Microstructureand Electrochemical Performance ofLi<sub>2</sub>CO<sub>3</sub>‑Modified Submicron SiO as an Anodefor Lithium-Ion Batteries

Silicon monoxide (SiO) holds great potential as a next-generation anode material for commercial lithium-ion batteries due to its high theoretical specific capacity. However, poor cycling stability and low initial Coulombic efficiency (ICE) present substantial challenges for its practical application. Herein, we modified the structure of commercial SiO through ball milling, followed by heating with the addition of the network modifier Li<sub>2</sub>CO<sub>3</sub>. The submicrometer-sized SiO reduces Li<sup>+</sup> diffusion pathways within the SiO bulk, facilitating the Li<sup>+</sup> insertion/extraction process and enabling excellent rate performance. Controlling the size of silicon nanodomains within SiO enhances the structural stability of the material during cycling, thereby significantly improving its cycling stability. The increased crystallinity of SiO<sub>2</sub> suppresses irreversible reactions, leading to a higher ICE. Moreover, Li<sup>+</sup> ions trapped within the Si–O–Si network form a lithium silicate glass-like phase, which provides efficient pathways for Li<sup>+</sup> diffusion within the material, thereby enhancing its electrochemical performance. The optimized submicrometer SiO was mixed with graphite and coated with carbon to produce a submicrometer SiO/graphite@carbon composite anode. When assembled into a half-cell, the composite anode exhibited an initial discharge specific capacity of 1277.0 mA h g<sup>–1</sup> at 0.1 A g<sup>–1</sup>, with an ICE of 74.3%. And this anode demonstrated a capacity retention of 79.7% after 300 cycles at 0.5 A g<sup>–1</sup>. Furthermore, during rate capability testing, it achieved a discharge specific capacity of 428.9 mA h g<sup>–1</sup> at 1.6 A g<sup>–1</sup>.

Publication Details

Journal
Figshare
Published
2025-03-24
DOI
https://doi.org/10.1021/acsami.4c21119.s001
Primary Topic
Advancements in Battery Materials
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article
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Microstructureand Electrochemical Performance ofLi2CO3‑Modified Submicron SiO as an Anodefor Lithium-Ion Batteries

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Advancements in Battery Materials
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Microstructureand Electrochemical Performance ofLi2CO3‑Modified Submicron SiO as an Anodefor Lithium-Ion Batteries

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Abstract

Silicon monoxide (SiO) holds great potential as a next-generation anode material for commercial lithium-ion batteries due to its high theoretical specific capacity. However, poor cycling stability and low initial Coulombic efficiency (ICE) present substantial challenges for its practical application. Herein, we modified the structure of commercial SiO through ball milling, followed by heating with the addition of the network modifier Li<sub>2</sub>CO<sub>3</sub>. The submicrometer-sized SiO reduces Li<sup>+</sup> diffusion pathways within the SiO bulk, facilitating the Li<sup>+</sup> insertion/extraction process and enabling excellent rate performance. Controlling the size of silicon nanodomains within SiO enhances the structural stability of the material during cycling, thereby significantly improving its cycling stability. The increased crystallinity of SiO<sub>2</sub> suppresses irreversible reactions, leading to a higher ICE. Moreover, Li<sup>+</sup> ions trapped within the Si–O–Si network form a lithium silicate glass-like phase, which provides efficient pathways for Li<sup>+</sup> diffusion within the material, thereby enhancing its electrochemical performance. The optimized submicrometer SiO was mixed with graphite and coated with carbon to produce a submicrometer SiO/graphite@carbon composite anode. When assembled into a half-cell, the composite anode exhibited an initial discharge specific capacity of 1277.0 mA h g<sup>–1</sup> at 0.1 A g<sup>–1</sup>, with an ICE of 74.3%. And this anode demonstrated a capacity retention of 79.7% after 300 cycles at 0.5 A g<sup>–1</sup>. Furthermore, during rate capability testing, it achieved a discharge specific capacity of 428.9 mA h g<sup>–1</sup> at 1.6 A g<sup>–1</sup>.

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Microstructureand Electrochemical Performance ofLi<sub>2</sub>CO<sub>3</sub>‑Modified Submicron SiO as an Anodefor Lithium-Ion Batteries · Figshare (2025) | TGRS Research Map | TGRS