Π‐Conjugation Induced Anchoring of Ferrocene on Graphdiyne Enable Shuttle‐Free Redox Mediation in Lithium‐Oxygen Batteries. Issue 4 (25th November 2021)

• Record Type: Journal Article
• Authors: Li, Xudong; Han, Guokang; Qian, Zhengyi; Liu, Qingsong; Qiang, Zhuomin; Song, Yajie; Huo, Hua; Du, Chunyu; Lou, Shuaifeng; Yin, Geping
• Is Part Of: Advanced science. Volume 9:Issue 4(2022)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2021-11-25
• Subjects: electron interactions -- graphdiyne -- lithium‐oxygen batteries -- redox mediators -- shuttle phenomena; Science -- Periodicals; 505
• DOI: 10.1002/advs.202103964
• Languages: English
• ISSNs: 2198-3844

Abstract

Abstract: Soluble redox mediators (RMs), an alternative to conventional solid catalysts, have been considered an effective countermeasure to ameliorate sluggish kinetics in the cathode of a lithium–oxygen battery recently. Nevertheless, the high mobility of RMs leads to serious redox shuttling, which induces an undesired lithium‐metal degeneration and RM decomposition during trade‐off catalysis against the sustainable operation of batteries. Here, a novel carbon family of graphdiyne matrix is first proposed to decouple the charge‐carrying redox property of ferrocene and the shuttle effects. It is demonstrated that a ferrocene‐anchored graphdiyne framework can function as stationary RM, not only preserving the redox‐mediating capability of ferrocene, but also promoting the local orientated three‐dimensional (3D) growth of Li2 O2 . As a result, the RM‐assisted catalysis in lithium–oxygen battery remains of remarkable efficiency and stability without the depletion of oxidized RMs or lithium degradation, resulting in a significantly enhanced electrochemical performance. Abstract : Ferrocene‐anchored graphdiyne framework decouples the charge‐carrying redox property of ferrocene‐redox mediators and the shuttle effects, suppressing the consumption of oxidized ferrocene and degradation of the Li‐metal anode. Such ferrocene‐assisted catalysis results in a significantly enhanced electrochemical performance of LiO2 batteries.