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1.
Angew Chem Int Ed Engl ; 62(42): e202310832, 2023 Oct 16.
Article in English | MEDLINE | ID: mdl-37646238

ABSTRACT

The application of hydrogels often suffers from their inherent limitation of poor mechanical properties. Here, a carboxyl-functionalized and acryloyl-terminated hyperbranched polycaprolactone (PCL) was synthesized and used as a macro-cross-linker to fabricate a super strong and ultra-tough ionic hydrogel. The terminal acryloyl groups of hyperbranched PCL are chemically incorporated into the network to form covalent cross-links, which contribute to robust networks. Meanwhile, the hydrophobic domains formed by the spontaneous aggregation of PCL chains and coordination bonds between Fe3+ and COO- groups serve as dynamic non-covalent cross-links, which enhance the energy dissipation ability. Especially, the influence of the hyperbranched topological structure of PCL on hydrogel properties has been well investigated, exhibiting superior strengthening and toughening effects compared to the linear one. Moreover, the hyperbranched PCL cross-linker also endowed the ionic hydrogel with higher sensitivity than the linear one when used as a strain sensor. As a result, this well-designed ionic hydrogel possesses high mechanical strength, superior toughness, and well ionic conductivity, exhibiting potential applications in the field of flexible strain sensors.

2.
Chem Commun (Camb) ; 59(13): 1789-1792, 2023 Feb 09.
Article in English | MEDLINE | ID: mdl-36722415

ABSTRACT

A novel responsive hydrogel exhibiting self-reinforcement and self-healing capacity was developed based on the hydrophobic aggregation of strained 1,2-dithiolane rings. Oligomerization of 1,2-dithiolane within hydrophobic domains under UV irradiation not only reinforced the hydrogel but also maintained its dynamic cross-linked nature by converting the intraring dynamic S-S bond to an outer one.

3.
Angew Chem Int Ed Engl ; 61(41): e202211713, 2022 Oct 10.
Article in English | MEDLINE | ID: mdl-35982028

ABSTRACT

An efficient "one-pot" strategy for the structure-controlled synthesis of hyperbranched polymers (HBPs) based on a "latent" inimer (LI-Br), containing a furan-protected maleimide monomer and a haloalkane initiator, is presented. At high temperatures, the "latent" inimer is converted to a "real" inimer after releasing maleimide (MI) via a retro-Diels-Alder (r-DA) reaction and then copolymerized with methyl methacrylate by self-condensing vinyl copolymerization. Due to the dynamic characteristic of the r-DA reaction, the release of naked MI and the subsequent copolymerization can be regulated by the temperature or stereochemistry of Diels-Alder (DA) adducts. Thus, the "one-pot" structure-controlled synthesis of HBPs with various degrees of branching was achieved. By further implementation of a programmable temperature change, some valuable hyperbranched topologies such as star-shaped and long-chain hyperbranched polymers can be constructed avoiding sophisticated synthetic routes.

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