Redox-Driven Lithium Perfusion to Fabricate Li@Ni-Foam Composites for High Lithium-Loading 3D Anodes

Area of Science:

• Materials Science
• Electrochemistry
• Surface Chemistry

Background:

• Conventional lithium metal anodes suffer from volume expansion and dendrite growth due to their hostless nature.
• Developing composite electrode structures is crucial for improving lithium plating/stripping and mitigating these issues.

Purpose of the Study:

• To fabricate a composite lithium anode (Li@NF) with enhanced lithium plating/stripping behaviors.
• To investigate the underlying mechanisms for improved performance and stability.

Main Methods:

• Fabrication of Li@NF anode via lithium perfusion into nickel foam decorated with NiO nanosheets.
• Density functional theory (DFT) calculations and control studies (Fe2O3@NF, pristine NF, Cu2O@CF).
• Ex situ scanning electron microscopy (SEM) and in situ optical microscopy.

Main Results:

• Achieved high areal lithium loading (53.2 mg cm⁻²).
• Demonstrated suppressed dendrite formation and volume expansion.
• Exhibited improved Coulombic efficiency and extended cycling stability in half, symmetric, and full cells.
• Revealed a redox-driven Li perfusion process correlated with surface reaction thermodynamics and lithiophilicity.

Conclusions:

• The conductive 3D scaffolds of Li@NF homogenize Li⁺ flux and accommodate multidirectional Li deposition, enhancing performance.
• The study provides insights into thermal Li perfusion for designing safe and stable lithium metal anodes.