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A ZIF-derived ZnS@Co3S4 coupled with MXene and Ni-LDH on Ni foam: constructing a honeycomb-like electrode for advanced supercapacitor

Xiang Luo, Kexin Li, Gentian Yue, Yueyue Gao, Chen Dong and Furui Tan

+ Author Affiliations

 Corresponding author: Gentian Yue, yuegentian@126.com; Furui Tan, frtan@henu.edu.cn

DOI: 10.1088/1674-4926/25060002CSTR: 32376.14.1674-4926.25060002

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Abstract: Zeolite imidazolate framework (ZIF)-derived bimetallic sulfides and layered double hydroxides (LDHs) have emerged as promising electrode materials for supercapacitors, owing to their porous layered structures, high electrochemical activity, tunable molecular architectures, low cost, and high specific capacitance. In this study, a unique composite material comprising ZIF-derived ZnCo bimetallic sulfide and LDH with a honeycomb-like structure was in situ grown on nickel foil (NF) via a controlled self-sacrificial template strategy. In contrast to previous reports, the resulting ZnS@Co3S4@MXene@Ni-LDH/NF composite integrates the advantages of MXene, LDH, and sulfides, leading to significantly enhanced conductivity, structural stability, and catalytic activity. The ZnS@Co3S4@MXene@Ni-LDH/NF electrode exhibits a uniform network structure with a thickness of approximately 1 µm coated on NF, and delivers a high specific capacitance of 1356.1 F·g−1 at a current density of 2 A·g−1. Furthermore, an asymmetric supercapacitor assembled with ZnS@Co3S4@MXene@Ni-LDH/NF as the positive electrode and activated carbon as the negative electrode achieves a high energy density of 34.08 Wh·kg−1 and a power density of 742.3 W·kg−1 at 1 A·g−1. This device successfully powers LED lights for 5 min, demonstrating its practical applicability. These results underscore the outstanding electrochemical performance of the ZnS@Co3S4@MXene@Ni-LDH/NF electrode, highlighting its potential for applications in supercapacitors and related energy storage fields.

Key words: supercapacitor, metal−organic frameworks, layered double hydroxide, ZIF, MXene



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Fig. 1.  (Color online) The synthetic route of the ZnS@Co3S4@MXene@Ni-LDH/NF sample.

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Fig. 2.  (Color online) SEM images of (a) ZnCo-ZIF-L/NF, (b) and (c) ZnCo-ZIF-L@MXene/NF, (d) ZnS@Co3S4@MXene/NF, (e) and (f) ZnS@Co3S4@MXene@Ni-LDH/NF. (g) and (m) TEM images and (h)−(l) elemental mapping images of ZnS@Co3S4@MXene@Ni-LDH/NF.

DownLoad: Full-Size Img PowerPoint
Fig. 3.  (Color online) The XRD patterns of (a) ZnCo-ZIF-L/NF, ZnCo-ZIF-L@MXene/NF, and (b) ZnS@Co3S4@MXene/NF, ZnS@Co3S4@MXene@Ni-LDH/NF; the XPS spectra of ZnS@Co3S4@MXene@Ni-LDH/NF (c) survey, (d) Co 2p, (e) Zn 2p, (f) Ti 2p, (g) S 2p, (h) Ni 2p.

DownLoad: Full-Size Img PowerPoint
Fig. 4.  (Color online) (a) The CVs and (b) GCD curves of different electrodes; (c) the CVs of the ZnS@Co3S4@MXene@Ni-LDH/NF electrode at various scan rates; (d) log-line plots of peak currents and scan rates for various electrodes; (e) and (f) capacitive contribution and diffusion-controlled contribution percentages of different electrodes; (g) and (h) the ratios of capacitive contribution and diffusion-controlled contribution at different scan rates of different electrodes; (i) EIS spectra, (j) GCD curves and (k) corresponding specific capacities of the ZnS@Co3S4@MXene@Ni-LDH/NF electrode; (l) the post-cycling SEM image of the ZnS@Co3S4@MXene@Ni-LDH/NF electrode.

DownLoad: Full-Size Img PowerPoint
Fig. 5.  (Color online). (a) The schematic diagram of device operation; (b) CV curves of the AC and ZnS@Co3S4@MXene@Ni-LDH/NF at 50 mV·s−1; (c) CV curves of the ASC device at 5−50 mV/s scan rates; (d) GCD curves of the ASC device at various current densities and (e) the corresponding specific capacitance; (f) Ragone plot; (g) cycling performance of ASC device at current density of 5 A/g and image of the LEDs lighted.

