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Neutron capture therapy, such as boron neutron capture therapy (BNCT) and gadolinium neutron capture therapy (GdNCT), has been attracting much attention as a next-generation radiotherapy. Nanoparticles containing both boron and gadolinium can accumulate in tumours because of the enhanced permeability and retention (EPR) effect, thereby simultaneously rendering the benefits of BNCT and GdNCT. In this study, we obtained flake-shaped gadolinium borate (GdBO3) nanoparticles, approximately 80 nm in length and 20 nm in width, by hydrothermal treatment of a solution containing gadolinium chloride, boric acid, and polyethylene glycol at 220 °C for 24 h. These GdBO3 nanoparticles did not show any serious cytotoxic effect against human umbilical vein endothelial cells over a concentration range of 3–300 µg·mL–1. The results suggest that GdBO3 nanoparticles can accumulate in tumours because of the EPR effect and can function as boron and gadolinium nanocarriers for neutron capture therapy. However, further in vitro and in vivo studies are needed for the application of these nanoparticles in neutron capture therapy. [ABSTRACT FROM AUTHOR]

Octacalcium phosphate (OCP; Ca8(HPO4)2(PO4)4 ∙ 5H2O) is a precursor of hydroxyapatite found in human bones and teeth, and is among the inorganic substances critical for hard tissue formation and regeneration in the human body. OCP has a layered structure and can incorporate carboxylate ions into its interlayers. However, studies involving the incorporation of tetracarboxylic and multivalent (pentavalent and above) carboxylic acids into OCP have not yet been reported. In this study, we investigate the incorporation of pyromellitic acid (1,2,4,5-benzenetetracarboxylic acid), a type of tetracarboxylic acid, into OCP. We established that pyromellitate ions could be incorporated into OCP by a wet chemical method using an acetate buffer solution containing pyromellitic acid. The derived OCP showed a brilliant blue emission under UV light owing to the incorporated pyromellitate ions. Incorporation of a carboxylic acid into OCP imparted new functions, which could enable the development of novel functional materials for biomedical applications. Octacalcium phosphate is a precursor to a key component of human bone and tooth enamel which can incorporate carboxylate species, but the effect of multivalent carboxylates is not well understood. Here the incorporation of tetracarboxylic acids into OCP is shown to influence the structural and optical properties of the resultant composite. [ABSTRACT FROM AUTHOR]

Raw silk has the potential to be a flexible, osteoconductive material because it forms bone-like apatite on its surface in acellular simulated body fluid with ion concentrations nearly 1.5 times greater than that of human plasma (1.5SBF). It has been reported that silk—which has many similarities to raw silk—develops antibacterial properties when heated in inert gas, which may be advantageous in preventing bacterial infection. Hence, raw silk heated in inert gas may be a flexible, osteoconductive material with antibacterial activity. Thus, we examined the effect of the heat treatment of raw silk fabric on its apatite-forming ability in 1.5SBF and on the growth of Escherichia coli. Raw silk fabric was heated in argon gas at several temperatures, to a maximum of 500 °C. The results of soaking tests in 1.5SBF indicate that the apatite-forming ability of raw silk decreases with increasing temperature. This may be because favourable structures for apatite formation, such as carboxyl groups, are thermally decomposed. The results of bacterial tests indicate that raw silk fabrics heated to 300 °C or 500 °C exhibit reduced bacterial growth compared to those that were not heated or were heated only to 100 °C. This might be because hydrophobic surfaces inhibit bacterial adhesion, or because the thermal decomposition of sericin—a component of raw silk—leads to a lack of available nutrients for the bacteria. Although this study did not demonstrate the expected material properties needed for clinical applications, this research contributes to a better understanding of silk biomaterials. [ABSTRACT FROM AUTHOR]

Common cancer treatments are invasive and lack specificity, leading to unwanted side effects. Because hyperthermia can kill cancer cells and damage proteins and structures within cells, it has been considered a novel, minimally invasive cancer treatment. However, many hyperthermia treatments cannot heat deep-seated tumors effectively and locally. Heat-generating magnetic microspheres can help address this challenge. However, current research has not produced microspheres that can be sufficiently heated. We prepared magnetic titania (TiO) microspheres by introducing magnetite nanoparticles (MNPs) into the sol-gel process during water-in-oil emulsion for in situ hyperthermia treatment of cancers. Two types of MNPs were used in this study: One type was synthesized by a chemical coprecipitation method, and the other type was commercially available MNPs. The obtained microspheres contained up to 46.7 wt% MNPs, and their saturation magnetization and coercive force were 34.2 emu/g and 103 Oe, respectively. The particles' in vitro heating efficiency in an agar phantom was measured in an alternating magnetic field of 300 Oe and 100 kHz. The temperature increase in the agar phantom within 300 s was 4.5 °C for microspheres with MNPs that were synthesized by chemical coprecipitation and 53 °C for microspheres with commercially available MNPs. The excellent heating efficiency of the microspheres may be attributed to the hysteresis losses of the magnetic particles. These microspheres are believed to be promising thermoseeds for hyperthermic treatment of cancer. Graphical abstract: [Figure not available: see fulltext.][Figure not available: see fulltext.] Magnetic TiO microspheres with a diameter of 7-15 μm were obtained by directly introducing preformed magnetic MNPs into a sol-gel process from TTIP in water-in-oil emulsion. The magnetic TiO microspheres containing FeO at a content higher than 46 wt% increased the temperature of the agar phantom to above 43 °C in 3 min. They are expected to be useful for arterial embolization hyperthermic treatment of cancer, but control of their diameter is essential. [ABSTRACT FROM AUTHOR]

