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submitted on 17.02.2020, 20:59 and posted on 20.02.2020, 05:39by 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.