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Lithium aluminum titanium phosphate (LATP) is one of the materials under consideration as an electrolyte in future all-solid-state lithium-ion batteries. In ceramic processing, the presence of secondary phases and porosity play an important role. In a presence of more than one secondary phase and pores, image analysis must tackle the difficulties about distinguishing between these microstructural features. In this study, we study the phase evolution of LATP ceramics sintered at temperatures between 950 and 1100 ℃ by image segmentation based on energy-dispersive X-ray spectroscopy (EDS) elemental maps combined with quantitative analysis of LATP grains. We found aluminum phosphate (AlPO4) and another phosphate phase ((Lix)PyOz). The amount of these phases changes with sintering temperature. First, since the grains act as an aluminum source for AlPO4 formation, the aluminum content in the LATP grains decreases. Second, the amount of secondary phase changes from more (Lix)PyOz at 950 ℃ to mainly AlPO4 at 1100 ℃ sintering temperature. We also used scanning electron microscopy (SEM) and confocal laser scanning microscopy (CLSM) to study the evolution of the LATP grains and AlPO4, and LATP grain size increases with sintering temperature. In addition, transmission electron microscopy (TEM) was used for the determination of grain boundary width and to identify the amorphous structure of AlPO4.


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Combined quantitative microscopy on the microstructure and phase evolution in Li1.3Al0.3Ti1.7(PO4)3 ceramics

Show Author's information Deniz Cihan GUNDUZa,b,c( )Roland SCHIERHOLZa( )Shicheng YUaHermann TEMPELaHans KUNGLaRüdiger-A. EICHELa,b,c
Forschungszentrum Jülich, Institute of Energy and Climate Research (IEK-9: Fundamental Electrochemistry), Jülich D-52425, Germany
Forschungszentrum Jülich, Institute of Energy and Climate Research (IEK-12: Helmholtz-Institute Münster: Ionics in Energy Storage), Münster D-48149, Germany
RWTH Aachen University, Institute of Physical Chemistry, Aachen D-52074, Germany

Abstract

Lithium aluminum titanium phosphate (LATP) is one of the materials under consideration as an electrolyte in future all-solid-state lithium-ion batteries. In ceramic processing, the presence of secondary phases and porosity play an important role. In a presence of more than one secondary phase and pores, image analysis must tackle the difficulties about distinguishing between these microstructural features. In this study, we study the phase evolution of LATP ceramics sintered at temperatures between 950 and 1100 ℃ by image segmentation based on energy-dispersive X-ray spectroscopy (EDS) elemental maps combined with quantitative analysis of LATP grains. We found aluminum phosphate (AlPO4) and another phosphate phase ((Lix)PyOz). The amount of these phases changes with sintering temperature. First, since the grains act as an aluminum source for AlPO4 formation, the aluminum content in the LATP grains decreases. Second, the amount of secondary phase changes from more (Lix)PyOz at 950 ℃ to mainly AlPO4 at 1100 ℃ sintering temperature. We also used scanning electron microscopy (SEM) and confocal laser scanning microscopy (CLSM) to study the evolution of the LATP grains and AlPO4, and LATP grain size increases with sintering temperature. In addition, transmission electron microscopy (TEM) was used for the determination of grain boundary width and to identify the amorphous structure of AlPO4.

Keywords:

lithium aluminum titanium phosphate (LATP), microstructure, quantitative microscopy, grain size, confocal laser scanning microscopy (CLSM), NASICON
Received: 12 May 2019 Revised: 05 October 2019 Accepted: 02 November 2019 Published: 07 April 2020 Issue date: April 2020
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Received: 12 May 2019
Revised: 05 October 2019
Accepted: 02 November 2019
Published: 07 April 2020
Issue date: April 2020

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© The author(s) 2019

Acknowledgements

The FEI Helios NanoLab 460F1 and Quanta FEG 650 were funded by the German Federal Ministry of Education and Research (BMBF) via the project SABLE (SABLE- Skalenübergreifende, multi-modale 3D-Bildgebung Elektrochemischer Hochleistungskomponenten) under support code 03EK3543.

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