Mussel‐Inspired, Underwater Self‐Healing Ionoelastomers Based on α‐Lipoic Acid for Iontronics

Weak adhesion and lack of underwater self-healability hinder advancing soft iontronics particularly in wet environments like sweaty skin and biological fluids. Mussel-inspired, liquid-free ionoelastomers are reported based on seminal thermal ring-opening polymerization of a biomass molecule of α-lipoic acid (LA), followed by sequentially incorporating dopamine methacrylamide as a chain extender, N,N'-bis(acryloyl) cystamine, and lithium bis(trifluoromethanesulphonyl) imide (LiTFSI). The ionoelastomers exhibit universal adhesion to 12 substrates in both dry and wet states, superfast self-healing underwater, sensing capability for monitoring human motion, and flame retardancy. The underwater self-repairabilitiy prolongs over three months without deterioration, and sustains even when mechanical properties greatly increase. The unprecedented underwater self-mendability benefits synergistically from the maximized availability of dynamic disulfide bonds and diverse reversible noncovalent interactions endowed by carboxylic groups, catechols, and LiTFSI, along with the prevented depolymerization by LiTFSI and tunability in mechanical strength. The ionic conductivity reaches 1.4 × 10-6 -2.7 × 10-5 S m-1 because of partial dissociation of LiTFSI. The design rationale offers a new route for creating a wide range of LA- and sulfur-derived supramolecular (bio)polymers with superior adhesion, healability, and other functionalities, and thus has technological implications for coatings, adhesives, binders and sealants, biomedical engineering and drug delivery, wearable and flexible electronics, and human-machine interfaces.