<p>Biomass-derived self-supporting carbon materials are considered promising cathodes for zinc-ion capacitors owing to their structural tunability and cost-effectiveness. Natural ramie fibers form a 3D interpenetrating network, which provides excellent mechanical support for flexible electrodes. However, conventional high-temperature activation often induces structural collapse. Although surface etching preserves flexible frameworks, it limits pore development, resulting in underutilized surface area and poor pore-carrier compatibility. These limitations create a trade-off between electrochemical performance and structural flexibility. This study presents a top–down intercalation activation strategy for precise pore regulation in natural plant fiber-derived carbon. To completely preserve the flexible fiber skeleton, this approach successfully constructs an interconnected hierarchical channel system, which effectively reduces the ion diffusion barrier. Consequently, the flexible electrode exhibits abundant defect structures and a high specific surface area of 2477&#xa0;m<sup>2</sup>&#xa0;g<sup>−1</sup>, which is 50 times that of directly carbonized ramie fibers. These features significantly increase the number of active sites available for charge storage. The assembled zinc-ion hybrid capacitor exhibits an excellent specific capacity of 212&#xa0;mAh&#xa0;g<sup>−1</sup> at 0.2&#xa0;A&#xa0;g<sup>−1</sup> and an energy density of 168&#xa0;Wh&#xa0;kg<sup>−1</sup>, and retains 91% of its capacity after 50,000 cycles. Notably, the assembled flexible device maintains normal operations under multi-angle bending conditions, indicating excellent stability. The proposed strategy provides an innovative approach for the precise regulation of pore size in biomass-derived carbon fibers and enables the efficient preparation of other cellulose-based self-supporting carbon materials.</p> Graphical Abstract <p></p>

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Overcoming Hydrated Zn2+ Diffusion Barriers via Molecular Intercalation Activation of Ramie Fiber-Derived Flexible Zinc-Ion Hybrid Capacitors with High Energy Density

  • Zhiwei Tian,
  • Zixuan Guo,
  • Gaigai Duan,
  • Jingquan Han,
  • Weijun Li,
  • Yong Huang,
  • Xiaoshuai Han,
  • Chunmei Zhang,
  • Shuijian He,
  • Haoqing Hou,
  • Shaohua Jiang

摘要

Biomass-derived self-supporting carbon materials are considered promising cathodes for zinc-ion capacitors owing to their structural tunability and cost-effectiveness. Natural ramie fibers form a 3D interpenetrating network, which provides excellent mechanical support for flexible electrodes. However, conventional high-temperature activation often induces structural collapse. Although surface etching preserves flexible frameworks, it limits pore development, resulting in underutilized surface area and poor pore-carrier compatibility. These limitations create a trade-off between electrochemical performance and structural flexibility. This study presents a top–down intercalation activation strategy for precise pore regulation in natural plant fiber-derived carbon. To completely preserve the flexible fiber skeleton, this approach successfully constructs an interconnected hierarchical channel system, which effectively reduces the ion diffusion barrier. Consequently, the flexible electrode exhibits abundant defect structures and a high specific surface area of 2477 m2 g−1, which is 50 times that of directly carbonized ramie fibers. These features significantly increase the number of active sites available for charge storage. The assembled zinc-ion hybrid capacitor exhibits an excellent specific capacity of 212 mAh g−1 at 0.2 A g−1 and an energy density of 168 Wh kg−1, and retains 91% of its capacity after 50,000 cycles. Notably, the assembled flexible device maintains normal operations under multi-angle bending conditions, indicating excellent stability. The proposed strategy provides an innovative approach for the precise regulation of pore size in biomass-derived carbon fibers and enables the efficient preparation of other cellulose-based self-supporting carbon materials.

Graphical Abstract