Anionic Te-Substitution Boosting the Reversible Redox in CuS Nanosheet Cathodes for Magnesium Storage

The conversion-type copper chalcogenide cathode materials hold great promise for realizing the competitive advantages of rechargeable magnesium batteries among next-generation energy storage technologies; yet, they suffer from sluggish kinetics and low redox reversibility due to large Coulombic resistance and ionic polarization of Mg²⁺ ions. Here we present an anionic Te-substitution strategy to promote the reversible Cu⁰/Cu⁺ redox reaction in Te-substituted CuS_1-Te nanosheet cathodes. X-ray absorption fine structure analysis demonstrates that Te dopants occupy the anionic sites of sulfur atoms and result in an improved oxidation state of the Cu species. The kinetically favored CuS_1-Te (x = 0.04) nanosheets deliver a specific capacity of 446 mAh g^-1 under a 20 mA g^-1 current density and a good long-life cycling stability upon 1500 repeated cycles with a capacity decay rate of 0.0345% per cycle at 1 A g^-1. Furthermore, the CuS_1-Te (x = 0.04) nanosheets can also exhibit an enhanced rate capability with a reversible specific capacity of 100 mAh g^-1 even under a high current density of 1 A g^-1. All the obtained electrochemical characteristics of CuS_1-Te nanosheets significantly exceed those of pristine CuS nanosheets, which can contribute to the improved redox reversibility and favorable kinetics of CuS_1-Te nanosheets. Therefore, anionic Te-substitution demonstrates a route for purposeful cathode chemistry regulation in rechargeable magnesium batteries.