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Title: | Phase Engineering via Aluminum Doping Enhances the Electrochemical Stability of Lithium-Rich Cobalt-Free Layered Oxides for Lithium-Ion Batteries | Authors: | DE SLOOVERE, Dries MYLAVARAPU, Satish Kumar D'HAEN, Jan Thersleff, Thomas Jaworski, Aleksander Grins, Jekabs Svensson, Gunnar Stoyanova, Radostina Josang, Leif Olav Prakasha, Kunkanadu Rajappa Merlo, Maximiliano Martinez, Elias Nel-lo Pascual, Marc Jacas Biendicho, Jordi VAN BAEL, Marlies HARDY, An |
Issue Date: | 2024 | Publisher: | WILEY-V C H VERLAG GMBH | Source: | Small, | Status: | Early view | Abstract: | Lithium-rich, cobalt-free oxides are promising potential positive electrode materials for lithium-ion batteries because of their high energy density, lower cost, and reduced environmental and ethical concerns. However, their commercial breakthrough is hindered because of their subpar electrochemical stability. This work studies the effect of aluminum doping on Li1.26Ni0.15Mn0.61O2 as a lithium-rich, cobalt-free layered oxide. Al doping suppresses voltage fade and improves the capacity retention from 46% for Li1.26Ni0.15Mn0.61O2 to 67% for Li1.26Ni0.15Mn0.56Al0.05O2 after 250 cycles at 0.2 C. The undoped material has a monoclinic Li2MnO3-type structure with spinel on the particle edges. In contrast, Al-doped materials (Li1.26Ni0.15Mn0.61-xAlxO2) consist of a more stable rhombohedral phase at the particle edges, with a monoclinic phase core. For this core-shell structure, the formation of Mn3+ is suppressed along with the material's decomposition to a disordered spinel, and the amount of the rhombohedral phase content increases during galvanostatic cycling. Whereas previous studies generally provided qualitative insight into the degradation mechanisms during electrochemical cycling, this work provides quantitative information on the stabilizing effect of the rhombohedral shell in the doped sample. As such, this study provides fundamental insight into the mechanisms through which Al doping increases the electrochemical stability of lithium-rich cobalt-free layered oxides. This study investigates the impact of aluminum doping on Li1.26Ni0.15Mn0.61O2, a lithium-rich, cobalt-free layered oxide. The undoped material has a monoclinic structure, while the Al-doped materials contain a more stable rhombohedral phase at the particle edges. This work quantitatively elucidates the stabilizing effect of the rhombohedral shell, shedding light on mechanisms that enhance the electrochemical stability of lithium-rich layered oxides. image | Notes: | De Sloovere, D; Hardy, A (corresponding author), UHasselt, Inst Mat Res Imo Imomec, Bldg D, B-3590 Diepenbeek, Belgium.; De Sloovere, D; Hardy, A (corresponding author), Imec, Bldg D, B-3590 Diepenbeek, Belgium.; De Sloovere, D; Hardy, A (corresponding author), EnergyVille, Thor Pk 8320, B-3600 Genk, Belgium. dries.desloovere@uhasselt.be; an.hardy@uhasselt.be |
Keywords: | aluminium;Co-free;cycle life;Li-rich;voltage fade | Document URI: | http://hdl.handle.net/1942/42686 | ISSN: | 1613-6810 | e-ISSN: | 1613-6829 | DOI: | 10.1002/smll.202400876 | ISI #: | 001174108400001 | Rights: | 2024 Wiley-VCH GmbH | Category: | A1 | Type: | Journal Contribution |
Appears in Collections: | Research publications |
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File | Description | Size | Format | |
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Small - 2024 - De Sloovere - Phase Engineering via Aluminum Doping Enhances the Electrochemical Stability of Lithium‐Rich.pdf Restricted Access | Early view | 5.27 MB | Adobe PDF | View/Open Request a copy |
autheursversie.pdf | Peer-reviewed author version | 7.78 MB | Adobe PDF | View/Open |
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