Thermodynamically Stable Synthesis of the 1T-MoS₂/g-CN Superstructure with Rapid Redox Kinetics for Robust Capacitive...

Artificial superstructures with advanced physicochemical properties and electronic interfaces are of great importance for capacitive energy storage. Herein, by one-step phase transition and interfacial bridging, we achieve thermodynamically stable synthesis of the 1T-MoS₂/graphitic carbon nitride (g-CN) superstructure, where the carbon atoms of g-CN are covalently bridged on molybdenum atoms of the 1T phase molybdenum disulfide (1T-MoS₂) interface via C-Mo bonds. The DFT and MD calculations reveal that the 1T-MoS₂/g-CN superstructure with a strong interfacial interaction (covalent character: 97%), superior electron conduction (d-band center: -1.2 eV), abundant accessible channels (free volume: 53% whole space), and expedited redox kinetics (reaction energy barriers: 0.9 eV) can enhance interfacial charge transfer and faradaic ion accumulation. Therefore, the 1T-MoS₂/g-CN superstructure delivers a high specific capacitance of 2080 F g^-1 and excellent structural stability in KOH solution. Moreover, the solid-polymer-electrolyte chip-based 1T-MoS₂/g-CN supercapacitors can achieve a large energy density (73 mWh g^-1), outstanding cycling stability (91% capacitance retention after 10,000 cycles), and desired self-powered application.