In contrast to the borrowing hydrogentype N-alkylation reactions, in which alcohols were activated by transition metal-catalyzed anaerobic dehydrogenation, the addition of external aldehydes was accidentally found to be a simple and effective protocol for alcohol activation. This interesting finding subsequently led to an efficient and green, practical and scalable aldehyde-catalyzed transition metal-free dehydrative N-alkylation method for a variety of amides, amines, and alcohols. Mechanistic studies revealed that this reaction most possibly proceeds via a simple but interesting transition metal-free relay race mechanism.

An air-stable oxidation state is observed in an electrochromic triphenylamine–triazine polymer energy storage system after the removal of the applied potential.

Addressing the conflict between achieving high mechanical properties and room-temperature self-healing ability is extremely significant to achieving a breakthrough in the application of self-healing materials. Therefore, inspired by natural spider silk and nacre, a room-temperature self-healing supramolecular material with ultrahigh strength and toughness is developed by synergistically incorporating flexible disulfide bonds and dynamic sextuple hydrogen bonds (H-bonds) into polyurethanes (PUs). Simultaneously, abundant H-bonds are introduced at the interface between graphene oxide nanosheets with dynamic multiple H-bonds and the PU matrix to afford strong interfacial interactions. The resulting urea-containing PU material with an inverse artificial nacre structure has a record mechanical strength (78.3 MPa) and toughness (505.7 MJ m −3 ), superior tensile properties (1273.2% elongation at break), and rapid room-temperature self-healing abilities (88.6% at 25 °C for 24 h), forming the strongest room-temperature self-healing elastomer reported to date and thus upending the previous understanding of traditional self-healing materials. In addition, this bionic PU−graphene oxide network endows the fabricated flexible intelligent robot with functional repair and shape memory capabilities, thus providing prospects for the fabrication of flexible functional devices.