Relatively high aspect ratio exfoliated graphite (EFG) particles with an average size of 7.4 µm and a nanometer sized thickness of 30-50 nm were successfully prepared by thermal treatment at 1050• C and subsequent ultrasonication for application as a filler to improve the physical properties of eco-friendly poly(propylene carbonate) (PPC). A series of poly(propylene carbonate)/exfoliated graphite (PPC/EFG) nanocomposite films with different EFG contents were prepared via a solution blending method. The physical properties were strongly dependent upon the chemical and morphological structures originating from the differences in EFG composition. The morphological structures, thermal properties, mechanical properties and barrier properties of the nanocomposite films were investigated as a function of the EFG content. While all of the PPC/EFG nanocomposite films exhibited good dispersion of EFG to some extent, Fourier transform infrared and SEM results revealed that solution blending did not lead to strong interactions between PPC and EFG. As a result, poor dispersion occurred in composite films with a high EFG content. By loading EFG particles, the oxygen permeabilities, moisture permeabilities and water uptake at equilibrium decreased as the EFG content increased. Compared with pure PPC, PPC/EFG nanocomposite films have enhanced molecular ordering. Specifically, the 2% PPC/EFG composite film shows greater molecular ordering than the other composite films, which results in the highest mechanical strength. In future work, the compatibility and dispersion of the PPC matrix polymer and EFG filler particles should be increased by modifying the EFG surface or introducing additives.

Ionogels are good candidates for flexible electronics owing to their excellent mechanical and electrical properties, including stretchability, high conductivity, and stability. In this study, conducting ionogels comprising a double network (DN) of poly(N‐isopropylacrylamide‐co‐N,N′‐diethylacrylamide)/chitosan which are further reinforced by the ionic and covalent crosslinking of the chitosan network by tripolyphosphate and glutaraldehyde, respectively, are prepared. Based on their excellent mechanical properties and high conductivity, the developed DN ionogels are envisioned as stretchable ionic conductors for extremely stretchable alternating‐current electroluminescent (ACEL) devices. The ACEL device fabricated with the developed ionogel exhibits stable working operation under an ultrahigh elongation of over 1200% as well as severe mechanical deformations such as bending, rolling, and twisting. Furthermore, the developed ACEL devices also display stable luminescence over 1000 stretch/release cycles or at temperatures as harsh as 200 °C.

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Strain sensors with high sensitivity and stretchability are required for wearable or implantable sensors to detect human motion. In this study, highly stretchable double‐network (DN) of soft polyacrylamide and brittle calcium‐alginate microfibers containing poly(3,4‐ethylenedioxythiphene)‐poly(styrenesulfonate) (PEDOT:PSS) are prepared using microfluidic devices. The resistance changes in response to the stretching of the microfiber due to the connection/partial disconnection of the PEDOT:PSS domains; it could be monitored up to 300% elongation with a resolution of 0.1%. Furthermore, these changes are fully reversible and repeatable over 10 000 cycles of 200% elongation. Owing to such mechanical and electronic properties, DN microfibers are envisioned to be useful in stretchable strain sensors to detect human motion in real time, including bending of the fingers, walking, and running. It is also demonstrated that the developed sensor can be stably used outdoors by measuring the growth of a bamboo planted in a garden.

To avoid the problem of reduced graphene oxide (rGO) restacking in aqueous solution, the preparation of light-responsive poly(N-isopropylacrylamide) incorporating rGO (PNIPAm/rGO) was achieved by the chemical reduction of GO dispersed in the hydrogel matrix. Due to the enhanced photothermal efficiency of the rGO, the prepared PNIPAm/rGO underwent large volume reductions in response to irradiation by visible light of modest intensity. With respect to potential applications, bilayer-type photo-actuators comprising a PNIPAm/rGO active layer and poly(acrylamide) passive layer were fabricated; these achieved a full bending motion upon visible-light exposure. Adjusting the swelling ratio of each layer in the initial state yielded bidirectional photo-actuators that showed the active motion of turning inside out. Furthermore, we demonstrated that the fabricated actuation system would exhibit controlled bending motion in response to solar radiation.

In order to achieve a hydrogel capable of programmable volume change, poly(N-isopropylacrylamide)graf t-methylcellulose hydrogel (PNIPAm-g-MC) was prepared through the grafting of PNIPAm onto a MC backbone and simultaneous cross-linking of the chains. PNIPAm-g-MC exhibited large thermal hysteresis in its volume change, which results from the stable hydrophobic junctions between the MC strands formed during heating. By combining photothermal magnetite nanoparticles as a heat transducer with the prepared hydrogel, programmable volume phase transition between the shrunken and swollen state could be triggered by visible light irradiation and excessive cooling, respectively. Based on this programmable feature, a bilayer actuator capable of static bending was fabricated. The developed programmable hydrogels are expected to provide a platform for the next generation of origami, microvalves, and drug delivery systems.

To overcome the slow kinetics of the volume phase transition of stimuli-responsive hydrogels as platforms for soft actuators, thermally responsive comb-type hydrogels were prepared using synthesized poly(N-isopropylacrylamide) macromonomers bearing graft chains. Fast responding light-responsive hydrogels were fabricated by combining a comb-type hydrogel matrix with photothermal magnetite nanoparticles (MNP). The MNPs dispersed in the matrix provide heat to stimulate the volume change of the hydrogel matrix by converting absorbed visible light to thermal energy. In this process, the comb-type hydrogel matrix exhibited a rapid response due to the free, mobile grafted chains. The comb-type hydrogel exhibited significantly enhanced light-induced volume shrinkage and rapid recovery. The comb-type hydrogels containing MNP were successfully used to fabricate a bilayer-type photo-actuator with fast bending motion.