Uranium is a unique, multifaceted element that possesses rich chemistry and promise for challenging reactions. Pressing demands within nuclear stockpile stewardship and the nuclear energy sector call for development of this relatively understudied element. Uranium metal–organic frameworks (U-MOFs), a class of nanoscale hybrid materials, harness the exceptional attributes of uranium while also further developing its fundamental chemistry. While structure-property relationships in U-MOFs correlate the physical arrangement of atoms in a U-MOF lattice to the resulting material behavior, energy-structure-property relationships allow researchers to rationalize these correlations. In my thesis research, I identified and investigated energy-structure-property relationships in U-MOFs through the study of their dynamic crystalline structural transformations. I first illustrated separate aspects of energy-structure-property relationships as individual vignettes (structure-property relationships, energy-structure relationships, energy-property relationships). Finally, I tied energy, structure, and property together to explain why structure produces function. My thesis research ultimately offers a deeper understanding of U-MOF behavior, discovers novel U-MOF phenomena, and delineates design rules for the budding U-MOF field.
