Effects of gradient concentration on the microstructure and electrochemical performance of LiNi_0.6Co_0.2Mn_0.2O₂ cathode materials

Abstract

Nickel(Ni)-rich layered materials have attracted considerable interests as promising cathode materials for lithium ion batteries (LIBs) owing to their higher capacities and lower cost. Nevertheless, Mn-rich cathode materials usually suffer from poor cyclability caused by the unavoidable side-reactions between Ni⁴⁺ ions on the surface and electrolytes. The design of gradient concentration (GC) particles with Ni-rich inside and Mn-rich outside is proved to be an efficient way to address the issue. Herein, a series of LiNi_0.6Co_0.2Mn_0.2O₂ (LNCM622) materials with different GCs (the atomic ratio of Ni/Mn decreasing from the core to the outer layer) have been successfully synthesized via rationally designed co-precipitation process. Experimental results demonstrate that the GC of LNCM622 materials plays an important role in their microstructure and electrochemical properties. The as-prepared GC3.5 cathode material with optimal GC can provide a shorter pathway for lithium-ion diffusion and stabilize the near-surface region, and finally achieve excellent electrochemical performances, delivering a discharge capacity over 176 mAh·g⁻¹ at 0.2 C rate and exhibiting capacity retention up to 94% after 100 cycles at 1 C. The rationally-designed co-precipitation process for fabricating the Ni-rich layered cathode materials with gradient composition lays a solid foundation for the preparation of high-performance cathode materials for LIBs.

Graphical abstract

Keywords

gradient concentration / Ni-rich / LiNi_0.6Co_0.2-Mn_0.2O₂ / electrochemical performance / lithium-ion battery

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