Beyond the Cocktail Effect: Pseudocapacitive Kinetics and Cycling-Induced Activation in a Ten-Cation High-Entropy Oxide Anode

Building on a previously established metal–organic framework (MOF)-inspired deca-nary high-entropy oxide anode/alternating current electrophoretic deposition (AC-EPD) platform, this study elucidates the multication distribution, charge-storage kinetics, and long-term cycling advantage of a binder- and conductive-agent-free deca-nary high-entropy anode. The active material was synthesized using a metal–organic framework 74 (MOF-74)-inspired deca-metal solvothermal coordination approach. Although the product evolved into a crystalline multi-metal oxide derivative rather than retaining the MOF-74 topology, energy-dispersive X-ray spectroscopy (EDS) confirmed the atomic-level homogeneous distribution of ten distinct cations (Mg, Ca, Sr, Ba, Mn, Fe, Co, Ni, Zn, Cd). The additive-free AC-EPD approach maximized the active material density and demonstrated the intrinsic electrochemical robustness of the high-entropy structure. Consequently, the electrode exhibited exceptional reversibility and superior rate capability (recovering ~310 mAh g−1 after 5.0 C cycling). Kinetic analysis revealed a dominant pseudocapacitive contribution (87% capacitive at 1.0 mV s−1), facilitating rapid lithium-ion transport. This work highlights a synergistic strategy combining MOF-inspired synthesis and electrophoretic fabrication for advanced high-entropy electrodes.