Supramolecular Ionogels for Use in Locating Damage to Underwater Infrastructure.

The capacity to self-detect and locate damage to underwater infrastructure in emergencies is vital, as materials and technologies that securely facilitate energy and information transmission are crucial in several fields. Herein, the development of a multifunctional supramolecular ionogel (SIG) and SIG-based devices for use in detecting and locating damage to underwater infrastructure is reported. The SIG is fabricated via the single-step photoinitiated copolymerization of hydroxy and fluorinated monomers in a fluorinated ionic liquid. Hydrogen-bond/ion-dipole-interaction synergy ensures that the SIG is highly ionically conductive and extremely mechanically strong, with underwater self-healing and adhesion properties. It can be used as an underwater ionic cable to provide reporting signals via changes in strain; furthermore, SIG-based devices can be fixed to underwater infrastructure to locate damage via resistance monitoring. The SIG can also be attached to the human body for use in underwater communication, thereby safeguarding maintenance personnel while repairing underwater infrastructure. This study provides a novel pathway for developing supramolecular materials and devices.

Elastomeric Liquid-Free Conductor for Iontronic Devices.

For a long time, the potential application of gel-based ionic devices was limited by the problem of liquid leakage or evaporation. Here, we utilized amorphous, irreversible and reversible cross-linked polyTA (PTA) as a matrix and lithium bis(trifluoromethane sulfonamide) (LiTFSI) as an electrolyte to prepare a stretchable (495%) and self-healing (94%) solvent-free elastomeric ionic conductor. The liquid-free ionic elastomer can be used as a stable strain sensor to monitor human activities sensitively under extreme temperatures. Moreover, the prepared elastic conductor (TEOA0.10-PTA@LiTFSI) was also considered an electrode to assemble with self-designed repairable dielectric organosilicon layers (RD-PDMS) to develop a sustainable triboelectric nanogenerator (SU-TENG) with outstanding performance. SU-TENG maintained good working ability under extreme conditions (-20 °C, 60 °C, and 200% strain). This work provided a low-cost and simple idea for the development of reliable iontronic equipment for human-computer interaction, motion sensing, and sustainable energy.

Self-reporting of damage in underwater hierarchical ionic skins via cascade reaction-regulated chemiluminescence.

Self-reporting of damage in underwater materials allows on-demand maintenance and, therefore, improves the reliability of materials used in aquatic environments. Here, we report a chemiluminescence-based strategy to self-report the mechanical damage (e.g., fracture or puncture) in underwater hierarchical ionic skins (HI-skins). The chemiluminescence-based self-reporting is regulated by a cascade reaction, which first occurs at the interface between water and the damage location and then spreads through the whole material. When the HI-skins were mechanically damaged underwater, the pre-embedded calcium peroxide became exposed to and reacted with water to generate hydrogen peroxide that further activated the peroxyoxalate chemiluminescence reaction for reporting the damage. The luminescence wavelength could be tuned (439, 508, or 603 nm) and the damage-induced luminescence lasted for up to 12 h. The self-reporting HI-skins also displayed high mechanical and electronic restorability (93% healing efficiency), excellent stretchability (1600%), impressive room-temperature ionic conductivity (1.7 × 10-4 S cm-1), and durable strain sensing performance (highly reproducible electrical response over 1000 uninterrupted strain cycles), making them suitable and reliable candidates for underwater soft ionotronics.

Tailoring Azlactone-Based Block Copolymers for Stimuli-Responsive Disassembly of Nanocarriers.

Stimuli-responsive nanoparticles based on a reactive block copolymers (BCPs) of poly(ethylene glycol)-b-poly(2-vinyl-4,4-dimethylazlactone) (PEG-b-PVDMA) have been fabricated for loading and controlled release of molecular cargoes. Microphase segregation of PEG-b-PVDMA BCPs enables the construction of well-defined nanoparticles in aqueous solutions. The azlactone groups in VDMA repeat units offer active sites for hydrophilization of the BCPs and functionalization by primary amines. The hydrophilization of PEG-b-PVDMA BCPs induces gradual reconstruction and dissociation of the BCP nanoparticles. Functional primary amines can be conjugated to PEG-b-PVDMA BCPs, yielding azobenzene- and pyridine-containing BCPs. The self-assembled nanoparticles made from the functionalized BCPs can disassemble in response to different external stimuli (e.g., addition of ß-cyclodextrin and pH changes). The gradual reconstruction of functionalized PEG-b-PVDMA BCP nanoparticles caused by hydrolysis of residual azlactone groups provides a novel method to engineer sub-50 nm, well-dispersed, stimuli-responsive nanoparticles. These nanoparticles can incorporate molecular cargoes and release them upon external stimuli, making the azlactone-containing BCPs attractive platforms for the development of controlled delivery vehicles.