Isomerisation and Insertion Chemistry of Imidosilanes Enabled by Reversible Si(IV)/Si(II) Redox Shuttling

J Jianqin Tang (Inorganic Chemistry Laboratory Department of Chemistry University of Oxford South Parks Road Oxford OX1 3QR UK) Y Yuwen Wang (Qingdao University , , ,) A Agamemnon E. Crumpton (Chemistry Research Laboratory, Department of Chemistry, University of Oxford, 12 Mansfield Road, Oxford OX1 3TA, U.K.) C Caitilín McManus (Inorganic Chemistry Laboratory Department of Chemistry University of Oxford South Parks Road Oxford OX1 3QR UK) S Simon Aldridge (Inorganic Chemistry Laboratory, Department of Chemistry, University of Oxford, South Parks Road, Oxford OX1 3QR, U.K.)

Abstract

Abstract Spontaneous redox shuttling at silicon is very rare, primarily reflecting the thermodynamic challenges associated with reduction processes for lighter p ‐block elements. Here we show that the reactions of boryl‐substituted silylene {PhC( t BuN) 2 }Si{B(NDippCH) 2 } with an organo‐azide proceed through a Si(IV)‐Si(II)‐Si(IV) series of redox processes involving both oxidative and reductive ligand migration steps. Each of the isomeric compounds related through this reaction manifold is isolable (and can be structurally characterised by X‐ray crystallography), with the overall free energy profile being close to thermo‐neutral. Broader studies within group 14 imply that this redox shuttling is unique to silicon and that reductive ligand migration also plays a role in O‐atom insertion chemistry.

Article Details

Volume / Issue Vol. 64, Issue 26
Published June 24, 2025
ISSN 1433-7851
Publisher Wiley

Journal Info

Angewandte Chemie International Edition

Wiley

ISSN: 1433-7851 Physical Sciences

Authors (5)

J

Jianqin Tang

Inorganic Chemistry Laboratory Department of Chemistry University of Oxford South Parks Road Oxford OX1 3QR UK

Y

Yuwen Wang

Qingdao University , , ,

A

Agamemnon E. Crumpton

Chemistry Research Laboratory, Department of Chemistry, University of Oxford, 12 Mansfield Road, Oxford OX1 3TA, U.K.

C

Caitilín McManus

Inorganic Chemistry Laboratory Department of Chemistry University of Oxford South Parks Road Oxford OX1 3QR UK

S

Simon Aldridge

Inorganic Chemistry Laboratory, Department of Chemistry, University of Oxford, South Parks Road, Oxford OX1 3QR, U.K.