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Research Article | Open Access

Activating lithium storage in 2D CaSi2 anode via enhancing pseudocapacitive properties with oxygen modification engineering

Yongzheng Zhang2, Lu Sun3( ), Kailin Yang1, Youwang Ye1, Liang Zhan2, Qi Wei4( ), Jianan Gu1( )
Institute of Energy Power Innovation, North China Electric Power University, Beijing 100096, China
State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China
State Key Laboratory of Mesoscience and Engineering, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China
Aviation Key Laboratory of Science and Technology on Advanced Surface Engineering, AVIC Manufacturing Technology Institute, Beijing 100024, China
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Graphical Abstract

We employ a two-dimensional (2D) oxygen modification engineering approach to fabricate 2D oxygen-functionalized CaSi2 (CaSi2Ox) layers. The resulting 2D CaSi2Ox layers have a thickness of 3–5 nm, closely matching the theoretical thickness of 6–10 layers. When utilized as lithium anodes, the 2D CaSi2Ox layers exhibit exceptional electrochemical performance.

Abstract

Silicon (Si) has emerged as a promising anode material for lithium-ion batteries (LIBs) due to its extremely high theoretical capacity of 4200 mAh·g−1. However, its practical application is limited by several critical challenges, including severe volume expansion and poor electrical conductivity. Herein, we employ a two-dimensional (2D) oxygen modification engineering approach to fabricate 2D oxygen-functionalized CaSi2 (CaSi2Ox) layers. During the preparation of 2D CaSi2 layers, O atoms are gradually incorporated onto their surface. The resulting 2D CaSi2Ox layers have a thickness of 3–5 nm, closely matching the theoretical thickness of 6–10 layers. When used as lithium anodes, the 2D CaSi2Ox layers exhibit exceptional electrochemical performance, maintaining stability over 3000 cycles at an ultrahigh current density of 30 A·g−1. By tailoring the surface properties, their pseudocapacitive charge storage mechanism is significantly enhanced, effectively overcoming the intrinsic limitations of traditional Si anodes. This study highlights the promise of 2D surface engineering in the development of advanced materials for next-generation LIBs.

Keywords

two-dimensional (2D) CaSi2OxSi anodevolume changepseudocapacitivesurface modificationlithium storage

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Nano Research
Volume 18 Issue 4,
April 2025
Article number: 94907277
DOI: 10.26599/NR.2025.94907277
Cite this article:
Zhang Y, Sun L, Yang K, et al. Activating lithium storage in 2D CaSi2 anode via enhancing pseudocapacitive properties with oxygen modification engineering. Nano Research, 2025, 18(4): 94907277. https://doi.org/10.26599/NR.2025.94907277
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Received: 08 December 2024
Revised: 17 January 2025
Accepted: 27 January 2025
Published: 01 April 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/).
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