Phase‐Reconfiguration‐Induced NiS/NiFe₂O₄ Composite for Performance‐Enhanced Zinc−Air Batteries

Abstract Constructing composite structures is an essential approach for obtaining multiple functionalities in a single entity. Available synthesis methods of the composites need to be urgently exploited; especially in situ construction. Here, a NiS/NiFe₂O₄ composite through a local metal−S coordination at the interface is reported, which is derived from phase reconstruction in the highly defective matrix. X‐ray absorption fine structure confirms that long‐range order is broken via the local metal−S coordination and, by using electron energy loss spectroscopy, the introduction of NiS/NiFe₂O₄ interfaces during the irradiation of plasma energy is identified. Density functional theory (DFT) calculations reveal that in situ phase reconfiguration is crucial for synergistically reducing energetic barriers and accelerating reaction kinetics toward catalyzing the oxygen evolution reaction (OER). As a result; it leads to an overpotential of 230 mV @10 mA cm⁻² for the OER and a half‐wave potential of 0.81 V for the oxygen reduction reaction (ORR); as well as an excellent zinc−air battery (ZAB) performance with a power density of 148.5 mW cm⁻². This work provides a new compositing strategy in terms of fast phase reconstruction of bifunctional catalysts.