A unique dual-shell encapsulated structure design achieves stable and high-rate lithium storage of Si@a-TiO₂@a-C anode

Abstract

Due to high theoretical capacity and low lithium-storage potential, silicon (Si)-based anode materials are considered as one kind of the most promising options for lithium-ion batteries. However, their practical applications are still limited because of significant volume expansion and poor conductivity during cycling. In this study, we prepared a double core‒shell nanostructure through coating commercial Si nanoparticles with both amorphous titanium dioxide (a-TiO₂) and amorphous carbon (a-C) via a facile sol‒gel method combined with chemical vapor deposition. Elastic behaviors of a-TiO₂ shells allowed for the release of strain, maintaining the integrity of Si cores during charge‒discharge processes. Additionally, outer layers of a-C provided numerous pore channels facilitating the transport of both Li⁺ ions and electrons. Using the distribution of relaxation time analysis, we provided a precise kinetic explanation for the observed electrochemical behaviors. Furthermore, the structural evolution of the anode was explored during cycling processes. The Si@a-TiO₂@a-C-6 anode was revealed to exhibit excellent electrochemical properties, achieving a capacity retention rate of 86.7% (877.1 mA·h·g⁻¹ after 500 cycles at a 1 A·g⁻¹). This result offers valuable insights for the design of high-performance and cyclically stable Si-based anode materials.

Graphical abstract

Keywords

lithium-ion battery / Si anode / distribution of relaxation time analysis / dual-shell encapsulated structure / high-rate lithium storage

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Authors’ contributions

Guang Ma: writing — review & editing, formal analysis, and writing — original draft; Chong Xu: writing — review & editing, formal analysis, and writing — original draft; Dongyuan Zhang: formal analysis and writing — original draft; Sai Che: writing — review & editing; Yuxin Liu: formal analysis; Gong Cheng: writing — review & editing; Chenlin Wang: writing — original draft; Kexin Wei: writing — review & editing and formal analysis; Yongfeng Li: writing — review & editing and supervision.

Declaration of competing interests

The authors declare no conflict of interests.

Acknowledgements

We gratefully acknowledge the financial support from the National Natural Science Foundation of China (Grant Nos. 22238012, 22178384, 22108301, and 22408398) and the Science Foundation of China University of Petroleum, Beijing (Grant No. ZX20230242).

Online appendix

Electronic supplementary material (ESM) can be found in the online version at https://doi.org/10.1007/s11706-024-0708-6 and https://journal.hep.com.cn/foms/EN/10.1007/s11706-024-0708-6 that includes Figs. S1–S12 and Table S1.

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