Reactive Oxygen Species Resistive Redox Mediator in Lithium-Oxygen Batteries

Abstract

The utilization of redox mediators (RMs) in lithium-oxygen batteries (LOBs) has underscored their utility in high overpotential during the charging process. Among the currently known RMs, it is exceptionally challenging to identify those with a redox potential capable of attenuating singlet oxygen (1O2) generation while resisting degradation by reactive oxygen species (ROS), such as 1O2 and superoxide (O2 center dot-). In this context, computational and experimental approaches for rational molecular design have led to the development of 7,7 '-bi-7-azabicyclo[2.2.1]heptane (BAC), a newly suggested RM incorporating N-N interconnected aza-bicycles. BAC harnesses the advantages of falling within the potential range that suppresses 1O2 generation, as previously reported N-N embedded non-bicyclic RMs, and effectively defends against ROS-induced degradation due to the incorporation of a novel bicyclic moiety. Unlike the non-bicyclic RMs, which exhibit reduced O2 evolution after exposure to 1O2, BAC maintains consistent O2 profiles during charging, indicating its superior 1O2 resistance and steady redox-catalyst performance in LOBs. This study introduces a precise and rational design strategy for low-molecular-weight RMs, marking a significant step forward in advancing LOB development by improving efficiency, stability, and practical applicability.

Publisher

Wiley

Publication Date

4-16-2025

Publication Title

Advanced Materials

Department

Chemistry and Biochemistry

Document Type

Article

DOI

https://doi.org/10.1002/adma.202570119

Keywords

Lithium-oxygen batteries, Reactive oxygen species, Redox mediator, Singlet oxygen, Superoxide

Language

English

Format

text

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