Multifunctional bioceramic-based composites reinforced with silica-coated carbon nanotube core-shell structures

Abstract Carbon nanotube (CNT) possesses eminent mechanical properties and has been widely utilized to toughen bioceramics. Major challenges associated with CNT-reinforced bioceramics include the inhomogeneous dispersion of CNTs and the insufficient interfacial strength between the two phases. To address such issues, this research describes the first use of silica-coated CNT (S-CNT) core-shell structures to reinforce bioceramics using hydroxyapatite (HA) as a representative matrix. HA-based composites with 0.1–2 wt% S-CNT are sintered by spark plasma sintering to investigate their mechanical and biological properties. It is found that when 1 wt% raw CNT (R-CNT) is added, very limited increases in fracture toughness ( K IC ) is observed. By contrast, the incorporation of 1 wt% S-CNT increased the K IC of HA by 101.7%. This is attributed to more homogeneously dispersed fillers and stronger interfacial strengths. MG63 cells cultured on the 1 wt% S-CNT/HA pellets are found to proliferate faster and possess significantly higher alkaline phosphatase activities than those grown on the HA compacts reinforced with 1 wt% R-CNT, probably by virtue of the released Si ions from the SiO2 shell. Therefore, the S-CNT core-shell structures can improve both mechanical and biological properties of HA more effectively than the conventionally used R-CNTs. The current study also presents a novel and effective approach to the enhancement of many other biomedical and structural materials through S-CNT incorporation.

[1]  Nunzio Bottini,et al.  PEG-modified carbon nanotubes in biomedicine: current status and challenges ahead. , 2011, Biomacromolecules.

[2]  N. Herlin‐Boime,et al.  In vitro investigation of oxide nanoparticle and carbon nanotube toxicity and intracellular accumulation in A549 human pneumocytes. , 2008, Toxicology.

[3]  K. Khor,et al.  Optical and biological properties of transparent nanocrystalline hydroxyapatite obtained through spark plasma sintering. , 2016, Materials science & engineering. C, Materials for biological applications.

[4]  Y. Kim,et al.  Surface chemistry in the process of coating mesoporous SiO2 onto carbon nanotubes driven by the formation of Si-O-C bonds. , 2011, Chemistry.

[5]  A. Boccaccini,et al.  45S5 Bioglass®–MWCNT composite: processing and bioactivity , 2015, Journal of Materials Science: Materials in Medicine.

[6]  A. Maiti,et al.  Structural flexibility of carbon nanotubes , 1996 .

[7]  Bengt Fadeel,et al.  Programmed cell death: molecular mechanisms and implications for safety assessment of nanomaterials. , 2013, Accounts of chemical research.

[8]  I. Martin,et al.  Nanoscale Engineering of Biomaterial Surfaces , 2007 .

[9]  A. Boccaccini,et al.  45S5 Bioglass®-derived scaffolds coated with organic-inorganic hybrids containing graphene. , 2013, Materials science & engineering. C, Materials for biological applications.

[10]  K. A. Khora,et al.  Effect of spark plasma sintering on the microstructure and in vitro behavior of plasma sprayed HA coatings , 2003 .

[11]  J. Skepper,et al.  Effect of sintered silicate-substituted hydroxyapatite on remodelling processes at the bone-implant interface. , 2004, Biomaterials.

[12]  Hua Li,et al.  Effect of spark plasma sintering on the microstructure and in vitro behavior of plasma sprayed HA coatings. , 2003, Biomaterials.

[13]  T. Akasaka,et al.  Apatite formation on carbon nanotubes , 2006 .

[14]  G. Reilly,et al.  Differential alkaline phosphatase responses of rat and human bone marrow derived mesenchymal stem cells to 45S5 bioactive glass. , 2007, Biomaterials.

[15]  Fanhao Meng,et al.  Proliferation and gene expression of osteoblasts cultured in DMEM containing the ionic products of dicalcium silicate coating. , 2009, Biomedicine & pharmacotherapy = Biomedecine & pharmacotherapie.

[16]  Yong Wang,et al.  Fabrication of Ruthenium–Carbon Nanotube Nanocomposites in Supercritical Water , 2005 .

[17]  Seishiro Hirano,et al.  Multi-walled carbon nanotubes injure the plasma membrane of macrophages. , 2008, Toxicology and applied pharmacology.

[18]  Teruyuki Nagamune,et al.  Bone-like tissue formation by three-dimensional culture of MG63 osteosarcoma cells in gelatin hydrogels using calcium-enriched medium. , 2006, Tissue engineering.

[19]  Xiao Hu,et al.  Single-Step Process toward Achieving Superhydrophobic Reduced Graphene Oxide. , 2016, ACS applied materials & interfaces.

[20]  Dayong Li,et al.  Improvement of the Biodegradation Property and Biomineralization Ability of Magnesium-Hydroxyapatite Composites with Dicalcium Phosphate Dihydrate and Hydroxyapatite Coatings. , 2016, ACS biomaterials science & engineering.

[21]  A. Seifalian,et al.  A concise review of carbon nanotube's toxicology , 2013, Nano reviews.

[22]  Khiam Aik Khor,et al.  Preparation and characterization of a novel hydroxyapatite/carbon nanotubes composite and its interaction with osteoblast-like cells , 2009 .

[23]  A. Agarwal,et al.  Carbon nanotube reinforced hydroxyapatite composite for orthopedic application: A review. , 2012, Materials science & engineering. C, Materials for biological applications.

[24]  Xizhong Shen,et al.  Comparison of cytotoxicity of pristine and covalently functionalized multi-walled carbon nanotubes in RAW 264.7 macrophages. , 2012, Journal of nanoscience and nanotechnology.

