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- Title
Functionalization of Cathode–Electrolyte Interface with Ionic Liquids for High-Performance Quasi-Solid-State Lithium–Sulfur Batteries: A Low-Sulfur Loading Study.
- Authors
Koralalage, Milinda Kalutara; Shreyas, Varun; Arnold, William R.; Akter, Sharmin; Thapa, Arjun; Narayanan, Badri; Wang, Hui; Sumanasekera, Gamini U.; Jasinski, Jacek B.
- Abstract
We introduce a quasi-solid-state electrolyte lithium-sulfur (Li–S) battery (QSSEB) based on a novel Li-argyrodite solid-state electrolyte (SSE), Super P–Sulfur cathode, and Li-anode. The cathode was prepared using a water-based carboxymethyl cellulose (CMC) solution and styrene butadiene rubber (SBR) as the binder while Li6PS5F0.5Cl0.5 SSE was synthesized using a solvent-based process, via the introduction of LiF into the argyrodite crystal structure, which enhances both the ionic conductivity and interface-stabilizing properties of the SSE. Ionic liquids (IL) were prepared using lithium bis(trifluoromethyl sulfonyl)imide (LiTFSI) as the salt, with pre-mixed pyrrolidinium bis(trifluoromethyl sulfonyl)imide (PYR) as solvent and 1,3-dioxolane (DOL) as diluent, and they were used to wet the SSE–electrode interfaces. The effect of IL dilution, the co-solvent amount, the LiTFSI concentration, the C rate at which the batteries are tested and the effect of the introduction of SSE in the cathode, were systematically studied and optimized to develop a QSSEB with higher capacity retention and cyclability. Interfacial reactions occurring at the cathode–SSE interface during cycling were also investigated using electrochemical impedance spectroscopy, cyclic voltammetry, and X-ray photoelectron spectroscopy supported by ab initio molecular dynamics simulations. This work offers a new insight into the intimate interfacial contacts between the SSE and carbon–sulfur cathodes, which are critical for improving the electrochemical performance of quasi-solid-state lithium–sulfur batteries.
- Subjects
LITHIUM sulfur batteries; POLYELECTROLYTES; IONIC liquids; SUPERIONIC conductors; INTERFACIAL reactions; X-ray photoelectron spectroscopy; SOLID electrolytes; CARBOXYMETHYLCELLULOSE
- Publication
Batteries, 2024, Vol 10, Issue 5, p155
- ISSN
2313-0105
- Publication type
Article
- DOI
10.3390/batteries10050155