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Structural engineering of hard carbon through spark plasma sintering for enhanced sodium-ion storage

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Abstract

Hard carbon (HC) has emerged as one of the superior anode materials for sodium-ion batteries (SIBs), with its electrochemical performance significantly influenced by the presence of oxygen functional groups and its closed pore structure. However, current research on the structural adjustment of these oxygen functional groups and the closed pore architecture within HC remains limited. Herein, energy-efficient and contamination-free spark plasma sintering technology was employed to tune the structure of coconut-shell HC, resulting in significant adjustments to the content of carboxyl (decreasing from 5.71 at% to 2.12 at%) and hydroxyl groups (decreasing from 7.73 at% to 6.26 at%). Crucially, these modifications reduced the irreversible reaction of oxygen functional groups with Na+. Simultaneously, a substantial number of closed pores with an average diameter of 1.22 nm were generated within the HC, offering an ideal environment for efficient Na+ accommodation. These structural changes resulted in a remarkable improvement in the electrochemical performance of the modified HC. The reversible specific capacity of the modified HC surged from 73.89 mAh·g−1 to an impressive 251.97 mAh·g−1 at a current density of 50 mA·g−1. Even at 400 mA·g−1, the reversible specific capacity increased significantly from 14.55 to 85.44 mAh·g−1. Hence, this study provides a novel perspective for designing tailored HC materials with the potential to develop high-performance SIBs.

Graphical abstract

摘要

硬炭 (HC) 作为钠离子电池中的优良负极材料, 其储钠性能受到氧官能团和闭孔结构的显著影响。本文采用高效快速的放电等离子体烧结技术对椰壳炭进行了表面改性和孔结构调控, 将羧基含量从5.71 at%降低到2.12 at%和羟基从7.73 at%降低到6.26 at%。这些调控减少了氧官能团与Na+的不可逆反应。与此同时, 在HC内产生了大量的闭孔, 平均孔径为1.22 nm, 为高效储钠提供了理想的空间, 使其电化学性能有了显著的提升。在电流密度为50 mA·g−1时, 可逆储钠容量从73.89 mAh·g−1增长到251.97 mAh·g−1。因此, 本研究为设计和开发高性能钠离子电池负极材料的制备提供了新的视角。

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (No. 52062012), Guangdong Province Key Discipline Construction Project (No. 2021ZDJS102), the Innovation Team of Universities of Guangdong Province (No. 2022KCXTD030), the Special Fund for Science and Technology Innovation Cultivation of Guangdong University Students (No. pdjh2023b0549) and the Student Academic Fund of Foshan University (No. xsjj202206kjb02).

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  1. Hao-Ming Xiao and Heng Zheng have contributed equally to this work.

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  1. Guangdong Key Laboratory for Hydrogen Energy Technologies, School of Materials Science and Hydrogen Energy, Foshan University, Foshan, 528000, China

    Hao-Ming Xiao, Jun-Hui Luo, Lin-Lin Shen, Jie-Feng Tan, Xian-You Luo & Yong Chen

  2. State Key Laboratory of Marine Resource Utilization in South China Sea, Hainan Provincial Key Laboratory of Research on Utilization of Si-Zr-Ti Resources, Hainan University, Haikou, 570228, China

    Heng Zheng, Ping Yuan & De Li

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Xiao, HM., Zheng, H., Yuan, P. et al. Structural engineering of hard carbon through spark plasma sintering for enhanced sodium-ion storage. Rare Met. (2024). https://doi.org/10.1007/s12598-024-02716-7

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