Stretchable supercapacitors (SCs) have attracted significant attention in developing power‐independent stretchable electronic systems due to their intrinsic energy storage function and unique mechanical properties. Most current SCs are generally limited by their low stretchability, complicated fabrication process, and insufficient performance and robustness. This study presents a facile method to fabricate arbitrary‐shaped stretchable electrodes via 4D printing of conductive composite from reduced graphene oxide, carbon nanotube, and poly(3,4‐ethylenedioxythiophene) polystyrene sulfonate. The electrode patterns of an arbitrary shape can be deposited onto prestretched substrates by aerosol‐jet printing, then self‐organized origami (ridge) patterns are generated after releasing the substrates from holding stretchers due to the mismatched strains. The stretchable electrodes demonstrate superior mechanical robustness and stretchability without sacrificing its outstanding electrochemical performance. The symmetric SC prototype possesses a gravimetric capacitance of ≈21.7 F g−1at a current density of 0.5 A g−1and a capacitance retention of ≈85.8% from 0.5 to 5 A g−1. A SC array with arbitrary‐shaped electrodes is also fabricated and connected in series to power light‐emitting diode patterns for large‐scale applications. The proposed method paves avenues for scalable manufacturing of future energy‐storage devices with controlled extensibility and high electrochemical performance.
Formation of thick, high energy density, flexible solid supercapacitors is challenging because of difficulties infilling gel electrolytes into porous electrodes. Incomplete infilling results in a low capacitance and poor mechanical properties. Here we report a bottom-up infilling method to overcome these challenges. Electrodes up to 500 μm thick, formed from multi-walled carbon nanotubes and a composite of poly(3,4-ethylenedioxythiophene), polystyrene sulfonate and multi-walled carbon nanotubes are successfully infilled with a polyvinyl alcohol/phosphoric acid gel electrolyte. The exceptional mechanical properties of the multi-walled carbon nanotube-based electrode enable it to be rolled into a radius of curvature as small as 0.5 mm without cracking and retain 95% of its initial capacitance after 5000 bending cycles. The areal capacitance of our 500 μm thick poly(3,4-ethylenedioxythiophene), polystyrene sulfonate, multi-walled carbon nanotube-based flexible solid supercapacitor is 2662 mF cm–2at 2 mV s–1, at least five times greater than current flexible supercapacitors.
more » « less- NSF-PAR ID:
- 10154313
- Publisher / Repository:
- Nature Publishing Group
- Date Published:
- Journal Name:
- Nature Communications
- Volume:
- 9
- Issue:
- 1
- ISSN:
- 2041-1723
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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