PREPARATION OF SR-DOPED BIOACTIVE GLASS / STARCH COMPOSITE FROM SODIUM METASILICATE

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ABSTRACT

Bioactive glasses have been well established has third generation biomaterials for the treatment of bone defects, devoid of adverse immunological response. This is due to the formation of hydroxylapitite, having similar chemical composition to natural bone on the glass surface when immersed in biological fluids. Bioactive glasses containing Strontium (Sr) are well known for stimulating high degree of cellular responses leading to high rate of bone regeneration in-vivo and in-vitro. The current study investigated the performance of a bioactive glass composite prepared using a Sr-substituted glass encapsulated in starch as a biomaterial while sodium metasilicate was used as a low-cost substitute for alkoxysilane precursors. The glass was prepared using a new solution precipitation method followed by a sodium wash-out technique to remove the residual sodium that impregnated the gel network structure. The obtained materials were characterizied using scanning electron microscopy (SEM), X-ray diffractometry (XRD) and Fourier transform infrared spectroscopy (FTIR). The results obtained showed that the composite gave a better surface morphology compared with the parent glass. Furthermore, the diffraction pattern of the bioglass composite gave a better ordering of the material structure. Bioactivity assessment showed the formation of hydroxyapatite after immersion in stimulated body fluid which increased in density after 14 days incubation. The composite gave a higher apatite nucleation reaction in SBF during the same period of immersion. Degradability in SBF was also observed, which gave an indication that the materials could undergo controlled degradability in biological fluids, which is a key requirement for a material intended for use in bone regeneration. The performance of the materials indicates that they could serve as low-cost potential candidate biomaterials for use in bone regeneration.


 

Table of Contents

TITLE PAGE                                                                                                

DECLARATION   iii

CERTIFICATION   iv

DEDICATION   v

ACKNOWLEDGEMENT  vi

ABSTRACT  viii

TABLE OF CONTENT  ix

TABLE OF FIGURE  xi

LIST OF TABLE  xii

CHAPTER ONE  1

1.0. INTRODUCTION   1

1.1 Background to the Study  1

1.2. Statement of the Problem   3

1.3. Aim of the Study  3

1.4   Specific Objectives  3

1.5.   Significance of the Study  4

1.6. Operational Definition of Terms  4

CHAPTER TWO   8

2.0. LITERATURE REVIEW    8

2.1. A Historical Overview   8

2.1. Bioactive Glass (BGs) 12

2.2.   Interaction of BGs with the Physiological Environment: General Features. 13

2.2.1. Classes of Bioactivity  13

2.3.   Mechanism of Bioactivity  17

2.4.   Melt-Derived Bioactive Glasses  20

2.5.   Sol–Gel-Derived Bioactive Glasses  23

2.6.   Bone Regeneration  25

2.7.   Bioactive Glass Coatings. 27

2.8.   Strontium (Sr) containing Bioglasses  29

2.8.1.   Silicate Sr-doped BGs  32

2.8.2.   Borate Sr-doped BGs  33

2.8.3.   Phosphate Sr-doped BGs  34

CHAPTER THREE  37

3.0. METHODOLOGY, MATERIALS AND METHODS  37

3.1. Materials  37

3.2. METHODS  38

3.2.1. Synthesis of Sr–doped bioactive glass by the Sol-Gel method  38

3.2.2. Preparation of Starch/PVA   39

3.2.3. Incoporation of Sr-doped bioactive glass/Starch  39

3.2.4 Preparation procedure of SBF  39

3.3.5. Bioactivty test in SBF  40

3.3.6.   Characterisation techniques  41

3.3.6.1.   Morphology and Elemental composition  41

3.2.6.2.   Phase composition  41

3.2.6.3.   Nature of bonds present 41

CHAPTER FOUR   42

4.0.     RESULTS AND DISCUSSION   42

4.1.    SCANNING ELECTRON MICROSCOPY (SEM) 42

4.1.1.   Sr-doped Glass and composite  42

4.1.2.   Sr-doped Bioglass Composite  44

4.2.    X-Ray Diffractometry (XRD) Analysis  45

4.2.1.   Diffraction patterns of the Sr-doped Bioactive Glass  45

4.2.2.   Diffraction patterns of the Sr-doped Bioglass Composite  46

4.3. FOURIER TRANSFORM INFRARED (FTIR) ANALYSIS  47

CHAPTER FIVE  51

CONCLUSION AND RECOMMENDATION   51

5.0. Conclusion  51

REFERENCES  52

Jones, R. J., Gentleman, E., and Polak, J. (2007) Bioactive Glass Scaffolds for Bone Regeneration. Journal of mineralogical of American, 3 (6): 393–399. 56

 

 

 

