Architected Low-Tortuosity Electrodes with Tunable Porosity from Nonequilibrium Soft-Matter Processing

Area of Science:

• Materials Science
• Electrochemistry
• Chemical Engineering

Background:

• Mass transport limitations hinder energy storage device performance, especially at high current rates.
• Optimizing energy and power density requires tailored electrode architectures and efficient diffusion pathways.

Purpose of the Study:

• To develop a material-agnostic fabrication process for advanced composite electrodes.
• To investigate the impact of tunable electrode architectures on electrochemical performance and stability.

Main Methods:

• A nonequilibrium soft-matter process was employed to create free-standing inorganic composite electrodes.
• Electrodes featured straight, accessible channels (5-30 µm diameter) and adjustable thicknesses (100s of µm).
• Tunable material-to-pore ratios and electrochemical cycling were utilized.

Main Results:

• Fabricated anode and cathode electrodes demonstrated electrochemical and architectural stability during extended cycling.
• Mass-transport limitations were observed at high current densities, with lithiation identified as rate-limiting due to ion supply issues.
• The study confirmed the feasibility of tunable electrode architectures for enhanced performance.

Conclusions:

• Tailored electrode architectures with optimized dimensional ratios are crucial for meeting coupled power and energy storage demands.
• The developed soft-matter process offers a versatile route to engineer electrodes for next-generation energy storage systems.