期刊
JOURNAL OF MATERIALS CHEMISTRY A
卷 10, 期 31, 页码 16420-16429出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d2ta02865d
关键词
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资金
- Natural Science Foundation of Shandong Province [ZR2020QE062]
- National Natural Science Foundation of China [52102252]
- Natural Science Foundation of the Jiangsu Higher Education Institutions of China [20KJB150034]
- Independent Cultivation Program of Innovation Team of Jinan City [2019GXRC011]
- Research Grants Council of the Hong Kong Special Administrative Region, China [PolyU152208/18E, PolyU152178/20E]
- Science and Technology Program of Guangdong Province of China [2020A0505090001]
This study proposes a method to synthesize single crystal Ni-rich cathodes using lithium-containing spinel oxide as a transition phase. The introduction of the spinel phase improves the kinetics of crystal growth and prevents phase segregation. The synthesized single crystal cathodes show improved cycling stability and thermal properties compared to polycrystalline cathodes.
Single crystal cathodes with good structural stability and high volumetric energy-density have attracted considerable attention in lithium-ion batteries (LIBs). However, the general flux-free synthesis of single crystal Ni-rich cathodes is still very challenging because it requires overcoming the differences in thermodynamic stability of lithium-containing ternary metal oxide components and improving the kinetics of crystal growth during solid-state reactions. Herein, lithium-containing spinel oxide is introduced as a transition phase to overcome these issues in the synthesis of single crystal Ni-rich cathodes. Density functional theory calculations demonstrate that the spinel phase has much lower formation energy and higher thermal stability than the layered phase. Thus, the innovative introduction of the spinel phase availably enhances the kinetics of crystal growth and avoids the phase segregation of the NiO rock-salt phase. Single crystal Ni-rich Li[Ni0.6Co0.2Mn0.2]O-2 and Li[Ni0.8Co0.1Mn0.1]O-2 are synthesized by the further reaction of the-said spinel phase with Ni and Li sources. The former single crystal cathode shows improved cycling stability and thermal properties compared with those of the polycrystalline cathode. The full cells composed of this single crystal positive and mesocarbon microbead negative present high energy-density and a long-term lifespan. This proposed strategy offers a general approach to the preparation of single crystal Ni-rich cathodes for advanced LIBs.
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