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<p>As next-generation high-energy storage systems, lithium metal batteries (LMBs) show significant promise for electric vehicles and aerospace applications. While gel polymer electrolytes (GPEs) mitigate liquid electrolyte volatility, accommodate lithium anode volume changes, and enhance cycling stability in solid-state LMBs, their mechanical strength remains inadequate. Here, we fabricate a cellulose nanocrystal (CNC)-reinforced poly(ethylene oxide) (PEO)-based GPE via blade-coating onto poly(ethylene terephthalate) nonwoven fabric (NW PET), followed by gelation with 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl) imide (EMIM TFSI) ionic liquid (IL). Compared to the GPE with NW PET and without CNC modification (denoted as NW GPE), the CNC-modified GPE (denoted as NW GPE-C<sub>10</sub>) displays improved mechanical strength, thermal stability, ionic conductivity and lithium ion transference number (<i>t</i><sub>+</sub>) owing to the enhanced interaction between CNC and bis(trifluoromethylsulfonyl)imide anion (TFSI<sup>−</sup>) that could limit the transportation of TFSI<sup>−</sup>, resulting in superior electrochemical performance of LMBs. The NW GPE-C<sub>10</sub>-based cell exhibits an ionic conductivity of 5.75 × 10<sup>−4</sup>&#xa0;S&#xa0;cm<sup>−1</sup> (vs. 4.21 × 10<sup>−4</sup>&#xa0;S&#xa0;cm<sup>−1</sup> for NW GPE) at room temperature and a <i>t</i><sub>+</sub> of 0.41 (vs. 0.20 for NW GPE). The Li|NW GPE-C<sub>10</sub>|LFP full cell shows an initial specific capacity of 122.8&#xa0;mAh g<sup>−1</sup> at 0.5 C with a relatively good capacity retention of 90.6% after 180 cycles and an average coulombic efficiency (CE) of 97.25%. In terms of the convenient preparation protocol and excellent performances, the NW GPE-C<sub>10</sub> could pave a new avenue in future to expand the application prospect of solid state LMBs.</p>

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Cellulose nanocrystal improved poly(ethylene terephthalate)-supported poly(ethylene oxide)/ionic liquid-based gel polymer electrolytes for solid state lithium metal batteries

  • 期刊论文

  • 发表日期：

    2025年10月21日

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  • Shuqiu Wu,
  • Xingyu Li,
  • Cai Qi,
  • Liying Liu,
  • Xi Ke,
  • Ruijie Xu,
  • Xubing Fu,
  • Caihong Lei

摘要

As next-generation high-energy storage systems, lithium metal batteries (LMBs) show significant promise for electric vehicles and aerospace applications. While gel polymer electrolytes (GPEs) mitigate liquid electrolyte volatility, accommodate lithium anode volume changes, and enhance cycling stability in solid-state LMBs, their mechanical strength remains inadequate. Here, we fabricate a cellulose nanocrystal (CNC)-reinforced poly(ethylene oxide) (PEO)-based GPE via blade-coating onto poly(ethylene terephthalate) nonwoven fabric (NW PET), followed by gelation with 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl) imide (EMIM TFSI) ionic liquid (IL). Compared to the GPE with NW PET and without CNC modification (denoted as NW GPE), the CNC-modified GPE (denoted as NW GPE-C10) displays improved mechanical strength, thermal stability, ionic conductivity and lithium ion transference number (t+) owing to the enhanced interaction between CNC and bis(trifluoromethylsulfonyl)imide anion (TFSI−) that could limit the transportation of TFSI−, resulting in superior electrochemical performance of LMBs. The NW GPE-C10-based cell exhibits an ionic conductivity of 5.75 × 10−4 S cm−1 (vs. 4.21 × 10−4 S cm−1 for NW GPE) at room temperature and a t+ of 0.41 (vs. 0.20 for NW GPE). The Li|NW GPE-C10|LFP full cell shows an initial specific capacity of 122.8 mAh g−1 at 0.5 C with a relatively good capacity retention of 90.6% after 180 cycles and an average coulombic efficiency (CE) of 97.25%. In terms of the convenient preparation protocol and excellent performances, the NW GPE-C10 could pave a new avenue in future to expand the application prospect of solid state LMBs.