Single-atom catalysts (SACs) have recently been shown to have high performance in catalyzing the synthesis of NH 3 from N 2 . Here, we systematically investigated a series of single transition metal atoms anchored on stepped CeO 2 (CeO 2 -S) to screen the potential electrocatalysts for a N 2 reduction reaction (NRR) via density functional theory computations. We first demonstrated that these SACs are stable via large calculated binding energies. Second, we evaluated the adsorption of *N 2 over CeO 2 -Ssupported single atoms. Here, those systems that can activate N 2 molecules were selected as candidates. We then showed that CeO 2 -S-supported single Mo and Ru atoms have high catalytic activity for NRR via low limiting potentials of −0.52 and −0.35 V, respectively. Meanwhile, the competitive hydrogen evolution reaction is highly suppressed over these two SACs because the adsorption of *N 2 is prior to *H. Finally, the origin of the NRR activity over these SACs was investigated. This work offers useful insights into designing high-performance CeO 2 -based electrocatalysts for NRR.

A phosphotungstic acid-supported single metal atom is a potential electrocatalyst for the nitrogen reduction reaction with high activity and high selectivity.

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