<p>Organic electrode materials offer a versatile, sustainable approach for next-generation lithium-ion batteries but are limited by low working voltages and poor cycling stability. Here we report a solid-solvation-structure design strategy to improve both the voltage and stability of organic electrode materials in all-solid-state batteries. As a proof of concept, we incorporate halide electrolytes as solid solutes and tetrachloro-<i>o</i>-benzoquinone as a solid solvent to form homogeneous solid cathode solutions. Systematic optimization of the inner solvation configuration enables tetrachloro-<i>o</i>-benzoquinone to achieve a high working voltage (3.6 V vs. Li<sup>+</sup>/Li) at room temperature within an asymmetric solid solvation sheath. Moreover, the equilibrium redox pathway and electrostatically driven self-healing interfaces revealed rapid redox kinetics and stable performance over 7,500 cycles in all-solid-state batteries under low stack pressures. This work demonstrates that organic electrode materials can serve as viable, durable and cost-effective alternatives to transition metal oxides in all-solid-state batteries.</p><p></p>

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Solid solvation structure design improves all-solid-state organic batteries

  • Yang Hu,
  • Han Su,
  • Jiamin Fu,
  • Jing Luo,
  • Qihang Yu,
  • Feipeng Zhao,
  • Weihan Li,
  • Sixu Deng,
  • Yu Liu,
  • Yi Yuan,
  • Yi Gan,
  • Yijia Wang,
  • Jung Tae Kim,
  • Ning Chen,
  • Mohsen Shakouri,
  • Xiaoge Hao,
  • Yingjie Gao,
  • Tianlu Pang,
  • Nian Zhang,
  • Ming Jiang,
  • Xia Li,
  • Yang Zhao,
  • Jiangping Tu,
  • Changhong Wang,
  • Xueliang Sun

摘要

Organic electrode materials offer a versatile, sustainable approach for next-generation lithium-ion batteries but are limited by low working voltages and poor cycling stability. Here we report a solid-solvation-structure design strategy to improve both the voltage and stability of organic electrode materials in all-solid-state batteries. As a proof of concept, we incorporate halide electrolytes as solid solutes and tetrachloro-o-benzoquinone as a solid solvent to form homogeneous solid cathode solutions. Systematic optimization of the inner solvation configuration enables tetrachloro-o-benzoquinone to achieve a high working voltage (3.6 V vs. Li+/Li) at room temperature within an asymmetric solid solvation sheath. Moreover, the equilibrium redox pathway and electrostatically driven self-healing interfaces revealed rapid redox kinetics and stable performance over 7,500 cycles in all-solid-state batteries under low stack pressures. This work demonstrates that organic electrode materials can serve as viable, durable and cost-effective alternatives to transition metal oxides in all-solid-state batteries.