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

Abstract

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.