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Wei, Xianshuo ; Xue, Yaoting ; Sun, Ye ; Chen, Lian ; Zhang, Chunmei ; Wu, Qijun ; Peng, Shuyi ; Ma, Chunxin ; Liu, Zhenzhong ; Jiang, Shaohua ; Yang, Xuxu ; Agarwal, Seema ; Duan, Gaigai

Chemical Engineering Journal, 2023. https://doi.org/10.1016/j.cej.2022.139373

Intelligent hydrogels are promising for biomimetic actuators, but acquiring actuations with both high speed and powerful force is still extremely difficult. Herein, a new robust polypyrrole (PPy)-coated copoly(isopropylacrylamide-4-benzoylphenyl acrylate) [P(NIPAM-ABP)] electrospun light-responsive hydrogel is explored. The (PPy)-coated P(NIPAM-ABP) hydrogel can be obtained via in-situ polymerization of pyrroles on the nanofiber-oriented electrospun P(NIPAM-ABP) hydrogel. Compared with original P(NIPAM-ABP) hydrogel, this PPy-coated P(NIPAM-ABP) hydrogel can integrate highly-enhanced mechanical strength (from 1.21 to 5.12 MPa of tensile strength) and ultrahigh-efficiency of photothermal conversion together. In addition, the orientation of P(NIPAM-ABP) nanofibers can still maintain well for programmable complex deformations. Consequently, the as-prepared robust bi-hydrogel actuator with ultrafast and complex deformations has been achieved, through bonding the PPy-P(NIPAM-ABP) hydrogel membrane with a polyethylene glycol diacrylate-cellulose nanofiber (PEGDA-CNF) composite hydrogel membrane via interfacial ultraviolet (UV) polymerization of PEGDA monomers. Several light-responsive biomimetic actuating devices have been achieved, which owning powerful force (can grab up 100 times of self-weight), rapid speed (1285.71°/s of folding) or precisely programmable complex deformations. Furthermore, two biomimetic devices with synergistic functions of the three advantages above have been explored, which can mimic the child’s sit-up and the starfish’s continuous crawling movement respectively. This work provides a robust remotely-controlled light-responsive hydrogel actuator with powerful force, ultrafast speed and programmable complex actuations, which will inspire the design and fabrication of novel soft biomimetic actuating materials and systems.