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Fast single metal cation conduction in ion-water aggregated aqueous battery electrolytes

Author

Listed:
  • Chen Xu

    (Hunan University)

  • Huijian Wang

    (Hunan University)

  • Chengjun Lei

    (Hunan University)

  • Jinye Li

    (Hunan University)

  • Wenjiao Ma

    (Hunan University)

  • Xiao Liang

    (Hunan University
    Greater Bay Area Institute for Innovation, Hunan University)

Abstract

Metal ion transport in solution is closely linked to its interactions with counter anions and solvent molecules. This interplay creates a longstanding trade-off between transference number (tMn⁺), ionic conductivity (δ), and solvation process. Advanced aqueous batteries with metal negative electrode require electrolytes with unity tMn⁺, high δ and low solvation energy. Here we introduce guanidinium sulfate (Gdm2SO4) into metal sulfate aqueous solutions to construct the ion-water aggregated electrolytes. These electrolytes exhibit fast single ion conduction, approaching unity tMn⁺ and high δ over 50 mS cm−1 for various metal cations (M= Zn, Cu, Fe, Sn and Li). The ion-water aggregates, dynamically formed by strong hydrogen bonding between sulfate anions, guanidinium cations and water, featuring an unfrustrated topological structure to suppress both anion mobility and water activity. This general configuration decouples the metal charge carrier from its coordination sheath, resulting in decreased solvation energy. These merits lead to homogeneous metal plating/stripping behavior with high coulombic efficiency of 99.9%. Moreover, the ion-water aggregates with reinforced kosmotropic characteristics significantly decrease the freezing point of the sulfate-based electrolytes to –28 oC, making them widely applicable in aqueous metal batteries for both intercalation and conversion positive electrodes.

Suggested Citation

  • Chen Xu & Huijian Wang & Chengjun Lei & Jinye Li & Wenjiao Ma & Xiao Liang, 2025. "Fast single metal cation conduction in ion-water aggregated aqueous battery electrolytes," Nature Communications, Nature, vol. 16(1), pages 1-10, December.
  • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-59958-x
    DOI: 10.1038/s41467-025-59958-x
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    References listed on IDEAS

    as
    1. Qiu Zhang & Yilin Ma & Yong Lu & Lin Li & Fang Wan & Kai Zhang & Jun Chen, 2020. "Modulating electrolyte structure for ultralow temperature aqueous zinc batteries," Nature Communications, Nature, vol. 11(1), pages 1-10, December.
    2. Dejian Dong & Tairan Wang & Yue Sun & Jun Fan & Yi-Chun Lu, 2023. "Hydrotropic solubilization of zinc acetates for sustainable aqueous battery electrolytes," Nature Sustainability, Nature, vol. 6(11), pages 1474-1484, November.
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