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A special issue of Journal of Functional Biomaterials (ISSN 2079-4983).

Deadline for manuscript submissions: closed (31 August 2019) | Viewed by 41203

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Prof. Dr. Adriana Bigi

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Department of Chemistry “Giacomo Ciamician”, University of Bologna, Via F. Selmi 2, I-40126 Bologna, Italy
Interests: biomimetic materials chemistry; biomaterials; functionalized calcium phosphates; bone cements; bioactive coatings; calcium phosphates-biodegradable polymers composites; scaffolds for regenerative medicine
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Dr. Elisa Boanini

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Guest Editor

Department of Chemistry “Giacomo Ciamician”, Via F. Selmi 2, University of Bologna, I-40126 Bologna, Italy
Interests: biomaterials; biomimetic materials chemistry; bioceramics; nanocrystals; hydroxyapatite; octacalcium phosphate; metal nanoparticles; bioactive coatings
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

The continuously increasing number of age-related muscoskeletal disorders requires the development of suitable materials for the substitution and repair of impaired tissues. One of the most relevant requirements of a biomaterial is the ability to bond to the surrounding biological tissue, which is favored by the similarity between the synthetic and the biological materials in terms of composition, structure and morphology. This is the reason for the key role played by calcium phosphates (CaPs) in this field. The interest towards these compounds includes not only hydroxyapatite, which is the CaP most similar to the inorganic phase of bone, but also a variety of different calcium orthophosphates, such as octacalcium phosphate, tricalcium phosphate, dicalcium phosphate in the dihydrate and anhydrous forms, and tetracalcium phosphate.

The performance of CaPs as biomaterials has recently registered significant improvement thanks to innovative approaches based on biomimetic strategies, as well as to their functionalization with biological relevant ions, molecules and macromolecules, growth factors and drugs. Applications of functionalized and multi-functionalized CaPs range from coatings to bone cements, scaffolds for regenerative medicine, delivery systems for therapeutic agents.

This Special Issue is focused on the recent developments of research into the synthesis and characterization of functionalized and multi-functionalized biomimetic CaPs, as well as on their applications as biomaterials for the substitution/repair of the musculoskeletal system.

Prof. Dr. Adriana Bigi
Prof. Elisa Boanini
Guest Editors

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Keywords

Functionalization
Calcium phosphates
Bone cements
Coatings
Scaffolds for regenerative medicine
Delivery systems

Published Papers (6 papers)

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Research

20 pages, 4520 KiB

Open AccessArticle

Phosphoserine Functionalized Cements Preserve Metastable Phases, and Reprecipitate Octacalcium Phosphate, Hydroxyapatite, Dicalcium Phosphate, and Amorphous Calcium Phosphate, during Degradation, In Vitro

by Joseph Lazraq Bystrom and Michael Pujari-Palmer

J. Funct. Biomater. 2019, 10(4), 54; https://doi.org/10.3390/jfb10040054 - 27 Nov 2019

Cited by 8 | Viewed by 6945

Abstract

Phosphoserine modified cements (PMC) exhibit unique properties, including strong adhesion to tissues and biomaterials. While TTCP-PMCs remodel into bone in vivo, little is known regarding the bioactivity and physiochemical changes that occur during resorption. In the present study, changes in the mechanical strength and composition were evaluated for 28 days, for three formulations of αTCP based PMCs. PMCs were significantly stronger than unmodified cement (38–49 MPa vs. 10 MPa). Inclusion of wollastonite in PMCs appeared to accelerate the conversion to hydroxyapatite, coincident with slight decrease in strength. In non-wollastonite PMCs the initial compressive strength did not change after 28 days in PBS (p > 0.99). Dissolution/degradation of PMC was evaluated in acidic (pH 2.7, pH 4.0), and supersaturated fluids (simulated body fluid (SBF)). PMCs exhibited comparable mass loss (<15%) after 14 days, regardless of pH and ionic concentration. Electron microscopy, infrared spectroscopy, and X-ray analysis revealed that significant amounts of brushite, octacalcium phosphate, and hydroxyapatite reprecipitated, following dissolution in acidic conditions (pH 2.7), while amorphous calcium phosphate formed in SBF. In conclusion, PMC surfaces remodel into metastable precursors to hydroxyapatite, in both acidic and neutral environments. By tuning the composition of PMCs, durable strength in fluids, and rapid transformation can be obtained. Full article

(This article belongs to the Special Issue Functionalized Biomimetic Calcium Phosphates)

