Dual-Site Geometry Mediates Dynamic LiO₂ Binding for Efficient Lithium-Oxygen Batteries

Area of Science:

• Materials Science
• Electrochemistry
• Catalysis

Background:

• Lithium-oxygen batteries (LOBs) promise high energy density but suffer from unstable intermediates like lithium superoxide (LiO2) due to complex reaction kinetics.
• Poor reversibility and limited cycling stability hinder the practical application of LOBs.

Purpose of the Study:

• To propose an electronegativity-mediated strategy for dynamically regulating LiO2 binding on catalyst surfaces.
• To enhance the performance of lithium-oxygen batteries through atomic-scale catalyst design.

Main Methods:

• Tuning the geometry and spacing of dual-active sites (DAS) to reshape orbital interactions and control electron density.
• Establishing an atomic-scale regulation to create a
• bridged adsorption
• mode for intermediates.
• Investigating the impact of DAS spacing on oxygen electrocatalysis and overcoming linear scaling relationships (LSRs).

Main Results:

• The proposed strategy dynamically regulates LiO2 binding, stabilizing key intermediates and optimizing the Li-O bond activation.
• Lithium-oxygen batteries demonstrated high capacity and significantly prolonged cycling stability.
• A universal DAS spacing descriptor was identified, integrating symmetry breaking and electronic configuration.

Conclusions:

• Electronegativity-mediated regulation of dual-active sites provides a general design principle for advanced oxygen electrocatalysis.
• This approach overcomes limitations imposed by linear scaling relationships, unlocking intrinsic catalytic activity.
• The findings pave the way for designing highly efficient and stable lithium-oxygen batteries.