Boosting OER activity of Fe-N Moieties via Ni induced d-Orbital Tailoring for durable rechargeable Zn-Air batteries

Fe-N-C-based catalysts are considered the most promising Pt candidates due to their high oxygen reduction reaction (ORR) activity and low cost, whereas their oxygen evolution reaction (OER) performance is extremely poor due to the sluggish O-O coupling process, which hampers the practical application of rechargeable zinc-air batteries. Here, we in situ infiltrate Ni and Fe ions into metal triazolidine (MET)-derived N-doped porous carbon via a microporous confinement-pyrolysis strategy to enhance the OER activity of the Fe-N sites. The introduction of Ni induced the electronic delocalization of Fe atoms at the Fe-N center, which lowered the adsorption energy barriers for the decisive velocity step (O*-> OOH*), thus accelerating the O-O bond coupling and OER kinetics. In addition, the preferential formation of NiOOH at high OER potentials ensures the catalytic stability of zinc-air batteries by trapping Fe ions escaping from carbon corrosion to form FeOOH. The optimized catalyst (FeNiNC) has an overpotential of only 351 mV at a current density of 50 mA cm(-2) under alkaline conditions. More importantly, the assembled ZABs can be stably charged and discharged for more than 500 h at 10 mA cm(-2), demonstrating excellent battery charging and discharging stability. This work shows the great potential of strong electronic interactions between polymetals to improve Fe-N-C catalysts.