Structuring and Shaping of Mechanically Robust and Functional Hydrogels toward Wearable and Implantable Applications.

Hydrogels possess unique features such as softness, wetness, responsiveness, and biocompatibility, making them highly suitable for biointegrated applications that have close interactions with living organisms. However, conventional man-made hydrogels are usually soft and brittle, making them inferior to the mechanically robust biological hydrogels. To ensure reliable and durable operation of biointegrated wearable and implantable devices, mechanical matching and shape adaptivity of hydrogels to tissues and organs are essential. Recent advances in polymer science and processing technologies have enabled mechanical engineering and shaping of hydrogels for various biointegrated applications. In this review, polymer network structuring strategies at micro/nanoscales for toughening hydrogels are summarized, and representative mechanical functionalities that exist in biological materials but are not easily achieved in synthetic hydrogels are further discussed. Three categories of processing technologies, namely, 3D printing, spinning, and coating for fabrication of tough hydrogel constructs with complex shapes are reviewed, and the corresponding hydrogel toughening strategies are also highlighted. These developments enable adaptive fabrication of mechanically robust and functional hydrogel devices, and promote application of hydrogels in the fields of biomedical engineering, bioelectronics, and soft robotics.

Fiber-spinning Asymmetric Assembly for Janus-structured Bifunctional Nanofiber Films towards All-Weather Smart Textile.

Given health threat by global warming and increased energy consumption in regulating body temperature, it is an urgent need to construct smart temperature-regulating materials. Herein, a novel fiber-spinning asymmetric chemical assembly (FACA) method is proposed to construct nanofiber materials with asymmetric photothermal properties. The silver nanowires (AgNWs) and poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) with opposite thermal radiation are assembled on reduced graphene oxide (rGO) film, imparting AgNW/rGO/PVDF-HFP film with Janus structure that can realize the AgNWs side consistently keeps temperature of ca. 11 °C lower than the side of PVDF-HFP nanofiber regardless of the irradiation directions under 1 sun, suggesting the adjustable photothermal regulation. Such photothermally selective hybrid nanofiber film provides great potential as fabrics to achieve all-weather smart clothes, promoting controllable and comprehensive utilization of solar energy.

Conformal Microfluidic-Blow-Spun 3D Photothermal Catalytic Spherical Evaporator for Omnidirectional Enhanced Solar Steam Generation and CO2 Reduction.

Solar-driven water evaporation and valuable fuel generation is an environmentally friendly and sustainable way for clean water and energy production. However, a few bottlenecks for practical applications are high-cost, low productivity, and severe sunlight angle dependence. Herein, solar evaporation with enhanced photocatalytic capacity that is light direction insensitive and of efficiency breakthrough by virtue of a three-dimensional (3D) photothermal catalytic spherical isotopic evaporator is demonstrated. A homogeneous layer of microfluidic blow spun polyamide nanofibers loaded with efficient light absorber of polypyrrole nanoparticles conformally wraps onto a lightweight, thermal insulating plastic sphere, featuring favorable interfacial solar heating and efficient water transportation. The 3D spherical geometry not only guarantees the omnidirectional solar absorbance by the light-facing hemisphere, but also keeps the other hemisphere under shadow to harvest energy from the warmer environment. As a result, the light-to-vapor efficiency exceeds the theoretical limit, reaching 217% and 156% under 1 and 2 sun, respectively. Simultaneously, CO2 photoreduction with generated steam reveals a favorable clean fuels production rate using photocatalytic spherical evaporator by secondary growth of Cu2 O nanoparticles. Finally, an outdoor demonstration manifests a high evaporation rate and easy-to-perform construction on-site, providing a promising opportunity for efficient and decentralized water and clean fuel production.

Self-contained Janus Aerogel with Antifouling and Salt-Rejecting Properties for Stable Solar Evaporation.

Janus structural interfacial vaporization by separating the solar absorber from the bulk working fluid has attracted tremendous attention due to its low heat losses and high solar conversion efficiency for desalination, water purification, energy generation, etc. However, a totally separated double-deck structure with a discontinuous interfacial transition and inefficient photothermic materials undermines its long-term use and large-scale practical exploitation. Herein, a low-cost Janus monolithic chitosan aerogel with continuous aligned run-through microchannels has been demonstrated to have a highly efficient photothermic effect on seawater desalination and wastewater purification. The top solar absorber layer enhances broadband light absorption and photothermal conversion efficiency via the multiple internal reflection of incident light in the aligned microchannels. Moreover, the insulating/hydrophilic bottom layer promotes water transportation and heat localization, and simultaneously prevents salt/fouling accumulation. As a result, a long-term solar vaporization rate of ∼1.76 kg m-2 h-1 is achieved, corresponding to a light-to-vapor efficiency of ∼91% under 1 sun irradiation. Notably, the large-vessel microchannels throughout the aerogel and favorable swelling property provide sufficient water replenishment and storage for completely isolating self-contained evaporation, illustrating an enhanced and time-extended self-contained solar steam generation. Such a low-cost bilayer aerogel with remarkable cycling stability in various fluids offers potential opportunities for freshwater production in remote rural areas.