[25]  Y. Mai,et al.  A facile method to fabricate silica-coated carbon nanotubes and silica nanotubes from carbon nanotubes templates , 2009 .

[26]  Yuliang Zhao,et al.  Cytotoxicity of carbon nanomaterials: single-wall nanotube, multi-wall nanotube, and fullerene. , 2005, Environmental science & technology.

[27]  M. Prato,et al.  Organic functionalization of carbon nanotubes. , 2002, Journal of the American Chemical Society.

[28]  Peter X. Ma,et al.  Scaffolds for tissue fabrication , 2004 .

[29]  P. Bandaru,et al.  Toxicity issues in the application of carbon nanotubes to biological systems. , 2010, Nanomedicine : nanotechnology, biology, and medicine.

[30]  Rutao Liu,et al.  Recent progress and perspectives on the toxicity of carbon nanotubes at organism, organ, cell, and biomacromolecule levels. , 2012, Environment international.

[31]  S. Tor,et al.  Spark plasma sintering of hydroxyapatite powders. , 2002, Biomaterials.

[32]  W. N. Chen,et al.  Comparative proteomics profile of osteoblasts cultured on dissimilar hydroxyapatite biomaterials: An iTRAQ‐coupled 2‐D LC‐MS/MS analysis , 2008, Proteomics.

[33]  Bioceramics , 2022, An Introduction to Biomaterials Science and Engineering.

[34]  M. H. Fernandes,et al.  Effect of partial crystallization on the mechanical properties and cytotoxicity of bioactive glass from the 3CaO.P(2)O(5)-SiO(2)-MgO system. , 2012, Journal of the mechanical behavior of biomedical materials.

[35]  W. Bonfield,et al.  The response of osteoblasts to nanocrystalline silicon-substituted hydroxyapatite thin films. , 2006, Biomaterials.

[36]  R. Stevens,et al.  3D interconnected porous HA scaffolds with SiO2 additions: effect of SiO2 content and macropore size on the viability of human osteoblast cells. , 2013, Journal of biomedical materials research. Part A.

[37]  Fwu-Hsing Liu,et al.  Synthesis of biomedical composite scaffolds by laser sintering: Mechanical properties and in vitro bioactivity evaluation , 2014 .

[38]  K. Balani,et al.  Carbon Nanotube Functionalization Decreases Osteogenic Differentiation in Aluminum Oxide Reinforced Ultrahigh Molecular Weight Polyethylene. , 2016, ACS biomaterials science & engineering.

[39]  Khiam Aik Khor,et al.  Tuneable electrochromism in weavable carbon nanotube/polydiacetylene yarns , 2016 .

[40]  A. Schilling,et al.  Influence of processing parameters on microstructure and biocompatibility of surface laser sintered hydroxyapatite-SiO2 composites. , 2013, Journal of biomedical materials research. Part B, Applied biomaterials.

[41]  S. Seal,et al.  Carbon nanotube toughened hydroxyapatite by spark plasma sintering: Microstructural evolution and multiscale tribological properties , 2010 .

[42]  Wei Cui,et al.  Effect of silica coating thickness on the thermal conductivity of polyurethane/SiO2 coated multiwalled carbon nanotube composites , 2014 .

[43]  Hua Li,et al.  Nanostructural characteristics, mechanical properties, and osteoblast response of spark plasma sintered hydroxyapatite. , 2007, Journal of biomedical materials research. Part A.

[44]  Y. Mai,et al.  A simple and controllable graphene-templated approach to synthesise 2D silica-based nanomaterials using water-in-oil microemulsions. , 2016, Chemical communications.

[45]  C. Hsieh,et al.  Thermally conductive and electrically insulating epoxy nanocomposites with thermally reduced graphene oxide-silica hybrid nanosheets. , 2013, Nanoscale.

[46]  A. Nakahira,et al.  A metastable phase in thermal decomposition of Ca-deficient hydroxyapatite , 2003, Journal of materials science. Materials in medicine.

[47]  Paola Petrini,et al.  Cross-linked poly(acrylic acids) microgels and agarose as semi-interpenetrating networks for resveratrol release , 2015, Journal of Materials Science: Materials in Medicine.

[48]  Andreas Hirsch,et al.  Sidewall Functionalization of Carbon Nanotubes. , 2001, Angewandte Chemie.

[49]  Chengtie Wu,et al.  A review of bioactive silicate ceramics , 2013, Biomedical materials.

[50]  A. Ureña,et al.  Effect of silica coatings on interfacial mechanical properties in aluminium-SiC composites characterized by nanoindentation , 2005 .

[51]  Shuhui Yu,et al.  Encapsulating carbon nanotubes with SiO2: a strategy for applying them in polymer nanocomposites with high mechanical strength and electrical insulation , 2015 .

[52]  V. Castranova,et al.  Direct and indirect effects of single walled carbon nanotubes on RAW 264.7 macrophages: role of iron. , 2006, Toxicology letters.

[53]  S. Jurga,et al.  Nanomechanical properties of silica-coated multiwall carbon nanotubes-poly(methyl methacrylate) composites. , 2005, Langmuir : the ACS journal of surfaces and colloids.

[54]  A. Barron,et al.  Synthesis of silica–ammonium chloride macrofibers generated by anionic surfactant templated nanotubes , 2008 .

[55]  W. Stark,et al.  The degree and kind of agglomeration affect carbon nanotube cytotoxicity. , 2007, Toxicology letters.

[56]  M. Prato,et al.  Tissue histology and physiology following intravenous administration of different types of functionalized multiwalled carbon nanotubes. , 2008, Nanomedicine.