Abstract
Cation solvation is well understood in the bulk solution phase, but knowledge is limited regarding the electrode–electrolyte interface. The process by which cation solvation conforms to the interfacial field to form interphases remains unclear. Here we examine the synergistic effects of external and intramolecular fields on accommodating Li+ solvates to the Li-metal anode, leading to dielectric-mediated transfer dynamics on the interface. At charged interfaces, cation–anion pairs arrange in a periodic oscillatory distribution. A low-oscillation amplitude exacerbates the electrolyte decomposition and increases surface impedance. We propose a dielectric protocol that maintains cation–anion coordination with a high oscillation amplitude at the interfaces, addressing these issues. Accordingly, we demonstrate a Li-metal pouch cell with an energy density of 500 Wh kg−1 at the Ah level using an ultra-lean electrolyte (1 g Ah−1). Our study offers insights into solid/liquid interfaces that are crucial in advancing battery technologies.
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Acknowledgements
This work is supported by the Key R&D Program of Zhejiang (2023C01128), National Natural Science Foundation of China (22072134, 22161142017 and U21A2081), Natural Science Foundation of Zhejiang Province (LR23B030002 and LZ21B030002), the Fundamental Research Funds for the Central Universities (226-2024-00075) and ‘Hundred Talents Program’ of Zhejiang University. We acknowledge R. Huang from Vacuum Interconnected Nanotech Workstation (Nano-X), Suzhou Institute of Nano-Tech and Nano-Bionics for her assistance in ToF-SIMS characterization.
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S.Z., R.L. and X.F. conceived the idea and designed the experiments. S.Z. performed electrochemical measurements and the material characterizations. R.L. performed the theoretical calculations. S.Z., R.L., T.D. and X.F. analysed the results and revised the paper. R.Z., Hao Zhang, S.D. and Y.W. conducted the machine learning. Q.M. and X.H. performed the cycle test of 500 mAh pouch cell. R.G. and Y.L. carried out the electrochemical test of 6 Ah pouch cell. Y.S. helped the ToF-SIMS experiment. H. Zhu, M.L., Haikuo Zhang, D.L., B.M., L.L. and L.C. participated in the scientific discussion and data analysis. X.F. supervised all the studies.
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Nature Energy thanks Qiang Zhang and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.
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Zhang, S., Li, R., Deng, T. et al. Oscillatory solvation chemistry for a 500 Wh kg−1 Li-metal pouch cell. Nat Energy (2024). https://doi.org/10.1038/s41560-024-01621-8
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DOI: https://doi.org/10.1038/s41560-024-01621-8
