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Dinitrogen cleavage by a dinuclear uranium(iii) complex.

Nadir Jori1, Megan Keener1, Thayalan Rajeshkumar2

  • 1Insititut des Sciences et Ingénierie Chimiques, Ecole Polytechnique Fédérale de Lausanne (EPFL) 1015 Lausanne Switzerland marinella.mazzanti@epfl.ch.

Chemical Science
|November 30, 2023
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Summary
This summary is machine-generated.

Removing alkali ions from uranium complexes enhances their ability to cleave dinitrogen (N2). This study reveals a new tetranuclear intermediate, enabling a six-electron transfer for N2 cleavage and functionalization.

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Area of Science:

  • Inorganic Chemistry
  • Organometallic Chemistry
  • Materials Science

Background:

  • Designing complexes for dinitrogen (N2) cleavage and functionalization requires understanding multimetallic cooperativity and alkali ion-binding effects.
  • Previous work established a K2-bound dinuclear uranium(III) complex for N2 reduction.

Purpose of the Study:

  • To investigate the impact of removing alkali metal ions from the second coordination sphere on the reactivity of dinuclear uranium(III) complexes towards N2.
  • To elucidate the reaction products and mechanism of N2 reduction in the absence of coordinated K+ ions.

Main Methods:

  • Synthesis and characterization of dinuclear uranium(III) complexes with varying K+ ion coordination.
  • Electrochemical studies (cyclic voltammetry) to assess reducing ability.
  • Reaction product analysis upon N2 addition.

Main Results:

  • Complete removal of K+ ions from the coordination sphere enhances the reducing ability of the uranium complex.
  • N2 addition to the K+-free complex yields a U(III)/U(IV) complex and a bis-nitride, terminal-oxo complex.
  • Evidence for a tetranuclear uranium-N2 intermediate, facilitating six-electron transfer and N2 cleavage.

Conclusions:

  • The absence of coordinated alkali ions is crucial for forming a tetranuclear intermediate and achieving N2 cleavage.
  • Demonstrates the possibility of a three-electron transfer from U(III) to N2.
  • Highlights the tunability of alkali ion binding and multimetallic cooperativity for N2 functionalization.