Lattice Engineering on Li<sub>2</sub>CO<sub>3</sub>-Based Sacrificial Cathode Prelithiation Agent for Improving the Energy Density of Li-Ion Battery Full-Cell.

Zhu, Yuanlong; Chen, Yilong; Chen, Jianken; Yin, Jianhua; Sun, Zhefei; Zeng, Guifan; Wu, Xiaohong; Chen, Leiyu et al. · Adv Mater · 2024

basic_science · Level V

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Abstract

Developing sacrificial cathode prelithiation technology to compensate for active lithium loss is vital for improving the energy density of lithium-ion battery full-cells. Li<sub>2</sub>CO<sub>3</sub> owns high theoretical specific capacity, superior air stability, but poor conductivity as an insulator, acting as a promising but challenging prelithiation agent candidate. Herein, extracting a trace amount of Co from LiCoO<sub>2</sub> (LCO), a lattice engineering is developed through substituting Li sites with Co and inducing Li defects to obtain a composite structure consisting of (Li<sub>0.906</sub>Co<sub>0.043</sub>▫<sub>0.051</sub>)<sub>2</sub>CO<sub>2.934</sub> and ball milled LiCoO<sub>2</sub> (Co-Li<sub>2</sub>CO<sub>3</sub>@LCO). Notably, both the bandgap and Li─O bond strength have essentially declined in this structure. Benefiting from the synergistic effect of Li defects and bulk phase catalytic regulation of Co, the potential of Li<sub>2</sub>CO<sub>3</sub> deep decomposition significantly decreases from typical >4.7 to ≈4.25 V versus Li/Li<sup>+</sup>, presenting >600 mAh g<sup>-1</sup> compensation capacity. Impressively, coupling 5 wt% Co-Li<sub>2</sub>CO<sub>3</sub>@LCO within NCM-811 cathode, 235 Wh kg<sup>-1</sup> pouch-type full-cell is achieved, performing 88% capacity retention after 1000 cycles.