Thermodynamically Stable Dual-Modified LiF&FeF3 layer Empowering Ni-Rich Cathodes with Superior Cyclabilities,Advanced Materials

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Thermodynamically Stable Dual-Modified LiF&FeF3 layer Empowering Ni-Rich Cathodes with Superior Cyclabilities
Advanced Materials ( IF 27.4 ) Pub Date : 2023-03-13 , DOI: 10.1002/adma.202212308
Youqi Chu _{1,

2,

3} , Yongbiao Mu _{1,

2,

3} , Lingfeng Zou _{1,

2,

3} , Yan Hu _{1,

2,

3} , Jie Cheng ₄ , Buke Wu _{1,

2,

3} , Meisheng Han _{1,

2,

3} , Shibo Xi ₅ , Qing Zhang _{1,

2,

3} , Lin Zeng _{1,

2,

3}

Affiliation

Pushing the limit of cutoff potentials allows nickel-rich layered oxides to provide greater energy density and specific capacity whereas reducing thermodynamic and kinetic stability. Herein, a one-step dual-modified method is proposed for in situ synthesizing thermodynamically stable LiF&FeF₃ coating on LiNi_0.8Co_0.1Mn_0.1O₂ surfaces by capturing lithium impurity on the surface to overcome the challenges suffered. The thermodynamically stabilized LiF&FeF₃ coating can effectively suppress the nanoscale structural degradation and the intergranular cracks. Meanwhile, the LiF&FeF₃ coating alleviates the outward migration of O^α− (α<2), increases oxygen vacancy formation energies, and accelerates interfacial Li⁺ diffusion. Benefited from these, the electrochemical performance of LiF&FeF₃ modified materials is improved (83.1% capacity retention after 1000 cycles at 1C), even under exertive operational conditions of elevated temperature (91.3% capacity retention after 150 cycles at 1C). This work demonstrates that the dual-modified strategy can simultaneously address the problems of interfacial instability and bulk structural degradation and represents significant progress in developing high-performance lithium-ion batteries (LIBs).

中文翻译：

热力学稳定的双改性 LiF 和 FeF3 层赋予富镍阴极卓越的可循环性

推动截止电位的极限允许富镍层状氧化物提供更高的能量密度和比容量，同时降低热力学和动力学稳定性。在此，提出了一种通过捕获表面上的锂杂质在 LiNi _0.8 Co _0.1 Mn _0.1 O ₂表面上原位合成热力学稳定的 LiF&FeF _{3涂层的一步双改性方法，以克服所面临的挑战。}热力学稳定的LiF&FeF ₃涂层可有效抑制纳米级结构退化和晶间裂纹。同时，LiF&FeF _{3涂层减轻了O}^α−的向外迁移(α<2)，增加氧空位形成能，加速界面Li ⁺扩散。得益于这些，LiF&FeF ₃改性材料的电化学性能得到改善（1C 下 1000 次循环后容量保持率为 83.1%），即使在高温的剧烈操作条件下（1C 下 150 次循环后容量保持率为 91.3%）。这项工作表明，双改性策略可以同时解决界面不稳定和体积结构退化的问题，代表了开发高性能锂离子电池（LIB）的重大进展。

更新日期：2023-03-13

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