Rechargeable lithium-CO2 batteries are emerging as attractive energy storage devices due to their potential for high capacity and efficient CO2 reduction, making them promising candidates for post-lithium-ion batteries with high energy densities. However, their practical applications have been restricted by low reversibility, poor cycle life, and sluggish redox kinetics induced by the high potential required for decomposing the discharge product Li2CO3. Despite the various cathode catalysts explored, their application is often limited by availability, high cost, and complexity of synthesis. Herein, caesium phosphomolybdate (CPM) is synthesized through a facile and low-cost method. The Li‒CO2 battery based on the CPM cathode demonstrates a high discharge capacity of 15,440 mAh g-1 at 50 mA g-1 with 97.3% coulombic efficiency. It further exhibits robust stability, operating effectively over 100 cycles at 50 mA g-1 with a capacity limitation of 500 mAh g-1. Remarkably, the CPM catalyst yields a low overpotential of 0.67 V, surpassing most catalysts reported in prior research. This study reports, for the first time, the application of a Keggin-type polyoxometalate as a bifunctional redox catalyst, significantly improving the reversible cycling of rechargeable Li–CO2 batteries.
- Ultralow Overpotential in Rechargeable Li–CO2 Batteries Enabled by Caesium Phosphomolybdate as an Effective Redox Catalyst
- Mahsa Masoudi - University of Surrey, Mechanical Engineering SciencesNeubi F. Xavier Jr. (Author) - University of Surrey, School of Chemistry & Chemical EngineeringJames Wright (Author) - University of Surrey, School of Chemistry & Chemical EngineeringThomas M. Roseveare (Author) - University of SheffieldSteven Hinder (Author) - University of Surrey, Mechanical Engineering SciencesVlad Stolojan (Author) - University of Surrey, School of Computer Science & Electronic EngineeringQiong Cai (Author) - University of Surrey, School of Chemistry & Chemical EngineeringRobert C. T. Slade (Author) - University of SurreyDaniel Commandeur (Corresponding Author) - University of Surrey, School of Chemistry & Chemical EngineeringSiddharth Gadkari (Corresponding Author) - University of Surrey, School of Chemistry & Chemical Engineering
- Advanced Science, Vol.12(27), 2502553
- Wiley
- 14
- 30/04/2025
- 17/07/2025
- 21/04/2025
- University of Surrey (United Kingdom, Guildford)
- The authors would like to thank the University of Surrey for providing financial support through the Breaking Barrier Award. The authors also sincerely appreciate Dr. Ian Riddlestone for his valuable contribution to this work.
- 99989866502346; WOS:001479470400001
- © 2025 The Author(s). Advanced Science published by Wiley-VCH GmbH. This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.
- School of Chemistry & Chemical Engineering; Mechanical Engineering Sciences; School of Computer Science & Electronic Engineering
- English
- Journal article
- The data that supports the findings of this study can be shared by corresponding authors upon request.