Geometric Deformation of Single-Active Sites Enhances Intermediate Adsorption-Activation-Coupling for Stable Lithium-Oxygen Batteries

Single-dispersed active sites show great promise for lithium-oxygen batteries (LOBs) due to their unique chemical environments and high utilization rates. However, the inherent limitations of surface orbital steric effects and internal electronic coupling yield a detrimental impact on the stability of the active center, particularly during multipathway transformations and electronic recombination evolution of reaction intermediates. In this work, we introduce a curvature-triggered geometric deformation engineering to enhance the dynamic evolution of adsorption and activation processes for intermediates. By optimizing the dynamic geometric deformation of planar molecules through reasonable substrate strain, the deposition and decomposition kinetics of discharge products via dual growth pathways were facilitated, enabling the development of a highly stable LOBs with an impressive cycle life exceeding 1800 hours. Our research uncovers the multi-dimensional correlations among orbital rehybridization, the depth of electronic structure recombination, and the LiO 2 intermediate adsorption energy landscape under spatial confinement effects, providing valuable insights for their future design and activity promotion.