Abstract
We report here our successful attempt to obtain self-healing supramolecular hydrogels with new metal-containing monomers (MCMs) with pendent 4-phenyl-2,2′:6′,2″-terpyridine metal complexes as reversible moieties by free radical copolymerization of MCMs with vinyl monomers, such as acrylic acid and acrylamide. The resulting metal-polymer hydrogels demonstrate a developed system of hydrogen, coordination and electron-complementary π–π stacking interactions, which play a critical role in achieving self-healing. Kinetic data show that the addition of a third metal-containing comonomer to the system decreases the initial polymerization rate, which is due to the specific effect of the metal group located in close proximity of the active center on the growth of radicals.
Highlights
Self-healing polymers (SHPs) are one of the most important classes of materials discovered in the 20th century, and they can be characterized as systems capable of healing local mechanical damage, such as cracks or scratches [1,2]
We report here our successful attempt to obtain self-healing supramolecular hydrogels bearing terpyridine-metal complexes by free radical copolymerization of metal-containing monomers (MCMs) with vinyl monomers, such as acrylic acid (AA) and acrylamide (AM)
We have designed a new kind of self-healing supramolecular materials with metal-containing monomers (MCMs) with pendent 4-phenyl-2,2 :6,2 -terpyridine metal complexes as reversible moieties
Summary
Self-healing polymers (SHPs) are one of the most important classes of materials discovered in the 20th century, and they can be characterized as systems capable of healing local mechanical damage, such as cracks or scratches [1,2]. Intrinsic SHPs contain physical, supramolecular interactions, or specific chemical bonds in their own structure, the change in the configuration of which allows easy/quick recover after damage, leading to a faster self-healing process [6]. Such systems usually have reversible covalent bonds based on the Diels–Alder reaction [7,8], disulfide bonds [9], [2+2] cycloadditions [10], or non-covalent interactions, such as π–π interactions [11], hydrogen bonds [12], host-guest interactions [13], ionic interactions [14], metal-ligand (M-L) interactions [15], and/or their orthogonal combinations [16]. The first stage is the general procedure for the synthesis of supramolecular systems, such as ionic and free radical (co)polymerization of vinyl monomers (for example, using 4 -vinylterpyridine monomer in the case of the introduction of terpyridine moieties into the polymer backbone [37]) or reversible addition-fragmentation chain-transfer polymerization [38], and more recently, ring-opening metathesis polymerization [33] with subsequent crosslinking of polymer chains using a solution of salts of various metals (Scheme 1) [39]
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