Abstract
Aqueous Zn metal batteries offer a safe, low-cost route to grid-scale energy storage yet suffer from dendrite growth and corrosion issues. Conventional electrolyte designs largely overlook electric-field-driven interfacial dynamics such as solvation structure evolution and component redistribution during operation. Here, we propose an affinitive additive strategy featuring high donor number and dipole moment, exemplified by N,N-dimethylurea (DMU), to dynamically modulate Zn2+ solvation and the structure of the electric double layer under operational electric fields. Guided by physically grounded molecular descriptors, we identify additives capable of electric-field-induced interfacial enrichment, during which strong dipole-field coupling promotes their incorporation into the Zn2+ solvation shell and promotes more uniform Zn deposition. As a result, the optimized electrolyte achieves a coulombic efficiency of ~99.9% for Zn plating/stripping with only 2 wt% additive. It also sustains stable operation for 700 h at 60% depth of discharge, outperforming the baseline electrolyte. Descriptor-guided screening further reveals that other candidates follow the same pattern, suggesting broader applicability of this approach. Practical Zn | |ZnI2 full cells with high areal capacity (~3 mAh cm-2) and low N/P ratio (~1.8) achieve 750 stable cycles at 0.15 A g−1 with 84.5% capacity retention.
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Source data are provided with this paper. All computational data files related to descriptor selection, theoretical calculations and simulations have been deposited in “MaterialsCloud” under accession code DOI link59. Source data are provided with this paper.
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The code for machine learning in this work has been deposited in “MaterialsCloud” under accession code DOI link59.
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Acknowledgements
B.Z. acknowledges the financial support from the National Natural Science Foundation of China (no. 22509023) and the Sichuan Science and Technology Program (no. 2025ZNSFSC0964). W.S. acknowledges the National Natural Science Foundation of China (nos. U2330119 and 52302221). H.Z.W. acknowledges the support from the National Natural Science Foundation of China (no. 52272198). The authors also acknowledge the support of computational resources provided by the High-performance Computing Platform of UESTC.
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W.S., H.Z.W., H.W., B.Z., and M.Y. conceived the idea and designed the experiments. M.Y. and B.Z. performed materials characterizations and electrochemical measurements with assistance from A.D., S.L., L.Y.G., J.Q.W., Y.X.Z., Y.F., X.H., Y.Y.T., and J.Y. B.Z. performed the MD simulations, DFT calculations, and machine-learning analyses. M.Y. and B.Z. co-wrote the paper. All authors discussed the results and commented on the manuscript.
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The authors declare that a patent application related to the electrolyte formulation described in this work has been filed (patent no. 2025108426814).
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Yang, M., Zhang, B., Duan, A. et al. Electric-field-reinforced affinitive electrolytes for highly reversible aqueous zinc metal batteries. Nat Commun (2026). https://doi.org/10.1038/s41467-026-70366-7
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DOI: https://doi.org/10.1038/s41467-026-70366-7
