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research article

A Route to Stabilize Uranium(II) and Uranium(I) Synthons in Multimetallic Complexes

Keerthi Shivaraam, R. A.  
•
Keener, Megan  
•
Modder, Dieuwertje K.  
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April 4, 2023
Angewandte Chemie International Edition

Herein, we report the redox reactivity of a multimetallic uranium complex supported by triphenylsiloxide (−OSiPh3) ligands, where we show that low valent synthons can be stabilized via an unprecedented mechanism involving intramolecular ligand migration. The two- and three-electron reduction of the oxo-bridged diuranium(IV) complex [{(Ph3SiO)3(DME)U}2(μ-O)], 4, yields the formal “UII/UIV”, 5, and “UI/UIV”, 6, complexes via ligand migration and formation of uranium-arene δ-bond interactions. Remarkably, complex 5 effects the two-electron reductive coupling of pyridine affording complex 7, which demonstrates that the electron-transfer is accompanied by ligand migration, restoring the original ligand arrangement found in 4. This work provides a new method for controlling the redox reactivity in molecular complexes of unstable, low-valent metal centers, and can lead to the further development of f-elements redox reactivity.

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Angew Chem Int Ed - 2023 - Shivaraam - A Route to Stabilize Uranium II and Uranium I Synthons~.pdf

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Postprint

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http://purl.org/coar/version/c_ab4af688f83e57aa

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openaccess

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CC BY

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1.91 MB

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Adobe PDF

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a25302d7769d4480cabf12aafc69b0ee

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