TABLE OF FIGURE

Figure 1 Compositional diagram for bone-bonding  11

Figure 2 Schematic representation of (A) melt-quenching and (B) sol-gel route for bioactive glass synthesis and final products (Kargozar et al., 2019). 22

Figure 3 Schematic of reactions in the sol–gel process: formation of silica tetrahedral and nanoparticles at room temperature  25

Figure 4 Diagram illustrating how a porous bioactive glass scaffold could be used to regenerate a bone defect 27

Figure 5 Figure 4.1: (a) Sr-doped bioglass after sinitering and (b) Sr-doped bioglass composite  43

Figure 6Figure 4.2: SEM images of samples after immersion in SBF (a) Sr-doped glass, (b) composite for 7 days, (c) Sr-doped glass and (d) composite for 14 days  44

Figure 7 Figure 4.3:  XRD result (a) Sr-doped and (b) composite for 0 day in SBF  46

Figure 8 Figure 4.4: XRD result, (a) Sr-doped bioglass for 7 days, (b) composite for 7 days, (c) for Sr-doped bioglass for 14 days and (d) for composite for 14 days in SBF  47

Figure 9 Figure 4.5: FTIR result (a) Sr-doped glass, (b) composite at 0 day  49

Figure 10 Figure 4.6: FTIR result, samples after immersion in SBF (a) Sr-doped glass, (b) composite for 7 days, (c) Sr-doped glass and (d) composite for 7 days  49

Figure 11 Figure 4.7: FTIR result, samples after immersion in SBF (a) Sr-doped glass, (b) composite for 14 days, (c) Sr-doped glass and (d) composite for 14 days  50

LIST OF TABLE

Table 1 Tables 3.0: List of reagents used for the experiment 37

Table 2 Tables 3.1: List of equipments/ apparatus. 37

Table 3 Table 3.2: Composition of the Sr-doped bioactive glass  38

Table 4 Table 3.3: Nominal ion concentration of SBF in comparison with those in human blood plasma  40

Table 7 Table 4.1: The spectra frequency and their assignment of Sr-doped glass and composite at 0 day  48

 

CHAPTER ONE

1.0.  INTRODUCTION

 

1.1  Background to the Study

 

Bioactive glasses are amorphous, silicate-based materials that bond to bone and stimulate new bone growth while degrading over time, making them candidate materials for bone regeneration.   It has been traditionally used in the clinical practice to fill and restore osseous defects due to their unique ability to bond to host bone and stimulate new bone growth without eliciting adverse immunological response (Baino, 2016).

In 2016 Baino reported that BGs are able to stimulate more bone regeneration than other bioactive ceramics used in the past but they lag behind other bioactive ceramics in terms of commercial success, thought it has not yet reached its potential but research activity is growing.

After a preliminary definition of biomaterial in the 1950s, mainly based on the criterion of maximum biochemical and biological inertness in contact with body fluids (first-generation materials) (Hench , 2010 and Elisa et al., 2018), the discovery of Bioglass® by Larry L. Hench in 1969 (Hench, 2006) constituted for the first time in the story of biomaterials an alternative, extending the concept of biocompatibility to all those materials which were able to enhnce and to promote a positive response of the living system through the formation of a strong tissue implant bond (second-generation materials) and the genetic activation of specific cell pathways (third generation smart materials) (Hench ,1998).

 

Bioglass® actually represents the first example of a biomaterial belonging to the third generation, this so because of the biological role played by its ionic dissolution products, which is directly released in the physiological environment (Hoppe, 2011), in addition to its capability to strongly bond the host tissue (primarily bone) with the formation of an interfacial calcium phosphate layer (Andersson, 1990, 1991).

According to Jones in 2013, the first artificial material that was found to form a chemical bond with bone, launching the field of bioactive ceramics. The in vivo studies shows that bioactive glasses bond with bone more rapidly than other bioceramics materials, and these studies indicated that their osteogenic properties are due to their dissolution products, stimulating osteoprogenitor cells at the genetic level.  Hence, hydroxyapatite (HA) is highly osteoconductive and is able to form a strong bond with the surrounding living bone (Bates, 2007).

 

Since its discovery, 45S5 Bioglass® (45S5) opened unimaginable scenarios in the field of tissue regeneration, mainly thanks to its osteoinductive and osteoconductive ability (Cho, 2002). In vitro studies reported that, during the dissolution of 45S5, the ion release seems to induce angiogenesis and stimulate osteoblasts proliferation and new bone growth (Audigé, 2005).

However, some bioactive glasses are able to bond to bone. According to Li et al, 2017 bone regeneration is necessary to address various degrees and locations of bone defects. Regardless of whether large bone defects are caused by trauma, infection, tumor excision, and skeletal necrosis or by periodontitis, insufficient implant bone, and osteoporosis, they all require treatment involving bone regeneration.

