Atomically Dispersed Uranium Enables an Unprecedentedly High NH 3 Yield Rate.

The low NH 3 yield rate is a grand challenge for electrocatalytic N 2 reduction to NH 3 . Herein, we report the first uranium single-atom catalyst (SAC) capable of catalyzing the electrochemical N 2 reduction reaction (NRR). The uranium SAC features a low limiting potential (<0.5 V) and near-zero free energy changes for N 2 adsorption and NH 3 desorption. The integration of these merits enables the uranium SAC to afford an unprecedentedly high NH 3 yield rate, 3-4 orders of magnitude higher than that of the Ru(0001) surface, which is widely recognized as an excellent NRR electrocatalyst. Further theoretical analysis reveals that the N 2 reduction catalyzed by the uranium SAC is synergistically regulated by the d and f electrons of atomic uranium. This work proposes a promising solution (that is, atomically dispersed uranium) to the daunting challenge associated with the low NH 3 yield rate, thus enabling the scalable production of NH 3 via electrochemical N 2 reduction.