Additional‐Heating‐Enhanced Large‐Scale Metallic Molybdenum Disulfide Nanosheet Exfoliation for Free‐Standing Films and Flexible High‐Performance Supercapacitors

Abstract Octahedral metal phase molybdenum disulfide (1T‐MoS₂) shows excellent capacitive behaviour by storing charge via double layers over individual two‐dimensional (2D) layers and through Faradaic reactions on the Mo centre because of its multiple oxidation states. In this study, we fabricate a free‐standing film based on large‐scale 1T‐MoS₂ nanosheets and use it as an electrode for a flexible supercapacitor without any additives. The resulting free‐standing electrodes have a layered structure, hydrophilicity and high electrical conductivity, which are beneficial for electrolyte accessibility and fast ions transport. The specific volumetric capacitance of this pure 1T‐MoS₂‐based electrode is up to 407.1 F ⋅ cm⁻³ (the corresponding mass and area capacitance were 26.1 F ⋅ g⁻¹ and 184.8 mF ⋅ cm⁻², respectively). The all‐solid‐state 1T‐MoS₂ based supercapacitor shows extended stability (92.8% retention after 12, 000 cycles), high flexibility (only 12% drop after bending 180 degrees for 100 cycles) and bending cycling stability (86.2% retention after in‐situ bending 1500 times).