Multiscale Understanding of Anode-Electrolyte Interfaces Challenges in Sulfide-Based All-Solid-State Lithium-Metal...

Area of Science:

• Materials Science and Engineering
• Electrochemistry
• Battery Technology

Background:

• All-solid-state batteries (ASSBs) offer superior safety and energy density over liquid-electrolyte batteries.
• The lithium (Li) metal anode/solid-state electrolyte (SSE) interface is a major obstacle for ASSB performance.
• Interfacial issues include poor contact, instability, and mechanical degradation during battery cycling.

Purpose of the Study:

• To systematically review the multiscale interfacial challenges between Li metal anodes and sulfide SSEs in ASSBs.
• To elucidate the fundamental origins of these interfacial issues from atomic to macro scales.
• To summarize mitigation strategies for improving the Li/SSE interface.

Main Methods:

• Literature review focusing on sulfide electrolytes.
• Analysis of interfacial phenomena across atomic, mesoscale, and macroscale levels.
• Synthesis of current understanding and proposed solutions for Li/SSE interface engineering.

Main Results:

• Interfacial problems stem from atomic diffusion/reactions, mesoscale morphological changes, and macroscale electro-chemo-mechanical coupling.
• Sulfide electrolytes present unique challenges and opportunities for interface stabilization.
• Various strategies exist to address poor contact, chemical/electrochemical instability, and mechanical degradation.

Conclusions:

• Addressing multiscale interfacial issues is crucial for advancing ASSB technology.
• Rational design of the Li/SSE interface is key to unlocking the full potential of Li metal ASSBs.
• Further research is needed to integrate solutions across different scales for robust ASSB performance.