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A new mechanism for the conversion of transition metal azides to imido complexes.

Density functional calculations reveal a new mechanism for the decomposition of rhenium alkyl azide. PhN3 binds to the rhenium center in an η1-diazoamino mode ([Re]—N(Ph)—N≡N) rather than the more common η1-terminal mode ([Re]—N═N═N—Ph). From this new intermediate direct loss of N2 is fast, while the previously postulated cyclic 4-centered intermediate/transition state are very unfavorable in this system.