Ultralow Overpotential in Rechargeable Li–CO2 Batteries Enabled by Caesium Phosphomolybdate as an Effective Redox Catalyst
Abstract 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 b...
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Wiley
2025-07-01
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| Series: | Advanced Science |
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| Online Access: | https://doi.org/10.1002/advs.202502553 |
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| author | Mahsa Masoudi Neubi F. Xavier Jr James Wright Thomas M Roseveare Steven Hinder Vlad Stolojan Qiong Cai Robert C. T. Slade Daniel Commandeur Siddharth Gadkari |
| author_facet | Mahsa Masoudi Neubi F. Xavier Jr James Wright Thomas M Roseveare Steven Hinder Vlad Stolojan Qiong Cai Robert C. T. Slade Daniel Commandeur Siddharth Gadkari |
| author_sort | Mahsa Masoudi |
| collection | DOAJ |
| description | Abstract 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. |
| format | Article |
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| institution | Kabale University |
| issn | 2198-3844 |
| language | English |
| publishDate | 2025-07-01 |
| publisher | Wiley |
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| series | Advanced Science |
| spelling | doaj-art-21a8ae7fe72b49d0ba607a415eb906a22025-08-20T03:30:37ZengWileyAdvanced Science2198-38442025-07-011227n/an/a10.1002/advs.202502553Ultralow Overpotential in Rechargeable Li–CO2 Batteries Enabled by Caesium Phosphomolybdate as an Effective Redox CatalystMahsa Masoudi0Neubi F. Xavier Jr1James Wright2Thomas M Roseveare3Steven Hinder4Vlad Stolojan5Qiong Cai6Robert C. T. Slade7Daniel Commandeur8Siddharth Gadkari9School of Chemistry and Chemical Engineering Faculty of Engineering and Physical Sciences University of Surrey Guildford GU2 7XH UKSchool of Chemistry and Chemical Engineering Faculty of Engineering and Physical Sciences University of Surrey Guildford GU2 7XH UKSchool of Chemistry and Chemical Engineering Faculty of Engineering and Physical Sciences University of Surrey Guildford GU2 7XH UKDepartment of Chemistry University of Sheffield Brook Hill Sheffield S3 7HF UKSchool of Mechanical Engineering Sciences Faculty of Engineering and Physical Sciences University of Surrey Guildford GU2 7XH UKAdvanced Technology Institute School of Computer Science and Electronic Engineering Faculty of Engineering and Physical Sciences University of Surrey Guildford GU2 7XH UKSchool of Chemistry and Chemical Engineering Faculty of Engineering and Physical Sciences University of Surrey Guildford GU2 7XH UKSchool of Chemistry and Chemical Engineering Faculty of Engineering and Physical Sciences University of Surrey Guildford GU2 7XH UKSchool of Chemistry and Chemical Engineering Faculty of Engineering and Physical Sciences University of Surrey Guildford GU2 7XH UKSchool of Chemistry and Chemical Engineering Faculty of Engineering and Physical Sciences University of Surrey Guildford GU2 7XH UKAbstract 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.https://doi.org/10.1002/advs.202502553caesium phosphomolybdateelectrocatalystslithium‒CO2 batteriespolyoxometalatesstabilityultralow overpotential |
| spellingShingle | Mahsa Masoudi Neubi F. Xavier Jr James Wright Thomas M Roseveare Steven Hinder Vlad Stolojan Qiong Cai Robert C. T. Slade Daniel Commandeur Siddharth Gadkari Ultralow Overpotential in Rechargeable Li–CO2 Batteries Enabled by Caesium Phosphomolybdate as an Effective Redox Catalyst Advanced Science caesium phosphomolybdate electrocatalysts lithium‒CO2 batteries polyoxometalates stability ultralow overpotential |
| title | Ultralow Overpotential in Rechargeable Li–CO2 Batteries Enabled by Caesium Phosphomolybdate as an Effective Redox Catalyst |
| title_full | Ultralow Overpotential in Rechargeable Li–CO2 Batteries Enabled by Caesium Phosphomolybdate as an Effective Redox Catalyst |
| title_fullStr | Ultralow Overpotential in Rechargeable Li–CO2 Batteries Enabled by Caesium Phosphomolybdate as an Effective Redox Catalyst |
| title_full_unstemmed | Ultralow Overpotential in Rechargeable Li–CO2 Batteries Enabled by Caesium Phosphomolybdate as an Effective Redox Catalyst |
| title_short | Ultralow Overpotential in Rechargeable Li–CO2 Batteries Enabled by Caesium Phosphomolybdate as an Effective Redox Catalyst |
| title_sort | ultralow overpotential in rechargeable li co2 batteries enabled by caesium phosphomolybdate as an effective redox catalyst |
| topic | caesium phosphomolybdate electrocatalysts lithium‒CO2 batteries polyoxometalates stability ultralow overpotential |
| url | https://doi.org/10.1002/advs.202502553 |
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