Moreover, this approach carries the risk of disease transmission and unsatisfactory bone integration.

Technological advancement has brought about 3D-printed scaffolds which have aroused wide concern over the past few decades due to their unique physical properties for tissue regeneration engineering and vascularized bone regeneration (Zhang, 2017).

Over the last 50 years, numerous studies have been conducted to optimize the response of the body to BGs and extend their use to a wider range of specific clinical application (Brink, 1997 and Oudadesse, 2011).

 

1.2. Statement of the Problem

The improvement and acceleration of bone repair still are partially unmet needs in bone regenerative therapies. Hence, strontium (Sr)-containing bioactive glasses (BGs) is regarded as a highly promising materials to tackle this challenge.

In the present study, we provide a comprehensive overview of Sr-containing glasses along with the current state of their clinical use and general route to sol-gel bioactive glasses involve the use alkoxysilane silica precursors. Alkoxysilanes are generally very expensive and toxic on inhalation

1.3. Aim of the Study

The aim of this study is to prepare Sr-doped bioactive glass composite by solution precipitation technique using sodium metasilicate as an inexpensive substitute to alkoxysilane precursors.

1.4   Specific Objectives

       To prepare the bioactive glass doped with strontium.

       To prepare the bioactive glass and bioactive glass/polymer composite.

       To characterize the Sr-doped bioactive glass and starch-based composite to evaluate their bone bonding ability.

 1.5.   Significance of the Study

·       The design of a novel route for preparing bioactive glasses and composites from metal silicates.

·       Economic and less toxic route for preparing bioactive glasses and composites attractive for commercial scale production.

1.6. Operational Definition of Terms

• Bioactive Glasses

Bioactive glasses are amorphous silicate-based materials which are compatible with the human body, bond to bone and can stimulate new bone growth while dissolving over time (Baino, 2016).

Bone Regeneration

Bone regeneration is called Bone healing, or fracture healing, is a proliferative physiological process in which the body facilitates the repair of a bone fracture.

• Maxillofacial

Maxillofacial refers to the face and jaws.

• Mesoporous Material

A mesoporous material has openings within its structure that are between 2 and 50 nanometers (nm) in diameter.

• Musculoskeletal

This system includes bones, muscles, tendons, ligaments and soft tissues.

• Necrosis

It is the death of most or all of the cells in an organ or tissue due to disease, injury, or failure of the blood supply.

•Osteoconduction

This simply means that bone grows on a surface. The phenomenon is regularly seen in the case of bone implants. Implant materials of low biocompatibility such as copper, silver and bone cement shows little or no osteoconduction.

• Osteoclast & Osteoblast

Aged bone resorption is refers to as osteoclasts while osteoblasts are responsible for new bone formation

• Osteoarthritis

This is the degeneration of joint cartilage and the underlying bone, most common from middle age onward. It causes pain and stiffness, especially in the hip, knee, and thumb joints.

• Osteoporosis

Osteoporosis is a medical condition in which the bones become brittle and fragile from loss of tissue, typically as a result of hormonal changes, or deficiency of calcium or vitamin D.

• Osteogenesis & Osteogenesis Imperfecta (Oi)

Osteogenesis is the development and formation of bone.

Osteogenesis imperfecta (OI) is a genetic or heritable disease in which bones fracture (break) easily, often with no obvious cause or injury. OI is also known as brittle bone disease, and the symptoms can range from mild with only a few fractures to severe with many medical complications (Kang et al., 2017).

• Periodontitis

This is an inflammation of the tissue around the teeth, often causing shrinkage of the gums and loosening of the teeth.

• Prostheses

The term prostheses is an artificial body part, such as a limb, a heart, or a breast implant.

A prosthesis substitutes for a part of the body that may have been missing at birth, or that is lost in an accident or through amputation.

• Scaffolds

Scaffolds can be said to be the masterpiece of bone tissue engineering. A bone scaffold is the 3D matrix that allows and stimulates the attachment and proliferation of osteoinducible cells on its surfaces.

• Skeletogenesis

Skeletogenesis is simply the process of skeleton formation.

• Strontium Ranelate (Sr)

Strontium ranelate is a medication used for the management of severe osteoporosis in high-risk postmenopausal women and adult men.

• In-Vitro, In-Vivo & In-Situ

In vitro is Latin for “within the glass.” When something is performed in vitro, it happens outside of a living organism.

In vivo is Latin for “within the living.” It refers to work that’s performed in a whole, living organism.

In situ means “in its original place.” It lies somewhere between in vivo and in vitro. Something that’s performed in situ means that it’s observed in its natural context, but outside of a living organism.

• Ossification

Ossification is the natural process of bone formation; it is the hardening (as of muscular tissue) into a bony substance.



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