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Unravelling the Roles of Solvophobic Effects and π⋅⋅⋅π Stacking Interactions in the Formation of [2]Catenanes Featuring Di‐(N‐Heterocyclic Carbene) Building Blocks

Ya‐Wen Zhang, Ye Lu, Li‐Ying Sun, Patrick D. Dutschke, Ming‐Ming Gan, Le Zhang, Alexander Hepp, Ying‐Feng Han, F. Ekkehardt Hahn

2023Angewandte Chemie International Edition26 citationsDOIOpen Access PDF

Abstract

Abstract A series of [2]catenanes has been prepared from di‐NHC building blocks by utilizing solvophobic effects and/or π⋅⋅⋅π stacking interactions. The dinickel naphthobiscarbene complex syn ‐[ 1 ] and the kinked biphenyl‐bridged bipyridyl ligand L 2 yield the [2]catenane [ 2‐IL ](OTf) 4 by self‐assembly. Solvophobic effects are pivotal for the formation of the interlocked species. Substitution of the biphenyl‐linker in L 2 for a pyromellitic diimide group gave ligand L 3 , which yielded in combination with syn ‐[ 1 ] the [2]catenane [ 3‐IL ](OTf) 4 . This assembly exhibits enhanced stability in diluted solution, aided by additional π⋅⋅⋅π stacking interactions. The π⋅⋅⋅π stacking was augmented by the introduction of a pyrene bridge between two NHC donors in ligand L 4 . Di‐NHC precursor H 2 ‐ L 4 (PF 6 ) 2 reacts with Ag 2 O to give the [Ag 2 L 4 2 ] 2 [2]catenane [ 4‐IL ](PF 6 ) 4 , which shows strong π⋅⋅⋅π stacking interactions between the pyrene groups. This assembly was readily converted into the [Au 2 L 4 2 ] 2 gold species [ 5‐IL ](PF 6 ) 4 , which exhibits exceptional stability based on the strong π⋅⋅⋅π stacking interactions and the enhanced stability of the Au‐C NHC bonds.

Topics & Concepts

SolvophobicCatenaneStackingChemistryLigand (biochemistry)AtropisomerPyrenePeryleneCrystallographyCarbeneStereochemistryOrganic chemistryMoleculeCatalysisReceptorBiochemistryN-Heterocyclic Carbenes in Organic and Inorganic ChemistryCatalytic Cross-Coupling ReactionsSupramolecular Chemistry and Complexes
Unravelling the Roles of Solvophobic Effects and π⋅⋅⋅π Stacking Interactions in the Formation of [2]Catenanes Featuring Di‐(N‐Heterocyclic Carbene) Building Blocks | Litcius