Ferric ion-assisted assembly of MXene/TiO2-graphene aerogel for ionic liquid-based supercapacitors

To achieve pseudocapacitance by driving reversible redox reactions is scientifically appealing to realize high energy density of supercapacitors (SCs). In this work, a unique ferric ions-assisted self-assembly MXene/TiO2-graphene aerogel composite (MXene/TiO2-Fe-G) is developed. The MXene/TiO2-Fe-G composite has a 3D hierarchical porous framework, large accessible specific surface area, and amorphous TiO2 modified on the surface of MXene nanosheets. Importantly, amorphous TiO2, generated from the partial oxidation of MXene, can contribute enormous pseudocapacitance via the reversible redox reaction with Lithium ions. In addition, ferric cations with variable valence states can also provide pseudocapacitance. A trinary ionic liquid-based electrolyte (1-ethyl-3-methylimidazolium bis(trifluoromethanesulfonyl)imide-acetonitrile-lithium bis(trifluoromethanesulfonyl)imide, EmimTFSI-ACN-LiTFSI) with a wide electrochemical stability potential window is also formulated to match the new material. Consequently, the MXene/TiO2-Fe-G composite as the negative electrode shows a superb specific capacitance of 196.4 F g−1 at 1 A g−1. An asymmetric supercapacitor assembled with the MXene/TiO2-Fe-G anode and self-synthesized nitrogen-doped reduced graphene oxide aerogel (N-RGA) cathode can deliver a high energy density of 54 Wh kg−1 at a high-power density of 1737 W kg−1. This work provides a possibility of implementing pseudocapacitance by changing the morphology and structure of MXene composites to match the ionic liquid-based electrolyte, which can considerably enhance the performance of MXene-based SCs.