Simultaneous Substitution of Fe and Sr in Beta-Tricalcium Phosphate: Synthesis, Structural, Magnetic, Degradation, and Cell Adhesion Properties

β-tricalcium phosphate is a promising bone graft substitute material with biocompatibility and high osteoinductivity. However, research on the ideal degradation and absorption for better clinical application remains a challenge. Now, we focus on modifying physicochemical properties and improving biological properties through essential ion co-substitution (Fe and Sr) in β-TCPs. Fe- and Sr-substituted and Fe/Sr co-substituted β-TCP were synthesized by aqueous co-precipitation with substitution levels ranging from 0.2 to 1.0 mol%. The β-TCP phase was detected by X-ray diffraction and Fourier transform infrared spectroscopy. Changes in Ca–O and P–O bond lengths of the co-substituted samples were observed through X-ray photoelectron spectroscopy. The results of VSM represent the M-H graph having a combination of diamagnetic and ferromagnetic properties. A TRIS–HCl solution immersion test showed that the degradation and resorption functions act synergistically on the surface of the co-substituted sample. Cell adhesion tests demonstrated that Fe enhances the initial adhesion and proliferation behavior of hDPSCs. The present work suggests that Fe and Sr co-substitution in β-TCP can be a candidate for promising bone graft materials in tissue engineering fields. In addition, the possibility of application of hyperthermia for cancer treatment can be expected.

[1]  Giovanni Urruth,et al.  Influence of dopants on thermal stability and densification of β-tricalcium phosphate powders , 2021 .

[2]  Wudan Li,et al.  Hydroxyapatite Based Materials for Bone Tissue Engineering: A Brief and Comprehensive Introduction , 2021, Crystals.

[3]  S. Hiromoto,et al.  Effects of Incorporating Β-Tricalcium Phosphate with Reaction Sintering into Mg-Based Composites on Degradation and Mechanical Integrity , 2021, Metals.

[4]  Seog-Young Yoon,et al.  Fe-doped tricalcium phosphates: crystal structure and degradation behavior , 2020, Materials Research Express.

[5]  E. Salahi,et al.  Effect of Heat Treatment on Grain Growth of Magnetic Nanocrystalline Hydroxyapatite Powder , 2020 .

[6]  S. Shih,et al.  Preparation, characterization and investigation of antibacterial silver-zinc co-doped β-tricalcium phosphate by spray pyrolysis , 2020 .

[7]  M. Bohner,et al.  β-Tricalcium Phosphate for Bone Substitution: Synthesis and Properties. , 2020, Acta biomaterialia.

[8]  F. Goetz-Neunhoeffer,et al.  Cu2+ doped β-tricalcium phosphate: Solid solution limit and crystallographic characterization by rietveld refinement , 2020 .

[9]  A. Bakulin,et al.  Radio frequency magnetron sputtering of Sr- and Mg-substituted β-tricalcium phosphate: Analysis of the physicochemical properties and deposition rate of coatings , 2020 .

[10]  R. Panneerselvam,et al.  Impact of different transition metal ions in the structural, mechanical, optical, chemico-physical and biological properties of nanohydroxyapatite , 2020 .

[11]  Xing‐dong Zhang,et al.  A bioceramic scaffold composed of strontium-doped three-dimensional hydroxyapatite whiskers for enhanced bone regeneration in osteoporotic defects , 2020, Theranostics.

[12]  S. Bose,et al.  Regulation of Osteogenic Markers at Late Stage of Osteoblast Differentiation in Silicon and Zinc Doped Porous TCP , 2019, Journal of functional biomaterials.

[13]  Tao Xu,et al.  Three-dimensional Printed Mg-Doped β-TCP Bone Tissue Engineering Scaffolds: Effects of Magnesium Ion Concentration on Osteogenesis and Angiogenesis In Vitro , 2019, Tissue Engineering and Regenerative Medicine.

