DOI: 10.1073/pnas.2628659123 ISSN: 0027-8424

Capture and reduction of singlet oxygen via an anthracene-based framework for stable Li-O 2 batteries

Zhuoliang Jiang, Zhao Zhao, Liang Gao, Yifei Ma, Ke Liu, Jiaxuan An, Yaohui Huang, Zikang Chen, Xinlong Tian, Fujun Li

Given the increasing global energy demand and rapid advancement of low-carbon technologies, Li-O 2 batteries have attracted considerable attention owing to their exceptionally high theoretical energy density, offering great promise for advanced energy systems. However, the formation of harmful singlet oxygen ( 1 O 2 ) in both discharge and charge processes induces parasitic reactions that deteriorate round-trip efficiency and cycling stability. Herein, an anthracene-based covalent-organic framework (AntCOF) is introduced as a highly effective catalyst for the 1 O 2 reduction reaction (SORR) in Li-O 2 batteries. The conjugated porous framework selectively captures electrophilic 1 O 2 , enabling effective charge transfer from AntCOF to the empty π* orbital of 1 O 2 and promoting SORR in subsequent discharge processes. This mechanism suppresses 1 O 2 diffusion and mitigates associated side reactions, leading to reduced overpotentials and improved cycling performance when coupled with a RuO 2 catalyst. This work may enlighten further investigations into 1 O 2 -related chemistry across a broad range of oxygen-redox electrochemical systems.

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