臺灣博碩士論文加值系統

生物活性玻璃(bioactive glass, BG)是一種作為骨頭移植的重要生醫材料，由於其具有優異的生物活性以及與骨頭進行化學鍵結的能力，然而生物活性玻璃不具有抗菌之能力。因此本研究為了克服其所在的應用困難，因此藉由摻雜氧化石墨稀(graphene oxide, GO)來達到其目的。
於本研究當中，我們使用一階段噴霧熱解法(spray pyrolysis)製備氧化石墨稀摻雜生物活性玻璃，此外，GO使用不同的製備方法(modify Hummer’s methods)用於探討不同性質之材料對於摻雜後之影響。本研究對於GO，BG以及經GO摻雜BG之樣品對其性質之分析結果包含:相組成，形貌以及內部結構，比表面積，化學結構，抗菌測試，體內以及體外生物活性檢測。
由結果顯示使用硝酸鈉(硝酸)作為二次酸所製備之GO (N-GO)具有最高的抗菌活性對於大腸桿菌大約98.2%之抗菌能力，由於二次酸在氧化反應期間提升之化學選擇性。同時於石墨稀摻雜生物活性玻璃結果方面指出，N-GO摻雜BG(N-GO-BG)之樣品展現出最高的氧化/結構混亂之程度，更進一步，N-GO-BG展現出最高的抗菌活性(82.7對於大腸桿菌和98.0%對於金黃色葡萄球菌)，但是卻具有最低的生物活性。於活體實驗的結果顯示，我們的BG以及N-GO-BG樣品展現出良好的生物相容性，並且對於新生組織帶來好處，同時沒有明顯的發炎反應產生。最後，GO在本研究中對於抗菌性及生物活性之探討皆詳細於本研究中討論。

Bioactive glasses (BGs) are important biomaterial as bone implant due to those excellent bioactivity and bone bonding ability; However, BGs lack of intrinsic antibacterial activity. In order to overcomes one of the remaining challenges to the application, doping BGs with graphene oxide (GO) to overcome this problem in this study.
In the present work, we demonstrate that GO doped BG can be prepared with a one-step spray pyrolysis (SP) process, moreover, different treatment methods (modify Hummer’s methods) of GOs have been applied on this study as well. The phase composition, morphology, inner structure, specific surface area, chemical structure, antibacterial tests, in-vitro, and in-vivo bioactive tests of GO, BG, and GO doped BG samples were characterized in this study.
The results suggest that use sodium nitrate (nitric acid) as second acid treated-GO (N-GO) has highest against E.coli activity to ~98.2% due to the second acids enhancing chemoselectivity during oxidation process. Following the GO doped BG results, N-GO doped BG (N-GO-BG) has highest degree of oxidation/ structural disorder; furthermore, the N-GO-BG demonstrates highest antibacterial activity (82.7% to E.coli and 98.0% to S. aureus) but lowest bioactive activity. In-vivo test results suggest that our BG and N-GO-BG samples with good biocompatibility and bring a benefit to the new tissues generation without observably inflammation reaction. Finally, the role of GO on the antibacterial and bioactive properties has been discussed in this study.

摘要 I
Abstract III
Acknowledgements V
Contents VI
List of Tables X
List of Figures XI
Chapter 1. Introduction 1
1.1 Motivation of Developing of Antibacterial Bioactive glass 1
1.2 Aim of Work 3
Chapter 2. Literature Review 5
2.1 Bone and Tissue Engineering 5
2.1.1 Fundamentals of Bone 5
2.1.2 The Concept of Bone and Tissue Engineering 8
2.2 Bioceramics 13
2.2.1 Type of Bioceramics 13
2.2.2 Bone Bonding Mechanism of Bioactive Glass 16
2.2.3 Application of Bioactive Blass 18
2.3 Bacterial 22
2.3.1 Gram-Bacteria 25
2.3.2 Pathological Response 29
2.4 Antibacterial Agents 38
2.4.1 Antibiotics and Resistance 39
2.4.2 Other Antibacterial Methods 42
2.4.3 Antibacterial Activity of Graphene Materials 46
2.5 Biomedical Test 56
2.5.1 Antibacterial Test 56
2.5.2 In-vitro Bioactive Test 58
2.5.1 In-vivo Test 59
Chapter 3. Materials and experimental procedure 62
3.1 Materials 62
3.1.1 Experimental Materials 63
3.1.2 Experimental Instrument 64
3.2 Experimental Procedure 65
3.2.1 Synthesis of Bioactive Glass 65
3.2.2 Synthesis of GOs 66
3.2.3 Synthesis of GO Doped BG 67
3.2.4 Bulk Samples preparation 68
3.3 Characterization of the Materials 69
3.3.1 X-Ray Diffractometer (XRD) 69
3.3.2 Scanning Electron Microscope (SEM) 69
3.3.3 Transmission Electron Microscope (TEM) 70
3.3.4 Brunaeur Emmet Teller (BET) 71
3.3.5 Microscope Raman Spectrometer 71
3.4 In-Vitro Bioactive Tests 72
3.5 In-Vitro Antibacterial Tests 72
3.6 In-Vivo Tests 73
Chapter 4. Results 75
4.1 Graphene Oxide 75
4.1.1 Crystal Structure Analysis of GO 76
4.1.2 Morphologies and particle sizes of GO 77
4.1.3 Chemical Structure of GO 79
4.1.4 Antibacterial Test of GOs 80
4.2 Graphene Oxide doped Bioactive Glass 82
4.2.1 Phase composition of BG and GO doped BG 82
4.2.2 Morphology of BG and GO doped BG 83
4.2.3 Inner Structure of BG and GO doped BG 87
4.2.4 Chemical Structure of BG and GO doped BG 91
4.2.5 In-Vitro Bioactivity of BG and GO doped BG 92
4.2.6 Antibacterial Test of BG and GO doped BG 94
4.2.7 In-Vivo Test of BG and N-GO-BG 98
Chapter 5. Discussion 103
5.1 The different of GO 103
5.2 Identification of GO doped BG 107
Chapter 6. Conclusions 118
Chapter 7. Future Works 119
References 120

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