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Iron doping of NiSe2 nanosheets to accelerate reaction kinetics in sodium-ion half/full batteries

电子堆积工程调控二硒化镍纳米片助力具有快速动力学的钠离子电池

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Abstract

Transition metal selenides are important functional materials owing to their large sodium storage capacity. When used as the anode material of sodium-ion batteries (SIBs), the selenides undergo large volume changes during the (de)embedding process, resulting in electrode pulverization followed by rapid capacity decay. The poor conductivity of metal selenides further limits their rate capacity. In this work, Fe-doped NiSe2@C (Fe−NiSe2@C) nanosheets (NSs) with a porous structure were prepared through two-dimensional binary metal-organic framework templating and subsequent in situ selenization. The NSs exhibited an enhanced electronic transportation structure with a hierarchical porous architecture and fully exposed electrochemically active sites. Moreover, compared with NiSe2, the Fe−NiSe2@C NSs exhibited higher capacity (406 mA h g−1 at 1 A g−1 after 100 cycles), better cycle stability (99% capacity retention after 1000 cycles), and higher rate performance, attributed to the optimized stable porous structure and improved Na+ mobility. Furthermore, a high energy density of 107 W h kg−1 in sodium-ion full batteries was achieved. The storage mechanism of Na+ in Fe−NiSe2@C NSs was confirmed through theoretical calculations and a series of ex-situ characterizations. This study provides a reasonable design for improving metal selenides in SIBs.

摘要

近年来, 钠离子电池电极材料引起了研究者们极大的兴趣. 过渡金属硒化物具有高钠离子存储容量, 是一种具有前景的钠离子电池负极材料. 然而, 该类材料较低的电导率以及钠离子脱嵌过程中巨大的体积膨胀, 导致了其较差的钠离子电池倍率性能和循环寿命. 本工作采用二维的双金属有机框架材料为模板, 设计制造了多孔铁掺杂NiSe2纳米片材料(Fe−NiSe2@C NSs), 该结构具有充分暴露的活性位点, 增强的电导率, 丰富的空隙和短电子传输路径, 易于适应钠离子脱嵌带来的体积膨胀应力, 并具有快速的电荷转移动力学. 作为钠离子电池负极材料时, Fe−NiSe2@C NSs表现出高比容量(5 A g−1电流密度下为302 mA h g−1)和优异的循环稳定性(5 A g−1的电流密度下循环1000圈容量保持率为99%). 此外, 该材料在与Na3V2(PO4)2O2F正极材料组成的钠离子全电池中也表现出了高能量密度(107 W h kg−1). 大量非原位表征和理论计算进一步验证了Fe掺杂使电子密度增大, 对于提升Fe−NiSe2@C NSs的钠离子电池综合性能具有重要意义. 本研究为制备高性能钠离子电池电极材料提供了新思路.

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (51801030), the Science and Technology Development Plan of Suzhou (ZXL2021176), China Postdoctoral Science Foundation (2022M711686) and Jiangsu Provincial Funds for the Young Scholars (BK20190978).

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  1. These authors contributed equally to this paper.

Authors and Affiliations

  1. School of Electronic and Information Engineering, Changshu Institute of Technology, Changshu, 215500, China

    Jing Liu  (刘静), Chencheng Sun  (孙陈诚) & Hongbo Geng  (耿洪波)

  2. School of Material Science & Engineering, Jiangsu University of Science and Technology, Zhenjiang, 212003, China

    Jun Yang  (杨骏)

  3. School of Materials Engineering, Changshu Institute of Technology, Changshu, 215500, China

    Jing Liu  (刘静), Juan Xie  (谢娟), Huilong Dong  (董慧龙) & Hongbo Geng  (耿洪波)

  4. School of Chemistry and Life Sciences, Suzhou University of Science and Technology, Suzhou, 215009, China

    Huaixin Wei  (魏怀鑫)

  5. School of Materials Science and Engineering, Jiangsu University, Zhenjiang, 212013, China

    Juan Xie  (谢娟)

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  1. Jing Liu  (刘静)
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Contributions

Liu J performed the experiments, characterized the samples, analyzed the data and wrote the original draft. Xie J and Dong H conducted the DFT calculation. Wei H participated in the investigation and revised the paper. Yang J and Sun C conducted the conceptualization and revised the paper. Geng H provided the resources and revised the paper. All authors contributed to the general discussion.

Corresponding authors

Correspondence to Chencheng Sun  (孙陈诚), Jun Yang  (杨骏) or Hongbo Geng  (耿洪波).

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Conflict of interest

The authors declare that they have no conflict of interest.

Supplementary information

Supporting data are available in the online version of the paper.

Jun Yang received his PhD degree from Nanjing Tech University in 2018. He is now working as a lecturer at Jiangsu University of Science and Technology. His research focuses on functional materials for energy-related applications.

Chencheng Sun is currently working as an assistant professor at Changshu Institute of Technology. He obtained his PhD degree from Nanjing Tech University in 2016. His research mainly focuses on the design and fabrication of energy storage materials and devices, such as metal chalcogenides, flexible supercapacitors and lithium/sodium-ion batteries.

Hongbo Geng received his PhD degree from Soochow University in 2017. He is now working as a full professor at Changshu Institute of Technology. His current research interests focus on functional nanomaterials for electrochemical storage.

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Liu, J., Xie, J., Dong, H. et al. Iron doping of NiSe2 nanosheets to accelerate reaction kinetics in sodium-ion half/full batteries. Sci. China Mater. 66, 69–78 (2023). https://doi.org/10.1007/s40843-022-2139-3

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