Taming Interfacial Ion-Dipole Interactions With d-Orbital Delocalized Electron Catalysis Expediates Low-Temperature...

Area of Science:

• Materials Science
• Electrochemistry
• Energy Storage

Background:

• Low-temperature lithium metal batteries (LT-LMBs) offer high energy density but face challenges like electrolyte solidification and lithium dendrite formation.
• Strong ion-dipole interactions in larger solvation shells hinder Li+ kinetics at low temperatures.

Purpose of the Study:

• To develop a catalytic strategy for accelerating Li+ dissociation and improving LT-LMB performance.
• To overcome the limitations of organic electrolyte solidification and dendrite growth in LT-LMBs.

Main Methods:

• Systematic screening of d-orbital metal oxides (Ti, V, Fe, Co) with oxygen defect modulation for interfacial catalysis.
• Electrochemical and theoretical experiments to investigate the catalytic effect on ion-dipole interactions.
• Fabrication and testing of Li-S and Li-metal oxide full cells under various low-temperature conditions.

Main Results:

• Optimized titanium oxide demonstrated effective interfacial catalysis, breaking ion-dipole interactions and accelerating Li+ dissociation.
• The modified Li electrodes exhibited robustness from 25°C to -50°C, with stable cycling for 1800 hours and high Coulombic efficiency at -20°C.
• Li-S full cells maintained 88% capacity retention over 200 cycles, and high-loading Li-metal oxide cells showed ≈100% retention at 0°C.

Conclusions:

• Interfacial catalysis using electron-delocalized d-orbital metal oxides is a viable strategy for advancing LT-LMBs.
• The developed catalytic approach enhances Li kinetics and suppresses dendrite formation, enabling reliable battery operation at low temperatures.
• This work provides a new guideline for designing high-performance LT-LMBs through catalytic interface engineering.