DownLoad: Full-Size Img PowerPoint
[1]
Molahalli V, Chaithrashree K, Singh M K, et al. Past decade of supercapacitor research−lessons learned for future innovations. J Energy Storage, 2023, 70, 108062 doi: 10.1016/j.est.2023.108062
[2]
Wang Y X, Zhang M, Xu T, et al. Nanocellulose-based advanced materials for flexible supercapacitor electrodes. Ind Crops Prod, 2023, 204, 117378 doi: 10.1016/j.indcrop.2023.117378
[3]
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[4]
Qiao F, Liu W J, Wang S Z, et al. Hierarchical Co3S4/CoS/MoS2 leaf-like nanoflakes array derived from Co-ZIF-L as an advanced anode for flexible supercapacitor. J Alloy Compd, 2021, 870, 159393 doi: 10.1016/j.jallcom.2021.159393
[5]
Wang W P, Wang W J, Xu Y, et al. Synthesis of Ni3S4/NiS2/FeS2 nanoparticles for hydrogen and oxygen evolution reaction. Appl Surf Sci, 2021, 560, 149985 doi: 10.1016/j.apsusc.2021.149985
[6]
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[7]
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[8]
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[9]
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[10]
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[11]
Yang Z, Cheng Q H, Li W W, et al. Construction of 2D ZIF-derived hierarchical and hollow NiCo-LDH "nanosheet-on-nanosheet" arrays on reduced graphene oxide/Ni foam for boosted electrochemical energy storage. J Alloy Compd, 2021, 850, 156864 doi: 10.1016/j.jallcom.2020.156864
[12]
da Silva M I, Machado Í R, Toma H E, et al. Recent progress in water-splitting and supercapacitor electrode materials based on MOF-derived sulfides. J Mater Chem A, 2022, 10(2), 430 doi: 10.1039/D1TA05927K
[13]
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[14]
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[15]
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[16]
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[17]
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[18]
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[19]
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[20]
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[21]
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[22]
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[23]
He Y Z, Zhang X L, Wang J M, et al. Constructing Co(OH)F nanorods@NiCo-LDH nanocages derived from ZIF-67 for high-performance supercapacitors. Adv Mater Interfaces, 2021, 8(17), 2100642 doi: 10.1002/admi.202100642
[24]
Yilmaz G, Yam K M, Zhang C, et al. In situ transformation of MOFs into layered double hydroxide embedded metal sulfides for improved electrocatalytic and supercapacitive performance. Adv Mater, 2017, 29(26), 1606814 doi: 10.1002/adma.201606814
[25]
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[26]
Wen Y Y, Rufford T E, Chen X Z, et al. Nitrogen-doped Ti3C2Tx MXene electrodes for high-performance supercapacitors. Nano Energy, 2017, 38, 368 doi: 10.1016/j.nanoen.2017.06.009
[27]
Yan J, Ren C E, Maleski K, et al. Flexible MXene/graphene films for ultrafast supercapacitors with outstanding volumetric capacitance. Adv Funct Mater, 2017, 27(30), 1701264 doi: 10.1002/adfm.201701264
[28]
Li H, Chen X, Zalnezhad E, et al. 3D hierarchical transition-metal sulfides deposited on MXene as binder-free electrode for high-performance supercapacitors. J Ind Eng Chem, 2020, 82, 309 doi: 10.1016/j.jiec.2019.10.028
[29]
Pan J, Li S B, Zhang L, et al. Reduced graphene oxide/Ni foam supported ZIF-67 derived CuCo2S4@CoS2 core-shell heterostructure for boosted electrochemical energy storage. J Energy Storage, 2022, 47, 103550 doi: 10.1016/j.est.2021.103550
[30]
Xu D D, Xue Z, Han L, et al. Interface engineered Zn/Co-S@CeO2 heterostructured nanosheet arrays as efficient electrodes for supercapacitors. J Alloy Compd, 2023, 946, 169399 doi: 10.1016/j.jallcom.2023.169399
[31]
Wang W H, Yan H W, Anand U, et al. Visualizing the conversion of metal organic framework nanoparticles into hollow layered double hydroxide nanocages. J Am Chem Soc, 2021, 143(4), 1854 doi: 10.1021/jacs.0c10285
[32]
Xie Y M, Li J Q, Cao M J, et al. Self-templated transformation of Co-ZIF-L into hierarchical porous CoS2/Co-Ni LDHs with improved electrochemical activities. J Colloid Interface Sci, 2023, 629, 786 doi: 10.1016/j.jcis.2022.08.140
[33]
Rösler C, Aijaz A, Turner S, et al. Hollow Zn/Co zeolitic imidazolate framework (ZIF) and yolk-shell metal@Zn/Co ZIF nanostructures. Chemistry, 2016, 22(10), 3304 doi: 10.1002/chem.201503619
[34]
Gu Q L, Albert Ng T C, Sun Q M, et al. Heterogeneous ZIF-L membranes with improved hydrophilicity and anti-bacterial adhesion for potential application in water treatment. RSC Adv, 2019, 9(3), 1591 doi: 10.1039/C8RA08758J
[35]
Li Y, Du Q X, Cui J, et al. Identifying the intrinsic active site in bimetallic Co3S4/Ni3S2 feathers on MXene nanosheets as a heterostructure for efficient oxygen evolution reaction. Inorg Chem Front, 2023, 10(1), 184 doi: 10.1039/D2QI01830F
[36]
Zhu X J, Dai J L, Li L G, et al. Hierarchical carbon microflowers supported defect-rich Co3S4 nanoparticles: an efficient electrocatalyst for water splitting. Carbon, 2020, 160, 133 doi: 10.1016/j.carbon.2019.12.072
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    Received: 02 June 2025 Revised: 10 September 2025 Online: Accepted Manuscript: 08 October 2025Uncorrected proof: 11 October 2025

