High entropy alloy nanoparticles decorated carbon-based electrode as interfacial Li-ion localized accelerators for anode-free lithium metal batteries

Abstract

Lithium metal is deemed as the main representative of the material for next-generation energy storage cells. Nevertheless, the problems of lithium dendrite growth and anode electrode volume expansion have become difficult problems in practical applications. Here, we introduced lithophilic CuInNiSnCd HEA-NPs on the surface of three-dimensional (3D) carbon hosts through a high-temperature redox strategy (HEA/CF). The application of the HEA/CF 3D framework can effectively decrease the non-uniform current density of the anode electrode, thereby slowing down the volume expansion of lithium metal during cycling. The introduction of CuInNiSnCd HEA-NPs improves the lithophilic of the carbon substrate and reduces the nucleation potential of lithium. Meanwhile, their evolution process was monitored in situ by the dynamic electrochemical impedance spectroscopy (DEIS) with relaxation time (DRT) distribution analysis, and the introduction of the HEA was beneficial to improving Li⁺ migration kinetics. Consequently, the symmetric battery with Li@HEA/CF anode has an excellent cycle life of over 3000 h (10 mA cm^-2/10 mAh cm^-2). Furthermore, the anode-free HEA/CF assembled full cell has excellent rate performance with a stable CE of more than 99.2% after 160 cycles at 1C. This research contributes to the use of high-entropy materials in advanced energy storage batteries and provides valuable guidance for enhancing the performance of lithium batteries.