A Redox-Active Iron-Organic Framework Cathodes for Sustainable Magnesium Metal Batteries.

Rechargeable magnesium metal batteries (RMBs) have shown promising prospects in sustainable energy storage due to the high crustal abundance, safety, and potentially large specific capacity of magnesium. However, their development is constrained by the lack of effective cathode materials that can achieve high capacity and stable magnesium storage at a practically reasonable rate. Herein, we construct a three-dimensional (3D) iron(III)-dihydroxy-benzoquinone (Fe(DHBQ)) metal-organic framework (MOF) material with dual redox centers of Fe cations and DHBQ anions for reversible storage of Mg in RMBs. Spectroscopic analysis and density functional theory (DFT) calculations reveal the redox chemistry of both Fe ions and carbonyls from DHBQ ligands during electrochemical processes. Benefiting from the rational structure, the Fe(DHBQ)∥Mg cells exhibit a high reversible capacity of 395.3 mAh/g, large energy density of 463.5 Wh/kg, and high power density of 2456.0 W/kg. Moreover, the high electronic conductivity (8.35 × 10 S/cm) and favorable diffusion path of Mg in Fe(DHBQ) endow the cells with exceptional cycling stability and rate capability with a long life of 5000 cycles at 2000 mA/g. The dual redox-active MOF demonstrates a category of advanced cathode materials for high-performance RMBs.