Lattice Engineering on Li2CO3-Based Sacrificial Cathode Prelithiation Agent for Improving the Energy Density of Li-Ion Battery Full-Cell

Yuanlong Zhu; Yilong Chen; Jianken Chen; Jianhua Yin; Zhefei Sun; Guifan Zeng; Xiaohong Wu; Leiyu Chen; Xiaoyu Yu; Haiyan Luo; Yawen Yan; Haitang Zhang; Baodan Zhang; Xiaoxiao Kuai; Yonglin Tang; Juping Xu; Wen Yin; Yongfu Qiu; Qiaobao Zhang; Yu Qiao; Shi-Gang Sun

doi:10.1002/adma.202312159

Lattice Engineering on Li₂CO₃-Based Sacrificial Cathode Prelithiation Agent for Improving the Energy Density of Li-Ion Battery Full-Cell

Adv Mater. 2024 Mar;36(13):e2312159. doi: 10.1002/adma.202312159. Epub 2023 Dec 27.

Authors

Yuanlong Zhu^{1

2}, Yilong Chen¹, Jianken Chen¹, Jianhua Yin¹, Zhefei Sun³, Guifan Zeng¹, Xiaohong Wu¹, Leiyu Chen¹, Xiaoyu Yu¹, Haiyan Luo¹, Yawen Yan¹, Haitang Zhang¹, Baodan Zhang¹, Xiaoxiao Kuai^{1

2}, Yonglin Tang¹, Juping Xu^{4

5}, Wen Yin^{4

5}, Yongfu Qiu⁶, Qiaobao Zhang³, Yu Qiao², Shi-Gang Sun¹

Affiliations

¹ State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China.
² Fujian Science & Technology Innovation Laboratory for Energy Materials of China (Tan Kah Kee Innovation Laboratory), Xiamen, 361005, China.
³ Country State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Materials, Xiamen University, Xiamen, 361005, China.
⁴ Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, 100049, China.
⁵ Spallation Neutron Source Science Center, Dongguan, 523803, China.
⁶ School of Materials Science and Engineering, Dongguan University of Technology, Guangdong, 523808, China.

PMID: 38117030
DOI: 10.1002/adma.202312159

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. Li₂CO₃ 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 LiCoO₂ (LCO), a lattice engineering is developed through substituting Li sites with Co and inducing Li defects to obtain a composite structure consisting of (Li_0.906Co_0.043▫_0.051)₂CO_2.934 and ball milled LiCoO₂ (Co-Li₂CO₃@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 Li₂CO₃ deep decomposition significantly decreases from typical >4.7 to ≈4.25 V versus Li/Li⁺, presenting >600 mAh g^-1 compensation capacity. Impressively, coupling 5 wt% Co-Li₂CO₃@LCO within NCM-811 cathode, 235 Wh kg^-1 pouch-type full-cell is achieved, performing 88% capacity retention after 1000 cycles.

Keywords: Li2CO3 decomposition; anionic redox; cathode prelithiation agent; lattice engineering; transition metal implantation.

Abstract

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