The development of waterproof ionogels with high stretchability and fast self-healing performance is essential for stretchable ionic conductors in sophisticated skin-inspired wearable sensors but can be rarely met in one material. Herein, a semicrystalline fluorinated copolymer ionogel (SFCI) with extremely high stretchability, underwater stability, and fast self-healability was fabricated, among which hydrophobic ionic liquids ([BMIM]­[TFSI]) were selectively enriched in fluoroacrylate segment domains of the fluorinated copolymer matrix through unique ion–dipole interactions. Benefiting from the reversible ion–dipole interactions between the [BMIM]­[TFSI] and fluoroacrylate segment domains as well as the physical cross-linking effects of semicrystalline oligoethylene glycol domains, the SFCI exhibited ultrastretchability (>6000%), fast room-temperature self-healability (>96% healing efficiency after cutting and self-healing for 30 min), and outstanding elasticity. In addition, the representative SFCI also exhibited high-temperature tolerance up to 300 °C, antifreezing performance as low as −35 °C, and high transparency (>93% visible-light transmittance). As a result, the as-obtained SFCI can readily be used as a highly stretchable ionic conductor in skin-inspired wearable sensors with waterproof performance for real-time detecting physiological human activities. These attractive features illustrate that the developed ultrastretchable and rapidly self-healable ionogels with unique waterproofness are promising candidates especially for sophisticated wearable strain sensing applications in complex and extreme environments.

The development of ionic conductors with extreme stretchability, superior ionic conductivity, and harsh‐environment resistance is urgent while challenging because the tailoring of these performances is mutually exclusive. Herein, a hydrophobicity‐constrained association strategy is presented for fabricating a liquid‐free ion‐conducting fluorinated elastomer (ICFE) with microphase‐separated structures. Hydrophilic nanodomains with long‐range ordering and selectively enriched Li ions provided high‐efficient conductive pathways, yielding impressive room‐temperature ionic conductivity of 3.5 × 10–3 S m–1. Hydrophobic nanodomains with abundant and reversible hydrogen bonds endow the ICFE with superior damage‐tolerant performances including ultrastretchability (>6000%), large toughness (17.1 MJ m–3) with notch insensitivity, antifatigue ability, and high‐efficiency self‐healability. Due to its liquid‐free characteristic and surface‐enriched hydrophobic nanodomains, the ICFE demonstrates an extreme temperature tolerance (−20 to 300 °C) and unique underwater resistance. The resultant ICFE is assembled into a proof‐of‐concept skin‐inspired sensor, showing impressive capacitive sensing performance with high sensitivity and wide‐strain‐range linearity (gauge factor to 1.0 in a strain range of 0–350%), excellent durability (>1000 cycles), and unique waterproofness in monitoring of complex human motions. It is believed that the hydrophobicity‐constrained association method boosts the fabrication of stretchable ionic conductors holding a great promise in skin‐inspired ionotronics with harsh‐environment tolerance.

No abstract

Harvesting water from air in sorption‐based devices is a promising solution to decentralized water production, aiming for providing potable water anywhere, anytime. This technology involves a series of coupled processes occurring at distinct length scales, ranging from nanometer to meter and even larger, including water sorption/desorption at the nanoscale, condensation at the mesoscale, device development at the macroscale and water scarcity assessment at the global scale. Comprehensive understanding and bespoke designs at every scale are thus needed to improve the water‐harvesting performance. For this purpose, a brief introduction of the global water crisis and its key characteristics is provided to clarify the impact potential and design criteria of water harvesters. Next the latest molecular‐level optimizations of sorbents for efficient moisture capture and release are discussed. Then, novel microstructuring of surfaces to enhance dropwise condensation, which is favorable for atmospheric water generation, is shown. After that, system‐level optimizations of sorbent‐assisted water harvesters to achieve high‐yield, energy‐efficient, and low‐cost water harvesting are highlighted. Finally, future directions toward practical sorption‐based atmospheric water harvesting are outlined.