<p>To meet the demand for high-energy density lithium-ion batteries in the future, silicon-based anodes have become a focal point of research. In this study, a yolk–shell-structured black phosphorus-composite polyaniline-derived porous silicon-carbon material was successfully prepared via a sacrificial templating method combined with a solvothermal process. Characterization results indicate that during the composite process with black phosphorus, stable P–C and Si–P bonds were formed between the carbon shell and the silicon core under high temperature and pressure. These chemical modifications effectively enhance the mechanical strength and ion diffusion rate of the material. Meanwhile, the yolk–shell structure provides sufficient internal voids to accommodate the substantial volume expansion inherent to silicon during cycling. The black phosphorus-composite porous silicon-carbon material demonstrates outstanding overall electrochemical performance. It exhibits an initial Coulombic efficiency of 79.99% at a current density of 0.1 A g<sup>−1</sup>, and after 150 cycles, it still maintains a capacity of approximately 700 mAh g<sup>−1</sup> with a steady upward trend in capacity. After 1000 cycles at a high current density of 2 A g<sup>−1</sup>, it maintains a reversible capacity of approximately 417.2 mAh g<sup>−1</sup>. Subsequently, using the same cycling protocol but at a lower current density of 0.1 A g<sup>−1</sup>, the capacity recovers to around 1000 mAh g<sup>−1</sup>, indicating excellent reversibility. Even after 2000 cycles (at 2 A g<sup>−1</sup>), the capacity remains at 213.32 mAh g<sup>−1</sup>. Furthermore, it demonstrates excellent rate capability (capacity retention of 97.6%) and robust structural integrity. This work proposes an effective strategy for the design and engineering of high-performance silicon-based anode materials through the combination of structural optimization and black phosphorus compositing.</p>

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Preparation of high-performance black phosphorus-composited yolk–shell porous Si@C anodes for lithium-ion batteries

  • Siran Bao,
  • Haojuan Sun,
  • Xiwei Ye,
  • Xinru Ma,
  • Gongxun Wang,
  • Yongfei Nie,
  • Zisheng Guan

摘要

To meet the demand for high-energy density lithium-ion batteries in the future, silicon-based anodes have become a focal point of research. In this study, a yolk–shell-structured black phosphorus-composite polyaniline-derived porous silicon-carbon material was successfully prepared via a sacrificial templating method combined with a solvothermal process. Characterization results indicate that during the composite process with black phosphorus, stable P–C and Si–P bonds were formed between the carbon shell and the silicon core under high temperature and pressure. These chemical modifications effectively enhance the mechanical strength and ion diffusion rate of the material. Meanwhile, the yolk–shell structure provides sufficient internal voids to accommodate the substantial volume expansion inherent to silicon during cycling. The black phosphorus-composite porous silicon-carbon material demonstrates outstanding overall electrochemical performance. It exhibits an initial Coulombic efficiency of 79.99% at a current density of 0.1 A g−1, and after 150 cycles, it still maintains a capacity of approximately 700 mAh g−1 with a steady upward trend in capacity. After 1000 cycles at a high current density of 2 A g−1, it maintains a reversible capacity of approximately 417.2 mAh g−1. Subsequently, using the same cycling protocol but at a lower current density of 0.1 A g−1, the capacity recovers to around 1000 mAh g−1, indicating excellent reversibility. Even after 2000 cycles (at 2 A g−1), the capacity remains at 213.32 mAh g−1. Furthermore, it demonstrates excellent rate capability (capacity retention of 97.6%) and robust structural integrity. This work proposes an effective strategy for the design and engineering of high-performance silicon-based anode materials through the combination of structural optimization and black phosphorus compositing.