Geomag Mimetic Dynamically Reconfigurable POSS Framework Enables Antifatigue Solid Electrolyte Interphases for...

Area of Science:

• Materials Science
• Electrochemistry
• Nanotechnology

Background:

• Lithium metal anodes face limitations due to solid electrolyte interphase (SEI) fatigue and instability during plating/stripping.
• Developing stable SEIs is crucial for next-generation high-energy-density batteries.

Purpose of the Study:

• To design and demonstrate a novel stress-adaptive molecular interphase for lithium metal anodes.
• To improve the mechanical robustness and ion transport properties of the SEI.

Main Methods:

• Constructed an interphase using polyhedral oligomeric silsesquioxane (POSS) nanocages and reversible hydrogen bonds.
• Utilized a modular, "Geomag"-like architecture for autonomous reconfigurability.
• Investigated stress-triggered disconnect-reconnect behavior of the interphase.

Main Results:

• The interphase effectively dissipates local strain and homogenizes ion flux.
• Demonstrated suppression of dendrite nucleation and enhanced interfacial stability.
• Achieved ultralong cycling (>2000 h) in Li || LTO cells and stable performance in pouch cells.

Conclusions:

• The stress-adaptive molecular interphase offers a new paradigm for durable lithium metal batteries.
• Autonomous self-regulation of SEIs is key to overcoming lithium metal anode limitations.
• This approach paves the way for more stable and long-lasting energy storage devices.