Charge-Compensation in a Displacement Mg2+ Storage Cathode through Polyselenide-Mediated Anion Redox

Chalcogenides have been viewed as important conversion-type Mg2+-storage cathodes to fulfill the high volumetric energy density promise of magnesium (Mg) batteries. However, the low initial Columbic efficiency and the rapid capacity degradation remain challenges for the chalcogenide cathodes, as the clear Mg2+-storage mechanism has yet to be clarified. Herein, we illustrate that the charge storage mechanism of the Cu2-xSe cathode is a reversible displacement reaction along with a polyselenide (PSe) mediated solution process of anion-compensation. The unique anion redox improves charge storage, while the dissolution of PSe also leads to performance degradation. To address this issue, we introduce Mo6S8 into the Cu2-xSe cathode to immobilize PSe, which significantly improves performance, especially the reversible capacity (from 140 mAh g(-1) to 220 mAh g(-1)). This work provides inspiration for the modification of the Mg2+-storage cathode, which is a milestone for high-performance Mg batteries.

Automated summary

The charge storage mechanism of Cu2-xSe cathode is a reversible displacement reaction with a PSe mediated solution process. The anion redox enhances charge storage, but the dissolution of PSe leads to performance degradation. The introduction of Mo6S8 to immobilize PSe significantly improves the performance of the Cu2-xSe cathode. This work provides inspiration for the modification of Mg2+-storage cathodes.