Catalytic dinitrogen reduction by earth-abundant lanthanide complexes

06 October 2022, Version 1
This content is a preprint and has not undergone peer review at the time of posting.

Abstract

New man-made routes to convert atmospheric nitrogen into amines for fertilizer or advanced fuel cycles would ideally avoid the high temperatures and pressures that the Haber–Bosch process uses to fix half of the dinitrogen used worldwide. Furthermore, routes that operate at ambient conditions are also desirable for remote applications. In attempts to mimic nature, metal complexes from the d-block of the periodic table have long been targets for the nitrogen reduction reaction (N2RR), with hundreds of N2-bound compounds reported, but only a handful of catalysts made. Even now, N2 binding to an f-block complex is considered rare. Here we report simple catalysts made from earth-abundant members of the f-elements that can catalyze the N2RR reaction at ambient conditions. Moreover, their molecular shape enables us to tune for production of either bis- or tris- substituted amines. These results suggest new catalytic applications for f-block ions that are as abundant as copper, and less toxic than iron.

Keywords

lanthanide
rare earth
N2RR
dinitrogen activation
O-ligands

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