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Amorphous and perovskite Li3xLa(2/3)−xTiO3 (thin) films via chemical solution deposition: solid electrolytes for all-solid-state Li-ion batteries

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Abstract

Thin films of amorphous and crystalline perovskite Li3xLa(2/3)−xTiO3 (LLT) (x = 0.117) are prepared by means of aqueous chemical solution deposition onto rutile TiO2 thin films as an anode, yielding an electrochemical half-cell. The Li-ion conductivity of the pin-hole free, amorphous LLT thin film (90 nm thick) is 3.8 × 10−8 S cm−1 on Pt and 1.3 × 10−8 S cm−1 on rutile TiO2, while measuring perpendicular to the thin film direction with impedance spectroscopy. Grazing angle attenuated total reflectance-Fourier transform infrared spectroscopy shows that all organic precursor molecules have been decomposed at 500 °C. In addition, in situ (heating) X-ray diffraction analysis shows that phase pure crystalline perovskite LLT (x = 0.117) is formed on top of the rutile TiO2 anode at 700 °C. Furthermore, thickness control is possible by varying the precursor solution concentration and the number of deposition cycles. The current study presents a promising synthesis route to develop all-solid-state battery devices based on multi-metal oxide materials using aqueous precursor chemistry.

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Acknowledgments

The authors acknowledge financial support by the IWT Flanders (SBO project SOSLion). Christopher De Dobbelaere is a Post-Doctoral Research Fellow of the Research Foundation Flanders (FWO-Vlaanderen). Tim Vangerven and Peter-Paul Harks are acknowledged for preparing and starting up the impedance spectroscopy measurements. Thanks to Elsy Thijssen for performing the ICP-AES measurements and Hanne Damm for the thermal analysis. Special thanks to Bart Ruttens for all the work regarding SEM and XRD samples.

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Authors and Affiliations

  1. Institute for Materials Research; Inorganic and Physical Chemistry and IMEC, Division IMOMEC, Hasselt University, Martelarenlaan 42, 3500, Hasselt, Belgium

    E. J. van den Ham, N. Peys, C. De Dobbelaere, A. Hardy & M. K. Van Bael

  2. Institute for Materials Research, Material Physics and IMEC, Division IMOMEC, Hasselt University, Martelarenlaan 42, 3500, Hasselt, Belgium

    J. D’Haen

  3. Department of Solid State Sciences, Ghent University, Krijgslaan 281, 9000, Ghent, Belgium

    F. Mattelaer & C. Detavernier

  4. Energy Materials and Devices, Eindhoven University of Technology, 5600 MB, Eindhoven, The Netherlands

    P. H. L. Notten

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  1. E. J. van den Ham
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  7. P. H. L. Notten
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  8. A. Hardy
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  9. M. K. Van Bael
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Correspondence to E. J. van den Ham.

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van den Ham, E.J., Peys, N., De Dobbelaere, C. et al. Amorphous and perovskite Li3xLa(2/3)−xTiO3 (thin) films via chemical solution deposition: solid electrolytes for all-solid-state Li-ion batteries. J Sol-Gel Sci Technol 73, 536–543 (2015). https://doi.org/10.1007/s10971-014-3511-5

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