Citation: Yao Wang, Jun Ouyang, Huadong Yuan, Jianmin Luo, Shihui Zou, Jianwei Nai, Xinyong Tao, Yujing Liu. Impact of local amorphous environment on the diffusion of sodium ions at the solid electrolyte interface in sodium-ion batteries[J]. Chinese Chemical Letters, ;2025, 36(10): 110412. doi: 10.1016/j.cclet.2024.110412 shu

Impact of local amorphous environment on the diffusion of sodium ions at the solid electrolyte interface in sodium-ion batteries

Yao Wang ^{a, b, 1} ,
Jun Ouyang ^{a, 1} ,
Huadong Yuan ^a ,
Jianmin Luo ^a ,
Shihui Zou ^a ,
Jianwei Nai ^a ,
Xinyong Tao ^a ,
Yujing Liu ^{a, *,}

a.
College of Materials Science and Engineering, Zhejiang University of Technology, Hangzhou 310014, China
b.
Moganshan Research Institute at Deqing County, Zhejiang University of Technology, Huzhou 313000, China

yujingliu@zjut.edu.cn

Received Date: 19 June 2024
Revised Date: 16 August 2024
Accepted Date: 5 September 2024
Available Online: 6 September 2024

Figures(6)

The in-depth study of the transport properties of the solid electrolyte interface (SEI) is crucial for the development of ultra-high-rate, and long lifespan sodium-ion batteries (SIBs). However, there remains a lack of theoretical investigation into the transport mechanisms of the main inorganic components of the SEI, namely NaF, Na₂O, and Na₂CO₃. To address this research gap, we performed classical molecular dynamics simulations in this work to study the diffusion mechanisms of sodium ions in these inorganic components of the SEI, with special emphasis on the impact of the amorphous SEI environment on the diffusion behavior of sodium ions. The results have shown that amorphous SEI components significantly enhance the diffusion rate of sodium ions at room temperature compared to crystalline components. Within these amorphous SEI components, we reveal that the diffusion coefficients of sodium ions in amorphous Na₂O and Na₂CO₃ are more than an order of magnitude higher than that of NaF, suggesting that amorphous Na₂O and Na₂CO₃ are more effective in facilitating the Na ion diffusion. Analysis of the local atomic structure indicates that the amorphous local structures are dominant in Na₂O and Na₂CO₃ at room temperature, maintaining a disordered amorphous phase. In contrast, amorphous NaF undergoes a spontaneously transformation into an ordered structure, exhibiting crystalline characteristics that restrict the diffusion of sodium ions. In summary, our work provides atomic insights into the impact of local amorphous environments on Na ion diffusion in SEI and suggests that amorphous SEI components play a critical role in improving battery performance.
- Sodium ions diffusion,
- Solid electrolyte interphase,
- Amorphous,
- Molecular dynamics,
- Sodium-ion batteries
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