Issue 47, 2022

Vacancy-controlled quaternary sulfide Na3−xZn1−xGa1+xS4 with improved ionic conductivity and aqueous stability

Abstract

Solid electrolyte containing mobile alkaline ions is a key component in all-solid-state rechargeable batteries. In this work, a relatively new Na+-conducting solid electrolyte, Na3ZnGaS4, is investigated for a significant increase in ionic conductivity (σion) to a reasonable level. An adjustment in the Zn/Ga ratio results in vacancy formation in Na(2) sites, which leads to a steep increase in σion and to a simultaneous decrease in activation energies (0.32 mS cm−1 and 0.30 eV for hot-pressed Na2.8Zn0.8Ga1.2S4 at 30 °C). This strategy is ineffective in Na3ZnGaSe4, which possesses pre-existing vacancy defects. The preferential formation of vacancies in mobile Na(2), possibility for further improvement of σion, and excellent electrochemical stability are theoretically and experimentally verified. The perfect inertness of Na2.8Zn0.8Ga1.2S4 in aqueous dispersions (neither decomposition nor hydration) is also confirmed, which suggests that the vacancy-incorporated Na3−xM(II)1−xM(III)1+xS4 could be a promising class of Na+-conducting electrolytes.

Graphical abstract: Vacancy-controlled quaternary sulfide Na3−xZn1−xGa1+xS4 with improved ionic conductivity and aqueous stability

Supplementary files

Article information

Article type
Paper
Submitted
13 Okt 2022
Accepted
05 Nov 2022
First published
07 Nov 2022

J. Mater. Chem. A, 2022,10, 25039-25046

Vacancy-controlled quaternary sulfide Na3−xZn1−xGa1+xS4 with improved ionic conductivity and aqueous stability

S. Han, J. Y. Seo, W. B. Park, A. B. Ikhe, S. Y. Choi, S. C. Han, K. Sohn and M. Pyo, J. Mater. Chem. A, 2022, 10, 25039 DOI: 10.1039/D2TA08011G

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