Bone cement containing alumina particles with a specific crystalline structure exhibits the ability to bond with bone. These particles (AL-P) are mainly composed of delta-type alumina (δ-AlO). It is likely that some of the proteins present in the body environment are adsorbed onto the cement and influence the expression of its bioactivity. However, the effect that this adsorption of proteins has on the bone-bonding mechanism of bone cement has not yet been elucidated. In this study, we investigated the characteristics of the adsorption of bovine serum albumin (BSA) onto AL-P and compared them with those of its adsorption onto hydroxyapatite (HA), which also exhibits bone-bonding ability, as well as with those of adsorption onto alpha-type alumina (α-AlO), which does not bond with bone. The adsorption characteristics of BSA onto AL-P were very different from those onto α-AlO but quite similar to those onto HA. It is speculated that BSA is adsorbed onto AL-P and HA by interionic interactions, while it is adsorbed onto α-AlO by electrostatic attraction. The results suggest that the specific adsorption of albumin onto implant materials might play a role in the expression of the bone-bonding abilities of the materials. [ABSTRACT FROM AUTHOR]

Recently, organic-inorganic hybrids composed of derivatives of dextran, a polysaccharide, and magnetite nanoparticles have attracted much attention as novel thermoseeds. If they can be fabricated into microspheres of size 20-30 μm, they are expected to show not only hyperthermia effects but also embolization effects in human liver and kidney cancers. In this study, we examined the fabrication of carboxymethyldextran/magnetite microspheres using a water/oil emulsion as the reaction medium. Improvement of the chemical stability of the microcapsules by coating with silica using a sol-gel process was also investigated. The obtained hollow microspheres contained particles of size 20-30 μm. Silica coating using an appropriate catalyst for hydrolysis and polycondensation of alkoxysilanes was found to be effective for preventing dissolution and collapse in simulated body environments. [ABSTRACT FROM AUTHOR]

We prepared iron nanoparticle-encapsulating silica (FeSi) microspheres and tested their suitability as thermal seeds for hyperthermia in cancer therapy. These microspheres were prepared by introducing a ferric ion (Fe) into microspheres of a SiO gel matrix derived from the hydrolysis of tetramethoxysilane in a water-in-oil emulsion that was then heat-treated at 850 °C in an argon atmosphere. The particles obtained were 5-30 μm in size and had a saturation magnetization up to 21 emu g and a coercive force of 86-133 Oe. Heat generation in an alternating current magnetic field of 300 Oe at 100 kHz was estimated to be 7.7-28.9 W g. The in vitro cell biocompatibility of the microspheres was assessed by culturing rat fibroblast Rat-1 cells in medium supplemented with microspheres containing 6.7 % of iron nanoparticles. At microsphere concentrations of <7.5 g L proliferation of Rat-1 cells was not significantly inhibited. [ABSTRACT FROM AUTHOR]

We prepared low-crystalline apatite nanoparticles and coated them onto a surface of a Au/Cr-plated quartz substrate by the electrophoretic deposition (EPD) method or by using a self-assembled monolayer of 11-mercaptoundecanoic acid (SAM method). Low-crystalline apatite nanoparticles around 10 nm in size with extremely low contents of undesirable residual products were obtained by adding (NH)HPO aqueous droplets into a modified synthetic body fluid solution that contained Ca(CHCOO). The apatite nanoparticles were successfully coated by either the EPD method or the SAM method; the nanoparticle coating achieved by the SAM method was more uniform than that achieved by the EPD method. The present SAM method is expected to be a promising technique for obtaining a quartz substrate coated with apatite nanoparticles, which can be used as a quartz crystal microbalance device. [ABSTRACT FROM AUTHOR]

