Synergistic Al−Al Dual‐Atomic Site for Efficient Artificial Nitrogen Fixation

Abstract Synthesis of ammonia by electrochemical nitrogen reduction reaction (NRR) is a promising alternative to the Haber–Bosch process. However, it is commonly obstructed by the high activation energy. Here, we report the design and synthesis of an Al−Al bonded dual atomic catalyst stabilized within an amorphous nitrogen‐doped porous carbon matrix (Al 2 NC) with high NRR performance. The dual atomic Al 2 ‐sites act synergistically to catalyze the complex multiple steps of NRR through adsorption and activation, enhancing the proton‐coupled electron transfer. This Al 2 NC catalyst exhibits a high Faradaic efficiency of 16.56±0.3 % with a yield rate of 29.22±1.2 μg h −1 mg cat −1 . The dual atomic Al 2 NC catalyst shows long‐term repeatable, and stable NRR performance. This work presents an insight into the identification of synergistic dual atomic catalytic site and mechanistic pathway for the electrochemical conversion of N 2 to NH 3 .