Multilayer Sulfide-Electrolyte Engineering Stabilizes Interfaces for Long-Cycling, Wide-Temperature Lithium-Organic...

Area of Science:

• Materials Science
• Electrochemistry
• Energy Storage

Background:

• Interfacial instability is a major challenge in sulfide electrolyte-based all-solid-state lithium-organic batteries (ASSLOBs).
• Previous research focused on chemical compatibility, largely ignoring the impact of mechanical stress on interfacial degradation.

Purpose of the Study:

• To investigate the role of mechanical stress in interfacial degradation in ASSLOBs.
• To develop a novel electrolyte architecture that mitigates stress accumulation and enhances interfacial stability.

Main Methods:

• Utilized dibenzo[b,i]thianthrene-5,7,12,14-tetraone (DTT) as a conductive organic cathode.
• Employed a Li6PS5Cl-Li10GeP2S12-Li6PS5Cl trilayer electrolyte with a lithium metal anode.
• Conducted linear sweep voltammetry (LSV), operando pressure monitoring, and in situ electrochemical impedance spectroscopy with distribution of relaxation times (EIS-DRT).
• Performed cross-sectional backscattered scanning electron microscopy (BSEM) and energy-dispersive X-ray spectroscopy (EDS) for structural analysis.

Main Results:

• The trilayer electrolyte design effectively reduced stress accumulation and suppressed interfacial degradation.
• Demonstrated superior structural integrity of the battery components.
• Achieved a high capacity of 296 mAh g⁻¹ (at 0.1C) with remarkable long-term stability (90.2% retention after 4800 cycles at 2C, 60°C).
• Exhibited excellent low-temperature and high-loading performance.

Conclusions:

• Electrolyte architecture engineering is a versatile strategy for developing high-rate, durable, and temperature-resilient solid-state batteries.
• The reported ASSLOB demonstrates state-of-the-art performance for lithium anode-based systems.
• This work paves the way for more robust and efficient solid-state battery technologies.