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Solid-state lithium oxygen batteries (LOBs) are known for their enhanced safety, higher electrochemical stability, and improved energy density compared to liquid-state LOBs. However, the investigation of solid-state LOBs is limited with little understanding of their discharge and charge processes. In this work, a polymer-based solid-state LOB is used to investigate the effect of discharge rate on lithium peroxide (Li2O2) formation, the oxygen evolution reaction (OER), and cycle performance. Notably, we observe a counterintuitive trend: Li2O2 particle size increases with increasing discharge current density, in contrast to liquid systems. This behavior arises from inherent space charge layers that restrict Li⁺ transport under high current, and spatially heterogeneous active sites at the solid electrolyte–cathode interface, directly evidenced by small angle X-ray scattering (SAXS), which govern nucleation accessibility and promote site-selective Li2O2 growth. Furthermore, higher current densities improve ORR and OER efficiency but accelerate anode degradation, while lower currents promote side reactions. These opposing effects result in a trade-off that defines an optimal discharge rate (0.1 mA cm⁻2) for maximizing cycle life. This study provides a new mechanistic perspective on discharge-driven processes in solid-state LOBs and offers practical guidelines for performance optimization in future high-energy battery systems.

Rights:

• Creative Commons BY-NC-ND Attribution-NonCommercial-NoDerivs 4.0 International
  

Keyword: Solid-State Li-O2 Batteries

Date published: 2025-09-08

Publisher: Wiley

Journal:

• Angewandte Chemie International Edition (ISSN: 14337851) vol. 64 issue. 37 e202507967

Funding:

• U.S. Department of Energy
• Vehicle Technologies Office DE‐AC02‐06CH11357
• Argonne National Laboratory DE‐AC02‐06CH11357

Manuscript type: Publisher's version (Version of record)

MDR DOI:

First published URL: https://doi.org/10.1002/anie.202507967

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Updated at: 2025-09-24 12:30:27 +0900

Published on MDR: 2025-09-24 12:18:52 +0900