Surface State Control of Apatite Nanoparticles by pH Adjusters for Highly Biocompatible Coatings Kazuto Sugimoto, Ryota Akutsu, Shota Yamada, Tania Guadalupe Peñaflor Galindo, Motohiro Tagaya ACS Applied Materials and Interfaces, 2025 Apatite nanoparticles are biocompatible nanomaterials, so their film formation on biodevices is expected to provide effective bonding with living organisms. However, the biodevice-apatite interfaces have not yet been elucidated because there is little experimental evaluation and discussion on the nanoscale interactions, as well as the apatite surface reactivities. Our group has demonstrated the biomolecular adsorption properties on a quartz crystal microbalance with dissipation (QCM-D) sensor coated with apatite nanoparticles, demonstrating the applicability of apatite nanoparticle films on devices. Therefore, it is important to clarify the biodevice-apatite nanointerfaces by characterizing their physicochemical properties. This research aims to control the apatite nanoparticle surfaces using different types of pH adjusters as well as to investigate biodevice-apatite interfaces. In this study, tetramethylammonium hydroxide, sodium hydroxide, and potassium hydroxide were used to adjust the pH during the synthesis of apatite nanoparticles. As a result, it was found that the ratio of Ca-deficient hydroxyapatite phase to B-type carbonate ion-substituted hydroxyapatite phase could be controlled by adjusting the OH- concentration and that the formation of B-type carbonate ion substituted hydroxyapatite phase was demonstrated in terms of the charge compensation because hydrogen phosphate ion in the non-apatitic layer would be diffused and substituted inside the apatite core structure by the replacement of carbonate ion. By contrast, the phosphate ions in the core structure were moved and contained in the non-apatitic layer, and the proportion of phosphate ions in the non-apatitic layer increased. The surface changes of the nanoparticles provide an effective biodevice surface coating. It was observed that the thickness of the electrophoretically deposited nanoparticles clearly increased with the proportion of phosphate ions in the non-apatitic layer. Furthermore, the formation of the hydration layer with immersion in biological fluid was evaluated. It was inferred that the water molecules in the hydration layer interacted with the substituted ions and remained as nonfreezing water layer on the top surface of the nanoparticles, while the abundant phosphate ions newly interacted with the water molecules in the non-apatitic layer, thus increasing the proportion of intermediate water. These results indicated that the hydrogen phosphate and phosphate ions were retained in the non-apatitic layer on the top surfaces of apatite nanoparticles, so that the thickness of the electrophoretically deposited film and the weight fraction of the hydrated layer can be controlled by the component ratio of phosphate ions in the non-apatitic layer. It is expected that surface coating technology using apatite nanoparticles will be applied for biodevices.
Surface functionalization of hydroxyapatite nanoparticles for biomedical applications Takuya Kataoka, Zizhen Liu, Iori Yamada, Tania Guadalupe Peñaflor Galindo, Motohiro Tagaya Journal of Materials Chemistry B, 2024 This review described the highlight of surface engineering of hydroxyapatite nanoparticles and their interactions with ions and molecules, and summarized how the surface functionalization effectively work in biological situations.
Investigation of Surface Layers on Biological and Synthetic Hydroxyapatites Based on Bone Mineralization Process Kazuto Sugimoto, Yanni Zhou, Tania Guadalupe Peñaflor Galindo, Reo Kimura, Motohiro Tagaya Biomimetics, 2023 In this review, the current status of the influence of added ions (i.e., SiO44−, CO32−, etc.) and surface states (i.e., hydrated and non-apatite layers) on the biocompatibility nature of hydroxyapatite (HA, Ca10(PO4)6(OH)2) is discussed. It is well known that HA is a type of calcium phosphate with high biocompatibility that is present in biological hard tissues such as bones and enamel. This biomedical material has been extensively studied due to its osteogenic properties. The chemical composition and crystalline structure of HA change depending on the synthetic method and the addition of other ions, thereby affecting the surface properties related to biocompatibility. This review illustrates the structural and surface properties of HA substituted with ions such as silicate, carbonate, and other elemental ions. The importance of the surface characteristics of HA and its components, the hydration layers, and the non-apatite layers for the effective control of biomedical function, as well as their relationship at the interface to improve biocompatibility, has been highlighted. Since the interfacial properties will affect protein adsorption and cell adhesion, the analysis of their properties may provide ideas for effective bone formation and regeneration mechanisms.
