1.中南大学化学化工学院,湖南 长沙 410000
2.中南大学粉末冶金研究院,湖南 长沙 410000
3.胜华新材料科技(眉山)有限公司,四川 眉山 620000
袁新烨(2001—),男,硕士研究生,232311099@csu.edu.cn
韩凯(1986—),男,博士,教授,kaihan@csu.edu.cn
收稿:2025-05-06,
修回:2025-07-15,
纸质出版:2025-12-31
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袁新烨, 邢显博, 刘登华, 丁伟涛, 范博瑞, 钟华, 韩凯. 气相沉积硅碳中硅结晶度对电化学性能的影响[J]. 化工学报, 2025, 76(12): 6708-6717
YUAN Xinye, XING Xianbo, LIU Denghua, DING Weitao, FAN Borui, ZHONG Hua, HAN Kai. Effect of silicon crystallinity on electrochemical performance for chemical vapor deposited silicon-carbon composites[J]. CIESC Journal, 2025, 76(12): 6708-6717
袁新烨, 邢显博, 刘登华, 丁伟涛, 范博瑞, 钟华, 韩凯. 气相沉积硅碳中硅结晶度对电化学性能的影响[J]. 化工学报, 2025, 76(12): 6708-6717 DOI: 10.11949/0438-1157.20250494.
YUAN Xinye, XING Xianbo, LIU Denghua, DING Weitao, FAN Borui, ZHONG Hua, HAN Kai. Effect of silicon crystallinity on electrochemical performance for chemical vapor deposited silicon-carbon composites[J]. CIESC Journal, 2025, 76(12): 6708-6717 DOI: 10.11949/0438-1157.20250494.
硅作为高能量密度锂离子电池的新一代负极材料,其商业化应用的关键技术路径之一是与碳材料复合构建核壳结构的硅碳材料。如何实现硅晶粒形态的精确控制是当前硅碳材料产业化量产过程中的难题之一。采用化学气相沉积法将纳米/亚纳米尺寸硅均匀沉积在多孔碳基体中制备气相沉积硅碳复合材料,通过调控最终碳层封装温度实现了硅结晶度的可控调节。结果表明,拉曼光谱技术较X射线衍射方法在硅结晶度表征方面具有更高的灵敏度与准确率优势;碳层封装温度影响硅碳中硅的结晶度水平,硅结晶度升高会对材料的整体电化学性能有负面影响。碳层封装温度在550℃时制备的硅碳表现出1599 mAh·g
-1
的首圈放电容量和91.62%的首次库仑效率,升高到800℃时降低到了709 mAh·g
-1
和80.97%。研究结果为气相沉积硅碳材料量产过程实现硅结晶度的准确控制提供了可靠方法,可实现高性能低结晶度硅碳负极量产过程中的高精度一致性管控。
Silicon
as a new generation anode material for high-energy-density lithium-ion batteries
is a key technological path for its commercial application by combining it with carbon materials to construct core-shell silicon-carbon materials. Achieving precise control over the morphology of silicon grains is one of the challenges in the current industrial-scale mass production of silicon-carbon materials. Silicon was uniformly deposited into a porous carbon matrix
via
chemical vapor deposition (CVD)
followed by modulating the crystallinity of silicon through controlled carbon encapsulation temperatures. Systematic characterization revealed that Raman spectroscopy exhibits superior sensitivity and accuracy over X-ray diffraction in quantifying silicon crystallinity. The carbon encapsulation temperat
ure was found to exert a significant influence on the crystallinity of silicon
with elevated crystallinity levels markedly degrading the overall electrochemical performance. Specifically
elevation of carbon encapsulation temperature from 550℃ to 800℃ induced a 55.7% capacity loss (1599→709 mAh·g
-1
) and 10.65% efficiency decay (91.62%→80.97%) in initial cycling
quantitatively demonstrating the crystallinity-dependent degradation mechanism in silicon-carbon anodes. These findings confirm that Raman spectroscopy serves as a precise diagnostic tool for optimizing CVD process parameters
enabling high-precision consistency control in the mass production of high-performance
low-crystallinity silicon-carbon anodes.
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