Divergent Stabilities of Tetravalent Cerium, Uranium, and Neptunium Imidophosphorane Complexes

Otte, Kaitlyn S.; Niklas, Julie E.; Studvick, Chad M.; Boggiano, Andrew C.; Bacsa, John; Popov, Ivan A.; La Pierre, Henry S.

doi:10.1002/anie.202306580

Title: Divergent Stabilities of Tetravalent Cerium, Uranium, and Neptunium Imidophosphorane Complexes

Journal Article · Fri Jun 16 00:00:00 UTC 2023 · Angewandte Chemie (International Edition)

DOI: https://doi.org/10.1002/anie.202306580 · OSTI ID:2421235

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^[3]; La Pierre, Henry S. ^[2]

Georgia Institute of Technology, Atlanta, GA (United States); OSTI
Georgia Institute of Technology, Atlanta, GA (United States)
University of Akron, OH (United States)

The study of the redox chemistry of mid-actinides (U–Pu) has historically relied on cerium as a model, due to the accessibility of trivalent and tetravalent oxidation states for these ions. Recently, dramatic shifts of lanthanide 4+/3+ non-aqueous redox couples have been established within a homoleptic imidophosphorane ligand framework. Herein we extend the chemistry of the imidophosphorane ligand (NPC=[N=P^tBu(pyrr)₂]^–; pyrr=pyrrolidinyl) to tetrahomoleptic NPC complexes of neptunium and cerium (1-M, 2-M, M=Np, Ce) and present comparative structural, electrochemical, and theoretical studies of these complexes. Large cathodic shifts in the M^4+/3+ (M=Ce, U, Np) couples underpin the stabilization of higher metal oxidation states owing to the strongly donating nature of the NPC ligands, providing access to the U^5+/4+, U^6+/5+, and to an unprecedented, well-behaved Np^5+/4+ redox couple. Furthermore, the differences in the chemical redox properties of the U vs. Ce and Np complexes are rationalized based on their redox potentials, degree of structural rearrangement upon reduction/oxidation, relative molecular orbital energies, and orbital composition analyses employing density functional theory.

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Research Organization:: Georgia Institute of Technology, Atlanta, GA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0019385

OSTI ID:: 2421235

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 34 Vol. 62; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Chemistry
coordination chemistry
density functional calculations
electrochemistry
ligand design
neptunium

CCDC 2246290: Experimental Crystal Structure Determination S., Otte, Kaitlyn; E., Niklas, Julie; M., Studvick, Chad https://doi.org/10.5517/ccdc.csd.cc2fdfz8 The current record is supplemented by this dataset	dataset	January 2023
CCDC 2246291: Experimental Crystal Structure Determination S., Otte, Kaitlyn; E., Niklas, Julie; M., Studvick, Chad https://doi.org/10.5517/ccdc.csd.cc2fdg0b The current record is supplemented by this dataset	dataset	January 2023
CCDC 2246292: Experimental Crystal Structure Determination S., Otte, Kaitlyn; E., Niklas, Julie; M., Studvick, Chad https://doi.org/10.5517/ccdc.csd.cc2fdg1c The current record is supplemented by this dataset	dataset	January 2023
CCDC 2246293: Experimental Crystal Structure Determination S., Otte, Kaitlyn; E., Niklas, Julie; M., Studvick, Chad https://doi.org/10.5517/ccdc.csd.cc2fdg2d The current record is supplemented by this dataset	dataset	January 2023
CCDC 2246294: Experimental Crystal Structure Determination S., Otte, Kaitlyn; E., Niklas, Julie; M., Studvick, Chad https://doi.org/10.5517/ccdc.csd.cc2fdg3f The current record is supplemented by this dataset	dataset	January 2023

Title: Divergent Stabilities of Tetravalent Cerium, Uranium, and Neptunium Imidophosphorane Complexes

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