Single or Double: Which Is the Altar of Atomic Catalysts for Nitrogen Reduction Reaction?

Abstract Converting N 2 to NH 3 is an extremely valuable process but a long‐standing challenge in chemistry. The crux is the choice of catalysts, where single atomic catalysts (SAC) are always pursued as the altar of atomic catalysts. In this paper, double atomic catalysts (DAC) of TM 2 ‐C 2 N with SAC of TM‐C 2 N (TM = Cr, Mn, Fe, Co, and Ni) for nitrogen reduction reaction (NRR) are systematically compared. Unexpectedly, TM 2 ‐C 2 N are more suitable than TM‐C 2 N as catalysts for NRR. Moreover, the Mn 2 ‐C 2 N endows the highest catalytic activity with the lowest potential of −0.23 V versus RHE, which is the best among all reported calculation results for NRR under ambient conditions. As a result, a new way to design catalysts with DAC is provided.