Boosting a practical lithium carbon dioxide battery through a decoupled electrolyte

Fangli Zhang, Jodie A. Yuwono, Ruizhi Zhang, Lars Thomsen, Shuixin Xia, Wenchao Zhang (), Liyuan Chai and Zaiping Guo ()
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Fangli Zhang: The University of Adelaide, School of Chemical Engineering and Advanced Materials
Jodie A. Yuwono: The University of Adelaide, School of Chemical Engineering and Advanced Materials
Ruizhi Zhang: The University of Adelaide, School of Chemical Engineering and Advanced Materials
Lars Thomsen: Australian Nuclear Science and Technology Organization, Australian Synchrotron
Shuixin Xia: The University of Adelaide, School of Chemical Engineering and Advanced Materials
Wenchao Zhang: Central South University, School of Metallurgy and Environment
Liyuan Chai: Central South University, School of Metallurgy and Environment
Zaiping Guo: The University of Adelaide, School of Chemical Engineering and Advanced Materials

Nature Communications, 2025, vol. 16, issue 1, 1-12

Abstract: Abstract Highly conductive electrolytes and stable electrolyte|electrode interfaces are desired for next-generation batteries. Constructing solid-electrolyte interphases on electrodes is a prevailing strategy for enhancing interfacial stability but fails to prevent inevitable breakdown and reformation of interphases during prolonged cycling. Herein, a decoupled electrolyte is designed by introducing a co-solvent (tetraethylene glycol dimethyl ether) with high stability and high positive electrostatic potential values into highly conductive dimethylformamide-based electrolytes, which suffer from electrolyte|positive electrode instability. The preferential adsorption of cations solvated with co-solvents on the positive electrode during discharge induces the formation of a co-solvent-rich localized environment, inhibiting side reactions and contributing to long cyclability. Meanwhile, dimethylformamide in the bulk electrolyte helps to maintain high ionic conductivity, thus improving kinetics. Notably, lithium-carbon dioxide cells with this decoupled electrolyte demonstrate a significantly improved cycle life of ~ 2600 hours and a low overpotential of ~ 1 V, even with a metal-free commercial reduced graphene oxide catalyst. Our work provides an alternative strategy to solid-electrolyte interphase construction for stabilizing electrolyte|electrode interface and unlocks the potential of previously underexplored solvents in batteries.

Date: 2025
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DOI: 10.1038/s41467-025-64369-z

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