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Dense inorganic electrolyte particles as a lever to promote composite electrolyte conductivity

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Abstract

Solid-state batteries are seen as key to the development of safer and higher-energy-density batteries, by limiting flammability and enabling the use of the lithium metal anode, respectively. Composite polymer–ceramic electrolytes are a possible solution for their realization, by benefiting from the combined mechanical properties of the polymer electrolyte and the thermal stability and high conductivity of the ceramic electrolyte. In this study we used different liquid electrolyte chemistries as models for the polymer electrolytes, and evaluated the effect of adding a variety of porous and dense ceramic electrolytes on the conductivity. All the results could be modelled with the effective medium theory, allowing prediction of the conductivity of electrolyte combinations. We unambiguously determined that highly conductive porous particles act as insulators in such systems, whereas dense particles act as conductors, thereby advancing our understanding of composite electrolyte conductivity.

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Fig. 1: Possible factors that can affect the effective conductivity of composite electrolytes.
Fig. 2: Conductivity of composites with porous particles.
Fig. 3: Effective conductivity of porous particles.
Fig. 4: Modelling the conductivity of aggregated CE particles as non-conducting.
Fig. 5: Conductivity of composites containing dense particles.

Data availability

The data that support the findings of this study are available from the corresponding author upon reasonable request.

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Acknowledgements

We thank B. Simon from the company SAFT for the mercury porosimetry measurements. The Agence de la Transition Ecologique (ADEME) is acknowledged for funding through the project IDOLES (grant no. 1982C0016).

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Contributions

R.B. designed the study. J.A.I. collected the experimental data. Data analysis and interpretation were performed by J.A.I. with the help of R.B. and D.D. The manuscript was written by J.A.I., R.B. and D.D. All authors have approved the final version of the manuscript.

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Correspondence to Renaud Bouchet.

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Supplementary Figs. 1–8, Tables 1 and 2, description of the microstructures of CE powders and experimental procedure for measuring the conductivity of LATP.

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Isaac, J.A., Devaux, D. & Bouchet, R. Dense inorganic electrolyte particles as a lever to promote composite electrolyte conductivity. Nat. Mater. (2022). https://doi.org/10.1038/s41563-022-01343-w

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