[14]  Durga Sankar Vavilapalli,et al.  Thermally Modified Iron-Inserted Calcium Phosphate for Magnetic Hyperthermia in an Acceptable Alternating Magnetic Field. , 2019, The journal of physical chemistry. B.

[15]  M. Gazzano,et al.  Strontium and Zinc Substitution in β-Tricalcium Phosphate: An X-ray Diffraction, Solid State NMR and ATR-FTIR Study , 2019, Journal of functional biomaterials.

[16]  J. Chevalier,et al.  Effect of grain orientation and magnesium doping on β-tricalcium phosphate resorption behavior. , 2019, Acta biomaterialia.

[17]  P. Janoš,et al.  Effect of Iron Impurities on Magnetic Properties of Nanosized CeO2 and Ce-Based Compounds , 2019, Metals.

[18]  Nathaniel S. Hwang,et al.  Bioactive calcium phosphate materials and applications in bone regeneration , 2019, Biomaterials Research.

[19]  Sui-lin Liu,et al.  Fe/Zn-modified tricalcium phosphate (TCP) biomaterials: preparation and biological properties , 2019, RSC advances.

[20]  A. M. Aragon,et al.  Exchange-spring behavior below the exchange length in hard-soft bilayers in multidomain configurations , 2018, Physical Review B.

[21]  S. Lei,et al.  Simultaneous co-substitution of Sr2+/Fe3+ in hydroxyapatite nanoparticles for potential biomedical applications , 2018, Ceramics International.

[22]  Teddy Tite,et al.  Cationic Substitutions in Hydroxyapatite: Current Status of the Derived Biofunctional Effects and Their In Vitro Interrogation Methods , 2018, Materials.

[23]  P. Shetty,et al.  Hyperthermia effect and antibacterial efficacy of Fe3+ /Co2+ co-substitutions in β-Ca3 (PO4 )2 for bone cancer and defect therapy. , 2018, Journal of biomedical materials research. Part B, Applied biomaterials.

[24]  M. Ginebra,et al.  In vitro degradation of calcium phosphates: Effect of multiscale porosity, textural properties and composition. , 2017, Acta biomaterialia.

[25]  M. Srivastava,et al.  Iron doped β-Tricalcium phosphate: Synthesis, characterization, hyperthermia effect, biocompatibility and mechanical evaluation. , 2017, Materials science & engineering. C, Materials for biological applications.

[26]  A. Srivastava,et al.  Effect of temperature on the magnetic properties of nano-sized M-type barium hexagonal ferrites , 2017 .

[27]  J. Ratnayake,et al.  Substituted hydroxyapatites for bone regeneration: A review of current trends. , 2017, Journal of biomedical materials research. Part B, Applied biomaterials.

[28]  A. Tampieri,et al.  Strontium doped calcium phosphate coatings on poly(etheretherketone) (PEEK) by pulsed electron deposition , 2017 .

[29]  G. A. Davydova,et al.  Tricalcium Phosphate Ceramics Doped with Silver, Copper, Zinc, and Iron (III) Ions in Concentrations of Less Than 0.5 wt.% for Bone Tissue Regeneration , 2017 .

[30]  S. Panseri,et al.  Sr-substituted bone cements direct mesenchymal stem cells, osteoblasts and osteoclasts fate , 2017, PloS one.

[31]  S. Bose,et al.  Effects of Iron on Physical and Mechanical Properties, and Osteoblast Cell Interaction in β-Tricalcium Phosphate , 2017, Annals of Biomedical Engineering.

[32]  M. Bohner,et al.  Hydrogen-substituted β-tricalcium phosphate synthesized in organic media , 2016, Acta crystallographica Section B, Structural science, crystal engineering and materials.

[33]  A. Waseem,et al.  A review of Human Biomonitoring studies of trace elements in Pakistan. , 2016, Chemosphere.

[34]  Monica Montesi,et al.  Novel Osteointegrative Sr-Substituted Apatitic Cements Enriched with Alginate , 2016, Materials.

