Synthetic Control of Kinetic Reaction Pathway and Cationic Ordering in High‐Ni Layered Oxide Cathodes |
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| Authors: | Dawei Wang Ronghui Kou Yang Ren Cheng‐Jun Sun Hu Zhao Ming‐Jian Zhang Yan Li Ashifia Huq J. Y. Peter Ko Feng Pan Yang‐Kook Sun Yong Yang Khalil Amine Jianming Bai Zonghai Chen Feng Wang |
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| Affiliation: | 1. Sustainable Energy Technologies Department, Brookhaven National Laboratory, Upton, NY, USA;2. Collaborative Innovation Center of Chemistry for Energy Materials, State Key Laboratory Physical Chemistry Solid Surfaces, Department of Chemistry, Xiamen University, Xiamen, Fujian, China;3. X‐Ray Science Division, Advanced Photon Source, Argonne National Laboratory, Argonne, IL, USA;4. School of Advanced Materials, Peking University Shenzhen Graduate School, Shenzhen, Guangdong, P. R. China;5. Chemical Sciences and Engineering Division, Argonne National Laboratory, Argonne, IL, USA;6. Chemical and Engineering Materials Division, Oak Ridge National Laboratory, Oak Ridge, TN, USA;7. The Cornell High Energy Synchrotron Source, Cornell University, Ithaca, NY, USA;8. Department of Energy Engineering, Hanyang University, Seoul, South Korea;9. National Synchrotron Light Source II, Brookhaven National Laboratory, Upton, NY, USA |
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| Abstract: | Nickel‐rich layered transition metal oxides, LiNi1?x (MnCo)x O2 (1?x ≥ 0.5), are appealing candidates for cathodes in next‐generation lithium‐ion batteries (LIBs) for electric vehicles and other large‐scale applications, due to their high capacity and low cost. However, synthetic control of the structural ordering in such a complex quaternary system has been a great challenge, especially in the presence of high Ni content. Herein, synthesis reactions for preparing layered LiNi0.7Mn0.15Co0.15O2 (NMC71515) by solid‐state methods are investigated through a combination of time‐resolved in situ high‐energy X‐ray diffraction and absorption spectroscopy measurements. The real‐time observation reveals a strong temperature dependence of the kinetics of cationic ordering in NMC71515 as a result of thermal‐driven oxidation of transition metals and lithium/oxygen loss that concomitantly occur during heat treatment. Through synthetic control of the kinetic reaction pathway, a layered NMC71515 with low cationic disordering and a high reversible capacity is prepared in air. The findings may help to pave the way for designing high‐Ni layered oxide cathodes for LIBs. |
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| Keywords: | cationic ordering high‐energy X‐ray diffraction layered oxide cathodes lithium‐ion batteries X‐ray absorption spectroscopy |
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