Operando multi-edge XAS to unlock the Co removal effect in Li- and Mn rich NMC cathodes
Laura Simonelli a, Oleg Usoltsev a, Shehab E. Ali a b, Andrea Sorrentino a, Hyeongseon Choi c d, Matthias Kuenzel c d, Stefano Passerini c d, Dino Tonti e
a ALBA Synchrotron Light Facility, Carrer de la Llum 2-26, 08290, Cerdanyola del Valles, Spain
b Physics Department, Faculty of Science, Suez Canal University, Ismailia, Egypt
c Helmholtz Institute Ulm (HIU), Helmholtzstrasse 11, 89081, Ulm, Germany
d Karlsruhe Institute of Technology (KIT), PO Box 3640, 76021, Karlsruhe, Germany
e Institut de Ciència de Materials de Barcelona (ICMAB), CSIC, Campus UAB Bellaterra, Spain
Materials for Sustainable Development Conference (MATSUS)
Proceedings of MATSUS Spring 2025 Conference (MATSUSSpring25)
In situ/operando characterization of electrochemical energy materials with synchrotron X-ray techniques - #Operax
Sevilla, Spain, 2025 March 3rd - 7th
Organizers: Carlos Escudero and Juan Jesús Velasco Vélez
Oral, Laura Simonelli, presentation 469
DOI: https://doi.org/10.29363/nanoge.matsusspring.2025.469
Publication date: 16th December 2024

Thanks to the operating high voltages and delivered capacities, Li-rich transition metal (TM) oxide cathodes are among the most promising materials for next-generation lithium-ion-batteries, where Co-free Li-rich cathodes join reduced costs with competitive performances. However, their cycle-life remains limited, and the individual role of TMs is still not fully understood. The investigation of the TM chemical species evolution along the first charge for the Li1.2Mn0.56Ni0.16Co0.08O2 and Li1.2Mn0.6Ni0.2O2 systems have been accessed by means of operando multi-edge XAS. The charge compensation mechanism has been studied and the effect induced by removing Co has been revealed. Statistical data analysis methods reveal that the absence of Co results to accelerate and complete the Ni oxidation along the first charge and to inhibit the undesired spinel formation and oxygen release at the end of the first voltage plateau. The reasons of the oxygen release in the Co-containing electrode and its relation to structural modifications will be presented.

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