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Research Article | Open Access

Volume expansion restriction by TiO2 structural unit in silicon anodes with yolk–shell structure for lithium-ion batteries

Yuan Li1,2Shengkai Sun1,3Junjie Tang1,2Sihui Han1,3Yu Yang3Jun Xing1,3Lingbo Zong1,3Lei Wang1,3 ( )Bin Li1,2 ( )
State Key Laboratory of Eco-Chemical Engineering, International Science and Technology Cooperation Base of Eco-chemical Engineering and Green Manufacturing, Qingdao University of Science and Technology, Qingdao 266042, China
College of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, China
College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao 266042, China
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Abstract

Silicon, due to its high theoretical capacity and abundant resources, has emerged as a potential anode material for lithium-ion batteries (LIBs). However, it suffers from intrinsic capacity decay and rapid degradation, coupled with huge volume expansion that leads to unstable growth of solid electrolyte interface (SEI). Here, we present a straightforward method to construct yolk–shell (YS)-Si/SiO2-Ti@C materials with YS structure by reducing titanium silicalite-1 (TS-1) with magnesium and altering depositing carbon sequence. Besides, the intermediate space can effectively accommodate the expansion of internal silicon nanoparticles. TiO2 structural units anchored in the silica alleviate stress–strain in the Si nanoparticles to enhance the cycling stability. The obtained YS-Si/SiO2-Ti@C composites anode exhibits exceptional reversible capacity and cycling stability compared to YS-Si/SiO2@C (without TiO2) and commercial Si electrodes. Notably, the YS-Si/SiO2-Ti@C composite anode achieves a high specific capacity (1290 mAh·g−1 after 200 cycles at 0.8 A·g−1) and a stable SEI film. Specially, the YS-Si/SiO2-Ti@C electrode delivers impressive capacity of 1590, 1521, 1222, and 646 mAh·g−1 at 0.8, 2, 4, and 8 A·g−1, respectively. This study paves an avenue for addressing challenge of drastic volume change in silicon during lithiation/delithiation process to improve cycling stability of LIBs.

Graphical Abstract

Yolk–shell (YS)-Si/SiO2-Ti@C nanoparticles which feature internal voids and in situ-modified TiO2 structural units, can be simply obtained by magnesium reduction, chemical vapor deposition (CVD) and HCl pickling. The internal TiO2 structural units help mitigate the stress–strain during the silicon alloying process, while the internal void space alleviates the volume expansion issue during cycling. This results in superior cycling performance.

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Nano Research
Article number: 94907474

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Cite this article:
Li Y, Sun S, Tang J, et al. Volume expansion restriction by TiO2 structural unit in silicon anodes with yolk–shell structure for lithium-ion batteries. Nano Research, 2025, 18(6): 94907474. https://doi.org/10.26599/NR.2025.94907474
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Received: 17 February 2025
Revised: 13 April 2025
Accepted: 15 April 2025
Published: 16 June 2025
© The Author(s) 2025. Published by Tsinghua University Press.

This is an open access article under the terms of the Creative Commons Attribution 4.0 International License (CC BY 4.0, https://creativecommons.org/licenses/by/4.0/).