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Journal Article•DOI•

Accurate characterization of pure silicon-substituted hydroxyapatite powders synthesized by a new precipitation route

David Marchat1, Maria Zymelka1, Cristina Coelho2, Laurent Gremillard3, Lucile Joly-Pottuz3, Florence Babonneau2, Claude Esnouf3, Jérôme Chevalier3, Didier Bernache-Assollant1 •
Ecole nationale supérieure des mines de Saint-Étienne1, Pierre-and-Marie-Curie University2, University of Lyon3
01 Jun 2013-Acta Biomaterialia (Acta Biomater)-Vol. 9, Iss: 6, pp 6992-7004
TL;DR: The results, particularly those from infrared spectroscopy, raise serious reservations about the phase purity of previously prepared and biologically evaluated SiHA powders, pellets and scaffolds in the literature.
About: This article is published in Acta Biomaterialia.The article was published on 2013-06-01 and is currently open access. It has received 88 citations till now. The article focuses on the topics: Infrared spectroscopy & Fourier transform infrared spectroscopy.

Summary (1 min read)

Jump to: [1. Introduction] – [2.1 Powder synthesis] – [2.2.1 X-ray powder diffraction and Rietveld refinement] – [2.2.4 Electron microscopy (HR-TEM, SAED and EDX)] and [3.2.4 Electron microscopy]

1. Introduction

  • In order to correctly describe the physical, chemical and biological properties of SiHAs and to compare them to routinely implanted HA and β-TCP, well-characterized pure SiHAs powders first need to be prepared.
  • Therefore, this work was devoted to the development of a new route to synthesize monophasic SiHA powders with controlled stoichiometry.
  • To this purpose, a solution of soluble silicate was first prepared from TEOS via a sol-gel route, and then accurate powder analysis was carried out by means of ICP/AES, Xray powder diffraction, Rietveld refinement, high resolution electron transmission microscopy (HR-TEM) with energy dispersive spectroscopy (EDS) as well as infrared (FT-IR/ATR) and solid-state NMR spectroscopy.
  • Two pH levels of precipitation were studied, as well as six Si/P molar ratios.

2.1 Powder synthesis

  • The as-synthesized powders were heated under air using an alumina crucible.
  • The heating and cooling rate was fixed at 4°C min -1 .

2.2.1 X-ray powder diffraction and Rietveld refinement

  • Crystalline phases were identified by means of a Siemens D5000 θ/2θ X-ray diffractometer.
  • The evolution of the crystallinity of the samples after calcination at 1000°C for 15 h was evaluated by means of the full width at half maximum (FWHM) of the (211) peak at 2θ=31.8°, as it had the highest intensity and minimal overlap with neighboring peaks.

2.2.4 Electron microscopy (HR-TEM, SAED and EDX)

  • Gold was then distributed as crystallized nano-domains which were used as a reference in the selected area electron diffraction (SAED) patterns to calculate as precisely as possible the lattice parameters.
  • The SAED patterns obtained from regions with or without gold on the HA part were the same.

3.2.4 Electron microscopy

  • The results are the average of about ten intervals per pattern.
  • Moreover, other experimental patterns for different zone axes (not shown here) were obtained and compared to theoretical electron diffraction patterns calculated by means of the Java Electron Microscopy Simulation (JEMS) software [87] .
  • The results indicate that the experimental and simulated patterns are perfectly superimposed for 0.734 ≥ c/a ≥ 0.729.

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Figures (8)
Citations
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Journal Article•DOI•
Silicon: the evolution of its use in biomaterials.

[...]

James R. Henstock1, L. T. Canham, Susan I. Anderson2•
Keele University1, University of Nottingham2
01 Jan 2015-Acta Biomaterialia
TL;DR: This review discusses the current data obtained from original research in biochemistry and biomaterials science supporting the role of silicon in bone, comparing both the biological function of the element and analysing the evolution of silicon-containing biommaterials.

150 citations

Book Chapter•DOI•
Cationic and Anionic Substitutions in Hydroxyapatite

[...]

