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Polymer Hydrogels, Aerogels, and Foams As Biomimetics of the Extracellular Matrix

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Polymer Hydrogels, Aerogels, and Foams As Biomimetics of the Extracellular Matrix Polymer Hydrogels, Aerogels, and Foams as Biomimetics of the Extracellular Matrix by Mo Kit Chau A thesis submitted in conformity with the requirements for the degree of Doctor of Philosophy Department of Chemistry University of Toronto © Copyright by Mo Kit Chau 2016 Polymer Hydrogels, Aerogels, and Foams as Biomimetics of the Extracellular Matrix Mo Kit Chau Doctor of Philosophy Department of Chemistry University of Toronto 2016 Abstract Three-dimensional (3D) scaffolds that recapitulate the mammalian extracellular matrix (ECM) have potential applications as tissue engineering scaffolds and as in vitro cell culture material. This thesis describes the fabrication and characterization of microgels, aerogels, hydrogels, and foams that are biomimetics of the natural ECM. The ability to tune the mechanical property and structure of the resulting scaffolds is of particular importance. In Chapter 3, we explore a microfluidic platform for making biopolymer composite microgels in which the rigidity and structure can be tuned in high-throughput manner. Chapter 4 describes how cellulose nanocrystals can be used to make nanofibrillar hydrogels, in which the rheological properties and pore sizes can be controlled by the addition of inorganic salts. These properties are highly dependent on the size, charge, and concentration of the cations added. Chapter 5 describes the freeze-casting of aldehyde-functionalized cellulose nanocrystals and hydrazide-functionalized poly(oligoethylene glycol methacrylate) into anisotropic composite aerogels and their corresponding hydrogels. The aerogel structure could be tuned from fibrillar to columnar and lamellar by varying the freeze-cast composition. The Young’s modulus and swelling of the hydrogels differed parallel and perpendicular to the freeze-cast direction. Chapter 6 describes the freeze-casting of polyurethanes into anisotropic open-cell foams, which ii have anisotropic mechanical and thermal properties. The thermal conductivity of these foams could also be switched between anisotropic and isotropic modes. Key words: Hydrogel, microgel, foam, aerogel, extracellular matrix, thermal management, freeze-casting, polyurethane, biopolymer, polymer, anisotropic, cellulose nanocrystals, colloidal dispersion, agarose, gelatin, rheology, micropipette aspiration, mechanical properties, structure iii Acknowledgments I want to thank my supervisor, Professor Eugenia Kumacheva for her enthusiasm, motivation, and guidance throughout the years. You are an excellent researcher and teacher. I am grateful for the lessons you have given me in science and in life. I am always amazed by how you can manage so many diverse projects with such vision and success. You work hard to move projects forward, leading by example. As I said when we first met, I am a fan of your work and I always will be. It is an honor for me to have been in your group. I want to show my upmost appreciation for my committee members and teachers: Professor Mitch Winnik and Professor Dwight Seferos. Professor Winnik, you provided me the mental support during the most critical time of my PhD giving me the strength to carry on. Your scientific insight particularly with regards to the polyurethane project, was imperative for its completion. I want to say a heartfelt thank you. Your kindness will always be remembered. Anna Liza Villavelez, who helped me navigation through this program, I appreciate your years of diligence and your care for the students you work with. A special thanks to Professor Markus Retsch and his group for hosting me in Bayreuth Universität. I appreciate your hospitality and openness. To Professor Retsch, I really enjoyed the discussions we had about science and the intricacies of manuscript writing. I have benefited much from your guidance. I really like that you encourage discussion even/especially when the views are disparate. I think that highlights the spirit of how science should be. Thanks to Alexandra Phillips who trained me on the XFA, and Fabian Nutz and Patrick Hummel who performing experiments for us. Thanks to Dr. Sabine Rosenfeldt for her expertise in. I’d like to thank Bernd Kopera for his critical scientific contributions to this thesis. Your high IQ, wide knowledge base, and lack of fear for complicated equations gives me confidence to believe that you will excel in whatever you chose to do in the future. I want to thank NSERC CREATE IDEM for their years of funding and the NSERC CREATE IDEM group for encouraging a creative and collaborative. Thanks to Professor Harald Stover in particular for arranging this. I have enjoyed the wonderful NSERC CREATE meeting we had. They were fun and educational. I want to thank Professor Emily Cranston and Professor Todd iv Hoare for collaborating with us on the anisotropic hydrogel project. Kevin de France. Thank you for being an excellent partner to work with. Our tag-team approach was efficient and successful, allowing us to complete one task after another. Big thanks to the Ramachandran group, in particular