Unlocking Interlayer Confinement Enables All-Slope Hard Carbon with Ultrafast and Highly Reversible Sodium Storage

Addressing the rapid capacity decay of hard carbon anodes under high-current-density conditions remains a critical challenge for sodium-ion batteries. Conventional hard carbon materials suffer from strong interlayer confinement that severely hinders Na<sup>+</sup> diffusion, leading to sluggish kinetics and irreversible ion trapping. Although expanding the slope region by introducing more active sites can improve rate performance, it often accelerates excessive SEI formation and reduces the initial Coulombic efficiency (ICE). Herein, we develop an amino N-guided through-pore engineering strategy that effectively mitigates interlayer confinement and enables all-slope-dominated sodium storage with rapid and reversible kinetics. Using a facile gas-phase-assisted pyrolysis process, we achieve simultaneous conversion of irreversible nitrogen configurations into highly reversible pyridinic N sites and in situ construction of vertically aligned through-pores directed by amino species. These amino groups not only passivate reactive edge sites but also facilitate the formation of a thin, gradient SEI enriched with subsurface fluorides, greatly reducing sodium loss and achieving an ultrahigh ICE of 94.9%. The resulting anode exhibits a high reversible capacity of 400.3 mAh g<sup>-1</sup>, exceptional rate performance (208 mAh g<sup>-1</sup> at 50 A g<sup>-1</sup>), and outstanding cycling stability (92.5% capacity retention after 9000 cycles). This work highlights the crucial role of amino-mediated pore and defect management in synchronizing interfacial stability and ion transport kinetics, providing a viable design strategy for high-power alkali-ion batteries.

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Publication Details

Journal
ACS Nano
Published
2025-10-29
DOI
https://doi.org/10.1021/acsnano.5c14641
Citations
4
Primary Topic
Advancements in Battery Materials
Type
article
Field-Weighted Citation Impact
2.92
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article

Unlocking Interlayer Confinement Enables All-Slope Hard Carbon with Ultrafast and Highly Reversible Sodium Storage

Shendong Xu, Tianlai Xia, Xingqiao Wu, Jin Bai et al.
4 citations
ACS Nano
Advancements in Battery Materials
2.92
article

Unlocking Interlayer Confinement Enables All-Slope Hard Carbon with Ultrafast and Highly Reversible Sodium Storage

Shendong Xu, Tianlai Xia, Xingqiao Wu, Jin Bai, Siya Wang, Shulei Chou, Yongtao Li, Xiaojun He, Xuebin Zhu, Bangchuan Zhao, Yuping Sun, Peiyao Wang
article en
4 citations

Abstract

Addressing the rapid capacity decay of hard carbon anodes under high-current-density conditions remains a critical challenge for sodium-ion batteries. Conventional hard carbon materials suffer from strong interlayer confinement that severely hinders Na<sup>+</sup> diffusion, leading to sluggish kinetics and irreversible ion trapping. Although expanding the slope region by introducing more active sites can improve rate performance, it often accelerates excessive SEI formation and reduces the initial Coulombic efficiency (ICE). Herein, we develop an amino N-guided through-pore engineering strategy that effectively mitigates interlayer confinement and enables all-slope-dominated sodium storage with rapid and reversible kinetics. Using a facile gas-phase-assisted pyrolysis process, we achieve simultaneous conversion of irreversible nitrogen configurations into highly reversible pyridinic N sites and in situ construction of vertically aligned through-pores directed by amino species. These amino groups not only passivate reactive edge sites but also facilitate the formation of a thin, gradient SEI enriched with subsurface fluorides, greatly reducing sodium loss and achieving an ultrahigh ICE of 94.9%. The resulting anode exhibits a high reversible capacity of 400.3 mAh g<sup>-1</sup>, exceptional rate performance (208 mAh g<sup>-1</sup> at 50 A g<sup>-1</sup>), and outstanding cycling stability (92.5% capacity retention after 9000 cycles). This work highlights the crucial role of amino-mediated pore and defect management in synchronizing interfacial stability and ion transport kinetics, providing a viable design strategy for high-power alkali-ion batteries.

ACS NanoVol. 19(44)
University of Science and Technology of China (CN), Wenzhou University (CN), Anhui University of Science and Technology (CN), Chinese Academy of Sciences (CN), Institute of Solid State Physics (CN), Nano Carbon (Poland) (PL), University of Birmingham (GB), Anhui University of Technology (CN)
Openalex Percentile: Top 8%
Advancements in Battery Materials
2.92
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