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<p>Highly conductive electrolytes and stable electrolyte|electrodeinterfaces are desired for next-generation batteries. Constructing solid-electrolyteinterphases on electrodes is a prevailing strategy for enhancing interfacialstability but fails to prevent inevitable breakdown and reformation of interphasesduring prolonged cycling. Herein, a decoupled electrolyte is designed by introducinga co-solvent (tetraethylene glycol dimethyl ether) with high stability and highpositive electrostatic potential values into highly conductivedimethylformamide-based electrolytes, which suffer from electrolyte|positiveelectrode instability. The preferential adsorption of cations solvated withco-solvents on the positive electrode during discharge induces the formation of aco-solvent-rich localized environment, inhibiting side reactions and contributing tolong cyclability. Meanwhile, dimethylformamide in the bulk electrolyte helps tomaintain high ionic conductivity, thus improving kinetics. Notably, lithium-carbondioxide cells with this decoupled electrolyte demonstrate a significantly improvedcycle life of ~ 2600 hours and a low overpotential of ~ 1 V, even with a metal-freecommercial reduced graphene oxide catalyst. Our work provides an alternativestrategy to solid-electrolyte interphase construction for stabilizingelectrolyte|electrode interface and unlocks the potential of previouslyunderexplored solvents in batteries.</p>

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Boosting a practical lithium carbon dioxide battery through a decoupled electrolyte

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年10月21日

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  • Fangli Zhang,
  • Jodie A. Yuwono,
  • Ruizhi Zhang,
  • Lars Thomsen,
  • Shuixin Xia,
  • Wenchao Zhang,
  • Liyuan Chai,
  • Zaiping Guo

摘要

Highly conductive electrolytes and stable electrolyte|electrodeinterfaces are desired for next-generation batteries. Constructing solid-electrolyteinterphases on electrodes is a prevailing strategy for enhancing interfacialstability but fails to prevent inevitable breakdown and reformation of interphasesduring prolonged cycling. Herein, a decoupled electrolyte is designed by introducinga co-solvent (tetraethylene glycol dimethyl ether) with high stability and highpositive electrostatic potential values into highly conductivedimethylformamide-based electrolytes, which suffer from electrolyte|positiveelectrode instability. The preferential adsorption of cations solvated withco-solvents on the positive electrode during discharge induces the formation of aco-solvent-rich localized environment, inhibiting side reactions and contributing tolong cyclability. Meanwhile, dimethylformamide in the bulk electrolyte helps tomaintain high ionic conductivity, thus improving kinetics. Notably, lithium-carbondioxide cells with this decoupled electrolyte demonstrate a significantly improvedcycle life of ~ 2600 hours and a low overpotential of ~ 1 V, even with a metal-freecommercial reduced graphene oxide catalyst. Our work provides an alternativestrategy to solid-electrolyte interphase construction for stabilizingelectrolyte|electrode interface and unlocks the potential of previouslyunderexplored solvents in batteries.