Converting Li‐Rich Layered Oxide Cathode into Non‐Shrinking Sacrificial Prelithiation Agent
Abstract
Abstract To improve the energy density of Li‐ion batteries, conventional sacrificial prelithiation agents (Li 5 FeO 4 , Li 2 O and Li 2 CO 3 , etc.) are introduced to compensate for active lithium loss, but they undergo serious volumetric shrinkage during decomposition, generating voids that compromise electrode architecture integrity and deteriorate electrochemical performance. Herein, the typical Li‐rich layered oxide cathode is converted into Li‐rich disordered rocksalt oxide (LRDO) prelithiation agent, achieving 330 mAh g −1 charge capacity and retaining 130 mAh g −1 reversible capacity (contributing 200 mAh g −1 irreversible prelithiation capacity). Compared with the layered structure, the cation‐disordered structure in LRDO tunes the local oxygen environment, completely activating oxygen‐related anionic oxidation activity at lower potential (<4.5 V). Moreover, coupled with a fluorinated electrolyte additive, the nucleophilic oxygen species released during de‐lithiation of LRDO are synergistically utilized, constructing a gradient cathode‐electrolyte interphase architecture with enhanced interfacial stability during the cell formation process. Most importantly, the phase‐transition‐free nature of LRDO during prelithiation completely eradicates volume shrinkage, effectively preventing electrode architecture degradation. Furthermore, a long‐life graphite||LiFePO 4 pouch cell with high discharge capacity of 150.02 mAh (7.59% higher than without prelithiation) are achieved, maintaining 91.33% capacity after 1800 cycles.
Article Details
Authors (21)
Yilong Chen
State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Department of Chemistry, College of Chemistry and Chemical Engineering
Minwen Yang
School of Materials Sun Yat‐sen University Shenzhen 518107 P.R. China
Yuanlong Zhu
State Key Laboratory of Physical Chemistry of Solid Surfaces Department of Chemistry College of Chemistry and Chemical Engineering Xiamen University Xiamen 361005 China
Jianhua Yin
State Key Laboratory of Physical Chemistry of Solid Surfaces Department of Chemistry College of Chemistry and Chemical Engineering Xiamen University Xiamen 361005 P.R. China
Li Li
Jiyuan Xue
State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering Xiamen University Xiamen P. R. China
Baodan Zhang
Center of Advanced Electrochemical Energy, Institute of Advanced Interdisciplinary Studies, School of Chemistry and Chemical Engineering
Haiyan Luo
State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Department of Chemistry, College of Chemistry and Chemical Engineering
Kang Zhang
Qi Biodesign, Beijing, China.
Zixin Wu
College of Chemistry, Chemical Engineering and Materials Science, and State Key Laboratory of Radiation Medicine and Protection
Yuan Tian
Juping Xu
Institute of High Energy Physics
Wen Yin
Qingsong Wang
Na Liu
Yang Sun
Maolin Yang
Yongfu Qiu
School of Environment and Civil Engineering Research Institute of Interdisciplinary Science Dongguan University of Technology Dongguan Guangdong 523808 P.R. China
Xin Sun
Yu Qiao
Shi‐Gang Sun
State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical Engineering Xiamen University Xiamen P. R. China