2.4 V ultrahigh-voltage aqueous MXene-based asymmetric micro-supercapacitors with high volumetric energy density...

Two-dimensional MXenes are key high-capacitance electrode materials for micro-supercapacitors (MSCs) catering to integrated microsystems. However, the narrow electrochemical voltage windows of conventional aqueous electrolytes (≤ 1.23 V) and symmetric MXene MSCs (typically ≤ 0.6 V) substantially limit their output voltage and energy density. Highly concentrated aqueous electrolytes exhibit lower water molecule activity, which inhibits water splitting and consequently widens the operating voltage window. Herein, we report ultrahigh-voltage aqueous planar asymmetric MSCs (AMSCs) based on a highly concentrated LiCl-gel quasi-solid-state electrolyte with MXene (Ti₃C₂T ) as the negative electrode and MnO₂ nanosheets as the positive electrode (MXene//MnO₂-AMSCs). The MXene//MnO₂-AMSCs exhibit a high voltage of up to 2.4 V, attaining an ultrahigh volumetric energy density of 53 mWh cm^-3. Furthermore, the in-plane geometry and the quasi-solid-state electrolyte enabled excellent mechanical flexibility and performance uniformity in the serially/parallel connected packs of our AMSCs. Notably, the MXene//MnO₂-AMSC-based integrated microsystem, in conjunction with solar cells and consumer electronics, could efficiently realize simultaneous energy harvesting, storage, and conversion. The findings of this study provide insights for constructing high-voltage aqueous MXene-based AMSCs as safe and self-sufficient micropower sources in smart integrated microsystems.