<p>Hard carbon (HC) is currently recognized as the leading anode material for commercial sodium-ion batteries (SIBs). However, its low initial Coulombic efficiency (ICE) severely limits its broader application. Herein, we propose a microstructure regulation strategy for resin-derived HC through a synergistic approach involving a controllable precursor polymerization assisted by melamine and a subsequent crosslinking reaction with succinic anhydride. Structural characterizations reveal that the optimized HC (MPFS) exhibits an expanded interlayer spacing (0.38 nm), a reduced specific surface area (2.61 m<sup>2</sup> g<sup>-1</sup>), and abundant closed pores within the material, contrasting with the original resin-derived HC. These structural advantages enable the MPFS anode to achieve a remarkable ICE of 92.2% coupled with a high reversible capacity of 324.4 mA h g<sup>-1</sup>, which is superior to commercial HC (81.7%, 276.6 mA h g<sup>-1</sup>) and the original resin-derived HC (87.0%, 297.0 mA h g<sup>-1</sup>). This study establishes an effective methodology for enhancing the ICE of HC without sacrificing the reversible capacity through rational microstructure design, providing critical insights for advancing the development of SIBs.</p>

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Molecular-level polymerization and crosslinking regulation strategies to optimize resin-derived hard carbon for sodium-ion storage

  • Sishi Li,
  • Jiaqi Liu,
  • Yandong Xie,
  • Zhenyuan Miao,
  • Ziqiang Fan,
  • Yuecong Chen,
  • Shiyin Xie,
  • Yining Lao,
  • Jian Zhu,
  • Qingyun Dou,
  • Xingbin Yan

摘要

Hard carbon (HC) is currently recognized as the leading anode material for commercial sodium-ion batteries (SIBs). However, its low initial Coulombic efficiency (ICE) severely limits its broader application. Herein, we propose a microstructure regulation strategy for resin-derived HC through a synergistic approach involving a controllable precursor polymerization assisted by melamine and a subsequent crosslinking reaction with succinic anhydride. Structural characterizations reveal that the optimized HC (MPFS) exhibits an expanded interlayer spacing (0.38 nm), a reduced specific surface area (2.61 m2 g-1), and abundant closed pores within the material, contrasting with the original resin-derived HC. These structural advantages enable the MPFS anode to achieve a remarkable ICE of 92.2% coupled with a high reversible capacity of 324.4 mA h g-1, which is superior to commercial HC (81.7%, 276.6 mA h g-1) and the original resin-derived HC (87.0%, 297.0 mA h g-1). This study establishes an effective methodology for enhancing the ICE of HC without sacrificing the reversible capacity through rational microstructure design, providing critical insights for advancing the development of SIBs.