Oxygen-regulated spontaneous solid electrolyte interphase enabling ultra-stable solid-state Na metal batteries

Keshuang Cao; Yufan Xia; Haosheng Li; Huiqin Huang; Sikandar Iqbal; Muhammad Yousaf; Ben Bin Xu; Wenping Sun; Mi Yan; Hongge Pan; Yinzhu Jiang

doi:10.1016/j.scib.2023.11.017

Oxygen-regulated spontaneous solid electrolyte interphase enabling ultra-stable solid-state Na metal batteries

Sci Bull (Beijing). 2024 Jan 15;69(1):49-58. doi: 10.1016/j.scib.2023.11.017. Epub 2023 Nov 7.

Authors

Keshuang Cao¹, Yufan Xia¹, Haosheng Li¹, Huiqin Huang¹, Sikandar Iqbal², Muhammad Yousaf², Ben Bin Xu³, Wenping Sun⁴, Mi Yan⁵, Hongge Pan⁶, Yinzhu Jiang⁷

Affiliations

¹ School of Materials Science and Engineering, Zhejiang University, Hangzhou 310027, China; ZJU-Hangzhou Global Scientific and Technological Innovation Center, Zhejiang University, Hangzhou 311200, China.
² ZJU-Hangzhou Global Scientific and Technological Innovation Center, Zhejiang University, Hangzhou 311200, China.
³ Mechanical and Construction Engineering, Faculty of Engineering and Environment, Northumbria University, Newcastle upon Tyne NE1 8ST, UK.
⁴ School of Materials Science and Engineering, Zhejiang University, Hangzhou 310027, China.
⁵ School of Materials Science and Engineering, Zhejiang University, Hangzhou 310027, China; State Key Laboratory of Baiyunobo Rare Earth Resource Researches and Comprehensive Utilization, Baotou Research Institute of Rare Earths, Baotou 014030, China.
⁶ School of Materials Science and Engineering, Zhejiang University, Hangzhou 310027, China; Institute of Science and Technology for New Energy, Xi'an Technological University, Xi'an 710021, China.
⁷ School of Materials Science and Engineering, Zhejiang University, Hangzhou 310027, China; ZJU-Hangzhou Global Scientific and Technological Innovation Center, Zhejiang University, Hangzhou 311200, China; State Key Laboratory of Baiyunobo Rare Earth Resource Researches and Comprehensive Utilization, Baotou Research Institute of Rare Earths, Baotou 014030, China. Electronic address: yzjiang@zju.edu.cn.

PMID: 37973461
DOI: 10.1016/j.scib.2023.11.017

Abstract

Solid-state sodium metal batteries utilizing inorganic solid electrolytes (SEs) hold immense potentials such as intrinsical safety, high energy density, and environmental sustainability. However, the interfacial inhomogeneity/instability at the anode-SE interface usually triggers the penetration of sodium dendrites into the electrolyte, leading to short circuit and battery failure. Herein, confronting with the original nonuniform and high-resistance solid electrolyte interphase (SEI) at the Na-Na₃Zr₂Si₂PO₁₂ interface, an oxygen-regulated SEI innovative approach is proposed to enhance the cycling stability of anode-SEs interface, through a spontaneous reaction between the metallic sodium (containing trace amounts of oxygen) and the Na₃Zr₂Si₂PO₁₂ SE. The oxygen-regulated spontaneous SEI is thin, uniform, and kinetically stable to facilitate homogenous interfacial Na⁺ transportation. Benefitting from the optimized SEI, the assembled symmetric cell exhibits an ultra-stable sodium plating/stripping cycle for over 6600 h under a practical capacity of 3 mAh cm^-2. Quasi-solid-state batteries with Na₃V₂(PO₄)₃ cathode deliver excellent cyclability over 500 cycles at a rate of 0.5 C (1 C = 117 mA cm^-2) with a high capacity retention of 95.4%. This oxygen-regulated SEI strategy may offer a potential avenue for the future development of high-energy-density solid-state metal batteries.

Keywords: Anode interface; Na metal anode; NaSICON; Solid electrolyte interphase; Solid-state batteries.