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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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.
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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.
The authors declare no competing interests.
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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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