Ziyu Chen,Runhui Zhou,Jiaoya Huang,Huichen Xu,Zemin Li,Yushu Wang,Rongrong Bao,Jiang He,Caofeng Pan
The quest for stretchable properties is at the forefront of research dedicated to on-skin light–emitting devices. Inspired by the natural wonders of bioluminescence, electrochemiluminescent devices (ECLDs) are distinguished by straightforward design and reduced operating voltage, marking a departure from traditional current-driven electroluminescent devices (ACELDs). The primary challenge of fully-stretchable ECLDs lies in crafting electrodes that simultaneously satisfy the demands for conductivity, transparency, stretchability, oxidation resistance, and interface stability. This research introduces a groundbreaking wrinkled polymer-gold composite electrode. It extends to 50% stretchability, offers outstanding conductivity at 10 Ω sq −1 , achieves transparency above 60%, and withstands over 10 000 stretching cycles. Employing this material, alongside stretchable electrospinning fiber luminescent layers, enabled the creation of fully-stretchable ECLDs. These devices not only shine brightly at 30 Cd m −2 but also retain more than 90% of luminosity when stretched up to 50%. Furthermore, this work has engineered stretchable devices featuring singular patterns and multi-dot arrays. They exhibit consistent luminescent output under bending, twisting, and stretching when applied to skin. These findings not only highlight the potential of polymer-gold composite electrodes in overcoming challenges faced by stretchable electronic devices but also provide new ideas for wearable technology that seamlessly integrates with human body.
Biomimetic synthesis represents a cutting-edge topic in chemistry/materials science. Herein, we demonstrate poly(ethylene glycol) (PEG) short side-chain-assisted monomer complex coacervation and reaction-induced polyion complex compartmentalization that lead to oxygen-tolerant polymerization-induced electrostatic self-assembly (PIESA). This is achieved by the one-pot synthesis of a PEGylated anionic polyelectrolyte and heterogeneous iterative polymerization of a cationic monomer under ecofriendly ambient, in-air aqueous photo-RAFT conditions. Simultaneous reversible all-segment-participating ternary complex coacervation and Coulombic interdomain interactions lead to coacervate nanoreactors that are capable of immediate initiation and fast reversible addition–fragmentation chain transfer reactions. Approximately 2 nm monomer complex nanoclusters act as building blocks to drive liquid–liquid phase separation. Polymerization induces hierarchical self-assembly in a droplet nucleation–fusion–fission mechanism together with PEG-crowded polyion complex compartmentalization, using nanoclusters as building blocks, mechanistically similar to liquid–liquid phase separation through supramolecular polymerization. Consequently, protein-like, one-component multicompartment coacervate nanoreactors with oxygen-tolerant well-controlled fast reactions are achieved. This work provides important implications for the efficient precise synthesis of biomimetic coacervate nanodevices of increasing complexity.
Light-based three-dimensional (3D) bioprinting has been widely studied in tissue engineering. Despite the fact that free-radical chain polymerization-based bioinks like hyaluronic acid methacrylate (HAMA) and gelatin methacryloyl (GelMA) have been extensively explored in 3D bioprinting, the thiol–ene hydrogel system has attracted increasing attention for its ability in building hydrogel scaffolds in an oxygen-tolerant and cell-friendly way. Herein, we report a superfast curing thiol–ene bioink composed of norbornene-modified hyaluronic acid (NorHA) and thiolated gelatin (GelSH) for 3D bioprinting. A new facile approach was first introduced in the synthesis of NorHA, which circumvented the cumbersome steps involved in previous works. Additionally, after mixing NorHA with macro-cross-linker GelSH, the customized NorHA/GelSH bioinks exhibited fascinating superiorities over the gold standard GelMA bioinks, such as an ultrafast curing rate (1–5 s), much lowered photoinitiator concentration (0.03% w/v), and flexible physical performances. Moreover, the NorHA/GelSH hydrogel greatly avoided excess ROS generation, which is important for the survival of the encapsulated cells. Last, compared with the GelMA scaffold, the 3D-printed NorHA/GelSH scaffold not only exhibited excellent cell viability but also guaranteed cell proliferation, revealing its superior bioactivity. In conclusion, the NorHA/GelSH system is a promising candidate for 3D bioprinting and tissue engineering applications.
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