Design and Development of Sustainable Materials with Mechanically-Interlocked Polymer Topologies to Address Environmental Challenges and Technological Limitations

Abstract

Slide-ring networks are complex topologies comprised of both steady covalent connections and dynamic supramolecular interactions. Due to their mechanically-interlocked polymer topology, slide-ring networks have become an emerging concept for developing materials with advanced mechanical and physical properties, including softness, elasticity, high stretchability, toughness, and high absorption capacity. This dissertation focuses on combining sustainable materials synthesized from natural feedstocks with degradable linkages and mechanically-robust polymer topology to address the significant environmental challenges and novel technological development. To address the environmental problem, a series of glucose-based degradable superabsorbent hydrogels has been designed and fabricated with the potential to tackle issues associated with sustainability, flooding, and drought, which are exacerbated by climate change. These hydrophilic networks were constructed by integrating glucose as a primary building block, both into cyclic oligomers and block polymers, which were ultimately combined into mechanically-interlocked slide-ring crosslinked materials. To improve technological limitations, thiol-ene/ -yne click chemistry was introduced into slide-ring topology for the development of versatile photoprintable materials to expand the properties of 3D printing products. These projects aim to meet needs associated with global water resource challenges and technological development while considering degradability and recyclability, through the fundamental study of structure-topology-morphology-properties of the mechanically-interlocked slide ring network.