A Facile Strategy to Fabricate Tough and Adhesive Elastomers by In Situ Formation of Coordination Complexes as Physical Crosslinks

Abstract

Coordination bonds with a dynamic nature and wide‐spectrum bond energy have gained great popularity in use for fabricating tough soft materials. However, most existing coordination‐based elastomers are prepared through complicated procedures, usually involving elaborate synthesis of ligand‐containing monomers or polymers, ion diffusion to form coordination complexes, and removal of organic solvent during the synthesis, which are neither easy operation nor environmentally friendly. Here, a facile and effective strategy is demonstrated to fabricate tough metallosupramolecular elastomers by one‐pot polymerization of aqueous precursor solutions containing commercial agents, 2‐acrylamido‐2‐methyl‐1‐propanesulfonic acid, 2‐[2‐(2‐methoxyethoxy)ethoxy]ethyl acrylate, and Zr4+ ions. After solvent (i.e. water) evaporation, the obtained elastomers are transparent and extremely tough owing to the presence of sulfonate‐Zr4+ coordination complexes as physical crosslinks. Their mechanical properties are tunable over a wide spectrum by adjusting the composition of copolymers and the density of coordination bonds. This eco‐friendly strategy is further extended to various commercial monomers, manifesting good universality to toughen elastomers. Furthermore, the abundant functional groups of copolymers make the elastomers adhesive to various substrates including themselves, favoring applications such as interfacial adhesion and encapsulations. The easy fabrication, tunable mechanical properties, and adhesion ability endow the elastomers with great potential as the substrate of wearable soft electronics.

Highly Stretchable and Self-Healable Tough Polymer Elastomer through Dy3+ and Cu2+ Coordination Cross-Linking

“…The two elastomer films with different colors were first cut into two pieces. Then, the dark green (Cu/Dy mole ratio of 2:1) and light green (Cu/Dy mole ratio of 1:2) elastomer films were spliced together and placed in an oven at 80 °C for 1 h. Similar to other metallogels and metalloelastomers, − the two pieces of elastomer films were reassembled. The photo images clearly showed the remerging of surfaces.…”

Spider-silk-inspired strong and tough hydrogel fibers with anti-freezing and water retention properties

“…This indicated that the number of Zr 4+ crosslinking in the S-PAZr was reduced after the salting-out treatment, whereas the Zr 4+ coordination state was not significantly changed (Fig. 2c) 39 . The crystalline domain evolution of the S-PAZr was discussed by X-ray diffraction (XRD) analysis.…”

“…Benefiting from the elaborated ionic crosslinking and crystalline domains, the S-PAZr hydrogel fiber could synergistically dissipate energy through ionic decoordination and crystalline domain unfolding during stretching (Supplementary Figs. 4, 5) 39,[49][50][51] . As a result, the S-PAZr hydrogel fiber exhibited high mechanical properties, such as tensile stress of 24.43 ± 2.11 MPa, tensile strain of 844.44 ± 107.21%, elastic modulus of 36.81 ± 1.58 MPa, and toughness of 162.25 ± 21.99 MJ/m 3 (Fig.…”