Linker Defects Triggering Boosted Oxygen Reduction Activity of Co/Zn‐ZIF Nanosheet Arrays for Rechargeable Zn–Air batteries

Abstract The poor electronic conductivity and low intrinsically electrocatalytic activity of most metal–organic frameworks (MOFs) greatly limit their direct applications as oxygen reduction reaction (ORR) electrocatalysts. In this work, it is reported that introduction of linker defects can effectively trigger the ORR activity of leaf‐shaped zeolitic imidazolate framework (ZIF) by increasing the intrinsic activity of metal sites and electrical conductivity. Experimental results show that part of imidazole molecules is successfully removed from ZIF after a low‐temperature thermal treatment without destroying its structure integrity, resulting in the formation of unsaturated metal sites and faster electron transport rate. Consequently, the ZIF with imidazole molecules defects (D‐ZIF) exhibits a superior ORR activity than the pristine ZIF, possessing an onset potential of 0.86 V and higher half‐wave potential of 0.60 V. Furthermore, the home‐made Zn–air batteries with D‐ZIF as air cathode exhibit high open‐circuit voltage and well cycling stability. The developed linker‐deficient modulation strategy can provide a new prospect to enable MOF‐based electrocatalysts with efficient catalytic activity.