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Praseodymium in the Formal +5 Oxidation State
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Praseodymium in the Formal +5 Oxidation State

Andrew Boggiano, Chad Studvick, Sabyasachi Roy Chowdhury, Julie Niklas, Haruko Tateyama, Hongwei Wu, Johannes Leisen, Florian Kleemiss, Bess Vlaisavljevich, Ivan Popov, …
ChemRxiv
09/04/2024
DOI: 10.26434/chemrxiv-2024-cb3zj
url
https://doi.org/10.26434/chemrxiv-2024-cb3zjView
Preprint (Author's original)This preprint has not been evaluated by subject experts through peer review. Preprints may undergo extensive changes and/or become peer-reviewed journal articles. Open Access

Abstract

The pentavalent oxidation state of praseodymium – a long-sought connection between lanthanide, early-transition, and actinide metal redox chemistries – has only been identified in gas-phase or matrix isolation environments. We report the low-temperature characterization of a molecular praseodymium complex in the formal +5 oxidation state, [Pr5+(NP(tBu3)4][X–] (where tBu = tert-butyl and X– = tetrakis(pentafluorophenyl)borate or hexafluorophosphate). Single-crystal X-ray diffraction, solution-state spectroscopic, solution magnetometric, density functional theory, and multireference wavefunction-based methods indicate a highly multiconfigurational, singlet ground state. An inverted ligand field drives this unique electronic structure, which establishes a critical link in understanding the bonding of high-valent metal complexes across the periodic table.

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