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Engineering Bioactive Polymers for the Next Generation of Bone Repair

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Engineering Bioactive Polymers for the Next Generation of Bone Repair Engineering Bioactive Polymers for the Next Generation of Bone Repair A Thesis Submitted to the Faculty of Drexel University by Emily Y. Ho in partial fulfillment of the requirements for the degree of Doctor of Philosophy April 2005 © Copyright 2005 Emily Y. Ho. All Rights Reserved. ii Dedications To my father, Ferdinand Fook Hong Ho iii Acknowledgements I would like to give grace to God for His gifts and blessings. I am grateful to the kindness and guidance of my advisor, Dr. Michele Marcolongo. Without her continuous advice and financial support, this work would not be possible. Many people guided me throughout this study and I would especially like to mention, Dr. Anthony Lowman and Dr. Garland Fussell, for sharing their vast knowledge with me. Also I thank Dr. Wei-Heng Shih and Dr. Frank Ko for their suggestion in my pre-defense and defense presentations. I appreciated the contribution from Dr. Riad Gobran and Dr. Surya Kalidindi in my thesis proposal presentation. Further, I must extend thanks to my friends who assisted me in various experiments: Jonathan Thomas, Abhijeet Joshi and Marco Cannella on mechanical tests; Thomas Juliano on nano-indentation analyses; Hui Dong Li on viscosity measurements and Jennifer Vernengo on polymer characterizations. With their expertise, many of my experiments were made feasible. Many thanks to my friends, Dr. Grace Hsuan, Dianne Phelan, Kishore Tenneti, Ranjan Dash, Hoa Lam, Gwenaelle Proust, Rita Truongcao, Chris Massey, members of Marcolongo’s Lab and members of Lowman’s Lab, who helped me in countless ways. Special thanks to my Mom and Dad, Grace and Ferdinand Ho, for their care and patience; to my sister and brother, Maria and Alvin Ho, for their encouragement and emotional support; to my aunt and uncle, Oi Chun and William Lam, for their generosity and hospitality. Their endless love and blessing made my life fruitful. Without them, I could not have completed this thesis. iv Table of Contents List of Tables .............................................................................................................viii List of Figures.............................................................................................................. ix Abstract....................................................................................................................... xii 1. Introduction............................................................................................................. 1 2. Background............................................................................................................. 2 2.1. Human Bone.................................................................................................. 2 2.1.1. Structural and Material Properties of Bone.................................. 3 2.1.2. Mechanical Properties of Bone .................................................... 4 2.1.3. Bone Cells.................................................................................... 6 2.1.4. Bone Regeneration....................................................................... 7 2.2. Bone Replacements........................................................................................ 8 2.2.1. Motivation .................................................................................... 8 2.2.2. Requirements of Bone Replacement ............................................ 9 2.3. Natural Bone Replacement .......................................................................... 11 2.4. Synthetic Bone Replacement ....................................................................... 14 2.4.1. Calcium Phosphate Materials and Bioactive Glasses................. 14 2.4.2. Biodegradable and Non-biodegradable Polymers...................... 16 2.4.3. Ceramics / Polymer Composite.................................................. 19 2.5. Tissue Engineered Scaffold ......................................................................... 23 2.6. Injectable Materials...................................................................................... 24 2.6.1. Polymeric Injectable Materials................................................... 24 v 2.6.2. Ceramic Injectable Materials...................................................... 26 2.6.3. Injectable Composite Materials.................................................. 27 3. Research Goals...................................................................................................... 33 4. An Solid Bioactive Polymeric Composites: HA/PMMA ..................................... 35 4.1. Introduction.................................................................................................. 35 4.2. Materials and Methods................................................................................. 38 4.2.1. Material Processing.................................................................... 38 4.2.2. Bending Tests............................................................................. 39 4.2.3. Compression Test....................................................................... 39 4.2.4. Physicochemical Analysis.......................................................... 40 4.2.5. Nano-indentation........................................................................ 41 4.2.6. Data Analysis............................................................................. 43 4.3. Results.......................................................................................................... 43 4.3.1. Global Bending Behavior........................................................... 43 4.3.2. Local Mechanical Properties of HA........................................... 44 4.3.3. Local Interfacial Mechanical Properties..................................... 44 4.3.4. Surface Bioactivity..................................................................... 46 4.3.5. In vitro Global Elastic Mechanical Behavior............................. 46 4.3.6. In vitro Interfacial Mechanical Properties.................................. 47 4.4. Discussion.................................................................................................... 48 4.5. Conclusion ................................................................................................... 55 5. An Alternative Approach to Bone Replacement .................................................. 79 5.1. Introduction.................................................................................................. 79 vi 5.2. Hydrogels..................................................................................................... 80 5.3. Poly(N-isopropylacryamide)........................................................................ 81 5.4. Preliminary Studies...................................................................................... 83 5.4.1. PNIPAAm Co-polymer .............................................................. 83 5.4.2. Mechanical Properties of PNIPAAm-based Hydrogels ............. 84 5.4.3. Bioactive Material Component .................................................. 84 5.4.4. Phase Transformation................................................................. 86 5.4.5. Rigid Polymer Supplement ........................................................ 87 5.4.6. Polymerization Kinetics............................................................. 88 5.5. Summary...................................................................................................... 88 6. An injectable Bioactive Hydrogel Composite ...................................................... 97 6.1. Introduction.................................................................................................. 97 6.2. Materials and Methods............................................................................... 100 6.2.1. Synthesis PNIPAAm-MPS-PEGDM ....................................... 100 6.2.2. Polymer Characterization......................................................... 100 6.2.3. LCST Determination ................................................................ 101 6.2.4. Injectability and Viscosity Studies........................................... 101 6.2.5. Change in Volume Estimation ................................................. 102 6.2.6. Bioactivity Characterization..................................................... 102 6.2.7. In vitro Compressive Test ........................................................ 103 6.3. Results........................................................................................................ 104 6.3.1. Physical Properties................................................................... 104 6.3.2. Bioactivity Kinetics.................................................................. 106 vii 6.3.3. In vitro Mechanical Properties ................................................. 108 6.4. Discussion.................................................................................................. 108 6.5. Conclusion ................................................................................................. 115 7. Future Work........................................................................................................ 131 8. Novel Contributions............................................................................................ 133 List of References ..................................................................................................... 135 Vita...........................................................................................................................
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