dc.description.abstract | The development of sustainable cyclodextrin-derived polymer networks and their potential applications in selective molecular adsorption is described. Macrocycle-derived polymer networks represent a promising class of adsorbents that have been applied in solution phase adsorption, vapor adsorption, and vapor sensing. Despite their promising properties, these materials still face challenges in large-scale synthesis and processing.
This dissertation begins with an introduction into the properties of macrocycle-derived functional materials and a brief overview of their applications followed by a discussion of the challenges and future perspectives for the field.
The design and synthesis of cyclodextrin-derived polymer networks (CD-PN) is described in the second chapter. This new synthetic strategy is sustainable, suitable for large-scale production, and optimizes adsorption potential by enabling a high density of macrocyclic binding sites within the polymer network. The selective adsorption of organic molecules from aqueous solutions is demonstrated with CD-PNs exhibiting remarkable selective adsorption abilities.
Chapter three describes the development of polymer nanoparticles based on CD-PN. Non-aqueous, inverse emulsion polymerization was utilized for the synthesis of cyclodextrin-derived polymer nanoparticles (CD-PNP). The nanoparticle morphology enhances the accessibility of the cyclodextrin binding sites, while enabling solution processing of CD-PNP and facilitating their feasible incorporation into functional devices.
The fourth chapter describes the vapor adsorption applications of CD-PNPs towards benzene, toluene, ethylbenzene, and xylenes (BTEX). Benzene sorption isotherms and saturated vapor adsorption experiments were utilized to explore the adsorption properties of CD-PNPs. CD-PNPs boasted comparable adsorption capacities with benchmark materials, while exhibiting significantly improved selectivity. The application of this selectivity was explored in BTEX sensing with a composite chemiresistor device. The selectivity observed in BTEX adsorption by β-CD-PNP was maintained in the composite device responses to BTEX vapors. The presence of β-CD-PNP also significantly enhanced the device sensitivity.
Overall, this dissertation presents a versatile and sustainable synthetic strategy to develop functional cyclodextrin-based polymer networks. The feasible synthetic strategy allows for in situ crosslinking to form various morphologies, such as nanoparticles, to unlock the full potential of the macrocyclic material. This work highlights the promising applications of macrocycle-derived functional materials, while demonstrating the importance of material design for optimizing the corresponding material properties. | |