Advancement of Actinide Metal-Organic Framework Chemistry via Synthesis of Pu-UiO-66

Ashley M. Hastings, Debmalya Ray, Wooseok Jeong, Laura Gagliardi, Omar K. Farha, Amy E. Hixon

Research output: Contribution to journalArticle

Abstract

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 multifaceted computational methods were used to corroborate experimental values, examine inherent defects in the framework, decipher spectroscopic signatures, and elucidate the electronic structure. 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.

Original languageEnglish (US)
Pages (from-to)9363-9371
Number of pages9
JournalJournal of the American Chemical Society
Volume142
Issue number20
DOIs
StatePublished - May 20 2020

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