Over the last twenty years, coordination-driven self-assembly has emerged as a powerful tool for the synthesis of unique supramolecular structures which would otherwise be much more difficult to obtain. The combination of directionally-coordinating organic ligands with metal ions or metal-containing secondary building units (SBUs) can lead to the formation of discrete metal-organic polyhedra (MOPs) or continuous three-dimensional networks known as metal-organic frameworks (MOFs). These tunable materials typically feature remarkably high surface areas, well-defined porosities, and have attracted attention for a wide range of potential applications including storage and separations, drug delivery, and catalysis; however, they often lack the bulk strength, stability, or compatibility necessary for feasible, full-scale production and use outside of the laboratory. Recently, promising efforts to improve the processability of MOPs and MOFs have focused on integration into a polymer matrix to harness both functional and mechanical properties; nevertheless, the synthesis of a cost-effective, defect-free, and highly functional material remains as an ongoing challenge.<br/>We report novel methods of polymer-inorganic hybridization in which coordination-driven self-assembly is used to directly integrate MOFs or MOPs into a polymeric material. Direct covalent attachment of polymers to metal-organic crystals results in improved interaction and a more uniform dispersion of crystalline fillers. Using post-synthetic ligand exchange with donor moieties incorporated into a polymer backbone, interaction is limited to the surface of the crystals, allowing for preservation of functionalities within the porous structures. The versatility of hybridization is demonstrated through several different synthetic techniques, a variety of parent components, and performance-based characterization, addressing many of the challenges currently faced by polymer-inorganic hybrid materials and encouraging the design of new materials to overcome them.

Coordination-driven self-assembly in polymer-inorganic hybrid materials

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

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