In situ neutron diffraction to investigate the solid-state synthesis of Ni-rich cathode materials

Titelangaben

Goonetilleke, Damian ; Suard, Emmanuelle ; Bergner, Benjamin ; Janek, Jürgen ; Brezesinski, Torsten ; Bianchini, Matteo:
In situ neutron diffraction to investigate the solid-state synthesis of Ni-rich cathode materials.
In: Journal of Applied Crystallography. Bd. 56 (August 2023) Heft 4 . - S. 1066-1075.
ISSN 1600-5767
DOI der Verlagsversion: https://doi.org/10.1107/S1600576723004909

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Abstract

Studying chemical reactions in real time can provide unparalleled insight into the evolution of intermediate species and can provide guidance to optimize the reaction conditions. For solid-state synthesis reactions, powder diffraction has been demonstrated as an effective tool for resolving the structural evolution taking place upon heating. The synthesis of layered Ni-rich transition-metal oxides at a large scale (grams to kilograms) is highly relevant as these materials are commonly employed as cathodes for Li-ion batteries. In this work, ıt in situ neutron diffraction was used to monitor the reaction mechanism during the high-temperature synthesis of Ni-rich cathode materials with a varying ratio of Ni:Mn from industrially relevant hydroxide precursors. Rietveld refinement was further used to model the observed phase evolution during synthesis and compare the behaviour of the materials as a function of temperature. The results presented herein confirm the suitability of ıt in situ neutron diffraction to investigate the synthesis of batches of several grams of electrode materials with well-controlled stoichiometry. Furthermore, monitoring the structural evolution of the mixtures with varying Ni:Mn content in real time reveals a delayed onset of li\-thia\-tion as the Mn content is increased, necessitating the use of higher annealing temperatures to achieve layering.