Aliovalent cation substitution in Na3Zr2Si2PO12 for practical solid-state sodium metal batteries

Jingxin He, Shuaishuai Yang, Xiong Xiao*, Debao Fang, Runqing Miao, Chengzhi Wang, Lai Chen, Ning Li, Jingbo Li, Yuefeng Su, Haibo Jin

*此作品的通讯作者

科研成果: 期刊稿件文章同行评审

摘要

High-performance solid electrolytes with high conductivity and good electrode compatibility are critical for the operable solid-state sodium metal batteries. With the Na+ superionic conductor-typed Na3Zr2Si2PO12 as a matrix, an aliovalent cation substitution strategy using Ni2+, Mn3+, Nb5+, Mo6+ substituting Zr4+ is investigated on the ionic conductivity and interfacial performance of solid-state sodium metal batteries. The low-valence Ni2+ and Mn3+ show notable effect on both enlarging the bottlenecks in the grain lattices and reducing the barriers across the grain boundaries for Na+ migration, while the high-valence Nb5+ and Mo6+ mainly facilitate Na+ migration across the grain boundaries. By tuning the doping ratios, the Ni2+ doped Na3.4Zr1.8Ni0.2Si2PO12 achieves the optimal total conductivity of 2.284 mS cm-1 at 30 °C which is 6 times higher than the undoped Na3Zr2Si2PO12. Moreover, the aliovalent cation substitution essentially improves the interface compatibility with the sodium metal, achieving reduced interfacial resistances as low as 7.80 ohm cm2 and enlarged critical current densities as high as 1.0 mA cm-2. Besides, stable charge/discharge cycles at high rates for both the symmetric Na||Na cells over 3400 h and the full cells over 2400 cycles are achieved to signify the practical merits of the neat aliovalent cation substitution strategy.

源语言英语
文章编号104037
期刊Energy Storage Materials
75
DOI
出版状态已出版 - 2月 2025

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He, J., Yang, S., Xiao, X., Fang, D., Miao, R., Wang, C., Chen, L., Li, N., Li, J., Su, Y., & Jin, H. (2025). Aliovalent cation substitution in Na3Zr2Si2PO12 for practical solid-state sodium metal batteries. Energy Storage Materials, 75, 文章 104037. https://doi.org/10.1016/j.ensm.2025.104037