Robust Polyurethane Binders Intensified by Hydrogen Bonding, a Dynamic S–S Bond, and Metal-Ion Coordination for Silicon Anodes,ACS Applied Polymer Materials

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Robust Polyurethane Binders Intensified by Hydrogen Bonding, a Dynamic S–S Bond, and Metal-Ion Coordination for Silicon Anodes
ACS Applied Polymer Materials ( IF 4.4 ) Pub Date : 2024-01-10 , DOI: 10.1021/acsapm.3c02189
Jianghui Huang ₁ , Fei Wang ₁ , Xiang Ma ₁ , Lingli Jia ₁ , Jiamin Wang ₁ , Hongmei Liu ₁ , Qingping Wu ₂ , Jun Xu ₁

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Silicon (Si) anodes undergo severe volume expansion during charging and discharging, resulting in degradation of their electrochemical performance. Polymer binders are one of the most cost-effective ways to suppress the volume expansion of Si particles. In this paper, polyurethane (BFPU) containing conductive cycloalkane, a dynamic S–S bond, and multiple hydrogen bonds is synthesized. After that, polymeric cross-linked network binders with multiple functional bond groups are obtained by cross-linking BFPU and polydopamine (PDA) with metal ions like Zn²⁺, Fe³⁺, and Al³⁺ (PDA-M-BFPU; M = Zn, Fe, Al). The introduction of metal ions, hydrogen bonding, and a dynamic S–S bond network significantly improves the Li⁺ diffusion rate and mechanical strength, which effectively inhibits the volume expansion of the Si anode. With the addition of metal ions, the initial Coulombic efficiency (ICE) of half-cells increases from 76.5% to over 80%, especially for Si/PDA-Al-BFPU, which reaches 84.5%. Also, the capacity retention rate of Si/PDA-Al-BFPU is 76.8% after 200 cycles at 0.3 C. In addition, the full cell of NCM811//Si/PDA-Al-BFPU shows good cycle stability and rate performance. The robust BFPU binder intensified by hydrogen bonding, a dynamic S–S bond, and metal-ion coordination already exhibits great potential for application in Si anodes.

中文翻译：

通过氢键、动态 S-S 键和硅阳极金属离子配位增强的坚固聚氨酯粘合剂

硅（Si）阳极在充电和放电过程中会经历严重的体积膨胀，导致其电化学性能下降。聚合物粘合剂是抑制硅颗粒体积膨胀最经济有效的方法之一。本文合成了含有导电环烷烃、动态S-S键和多个氢键的聚氨酯（BFPU）。^{然后，通过BFPU和聚多巴胺(PDA)与Zn 2+}、Fe ³⁺和Al ³⁺等金属离子交联，得到具有多个功能键基团的聚合物交联网络粘合剂(PDA-M-BFPU；M = 锌、铁、铝）。金属离子、氢键和动态S-S键网络的引入显着提高了Li ⁺扩散速率和机械强度，有效抑制了Si负极的体积膨胀。随着金属离子的添加，半电池的初始库仑效率（ICE）从76.5%增加到80%以上，特别是Si/PDA-Al-BFPU，达到84.5%。此外，Si/PDA-Al-BFPU在0.3 C下循环200次后容量保持率为76.8%。此外，NCM811//Si/PDA-Al-BFPU全电池表现出良好的循环稳定性和倍率性能。通过氢键、动态 S-S 键和金属离子配位增强的坚固 BFPU 粘合剂已经在硅阳极中展现出巨大的应用潜力。

更新日期：2024-01-10

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