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<p>Silicon stands out as promising negative electrode for future lithium-ion batteries owing to its high specific capacity. However, drastic volume change during cycling results in significant loss of electronic/ionic conduction and poor cycling life, necessitating external stack pressure to confine volume expansion. In this work, we develop a gel polymer electrolyte by in situ co-polymerizing methyl methacrylate and 2-(3-(6-methyl-4-oxo-1,4-dihydropyrimidin-2-yl)ureido)ethyl methacrylate to enable pressure-free and energy-dense silicon-based lithium-ion batteries. Benefiting from the crosslinked polymer structure and self-healing property, the SiO<sub>x</sub> particles experience limited volume expansion and maintain robust interfacial contact with the gel electrolyte, leading to a capacity retention of 90.2% after 400 cycles (0.3 C, 500 mA g<sup>-1</sup>). Additionally, the gel electrolytes effectively supress electrode swelling and the formation of “dead silicon”, endowing 1000 cycles (0.5 C, 0.8 A) for Ah-scale silicon-based pouch cells free from external stack pressure. Such gel electrolytes also demonstrate safety superiority to conventional liquid electrolytes, which promotes the commercial viability of high-energy-density silicon-based batteries.</p>

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A gel polymer electrolyte with multiple hydrogen bonding for pressure-free Ah silicon-based pouch cells

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年11月28日

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  • Fangzheng Liu,
  • Yong Zeng,
  • Zenan Li,
  • Yushen Liu,
  • Xinyu Chen,
  • Yidong Jiang,
  • Huaiyu Shao,
  • Junpo Guo,
  • Xiaoxiong Xu,
  • Fangfang Pan,
  • Yonghong Deng,
  • Jun Wang,
  • Minhua Shao

摘要

Silicon stands out as promising negative electrode for future lithium-ion batteries owing to its high specific capacity. However, drastic volume change during cycling results in significant loss of electronic/ionic conduction and poor cycling life, necessitating external stack pressure to confine volume expansion. In this work, we develop a gel polymer electrolyte by in situ co-polymerizing methyl methacrylate and 2-(3-(6-methyl-4-oxo-1,4-dihydropyrimidin-2-yl)ureido)ethyl methacrylate to enable pressure-free and energy-dense silicon-based lithium-ion batteries. Benefiting from the crosslinked polymer structure and self-healing property, the SiOx particles experience limited volume expansion and maintain robust interfacial contact with the gel electrolyte, leading to a capacity retention of 90.2% after 400 cycles (0.3 C, 500 mA g-1). Additionally, the gel electrolytes effectively supress electrode swelling and the formation of “dead silicon”, endowing 1000 cycles (0.5 C, 0.8 A) for Ah-scale silicon-based pouch cells free from external stack pressure. Such gel electrolytes also demonstrate safety superiority to conventional liquid electrolytes, which promotes the commercial viability of high-energy-density silicon-based batteries.