Ilaria Cacciotti1•
Sapienza University of Rome1
01 Jan 2015

100 citations

Journal Article•DOI•
Biodegradable and Biocompatible Systems Based on Hydroxyapatite Nanoparticles

[...]

Pau Turon, Luis J. del Valle, Carlos Alemán, Jordi Puiggalí
06 Jan 2017-Applied Sciences
TL;DR: The present review is mainly focused on both the capability of HAp nanoparticles to encapsulate diverse compounds as well as the preparation methods of scaffolds incorporating HAp.
Abstract: Composites of hydroxyapatite (HAp) are widely employed in biomedical applications due to their biocompatibility, bioactivity and osteoconductivity properties. In fact, the development of industrially scalable hybrids at low cost and high efficiency has a great impact, for example, on bone tissue engineering applications and even as drug delivery systems. New nanocomposites constituted by HAp nanoparticles and synthetic or natural polymers with biodegradable and biocompatible characteristics have constantly been developed and extensive works have been published concerning their applications. The present review is mainly focused on both the capability of HAp nanoparticles to encapsulate diverse compounds as well as the preparation methods of scaffolds incorporating HAp. Attention has also been paid to the recent developments on antimicrobial scaffolds, bioactive membranes, magnetic scaffolds, in vivo imaging systems, hydrogels and coatings that made use of HAp nanoparticles.

83 citations

Journal Article•DOI•
In vitro three-dimensional bone tissue models: from cells to controlled and dynamic environment.

[...]

Guenaelle Bouet1, David Marchat, Magali Cruel, Luc Malaval, Laurence Vico •
French Institute of Health and Medical Research1
01 Feb 2015-Tissue Engineering Part B-reviews
TL;DR: This review focuses on state-of-the-art and the current advances in the development of 3D culture systems for bone biology research, and details main characteristics and challenges associated with its three main components, that is, scaffold, cells, and perfusion bioreactor systems.
Abstract: Most of our knowledge of bone cell physiology is derived from experiments carried out in vitro on polystyrene substrates However, these traditional monolayer cell cultures do not reproduce the complex and dynamic 3-dimensional (3D) environment experienced by cells in vivo Thus, there is a growing interest in the use of 3D culture systems as tools for understanding bone biology These in vitro engineered systems, less complex than in vivo models, should ultimately recapitulate and control the main biophysical, biochemical and biomechanical cues that define the in vivo bone environment, while allowing their monitoring This review focuses on state of the art and the current advances in the development of 3D culture systems for bone biology research It describes more specifically advantages related to the use of such systems, and details main characteristics and challenges associated with its three main components, ie scaffold, cells and perfusion bioreactor systems Finally, future challenges for non-invasive imaging technologies are addressed

80 citations

Journal Article•DOI•
Ionic substituted hydroxyapatite for bone regeneration applications: A review

[...]

Antonia Ressler1, Andreja Žužić1, Irena Ivanišević1, Nikhil Kamboj2, Hrvoje Ivanković1 •
University of Zagreb1, Tallinn University of Technology2
01 Jun 2021
TL;DR: In this paper, a review summarises recent and relevant studies on cationic and anionic substitutions in the HAp lattice that are commonly found in the human body.
Abstract: Biological apatites are characterised by various ionic substitutions within the HAp lattice that are crucial for bone metabolism. The introduction of key role elements within synthetic calcium phosphates (CaP), mainly hydroxyapatite (HAp), can increase osteogenesis and enhance bone regeneration process. The lattice structure of HAp enables cationic and anionic substitutions leading to the enhanced biological performance of synthetic bone graft materials. This review summarises recent and relevant studies on cationic and anionic substitutions in the HAp lattice that are commonly found in the human body. Furthermore, co-substituted HAp obtained from synthetic and biological precursors, along with their influence on the bone regeneration process, has been discussed. Finally, future perspectives for the use of substituted HAp have been presented.

77 citations

References
More filters
Journal Article•DOI•
Effect of Silicate-Substitution on Attachment and Early Development of Human Osteoblast-Like Cells Seeded on Microporous Hydroxyapatite Discs

[...]

