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<p>The incompatibility of conventional electrolytes with high-voltage cathodes and lithium metal anodes limits the performance of lithium metal batteries (LMBs). Here, an in situ cross-linked polyurethane gel electrolyte (G-P3 AR) is designed through atomic and molecular structure regulation. The polyester segments widen the highest occupied molecular orbital–lowest unoccupied molecular orbital gap, extending the electrochemical stability window to 4.97&#xa0;V for compatibility with NCM811 cathodes. Polyether segments exhibit a lower Li<sup>+</sup> binding energy, reducing the desolvation barrier and enhancing anode stability. At the atomic level, <i>sp</i><sup>2</sup>-hybridized boron in the chain extender immobilizes anions (TFSI<sup>−</sup> and DFOB<sup>−</sup>) through Lewis acid–base interactions, raising the Li<sup>+</sup> transference number to 0.78 and enabling exceptional rate capability (157.7&#xa0;mAh&#xa0;g<sup>−1</sup> at 2&#xa0;C in the Li||NCM811 cell). Hydrogen bonding between the polymer and solvent restructures the solvation sheath, promoting inorganic-rich interphases. The Li|G-P3 AR|NCM811 cell retains 81.7% capacity after 500 cycles at 0.5&#xa0;C charge/1&#xa0;C discharge, demonstrating a rational electrolyte design strategy for high-performance LMBs.</p>

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Atomic and Molecular Structure Regulated In Situ Cross-Linked Polyurethane Gel Electrolyte for High-Performance Lithium Metal Batteries

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年8月3日

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  • Jialun Ni,
  • Yong Zeng,
  • De Ning,
  • Xuan He,
  • Xiaokang Ju,
  • Xueling Liu,
  • Rui Gao,
  • Yingchun Xu,
  • Ruijie Du,
  • Dong Zhou,
  • Jun Wang,
  • Yongli Li

摘要

The incompatibility of conventional electrolytes with high-voltage cathodes and lithium metal anodes limits the performance of lithium metal batteries (LMBs). Here, an in situ cross-linked polyurethane gel electrolyte (G-P3 AR) is designed through atomic and molecular structure regulation. The polyester segments widen the highest occupied molecular orbital–lowest unoccupied molecular orbital gap, extending the electrochemical stability window to 4.97 V for compatibility with NCM811 cathodes. Polyether segments exhibit a lower Li+ binding energy, reducing the desolvation barrier and enhancing anode stability. At the atomic level, sp2-hybridized boron in the chain extender immobilizes anions (TFSI− and DFOB−) through Lewis acid–base interactions, raising the Li+ transference number to 0.78 and enabling exceptional rate capability (157.7 mAh g−1 at 2 C in the Li||NCM811 cell). Hydrogen bonding between the polymer and solvent restructures the solvation sheath, promoting inorganic-rich interphases. The Li|G-P3 AR|NCM811 cell retains 81.7% capacity after 500 cycles at 0.5 C charge/1 C discharge, demonstrating a rational electrolyte design strategy for high-performance LMBs.