Tailoring of Three-Atom Metal Cluster Catalysts for Ammonia Synthesis

Electrocatalytic nitrogen reduction reaction (NRR) can realize the green production of ammonia while developing electrocatalysts with high selectivity and ability is still an ongoing challenge. Two-dimensional (2D) graphitic carbon nitride (CN) frameworks provide abundant hollow sites for stably anchoring several transition metal (TM) atoms to facilitate single-cluster catalysis, promising overcome problems low activity poor in process synthesis. Herein, extensive density functional theory (DFT) calculations were performed investigate feasibility six bimetallic triatomic clusters FexMoy (x = 1, 2; x + y 3) supported on C6N6, C2N, N-doped porous graphene (NG) as NRR electrocatalysts. Through a systematic screening strategy, we found that Fe2Mo–NG possesses highest limiting potential –0.36 V through enzymatic mechanism could be catalyst NH3 The Fe2Mo moiety moderately regulates electron transfer between intermediates NG, which ascribed enhanced performance. This work accelerates rational design catalysts field contributes broadening understanding cluster catalysis.