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<p>Developing next-generation batteries that are high-energy, low-cost and eco-friendly is crucial for industrial applications. Lithium-rich manganese-based oxide positive electrodes offer substantial specific energy, enabled by their high specific capacity at high charging potential (&gt;4.6 V versus Li/Li<sup>+</sup>). However, stable operation at such high potentials remains challenging, as most electrolytes rely on environmentally unfriendly fluorinated solvents. Here we identified α-oxidation of the carbonyl group as the main oxidation mechanism of carboxylate esters. By removing all the reactive α-hydrogens of methyl acetate, we demonstrate that methyl trimethylacetate is a non-fluorinated, high-potential-stable solvent. This solvent exhibits outstanding oxidative stability up to 5.6 V versus Li/Li<sup>+</sup>, and electrochemical cells using methyl-trimethylacetate-based electrolytes maintain stable cycling at 4.6/4.7 V, outperforming many fluorinated systems. An industrial-scale 7.2-Ah pouch cell reached a maximum specific energy of 652.4 Wh kg<sup>−1</sup> with 94.5% capacity retention after 28 cycles at 0.1 C/0.2 C. This work provides a simple molecular design strategy that addresses specific energy, cost and sustainability in next-generation high-voltage lithium batteries.</p><p></p>

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Blocking oxidation of α-hydrogens enables non-fluorinated solvents to achieve high-potential stability in lithium batteries

  • 期刊论文

  • 发表日期：

    2026年5月26日

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  • Yu-Xin Huang,
  • Yi Yang,
  • Chen-Zi Zhao,
  • Pan Xu,
  • Zi-Yue Jiang,
  • Zi-Zhang Qiu,
  • Xing-Yu Zhong,
  • Zong-Yao Shuang,
  • Xue-Yan Huang,
  • Yong-Feng Li,
  • Wei-Jin Kong,
  • Yi-Fan Tan,
  • Xiang Chen,
  • Kaihang Zhang,
  • Jia-Qi Huang,
  • Qiang Zhang

摘要

Developing next-generation batteries that are high-energy, low-cost and eco-friendly is crucial for industrial applications. Lithium-rich manganese-based oxide positive electrodes offer substantial specific energy, enabled by their high specific capacity at high charging potential (>4.6 V versus Li/Li+). However, stable operation at such high potentials remains challenging, as most electrolytes rely on environmentally unfriendly fluorinated solvents. Here we identified α-oxidation of the carbonyl group as the main oxidation mechanism of carboxylate esters. By removing all the reactive α-hydrogens of methyl acetate, we demonstrate that methyl trimethylacetate is a non-fluorinated, high-potential-stable solvent. This solvent exhibits outstanding oxidative stability up to 5.6 V versus Li/Li+, and electrochemical cells using methyl-trimethylacetate-based electrolytes maintain stable cycling at 4.6/4.7 V, outperforming many fluorinated systems. An industrial-scale 7.2-Ah pouch cell reached a maximum specific energy of 652.4 Wh kg−1 with 94.5% capacity retention after 28 cycles at 0.1 C/0.2 C. This work provides a simple molecular design strategy that addresses specific energy, cost and sustainability in next-generation high-voltage lithium batteries.