Controllable Electrochemical Synthesis of Copper Sulfides as Sodium-Ion Battery Anodes with Superior Rate Capability and Ultralong Cycle Life

Sodium-ion batteries (SIBs) are prospective alternative to lithium-ion batteries for large-scale energy-storage applications, owing to the abundant resources of sodium. Metal sulfides are deemed to be promising anode materials for SIBs due to their low-cost and eco-friendliness. Herein, for the first time, series of copper sulfides (Cu2S, Cu7S4, and Cu7KS4) are controllably synthesized via a facile electrochemical route in KCl–NaCl–Na2S molten salts. The as-prepared Cu2S with micron-sized flakes structure is first investigated as anode of SIBs, which delivers a capacity of 430 mAh g–1 with a high initial Coulombic efficiency of 84.9% at a current density of 100 mA g–1. Moreover, the Cu2S anode demonstrates superior capability (337 mAh g–1 at 20 A g–1, corresponding to 50 C) and ultralong cycle performance (88.2% of capacity retention after 5000 cycles at 5 A g–1, corresponding to 0.0024% of fade rate per cycle). Meanwhile, the pseudocapacitance contribution and robust porous structure in situ formed during cycling endow the Cu2S anodes with outstanding rate capability and enhanced cyclic performance, which are revealed by kinetics analysis and ex situ characterization.