Tuning the interlayer spacing of graphene laminate films for efficient pore utilization towards compact capacitive energy storage


Supercapacitors have shown extraordinary promise for miniaturized electronics and electric vehicles, but are usually limited by electrodes with rather low volumetric performance, which is largely due to the inefficient utilization of pores in charge storage. Herein, we design a freestanding graphene laminate film electrode with highly efficient pore utilization for compact capacitive energy storage. The interlayer spacing of this film can be precisely adjusted, which enables a tunable porosity. By systematically tailoring the pore size for the electrolyte ions, pores are utilized optimally and thereby the volumetric capacitance is maximized. Consequently, the fabricated supercapacitor delivers a stack volumetric energy density of 88.1 Wh l−1 in an ionic liquid electrolyte, representing a critical breakthrough for optimizing the porosity towards compact energy storage. Moreover, the optimized film electrode is assembled into an ionogel-based, all-solid-state, flexible smart device with multiple optional outputs and superior stability, demonstrating enormous potential as a portable power supply in practical applications.

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Fig. 1: Preparation of the EGM-GO films with tunable interlayer spacing.
Fig. 2: Structural characterization of EGM-rGO films.
Fig. 3: Electrochemical characterization of EGM-rGO films-based supercapacitors in EMIMBF4.
Fig. 4: Optimizing the device performance towards compact EES.
Fig. 5: Fabrication of ASSC with high-voltage ionogel electrolyte.

Data availability

All data generated or analysed during the current study are included in this published article (and its Supplementary Information file). Additional datasets related to this study are available from the corresponding author on reasonable request.

Change history

  • 16 March 2020

    An amendment to this paper has been published and can be accessed via a link at the top of the paper.


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This work was supported by the National Science Foundation of China (grant nos. 51525206, 51521091 and 51372253), the Ministry of Science and Technology of China (grant nos. 2016YFA0200100 and 2016YFB0100100), the Strategic Priority Research Programme of Chinese Academy of Science (grant no. XDA22010602), the Key Research Programme of the Chinese Academy of Sciences (grant no. KGZD-EW-T06) and the EPSRC (grant nos. EP/R020973/1, EP/P009050/1, EP/L018330/1, EP/K002252/1 and EP/M009394/1). P.R.S. would like to acknowledge financial support from the Royal Academy of Engineering.

Author information




Z.L., S.G. and F.L. conceived and designed the research. Z.L., S.G. and H.L. performed the experiments and the characterization of the materials. Z.L., S.G., C.A.H., I.P.P. and F.L. analysed the data. S.G., C.A.H., D.J.L.B., P.R.S. and Z.G. contributed to the discussion of the results. Z.L., I.P.P. and F.L. wrote the manuscript. All the authors commented on and revised the manuscript.

Corresponding authors

Correspondence to Zhengxiao Guo or Ivan P. Parkin or Feng Li.

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Supplementary Information

Supplementary Figs. 1–17, Notes 1 and 2, Table 1 and refs. 1–16.

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Li, Z., Gadipelli, S., Li, H. et al. Tuning the interlayer spacing of graphene laminate films for efficient pore utilization towards compact capacitive energy storage. Nat Energy 5, 160–168 (2020). https://doi.org/10.1038/s41560-020-0560-6

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