Phase Engineering of Two-Dimensional WS2 Nanostructures for Superior Hybrid Supercapacitors

Abstract

Two-dimensional (2D) tungsten sulfide (WS2) has recently emerged as a nontrivial material for electrochemical applications; however, the boundaries associated with its 1T (instability) and 2H (low electrical conductivity) phases limit its electrochemical parameters. In this work, this issue is addressed using an exclusive chemical approach to evolve a dual-phase 1T-2H WS2 heterostructure that combines two different 1T (trigonal) and 2H (hexagonal) phases directly on the current collector which demonstrated 2D transformable phase structure, large interlayer distance, and highly exposed edge active sites. A simple inert-atmosphere annealing approach under phosphorus vapors is designed to elicit a fractional phase conversion of WS2 from conventional 2H to the 1T phase, where phosphorus is accommodated in the WS2 interspace and lattice, resulting in interlayer expansion. Theoretical calculations confirmed that the 1T WS2 structure formed after phosphorus doping exhibits semimetallic feature with no band gap, thereby elucidating the high electrical conductivity. The presence of edge-enriched metallic phase and interlayer engineering of 1T-2H WS2 heterostructure validates the exceptional sodium (Na+) ion intercalation when tested in hybrid supercapacitor (HSCs) against Prussian blue analog (PBA) cathodes. As a result, the assembled HSC cell with a 1T-2H WS2 heterostructured anode and a CuFe-PBA cathode shows superior specific energy of 65.5 Wh kg-1 at a specific power of 784 W kg-1, and maintains 75% rate capability and 95.7%cycling stability over 10,000 cycles. This work paves a technique for engineering a simple phase transition of 2D materials and sheds light on the expansion of high-performance next-generation energy storage systems.