NiCoSe2/Ni3Se2 lamella arrays grown on N-doped graphene nanotubes with ultrahigh-rate capability and long-term cycling for asymmetric supercapacitor

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  • ReceivedJul 18, 2019
  • AcceptedAug 19, 2019
  • PublishedSep 20, 2019


In this paper, we report a one-step electrodeposited synthesis strategy for directly growing NiCoSe2/Ni3Se2 lamella arrays (LAs) on N-doped graphene nanotubes (N-GNTs) as advanced free-standing positive electrode for asymmetric supercapacitors. Benefiting from the synergetic contribution between the distinctive electroactive materials and the skeletons, the as-constructed N-GNTs@NiCoSe2/Ni3-Se2 LAs present a specific capacitance of ~1308 F g−1 at a current density of 1 A g−1. More importantly, the hybrid electrode also reveals excellent rate capability (~1000 F g−1 even at 100 A g−1) and appealing cycling performance (~103.2% of capacitance retention over 10,000 cycles). Furthermore, an asymmetric supercapacitor is fabricated by using the obtained N-GNTs@NiCoSe2/Ni3Se2 LAs and active carbon (AC) as the positive and negative electrodes respectively, which holds a high energy density of 42.8 W h kg−1 at 2.6 kW kg−1, and superior cycling stability of ~94.4% retention over 10,000 cycles. Accordingly, our fabrication technique and new insight herein can both widen design strategy of multicomponent composite electrode materials and promote the practical applications of the latest emerging transition metal selenides in next-generation high-performance supercapacitors.

Funded by

The work was supported by the National Natural Science Foundation of China(51672144,51572137,51702181)

the Natural Science Foundation of Shandong Province(ZR2017BB013,ZR2019BEM042)

Higher Educational Science and Technology Program of Shandong Province(J17KA014,J18KA001,J18KA033)

Taishan Scholars Program of Shandong Province(ts201511034)

and Overseas Taishan Scholars Program.


The work was supported by the National Natural Science Foundation of China (51672144, 51572137 and 51702181), the Natural Science Foundation of Shandong Province (ZR2017BB013 and ZR2019BEM042), Higher Educational Science and Technology Program of Shandong Province (J17KA014, J18KA001 and J18KA033), Taishan Scholars Program of Shandong Province (ts201511034), and Overseas Taishan Scholars Program.

Interest statement

The authors declare no conflict of interest.

Contributions statement

Meng A, Zhao J and Li Z designed the project and the experiments. Shen T and Huang T performed the experiments. Song G and Tan S performed the products characterizations. Meng A wrote the paper with support from Zhao J and Li Z. All authors contributed to the general discussion.

Author information

Alan Meng is a professor in the College of Chemistry and Molecular Engineering at Qingdao University of Science & Technology. Her main research interest is on the development of new electrode nanomaterials for energy storage devices including supercapacitors and batteries.

Jian Zhao received his PhD degree from Qingdao University of Science & Technology in 2017. His research interests include the synthesis, characterization, electrochemical performances and mechanism of electrode materials for supercapacitors.


Supplementary information

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


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  • Figure 1

    Schematic diagram of the fabrication of N-GNTs@NiCoSe2/Ni3Se2 NSs electrode materials.

  • Figure 2

    SEM images (a, b) and TEM image (c) of the N-GNTs. The inset in (b) is the corresponding EDS spectrum, and the inset in (c) depicts the HRTEM plot. Low-magnification (d) and high-magnification (e) SEM images of N-GNTs@Ni-Co-Se-M, and the corresponding elemental mapping images (f–i) of Ni, Co, Se and C; TEM images (j, k) and HRTEM image (l) of the sample.

  • Figure 3

    XRD pattern (a), and XPS high-resolution spectra of Ni 2p (b), Co 2p (c) and Se 3d (d) of the N-GNTs@Ni-Co-Se-M.

  • Figure 4

    Comparative CV (a) and GCD (b) curves of these obtained electrodes at 20 mV s−1 and 1 A g−1 respectively. CV curves (c) of the N-GNTs@Ni-Co-Se-M electrode at different scan rates. GCD curves (d) of the N-GNTs@Ni-Co-Se-M electrode at various current densities. (e) Specific capacity versus current densities. EIS profiles (f) of these obtained electrodes. Cycling property (g) of these obtained electrodes at 20 A g−1 for 10,000 cycles.

  • Figure 5

    (a) A schematic diagram of the device assembly. (b) CV curves of N-GNTs@Ni-Co-Se-M and AC at 20 mV s−1. (c) CV curves of various voltage windows. (d) CV plots at different scan rates. (e) GCD plots at different current densities of the ASC device. (f) Specific capacitance and voltage drop vs. current densities of the ASC device.

  • Figure 6

    (a) Ragone profile (energy density vs. power density) of the assembled ASC device, and the comparison of the energy density between this work and the previous published reports. (b) Optical photograph of two ASC devices connected in series to power various electronic devices. (c) Cycling stability and corresponding coulombic efficiency of the ASC device. The inset displaying the first and last 20 cycles.

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