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Rechargeable magnesium batteries are attractive candidates for energy storage due to their high theoretical specific capacities, free of dendrite formation and natural abundance of magnesium. However, the development of magnesium secondary batteries is severely limited by the lack of high-performance cathode materials and the incompatibility of electrode materials with electrolytes. Herein, we report the application of CuS nanoflower cathode material based on the conversion reaction mechanism for highly reversible magnesium batteries with boosted electrochemical performances by adjusting the compatibility between the cathode and electrolyte. By applying non-nucleophilic electrolytes based on magnesium bis(hexamethyldisilazide) and magnesium chloride dissolved in the mixed solvent of tetrahydrofuran and N-butyl-N-methyl-piperidinium bis((trifluoromethyl)sulfonyl)imide (Mg(HMDS)2-MgCl2/THF-PP14TFSI) or magnesium bis(trifluoromethanesulfonyl)imide, magnesium chloride and aluminium chloride dissolved in dimethoxyethane (Mg(TFSI)2-MgCl2-AlCl3/DME), the magnesium batteries with CuS nanoflower cathode exhibit a high discharge capacity of ~207 mAh·g–1 at 100 mA·g–1 and a long life span of 1,000 cycles at 500 mA·g–1. This work suggests that the rational regulation of compatibility between electrode and electrolyte plays a very important role in improving the performance of multi-valent ion secondary batteries.
The authors thank the funding supports from the National Key R&D Program of China (No. 2017YFA0208200), the National Natural Science Foundation of China (Nos. 22022505 and 21872069), the Fundamental Research Funds for the Central Universities (Nos. 020514380266, 020514380272, and 020514380274) , the Scientific and Technological Innovation Special Fund for Carbon Peak and Carbon Neutrality of Jiangsu Province (BK20220008), the Nanjing International Collaboration Research Program (Nos. 202201007 and 2022SX00000955), and the 2021 Suzhou Gusu Leading Talents of Science and Technology Innovation and Entrepreneurship in Wujiang District (No. ZXL2021273).