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13 pages, 5676 KiB

Open AccessFeature PaperArticle

Regulation of Osteogenic Markers at Late Stage of Osteoblast Differentiation in Silicon and Zinc Doped Porous TCP

by Gary A. Fielding, Naboneeta Sarkar, Sahar Vahabzadeh and Susmita Bose

J. Funct. Biomater. 2019, 10(4), 48; https://doi.org/10.3390/jfb10040048 - 05 Nov 2019

Cited by 17 | Viewed by 5368

Abstract

Calcium phosphates (CaPs) are one of the most widely used synthetic materials for bone grafting applications in the orthopedic industry. Recent trends in synthetic bone graft applications have shifted towards the incorporation of metal trace elements that extend the performance of CaPs to have osteoinductive properties. The objective of this study is to investigate the effects of silicon (Si) and zinc (Zn) dopants in highly porous tricalcium phosphate (TCP) scaffolds on late-stage osteoblast cell differentiation markers. In this study, an oil emulsion method is utilized to fabricate highly porous SiO₂ doped β-TCP (Si-TCP) and ZnO doped β-TCP (Zn-TCP) scaffolds through the incorporation of 0.5 wt.% SiO₂ and 0.25 wt.% ZnO, respectively, to the β-TCP scaffold. Reverse transcriptase quantitative polymerase chain reaction (RT-qPCR) is utilized to analyze the mRNA expression of osteoprotegerin (OPG), receptor activator of nuclear kappa beta ligand (RANKL), bone morphogenetic protein 2 (BMP2), and runt-related transcription factor 2 (Runx2) at the later stage of osteoblast differentiation, day 21 and day 28. Results show that the addition of Si and Zn to the β-TCP structure inhibited the β to α-TCP phase transformation and enhance the density without affecting the dissolution properties. Normal BMP-2 and Runx2 transcriptions are observed in both Si-TCP and Zn-TCP scaffolds at the initial time point, as demonstrated by RT-qPCR. Moreover, the addition of both Si and Zn positively regulate the osteoprotegerin: receptor activator of nuclear factor k-β ligand (OPG:RANKL) ratio at 21-days for Si-TCP and Zn-TCP scaffolds. These results demonstrate the effects of Si and Zn doped porous β-TCP scaffolds on the upregulation of osteoblast marker gene expression including OPG, RANKL, BMP-2, and Runx2, indicating the role of trace elements on the effective regulation of late-stage osteoblast cell differentiation markers. Full article

(This article belongs to the Special Issue Functionalized Biomimetic Calcium Phosphates)

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11 pages, 3060 KiB

Open AccessArticle

Critical Defect Healing Assessment in Rat Calvaria Filled with Injectable Calcium Phosphate Cement

by Luis Eduardo Schmidt, Henrique Hadad, Igor Rodrigues de Vasconcelos, Luara Teixeira Colombo, Rodrigo Capalbo da Silva, Ana Flavia Piquera Santos, Lara Cristina Cunha Cervantes, Pier Paolo Poli, Fabrizio Signorino, Carlo Maiorana, Paulo Sérgio Perri de Carvalho and Francisley Ávila Souza

J. Funct. Biomater. 2019, 10(2), 21; https://doi.org/10.3390/jfb10020021 - 13 May 2019

Cited by 12 | Viewed by 6109

Abstract

(1) Background: The tissue engineering field has been working to find biomaterials that mimic the biological properties of autogenous bone grafts. (2) Aim: To evaluate the osteoconduction potential of injectable calcium phosphate cement implanted in critical defects in rat calvaria. (3) Methods: In the calvarial bone of 36 rats, 7-mm diameter critical size defects were performed. Afterwards, the animals were randomly divided into three groups according to filler material: a blood clot group (BC), blood clot membrane group (BCM), and an injectable β-tricalcium phosphate group (HBS) cement group. After periods of 30 and 60 days, the animals were euthanized, the calvaria was isolated, and submitted to a decalcification process for later blades confection. Qualitative and quantitative analysis of the neoformed bone tissue were conducted, and histometric data were statistically analyzed. (4) Results: Sixty days post-surgery, the percentages of neoformed bone were 10.67 ± 5.57 in group BC, 16.71 ± 5.0 in group BCM, and 55.11 ± 13.20 in group HBS. The bone formation values in group HBS were significantly higher (p < 0.05) than in groups BC and BCM. (5) Conclusions: Based on these results, it can be concluded that injectable calcium phosphate cement is an osteoconductive material that can be used to fill bone cavities. Full article

(This article belongs to the Special Issue Functionalized Biomimetic Calcium Phosphates)

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15 pages, 5054 KiB

Open AccessArticle

Strontium and Zinc Substitution in β-Tricalcium Phosphate: An X-ray Diffraction, Solid State NMR and ATR-FTIR Study

by Elisa Boanini, Massimo Gazzano, Carlo Nervi, Michele R. Chierotti, Katia Rubini, Roberto Gobetto and Adriana Bigi

J. Funct. Biomater. 2019, 10(2), 20; https://doi.org/10.3390/jfb10020020 - 05 May 2019

Cited by 48 | Viewed by 7258

Abstract

β-tricalcium phosphate (β-TCP) is one of the most common bioceramics, widely applied in bone cements and implants. Herein we synthesized β-TCP by solid state reaction in the presence of increasing amounts of two biologically active ions, namely strontium and zinc, in order to clarify the structural modifications induced by ionic substitution. The results of X-ray diffraction analysis indicate that zinc can substitute for calcium into a β-TCP structure up to about 10 at% inducing a reduction of the cell parameters, whereas the substitution occurs up to about 80 at% in the case of strontium, which provokes a linear increase of the lattice constants, and a slight modification into a more symmetric structure. Rietveld refinements and solid-state ³¹P NMR spectra demonstrate that the octahedral Ca(5) is the site of β-TCP preferred by the small zinc ion. ATR-FTIR results indicate that zinc substitution provokes a disorder of β-TCP structure. At variance with the behavior of zinc, strontium completely avoids Ca(5) site even at high concentration, whereas it exhibits a clear preference for Ca(4) site. The infrared absorption bands of β-TCP show a general shift towards lower wavenumbers on increasing strontium content. Particularly significant is the shift of the infrared symmetric stretching band at 943 cm⁻¹ due to P(1), that is the phosphate more involved in Ca(4) coordination, which further supports the occupancy preference of strontium. Full article

