Adv Polym Sci (2020) 285: 211–242
https://doi.org/10.1007/12_2019_55
© Springer Nature Switzerland AG 2020
Published online: 29 February 2020
Triblock Copolymer Micelle-Crosslinked
Hydrogels
Jun Fu
Contents
1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 212
2 Triblock Copolymer Micelle-Crosslinked Hydrogels . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 213
2.1 Mechanical Properties . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 215
2.2 Effect of Solvent on Structures and Properties . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 217
3 Multi-responsive Hydrogels . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 223
4 Macroscopically Assembled Devices . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 230
5 Supramolecular Micelle-Crosslinked Hydrogels . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 235
6 Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 237
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 238
Abstract This chapter reviews the preparation, structures, properties, and applications of tough and responsive hydrogels crosslinked by triblock copolymer micelles.
An amphiphilic triblock copolymer, Pluronic F127, is functionalized with reactive
groups. The functional F127 chains form polyfunctional micelles in aqueous solution, which are used for reaction with hydrophilic monomers or polymer chains to
form hydrophobically crosslinked network. Free radical polymerization, host-guest
interaction, and dynamic bonds have been utilized to connect the polymer chains
with the reactive micelle coronae. The obtained polymer hydrogels show outstanding strength and toughness, with the micelles serving as energy dissipation centers.
The structural evolution and energy dissipation mechanisms have been investigated
in detail. By incorporating functional monomers into the network, a series of
functional hydrogels responsive to pH, salt, electric field, and temperature have
been developed. The hydrogels have been utilized as building blocks to fabricate soft
actuators, shape-morphing devices, and biomaterials for tissue repair.
J. Fu (*)
School of Materials Science and Engineering, Sun Yat-sen University, Guangzhou, China
e-mail: fujun8@mail.sysu.edu.cn
https://doi.org/10.1007/12_2019_55
© Springer Nature Switzerland AG 2020
Published online: 29 February 2020
Triblock Copolymer Micelle-Crosslinked
Hydrogels
Jun Fu
Contents
1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 212
2 Triblock Copolymer Micelle-Crosslinked Hydrogels . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 213
2.1 Mechanical Properties . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 215
2.2 Effect of Solvent on Structures and Properties . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 217
3 Multi-responsive Hydrogels . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 223
4 Macroscopically Assembled Devices . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 230
5 Supramolecular Micelle-Crosslinked Hydrogels . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 235
6 Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 237
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 238
Abstract This chapter reviews the preparation, structures, properties, and applications of tough and responsive hydrogels crosslinked by triblock copolymer micelles.
An amphiphilic triblock copolymer, Pluronic F127, is functionalized with reactive
groups. The functional F127 chains form polyfunctional micelles in aqueous solution, which are used for reaction with hydrophilic monomers or polymer chains to
form hydrophobically crosslinked network. Free radical polymerization, host-guest
interaction, and dynamic bonds have been utilized to connect the polymer chains
with the reactive micelle coronae. The obtained polymer hydrogels show outstanding strength and toughness, with the micelles serving as energy dissipation centers.
The structural evolution and energy dissipation mechanisms have been investigated
in detail. By incorporating functional monomers into the network, a series of
functional hydrogels responsive to pH, salt, electric field, and temperature have
been developed. The hydrogels have been utilized as building blocks to fabricate soft
actuators, shape-morphing devices, and biomaterials for tissue repair.
J. Fu (*)
School of Materials Science and Engineering, Sun Yat-sen University, Guangzhou, China
e-mail: fujun8@mail.sysu.edu.cn