Engineering Versatile Particles and Films through Metal-Phenolic Chemistry
AffiliationChemical and Biomolecular Engineering
Document TypePhD thesis
Access StatusThis item is embargoed and will be available on 2023-06-10.
© 2021 Qizhi Zhong
Metal-phenolic chemistry, owing to its facile and versatile functions to manipulate dynamic interactions (e.g., interfacial adhesion and coordination crosslinking) at the molecular level, has emerged as a powerful tool for the rational design and engineering of hybrid metal-organic materials. In particular, leveraging a myriad of advantages, including a rich choice of building blocks, the combined properties of phenolics and metals, and dynamic coordination bonds, metal-phenolic network (MPN) particles and films have been explored in diverse fields such as drug delivery, functional elastomers, and water treatment. Despite significant progress, the mechanisms related to the kinetics (e.g., assembly process) and thermodynamics of MPNs are poorly understood, resulting in less control over the physicochemical properties of MPN particles and films. This thesis (1) reviews the fundamental insights about metal-phenolic interactions underpinning the dynamic nature of coordination bonds and universal adhesion to surfaces; (2) develops various assembly strategies, including oxidation-mediated assembly, enzyme-mediated assembly, and spray assembly, to endow MPN particles and films with controllable properties (e.g., thickness, pore size, roughness, and wettability) and functionalities (e.g., fluorescence, catalysis, radical scavenging, and UV-shielding), thereby (3) expanding the applications of MPN particles and films, specifically in gas separations, biomineralization, biomolecule conjugation, and oil-water separations; and (4) discusses the underlying mechanism governing the assembly process and resultant coordination states of MPNs by various characterization methods. Some unsolved challenges and perspectives related to MPN chemistry are also highlighted. This thesis provides insightful perspectives into the chemistry of MPN assembly and other metal-organic coordination complexes.
KeywordsMetal-organic films; Polyphenols; Self-assembly; Thin films; Nanoparticles; Surface modification; Oil-water separation; Patterned films; Spray assembly; Coordination assembly
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