[35]  Liyong He,et al.  Effects of strontium substitution on the phase transformation and crystal structure of calcium phosphate derived by chemical precipitation , 2016 .

[36]  P. Bhattacharya,et al.  Nutritional Aspects of Essential Trace Elements in Oral Health and Disease: An Extensive Review , 2016, Scientifica.

[37]  G. A. Davydova,et al.  Iron-substituted tricalcium phosphate ceramics , 2016, Doklady Chemistry.

[38]  V. Sglavo,et al.  Effect of Mg(2+) doping on beta-alpha phase transition in tricalcium phosphate (TCP) bioceramics. , 2016, Acta biomaterialia.

[39]  J. Ferreira,et al.  Antibiotic-loaded Sr-doped porous calcium phosphate granules as multifunctional bone grafts , 2016 .

[40]  G. A. Davydova,et al.  Copper-substituted tricalcium phosphates , 2016, Doklady Chemistry.

[41]  A. Bandyopadhyay,et al.  Doped tricalcium phosphate scaffolds by thermal decomposition of naphthalene: Mechanical properties and in vivo osteogenesis in a rabbit femur model. , 2015, Journal of biomedical materials research. Part B, Applied biomaterials.

[42]  M. Glogauer,et al.  Mechanisms of in Vivo Degradation and Resorption of Calcium Phosphate Based Biomaterials , 2015, Materials.

[43]  Monika Šupová,et al.  Substituted hydroxyapatites for biomedical applications: A review , 2015 .

[44]  Zohaib Khurshid,et al.  Biodegradable Materials for Bone Repair and Tissue Engineering Applications , 2015, Materials.

[45]  J. Jansen,et al.  Influence of ceramic disk material, surface hemispheres, and SBF volume on in vitro mineralization. , 2015, Journal of biomedical materials research. Part A.

[46]  M. Gelinsky,et al.  Strontium modified calcium phosphate cements - approaches towards targeted stimulation of bone turnover. , 2015, Journal of materials chemistry. B.

[47]  K. Mishima,et al.  Microscopic study on resorption of β-tricalcium phosphate materials by osteoclasts , 2015, Cytotechnology.

[48]  S. Kalkura,et al.  Physicochemical and biological properties of iron and zinc ions co-doped nanocrystalline hydroxyapatite, synthesized by ultrasonication , 2014 .

[49]  E. Montoneri,et al.  Paramagnetic iron-doped hydroxyapatite nanoparticles with improved metal sorption properties. A bioorganic substrates-mediated synthesis. , 2014, ACS applied materials & interfaces.

[50]  M. Bohner,et al.  Performance of β-tricalcium phosphate granules and putty, bone grafting materials after bilateral sinus floor augmentation in humans. , 2014, Biomaterials.

[51]  Alessio Adamiano,et al.  Biomimetic magnesium-carbonate-apatite nanocrystals endowed with strontium ions as anti-osteoporotic trigger. , 2014, Materials science & engineering. C, Materials for biological applications.

[52]  M. Otsuka,et al.  Bone Regeneration of Rat Tibial Defect by Zinc-Tricalcium Phosphate (Zn-TCP) Synthesized from Porous Foraminifera Carbonate Macrospheres , 2013, Marine drugs.

[53]  Zhongyong Fan,et al.  Degradation and osteogenic potential of a novel poly(lactic acid)/nano-sized β-tricalcium phosphate scaffold , 2012, International journal of nanomedicine.

[54]  S. Bose,et al.  Osteoclastogenesis and osteoclastic resorption of tricalcium phosphate: effect of strontium and magnesium doping. , 2012, Journal of biomedical materials research. Part A.

[55]  C. Hung,et al.  Intrinsically superparamagnetic Fe-hydroxyapatite nanoparticles positively influence osteoblast-like cell behaviour , 2012, Journal of Nanobiotechnology.

[56]  S. Dorozhkin,et al.  Biphasic, triphasic and multiphasic calcium orthophosphates. , 2012, Acta biomaterialia.

