One of the major challenges in the preparation of crystalline organic materials with predesigned properties is the application of the solid-state chemistry strategy of substitutional solid-solutions for high-precision fine-tuning of properties. In inorganic materials, this is easily achievable because most inorganic compounds are based on the packing of spheres, enabling high symmetry and predictable structures in materials with variable composition. The ability to control both structure and composition independently in organic crystals has been a major challenge, as their packing is unpredictable, their properties change drastically upon molecular aggregation/functionalization, and organic molecules naturally phase-separate. In this talk, we will present our strategy of utilizing multivariate frameworks as matrices with predictable and controllable crystal structure, whose composition can be varied easily varied by careful selection of multivariate molecular building blocks. As proof of concept, we prepared a variety of low-transitivity zirconia frameworks—those with high topological symmetry—that are predictable, stable, and enable the imposition of tailored properties such as redox conductivity, dilute and multicolor emission, molecular polarity, and tunable aggregation-induced emission. We also demonstrate how our strategy enables the preparation of materials in single-crystal, thin-film, and bulk powder form for their use as applied materials with fine-tuned properties.

Low-transitivity multivariate metal-organic frameworks as materials with tunable redox and optoelectronic properties

ACS Spring 2022

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