In Situ Nitrogen Functionalization of 2D-Ti3C2Tx-MXenes for High-Performance Zn-Ion Supercapacitor

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 Ti3C2Tx-MXene via a hydrothermal reaction with urea (denoted as N-Ti3C2Tx-MXene). N-functionalization into Ti3C2Tx-MXene raised Ti3C2Tx-MXene’s interlayer spacing and boosted the Zn-ion storage in 1 M ZnSO4 electrolyte. The N-Ti3C2Tx-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 Ti3C2Tx-MXene at identical conditions. Moreover, the N-Ti3C2Tx-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 Ti3C2Tx-MXene nanosheet restacking and aggregation and enhanced electrochemical performance. Further, this research elucidated N-Ti3C2Tx-MXene’s charge–storage process and offered a fresh approach to the rational design of novel electrode materials for ZISCs.