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Carbon cathode with heteroatom doping and ultrahigh surface area enabling enhanced capacitive behavior for potassium-ion hybrid capacitors

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Abstract

Potassium-ion hybrid capacitors (PIHCs) are widely regarded as highly promising energy storage devices, due to their exceptional energy density, impressive power density, and abundant potassium resources. Unfortunately, restricted by the inherent capacitive storage mechanism, the carbon cathodes possess a much lower specific capacity than battery-type anodes. Therefore, designing high-performance carbon cathodes is extremely urgent for the development of PIHCs. Herein, N, O co-doped porous carbon (NOPC) was fabricated through the NaCl hard template method and combined KOH/melamine chemical activation technique, displaying the characteristics of abundant N/O content (4.7 at%/16.9 at%), ultrahigh specific surface area (3092 m2·g?1) and hierarchical pore network. The designed NOPC cathode delivers a high specific capacity (164.4 mAh·g?1 at 0.05 A·g?1) and superior cyclability (95.1% retention ratio at 2 A·g?1 over 2500 cycles). Notably, the adjustable ratio of micropores to mesopores facilitates the achievement of the optimal balance between capacity and rate capability. Moreover, the pseudocapacitance can be further augmented through the incorporation of N/O functional groups. As expected, the graphite//NOPC based PIHC possesses a high energy density of 113 Wh·kg?1 at 747 W·kg?1 and excellent capacity retention of 84.4% after 4000 cycles at 1.0 A·g?1. This work introduces a novel strategy for designing carbon cathodes that enhances the electrochemical performance of PIHCs.

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摘要

钾离子混合电容器因其优异的能量密度、令人印象深刻的功率密度和丰富的钾资源而被广泛认为是非常有前途的储能器件。不幸的是，受固有电容存储机制的限制，碳正极比电池型负极具有低得多的比容量。因此，设计高性能的碳正极对PIHCs的发展迫在眉睫。本文通过NaCl硬模板法和KOH/三聚氰胺化学活化技术制备了N，O共掺杂多孔碳(NOPC)，具有丰富的N/O含量(4.7 at%/16.9 at%)，超高的比表面积(3092 m2·g−1)和多级孔隙网络特征。设计的NOPC正极具有高比容量(0.05 A·g−1时为164.4 mAh·g−1)和出色的循环性能(2500次循环后2 A·g−1时的保持率为95.1%)。值得注意的是，微孔与介孔的可调比例有助于实现容量和倍率性能之间的最佳平衡。此外，赝电容可以通过引入N/O官能团而进一步增加。正如所料，基于石墨//NOPC的PIHC在747 W·kg−1下具有113 Wh·kg−1的高能量密度，并且在1.0 A·g−1下经过4000次循环后具有84.4%的优异容量保持率。这项工作介绍了一种新的策略来设计碳正极，以提高PIHCs的电化学性能。

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (Nos. 22179123 and 52002138), Taishan Scholar Program of Shandong Province, China (No. tsqn202211048) and the Fundamental Research Funds for the Central Universities (Nos. 202262010 and 862201013190).

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  1. School of Materials Science and Engineering, Ocean University of China, Qingdao, 266100, China

    Yan Xiong, Ya-Fei Zhang, Chun-Liu Zhu, Lei Yang, Huan-Yu Liang, Jing Shi, Jing-Wei Chen, Wei-Qian Tian, Shuai Liu, Jing-Yi Wu & Huan-Lei Wang

  2. Department of Chemical and Materials Engineering, University of Alberta, Edmonton, AB, T6G 2V4, Canada

    Zhi Li

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  1. Yan Xiong
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Xiong, Y., Zhang, YF., Zhu, CL. et al. Carbon cathode with heteroatom doping and ultrahigh surface area enabling enhanced capacitive behavior for potassium-ion hybrid capacitors. Rare Met. 43, 2136–2149 (2024). https://doi.org/10.1007/s12598-023-02597-2

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