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. 2024 Oct 21;63(43):e202409789.
doi: 10.1002/anie.202409789. Epub 2024 Sep 17.

A Four-Coordinate Pr4+ Imidophosphorane Complex

Andrew C Boggiano  1 , Sabyasachi Roy Chowdhury  2 , Michael D Roy  1 , Maximilian G Bernbeck  1 , Samuel M Greer  3 , Bess Vlaisavljevich  2 , Henry S La Pierre  1   4
Affiliations

A Four-Coordinate Pr4+ Imidophosphorane Complex

Andrew C Boggiano et al. Angew Chem Int Ed Engl. .

Abstract

The imidophosphorane ligand, [NPtBu3]- (tBu=tert-butyl), enables isolation of a pseudo-tetrahedral, tetravalent praseodymium complex, [Pr4+(NPtBu3)4] (1-Pr), which is characterized by a suite of physical characterization methods including single-crystal X-ray diffraction, electron paramagnetic resonance, and L3-edge X-ray near-edge spectroscopies. Variable-temperature direct-current magnetic susceptibility data, supported by multiconfigurational quantum chemical calculations, demonstrate that the electronic structure diverges from the isoelectronic Ce3+ analogue, driven by increased crystal field. The four-coordinate environment around Pr4+ in 1-Pr, which is unparalleled in reported extended solid systems, provides a unique opportunity to study the interplay between crystal field splitting and spin-orbit coupling in a molecular tetravalent lanthanide within a pseudo-tetrahedral coordination geometry.

Keywords: Imidophosphoranes; Lanthanides; Praseodymium; Tetravalent lanthanide complexes.

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