(This article belongs to the Special Issue Functionalized Biomimetic Calcium Phosphates)

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19 pages, 4171 KiB

Open AccessFeature PaperArticle

Adsorption of Proteins on m-CPPD and Urate Crystals Inhibits Crystal-Induced Cell Responses: Study on Albumin-Crystal Interaction

by Felix Renaudin, Stéphanie Sarda, Laure Campillo-Gimenez, Childérick Séverac, Thibaut Léger, Cédric Charvillat, Christian Rey, Frédéric Lioté, Jean-Michel Camadro, Hang-Korng Ea and Christèle Combes

J. Funct. Biomater. 2019, 10(2), 18; https://doi.org/10.3390/jfb10020018 - 25 Apr 2019

Cited by 16 | Viewed by 7732

Abstract

The biological effects and cellular activations triggered by monosodium urate (MSU) and calcium pyrophosphate dihydrate (monoclinic: m-CPPD) crystals might be modulated by protein coating on the crystal surface. This study is aimed at: (i) Identifying proteins adsorbed on m-CPPD crystals, and the underlying mechanisms of protein adsorption, and (ii) to understand how protein coating did modulate the inflammatory properties of m-CPPD crystals. The effects of protein coating were assessed in vitro using primary macrophages and THP1 monocytes. Physico-chemical studies on the adsorption of bovine serum albumin (BSA) upon m-CPPD crystals were performed. Adsorption of serum proteins, and BSA on MSU, as well as upon m-CPPD crystals, inhibited their capacity to induce interleukin-1-β secretions, along with a decreased ATP secretion, and a disturbance of mitochondrial membrane depolarization, suggesting an alteration of NLRP3 inflammasome activation. Proteomic analysis identified numerous m-CPPD-associated proteins including hemoglobin, complement, albumin, apolipoproteins and coagulation factors. BSA adsorption on m-CPPD crystals followed a Langmuir-Freundlich isotherm, suggesting that it could modulate m-CPPD crystal-induced cell responses through crystal/cell-membrane interaction. BSA is adsorbed on m-CPPD crystals with weak interactions, confirmed by the preliminary AFM study, but strong interactions of BSA molecules with each other occurred favoring crystal agglomeration, which might contribute to a decrease in the inflammatory properties of m-CPPD crystals. These findings give new insights into the pathogenesis of crystal-related rheumatic diseases and subsequently may open the way for new therapeutic approaches. Full article

(This article belongs to the Special Issue Functionalized Biomimetic Calcium Phosphates)

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12 pages, 4643 KiB

Open AccessArticle

Role of Aspartic and Polyaspartic Acid on the Synthesis and Hydrolysis of Brushite

by Katia Rubini, Elisa Boanini and Adriana Bigi

J. Funct. Biomater. 2019, 10(1), 11; https://doi.org/10.3390/jfb10010011 - 01 Feb 2019

Cited by 19 | Viewed by 7102

Abstract

Dicalcium phosphate dihydrate (DCPD) is one of the mineral phases indicated as possible precursors of biological apatites and it is widely employed in the preparation of calcium phosphate bone cements. Herein, we investigated the possibility to functionalize DCPD with aspartic acid (ASP) and poly-aspartic acid (PASP), as models of the acidic macromolecules of biomineralized tissues, and studied their influence on DCPD hydrolysis. To this aim, the synthesis of DCPD was performed in aqueous solution in the presence of increasing concentrations of PASP and ASP, whereas the hydrolysis reaction was carried out in physiological solution up to three days. The results indicate that it is possible to prepare DCPD functionalized with PASP up to a polyelectrolyte content of about 2.3 wt%. The increase of PASP content induces crystal aggregation, reduction of the yield of the reaction and of the thermal stability of the synthesized DCPD. Moreover, DCPD samples functionalized with PASP display a slower hydrolysis than pure DCPD. On the other hand, in the explored range of concentrations (up to 10 mM) ASP is not incorporated into DCPD and does not influence its crystallization nor its hydrolysis. At variance, when present in the hydrolysis solution, ASP, and even more PASP, delays the conversion into the more stable phases, octacalcium phosphate and/or hydroxyapatite. The greater influence of PASP on the synthesis and hydrolysis of DCPD can be ascribed to the cooperative action of the carboxylate groups and to its good fit with DCPD structure. Full article

(This article belongs to the Special Issue Functionalized Biomimetic Calcium Phosphates)

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