Katharina Guth1, Charlie Campion2, Tom Buckland2, Karin A. Hing1•
Queen Mary University of London1, University of Hertfordshire2
01 Feb 2010-Advanced Engineering Materials
TL;DR: Microporosity did not diminish the effect of surface physiochemistry on cell adhesion, and enhanced cell attachment for SA appears to be mediated by differences in the quality of adsorbed protein rather than via direct effects of substrate chemistry.
Abstract: Hydroxyapatite (HA) is a well-established graft material used in bone repair. Silicon-substituted hydroxyapatite (SA; 0.8 wt% Si) has shown greater bone ingrowth and bone coverage than phase pure HA. To assess the effect of microporosity on sensitivity of cell attachment to surface physiochemistry, microporous SA and HA discs, and control Thermanox (TMX) discs were incubated with osteoblast-like cells (5 x 10 4 HOS-TE85 cells) under differing tissue culture conditions. To investigate early cellular attachment, organization, and differentiation, cells were also stained for integrin-α 5 β 1 , actin, and runt-related transcription factor (RUNX-2), respectively, after incubation on HA, SA, and TMX discs for 3 days. No significant differences emerged between HA, SA, and TMX discs in mean numbers of cells attached in serum free medium (SFM) over 90 min incubation. In contrast, significantly more cells were attached to SA than HA after 180 min incubation in complete medium (C-MEM) containing fetal calf serum (p < 0.05). Cell attachment to SA and HA discs pre-conditioned in SFM supplemented with fibronectin (FN) was lower than discs pre-conditioned in C-MEM, suggesting sensitivity of an active FN conformation to the presence of co-adsorbates. Confocal microscopy demonstrated significantly more co-localization of integrin α 5 β 1 and actin on SA than HA. Translocalization of RUNX-2 to the nucleus was stronger in cells incubated on SA. Microporosity did not diminish the effect of surface physiochemistry on cell adhesion, and enhanced cell attachment for SA appears to be mediated by differences in the quality of adsorbed protein rather than via direct effects of substrate chemistry.

27 citations

Journal Article•DOI•
Characterisation and conversion study into natural living bone of calcium phosphate bioceramics by solid state NMR spectroscopy

[...]

J.L. Miquel1, L. Facchini1, André Pierre Legrand1, X. Marchandise, P. Lecouffe, M. Chanavaz, M. Donazzan, Christian Rey1, J. Lernaitre2 •
Centre national de la recherche scientifique1, École Polytechnique2
01 Jan 1990-Clinical Materials
TL;DR: In this paper, high-resolution 31P and 1H NMR spectra at 40 MHz (31P) and 300 MHz (1H) were obtained by magic angle sample spinning (MASS) at spinning speeds up to 6·5 kHz and by high power proton decoupling (HPPD).

26 citations

Journal Article•
Design, production and biocompatibility of nanostructured porous HAp and Si-HAp ceramics as three-dimensional scaffolds for stem cell culture and differentiation

[...]

G Lehmann1, Paola Palmero, Ilaria Cacciotti, R. Pecci, Luisa Campagnolo, Rossella Bedini, G. Siracusa, Alessandra Bianco, Antonella Camaioni, Laura Montanaro •
University of Rome Tor Vergata1
01 Jan 2010-Ceramics-silikaty
TL;DR: The incorporation of small amounts of silicon within hydroxyapatite lattice significantly improves HAp solubility and rate of bone apposition, as well as the proliferation of human osteoblasts in vitro.
Abstract: Biocompatible and biodegradable scaffolds can provide a convenient support for stem cell differentiation leading to tissue formation. Porous hydroxyapatite (HAp) scaffolds are clinically used for applications such as spinal fusions, bone tumors, fractures, and in the replacement of failed or loose joint prostheses. The incorporation of small amounts of silicon within hydroxyapatite lattice significantly improves HAp solubility and rate of bone apposition, as well as the proliferation of human osteoblasts in vitro. In the present paper we report biocompatibility data obtained on a newly designed three-dimensional nano-structured porous scaffold made of pure and silicon-substituted hydroxyapatite. A suitable amount of porosity (60 vol%) was obtained within a well densified ceramic skeleton by using polyethylene spheres. Biocompatibility was tested by using murine embryonic stem cells (ES). Cell culture analysis indicated that ES cells adhere well on both hydroxyapatite and silicon-substituted hydroxyapatite scaffolds. Si-substitution, however, improved subsequent ES cell proliferation rate. Bioresorption of hydroxyapatite scaffolds was tested by using human osteoclasts obtained from peripheral blood monocytes, made to differentiate on disks and evaluated by SEM analysis.

