Focusing on the Subsequent Coulombic Efficiencies of SiOx: Initial High-Temperature Charge after Over-Capacity Prelithiation for High-Efficiency SiOx-Based Full-Cell Battery

SiO_x-based anode materials are considered to be promising and have been gradually commercialized due to their high specific capacity as well as the acceptable volume change during lithiation/delithiation and preferable cycling stability compared to that of Si. Nevertheless, their inherently low Coulombic efficiency hinders the large-scale application. Up to now, researchers have paid much attention to the initial Coulombic efficiency and developed a series of effective prelithiation strategies. However, the subsequent cycles (focusing on the 2nd to 10th), during which the SiO_x anode suffers great lithium consumption as well, have received scarcely any concerns. In this work, a strategy of high-temperature (50 °C) initial charge after an overcapacity prelithiation for a SiO_x-based full-cell battery is proposed. As high temperature can promote the reaction between lithium and the SiO₂ matrix of SiO_x, SiO₂ will experience a one-step thorough reduction rather than gradual conversion in subsequent cycles, improving the subsequent Coulombic efficiencies (SCEs) accordingly. Overcapacity prelithiation can be achieved safely at 50 °C without Li metal depositon, just enough to meet the more initial lithium demand of anode at 50 °C. Furthermore, the initial deeper reduction of SiO₂ will release extra Si, improving the reversible capacity consequently. With the 50 °C initial charge after an overcapacity prelithiation, the full-cell battery exhibits considerable capacity retention as expected. This work raises concerns on SCEs of SiO_x-based anode innovatively, providing a feasible avenue for improving the capacity retention of a SiO_x-based full-cell battery.