Decline Mechanism of Graphite/Lithium Metal Hybrid Anode and Its Stabilization by Inorganic-Rich Solid Electrolyte Interface

Abstract

The graphite/lithium metal hybrid anode shows great potential for achieving high-specific-energy lithium batteries. Despite the "dead lithium" problem caused by repeated stripping and deposition of Li component based on a conversion reaction, the degradation mechanism, based on intercalation reaction, of graphite in a hybrid anode is generally ignored. In this contribution, through in situ X-ray diffraction and in situ Raman analysis, we reveal that hysteresis and the mixed-phase state of graphite during deintercalation play a critical role in hybrid battery degradation. On the other hand, we successfully mitigated graphite degradation and increased the reversible capacity of the hybrid anode by introducing an inorganic-rich solid electrolyte interface. Remarkably, the hybrid anode (30% higher specific capacity compared to graphite) exhibits an average coulombic efficiency of 99.11% and retains 96.13% of initial capacity over 120 cycles. This work sheds new light on the advancement of high-specific-energy lithium secondary batteries.