Stress-homogenized spatial architectures via entropy-driven self-assembly enabling high-performance and durable...

Area of Science:

• Materials Science
• Electrochemistry
• Sustainable Energy

Background:

• Global transition to sustainable energy requires efficient lithium extraction from brines.
• Electrochemical lithium extraction using LiMn2O4 (LMO) is promising but limited by mechanical degradation due to volume changes and stress accumulation during cycling.

Purpose of the Study:

• To engineer stress-homogenized multilayer core-shell architectures for LMO to mitigate stress accumulation and enhance electrochemical stability.
• To optimize the internal geometric structure of LMO for improved stress-strain behavior, ion distribution, and transport kinetics.

Main Methods:

• Entropy-driven amphiphilic self-assembly strategy to create multilayer core-shell architectures.
• Hybrid capacitive deionization for lithium extraction.
• Finite element simulations to analyze stress evolution and ion diffusion.

Main Results:

• Achieved a lithium extraction capacity of 4.78 mmol g-1 with 96% retention over 100 cycles.
• Demonstrated synergistic enhancement in ion distribution, transport kinetics, and electrochemical stability.
• Finite element simulations showed a 48% reduction in maximum stress compared to disordered counterparts.

Conclusions:

• The hierarchical interlayer architecture effectively mitigates stress accumulation and preserves structural integrity during cycling.
• This approach provides a pathway for developing advanced, intrinsically stable materials for sustainable lithium extraction.
• Optimized LMO sets a dual benchmark for capacity and cycling stability in hybrid capacitive deionization.