期刊
ADVANCED SCIENCE
卷 8, 期 2, 页码 -出版社
WILEY
DOI: 10.1002/advs.202001809
关键词
LiNi0 8Co0 1Mn0 1O2; oxygen vacancies; structural stability; thermal stability; ZrB2
资金
- National Key R&D Program of China [2018YFB0104000]
- National Nature Science Foundation of China [21571189, 21771062, U19A2019]
- Hunan Provincial Science and Technology Major Project of China [2017GK1040]
- Hunan Provincial Science and Technology Plan Project, China [2017TP1001, 2016TP1007, 2020jj2042, 2018RS3009]
A three in one strategy using ZrB2 as a dopant is proposed to stabilize the crystal structure and surface of the Ni-rich cathode. Zr and B doping helps stabilize the crystal structure and prevent the formation of microcracks, while Zr also forms a coating with the surface lithium source to protect the surface and suppress interfacial phase transition.
LiNi0.8Co0.1Mn0.1O2 cathodes suffer from severe bulk structural and interfacial degradation during battery operation. To address these issues, a three in one strategy using ZrB2 as the dopant is proposed for constructing a stable Ni-rich cathode. In this strategy, Zr and B are doped into the bulk of LiNi0.8Co0.1Mn0.1O2, respectively, which is beneficial to stabilize the crystal structure and mitigate the microcracks. Meanwhile, during the high-temperature calcination, some of the remaining Zr at the surface combined with the surface lithium source to form lithium zirconium coatings, which physically protect the surface and suppress the interfacial phase transition upon cycling. Thus, the 0.2 mol% ZrB2-LiNi0.8Co0.1Mn0.1O2 cathode delivers a discharge capacity of 183.1 mAh g(-1) after 100 cycles at 50 degrees C (1C, 3.0-4.3 V), with an outstanding capacity retention of 88.1%. The cycling stability improvement is more obvious when the cut-off voltage increased to 4.4 V. Density functional theory confirms that the superior structural stability and excellent thermal stability are attributed to the higher exchange energy of Li/Ni exchange and the higher formation energy of oxygen vacancies by ZrB2 doping. The present work offers a three in one strategy to simultaneously stabilize the crystal structure and surface for the Ni-rich cathode via a facile preparation process.
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