Programmable supramolecular chirality in non-equilibrium systems affording a multistate chiroptical switch.

The dynamic regulation of supramolecular chirality in non-equilibrium systems can provide valuable insights into molecular self-assembly in living systems. Herein, we demonstrate the use of chemical fuels for regulating self-assembly pathway, which thereby controls the supramolecular chirality of assembly in non-equilibrium systems. Depending on the nature of different fuel acids, the system shows pathway-dependent non-equilibrium self-assembly, resulting in either dynamic self-assembly with transient supramolecular chirality or kinetically trapped self-assembly with inverse supramolecular chirality. More importantly, successive conducting of chemical-fueled process and thermal annealing process allows for the sequential programmability of the supramolecular chirality between four different chiral hydrogels, affording a new example of a multistate supramolecular chiroptical switch that can be recycled multiple times. The current finding sheds new light on the design of future supramolecular chiral materials, offering access to alternative self-assembly pathways and kinetically controlled non-equilibrium states.

A Full-Device Autonomous Self-Healing Stretchable Soft Battery from Self-Bonded Eutectogels.

Next-generation energy storage devices should be soft, stretchable, and self-healable. Previously reported self-healable batteries mostly possess limited stretchability and rely on healable electrodes or electrolytes rather than achieving full-device self-healability. Herein, an all-component self-bonding strategy is reported to obtain an all-eutectogel soft battery (AESB) that simultaneously achieves full-cell autonomous self-healability and omnidirectional intrinsic stretchability (>1000% areal strain) over a broad temperature range (-20~60 °C). Without requiring any external stimulus, the five-layered soft battery can efficiently recover both its mechanical and electrochemical performance at full-cell level. The developed AESB can be easily configured into various 3D architectures with highly interfacial compatible eutectogel electrodes, electrolyte, and substrate, presenting an excellent opportunity for the development of embodied energy technologies. The present work provides a general and user-friendly soft electronic material platform for fabricating a variety of intrinsic self-healing stretchable multi-layered electronics, which are promising beyond the field of energy storage, such as displays, sensors, circuits, and soft robots.

Low-molecular-weight supramolecular adhesives based on non-covalent self-assembly of a small molecular gelator.

Currently developed adhesives are overwhelmingly polymeric in nature. Herein, we highlight for the first time the potential of supramolecular eutectogels assembled from small molecules as robust low-molecular-weight (LMW) supramolecular adhesives in air, water and organic solvents, and under low temperatures. These supramolecular eutectogels were produced from commercial alkyl trimethyl ammonium bromide (CnTAB) in emerging deep eutectic solvents (DESs), which demonstrated rapid (∼2 min), robust, and tunable adhesion to both hydrophilic and hydrophobic surfaces at room temperature in air. Moreover, high adhesion performance was maintained even in liquid nitrogen (-196 °C), underwater, and in organic solvents. A study of the structure-property relationship of these adhesives and molecular dynamics (MD) simulations further clarified the assembly and adhesion mechanism of the C12TAB molecules in DESs. Compared with traditional polymer adhesives and several existing examples of LMW supramolecular adhesives with solvent-free dry network structures, the spontaneous self-assembly of LMW gelators in versatile DESs provides a new strategy for the facile construction of high-strength supramolecular adhesives with gel network structures for a diverse range of harsh environments.