Double Deprotonation of CH 3 CN by an Iron‐Aluminium Complex**

Abstract

Herein we present the first double deprotonation of acetonitrile (CH 3 CN) using two equivalents of a bimetallic iron‐aluminium complex. The products of this reaction contain an exceeding simple yet rare [CHCN] 2− dianion moiety that bridges two metal fragments. DFT calculations suggest that the bonding to the metal centres occurs through heavily polarised covalent interactions. Mechanistic studies reveal the intermediacy of a monomeric [CH 2 CN] − complex, which has been characterised in situ. Our findings provide an important example in which a bimetallic metal complex achieves a new type of reactivity not previously encountered with monometallic counterparts. [1, 2] The isolation of a [CHCN] 2− dianion through simple deprotonation of CH 3 CN also offers the possibility of establishing a broader chemistry of this motif.