期刊
NATURE COMMUNICATIONS
卷 5, 期 -, 页码 -出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/ncomms4529
关键词
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资金
- Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the U.S. Department of Energy under the Batteries for Advanced Transportation Technologies (BATT) Program [DE-AC02-05CH11231]
- US Department of Energy, Office of Basic Energy Sciences [DE-AC02-98CH10886]
- US Department of Energy (DOE) [DE-AC02-05CH11231]
- Office of Science of the US Department of Energy [DE-AC03-76SF00098]
- Extreme Science and Engineering Discovery Environment (XSEDE)
- National Science Foundation [OCI-1053575]
- NSF graduate research fellowship programme
The present study sheds light on the long-standing challenges associated with high-voltage operation of LiNixMnxCo1-2xO2 cathode materials for lithium-ion batteries. Using correlated ensemble-averaged high-throughput X-ray absorption spectroscopy and spatially resolved electron microscopy and spectroscopy, here we report structural reconstruction (formation of a surface reduced layer, R (3) over barm to Fm (3) over barm transition) and chemical evolution (formation of a surface reaction layer) at the surface of LiNixMnxCo1-2xO2 particles. These are primarily responsible for the prevailing capacity fading and impedance buildup under high-voltage cycling conditions, as well as the first-cycle coulombic inefficiency. It was found that the surface reconstruction exhibits a strong anisotropic characteristic, which predominantly occurs along lithium diffusion channels. Furthermore, the surface reaction layer is composed of lithium fluoride embedded in a complex organic matrix. This work sets a refined example for the study of surface reconstruction and chemical evolution in battery materials using combined diagnostic tools at complementary length scales.
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