Electronic coupling effect of multi-metallic heterostructure to enhance oxygen evolution reaction for quasi-solid-state Zn-air batteries

•A heterostructure consisting of Co@NC and NiMo-LDH was achieved.•Electron coupling in heterogeneous structures accelerates the electron transport rate.•The DFT results confirm the synergetic effect between the Co@NC and NiMo-LDH.•The assembled Zn-air battery exhibit a high paek density of 210 mW cm-2. It remains an urgent task to design electrocatalysts with fast oxygen evolution reaction (OER) kinetics and enriched active sites for flexible Zn-air batteries. In this paper, a structure engineering strategy is proposed to design an electrocatalyst with a heterostructure comprising Co@NC and NiMo-LDH on carbon cloth, which serves as an air electrode for a quasi-solid-state Zn-air battery. This unique heterostructure significantly enhances electrocatalytic activity, producing low OER overpotentials of 198 mV at 10 mA cm-2. Moreover, the assembled rechargeable Zn-air battery exhibits a high peak density and long cycle stability. Density functional theory calculations indicate that the multimetallic heterostructure induced synergistic and electronic coupling effects among the metal active sites, facilitating rapid ion and electron transport during the OER process. In addition, the migration of oxygen species at the Ni and Mo sites reduces the reaction potential barrier, resulting in a low OER overpotential of 160 mV. The construction of multi-metallic heterostructures enables optimisation of the electronic environment around the active sites and synergistic enhancement of the OER activity, leading to high performance quasi-solid-state Zn-air batteries. [Display omitted]