Robust and healable poly(disulfides) supramolecular adhesives enabled by dynamic covalent adaptable networks and noncovalent hydrogen-bonding interactions

Modern adhesives with a combined competence of reversible adhesion ability, self-healing function, and stimuliresponsive adhesion are in substantial demand for meeting their ever-expanding actual applications. In this work, we demonstrate a facile and powerful noncovalent bonding strategy that integrates natural thioctic acid and the volume-exclusion effect inspired mono-hydroxylated adamantane-functionalized poly(disulfide) backbone to realize a strong yet stable supramolecular adhesive materials. Profiting from the dynamic covalent poly(disulfides) network and reversible nanoconfined effect, optimized supramolecular adhesive featuring a solvent-free network can present fascinating reconfigurable ability upon repeated cooling and heating. Our results indicated that dynamic covalent disulfide bonds and high-density hydrogen bonds initiating dimeric forces could be significant driving forces for both rapid healing and robust adhering. Meanwhile, this dynamic supramolecular network ensured ultra-high adhesion strength on diverse substrate surfaces and excellent self-healing ability. This work provides valuable guidance for further developing rational theories of the mechanism of adhesive action and constructing high-performance adhesives based on small molecules.