Highly Stable Metal-Organic Framework with Redox-Active Naphthalene Diimide Core as Cathode Material for Aqueous...

Recently, metal-organic frameworks (MOFs) as the cathode materials for aqueous zinc-ion batteries (ZIBs) received growing attention. Herein, a novel MOF, Ni-Ndi-trz (Ndi-trz=2,7-di(4H-1,2,4-triazol-4-yl)benzo[lmn][3,8]phenanthroline-1,3,6,8(2H,7H)-tetraone) was synthesized through a solvothermal method. Its rational design using a naphthalene diimide (Ndi) core allowed the formation of a four-fold interpenetrated pcu (primitive cubic) topology. The as-synthesized Ni-Ndi-trz is highly stable over a wide pH range (0-12) for 30 days, which is critical to ensure the decent cyclability of zinc-ion batteries (ZIBs). When used as the cathode material of ZIBs, it shows a high initial specific capacity of 90.7 mAh g^-1 and excellent cycling stability. Remarkably, three-electrode system tests, ex situ FTIR, UV/Vis and XPS spectra revealed that the Ndi core of Ni-Ndi-trz undergoes a reversible interconversion between the keto and enol forms when interacting with Zn²⁺ ions. This work may shed light on the feasibility of designing novel MOFs and exploring their mechanisms for zinc ion batteries.