Issue 11, 2024

The glass phase in the grain boundary of Na3Zr2Si2PO12, created by gallium modulation

Abstract

Na3Zr2Si2PO12 has been proven to be a promising electrolyte for solid-state sodium batteries. However, its poor conductivity prevents application, caused by the large ionic resistance created by the grain boundary. Herein, we propose an additional glass phase (Na–Ga–Si–P–O phase) to connect the grain boundary via Ga ion introduction, resulting in enhanced sodium-ion conduction and electrochemical performance. The optimized Na3Zr2Si2PO12-0.15Ga electrolyte exhibits Na+ conductivity of 1.65 mS cm−1 at room temperature and a low activation energy of 0.16 eV, with 20% newly formed glass phase enclosing the grain boundary. Temperature-dependent NMR line shapes and spin-lattice relaxation were used to estimate the Na self-diffusion and Na ion hopping. The dense glass-ceramic electrolyte design strategy and the structure–dynamics–property correlation from NMR, can be extended to the optimization of other materials.

Graphical abstract: The glass phase in the grain boundary of Na3Zr2Si2PO12, created by gallium modulation

Supplementary files

Article information

Article type
Edge Article
Submitted
07 Dec 2023
Accepted
22 Jan 2024
First published
31 Jan 2024
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY-NC license

Chem. Sci., 2024,15, 3988-3995

The glass phase in the grain boundary of Na3Zr2Si2PO12, created by gallium modulation

C. Lou, W. Zhang, J. Liu, Y. Gao, X. Sun, J. Fu, Y. Shi, L. Xu, H. Luo, Y. Chen, X. Gao, X. Kuang, L. Su and M. Tang, Chem. Sci., 2024, 15, 3988 DOI: 10.1039/D3SC06578B

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