Janus molybdenum di-chalcogenides based van der Waals bilayers for supercapacitor electrode design- effects of interlayer stacking orientations on quantum capacitance

Abstract

In this work, for the first time, the quantum capacitance of an artificial two-dimensional (2D) material system based on van der Waals (vdW) bilayer heterostructures of Janus Molybdenum Di-chalcogenides, MoXY (X≠Y, X/YS, Se, Te) have been extensively investigated for electrode design of electrical double-layer (EDL) supercapacitor. The effects of different interlayer stacking orientations on local charge distribution, interlayer charge transfer, energy band structure, and density of states (DOS) have been comprehensively analyzed and correlated with the excess charge density and quantum capacitance variation with local electrode potential. Furthermore, the total capacitance reduction with respect to EDL capacitance has been analyzed over a wide range of EDL capacitance, and the performance of vdW Janus bilayers has been systematically benchmarked against the natural monolayers/bilayers and Janus monolayers of Molybdenum Di-chalcogenides. The results demonstrate that the large interlayer charge transfer induced built-in interlayer electric field significantly reduces the energy band gap of vdW Janus bilayers for S–Te and Se–Te interlayer stacking, thus leading to a significantly superior quantum capacitance. Finally, the favorable valley-dependent effective mass and band-degeneracy in MoSTe/MoSeTe have greatly enhanced quantum capacitance in S–Te and Se–Te stacking, rendering these bilayers a highly attractive candidate for supercapacitor electrode design.