Journal
ADVANCED ENERGY MATERIALS
Volume 9, Issue 43, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/aenm.201901915
Keywords
high-Ni layered oxide cathodes; lithium-ion batteries; quenching; solid-state synthesis; surface reconstruction
Categories
Funding
- U.S. Department of Energy (DOE) Office of Energy Efficiency and Renewable Energy, Vehicle Technologies Office [DE-SC0012704]
- Guangdong innovative team program [2013N080]
- Guangdong Key-lab Project [2017B0303010130]
- Shenzhen Science and Technology [ZDSYS201707281026184]
- Chinese postdoctoral science foundation [2015M570882, 2015M570894]
- U.S. DOE Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory [DE-SC0012704]
- U.S. Department of Energy, Office of Basic Energy Science, Division of Materials Science and Engineering [DE-SC0012704]
- US Department of Energy, Vehicle Technologies Office [DE-AC02-06CH11357]
- peacock plan [KYPT20141016105435850]
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Transition metal layered oxides have been the dominant cathodes in lithium-ion batteries, and among them, high-Ni ones (LiNixMnyCozO2; x >= 0.7) with greatly boosted capacity and reduced cost are of particular interest for large-scale applications. The high Ni loading, on the other hand, raises the critical issues of surface instability and poor rate performance. The rational design of synthesis leading to layered LiNi0.7Mn0.15Co0.15O2 with greatly enhanced rate capability is demonstrated, by implementing a quenching process alternative to the general slow cooling. In situ synchrotron X-ray diffraction, coupled with surface analysis, is applied to studies of the synthesis process, revealing cooling-induced surface reconstruction involving Li2CO3 accumulation, formation of a Li-deficient layer and Ni reduction at the particle surface. The reconstruction process occurs predominantly at high temperatures (above 350 degrees C) and is highly cooling-rate dependent, implying that surface reconstruction can be suppressed through synthetic control, i.e., quenching to improve the surface stability and rate performance of the synthesized materials. These findings may provide guidance to rational synthesis of high-Ni cathode materials.
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