Designing a stable solid–electrolyte interphase on a Li anode is imperative to developing reliable Li metal batteries. Herein, we report a suspension electrolyte design that modifies the Li+ solvation environment in liquid electrolytes and creates inorganic-rich solid–electrolyte interphases on Li. Li2O nanoparticles suspended in liquid electrolytes were investigated as a proof of concept. Through theoretical and empirical analyses of Li2O suspension electrolytes, the roles played by Li2O in the liquid electrolyte and solid–electrolyte interphases of the Li anode are elucidated. Also, the suspension electrolyte design is applied in conventional and state-of-the-art high-performance electrolytes to demonstrate its applicability. Based on electrochemical analyses, improved Coulombic efficiency (up to ~99.7%), reduced Li nucleation overpotential, stabilized Li interphases and prolonged cycle life of anode-free cells (~70 cycles at 80% of initial capacity) were achieved with the suspension electrolytes. We expect this design principle and our findings to be expanded into developing electrolytes and solid–electrolyte interphases for Li metal batteries.
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The authors declare that all the data and relevant information are available within the article and Supplementary Information. Additional data are available from the corresponding author upon reasonable request.
The MD and DFT simulation codes are available at https://github.com/prudnick94/LiSolvation_Li2OSuspension and https://github.com/exenGT/Li2O, respectively.
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We acknowledge support from the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the US Department of Energy under the Battery Materials Research Program and Battery 500 Consortium. Z.Z. acknowledges the support from the Stanford Interdisciplinary Graduate Fellowship. S.T.O. acknowledges support from the Knight Hennessy scholarship for graduate studies at Stanford University.
The authors declare no competing interests.
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Kim, M.S., Zhang, Z., Rudnicki, P.E. et al. Suspension electrolyte with modified Li+ solvation environment for lithium metal batteries. Nat. Mater. 21, 445–454 (2022). https://doi.org/10.1038/s41563-021-01172-3
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