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Research Article | Online first | Published: 13 April 2024

Entropy-modulated and interlayer-doped transition metal layered oxides enable high-energy-density sodium-ion capacitors

Show Author's Information Tiansheng Wang1,§,  Yadong Li1,§,  Zhengyuan Chen1,  Qingshan Liu1,  Jian Lang1,  Langyuan Wu2,  Wendi Dong2,  Zhengyu Ju3,  Hongsen Li1( ),  Xiaogang Zhang2,  Guihua Yu3( )
College of Physics, Qingdao University, Qingdao 266071, China
Jiangsu Key Laboratory of Materials and Technologies for Energy Storage, College of Materials Science and Technology, Nanjing University of Aeronautics and Astronautics, Nanjing 210016, China
Materials Science and Engineering Program and Walker Department of Mechanical Engineering, The University of Texas at Austin, Austin 78712, USA

§ Tiansheng Wang and Yadong Li contributed equally to this work.

Keywords:
high power density, long-term cycling, layered oxide, sodium-ion capacitors, entropy modulation
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Energy storage
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Wang T, Li Y, Chen Z, et al. Entropy-modulated and interlayer-doped transition metal layered oxides enable high-energy-density sodium-ion capacitors. Nano Research, 2024, https://doi.org/10.1007/s12274-024-6640-3
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Abstract Full text Electronic supplementary material About this article

In recent years, sodium-ion capacitors have attracted attention due to their cost-effectiveness, high power density and similar manufacturing process to lithium-ion capacitors. However, the utilization of oxide electrodes in traditional sodium-ion capacitors restricts their further advancement due to the inherent low operating voltage and electrolyte consumption based on their energy storage mechanism. To address these challenges, we incorporated Zn, Cu, Ti, and other elements into Na0.67Ni0.33Mn0.67O2 to synthesize P2-type Na0.7Ni0.28Mn0.6Zn0.05Cu0.02Ti0.05O2 with a modulated entropy and pillaring Zn. Through the synergistic interplay between the interlayer pillar and the entropy modulation within the layers, the material exhibits exceptional toughness, effectively shielding it from detrimental phase transitions at elevated voltage regimes. As a result, the material showcases outstanding kinetic properties and long-term cycling stability across the voltage range. By integrating these materials with hierarchical porous carbon nanospheres to form a "rocking chair" sodium-ion capacitor, the hybrid full device delivers a high energy density (171 Wh·kg−1) and high power density (5245 W·kg−1), as well as outstanding cycling stability (77% capacity retention after 3000 cycles). This work provides an effective material development route to realize simultaneously high energy and power for next-generation sodium-ion capacitors.


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Electronic supplementary material
About this article

Entropy-modulated and interlayer-doped transition metal layered oxides enable high-energy-density sodium-ion capacitors

Show Author's information Tiansheng Wang1,§, Yadong Li1,§, Zhengyuan Chen1, Qingshan Liu1, Jian Lang1, Langyuan Wu2, Wendi Dong2, Zhengyu Ju3, Hongsen Li1( ), Xiaogang Zhang2, Guihua Yu3( )
College of Physics, Qingdao University, Qingdao 266071, China
Jiangsu Key Laboratory of Materials and Technologies for Energy Storage, College of Materials Science and Technology, Nanjing University of Aeronautics and Astronautics, Nanjing 210016, China
Materials Science and Engineering Program and Walker Department of Mechanical Engineering, The University of Texas at Austin, Austin 78712, USA

§ Tiansheng Wang and Yadong Li contributed equally to this work.

Abstract

In recent years, sodium-ion capacitors have attracted attention due to their cost-effectiveness, high power density and similar manufacturing process to lithium-ion capacitors. However, the utilization of oxide electrodes in traditional sodium-ion capacitors restricts their further advancement due to the inherent low operating voltage and electrolyte consumption based on their energy storage mechanism. To address these challenges, we incorporated Zn, Cu, Ti, and other elements into Na0.67Ni0.33Mn0.67O2 to synthesize P2-type Na0.7Ni0.28Mn0.6Zn0.05Cu0.02Ti0.05O2 with a modulated entropy and pillaring Zn. Through the synergistic interplay between the interlayer pillar and the entropy modulation within the layers, the material exhibits exceptional toughness, effectively shielding it from detrimental phase transitions at elevated voltage regimes. As a result, the material showcases outstanding kinetic properties and long-term cycling stability across the voltage range. By integrating these materials with hierarchical porous carbon nanospheres to form a "rocking chair" sodium-ion capacitor, the hybrid full device delivers a high energy density (171 Wh·kg−1) and high power density (5245 W·kg−1), as well as outstanding cycling stability (77% capacity retention after 3000 cycles). This work provides an effective material development route to realize simultaneously high energy and power for next-generation sodium-ion capacitors.

Keywords: high power density, long-term cycling, layered oxide, sodium-ion capacitors, entropy modulation

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Received: 20 February 2024
Revised: 19 March 2024
Accepted: 19 March 2024
Published: 13 April 2024

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© Tsinghua University Press 2024

Acknowledgements

Acknowledgements

H. S. L. acknowledges the support from Taishan Scholar Program of Shandong Province (No. tsqn202211118), Excellent Youth Science Fund Project of Shandong China (No. ZR2023YQ008), Outstanding Youth Innovation Team of Universities in Shandong Province (No. 2021KJ020), and the National Natural Science Foundation of China (No. 51804173). G. H. Y. acknowledges the funding support from the Welch Foundation Award F-1861.

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