Nickel Single Atoms Anchored on Pyridinic N Dominated Porous Carbon for Enhanced Electrochemical 4‐Electron Oxygen Reduction

Abstract The four‐electron oxygen reduction reaction (ORR) is at the heart of key renewable energy technologies including fuel cells and rechargeable metal‐air batteries, but its wide use necessitates the development of efficient yet inexpensive catalysts. In this study, we have engineered single Ni atoms supported on nitrogen‐doped porous carbon with a high content of pyridinic nitrogen (referred to as Ni 1 –NC–G–NH 3 ). This was accomplished by pyrolyzing a Zn–Ni‐ZIF–glucose composite and subsequently treating it with ammonia. Remarkably, the glucose facilitates the formation of isolated Ni atoms within an ammonia reduction atmosphere. Furthermore, we have attained a substantial nitrogen doping level of up to 13 atomic percent, with a significant enrichment of pyridinic nitrogen, constituting 39.5% of the total nitrogen content. Owing to the synergistic interaction between the pyridinic nitrogen and the Ni–N x sites within the ZIF‐derived porous carbon matrix, the Ni 1 –NC–G–NH 3 catalyst demonstrates exceptional ORR catalytic activity and a nearly four‐electron selectivity that rivals the commercial Pt/C catalyst in alkaline environments.