Published September 7, 2021 | Version v1

High performance LATP thin film electrolytes for all-solid-state microbattery applications

  • 1. ROR icon Institut de Recerca en Energia de Catalunya
  • 2. ROR icon Instituto de Nanociencia y Materiales de Aragón
  • 3. ROR icon Universidad de Zaragoza
  • 4. Centre for Cooperative Research on Alternative Energies (CIC EnergiGUNE), Basque Research and Technology Alliance (BRTA), Alava Technology Park, Albert Einstein 48, Vitoria-Gasteiz, 01510, Spain
  • 5. ROR icon Institució Catalana de Recerca i Estudis Avançats

Description

The NASICON superionic solid electrolyte Li1+xAlxTi2-x(PO4)(3) (LATP) with 0.3 <= x <= 0.5 remains one of the most promising solid electrolytes thanks to its good ionic conductivity and outstanding stability in ambient air. Despite the intensive research for bulk systems, there are only very few studies of LATP in a thin film form (thickness < 1 mu m) and its implementation in all-solid-state batteries and microbatteries. The following study fills this gap by exploring the properties of high performance LATP thin films fabricated by large-area Pulsed Laser Deposition (PLD). The as-deposited thin films exhibit an ionic conductivity of around 0.5 mu S cm(-1) at room temperature (comparable to the state-of-the-art of LiPON) which increases to a remarkably high value of 0.1 mS cm(-1) after an additional annealing at 800 degrees C. A possible cause for this significant enhancement in ionic conductivity by two orders of magnitude is the formation of a glassy, intergranular phase. The performance of both as-deposited and annealed LATP films makes them suitable as solid electrolytes, which opens the path to a new family of stable and high performance all-solid-state thin film batteries.

Notes

This project has received funding from the European Union's Horizon 2020 research and innovation program under grant agreement No. 824072 (HARVESTORE), from the European Regional Development Fund under the FEDER Catalonia Operative Programme 2014-2020 (FEM-IoT, 001-P-00166) and the "Generalitat de Catalunya" (2017 SGR 1421, NANOEN). FIB, HRSTEM, EDS and EELS studies were conducted at the Laboratorio de Microscopias Avanzadas, Universidad de Zaragoza, Spain. R. A. gratefully acknowledges the support from the Spanish Ministry of Economy and Competitiveness (MINECO) and the MICINN through project grants MAT2016-79776-P (AEI/FEDER, UE) and PID2019-104739GB-I00 as well as from the European Union H2020 program "ESTEEM3" (823717). J. C. G.-R., acknowledges the financial support provided by the European Union's Horizon 2020 research and innovation program under the Marie Skodowska-Curie Grant Agreement No. 801342 (Tecniospring INDUSTRY), as well as by the Agency for Business Competitiveness of the Government of Catalonia. NMR measurements were supported and carried out at the Centre for Cooperative Research on Alternative Energies (CIC energiGUNE) as a member of the Basque Research and Technology Alliance (BRTA). Suitable Si3N4 substrates and microelectrodes have been provided by the Institute of Microelectronics of Barcelona IMB-CNM. Pt-covered Si substrates have been fabricated by the Interuniversity Microelectronics Centre (imec) in Leuven, Belgium. GI-XRD measurements have been collected at the Scientific and Technological Center (CCiT) at the University of Barcelona.

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