Chemists have spent more than a century trying to make d-block catalysts that can convert atmospheric dinitrogen to ammonia, or to directly to amines, under mild conditions. A few have been developed, but even binding of dinitrogen to an f-block metal cation is extremely rare. In contrast to exploiting the strongly reducing capacity of the U(III) ion to pre-bind and dinitrogen, the use of dinucleating aryloxide frameworks allows traditionally non-reducible f-block cations to work in concert with added group 1 metal reductant to catalyse the reduction and functionalisation of dinitrogen. Further structural control by the ligand framework enables the first catalytic conversion of dinitrogen into a secondary silylamine by any metal.

f-Block aryloxide complexes as simple, homogeneous catalysts for the conversion of dinitrogen to ammonia or secondary silylamines

ACS Spring 2022

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