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Open-Shell Early Lanthanide Terminal Imides.

Theresa E Rieser1, Renita Thim-Spöring1, Dorothea Schädle1

  • 1Institut für Anorganische Chemie, Eberhard Karls Universität Tübingen, Auf der Morgenstelle 18, 72076 Tübingen, Germany.

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|February 25, 2022
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Summary
This summary is machine-generated.

Researchers synthesized novel terminal lanthanide (Ln) imides for open-shell cations Ce(III), Nd(III), and Sm(III) using a new methane elimination reaction. This breakthrough overcomes previous limitations in synthesizing these important organometallic compounds.

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Area of Science:

  • Organometallic Chemistry
  • Lanthanide Chemistry
  • Inorganic Synthesis

Background:

  • Lanthanide (Ln) organometallic chemistry is dictated by ion size, electronegativity, and Lewis acidity.
  • Synthesizing terminal imides [Ln═NR] of smaller Ln ions (Sc(III), Lu(III), Y(III)) and Ce(IV) requires specific protocols.
  • Terminal imides of larger, open-shell Ln(III) cations (Ce(III), Nd(III), Sm(III)) have been challenging to synthesize.

Purpose of the Study:

  • To report the synthesis of terminal imides of open-shell lanthanide cations Ce(III), Nd(III), and Sm(III).
  • To investigate the factors governing the formation of these novel organometallic complexes.
  • To explore the reactivity and stability of these imide complexes.

Main Methods:

  • Reaction of Lewis acid-stabilized methylidene complexes [TpLn(μ3-CH2){(μ2-Me)MMe2}2] (Ln = Ce, Nd, Sm; M = Al, Ga) with 2,6-diisopropylaniline (H2NAr).
  • Methane elimination reaction to form arylimide complexes.
  • Characterization of products based on reaction conditions, including metal identity (M = Al, Ga), solvent, and amine properties.

Main Results:

  • Successful synthesis of terminal arylimides [TpLn(═NAr)(THF)2] for Ln = Ce, Nd, Sm, exclusively when M = Ga.
  • Formation of persistent Lewis acid-stabilized imides [TpLn(NAr)(AlMe3)] when M = Al.
  • Reversible formation of [GaMe3]-stabilized imides [TpLn(NAr)(GaMe3)] observed for Ln = Nd, Sm in noncoordinating solvents.

Conclusions:

  • A new reaction protocol enables the synthesis of previously elusive terminal imides of open-shell lanthanides.
  • The formation and stability of these imides are critically dependent on the lanthanide ion, Lewis acid, and steric/electronic properties of the amine.
  • This work expands the scope of lanthanide organometallic chemistry and provides access to new reactive intermediates.