[57]  R. Carrodeguas,et al.  α-Tricalcium phosphate: synthesis, properties and biomedical applications. , 2010, Acta biomaterialia.

[58]  A. Bandyopadhyay,et al.  Understanding the influence of MgO and SrO binary doping on the mechanical and biological properties of beta-TCP ceramics. , 2010, Acta biomaterialia.

[59]  Huipin Yuan,et al.  Osteoinductive ceramics as a synthetic alternative to autologous bone grafting , 2010, Proceedings of the National Academy of Sciences.

[60]  M. Gazzano,et al.  Ionic substitutions in calcium phosphates synthesized at low temperature. , 2010, Acta biomaterialia.

[61]  J. Ferreira,et al.  Synthesis and structural characterization of strontium- and magnesium-co-substituted beta-tricalcium phosphate. , 2010, Acta biomaterialia.

[62]  J. Ferreira,et al.  Brushite-Forming Mg-, Zn- and Sr-Substituted Bone Cements for Clinical Applications , 2010, Materials.

[63]  N. Matsumoto,et al.  Preparation and characterization of beta-tricalcium phosphate co-doped with monovalent and divalent antibacterial metal ions. , 2009, Acta biomaterialia.

[64]  S. Yamada,et al.  Beta-tricalcium phosphate and basic fibroblast growth factor combination enhances periodontal regeneration in intrabony defects in dogs. , 2009, Dental materials journal.

[65]  J. M. Merino,et al.  Magnetic properties of ZnO nanoparticles. , 2007, Nano letters.

[66]  A. Bandyopadhyay,et al.  Calcium Phosphate‐Based Resorbable Ceramics: Influence of MgO, ZnO, and SiO2 Dopants , 2006 .

[67]  D. Massiot,et al.  Effect of Sodium Doping in β-Tricalcium Phosphate on Its Structure and Properties , 2006 .

[68]  Katsumi Yoshida,et al.  Substitution Model of Monovalent (Li, Na, and K), Divalent (Mg), and Trivalent (Al) Metal Ions for β‐Tricalcium Phosphate , 2006 .

[69]  P. Marie.  Strontium as therapy for osteoporosis. , 2005, Current opinion in pharmacology.

[70]  P. Buma,et al.  Mechanism of bone incorporation of beta-TCP bone substitute in open wedge tibial osteotomy in patients. , 2005, Biomaterials.

[71]  Yong Han,et al.  Development of a strontium-containing hydroxyapatite bone cement. , 2005, Biomaterials.

[72]  F. Müller,et al.  Influence of magnesium doping on the phase transformation temperature of beta-TCP ceramics examined by Rietveld refinement. , 2005, Biomaterials.

[73]  S. P. Nielsen.  The biological role of strontium , 2004 .

[74]  S. Pors Nielsen.  The biological role of strontium. , 2004, Bone.

[75]  M. Sayer,et al.  Density functional study of structural, electronic and vibrational properties of mg- and zn-doped tricalcium phosphate biomaterials. , 2002, Biomaterials.

[76]  Takayuki Ishibashi,et al.  Room Temperature Ferromagnetism in Novel Diluted Magnetic Semiconductor Cd1¡xMnxGeP2 , 2000 .

[77]  B. Ratner,et al.  Surface characterization of hydroxyapatite and related calcium phosphates by XPS and TOF-SIMS. , 2000, Analytical chemistry.

[78]  M. Gazzano,et al.  Isomorphous substitutions in β-tricalcium phosphate: The different effects of zinc and strontium , 1997 .

[79]  P. Aggett,et al.  Physiology and metabolism of essential trace elements: an outline. , 1985, Clinics in endocrinology and metabolism.

[80]  W. Mertz.  The essential trace elements. , 1981, Science.

[81]  W. E. Brown,et al.  Crystallographic studies of the role of Mg as a stabilizing impurity in β-Ca3(PO4)2. II. Refinement of Mg-containing β-Ca3(PO4)2 , 1977 .