In this review, recent advances in bioceramics, metallic biomaterials, and their composites are discussed in terms of their material properties and new medical applications. Porous calcium phosphate ceramics have attracted a lot attention as scaffolds for tissue-engineering purposes since the porous structure allows bone ingrowth. The addition of biodegradable polymers like chitosan, gelatin, and collagen have modified the degradability of the ceramics and their mechanical properties. Titanium (Ti) alloys are being developed for the fabrication of medical devices for the replacement of hard tissue such as artificial hip joints, bone plates, and dental implants because they are very reliable from the viewpoint of mechanical performance. Physical treatment such as grooving or setting a spatial gap on the surface of materials is applicable to improve the apatite formation on the Ti alloys. Blood-compatible polymers such as poly(ethylene glycol) have been successfully fixed on the surface of Ti via chemical bonding by an electrodeposition method. New functions have been explored in Ni-free, Co-Cr-Mo alloys and Mg alloys. In addition, yttrium-containing or phosphorus-containing glass microspheres (20-30 μm in diameter) and ferrimagnetic ceramic particles have exhibited great potential to realize minimally invasive treatment of cancer without surgical operation via in situ radiotherapy or hyperthermia of cancer, but it is still a major challenge to clarify the biological reaction between the artificial implants and living body before their application. [ABSTRACT FROM AUTHOR]

Titania layers were successfully prepared on the surfaces of Ti-6Al-4V alloy via anodic oxidation in H2SO4 or Na2SO4 solutions at room temperature. The titania layers consisted of pure rutile or a mixture of anatase and rutile structures after the Ti-6Al-4V alloy had been anodized in 1.0 M H2SO4 solution at 150 V or 0.5M Na2SO4 solution at 100 or 130 V. Good apatite-forming ability was demonstrated in simulated body fluid. However, surface layers with mainly titanium metallic phase or a pure anatase structure did not possess the ability to induce apatite formation. Anodic oxidation is an effective method to prepare bioactive Ti-6Al-4V alloy that can be used as an artificial bone substitute under load-bearing applications. [ABSTRACT FROM AUTHOR]

Porous Y2O3 microparticles 500 μm in size were obtained, when 1 wt%-ammonium alginate aqueous solution was dropped into 0.5 M-YCl3 aqueous solution by a Pasteur pipette and the resultant gel microparticles were heat-treated at 1100°C. Small pores less than 1 μm were formed in the microparticles by the heat treatment. The bulk density of the heat-treated microparticle was as low as 0.66 g cm−3. The chemical durability of the heat-treated microparticles in simulated body fluid at pH = 6 and 7 was high enough for clinical application of in situ radiotherapy. Although the size of the microparticles should be decreased to around 25 μm using atomizing device such as spray gun for clinical application, we found that the porous Y2O3 microparticles with high chemical durability and low density can be obtained by utilizing gelation of ammonium alginate in YCl3 aqueous solution in this study. [ABSTRACT FROM AUTHOR]

Calcium phosphate crystals were synthesized by diffusing calcium ions into silica hydrogels containing phosphate ions. Hydroxyapatite [HAp, Ca10(PO4)6(OH)2] and octacalcium phosphate [OCP, Ca8(HPO4)2(PO4)4.5H2O] with different types of crystal morphology were formed in the gel. The HAp had an irregular or rod shape, a few micrometers in length, while the OCP had an irregular, spherulite, rod- or ribbonlike shape, ranging in size from a few micrometers to several tens of micrometers, depending on the amount of phosphoric acid added and the reaction temperature. The morphology of the OCP changed from an irregular shape to a ribbonlike or rod shape, via a spherulite shape, depending on the amount of phosphoric acid added and the reaction temperature. The degree of supersaturation of the reaction environment and the rate-determining step in the HAp and OCP crystal growth mechanism have been ascribed to the changes in crystal morphology of the HAp and OCP. [ABSTRACT FROM AUTHOR]

Ferrimagnetic materials can be expected to be useful as thermo seeds for hyperthermic treatment of cancer, especially where the cancer is located in deep parts of body, as they can generate heat by magnetic hysteretic loss when they are placed in an alternating magnetic field. Recently, it was reported that ferrimagnetic maghemite (γ-Fe2O3) microspheres 20–30 μm in diameter prepared in aqueous solution can show excellent heat generating ability. However, these microspheres have many cracks on their surfaces. In this study, the preparation conditions for the microspheres was further optimized in order to obtain crack-free ferrimagnetic microspheres, and the in vitro heat generation of the obtained microspheres was measured in an agar phantom under an alternating magnetic field. Crack-free γ-Fe2O3 microspheres 20–30 μm in diameter were obtained successfully. Their saturation magnetization and coercive force were 68 emu g−1 and 198 Oe, respectively. Their heat generation under an alternating magnetic field of 300 Oe at 100 kHz was estimated to be 42 W g−1. The microspheres showed in vitro heat generation when they were dispersed in an agar phantom and placed under an alternating magnetic field. It is believed that these microspheres may be useful for the in situ hyperthermic treatment of cancer. [ABSTRACT FROM AUTHOR]

