Chemists have spent more than a century trying to make d-block catalysts that can convert atmospheric dinitrogen to ammonia, or directly to amines, under mild conditions. In attempts to mimic nature, metal complexes from the d-block of the periodic table have been extensively explored as homogeneous catalysts for the nitrogen reduction reaction (N2RR), with hundreds of N2-bound compounds reported, but only a handful of catalysts made. Until recently, even N2 binding to an f-block complex was considered impossible. Here we report simple f-block catalysts for the N2RR reaction under ambient conditions. We use aryloxide frameworks that enable these traditionally non-reducible f-block cations to work in concert with added group 1 metal reductants as mild catalysts for the conversion of dinitrogen to different amine products.

f-block  aryloxide complexes as simple, homogeneous catalysts for the ambient conversion of N2 to bis- or tris- silylamines

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