The ability to tune the interfacial region in core-shell nanocomposites with a surface reconstruction as a source for surface energy (de)stabilization is presented. We consider Zn-doped nickel molybdate (NiMoO4) (ZNM) as a core crystal structure and AWO4 (A = Co or Mg) as a shell surface. Based on the density-functional theory method, the interfacial models of Zn-doped NiMoO4@AWO4 (ZNM@AW) core@shell structures are simulated and revealed to undergo surface reconstruction on the (-110) and (-202) surfaces of the AW shells, where the surface degradation of ZNM@MW(-110) is observed. The theoretical simulation is validated against the electrochemical performance of supercapacitor studies. To verify, we synthesize the hierarchical ZNM@AW core@shell semiconductor structured nanocomposites grown on a nickel foam conductive substrate using a facile and green two-step hydrothermal method. The morphology and chemical and electrochemical properties of the hierarchically structured nanocomposites are characterized in detail. The performance of the core@shell is significantly affected by the chosen intrinsic properties of metal oxides and exhibited high performance compared to a single-component system in supercapacitors. The proposed asymmetric device, Zn-doped NiMoO4@CoWO4 (ZNM@CW)||activated carbon, exhibits a superior pseudo-capacitance, delivering a high areal capacitance of 0.892 F cm-2 at a current density of 2 mA cm-2 and an excellent cycling stability of 96% retention of its initial capacitance after 1000 charge-discharge cycles. These fundamental theoretical and experimental insights with the extent of the surface reconstruction sufficiently explain the storage properties of the studied materials.
Keywords: ZNM@CW; ZNM@MW; core@shell; energy storage; interfacial; supercapacitor; surface reconstruction.