of a peripheral OCP-containing GelMA ring to mimic the cortical shell, and a central GelMA ring containing HUVEC spheroids to mimic the bone marrow space. We further demonstrate that OCP, which is evenly embedded in the GelMA, stimulates the osteoblastic differentiation of mesenchymal stem cells. We refined the design of a spheroid culture device to facilitate the rapid formation of a large number of HUVEC spheroids, which were embedded into different concentrations of GelMA hydrogels. It is shown that the concentration of GelMA modulates the extent of formation of the capillary-like structures originating from the HUVEC spheroids. This cell-loaded hydrogel-based bone construct with a biomimetic dual ring structure can be potentially used for bone tissue engineering.

Many studies have shown that it is important to use bone grafts that are easy to mold, bioabsorbable, and stable over time. We focused on Type H blood vessels, which were discovered by Kusumbe et al. in 2014 to be responsible for the interaction between angiogenesis and osteogenesis. The aim of this study was to assess the effect of octacalcium phosphate collagen (OCP/Col), on the healing processes of the extraction socket and the alveolar bone surrounding the extraction socket. Ridge preservation of rat lower first molars was conducted using OCP/Col, and a series of experiments involving micro-CT scanning, observations of new bone, bone morphometry measurements, histological and immunohistochemical analyses, and second harmonic generation imaging were conducted to analyze bone mass, bone quality, angiogenesis, and mechanical properties. The results demonstrate that the calcification level was not very high when using OCP/Col for RP. Moreover, the newly formed bone is rich in vascular components and collagen fibers that are essential for bone tissue remodeling. These characteristics of OCP/Col in RP could contribute significantly to the construction of a rich vascular network around dental implants immediately after implant placement and the subsequent acquisition of osseointegration and reconstruction of the surrounding tissue.

Octacalcium phosphate (OCP) has attracted much attention as an artificial bone substitute because of its excellent osteoconductive and bone replacement properties. Although numerous studies have investigated OCP powder fabrication, there are only a few studies on OCP block fabrication. Therefore, in this study, the feasibility of optimizing dicalcium hydrogen phosphate dihydrate (DCPD) blocks, as a precursor for OCP block fabrication, under a pH 6 adjusted acetate buffer solution at 70 °C for 2 days was investigated. When a DCPD block was immersed in acetate buffer, the block was partially converted to OCP, with a large amount of dicalcium hydrogen phosphate anhydrate (DCPA), and its macroscopic structure was maintained. When the DCPD block was immersed in a Ca-containing solution, it was converted to mainly hydroxyapatite (HAp) with DCPA. On the other hand, when the DCPD block was immersed in a PO4-containing solution, the block was converted to OCP, and its macroscopic structure was maintained. In other words, the PO4-induced calcium phosphate with a Ca/P molar ratio lower than 1.0 may represent an intermediate phase during the compositional transformation from a DCPD block to an OCP block through the dissolution–precipitation reaction.

Mesenchymal stem cells (MSCs) are a promising candidate for bone repair. However, the maintenance of MSCs injected into the bone injury site remains inefficient. A potential approach is to develop a bone-liked platform that incorporates MSCs into a biocompatible 3D scaffold to facilitate bone grafting into the desired location. Bone tissue engineering is a multistep process that requires optimizing several variables, including the source of cells, osteogenic stimulation factors, and scaffold properties. This study aims to evaluate the proliferation and osteogenic differentiation potentials of MSCs cultured on 2 types of 3D-printed hydroxyapatite, including a 3D-printed HA and biomimetic calcium phosphate-coated 3D-printed HA. MSCs from bone marrow (BM-MSCs) and umbilical cord (UC-MSCs) were cultured on the 3D-printed HA and coated 3D-printed HA. Scanning electron microscopy and immunofluorescence staining were used to examine the characteristics and the attachment of MSCs to the scaffolds. Additionally, the cell proliferation was monitored, and the ability of cells to differentiate into osteoblast was assessed using alkaline phosphatase (ALP) activity and osteogenic gene expression. The BM-MSCs and UC-MSCs attached to a plastic culture plate with a spindle-shaped morphology exhibited an immunophenotype consistent with the characteristics of MSCs. Both MSC types could attach and survive on the 3D-printed HA and coated 3D-printed HA scaffolds. The MSCs cultured on these scaffolds displayed sufficient osteoblastic differentiation capacity, as evidenced by increased ALP activity and the expression of osteogenic genes and proteins compared to the control. Interestingly, MSCs grown on coated 3D-printed HA exhibited a higher ALP activity and osteogenic gene expression than those cultured on the 3D-printed HA. The finding indicated that BM-MSCs and UC-MSCs cultured on the 3D-printed HA and coated 3D-printed HA scaffolds could proliferate and differentiate into osteoblasts. Thus, the HA scaffolds could provide a suitable and favorable environment for the 3D culture of MSCs in bone tissue engineering. Additionally, biomimetic coating with octacalcium phosphate may improve the biocompatibility of the bone regeneration scaffold.

The present paper reviews the methods and the performance of in situ formation of calcium phosphates (CaP) for the conservation of materials belonging to cultural heritage. The core idea is to form CaP (ideally hydroxyapatite, HAP, the most stable CaP at pH > 4) by reaction between the substrate and an aqueous solution of a phosphate salt. Initially proposed for the conservation of marble and limestone, the treatment has been explored for a variety of different substrates, including sandstones, sulphated stones, gypsum stuccoes, concrete, wall paintings, archaeological bones and paper. First, the studies aimed at identifying the best treatment conditions (e.g., nature and concentration of the phosphate precursor, solution pH, treatment duration, ionic and organic additions to the phosphate solution, mineralogical composition of the new CaP phases) are summarized. Then, the treatment performance on marble and limestone is reviewed, in terms of protective and consolidating effectiveness, compatibility (aesthetic, microstructural and physical) and durability. Some pilot applications in real case studies are also reported. Recent research aimed at extending the phosphate treatment to other substrates is then illustrated. Finally, the strengths of the phosphate treatment are summarized, in comparison with alternative products, and some aspects needing future research are outlined.

