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A Germapyramidane Switches Between 3D Cluster and 2D Cyclic Structures in Single‐Electron Steps

Peter Coburger, Fabio Masero, Jonas Bösken, Victor Mougel, Hansjörg Grützmacher

2022Angewandte Chemie International Edition21 citationsDOIOpen Access PDF

Abstract

Abstract Reaction of the imidazolium‐substituted iphosphate‐diide, (Ipr) 2 C 2 P 2 ( IDP ), with GeCl 2 ⋅ dioxane and KBArF 24 [(BarF 24 ) − =tetrakis[(3,5‐trifluoromethyl)phenyl]borate)] afforded the dicationic spherical‐aromatic nido ‐cluster [Ge(η 4 ‐ IDP )] 2+ ([ 1 ] 2+ ) (Ipr=1,3‐bis(2,6‐diisopropylphenyl)imidazolium‐2‐ylidene). This complex is a rare heavy analogue of the elusive pyramidane [C(η 4 ‐C 4 H 4 )]. [ 1 ] 2+ undergoes two reversible one‐electron reductions, which yield the radical cation [ 2 ]⋅ + and the neutral Ge II species 3 . Both [ 2 ]⋅ + and 3 rearrange in solution forming the 2D aromatic and planar imidazolium‐substituted digermolide [ 4 ] 2+ and germole‐diide 5 , respectively. Both planar species can be oxidized back to [ 1 ] 2+ using AgSbF 6 . These redox‐isomerizations correspond to the fundamental transformation of a 3D aromatic cluster into a 2D aromatic ring compound upon reduction and vice versa. The mechanism of these reactions was elucidated using DFT calculations and cyclic voltammetry experiments.

Topics & Concepts

ChemistryCyclic voltammetryCluster (spacecraft)RedoxRing (chemistry)Yield (engineering)TrifluoromethylAromaticityCrystallographyBoronElectron countingMedicinal chemistryStereochemistryElectronElectrochemistryMoleculeInorganic chemistryOrganic chemistryPhysical chemistryMaterials sciencePhysicsElectrodeAlkylComputer scienceMetallurgyProgramming languageQuantum mechanicsGraphene research and applicationsMolecular Junctions and NanostructuresSynthesis and Properties of Aromatic Compounds