Drug Molecular Immobilization and Photofunctionalization of Calcium Phosphates for Exploring Theranostic Functions Iori Yamada, Kota Shiba, Tania Guadalupe Peñaflor Galindo, Motohiro Tagaya Molecules, 2022 Theranostics (bifunction of therapeutics and diagnostics) has attracted increasing attention due to its efficiency that can reduce the physical and financial burden on patients. One of the promising materials for theranostics is calcium phosphate (CP) and it is biocompatible and can be functionalized not only with drug molecules but also with rare earth ions to show photoluminescence that is necessary for the diagnostic purpose. Such the CP-based hybrids are formed in vivo by interacting between functional groups of organic molecules and inorganic ions. It is of great importance to elucidate the interaction of CP with the photofunctional species and the drug molecules to clarify the relationship between the existing state and function. Well-designed photofunctional CPs will contribute to biomedical fields as highly-functional ormultifunctional theranostic materials at the nanoscales. In this review, we describe the hybridization between CPs and heterogeneous species, mainly focusing on europium(III) ion and methylene blue molecule as the representative photofunctional species for theranostics applications.
Investigation of Inclusion States of Silicate and Carbonate Ions in Hydroxyapatite Particles Prepared under the Presence of Sodium Silicate Tania Guadalupe Peñaflor Galindo, Kazuto Sugimoto, Shota Yamada, Taito Sugibuchi, Zizhen Liu, et al. Biomimetics, 2022 Biological hydroxyapatite (HA) contains the different minor ions which favour its bio-reactivity in vivo. In this study, the preparation of HA particles containing both silicate and carbonate ions under the presence of sodium silicate was investigated, and the physicochemical properties were evaluated according to the contents and states of silicate and carbonate ions. The increment in the silicate ion reduced the crystallinity and expanded the crystalline size along with a-axis. Solid-state 29Si–NMR spectra indicated the increase in the adsorption of oligomeric silicate species on the HA particle surfaces in addition to the substitution state of silicate ions, suggesting the occurrence of the surface coating of silicates on the surfaces. The possible states of carbonate and silicate ions at the HA surfaces will provide the bioactivity.
Effect of orotic acid addition on hydrolysis conversion of α-tricalcium phosphate to hydroxyapatite Iori Yamada, Tania Guadalupe Peñaflor Galindo, Daichi Noda, Motohiro Tagaya International Journal of Ceramic Engineering and Science, 2021 Alpha‐tricalcium phosphate (α‐TCP), which can be converted to calcium‐deficient hydroxyapatite (HA) by hydrolysis reaction, has been researched as a bone filling. Although the composites of α‐TCP with various organic molecules can exhibit a novel functionality, the reaction based on the addition of the interactive organic molecules has not been understood. Investigation of the hydrolysis conversion process under various conditions can lead to the elucidation of the biomineralization process. In this study, we investigated the hydrolysis conversion of α‐TCP to HA in the presence of orotic acid (Ort). As a result, the conversion rate from α‐TCP to HA at the reaction time of 3 h was improved to be more than five times as compared to that in the absence of Ort. Moreover, the addition of Ort promoted the crystal growth and suppressed the crystal growth in the m‐plane direction. Furthermore, the mechanism for promoting HA formation is assumed to be related to the molecular structure of Ort, which is capable of forming the interactions between carboxylate and Ca2+ ions.
Effect of Titanium Oxidized Treatment on Interfacial Characteristics of Ti/ZrO2 Sintered Bonding Materials N Aoyagi, K Kitamura, K Sekita, JFR Xiang, CK Lee, TGP Galindo Journal of the Japan Society of Powder and Powder Metallurgy 72 (Supplement … , 2025 2025
Evaluation of Compressive Strength for Sintered Porous Titanium Alloy and Composites with Biopolymers K Kimura, N Aoyagi, T Sorimachi, M Miyata, TGP Galindo Journal of the Japan Society of Powder and Powder Metallurgy 72 (Supplement … , 2025 2025
