Lithium-Rich Rock Salt Type Sulfides-Selenides

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Lithium-Rich Rock Salt Type Sulfides-Selenides ( lithium-rich-rock-salt-type-sulfides-selenides )

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materials Article Lithium-Rich Rock Salt Type Sulfides-Selenides (Li2TiSexS3−x): High Energy Cathode Materials for Lithium-Ion Batteries Yagmur Celasun, Jean-François Colin , Sébastien Martinet, Anass Benayad and David Peralta * Citation: Celasun, Y.; Colin, J.-F.; Martinet, S.; Benayad, A.; Peralta, D. Lithium-Rich Rock Salt Type Sulfides-Selenides (Li2TiSexS3−x): High Energy Cathode Materials for Lithium-Ion Batteries. Materials 2022, 15,3037. https://doi.org/10.3390/ ma15093037 Academic Editor: Alessandro Dell’Era Received: 9 March 2022 Accepted: 19 April 2022 Published: 22 April 2022 Publisher’s Note: MDPI stays neutral with regard to jurisdictional claims in published maps and institutional affil- iations. Copyright: © 2022 by the authors. Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (https:// creativecommons.org/licenses/by/ 4.0/). CEA, LITEN, University Grenoble Alpes, F-38054 Grenoble, France; yagmurcelasun@hotmail.com (Y.C.); jean-francois.colin@cea.fr (J.-F.C.); sebastien.martinet@cea.fr (S.M.); anass.benayad@cea.fr (A.B.) * Correspondence: david.peralta@cea.fr Abstract: Lithium-rich disordered rocksalt Li2TiS3 offers large discharge capacities (>350 mAh·g−1) and can be considered a promising cathode material for high-energy lithium-ion battery applications. However, the quick fading of the specific capacity results in a poor cycle life of the system, especially when liquid electrolyte-based batteries are used. Our efforts to solve the cycling stability problem resulted in the discovery of new high-energy selenium-substituted materials (Li2TiSexS3−x), which were prepared using a wet mechanochemistry process. X-ray diffraction analysis confirmed that all compositions were obtained in cation-disordered rocksalt phase and that the lattice parameters were expanded by selenium substitution. Substituted materials delivered large reversible capacities, with smaller average potentials, and their cycling stability was superior compared to Li2TiS3 upon cycling at a rate of C/10 between 3.0–1.6 V vs. Li+/Li. Keywords: high-energy materials; sulfides; anionic redox; wet mechanochemistry; selenium substitution; cyclic voltammetry 1. Introduction The rapid growth in electric vehicle market requires high performance, safe, and low-cost battery packs that should enable driving ranges exceeding 500 km. Current Li- Ion battery positive electrode materials can realize this objective by providing specific energies that exceed 250 Wh·kg−1 at cell level [1–4]. These materials still contain a small percentage of cobalt, and the concerns related to this critical element have increased, due to its price and availability. Recent research efforts have focused on the discovery of Co- poor or even Co-less positive electrode materials and the development of alternative high-energy materials, such as lithium sulfide and cation-disordered rocksalts [5–20]. Among them, cation-disordered rocksalts have recently received great interest, as a new generation of positive electrode materials for lithium ion batteries [16,17,21,22]. For instance, disordered rocksalt sulfides deliver high specific capacities (>400 mAh·g−1) at relatively low operating potentials (~2.2 V vs. Li+/Li), and their energy density is competitive with conventional layered materials [19]. This low operating potential may be considered an advantage of sulfide-type batteries, since they do not experience the serious electrolyte degradation problems occurring at higher voltages [23]. In addition, these materials allow the exchange of more than one Li per metal cation (multi-electrons redox reactions); thus, greater capacities could be produced [19,24,25]. Such a property was already noticed and reported in earlier studies, as TiS3 was able to host three Li+ ions during discharge [26,27]. However, only one lithium ion was reversibly intercalated [26]. More recently, new studies have paved the way for the discovery of novel Li-rich disordered rocksalt sulfides. Sakuda et al. highlighted that Li2TiS3 and Li3NbS4 materials with a disordered rocksalt cubic structure can provide capacities above 400 mAh·g−1 upon cycling between 3–1.5 V vs. Li+/Li [19,24]. Despite their promising reversible capacities, the retention performances of Li2TiS3 and Li3NbS4 were rather poor in conventional cells; Materials 2022, 15, 3037. https://doi.org/10.3390/ma15093037 https://www.mdpi.com/journal/materials

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