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The ionization of a molecule into a molecular ion inside the mass spectrometer causes instability in the molecule's structure due to the loss of an electron. This eventually leads to the fragmentation or breaking of some bonds in the molecule. The fragmentation occurs predominantly at specific bonds to yield relatively stable fragments.
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Nitrogen activation and cleavage by a multimetallic uranium complex.

Megan Keener1, Farzaneh Fadaei-Tirani1, Rosario Scopelliti1

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

Chemical Science
|August 3, 2022
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Summary
This summary is machine-generated.

New dinuclear uranium nitride complexes were synthesized to study nitrogen (N₂) cleavage. A uranium complex was reduced to a U(iii)/U(iii) species, enabling a 4-electron reduction of N₂ to nitride without alkali metals.

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Area of Science:

  • Organometallic Chemistry
  • Inorganic Chemistry
  • Materials Science

Background:

  • Multimetallic-multielectron cooperativity is crucial for metal-mediated nitrogen (N₂) cleavage to nitrides.
  • Low-valent uranium complexes can cleave N₂, but the exact electron transfer is often unclear.
  • Alkali metals are typically required as reducing agents for N₂ cleavage by uranium complexes.

Purpose of the Study:

  • To design and synthesize novel dinuclear uranium nitride complexes with diverse ancillary ligands.
  • To investigate the multielectron transformation of N₂ mediated by these uranium complexes.
  • To achieve N₂ cleavage to nitride using uranium complexes without alkali metal reductants.

Main Methods:

  • Synthesis of two heteroleptic diuranium nitride complexes: [K{UIV(OSi(OtBu)3)(N(SiMe3)2)2}2(μ-N)] (1) and [Cs{UIV(OSi(OtBu)3)2(N(SiMe3)2)}2(μ-N)] (3-Cs).
  • Electrochemical reduction of synthesized complexes to U(iii)/U(iv) and U(iii)/U(iii) analogues.
  • Isolation and characterization of N₂ reduction and cleavage products, including N₂4- and nitride species.

Main Results:

  • Successfully synthesized dinuclear uranium nitride complexes with varying ancillary ligands (OSi(OtBu)3 and N(SiMe3)2).
  • Demonstrated reduction of complexes to U(iii)/U(iv) and a U(iii)/U(iii) species capable of 4-electron N₂ reduction.
  • Isolated key N₂ reduction intermediates and cleavage products, including a N₂4- complex and nitride species, without alkali metals.

Conclusions:

  • The designed dinuclear uranium complexes facilitate multielectron N₂ transformations.
  • A U(iii)/U(iii) species was generated, enabling the 4-electron reduction of N₂ to N₂4-.
  • This study presents the first instance of N₂ cleavage to nitride by a uranium complex independent of alkali metal reducing agents.