Journal
ADVANCED MATERIALS
Volume 29, Issue 39, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.201606715
Keywords
cationic ordering; high-energy X-ray diffraction; layered oxide cathodes; lithium-ion batteries; X-ray absorption spectroscopy
Categories
Funding
- U.S. Department of Energy (DOE) Office of Energy Efficiency and Renewable Energy under the Advanced Battery Materials Research (BMR) program [DE-SC0012704]
- U.S. Department of Energy, Office of Basic Energy Sciences [DE-SC0012704]
- US Department of Energy-Basic Energy Sciences
- Canadian Light Source
- Advanced Photon Source
- U.S. Department of Energy [DE-AC02-06CH11357]
- National Natural Science Foundation of China [21233004, 21473148, 21428303, 21621091]
- NSLS-II
- U.S. Department of Energy (DOE) Office of Science User Facility [DE-SC0012704]
- Scientific User Facilities Division, Office of Basic Energy Sciences, US Department of Energy
- National Science Foundation [DMR-1332208]
- Global Frontier R&D Program on Center for Hybrid Interface Materials (HIM) - Ministry of Science, Information & Communication Technology (ICT) [2013M3A6B1078875]
- Human Resources Development program of the Korea Institute of Energy Technology Evaluation and Planning (KETEP) - Korea government Ministry of Trade, Industry and Energy [20154010200840]
- National Research Foundation of Korea [2013M3A6B1078875] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
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Nickel-rich layered transition metal oxides, LiNi1-x(MnCo)(x)O-2 (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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