A Cu-MOF Material with Multiple Redox Centers as a High-Energy-Density Cathode for Li-Ion Batteries

Designing metal–organic cathodes that combine high voltage and high capacity requires co-optimizing redox-active metal nodes with multielectron organic ligands while preserving structural integrity. Here we identified CuNA(H2O)2 (NA = nitranilate) as a cathode that couples metal–ligand dual redox with water-assisted Li+ transport. Our first-principles computations reveal a six-electron intercalation process with three voltage plateaus at 3.04, 2.65, and 2.10 V vs Li/Li+, giving a theoretical capacity of 490.35 mAh g–1. Water forms an extended H-bond network that suppresses dissolution and supplies Li+-relay sites, yielding a diffusion coefficient of 1.46 × 10–5 cm2 s–1. The predicted CuNA(H2O)2 was synthesized; XRM confirms the structure, and galvanostatic tests (at 1.8–4.2 V) deliver an initial specific capacity of 474.2 mAh g–1, close to the theoretical value. Comparative calculations show that the metal node sets the voltage floor (Cu > Co ≈ Zn), whereas electron-withdrawing ligand substituents (−NO2 vs −Cl) raise both voltage and accessible electron count. Together, these results outline a practical strategy for high-energy, durable metal–organic cathodes: pair high-potential metal centers with light, multiredox ligands, and retain coordinated H2O to accelerate Li+ transport and stabilize the framework.