Abstract
Aqueous zinc batteries (AZBs) are promising for sustainable energy storage due to their safety and affordability. Conventional ‘lean-water’ electrolytes improve cell cyclability and the electrochemical stability window by stabilizing the interface; however, ionic transport in the bulk is limited and the use of high-concentration salt jeopardizes their practical adaptability. Here we report a dual-salt electrolyte involving ZnSO4 and Zn(ClO4)2 that decouples the interfacial chemistry from the bulk. Specifically, SO42− ions populate the Zn/electrolyte interface, whereas ClO4− anions dominate in the bulk. Strongly hydrated SO42− stabilizes interfacial water, while weakly hydrated ClO4− disrupts bulk hydrogen-bond networks, suppressing electrolyte freezing and enabling fast Zn2+ transport. In the absence of high salt concentrations and organic solvents, our decoupled electrolyte achieves a high ionic conductivity of 15.1 mS cm⁻1 and Zn plating/stripping reversibility of 99.97% at −40 °C. Assembled Zn//NaV3O8 pouch cells under practical configurations show a daily self-discharge rate of 0.13%, retain 93% capacity after 900 cycles at 25 °C, and deliver full capacity retention over 3,000 cycles at −40 °C. This decoupled dual-salt electrolyte advances the practical deployment of AZBs and offers a strategy for rational and sustainable electrolyte design beyond aqueous systems.
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All data are available in the main text or the Supplementary Information, which can also be available from the corresponding author upon request. Source data are provided with this paper and are also available in figshare at https://doi.org/10.6084/m9.figshare.29941601 (ref. 65).
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Acknowledgements
This work was supported by the Australian Research Council (FL210100050 Z.G. and DE240100159 S.Z.). G.L. was supported by scholarships from the China Scholarship Council (grant no. 202006750014 to G.L.). J.A.Y. acknowledges the high-performance computing facilities provided by National Computational Infrastructure (NCI) Australia. Components of this research were undertaken on the powder diffraction and SAXS/wide-angle X-ray scattering beamlines at the Australian Synchrotron, part of ANSTO, through the merit-based beamtime proposals (M21781 to S.Z., M21924 to G.L.). We thank Q. Gu for invaluable support and expertise in our powder diffraction experiments; K. Davey for valuable insights and contributions to this work, and we remember him with deep gratitude; C. Wang for providing valuable guidance on the conceptual development of this paper; C. Zhang for valuable assistance with the QCM measurements; and T. Lu for support with the Kelvin probe force microscopy measurements.
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G.L., S.Z. and Z.G. conceived the research idea. G.L. and S.Z. designed the experiments. G.L., Q.C. and L.M. performed electrochemical measurements and material characterizations. J.A.Y. conducted the theoretical calculations. All authors discussed the results and contributed to the data analysis. G.L. and S.Z. wrote the paper with contributions from all authors. H.J. and Z.G. assisted in revising the paper. S.Z. and Z.G. supervised the work.
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Li, G., Cai, Q., Zhang, S. et al. Decoupled dual-salt electrolyte for practical aqueous zinc batteries. Nat Sustain (2025). https://doi.org/10.1038/s41893-025-01646-1
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DOI: https://doi.org/10.1038/s41893-025-01646-1