Retardation of Structure Densification by Increasing Covalency in Li-Rich Layered Oxide Positive Electrodes for Li-Ion Batteries

• DOI: 10.1021/acs.chemmater.2c00921
• Publication Date: 2022-07-21T02:20:17Z
• Authors: Anatolii V. Morozov; Ivan A. Moiseev; Aleksandra A. Savina; Anton O. Boev; Dmitry A. Aksyonov; Leiting Zhang; Polina A. Morozova; Victoria A. Nikitina; Egor M. Pazhetnov; Erik J. Berg; Stanislav S. Fedotov; Jean-Marie Tarascon; Evgeny V. Antipov; Artem M. Abakumov
• Keywords: 02 engineering and technology; 0210 nano-technology

Because of the outstanding discharge capacity provided by oxygen redox activity, Li-rich layered oxide positive electrode materials for Li-ion batteries attract tremendous attention. However, there is still no full consensus on role that ionocovalency transition metal (TM)–oxygen (O) chemical bonding plays in reversibility as well both local crystal and electronic structure transformations. Here, we managed to tune cationic/anionic contributions overall electrochemical activity using xLi2RuO3-(1 – x)Li1.2Ni0.2Mn0.6O2 solid solutions a model system possessing same morphology oxides. We conclusively traced whole cascade events from increasing covalency TM–O bond, suppressing irreversible oxidation generation reduced Mn species toward retarding "densification" The results demonstrate enhancing degree vitally important anchoring charge compensation mechanism occurring through partial oxidation.