Chirality-Induced Suppression of Singlet Oxygen in Lithium-Oxygen Batteries with Extended Cycle Life.

ABSTRACT: Lithium-oxygen (Li-O2) batteries are perceived as a promising breakthrough in sustainable electrochemical energy storage, utilizing ambient air as an energy source, eliminating the need for costly cathode materials, and offering the highest theoretical energy density (~ 3.5 kWh kg-1) among discussed candidates. Contributing to the poor cycle life of currently reported Li-O2 cells is singlet oxygen (1O2) formation, inducing parasitic reactions, degrading key components, and severely deteriorating cell performance. Here, we harness the chirality-induced spin selectivity effect of chiral cobalt oxide nanosheets (Co3O4 NSs) as cathode materials to suppress 1O2 in Li-O2 batteries for the first time. Operando photoluminescence spectroscopy reveals a 3.7-fold and 3.23-fold reduction in 1O2 during discharge and charge, respectively, compared to conventional carbon paper-based cells, consistent with differential electrochemical mass spectrometry results, which indicate a near-theoretical charge-to-O2 ratio (2.04 e-/O2). Density functional theory calculations demonstrate that chirality induces a peak shift near the Fermi level, enhancing Co 3d-O 2p hybridization, stabilizing reaction intermediates, and lowering activation barriers for Li2O2 formation and decomposition. These findings establish a new strategy for improving the stability and energy efficiency of sustainable Li-O2 batteries, abridging the current gap to commercialization.

SUBMITTER: Chae K 

PROVIDER: S-EPMC12378250 | biostudies-literature | 2025 Aug

REPOSITORIES: biostudies-literature