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      Xiang Luo, Kexin Li, Gentian Yue, Yueyue Gao, Chen Dong, Furui Tan. A ZIF-derived ZnS@Co3S4 coupled with MXene and Ni-LDH on Ni foam: constructing a honeycomb-like electrode for advanced supercapacitor[J]. Journal of Semiconductors, 2025, In Press. doi: 10.1088/1674-4926/25060002 ****X Luo, K X Li, G T Yue, Y Y Gao, C Dong, and F R Tan, A ZIF-derived ZnS@Co3S4 coupled with MXene and Ni-LDH on Ni foam: constructing a honeycomb-like electrode for advanced supercapacitor[J]. J. Semicond., 2025, accepted doi: 10.1088/1674-4926/25060002
      Citation:
      Xiang Luo, Kexin Li, Gentian Yue, Yueyue Gao, Chen Dong, Furui Tan. A ZIF-derived ZnS@Co3S4 coupled with MXene and Ni-LDH on Ni foam: constructing a honeycomb-like electrode for advanced supercapacitor[J]. Journal of Semiconductors, 2025, In Press. doi: 10.1088/1674-4926/25060002 ****
      X Luo, K X Li, G T Yue, Y Y Gao, C Dong, and F R Tan, A ZIF-derived ZnS@Co3S4 coupled with MXene and Ni-LDH on Ni foam: constructing a honeycomb-like electrode for advanced supercapacitor[J]. J. Semicond., 2025, accepted doi: 10.1088/1674-4926/25060002
      shu

      A ZIF-derived ZnS@Co3S4 coupled with MXene and Ni-LDH on Ni foam: constructing a honeycomb-like electrode for advanced supercapacitor

      DOI: 10.1088/1674-4926/25060002
      CSTR: 32376.14.1674-4926.25060002

      • Henan Key Laboratory of Quantum Materials and Quantum Energy, School of Quantum Information Future Technology, Henan University, Kaifeng 475004, China

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      • Xiang Luo received his BS degree in 2022 after graduating from Henan Normal University. Now he is a master's student at Henan University. Since September 2022, he has been working in Prof. Furui Tan's research group under the supervision of Associate Professor Gentian Yue. He current research focuses on DSSC and supercapacitors
      • Kexin Li received her BS degree in 2021 after graduating from Zhengzhou Normal University. Now she is a master's student at Henan University. Since September 2021, she has been working in Prof. Furui Tan's research group under the supervision of Associate Professor Gentian Yue. Her current research focuses on supercapacitors
      • Gentian Yue received his Ph.D. degree from Huaqiao University, China in 2013. Since then, he has been working as a full time associate professor at Henan Key Laboratory of Photo voltaic Materials, Henan University, China. His research interests include material synthesis and device fabrication of dye sensitized solar cells, supercapacitor, and energy capture and storage devices for wearable electronics
      • Yueyue Gao received his master’s degree in Chemical Engineering and Technology from Qiqihar University, China in 2014. And he received his Ph.D. degree from School of Chemistry and Chemical Engineering, Harbin Institute of Technology (HIT), China in 2018. Since then, he joined Henan Key Laboratory of Photovoltaic Materials, Henan University, China in 2018. His research interest mainly focuses on the design, synthesis and performance study of furan-based organic photovoltaic materials
      • Chen Dong received his Ph.D. degree from Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences (CAS), under the supervision of Prof. Xiuxun Han and Prof. Jinqing Wang. Since then, he joined Henan Key Laboratory of Photovoltaic Materials, Henan University, China in 2019. His research interest is all-inorganic perovskite solar cells
      • Furui Tan is currently an professor in the Henan Key Laboratory of Photovoltaic Materials, Henan University, China. He received his Ph.D. degree from Institute of Semiconductors, Chinese Academy of Sciences (ISCAS) in 2011. He joined the Sargent group in the Department of Electronics and Computer Engineering (ECE) in the University of Toronto, as a visiting scholar in June 2017 and June 2018. His research group focuses on organic and nanoscale materials for solar cells, photodetectors, and electro-catalysis, etc
      • Corresponding author: yuegentian@126.com; frtan@henu.edu.cn
      • Received Date: 2025-06-02
      • Revised Date: 2025-09-10
        • Available Online: 2025-10-08

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