25 citations

Journal Article•DOI•
Silicon-substituted hydroxyapatite ceramics (Si-HAp): densification and grain growth through the prism of sintering theories

[...]

V.I. Putlayev1, A. G. Veresov1, M.N. Pulkin1, A. V. Soin1, Vladimir V. Kuznetsov1 •
Moscow State University1
01 Jun 2006-Materialwissenschaft Und Werkstofftechnik
TL;DR: In this paper, a fabrication of Si-HAp with Ca10(Po4)6-x(SiO4)x(OH)2-x (x=0..1) nominal composition and evaluation the effect of Si on sintering of HAp ceramics.
Abstract: Ceramics based on calcium phosphates is known to be a prospective material for biomedical applications. Noticeable attention is paid to hydroxyapatite Ca10(PO4)6(OH)2 (HAp) due to its affinity to a bone mineral. It was recognized recently that Si-doped HAp is a highly promising material in sense of bioactivity improvement. In the frame of distinct research activity structured around this subject, some special problems are to be solved: (1) solubility of Si in the bulk of HAp lattice (and its limit) vs. segregation of Si to free surfaces and grain boundaries, (2) rationalization of Si effect on sintering of HAp ceramics, (3) charge compensation over aliovalent doping of HAp with Si and its interplay with thermal stability of HAp phase. The work was focused on a fabrication of Si-HAp with Ca10(Po4)6-x(SiO4)x(OH)2-x (x=0..1) nominal composition and evaluation the effect of Si on sintering of HAp ceramics. The limit of Si solubility in HAp lattice was estimated to be not higher than x=0.1 in the formula above (at 1000 °C, according to XRD and SEM/EDX). The essence of the silicon influence consists in significant suppression of grain growth during the initial stage of sintering. Silicon doping reduces grain boundary mobility (increasing activation energy of lattice diffusion) along with the increase of pore mobility (in fact, increasing grain boundary diffusion). We believe that the effect of Si on sintering behaviour can be treated in terms of its segregation to grain boundaries, the phenomenon arising from a lattice instability of Si-HAp due to the charge compensation in the course of aliovalent doping.

25 citations

Journal Article•DOI•
Electrophoretic deposition of silicon substituted hydroxyapatite coatings from n-butanol–chloroform mixture

[...]

Xiu Feng Xiao, Rong Fang Liu, Xiao Lian Tang
01 Jan 2008-Journal of Materials Science: Materials in Medicine
TL;DR: After immersion in simulated body fluid for 7 days, Si-HA coatings have the ability to induce the bone-like apatite formation and to improve the shear strength of the coatings.
Abstract: Silicon Substituted Hydroxyapatite (Si-HA) coatings were prepared on titanium substrates by electrophoretic deposition (EPD). The stability of Si-HA suspension in n-butanol and chloroform mixture has been studied by electricity conductivity and sedimentation test. The microstructure, shear strength and bioactivity in vitro has been tested. The stability of Si-HA suspension containing n-butanol and chloroform mixture as medium is better than that of pure n-butanol as medium. The good adhesion of the particles with the substrate and good cohesion between the particles were obtained in n-butanol and chloroform mixture. Adding triethanolamine (TEA) as additive into the suspension is in favor of the formation of uniform and compact Si-HA coatings on the titanium substrates by EPD. The shear strength of the coatings can reach 20.43 MPa after sintering at 700 °C for 2 h, when the volume ratio of n-butanol: chloroform is 2:1 and the concentration of TEA is 15 ml/L. Titanium substrates etched in H2O2/NH3 solution help to improve the shear strength of the coatings. After immersion in simulated body fluid for 7 days, Si-HA coatings have the ability to induce the bone-like apatite formation.

24 citations

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