Abstract

In this work, a new asymmetric amidine–imine ligand, using 1,8-diaminonaphthalene as a rigid platform, was synthesized and characterized, and its ability to form complexes with aluminum(III) was investigated. Several aluminum complexes were synthesized and characterized in solution and in the solid state. The synthesis of a dihalogenated aluminum(III) complex (AlI2 L) using a reducing agent revealed an atypical pathway, which was investigated using Density Functional Theory (DFT). The dimethylated aluminum complex AlMe2 L and the dihalogenated aluminum complex AlI2 L were evaluated as catalysts for the transformation of CO2 and epoxides into cyclic carbonates in the presence of Bu4 NI as a co-catalyst or in a single-component system, respectively. AlMe2 L/Bu4 NI appeared to be the most efficient system under 1 bar of CO2 at 90◦ C. © 2025 by the authors.