Oxygen- and Nitrogen-Embedded Zigzag Hydrocarbon Belts

Angew Chem Int Ed Engl. 2020 Dec 21;59(52):23649-23658. doi: 10.1002/anie.202013149. Epub 2020 Nov 16.

Abstract

Despite the aesthetically appealing structures and tantalizing physical and chemical properties, zigzag hydrocarbon belts and their heteroatom-embedded analogues remain challenging synthetic targets. We report herein the synthesis of diverse O/N-doped zigzag hydrocarbon belts based on selective bridging of the fjords of resorcin[4]arene derivatives through intramolecular SN Ar and palladium-catalyzed intermolecular C-N bond formation reactions. Preorganized conformations of mono-macrocyclic, half-belt and quasi-belt compounds were revealed to facilitate cyclization reactions to construct heteroatom-linked octahydrobelt[8]arenes. The acquired products had strained square-prism-shaped belt structures in which all six-membered heterocyclic rings adopted an unusual boat conformation with equatorially configured alkyl groups. The unprecedented heteroatom-bearing belts also exhibited different photophysical and redox properties to those of octahydrobelt[8]arene analogues.

Keywords: nucleophilic aromatic substitution; octahydrobelt[8]arenes; palladium-catalyzed C−N bond formation; strained macrocycles; zigzag hydrocarbon belts.