In Situ Insights into Cathode Calcination for Predictive Synthesis Kinetic Crystallization of LiNiO2 from Hydroxides

In Situ Insights into Cathode Calcination for Predictive Synthesis : Kinetic Crystallization of LiNiO2 from Hydroxides

© 2024 Brookhaven Science Associates, LLC and UChicago Argonne, LLC. Advanced Materials published by Wiley‐VCH GmbH.

Bibliographische Detailangaben
Veröffentlicht in:Advanced materials (Deerfield Beach, Fla.). - 1998. - 36(2024), 21 vom: 14. Mai, Seite e2312027
1. Verfasser: Tayal, Akhil (VerfasserIn)
Weitere Verfasser: Barai, Pallab, Zhong, Hui, Kahvecioglu, Ozgenur, Wang, Xiaoping, Pupek, Krzysztof Z, Ma, Lu, Ehrlich, Steven N, Srinivasan, Venkat, Qu, Xiaohui, Bai, Jianming, Wang, Feng
Format: Online-Aufsatz
Sprache:English
Veröffentlicht: 2024
Zugriff auf das übergeordnete Werk:Advanced materials (Deerfield Beach, Fla.)
Schlagworte:Journal Article calcination correlative in situ X‐ray absorption/scattering spectroscopy data‐driven analysis kinetic crystallization mesoscale modeling nickel‐based cathodes
Beschreibung
Zusammenfassung:© 2024 Brookhaven Science Associates, LLC and UChicago Argonne, LLC. Advanced Materials published by Wiley‐VCH GmbH.
Calcination is a solid-state synthesis process widely deployed in battery cathode manufacturing. However, its inherent complexity associated with elusive intermediates hinders the predictive synthesis of high-performance cathode materials. Here, correlative in situ X-ray absorption/scattering spectroscopy is used to investigate the calcination of nickel-based cathodes, focusing specifically on the archetypal LiNiO2 from Ni(OH)2. Combining in situ observation with data-driven analysis reveals concurrent lithiation and dehydration of Ni(OH)2 and consequently, the low-temperature crystallization of layered LiNiO2 alongside lithiated rocksalts. Following early nucleation, LiNiO2 undergoes sluggish crystallization and structural ordering while depleting rocksalts; ultimately, it turns into a structurally-ordered layered phase upon full lithiation but remains small in size. Subsequent high-temperature sintering induces rapid crystal growth, accompanied by undesired delithiation and structural degradation. These observations are further corroborated by mesoscale modeling, emphasizing that, even though calcination is thermally driven and favors transformation towards thermodynamically equilibrium phases, the actual phase propagation and crystallization can be kinetically tuned via lithiation, providing freedom for structural and morphological control during cathode calcination
Beschreibung:Date Revised 24.05.2024
published: Print-Electronic
Citation Status PubMed-not-MEDLINE
ISSN:1521-4095
DOI:10.1002/adma.202312027