Surface state control of apatite nanoparticles by pH adjusters for highly biocompatible coatings K Sugimoto, R Akutsu, S Yamada, TG Peñaflor Galindo, M Tagaya ACS Applied Materials & Interfaces 17 (4), 7131-7141 , 2025 2025 Citations: 7
Hydroxyapatite nanoparticle films with designed nanostructures for advanced cell culture Z Liu, D Noda, W Shi, TGP Galindo, Y Otsuka, M Tagaya Nanoscale , 2025 2025 Citations: 1
Surface functionalization of hydroxyapatite nanoparticles for biomedical applications T Kataoka, Z Liu, I Yamada, TGP Galindo, M Tagaya Journal of Materials Chemistry B 12 (28), 6805-6826 , 2024 2024 Citations: 20
Investigation of surface layers on biological and synthetic hydroxyapatites based on bone mineralization process K Sugimoto, Y Zhou, TGP Galindo, R Kimura, M Tagaya Biomimetics 8 (2), 184 , 2023 2023 Citations: 24
Drug molecular immobilization and photofunctionalization of calcium phosphates for exploring theranostic functions I Yamada, K Shiba, TGP Galindo, M Tagaya Molecules 27 (18), 5916 , 2022 2022 Citations: 6
Investigation of Inclusion States of Silicate and Carbonate Ions in Hydroxyapatite Particles Prepared under the Presence of Sodium Silicate TG Peñaflor Galindo, K Sugimoto, S Yamada, T Sugibuchi, Z Liu, ... Biomimetics 7 (2), 40 , 2022 2022 Citations: 1
Surface modification of hydroxyapatite nanoparticles for bone regeneration by controlling their surface hydration and protein adsorption states Z Liu, S Yamada, Y Otsuka, TGP Galindo, M Tagaya Dalton Transactions 51 (25), 9572-9583 , 2022 2022 Citations: 34
AEMac, Autonomous Evolution Machine: A Leap for Innovative Problem Solving KR Sone- Yamagishi, P Sariego-Pasten, PGT Guadalupe International Journal of Scientific Research and Engineering Development 4 … , 2021 2021
Effect of orotic acid addition on hydrolysis conversion of α‐tricalcium phosphate to hydroxyapatite I Yamada, TGP Galindo, D Noda, M Tagaya International Journal of Ceramic Engineering & Science 3 (6), 267-271 , 2021 2021 Citations: 2
Synthesis of luminescent Eu (III)-doped octacalcium phosphate particles hybridized with succinate ions and their reactive behavior in simulated body fluid I Yamada, D Noda, K Shinozaki, TG Peñaflor Galindo, M Tagaya Crystal Growth & Design 21 (4), 2005-2018 , 2021 2021 Citations: 16
Interfacial Effect of Hydration Structures of Hydroxyapatite Nanoparticle Films on Protein Adsorption and Cell Adhesion States TG Peñaflor Galindo, M Tagaya ACS Applied Bio Materials 2 (12), 5559-5567 , 2019 2019 Citations: 11
Hydroxyapatite nanoparticle coating on polymer for constructing effective biointeractive interfaces TGP Galindo, Y Chai, M Tagaya Journal of Nanomaterials 2019 (1), 6495239 , 2019 2019 Citations: 112
Studies on preparation of surfactant-assisted elliptical hydroxyapatite nanoparticles and their protein-interactive ability TGP Galindo, I Yamada, S Yamada, M Tagaya Materials Chemistry and Physics 221, 367-376 , 2019 2019 Citations: 14
Particulate Titania Coating on Poly (Dimethylsiloxane) Films for Improving Osteoconductive Ability TG Peñaflor Galindo, K Shiba, M Tagaya Key Engineering Materials 782, 151-157 , 2018 2018
Desarrollo de una metodología para sintetizar el composito PDMS/TiO2/HAp con habilidades osteoconductivas TGP Galindo, M Tagaya, MM Rosales, JAC Jáuregui, GG García Naturaleza y Tecnología , 2018 2018
Osteoblast-like Cell Growth and Differentiation Behaviors on the Phospholipid Vesicle-Interacted Calcium Phosphate Films Y Chai, T Yamaguchi, TGP Galindo, M Tagaya e-Journal of Surface Science and Nanotechnology 16, 156-162 , 2018 2018 Citations: 3
Modification of poly (dimethylsiloxane) by mesostructured siliceous films for constructing protein-interactive surfaces Y Maruko, TGP Galindo, M Tagaya e-Journal of Surface Science and Nanotechnology 16, 41-48 , 2018 2018 Citations: 6
Síntesis de Materiales de Alto Impacto y Bajo Costo para Remoción De [F-] De Agua Para Consumo DMV Zamarripa, TGP Galindo, JMM Rosales JÓVENES EN LA CIENCIA 2 (1), 289-293 , 2016 2016
MOST CITED SCHOLAR PUBLICATIONS
Hydroxyapatite nanoparticle coating on polymer for constructing effective biointeractive interfaces TGP Galindo, Y Chai, M Tagaya Journal of Nanomaterials 2019 (1), 6495239 , 2019 2019.0 Citations: 112
Preparation of nanocrystalline zinc-substituted hydroxyapatite films and their biological properties TGP Galindo, T Kataoka, S Fujii, M Okuda, M Tagaya Colloid and Interface Science Communications 10, 15-19 , 2016 2016.0 Citations: 39
