Enhancing the cycle-life of initial-anode-free lithium-metal batteries by pre-lithiation in Mn-based Li-rich spinel cathodes

Abstract

Anode-free lithium metal batteries (AF-LMBs) are attracting growing attention due to the burgeoning pursuit of high energy density. However, the poor reversibility of lithium-ion plating/stripping on the Cu anode triggers multiple issues, including rapid capacity loss, active lithium loss, and short lifetime. Herein, a cathode pre-lithiation strategy combined with a fluorine-containing electrolyte is introduced to achieve long-lifetime AF-LMBs. Furthermore, contact pre-lithiation, a more advanced and convenient strategy, has been introduced to precisely control the lithiation degree by adjusting the contact time. It has been demonstrated that over-lithiated Li_1.3Mn₂O₄ can deliver additional lithium ions during the charging process, thus exhibiting 94.4% capacity retention after 40 cycles.