Effect of Defects on Decay of Voltage and Capacity for Li[Li0.15Ni0.2Mn0.6]O2 Cathode Material

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• 作者：Wuwei Yan ; Yongning Liu ; Shengwu Guo ; Tao Jiang
• 刊名：ACS Applied Materials & Interfaces
• 出版年：2016
• 出版时间：May 18, 2016
• 年：2016
• 卷：8
• 期：19
• 页码：12118-12126
• 全文大小：772K
• 年卷期：0
• ISSN：1944-8252

文摘

Lithium-rich manganese metal layered oxides are very promising cathode materials for high-energy-density lithium-ion batteries, but improvement in voltage decay and capacity fade is a great challenge, which is mainly related to the structural instability or reconstruction of material’s surface. Defects, such as part lattice distortions, local cation disordering and atomic ununiformity, often aggravate the further structural changes upon cycling. In this paper, we found that PEG contributed to form better layered structure, well crystallinity, uniform composition and polyhedral nanoparticles for Li[Li_0.15Ni_0.2Mn_0.6]O₂ (LNMO). On the basis of the comparative trial, a mechanism of electronegativity difference is proposed to elucidate cation nonuniform distribution. Higher electronegativity of Ni (1.91) than Mn (1.55) show a stronger ability of attraction between Ni and O atoms, and then led to Ni atoms show stronger diffusion driving force toward particle surface to contact the rich O atoms during sintering in air. However, PEG polymer can form a better barrier for more O atoms to attract Ni and Mn atoms on particle surface so that facilitated a uniform distribution. The electrochemical test indicated that the decay of discharge capacity and working voltage was mitigated, which was identified by the result of HRTEM analysis that the initial less defect structure obviously retarded the phase transformation from the layered to spinel after 50 cycles. Therefore, defects are crucial for understanding the voltage fade and capacity decay, and the improvement of performance also demonstrates that designing optimum compositions and ordering atomic arrangements will contribute to stabilize the surface structure and restrain inherent phase transitions.