Titanium and its alloys have been widely used for orthopedic implants because of their good biocompatibility. We have previously shown that the crystalline titania layers formed on the surface of titanium metal via anodic oxidation can induce apatite formation in simulated body fluid, whereas amorphous titania layers do not possess apatite-forming ability. In this study, hot water and heat treatments were applied to transform the titania layers from an amorphous structure into a crystalline structure after titanium metal had been anodized in acetic acid solution. The apatite-forming ability of titania layers subjected to the above treatments in simulated body fluid was investigated. The XRD and SEM results indicated hot water and/or heat treatment could greatly transform the crystal structure of titania layers from an amorphous structure into anatase, or a mixture of anatase and rutile. The abundance of Ti–OH groups formed by hot water treatment could contribute to apatite formation on the surface of titanium metals, and subsequent heat treatment would enhance the bond strength between the apatite layers and the titanium substrates. Thus, bioactive titanium metals could be prepared via anodic oxidation and subsequent hot water and heat treatment that would be suitable for applications under load-bearing conditions. [ABSTRACT FROM AUTHOR]

A rectangular specimen of polyethylene terephthalate (PET) was soaked in a titania solution composed of titanium isopropoxide, water, ethanol and nitric acid at 25 °C for 1 h. An amorphous titanium oxide was formed uniformly on the surface of PET specimen, but did not form an apatite on its surface in a simulated body fluid (SBF) within 3 d. The PET plate formed with the amorphous titanium oxide was subsequently soaked in water or HCl solutions with different concentrations at 80 °C for different periods of time. The titanium oxide on PET was transformed into nano-sized anatase by the water treatment and into nano-sized brookite by 0.10 M HCl treatment at 80 °C for 8 d. The former did not form the apatite on its surface in SBF within 3 d, whereas the latter formed the apatite uniformly on its surface. Adhesive strength of the titanium oxide and apatite layers to PET plate was increased by pre-treatment of PET with 2 wt% NaOH solution at 40 °C for 2 h. A two-dimensional fabric of PET fibers 24 μm in diameter was subjected to the NaOH pre-treatment at 40 °C, titania solution treatment at 25 °C and subsequent 0.10 M HCl treatment at 80 °C. Thus treated PET fabric formed the apatite uniformly on surfaces of individual fibers constituting the fabric in SBF within 3 d. Two or three dimensional PET fabrics modified with the nano-sized brookite on surfaces of the individual fibers constituting the fabric by the present method are believed to be useful as flexible bone substitutes, since they could be integrated with living bone through the apatite formed on their constituent fibers. [ABSTRACT FROM AUTHOR]

An apatite layer was successfully formed on titanium substrates by electrochemical deposition in a metastable calcium phosphate solution, which had 1.5 times the ion concentrations of a normal simulated body fluid, but did not contain MgCl2·6H2O, at 41 °C for 40 or 60 min at 13 mA. The current did not produce large effects on the crystalline size of the apatite, but the thickness of the apatite layer could be controlled by deposition conditions such as electrolyte temperature, current and deposition time. It is expected that the present electrochemical deposition will be useful to rapidly coat apatite on metallic materials. [ABSTRACT FROM AUTHOR]

Poly(tetramethylene oxide) (PTMO)–CaO–Ta2O5 hybrids were prepared by hydrolysis and polycondensation of triethoxysilane-functionalized PTMO (Si–PTMO), tantalum ethoxide (Ta(OEt)5) and CaCl2. In the system CaO-free PTMO–Ta2O5, Si–PTMO/Ta(OEt)5 weight ratios were 30/70, 40/60 and 50/50 (hybrids PT30Ca0, PT40Ca0 and PT50Ca0, respectively). In the system PTMO–CaO–Ta2O5, the Si–PTMO/Ta(OEt)5 weight ratio was 40/60 and CaCl2/Ta(OEt)5 mole ratios were 0.05, 0.10 and 0.15 (hybrids PT40Ca5, PT40Ca10 and PT40Ca15, respectively). Crack-free transparent monolithic hybrids were obtained for all the examined compositions except for PT30Ca0. Even CaO-free hybrids PT40Ca0 and PT50Ca0 formed apatite on their surfaces in a simulated body fluid (SBF) within 14 days. Hybrid PT40Ca0 showed higher mechanical strength, which was increased by soaking in SBF, and larger strain to failure than human cancellous bone. The CaO-containing hybrids showed higher apatite-forming ability than the CaO-free hybrids, and its apatite-forming ability increased with increasing CaO content. Hybrids PT40Ca10 and PT40Ca15 formed apatite within 3 days. The mechanical strength of PT40Ca15 was, however, lower than PT40Ca0 and was decreased by soaking in SBF. Thus obtained flexible bioactive CaO-free PTMO–Ta2O5 hybrids are expected to be useful as bone substitutes. [ABSTRACT FROM AUTHOR]