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Engineering and Modeling Carbon Nanofiller-Based Scaffolds for Tissue Regeneration

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Engineering and Modeling Carbon Nanofiller-Based Scaffolds for Tissue Regeneration ENGINEERING AND MODELING CARBON NANOFILLER-BASED SCAFFOLDS FOR TISSUE REGENERATION Dissertation Submitted to The School of Engineering of the UNIVERSITY OF DAYTON In Partial Fulfillment of the Requirements for The Degree of Doctor of Philosophy in Engineering By Nuha Hamad Al Habis, M.S. UNIVERSITY OF DAYTON Dayton, Ohio August, 2017 ENGINEERING AND MODELING CARBON NANOFILLER-BASED SCAFFOLDS FOR TISSUE REGENERATION Name: Al Habis, Nuha Hamad APPROVED BY: Khalid Lafdi, Ph.D. Donald Klosterman, Ph.D. Advisor Committee Chairman Committee Member Professor; Wright Brothers Endowed Joint Appointment with University of Chair in Nanomaterials, Chemical & Dayton Research Institute, Chemical Materials Engineering Department & Materials Engineering Department Tony Saliba, Ph.D. Katia Del Rio-Tsonis, Ph.D. Committee Member Wilke Committee Member Distinguished Professor; Dean Professor; Department of Biology, Emeritus, Chemical & Materials Center for Visual Sciences at Miami Engineering Department University (CVSMU) Robert J. Wilkens, Ph.D.,P.E. Eddy M. Rojas, Ph.D., M.A., P. E. Associate Dean for Research and Dean, School of Engineering Innovation Professor School of Engineering ii Qc Copyright by Nuha Hamad Al Habis All rights reserved 2017 ABSTRACT ENGINEERING AND MODELING CARBON NANOFILLER-BASED SCAFFOLDS FOR TISSUE REGENERATION Name: Al Habis, Nuha Hamad University of Dayton Advisor: Dr. Khalid Lafdi Conductive biopolymers are starting to emerge as potential scaffolds of the future. These scaffolds exhibit some unique properties such as inherent conductivity, mechanical and surface properties. Traditionally, a conjugated polymer is used to constitute a conductive network. An alternative method currently being used is nanofillers as additives in the polymer. In this dissertation, we fabricated an intelligent scaffold for use in tissue engineering applications. The main idea was to enhance the mechanical, electrical properties and cell growth of scaffolds by using distinct types of nanofillers such as graphene, carbon nanofiber and carbon black. We identified the optimal concentrations of nano-additive in both fibrous and film scaffolds to obtain the highest mechanical and electrical properties without neglecting any of them. Lastly, we investigated the performance of these scaffold with cell biology. iii To accomplish these tasks, we first studied the mechanical properties of the scaffold as a function of morphology, concentration and variety of carbon nanofillers. Results showed that there was a gradual increase of the modulus and the fracture strength while using carbon black, carbon nanofiber and graphene, due to the small and strong carbon-to- carbon bonds and the length of the interlayer spacing. Moreover, regardless of the fabrication method, there was an increase in mechanical properties as the concentration of nanofillers increased until a threshold of 7 wt% was reached for the nanofiller film scaffold and 1%wt for the fibrous scaffold. Experimental results of carbon black exhibited a good agreement when compared with data obtained using numerical approaches and analytical models, especially in the case of lower carbon black fractions. Second, we examined the influence of electrical properties of nanofillers based on the concentration and the geometry of carbon nanofillers in the polymer matrix using experimental and numerical simulation approaches. The experimental results showed an increase in conductivity as the amount of nanofiller concentration increased. And regardless of nanofiller type, the trend remained the same. The percolation threshold was around 4-5wt% of nano-additive with PCL and PAN matrices, respectively. However, at the same concentrations, conductivity was higher in graphene-based nanocomposites than for CNF and carbon black-based nanocomposites. The numerical modeling highlighted the effect of nanofillers as constructing a conductive network due to the aggregation phenomenon. The conductivity trend for carbon black and carbon nanofiber-based composites by the numerical simulation approach was similar to the experimental approach. iv Lastly, we studied the effect of these carbon nanocomposite-based scaffolds on the behavior of cell growth. The results showed that regardless of the scaffold shape (film or fiber) and the additive’s type, when the concentration of nano-additives was increased, electrical conductivity and cell density increased also. For a given nano-additive concentration and type, cell density increased in the scaffolds with fiber shape vs. the film. Importantly, as the conductivity of the scaffolds increased, so did the cell density. Consequently, this study has highlighted the close relationship between electrical conductivity, cell density and scaffold orientation. An increase in conductivity can be achieved in two ways: by molecular orientation of the nanofillers or by the appropriate selection of nano-additives such as graphene and carbon nanofiber. v Dedicated to my parents (Hamad & Amira) and my sibling vi ACKNOWLEDGMENTS My special thanks are in order to Dr. Khalid Lafdi, my advisor, for providing the time and equipment necessary for the work contained herein, and for directing this thesis and bringing it to its conclusion with patience and expertise. Thank you for helping me grow as an individual, a researcher and an engineer. I would also like to express my appreciation to my dissertation committee. Thank you for your patience, guidance and advice throughout my studies. Dr. Klosterman, thank you for your assistance with helping me learn all of the instruments. Dr. Del Rio-Tsonis, thank you for allowing me to do my work in your lab at the Miami University. Dr. Saliba, thank you for your support and being part of my committee. It was an honor to share ideas, meetings and discussions. It was also an honor to have each of you on my committee and I hold your thoughts and advice at the highest level. To my friends, thank you for your patience, knowledge and support. This includes Robyn Bradford-Vialva, who patiently helped with proofreading and editing; Dana Tobias, who offered guidance with the burning rate measurements; Christian Gutierrez, who supported me by giving me his time and knowledge through parts of this work. Additionally, I thank my lab members in Kettering Lab, specifically Saja Nabat. Special thanks to Hassan Abd Al Majeed who supported and helped me to overcome tough times. vii TABLE OF CONTENTS ABSTRACT ....................................................................................................................... iii ACKNOWLEDGMENTS ................................................................................................ vii LIST OF FIGURES .......................................................................................................... xii LIST OF TABLES .......................................................................................................... xvii LIST OF ABBREVIATIONS AND NOTATIONS ...................................................... xviii CHAPTER I LITERATURE REVIEW .......................................................................... 1 Background ................................................................................................................... 1 1. Tissue Engineering.............................................................................................. 1 2. Skin Grafts and Organ Transplants ..................................................................... 3 Introduction ................................................................................................................... 4 1. Tissue Scaffolds .................................................................................................. 5 1.1. Hard Scaffolds ............................................................................................. 9 1.2. Soft Scaffolds ............................................................................................ 11 2. Materials Approach to Improved Scaffold ....................................................... 12 2.1 Biopolymer and Compatible Polymers. ..................................................... 12 2.1.1. Compatibility .................................................................................... 18 2.1.2. Structural Properties ......................................................................... 19 3. Conductive Scaffolds ........................................................................................ 20 3.1. Conductive Polymers Approach ................................................................ 21 3.1.1. Polypyrrole (PPy) ............................................................................. 23 3.1.2. Polyaniline (PANI) ........................................................................... 25 3.1.3. Polythiophene (PTh) ......................................................................... 26 3.1.4. Blend Polymers ................................................................................ 27 3.2. Carbon Additives Approach ...................................................................... 32 3.2.1 Conductivity. ..................................................................................... 38 3.2.2. Surface Properties ............................................................................. 40 3.2.3. Cell Viability .................................................................................... 46 3.2.4. Durability .........................................................................................
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