Publication date: 10th April 2024
In recent years, lithium tantalum phosphate LiTa2PO8 (LTPO) has emerged as a promising candidate for solid electrolyte applications, showcasing remarkable ionic conductivity, thermal, mechanical and chemical stability [1,2]. While LTPO boasts impressive bulk ionic conductivity, its overall performance is hindered by resistant grain boundaries [2]. To address this issue, doping at the Ta or P sites offers a promising way for enhancing electrical properties [3,4]. Doping is expected to improve grain conductivity by altering the crystalline structure, with the potential to increase grain boundary conductivity through microstructural modifications or secondary phase formation.
This study delves into the impact of zirconium doping on the tantalum site on the microstructural, structural, and electrical characteristics of LTPO ceramics. The introduction of Zr dopant is anticipated to increase Li ion concentration, thereby improving grain conductivity. Various ceramics with different chemical compositions were examined using a set of complementary techniques, including X-ray diffractometry (XRD), 6Li and 31P nuclear magnetic resonance (MAS NMR), Raman spectroscopy, scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDX), thermomechanical analysis (TMA), impedance spectroscopy (IS), density (Archimedes) and Hebb-Wanger polarization methods.
The samples prepared with different concentration of Zr dopant exhibited the highest value of σtot, ca. 0.9 mS/cm at 30°C. Notably, the grain conductivity remained constant at ca. 2 mS/cm, irrespective of the dopant content. The microstructural analysis unveiled correlations between variations in total ionic conductivity and changes in the concentration of secondary phases. Furthermore, the study shed light on the influence of grain arrangement on grain boundaries and porosity regions. Additionally, a determination of the location of zirconium within the material was performed.
The Polish group has received funding from the National Science Centre, grants MINIATURA 5, 2021/05/X/ST5/00530 and SONATA 18, 2022/47/D/ST5/00362, and IDUB MOBILITY PW as a part of “International scholarship exchange of doctoral students and academic staff”. The Spanish group has received funding from the MINECO MAT2016-78362-C4-2R and PID2019-106662RB-C42 projects.
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