Solvent-free and low temperature synthesis of chalcogenide Na superionic conductors for solid-state batteries

Halacoglu, Selim; Li, Yang; Arnold, William; Shreyas, Varun; Guo, Xiaolin; Jasinski, Jacek B.; Narayanan, Badri; Wang, Hui

doi:10.1016/j.cej.2023.143624

Title: Solvent-free and low temperature synthesis of chalcogenide Na superionic conductors for solid-state batteries

Journal Article · Fri May 19 00:00:00 EDT 2023 · Chemical Engineering Journal

DOI:https://doi.org/10.1016/j.cej.2023.143624· OSTI ID:2234232

Halacoglu, Selim ^[1]; Li, Yang ^[1]; Arnold, William ^[1]; Shreyas, Varun ^[1]; Guo, Xiaolin ^[1]; Jasinski, Jacek B. ^[1]; Narayanan, Badri ^[1]; Wang, Hui ^[1]

University of Louisville, KY (United States)

Sodium chalcogenide ionic conductors are attractive candidates as solid electrolytes (SEs) in solid-state Na metal batteries. They show the advantages of high ionic conductivity of 10^–4–10^–2 S cm^–1 at room temperature and great chemical stability in air. However, simple, efficient, and scalable approaches for the synthesis of chalcogenide solid electrolytes (SEs) are required. In this work, we report a solvent-free mixing to form dry intermediate products, which are subjected to different treatments (electron-beam assisted method or low temperature heating (≤150 °C)) to produce pure phase of Na₃SbS_4-ySe_y (0 ≤ y < 2) chalcogenides. Heavy Se-doping in Na₃SbS₄ results in the tetragonal-to-cubic phase transition as well as a significant change of Sb-S bonding in Raman spectra. Among all chalcogenide SEs, Na₃SbS₃Se showed the highest ionic conductivity of 3.75 × 10^–4 S cm^–1 at room temperature, 47% higher than that of pristine Na₃SbS₄. Moreover, the Se-dopant also enhanced the electrochemical stability towards Na metal in solid-state batteries. The solid-state Na||FeS₂ battery with Na₃SbS₃Se SE displayed long-term cycling ability up to 1,000 cycles within the voltage window of 1.0–2.7 V and retained a specific capacity of 105 mAh g^–1 after 600 cycles. As a result, this technique promotes the practical applications of chalcogenide SEs in solid-state batteries.

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Research Organization:: Univ. of Louisville, KY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0021257; AC02-05CH11231; AC02–06CH11357

OSTI ID:: 2234232

Alternate ID(s):: OSTI ID: 1975450

Journal Information:: Chemical Engineering Journal, Vol. 468; ISSN 1385-8947

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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25 ENERGY STORAGE
Chalcogenides
Synthesis
Solvent-free
Na-ion Conductors
Solid-state battery

Title: Solvent-free and low temperature synthesis of chalcogenide Na superionic conductors for solid-state batteries

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