Stabilizing Na3SbS4/Na interface by rational design via Cl doping and aqueous processing

doi:10.1016/j.jmst.2020.08.035

Abstract

Abstract:

Solution-synthesis method is attractive for solid electrolytes because it is a facile and scalable process to be used to permeate electrodes and to construct a thin electrolyte coating layer on active materials. In this work, we report Cl-doped Na₃SbS₄ prepared via aqueous-solution approach. Besides decent ionic conductivity, the aqueous-solution approached electrolyte demonstrates an improved interfacial stability toward Na metal compared to the solid-state sintered one because of the residual hydrate, nanosized microstructure, and Cl incorporation. All-solid-state batteries using the solution-prepared electrolytes have enhanced cycling performance, though the performance still needs to be further improved.

Key words: Interfacial stability, Sulfides, Solid electrolytes, Chemical synthesis, All-solid-state sodium battery

Haonan Cao, Meiqi Yu, Long Zhang, Zhaoxing Zhang, Xinlin Yan, Peng Li, Chuang Yu. Stabilizing Na₃SbS₄/Na interface by rational design via Cl doping and aqueous processing[J]. J. Mater. Sci. Technol., 2021, 70: 168-175.

Figures/Tables 6

Fig. 1. (a) The schematic illustration of the synthesis process of NSSC. (b) XRD patterns of NSSC. (c) SEM image of NSSC-0.05 powders. (d) The peak position of I1 (see the inset) peak as functions of x obtained from Raman spectra. The inset shows the Raman spectrum of selected sample. (e) DSC of NSSC-0.05 in the temperature range of 50-400 °C. The inset shows the TG curves of NSSC-0.05 in the temperature range of 30-300 °C.

Fig. 2. (a) Ionic conductivity as a function of Cl concentration in NSSC. Galvanostatic polarization cycling of the Na/SE/Na symmetric cells with the NSSC-0.05 (b) and NSSC-0 (c) electrolytes. (d) Galvanostatic intermittent cycling of the Na/NSSC-0.15/Na cell at a step-increased current density. (e) Galvanostatic cycling of the Na/STNSS/Na cell at 0.07 mA cm-2. The inset is an enlarged view of the initial 20 cycles. (f) The total resistances of the symmetric cells with STNSS, NSSC-0, and NSSC-0.05 electrolytes before and after galvanostatic cycling at 0.07 mA cm-2 for 20 cycles.

Fig. 3. (a) SEM cross-sectional image and corresponding EDS mapping of Na, Sb, and S elements for NSSC-0 after galvanostatic polarization cycling. (b) The electronic conductivity of the STNSS, NSSC-0, and NSSC-0.05 electrolytes.

Fig. 4. Cross-sectional SEM morphology images for the interface layer of NSSC-0.05 (a), NSSC-0 (b), and STNSS (c). (d) SEM image and EDS mapping of Na, Sb, and S elements for STNSS after galvanostatic cycling. (e) EDS mapping of Na, Sb, S, and Cl elements for NSSC-0.05 after galvanostatic cycling.

Fig. 5. The schematic illustration of the mechanism for the enhanced interfacial stability for NSSC-0.05.

Fig. 6. The charge-discharge profiles of the TiS2/STNSS/Na (a), TiS2/NSSC-0/Na (b), and TiS2/NSSC-0.05/Na (c) batteries. (d) Rate capability of the FeS2/NSSC-0.05/Na15Sn4 battery. (e) Representative charge-discharge curves of the FeS2/NSSC-0.05/Na15Sn4 battery at different current densities.

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Stabilizing Na₃SbS₄/Na interface by rational design via Cl doping and aqueous processing

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