Product Variation in Reactions of MI3(thf)4 with Bis(Mesitoyl)Phosphide Across the M = U, Np, Pu Series

Carpenter, Stephanie Hope; Jones, Margaret Rose; Lussier, Daniel Joseph; Gaunt, Andrew James; Murillo, Jesse; Tondreau, Aaron M.

doi:10.1021/acs.inorgchem.4c04433

Title: Product Variation in Reactions of MI₃(thf)₄ with Bis(Mesitoyl)Phosphide Across the M = U, Np, Pu Series

Journal Article · 03 April 2025 · Inorganic Chemistry

DOI: https://doi.org/10.1021/acs.inorgchem.4c04433 · OSTI ID:2547065

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Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

A series of reactions using sodium bis(mesitoyl)phosphide (^MesBAP^–) with the actinide starting material AnI₃(thf)₄ (An = U, Np, Pu) as well as the analogous reaction with CeI₃(thf)₄ was performed. Similar U and Np An(^MesBAP)₄ (An = U, Np) products were obtained in the +4-oxidation state. The thorium homologue was synthesized using ThI₄(dme)₂ to generate Th(^MesBAP)₄, which was employed as a diamagnetic and predominantly redox inert metal center for comparison. The resulting product isolated from the analogous reaction with PuI₃(thf)₄ was [Na(thf)][Pu(^MesBAP)₄], where the metal coordinated four ligands and retained the +3-oxidation state. This result is distinct from that obtained from the reaction with CeI₃(thf)₄, where the Ce³⁺ product was Ce(^MesBAP)₃(thf)₂. The compounds were isolated and characterized by X-ray diffraction, ultraviolet–visible (UV–vis)-nIR and NMR spectroscopies, and cyclic voltammetry. The synthetic results reveal how different redox stabilities across the 5f series can result in divergent reactivity of Pu. Electrochemical experiments produced redox features that suggest the potential to form reduced complexes supported by the ^MesBAP ligand framework.

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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC). Office of Basic Energy Sciences (BES)

Grant/Contract Number:: 89233218CNA000001; AC52-06NA25396

OSTI ID:: 2547065

Report Number(s):: LA-UR--24-20671

Journal Information:: Inorganic Chemistry, Journal Name: Inorganic Chemistry Journal Issue: 15 Vol. 64; ISSN 0020-1669

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Product Variation in Reactions of MI3(thf)4 with Bis(Mesitoyl)Phosphide Across the M = U, Np, Pu Series

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Title: Product Variation in Reactions of MI₃(thf)₄ with Bis(Mesitoyl)Phosphide Across the M = U, Np, Pu Series