Reusing the steel slag to design a gradient-doped high-entropy oxide for high-performance sodium ion batteries

Abstract

Herein, a high-entropy layered oxide (HEO) is proposed as an outstanding cathode material for long-life sodium-ion batteries. Based on the self-segregation of elements from surface to bulk phase, a multi-element gradient doped high-entropy cathode material is prepared by doping steel slag with available elements (Mg, Al, Si, Fe, Ca). The surface high-entropy region vastly improves the air stability of materials and reduces surface impurities and side reactions. The Na-O-Mg configuration of near-surface high-entropy region continuously stimulates the anionic redox activity, and the DEMS shows the high-strength Al-O bonding achieves zero oxygen release. Therefore, the LNSM-0.01 reveals a stable capacity of ∼24 mA h g−1 in the range of 4.0–4.5 V. The Ca2+ in bulk phase high-entropy region disrupts the Na+/vacancy ordering transition and enhances the kinetic performance (90 mA h g−1 at 1000 mA g−1), while Fe2+/3+ provides a large amount number of charge compensation. Further, DFT calculations prove that the entropy stability based on synergistic effect immeasurably reinforce the layered oxide configuration, building a more robust structural framework during cycling. This work deepens the understanding on multi-element gradient doping to prepare HEOs, and provides a novel pathway for resource utilization of solid waste.