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One-step architecture of bifunctional petal-like oxygen-deficient NiAl-LDHs nanosheets for high-performance hybrid supercapacitors and urea oxidation

一步法构筑双功能富含氧空位的花瓣状镍铝水滑石纳米薄片用于高性能超级电容器和尿素氧化

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Abstract

Nickel-based layered double hydroxides (LDHs) are promising electrode materials in the fields of energy storage (supercapacitors) and conversion (urea oxidation). The rational construction of atomic and electronic structure is crucial for nickel-based LDHs to realize their satisfactory electrochemical performance. Herein, we report a facile, ecofriendly, one-step synthesis process to construct petal-like oxygen-deficient NiAl-LDH nanosheets for hybrid super-capacitors (HSCs) and urea oxidation reaction (UOR). The asprepared NiAl−LDH nanosheets with rich oxygen vacancies possess a large specific surface area of 216.6 m2 g−1 and a desirable electronic conductivity of 3.45 × 10−4 S cm−1 to deliver an ultra-high specific capacitance of 2801 F g−1 (700 C g−1) at 1 A g−1. Furthermore, high specific energy of 50.0 W h kg−1 at 400 W kg−1 and excellent cycle stability with 91% capacitance retention after 10,000 cycles are achieved by the NiAl-LDHs/CFP (carbon fiber paper) (+)//YP-80F (a commercial activated carbon) (−) HSC. Besides, NiAl−LDH nanosheets also work as an efficient electrocatalyst for UOR, which only requires 1.42 V vs. reversible hydrogen electrode to drive 10 mA cm−2 in 1 mol L−1 KOH with 0.33 mol L−1 urea. This remarkable performance is superior to most reported values of previous candidates owing to the thin structure of NiAl−LDH nanosheets for exposing more active sites and abundant oxygen vacancies. In addition, various reaction parameters are investigated to optimize the electrochemical performance. In general, this work paves a new way for the architecture of multifunctional nanostructured energy materials.

摘要

镍基水滑石在能量存储(超级电容器)和转化(尿素氧化)领域是很有前景的电极材料. 合理构建镍基水滑石的原子和电子结构对于实现其理想的电化学性能至关重要. 本论文报道了一种简单、 环境友好的一步法制备富含氧空位的花瓣状镍铝水滑石(NiAl-LDHs)纳米薄片用于混合超级电容器和尿素氧化. 性能最好的富氧空位NiAl-LDHs纳米薄片具有216.6 m2 g−1的大比表面积和3.45 × 10−4 S cm−1的高电导率, 可在1 A g−1的比电流下展示出2801 F g−1(700 C g−1)的超高比电容. 基于NiAl-LDHs//商业活性炭组装的混合超级电容器在400 W kg−1比功率密度下可获得50.0 W h kg−1的比能量, 且循环10,000次后仍有91%的电容保持率. 同时, NiAl-LDHs纳米薄片作为高效的尿素氧化电催化剂, 在1 mol L−1 KOH和0.33 mol L−1尿素中仅需1.42 V vs.可逆氢电极的氧化电位就可达到10 mA cm−2的电流密度. 由于NiAl-LDHs的纳米薄片结构暴露了更多的活性位点和丰富的氧空位, 其电化学性能优于大部分报道的镍基水滑石. 因此, 本研究为多功能纳米能源材料的合理设计奠定了良好的基础.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (21776324 and 22078374), Guangdong Basic and Applied Basic Research Foundation (2019B1515120058 and 2020A1515011149), National Ten Thousand Talent Plan, National Key R&D Program of China (2018YFD0800703 and 2020YFC1807600), Key-Area Research and Development Program of Guangdong Province (2019B110209003), the Fundamental Research Funds for the Central Universities (19lgzd25), and the Hundred Talent Plan (201602) from Sun Yatsen University.

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Authors and Affiliations

  1. Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology, School of Environmental Science and Engineering, Sun Yat-sen University, Guangzhou, 510275, China

    Yuchen Wang  (王宇辰), Yaoyu Liu  (刘瑶钰), Man Zhang  (张曼), Biying Liu  (刘碧莹), Zhiyue Zhao  (赵志月) & Kai Yan  (严凯)

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  1. Yuchen Wang  (王宇辰)
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  2. Yaoyu Liu  (刘瑶钰)
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  3. Man Zhang  (张曼)
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  4. Biying Liu  (刘碧莹)
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  5. Zhiyue Zhao  (赵志月)
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  6. Kai Yan  (严凯)
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Contributions

Author contributions Yan K conceived the idea of this study and revised the paper; Wang Y and Liu Y conducted the experiments and performed the data analysis; Zhang M, Liu B and Zhao Z participated in literature search and manuscript preparation; Wang Y wrote the manuscript. All authors contributed to the general discussion.

Corresponding author

Correspondence to Kai Yan  (严凯).

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Conflict of interest The authors declare no conflict of interest.

Additional information

Yuchen Wang received his PhD degree in mechanical engineering from the University of Miami in 2017. He is currently a postdoc research associate at the School of Environmental Science and Engineering, Sun Yat-sen University. His present research interests focus on nanomaterials in energy storage and conversion applications.

Kai Yan is a full professor at the School of Environmental Science and Engineering, Sun Yat-sen University. He received his PhD degree from Max-Planck-Institute for Coal Research and RWTH Aachen University in 2011. Then he obtained an Ontario Government Postdoctoral Fellowship at Lakehead University (2012–2013) and joined Brown University as a senior postdoctoral research associate (2013–2016). His current interests include the synthesis of nanostructured materials for clean energy and environment-related applications.

Supplementary information Experimental details and supporting data are available in the online version of the paper.

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40843_2021_1978_MOESM1_ESM.pdf

One-step architecture of bifunctional petal-like oxygen-deficient NiAl-LDHs nanosheets for high-performance hybrid supercapacitors and urea oxidation

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Wang, Y., Liu, Y., Zhang, M. et al. One-step architecture of bifunctional petal-like oxygen-deficient NiAl-LDHs nanosheets for high-performance hybrid supercapacitors and urea oxidation. Sci. China Mater. 65, 1805–1813 (2022). https://doi.org/10.1007/s40843-021-1978-3

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