The inflammatory-associated corrosion of metallic dental and orthopedic implants causes significant complications, which may result in the implant’s failure. The corrosion resistance can be improved with coatings and surface treatments, but at the same time, it might affect the ability of metallic implants to undergo proper osteointegration. In this work, alginate hydrogels with and without octacalcium phosphate (OCP) were made on 3D-printed (patterned) titanium alloys (Ti Group 2 and Ti-Al-V Group 23) to enhance their anticorrosion properties in simulated normal, inflammatory, and severe inflammatory conditions in vitro. Alginate (Alg) and OCP-laden alginate (Alg/OCP) hydrogels were manufactured on the surface of 3D-printed Ti substrates and were characterized with wettability analysis, XRD, and FTIR. The electrochemical characterization of the samples was carried out with open circuit potential, potentiodynamic polarization, and electrochemical impedance spectroscopy (EIS). It was observed that the hydrophilicity of Alg/OCP coatings was higher than that of pure Alg and that OCP phase crystallinity was increased when samples were subjected to simulated biological media. The corrosion resistance of uncoated and coated samples was lower in inflammatory and severe inflammatory environments vs. normal media, but the hydrogel coatings on 3D-printed Ti layers moved the corrosion potential towards more nobler values, reducing the corrosion current density in all simulated solutions. These measurements revealed that OCP particles in the Alg hydrogel matrix noticeably increased the electrical charge transfer resistance at the substrate and coating interface more than with Alg hydrogel alone.

Tibia trabeculae and vertebrae of rats as well as human femur were investigated by high-resolution TEM at the atomic scale in order to reveal snapshots of the morphogenetic processes of local bone ultrastructure formation. By taking into account reflections of hydroxyapatite for Fourier filtering the appearance of individual alpha–chains within the triple–helix clearly shows that bone bears the feature of an intergrowth composite structure extending from the atomic to the nanoscale, thus representing a molecular composite of collagen and apatite. Careful Fourier analysis reveals that the non–collagenous protein osteocalcin is present directly combined with octacalcium phosphate. Besides single spherical specimen of about 2 nm in diameter, osteocalcin is spread between and over collagen fibrils and is often observed as pearl necklace strings. In high-resolution TEM, the three binding sites of the γ-carboxylated glutamic acid groups of the mineralized osteocalcin were successfully imaged, which provide the chemical binding to octacalcium phosphate. Osteocalcin is attached to the collagen structure and interacts with the Ca–sites on the (100) dominated hydroxyapatite platelets with Ca-Ca distances of about 9.5 Å. Thus, osteocalcin takes on the functions of Ca–ion transport and suppression of hydroxyapatite expansion.

The critical factor determining the in vivo effect of bone repair materials is the microenvironment, which greatly depends on their abilities to promote vascularization and bone formation. However, implant materials are far from ideal candidates for guiding bone regeneration due to their deficient angiogenic and osteogenic microenvironments. Herein, a double-network composite hydrogel combining vascular endothelial growth factor (VEGF)-mimetic peptide with hydroxyapatite (HA) precursor was developed to build an osteogenic microenvironment for bone repair. The hydrogel was prepared by mixing acrylated β-cyclodextrins and octacalcium phosphate (OCP), an HA precursor, with gelatin solution, followed by ultraviolet photo-crosslinking. To improve the angiogenic potential of the hydrogel, QK, a VEGF-mimicking peptide, was loaded in acrylated β-cyclodextrins. The QK-loaded hydrogel promoted tube formation of human umbilical vein endothelial cells and upregulated the expression of angiogenesis-related genes, such as Flt1, Kdr, and VEGF, in bone marrow mesenchymal stem cells. Moreover, QK could recruit bone marrow mesenchymal stem cells. Furthermore, OCP in the composite hydrogel could be transformed into HA and release calcium ions facilitating bone regeneration. The double-network composite hydrogel integrated QK and OCP showed obvious osteoinductive activity. The results of animal experiments showed that the composite hydrogel enhanced bone regeneration in skull defects of rats, due to perfect synergistic effects of QK and OCP on vascularized bone regeneration. In summary, improving the angiogenic and osteogenic microenvironments by our double-network composite hydrogel shows promising prospects for bone repair.

Calcium phosphate (CaP) materials are biocompatible and non-toxic to the body. However, they lack biointegration, exhibit a low resorption rate and can cause fibrous encapsulation throughout the implant material. A promising approach for dental or orthopedic regeneration is the use of dicalcium phosphate dihydrate (DCPD) and octacalcium phosphate (OCP), as they are well-suited to bone components. From a novel perspective, these apatites can be used as drug carriers for individuals with low tolerance to common excipients. In this study, the transformation of DCPD into different morphologies in DMEM was investigated using an induced dissolution and reprecipitation reaction solution. The DCPD transformation time was observed to be morphology-dependent and can occur between 48 and 168 h. In the interaction with simulated body fluid (SBF), simulated gastric fluid (SGF) and a combination of both (BFS/SGF), a higher mass loss was observed in SGF (~80%) than in the other fluids (~35%). The structural changes presented in DCPD and OCP before and after immersion in physiological fluids were analyzed by ATR-FTIR, SEM, XRD and EDS. The obtained OCP showed low stability in SGF compared to SBF and SBF/SGF, which indicates that it may be a suitable candidate for drug delivery in the digestive tract.