Tough and self-healable hydrogels have been prepared by the multiple supramolecular interactions of clay nanosheets with dendritic polymers or in situ-formed polymer. [ 10 ] Many workers have studied ionic gels formed by the supramolecular effect of ionic liquids and block copolymers with/without SiO 2 nanofi ller, which also demonstrate the high mechanical modulus. [ 11 ] Here, we employ a mild self-initiated UV polymerization to prepare an ionic conducting polymer gel, whose non-covalent crosslinking interaction can endow the conducting gel compressive toughness and self-recovering ability.Our system consists of four components: 1-ethyl-3-methylimidazolium chloride (EMIMCl), hydroxyethyl methacrylate (HEMA), chitosan (CS) and water, whose molecular structures have been shown in Figure 1 A. At fi rst, CS and HEMA are dissolved in EMIMCl via heating and cooling process, which forms a viscous solution from the solid of EMIMCl (Figures S1a and 1C). The destroy of crystal structure of EMIMCl is the main reason to form such homogeneous solution, which is caused by the dissolution of CS and HEMA through hydrogen bond. [ 12 ] Then, tough EMIMCl gels can be formed by irradiating the asprepared homogeneous solution with UV light (Figures S1b and S2; Figure 1 D). The UV-generated Cl radicals from EMIMCl (Figure 1 B) are the initiator for the polymerization of HEMA. [ 13 ] The physical gelation of our EMIMCl gel without crosslinker should be ascribed to the hydrogen bonding interactions between the hydroxyl group in PHEMA, the amine group of CS and imidazolium group in solvent. Interesting is that our EMIMCl gel is miscible with water, which has a slightly decrease strength but a sharply increase ionic conductivity (Figure 1 E). As shown in Figure S3, water exists in the form of free water and bound water, and is relatively stable at room temperature ( Figure S4). The fi nal EMIMCl/water gel exhibits the water and pressure controlled ionic conductivity, which is suitable as an appropriate electrolyte and separator in fl exible supercapacitors. The detailed preparation, mechanism and properties are shown as followed.The EMIMCl gels can be formed by irradiating the as-prepared homogeneous solution under 45 minutes UV light with intensity of 22.4 mw/cm 2 at 365 nm. The component ratio of the conducting gel is optimized by the comprehensive evaluation of the electrochemical performances and mechanical strength. Finally, a varying amount of water was injected into the EMIMCl gel to form EMIMCl/water gels with 5 to 50 wt% (by mass) water content (Figure 1 E). If the water was added in advance, the fi nal gel could not be obtained. The EMIMCl/water gel shows high toughness when they underwent large deformations and show good strength under compression ( Figure 2 Flexible devices are a mainstream direction in modern electronics and related multidisciplinary fi elds. [ 1 ] Concerning fl exible capacitors and batteries, the current research is mainly focused on the fabrication of fl exible electrode materials; [ 2 ] however, ele...

Dual amide hydrogen bond crosslinked and strengthened high strength supramolecular polymer conductive hydrogels were fabricated by simply in situ doping poly (N-acryloyl glycinamide-co-2-acrylamide-2-methylpropanesulfonic) (PNAGA-PAMPS) hydrogels with PEDOT/PSS. The nonswellable conductive hydrogels in PBS demonstrated high mechanical performances—0.22–0.58 MPa tensile strength, 1.02–7.62 MPa compressive strength, and 817–1709% breaking strain. The doping of PEDOT/PSS could significantly improve the specific conductivities of the hydrogels. Cyclic heating and cooling could lead to reversible sol-gel transition and self-healability due to the dynamic breakup and reconstruction of hydrogen bonds. The mending hydrogels recovered not only the mechanical properties, but also conductivities very well. These supramolecular conductive hydrogels could be designed into arbitrary shapes with 3D printing technique, and further, printable electrode can be obtained by blending activated charcoal powder with PNAGA-PAMPS/PEDOT/PSS hydrogel under melting state. The fabricated supercapacitor via the conducting hydrogel electrodes possessed high capacitive performances. These cytocompatible conductive hydrogels have a great potential to be used as electro-active and electrical biomaterials.

New‐era soft microrobots for biomedical applications need to mimic the essential structures and collective functions of creatures from nature. Biocompatible interfaces, intelligent functionalities, and precise locomotion control in a collective manner are the key parameters to design soft microrobots for the complex bio‐environment. In this work, a biomimetic magnetic microrobot (BMM) inspired by magnetotactic bacteria (MTB) with speedy motion response and accurate positioning is developed for targeted thrombolysis. Similar to the magnetosome structure in MTB, the BMM is composed of aligned iron oxide nanoparticle (MNP) chains embedded in a non‐swelling microgel shell. Linear chains in BMMs are achieved due to the interparticle dipolar interactions of MNPs under a static magnetic field. Simulation results show that, the degree and speed of assembly is proportional to the field strength. The BMM achieves the maximum speed of 161.7 µm s−1 and accurate positioning control under a rotating magnetic field with less than 4% deviation. Importantly, the locomotion analyses of BMMs demonstrate the frequency‐dependent synchronization under 8 Hz and asynchronization at higher frequencies due to the increased drag torque. The BMMs can deliver and release thrombolytic drugs via magneto‐collective control, which is promising for ultra‐minimal invasive thrombolysis.

As the first line of innate immune cells to migrate towards tumour tissue, neutrophils, can immediately kill abnormal cells and activate long-term specific adaptive immune responses. Therefore, the enzymes mediated elevation of reactive oxygen species (ROS) bioinspired by neutrophils can be a promising strategy in cancer immunotherapy. Here, we design a core-shell supramolecular hybrid nanogel via the surface phosphatase triggered self-assembly of oligopeptides around iron oxide nanoparticles to simulate productive neutrophil lysosomes. The cascade reaction of superoxide dismutase (SOD) and chloroperoxidase (CPO) within the bioinspired nanogel can convert ROS in tumour tissue to hypochlorous acid (HOCl) and the subsequent singlet oxygen (1O2) species. Studies on both cells and animals demonstrate successful 1O2-mediated cell/tumour proliferation inhibition, making this enzyme therapy capable for treating tumours without external energy activation.