A Sulfide‐Based Solid Electrolyte With High Humid Air Tolerance for Long Lifespan All‐Solid‐State Sodium Batteries

Author:

Guo Yayu1,Liu Kai1,Li Cheng2,Song Dawei1,Zhang Hongzhou1,Wang Zhenyu3,Yan Yufen1,Zhang Lianqi1ORCID,Dai Sheng45

Affiliation:

1. School of Materials Science and Engineering Tianjin University of Technology Tianjin 300384 China

2. Neutron Scattering Division Oak Ridge National Laboratory Oak Ridge TN 37830 USA

3. Guilin Electrical Equipment Scientific Research Institute Co., Ltd Guilin 541004 China

4. Chemical Sciences Division Oak Ridge National Laboratory Oak Ridge TN 37831 USA

5. Department of Chemistry University of Tennessee Knoxville TN 37996 USA

Abstract

AbstractSulfide‐based superionic conductors present great promise to achieve high energy density and safety for all‐solid‐state sodium batteries (ASSSBs). However, the poor electrolyte/electrode interface compatibility and humid air stability seriously hinder their deployment in ASSSBs. Herein, a series of high‐performance Na3‐□Sb1‐4x(SnWCaTi)xS4 sulfide‐based solid electrolytes (SSEs) are reported by coupling the vacancy effect with configurational entropy, which displays an excellent interface stability against sodium metal and an extraordinary tolerance toward the moist atmosphere, even for water. The optimized electrolyte effectively inhibits the detrimental mixed ion‐electron conducting interphase formation, achieving the ultra‐stable operation of Na–Na symmetric cell up to 1000 h. Furthermore, the Na+ diffusion kinetics is obviously enhanced by increasing the Na sites local anisotropy and Na vacancies. Eventually, the assembled TiS2//Na5Sn ASSSBs deliver a remarkable reversible capacity of 211.6 mAh g−1 at 0.5C with a long‐term cycling performance of 450 cycles at room temperature. More importantly, it achieves a steady running up to 100 cycles at 1C even if this electrolyte is placed in the air with a dew temperature of 13.8 °C for 30 min, the highest values in the state‐of‐the‐art sulfide‐based ASSSBs. The well‐designed SSEs open a new avenue for realizing the advanced and powerful ASSSBs.

Funder

National Natural Science Foundation of China

U.S. Department of Energy

Office of Science

Basic Energy Sciences

Materials Sciences and Engineering Division

Publisher

Wiley

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