Interfacial Charge‐Transfer Enhancement via High‐Entropy Alloy Regulated MXene Heterostructures for Asymmetric Supercapacitor Applications

MXenes exhibit exceptional chemical properties, which are primarily attributed to their diverse surface functional groups and tunable elemental composition. Chemical intercalation is commonly used to address interlayer stacking and improve MXene conductivity. Meanwhile, high‐entropy alloys (HEAs) are a groundbreaking category of materials with broad compositional flexibility that provide multiple active sites, facilitating electrochemical redox reactions in supercapacitors. Synergistically combining MXenes with HEAs offers significant potential for developing advanced energy storage technologies. Herein, a CrMnFeCoNi‐based HEA was successfully synthesized and doped with a Ti3C2F2 MXene through a hydrothermal approach. In a single‐electrode setup with a 1 m potassium hydroxide electrolyte, the prepared HEA@MXene exhibited an impressive specific capacitance of 872 F g−1 at a current density of 1 A g−1. Moreover, an asymmetric device constructed from this material exhibited an energy density of 72.66 Wh kg−1 at a power density of 640 W kg−1. Theoretical investigations using density functional theory (DFT) revealed that HEA integration enhances MXene conductivity and promotes hydroxide adsorption in solution, thereby improving supercapacitor performance.