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Phosphorous-doped bimetallic sulfides embedded in heteroatom-doped carbon nanoarrays for flexible all-solid-state supercapacitors

嵌入多原子掺杂碳纳米阵列中的磷掺杂双金属硫化物应用于柔性全固态超级电容器

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Abstract

Flexible supercapacitors (SCs) have become a popular research topic due to their extra-long service life, foldability, and wearability. Nevertheless, their low energy density restricts their applications. Here, we synthesized phosphorus-doped bimetallic sulfides embedded in heteroatom-doped (N, S, and P) carbon shells (P-ZCS/HC) using a simple approach to create high-performance flexible electrodes. The three-dimensional architecture made by interlaced nanosheets was preserved, and raised nanoparticles appeared on the rough surface during the annealing operation, increasing the specific surface area and potential exposure to the electrolyte. It is noteworthy that the optimal P-ZCS/HC electrode possessed a remarkable capacity of 1080 C g−1 at 1 A g−1 along with superb cycling stability. These extraordinary properties were primarily caused by plentiful redox reactions, enhanced conductivity, and synergic effects of the P-doped metal sulfides and heteroatom-doped carbon shells. Density functional theory simulations confirmed the good function of the P-doped electrodes and their ability to boost conductivity, improve reactive dynamics, and promote OH− adsorption. Notably, the assembled all-solid-state hybrid SC exhibited a maximum energy density of 62.9 W h kg−1 and a power density of 16 kW kg−1, while being able to maintain 92.0% of its initial capacity after 10,000 cycles. This systematic report provides new insight into the design and synthesis of electrodes with complex components and outstanding structures for the flexible energy field.

摘要

柔性超级电容器具有超长使用寿命、可折叠、可穿戴等特点, 已成为研究热点. 然而, 较低的能量密度限制了其更广泛的应用. 本文采用简单的方法合成了一种嵌入多原子(氮, 硫和磷原子)掺杂碳壳的磷掺杂双金属硫化物(P-ZCS/HC)作为高性能柔性电极. 在退火过程中, 前驱体的三维形貌保持不变, 同时纳米片表面有凸起的纳米球形颗粒形成, 这大大增加了电极的比表面积. 优化后的P-ZCS/HC电极在1 A g−1时具有1080 C g−1高比电容值, 且循环稳定性出色. 这些优异的性能主要是由于该电极材料可发生丰富的氧化还原反应, 磷化后增强的导电性, 以及磷掺杂金属硫化物和多原子掺杂碳壳之间的协同效应. 密度泛函理论模拟表明, 磷掺杂处理具有提高电导率、改善反应动力学和促进OH−吸附的积极作用.组装的全固态柔性混合超级电容器最高能量密度可达62.9 W h kg−1, 功率密度可达16 kW kg−1, 循环10,000次后仍能保持初始容量的92.0%. 这一完整和系统的研究为将来设计具有复杂成分和优异结构的柔性电极提供了一种新的思路.

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Acknowledgements

This work was supported by research projects from the Department of Science and Technology of Shandong Province (2018JMRH0211, ZR2019MEM052, 2019TSLH0101 and ZR2018ZB0105), and the Fundamental Research Funds of Shandong University (2017JC042 and 2017JC010). Jun Lou was supported by a Welch Foundation grant (C-1716).

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Authors and Affiliations

  1. Key Laboratory for Liquid-Solid Structural Evolution and Processing of Materials (Ministry of Education), Research Center for Carbon Nanomaterials, School of Materials Science and Engineering, Shandong University, Jinan, 250061, China

    Shuo Li  (李硕), Minghao Hua  (华明昊), Yuan Yang  (杨媛), Xiaowen Zheng  (郑小雯), Pengchao Si  (司鹏超) & Lijie Ci  (慈立杰)

  2. Department of Chemistry, Technical University of Denmark, DK-2800, Kongens Lyngby, Denmark

    Wei Huang  (黄卫)

  3. Department of Materials Science and NanoEngineering, Rice University, Houston, TX, 77005, USA

    Jun Lou  (楼峻)

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  1. Shuo Li  (李硕)
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  2. Minghao Hua  (华明昊)
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  6. Pengchao Si  (司鹏超)
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  8. Jun Lou  (楼峻)
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Contributions

Li S and Si P designed the project and wrote the paper; Li S carried out most of the experiments; Hua M performed the DFT simulations; Yang Y helped with the data processing; Zheng X conducted the Raman tests; Huang W conducted the TEM and XPS measurements; Si P, Ci L and Lou J provided constructive suggestions. All authors contributed to the general discussion.

Corresponding author

Correspondence to Pengchao Si  (司鹏超).

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Conflict of interest

The authors declare that they have no conflict of interest.

Shuo Li obtained her Bachelor degree in 2016 from the School of Materials Science and Engineering, Shandong University. She is currently a PhD student under the supervision of Prof. Pengchao Si at Shandong University. Her present research interests mostly concentrate on the transition metal sulfides and phosphides for energy storage applications.

Pengchao Si received his PhD degree in 2007 in natural science from Roskilde University, Denmark. Then he worked as a postdoctoral research fellow in the Department of Chemistry, Curtin University. He has been a full professor at the School of Materials Science and Engineering, Shandong University since 2010. His present research interests are mainly on the synthesis of nanomaterials for energy storage, conversion and electrochemical sensors.

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Phosphorous-doped bimetallic sulfides embedded in heteroatom-doped carbon nanoarrays for flexible all-solid-state supercapacitors

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Li, S., Hua, M., Yang, Y. et al. Phosphorous-doped bimetallic sulfides embedded in heteroatom-doped carbon nanoarrays for flexible all-solid-state supercapacitors. Sci. China Mater. 64, 2439–2453 (2021). https://doi.org/10.1007/s40843-020-1667-1

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