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. 2022 May 16;61(21):e202200748.
doi: 10.1002/anie.202200748. Epub 2022 Mar 8.

Self-Assembly of Molecular Trefoil Knots Featuring Pentadecanuclear Homoleptic AuI -, AuI /AgI -, or AuI /CuI -Alkynyl Coordination

Guang-Tao Xu  1 , Xiao-Yong Chang  2 , Kam-Hung Low  1 , Liang-Liang Wu  1 , Qingyun Wan  1 , Hui-Xing Shu  1 , Wai-Pong To  1 , Jie-Sheng Huang  1 , Chi-Ming Che  1
Affiliations

Self-Assembly of Molecular Trefoil Knots Featuring Pentadecanuclear Homoleptic AuI -, AuI /AgI -, or AuI /CuI -Alkynyl Coordination

Guang-Tao Xu et al. Angew Chem Int Ed Engl. .

Abstract

Metal-free and metal-containing molecular trefoil knots are fascinating ensembles that are usually covalently assembled, the latter requiring the rational design of di- or multidentate/multipodal ligands as connectors. In this work, we describe the self-assembly of pentadecanuclear AuI trefoil knots [Au15 (C≡CR)15 ] from monoalkynes HC≡CR (R=9,9-X2 -fluorenyl with X=nBu, n-hexyl) and [AuI (THT)Cl]. Hetero-bimetallic counterparts [Au9 M6 (C≡CR)15 ] (M=Cu/Ag) were self-assembled by reactions of [Au15 (C≡CR)15 ] with [Cu(MeCN)4 ]+ /AgNO3 and HC≡CR. The type of pentadecanuclear trefoil knots described herein is characterized by X-ray crystallography, 2D NMR and HR-ESI-MS. [Au9 Cu6 (C≡CR)15 ] is relatively stable in hexane; its excited state properties were investigated. DFT calculations revealed that non-covalent metal-metal and metal-ligand interactions, together with longer alkyl chain-strengthened inter-ligand dispersion interactions, govern the stability of the trefoil knot structures.

Keywords: Gold; Metal-Alkynyl Complexes; Metal-Metal Interactions; Supramolecular Chemistry; Trefoil Knots.

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