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A Self-Healing Crease-Free Supramolecular All-Polymer Supercapacitor.

ABSTRACT: While traditional three-layer structure supercapacitors are under mechanical manipulations, the high-stress region concentrates, inevitably causing persistent structural problems including interlayer slippage, crease formation, and delamination of the electrode-electrolyte interface. Toward this, an all-polymeric, all-elastic and non-laminated supercapacitor with high mechanical reliability and excellent electrochemical performance is developed. Specifically, a polypyrrole electrode layer is in situ integrated into a silk fibroin-based elastic supramolecular hydrogel film with extensive hydrogen and covalent bonds, where a non-laminate device is realized with structural elasticity at the device level. The non-laminate configuration can avoid slippage and delamination, while the elasticity can preclude crease formation. Furthermore, under more severe mechanical damage, the supercapacitors can restore the electrochemical performance through non-autonomous self-healing capabilities, where the supramolecular design of host-guest interactions in the hydrogel matrix results in a superior self-healing efficiency approaching ≈95.8% even after 30 cutting/healing cycles. The all-elastic supercapacitor delivers an areal capacitance of 0.37 F cm^-2 and a volumetric energy density of 0.082 mW h cm^-3, which can well-maintain the specific capacitance even at -20 °C with over 85.2% retention after five cut/healing cycles.

SUBMITTER: Mo F

PROVIDER: S-EPMC8224449 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:The formation of condensed matter typically involves a trade-off between structural order and flexibility. As the extent and directionality of interactions between atomic or molecular components increase, materials generally become more ordered but less compliant, and vice versa. Nevertheless, high levels of structural order and flexibility are not necessarily mutually exclusive; there are many biological (such as microtubules1,2, flagella 3 , viruses4,5) and synthetic assemblies (for example, dynamic molecular crystals6-9 and frameworks10-13) that can undergo considerable structural transformations without losing their crystalline order and that have remarkable mechanical properties8,14,15 that are useful in diverse applications, such as selective sorption 16 , separation 17 , sensing 18 and mechanoactuation 19 . However, the extent of structural changes and the elasticity of such flexible crystals are constrained by the necessity to maintain a continuous network of bonding interactions between the constituents of the lattice. Consequently, even the most dynamic porous materials tend to be brittle and isolated as microcrystalline powders 14 , whereas flexible organic or inorganic molecular crystals cannot expand without fracturing. Owing to their rigidity, crystalline materials rarely display self-healing behaviour 20 . Here we report that macromolecular ferritin crystals with integrated hydrogel polymers can isotropically expand to 180 per cent of their original dimensions and more than 500 per cent of their original volume while retaining periodic order and faceted Wulff morphologies. Even after the separation of neighbouring ferritin molecules by 50 ångströms upon lattice expansion, specific molecular contacts between them can be reformed upon lattice contraction, resulting in the recovery of atomic-level periodicity and the highest-resolution ferritin structure reported so far. Dynamic bonding interactions between the hydrogel network and the ferritin molecules endow the crystals with the ability to resist fragmentation and self-heal efficiently, whereas the chemical tailorability of the ferritin molecules enables the creation of chemically and mechanically differentiated domains within single crystals.

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A Self-Healing Crease-Free Supramolecular All-Polymer Supercapacitor.

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