Papers by Author: Fukue Nagata

Abstract: Tantalum-containing phosphate invert glasses were prepared using a liquid phase method under ambient conditions. In our previous study, the ion-releasing behavior (i.e. chemical durability) of phosphate glasses was controlled by the amount of intermediate oxides. In this work, Ta₂O₅ (intermediate oxide) was used to improve the chemical durability of the glasses. Ta-containing phosphate invert glasses were prepared and their structures were characterized. X-ray diffraction (XRD) patterns of the glasses exhibited broad halos, indicating an amorphous state. The amount of P₂O₅ in the glasses increased with increasing Ta₂O₅ content, while the amount of CaO decreased. The glasses prepared with a nominal P : Ta molar ratio of 2 : 1 showed a value of 1.87 : 1. Thus, almost all the Ta used in the synthesis was contained in the resulting glass. Raman spectra showed bands corresponding to short phosphate units such as ortho-and pyrophosphate, and the P-O-P peak was blue-shifted with increasing Ta₂O₅ content. The P-O-Ta bonds were formed with TaO₄ tetrahedra, as new peaks at 970 cm^-1 (P-O-Ta bonds) and 825 cm^-1 (observed in YTaO₄) were observed. The glasses containing higher amounts of Ta₂O₅ exhibited TaO₆-rich phases, as shown by the Raman band at 630 cm^-1 (Ta-O-Ta bonds) and broad XRD peaks at 2θ = 5 ~ 10°. Therefore, Ta in the phosphate invert glasses prepared by the liquid-phase method crosslinks phosphate units in the form of TaO₄ tetrahedra, and the excess Ta exists in the form of TaO₆ octahedra as a network modifier and/or Ta₂O₅-rich phase.

Abstract: Natural bone is a complex material with well-designed architecture. To achieve successful bone integration and regeneration, the constituent and structure of bone-repairing scaffolds need to be flexible and biocompatible. HAp, as the main composition of bone minerals, has excellent biocompatibility, while CMC comprised of a three-dimensional network were high flexibility. Therefore, CMC/HAp composite have been attracted attention due to the development of bone tissue engineering. In this work, carboxymethyl cellulose (CMC)/hydroxyapatite (Ca₁₀(PO₄)₆(OH)₂; HAp) composite have been developed as three-dimensional scaffold for bone tissue engineering. Scanning electron microscopy revealed that the CMC/HAp composite have sheet-like structure. The amount of precipitated HAp of CMC/HAp composite was investigated using Thermogravimetric analysis. The amount of precipitated HAp in products prepared with 100 mg CMC was 49.8 wt%, while the amount of precipitated HAp in products prepared with 1000 mg CMC was 22.3 wt%. These results revealed that the amount of precipitated HAp in CMC/HAp composite was affected by CMC amount as prepared.

Abstract: The surface structure of Hydroxyapatite (HAp) particles during hydrothermal synthesis and their protein adsorption behavior was investigated. The HAp particles were prepared by mixing calcium acetate solution and diammonium hydrogen phosphate solution by hydrothermal synthesis. When the temperature of mixture were heated up to 120°C, 150°C and 180°C, the HAp particles were collected during hydrothermal synthesis. The adsorption properties of proteins onto HAp were studied using three types of proteins: bovine serum albumin (BSA), myoglobin (MGB) and lysozyme (LSZ). Surface analysis by BET revealed that their pore volumes were decreased by increasing synthesis temperature. The adsorbed amount of BSA and LSZ per unit milligrams showed no obvious difference in all of the HAp particles prepared with synthesis temperature. In contrast, the amount of MGB adsorbed onto HAp particles synthesized at 120°C, 150°, and 180°C shows the decreasing with an increasing synthesis temperature. This result suggests that the adsorbed amount of MGB was decreased by decreasing pore volume of HAp particles.

Abstract: Deoxyribonucleic acid (DNA) adsorption onto particles has applications in biosensors, separation methods, and gene delivery. Mesoporous silica (MPS), which exhibits a high surface area and large pore volume, is used in these applications because its pore size is easily controlled and its surface functional groups are easily exchanged. In this study, three types of MPSs with different pore sizes (2.4, 5.6, and 11.8 nm) were functionalized with different aminosilane coupling reagents and the effects of the MPS pore size and surface functional groups on DNA adsorption were evaluated. As the pore size of MPS increased, MPSs with diethylenetriamine (–3NH₂) adsorbed higher amounts of DNA, whereas MPSs with hexylenediamine groups (–2HNH₂) adsorbed lower amounts of DNA. Moreover, the fitting of DNA adsorption equilibrium data to Langmuir and Freundlich isotherm models was investigated.

Abstract: A high magnetic field is a useful tool to control the crystal alignment of non-magnetic materials such as ceramics and polymers. In the case of Hydroxyapatite crystal, the a,b-axis is aligned parallel to the direction of an imposed magnetic field. This fact implies that the alignment of the c-axis is not controllable only using a high static magnetic field due to the freedom of the c-axis in a plane perpendicular to a magnetic field direction. In this study, a high static magnetic field and mold rotation was simultaneously so applied during a slip casting process as to align the c-axis of HAp poly crystals.

Abstract: Porous biodegradable microspheres were successfully obtained by an improvement single step and surfactant-free emulsion solvent evaporation method. The organic phase composed of PLA and dichloromethane was stirred in aqueous phase including Ca2+ ions to yield oil in water emulsion. During emulsification, stirring rate was increased so as to produce the W/O/W emulsion that results in microspheres with internal pores. The interface of internal water/oil was stable in W/O/W emulsion, which was explained that the bond between Ca2+ ions and carboxyl group of poly(lactic acid) would be stabilized the internal water/oil interface. Adding PO4 3- aqueous solution prompted to precipitate low crystallized hydroxyapatite on the external oil/water interface, and the precipitated hydroxyapatite would stabilizied microspheres formation. The resulting microspheres were approximately 100-500 µm with internal spherical pores of 10-200 µm in diameter. The porous biodegradable microspheres were expected to be utilized as injectable bone substitutes that allow bone ingrowth and bone regeneration.

Abstract: Protein loading on apatite hydrogel cake and its solubility was studied. A mixture of di-sodium hydrogen phosphate dodeca-hydrate and calcium chloride di-hydrate was dissolved in water, and kept at room temperature for 2 weeks in air or N2 atmosphere to make apatite hydrogel. The obtained apatite hydrogel contains carbonate ions, and its carbonate content strongly affect the aggregation of particles. With maturation period, the particle size of apatite hydrogel decreased in air, but increased in N2 atmosphere. The quantity of loaded Cytochrome C in apatite hydrogel formed in air was 0.490 wt%, while that in apatite hydrogel formed under N2 atmosphere was 0.305 wt%. But the quantity of loaded albumin in apatite hydrogel formed in air was less than that in apatite hydrogel formed under N2 atmosphere. The difference may be due to the relationship between isoelectric point of protein and apatite hydrogel. The apatite hydrogel containing protein was dried for 4 days in air at 40 % of relative humidity to make cakes, and the cakes were immersed in pure water or PBS solution. The dried specimen slowly dissolves in aqueous solution, and the decrease in weight of apatite cake prepared from hydrogel formed in air was larger than that from hydrogel formed under N2 atmosphere compared to the dissolved apatite, the released protein was less, which may be associated with recrystallization of the apatite hydrogel.