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submitted on 17.02.2020 and posted on 20.02.2020by Ashley Hastings, Debmalya Ray, WooSeok Jeong, Laura Gagliardi, Omar
K. Farha, Amy Hixon
We report the synthesis and characterization of the first plutonium metal-organic framework (MOF). Pu-UiO-66 expands the established UiO-66 series, which includes transition-metal, lanthanide, and early actinide elements in the hexanuclear nodes. The thermal stability and porosity of Pu-UiO-66 were experimentally determined and multi-faceted computational methods were used to corroborate experimental values, examine inherent defects in the framework and decipher spectroscopic signatures. The crystallization of a plutonium chain side product provides direct evidence of the competition that occurs between modulator and linker in MOF syntheses. Ultimately, the synthesis of Pu-UiO-66 demonstrates adept control of Pu(IV) coordination under hydrolysis-prone conditions, provides an opportunity to extend trends across isostructural UiO-66 frameworks and serves as the foundation for future plutonium MOF chemistry.