Nanosynthesis and Characterization of Cu1.8Se0.6S0.4 as a Potential Cathode for Magnesium Battery Applications.

ABSTRACT

Copper selenide (Cu-Se) and copper sulfide (Cu-S) are promising cathodes for magnesium-ion batteries. However, the low electronic conductivity of Cu-Se system results in a poor rate capability and unsatisfactory cycling performance. Mg-ion batteries based on the Cu-S cathode exhibited large kinetic barriers during the recharging process owing to the presence of polysulfide species. This work attempts to circumvent this dilemma by doping Cu1.8Se by sulfur, which replaces the selenium in the CuSe lattice to form Cu1.8Se0.6S0.4 nanocrystalline powder. The presence of sulfur will increase the electronic conductivity, and the presence of selenium will mitigate the effect of polysulfide species that hinder the kinetics of Mg2+. Herein, a Cu1.8Se0.6S0.4 nanocrystalline powder was synthesized by the solid-state reaction, yielding a highly pure and stoichiometric powder. The crystallographic structure of the nanopowder and the conversion-type storage mechanism have been attested via ex situ X-ray diffraction and energy-dispersive X-ray analysis. The nanocrystalline feature of Cu1.8Se0.6S0.4 was demonstrated by high-resolution transmission electron microscopy. An apparent surface morphology change during the charging/discharging process has been visualized by a field emission scanning electron microscope. Diffuse reflectance spectroscopy has discussed the variation of the band gap during charging and discharging. The full Mg/Cu1.8Se0.6S0.4 cells presented an initial discharge capacity of 387.99 mAh g-1 at a current density of 0.02 mA cm-2; moreover, they show moderate diffusion kinetics with DMg2+ ≈ 10-15 cm-2 s-1.