Citation: Zi-Hao Zuo, Jiang-Kui Hu, Xi-Long Wang, Shi-Jie Yang, Wei-Qi Mai, Yao-Hui Zhu, Zheng Liao, Jia Liu, Hong Yuan, Jia-Qi Huang. Oxygen defect-mediated Li-ion transport for long-cycle solid-state lithium metal batteries[J]. Chinese Chemical Letters, ;2026, 37(5): 110851. doi: 10.1016/j.cclet.2025.110851 shu

Oxygen defect-mediated Li-ion transport for long-cycle solid-state lithium metal batteries

Zi-Hao Zuo ^{a, b} ,
Jiang-Kui Hu ^{a, b} ,
Xi-Long Wang ^{a, b} ,
Shi-Jie Yang ^{a, b} ,
Wei-Qi Mai ^{a, d} ,
Yao-Hui Zhu ^{a, d} ,
Zheng Liao ^{a, b} ,
Jia Liu ^c ,
Hong Yuan ^{a, b, *,} ,
Jia-Qi Huang ^{a, b, *,}

a.
School of Materials Science & Engineering, Beijing Institute of Technology, Beijing 100081, China
b.
Advanced Research Institute of Multidisciplinary Science, Beijing Institute of Technology, Beijing 100081, China
c.
Beijing Key Laboratory of Lignocellulosic Chemistry, College of Materials Science and Technology, Beijing Forestry University, Beijing 100083, China
d.
Advanced Research Institute of Multidisciplinary Science, Beijing Institute of Technology, Zhuhai 519088, China

yuanhong@bit.edu.cn

jqhuang@bit.edu.cn

Received Date: 26 November 2024
Revised Date: 28 December 2024
Accepted Date: 14 January 2025
Available Online: 14 January 2025

Figures(5)

Solid-state lithium (Li) metal batteries have attracted significant attention due to their high energy density and improved safety performance. However, sluggish Li-ion transport and rapid anion migration in solid-state electrolytes often result in heterogeneous Li-ion flux distribution and thus Li dendrite growth. Herein, we developed a highly conductive composite solid electrolyte with an elevated Li-ion transference number through incorporating Gd-doped CeO₂ (GDC) nanofillers with abundant surface oxygen defects into poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) matrices. The defect concentrations were effectively controlled by regulating the Gd doping ratio in CeO₂. As a result, the highest oxygen concentration of 12.2% is achieved for the GDC with 10% Gd doping (GDC-10). The GDC-10 electrolyte demonstrated a high Li-ion transference number of 0.59 and an improved ionic conductivity of 0.40 mS/cm at room temperature, attributed to anion immobilization and enhanced Li-salt dissociation. This was due to the strong interactions between positively charged oxygen vacancies and anions, which effectively reduces surface concentration polarization and homogenizes Li-ion flux. Therefore, LiLi symmetric cells exhibited exceptional cycling stability of 1500 h without noticeable Li dendrite growth at 1 mA/cm² and 1 mAh/cm². Furthermore, LiLiFePO₄ full cell also stably cycles for 500 cycles with a capacity retention of 90.44% at 1 C. This work provides new insights into the design of composite solid electrolytes through the defect regulation of fillers.
- Solid-state batteries,
- Composite solid-state electrolytes,
- Li-ion transport,
- Anion immobilization,
- Li-ion transference number
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