Efficient and Stable Dual-Active-Site of Core-Shell NiFe-Layered Double Hydroxide Anchored on FeMnON-N-Doped Carbon Nanotubes as Bifunctional Oxygen Electrocatalysts for Zn-Air Batteries

The bifunctional air electrodes with numerous dual-active sites and low cost are desirable to modify the performance of Zn-air batteries (ZABs). Metal–oxygen-nitrogen–carbon substrate (M = Mn, Fe, Ni, etc.) and NiFe-layered double hydroxide (NiFe-LDH) nanosheets are excellent catalysts in the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) processes, respectively. Hereby, we investigate a bifunctional electrocatalytic substrate with a 3D core–shell hierarchical architecture by anchoring high OER-active NiFe-LDH on ORR-active FeMnZIF-8@gC 3 N 4 -derived FeMnON-N doped carbon nanotubes bamboo like (NiFe-LDH@FeMnON-NC). This nanocomposite has unique features such as robust synergistic effects, high conductivity, balance, and optimization of surface chemical valences of Fe, Mn, and Ni atoms to boost the bifunctional ORR and OER properties and stability in ZABs. The NiFe-LDH@FeMnON-NC nanocomposite not only exhibited superior OER electroactivity with a low onset overpotential of 235 mV (10 mA cm −2 ) but also had excellent ORR activity with a current density of −5.48 mA cm −2 and onset potential of 1.04 V, which is better than or comparable to those of commercial Pt/C and RuO 2 . Rechargeable ZABs constructed by bifunctional NiFe-LDH@FeMnON-NC have a peak power density (235.41 mW cm −2 ), open-circuit potential (OCV) (1.53 V), small discharge/charge band gap of 0.74 V and excellent discharge stability.