Abstract

Abstract[1+2] cycloaddition between a cyclic (alkyl)(amino)aluminyl anion (3) and diaryldiazomethane affords an AlN2three‐membered ring species (4). Compound (4) is thermally unstable and spontaneously releases N2gas under the mild reaction condition to generate an ion‐separated species5. An X‐ray study shows that the anionic part of5bears a considerable short exocyclic Al−C bond, and computational studies involving molecular orbital and natural bond orbital analysis indicate the Al=C π bonding character. The Al=C moiety of5undergoes intramolecular C−H activation. Moreover, reaction of5with a diazo compound leads to the reduction and complete cleavage of the N=N double bond.

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