Zinc (Zn) ion supercapacitors (ZISCs) have attracted considerable attention as a viable energy storage technology because they are cost-effective, safe, and environmentally friendly. However, cathode materials with suitable properties are rare and need to be explored. In this regard, metal carbides (MXenes) are a good choice for capacitive energy storage, but they exhibit low capacitance. The energy storage performance of MXenes can be bossed using functionalization with heteroatom doping, e.g., nitrogen (N), to simultaneously modify ZISCs' fundamental characteristics and electrochemical properties. Herein, we present an in-situ N-functionalization of Ti₃C₂T_x-MXene via a hydrothermal reaction with urea (denoted as N-Ti₃C₂T_x-MXene). N-functionalization into Ti₃C₂T_x-MXene raised Ti₃C₂T_x-MXene's interlayer spacing and boosted the Zn-ion storage in 1 M ZnSO₄ electrolyte. The N-Ti₃C₂T_x-MXene electrode delivered an excellent specific capacitance of 582.96 F/g at 1 A/g and retained an outstanding cycle stability of 94.62% after 5000 cycles at 10 A/g, which is 1.8 times higher than pristine Ti₃C₂T_x-MXene at identical conditions. Moreover, the N-Ti₃C₂T_x-MXene//Zn device demonstrated a maximum capacitance of 153.55 F/g at 1 A/g, retained 92% of its initial value after 5000 cycles, and its Coulombic efficiency was ~100%. This strategy considerably reduced Ti₃C₂T_x-MXene nanosheet restacking and aggregation and enhanced electrochemical performance. Further, this research elucidated N-Ti₃C₂T_x-MXene's charge-storage process and offered a fresh approach to the rational design of novel electrode materials for ZISCs.

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