Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume -, Issue -, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202219212
Keywords
Aluminium; C-H Activation; Dianions; Iron; Nitriles
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In this work, we report the first double deprotonation of acetonitrile (CH3CN) using a bimetallic iron-aluminium complex. The products of this reaction contain a 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 [CH2CN](-) complex, which has been characterised in situ. Our findings provide an important example of a bimetallic metal complex achieving a new type of reactivity not previously encountered with monometallic counterparts. The isolation of a [CHCN](2-) dianion through simple deprotonation of CH3CN also offers the possibility of establishing a broader chemistry of this motif.
Herein we present the first double deprotonation of acetonitrile (CH3CN) 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 [CH2CN](-) 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 CH3CN also offers the possibility of establishing a broader chemistry of this motif.
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