Surface modification of hydroxyapatite nanoparticles for bone regeneration by controlling their surface hydration and protein adsorption states Z Liu, S Yamada, Y Otsuka, TGP Galindo, M Tagaya Dalton Transactions 51 (25), 9572-9583 , 2022 2022.0 Citations: 34
Biodiesel production using layered double hidroxides and derived mixed oxides: The role of the synthesis conditions and the catalysts properties on biodiesel conversion GAF L.R. Reyna-Villanueva, J. M. Dias N.A. Medellín-Castillo, R. Ocampo ... Citations: 29
Investigation of surface layers on biological and synthetic hydroxyapatites based on bone mineralization process K Sugimoto, Y Zhou, TGP Galindo, R Kimura, M Tagaya Biomimetics 8 (2), 184 , 2023 2023.0 Citations: 24
Surface functionalization of hydroxyapatite nanoparticles for biomedical applications T Kataoka, Z Liu, I Yamada, TGP Galindo, M Tagaya Journal of Materials Chemistry B 12 (28), 6805-6826 , 2024 2024.0 Citations: 20
Synthesis of luminescent Eu (III)-doped octacalcium phosphate particles hybridized with succinate ions and their reactive behavior in simulated body fluid I Yamada, D Noda, K Shinozaki, TG Peñaflor Galindo, M Tagaya Crystal Growth & Design 21 (4), 2005-2018 , 2021 2021.0 Citations: 16
Morphosynthesis of Zn‐Substituted Stoichiometric and Carbonate Hydroxyapatite Nanoparticles and Their Cytotoxicity in Fibroblasts TG Peñaflor Galindo, T Kataoka, M Tagaya Journal of Nanomaterials 2015 (1), 376045 , 2015 2015.0 Citations: 16
Studies on preparation of surfactant-assisted elliptical hydroxyapatite nanoparticles and their protein-interactive ability TGP Galindo, I Yamada, S Yamada, M Tagaya Materials Chemistry and Physics 221, 367-376 , 2019 2019.0 Citations: 14
Interfacial Effect of Hydration Structures of Hydroxyapatite Nanoparticle Films on Protein Adsorption and Cell Adhesion States TG Peñaflor Galindo, M Tagaya ACS Applied Bio Materials 2 (12), 5559-5567 , 2019 2019.0 Citations: 11
Surface state control of apatite nanoparticles by pH adjusters for highly biocompatible coatings K Sugimoto, R Akutsu, S Yamada, TG Peñaflor Galindo, M Tagaya ACS Applied Materials & Interfaces 17 (4), 7131-7141 , 2025 2025.0 Citations: 7
Drug molecular immobilization and photofunctionalization of calcium phosphates for exploring theranostic functions I Yamada, K Shiba, TGP Galindo, M Tagaya Molecules 27 (18), 5916 , 2022 2022.0 Citations: 6
Modification of poly (dimethylsiloxane) by mesostructured siliceous films for constructing protein-interactive surfaces Y Maruko, TGP Galindo, M Tagaya e-Journal of Surface Science and Nanotechnology 16, 41-48 , 2018 2018.0 Citations: 6
Osteoblast-like Cell Growth and Differentiation Behaviors on the Phospholipid Vesicle-Interacted Calcium Phosphate Films Y Chai, T Yamaguchi, TGP Galindo, M Tagaya e-Journal of Surface Science and Nanotechnology 16, 156-162 , 2018 2018.0 Citations: 3
Effect of orotic acid addition on hydrolysis conversion of α‐tricalcium phosphate to hydroxyapatite I Yamada, TGP Galindo, D Noda, M Tagaya International Journal of Ceramic Engineering & Science 3 (6), 267-271 , 2021 2021.0 Citations: 2
Hydroxyapatite nanoparticle films with designed nanostructures for advanced cell culture Z Liu, D Noda, W Shi, TGP Galindo, Y Otsuka, M Tagaya Nanoscale , 2025 2025.0 Citations: 1
Investigation of Inclusion States of Silicate and Carbonate Ions in Hydroxyapatite Particles Prepared under the Presence of Sodium Silicate TG Peñaflor Galindo, K Sugimoto, S Yamada, T Sugibuchi, Z Liu, ... Biomimetics 7 (2), 40 , 2022 2022.0 Citations: 1
Effect of Titanium Oxidized Treatment on Interfacial Characteristics of Ti/ZrO2 Sintered Bonding Materials N Aoyagi, K Kitamura, K Sekita, JFR Xiang, CK Lee, TGP Galindo Journal of the Japan Society of Powder and Powder Metallurgy 72 (Supplement … , 2025 2025.0
Evaluation of Compressive Strength for Sintered Porous Titanium Alloy and Composites with Biopolymers K Kimura, N Aoyagi, T Sorimachi, M Miyata, TGP Galindo Journal of the Japan Society of Powder and Powder Metallurgy 72 (Supplement … , 2025 2025.0
AEMac, Autonomous Evolution Machine: A Leap for Innovative Problem Solving KR Sone- Yamagishi, P Sariego-Pasten, PGT Guadalupe International Journal of Scientific Research and Engineering Development 4 … , 2021 2021.0