Professor Arun Ramachandran, Suraj Borkar, Shashi Malladi, Rohit Sonthalia, and Ali Hussain Motagamwala, for their help on the pipette aspiration experiments. I would also like to thank everyone in the Kumacheva group for their continued support. It was a pleasure working with you all. Thanks to Diego Velasco and Ethan Tumarkin for guiding in me during my initial time in the group. A special thanks to Dr. Héloï se Thérien-Aubin, mentor, desk mate, and friend. You have been generous in sharing with me your vast knowledge. You have really been there for me over last five years. A special thanks Shivanthi Sriskandha. You are a hard-working and reliable individual. I think back to our time together, doing chemistry and occasionally being silly, with smiles and laughs (Oh, Heathcliff!). Vanessa Machado, thank you for working with me during my last year. You were immensely helpful. Big thanks to Sepehr Tehrani who took time to help us investigate polyurethanes by DSC. I would like to thank Ilya Gourevich, Dr. Neil Coombs, Dr. Battista Calvieri, and Dr. Steven Doyle for their technical support on electron microscopy. Also a thank you to the machine shop staff: Johnny Lo, John Ford, David Heath, Ahmed Bobat for their masterful creations for the freeze-casting projects. I’d like to thank staff in the NMR lab, Dima Pichugin and Darcy Burns, who are extremely competent at their job. I want to thank my original mentors, Dr. Robin Stoodley and Dr. Guillaume Bussiere who gave me my first shot at chemistry, and Professor Michael Wolf who initiated my interest in materials chemistry. To Mike: as I age, I appreciate more and more what you have done for me as a mentor and how you put the student’s well-being first. I would like to thank my friends from the department and friends back home for the years of encouragement and moral support. Finally and very importantly, I want to thank my family for raising me and providing me their unconditional love. To my mother, Ada Yip, who trained my mental discipline and stamina; my v father, Chak Chau, who endured hard labor to keep food on our table; my brother, Yu-Hang Chau, who aided my transition to Toronto in every way he could; and Aunty Lisa, who support us financially through the most difficult times of my childhood: I write this thesis in your honor. vi Preface This thesis has been organized as a series of manuscripts (see the list below) which have either been published in peer-reviewed scientific journals or is in the process of submission. As identified by primary authorship, all manuscripts were written by Mo Kit Chau with critical comments and revision by Eugenia Kumacheva and corresponding collaborators. The contributions of other authors are provided in detail below. Chapter 1 Polymer scaffolds as mimetics of the extracellular matrixes The results in this chapter are partly from manuscripts published in Supramolecular Nanofibrillar Polymer Hydrogels in Supramolecular Polymer Networks and Gels, Springer 2015. Authors: Mokit Chau, Shivanthi Sriskandha, Héloï se Thérien-Aubin, Eugenia Kumacheva Contributions: M. Chau contributed to the article writing and figure design. S. Sriskandha contributed to the article writing and figure design. H. Thérien-Aubin contributed to the article writing. Chapter 3 Microfluidic Generation of Composite Biopolymer Microgels with Tunable Compositions and Mechanical Properties The results in this chapter are mainly from manuscripts published in Biomacromolecules, 15, 2013. Authors: Mokit Chau, Milad Abolhasani, Héloï se Thérien-Aubin, Yang Li, Yihe Wang, Diego Velasco, Ethan Tumarkin, Arun Ramachandran, Eugenia Kumacheva Contributions: M. Chau contributed to the carrying out experiments, data analysis and interpretation, and article writing. M. Abolhasani, H. Thérien- Aubin, Y. Li, and Y. Wang helped with microfluidic experiments. D. Velasco and E. Tumarkin provided guidance. vii Chapter 4 Ion-Mediated Gelation of Aqueous Suspensions of Cellulose Nanocrystals The results in this chapter are mainly from manuscripts published in Biomacromolecules, 16, 2013. Authors: Mokit Chau, Shivanthi Sriskandha, Dmitry Pichugin, Héloï se Thérien-Aubin, Dmitro Nykypanchuk, Greǵory Chauve, Myriam Méthot, Jean Bouchard, Oleg Gang, Eugenia Kumacheva Contributions: M. Chau contributed to the carrying out experiments, data analysis and interpretation, and article writing. S. Sriskandha contributed to carrying out experiments and data analysis. D. Pichugin and H. Thérien-Aubin contributed to the NMR experiment and interpretation. D. Nykypanchuk and O. Gang contributed to the SAXS experiments and interpretation. G. Chauve, M. Méthot, J. Bouchard provided the raw materials. Chapter 5 Anisotropic Hydrogels Derived from Cellulose Nanocrystals The results in this chapter are mainly from a manuscript in preparation. Authors: Mokit Chau, Kevin J. De France, Bernd Kopera, Vanessa R. Machado, Sabine Rosenfeldt, Laura Reyes, Katelyn J. W. Chan, Stephan Förster, Emily Cranston, Todd Hoare, Eugenia Kumacheva Contributions: M. Chau contributed to the manuscript by designing and carrying out experiments, data analysis and interpretation, and article writing. B. Kopera helped with the freeze-casting setup design. K. J. De France and K. J.
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