Abstract
Sulfide-based all-solid-state lithium-sulfur batteries (ASSLSBs) hold immense promise for next-generation energy-storage due to their high theoretical energy density and enhanced safety. However, fatigue issues such as electrolyte cracking and interfacial damage caused by big volume changes of both elec- trodes and mechanical stress remain critical challenges. Herein, the distinct alternative against monotonical stress evolution is first analyzed in ASSLSBs employing pre-lithiated silicon-based anodes versus conventional lithium metal by using in-situ pressure-detection techniques. Notably, the pre-lithiated silicon-based system demonstrates an alternating stress dominance pattern that effectively stabilizes mechanical responses through stress cancellation effects. Moreover, the investigation shows that the stress-buffering effect of pre- lithiated silicon-based stems from the phase transition dynamics of intermedi- ate Li_(21)Si_5 during lithiation. The finite element modeling and micro-structural morphology analysis is employed to link phase transformation kinetics directly to mechanical stress modulation. This unique characteristic proves crucial in suppressing crack propagation within electrolytes while maintaining stable electrode/electrolyte interfaces. Consequently, the full-cell using pre-lithiated silicon-based achieves stable cycling performance with high S loading (4.5 mg cm~(−2)) at 0.5C (∼3.6 mA cm~(−2)), which outperforms conventional solid-state lithium-sulfur batteries. The discovered chemo-mechanical coupling principles provide new insights for developing high-stability ASSLSBs, particularly in mitigating interfacial degradation induced by large volume changes.
NETL
NSTL
Wiley