Surface Hydrophobization Provides Hygroscopic Supramolecular Plastics Based on Polysaccharides with Damage‐Specific Healability and Room‐Temperature Recyclability

Abstract Supramolecular materials with room‐temperature healability and recyclability are highly desired because they can extend materials lifetimes and reduce resources consumption. Most approaches toward healing and recycling rely on the dynamically reversible supramolecular interactions, such as hydrogen, ionic and coordinate bonds, which are hygroscopic and vulnerable to water. The general water‐induced plasticization facilitates the healing and reprocessing process but cause a troubling problem of random self‐adhesion. To address this issue, here it is reported that by modifying the hygroscopic surfaces with hydrophobic alkyl chains of dodecyltrimethoxysilane (DTMS), supramolecular plastic films based on commercial raw materials of sodium alginate (SA) and cetyltrimethylammonium bromide (CTAB) display extraordinary damage‐specific healability. Owing to the hydrophobic surfaces, random self‐adhesion is eliminated even under humid environment. When damage occurs, the fresh surfaces with ionic groups and hydroxyl groups expose exclusively at the damaged site. Thus, damage‐specific healing can be readily facilitated by water‐induced plasticization. Moreover, the films display excellent room‐temperature recyclability. After multiple times of reprocessing and re‐modifying with DTMS, the rejuvenated films exhibit fatigueless mechanical properties. It is anticipated that this approach to damage‐specific healing and room‐temperature recycling based on surface hydrophobization can be applied to design various of supramolecular plastic polysaccharides materials for building sustainable societies.