Surface Modification as a Key Factor for Spherical, Co-Free, High Capacity Li-Mn-Rich Layered Materials - from Small into the Kg Scale

Wednesday, 12 October 2022: 09:20
Galleria 8 (The Hilton Atlanta)
F. Klein, C. Pfeifer (Zentrum für Sonnenenergie- und Wasserstoff-Forschung (ZSW)), M. Lindén (Institute for Inorganic Chemistry II, Ulm University), M. Wohlfahrt-Mehrens, and P. Axmann (Zentrum für Sonnenenergie- und Wasserstoff-Forschung (ZSW))
Driven by the climate change the entire industry undergoes a structural change. Energy storage solutions, like lithium ion batteries (LIBs), become more and more important.1 The development of new materials with higher specific energy, lower costs and reduced amount of critical raw materials, such as Co and Ni, is one of the most important key points. Li‑Mn-rich layered oxides with the general formula of x Li2MnO3 · (1-x) LiMn1-y-zNiyCozO2 are one promising class of next-generation high-energy cathode materials for Li-ion batteries with specific energies beyond 900 Wh kg‑1 due to the combination of cationic and anionic redox reactions.2 However, this type of material suffers from high initial irreversible capacity loss, structural changes during long-term cycling, transition metal dissolution and a large voltage hysteresis.3 Commonly used mitigation strategies are doping to stabilize the crystal lattice and modifying the particle surface to minimize side-reactions of the active material with the electrolyte and the initial irreversible capacity loss.4

We will show the development and up-scaling of a Co-free Li-Mn-rich layered material with spherical morphology (HE-NMx), synthesized via coprecipitation reaction with subsequent lithiation and calcination process. Surface modification of the materials turned out to be one key factor influencing the specific capacity and electrochemical cycling stability of the HE-NMx. Based on the findings, the impact of selected post-treatment steps on electrochemical performance will be discussed and will be related to structural properties, obtained from a broad variety of analytical methods. Depending on the post-treatment specific capacities up to 274 mAh g-1 were reached. Scalability of the route will be shown by the successful scale-up of the most promising candidate into the 5 kg scale.

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  3. M. Armand, P. Axmann, D. Bresser, M. Copley, K. Edström, C. Ekberg, D. Guyomard, B. Lestriez, P. Novák, M. Petranikova, W. Porcher, S. Trabesinger, M. Wohlfahrt-Mehrens and H. Zhang, J. Power Sources, 479, 228708 (2020).
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