Water-responsive shape-memory polymers (SMPs) are desirable for biomedical applications, but their limited shape recovery process is problematic. Herein, we demonstrate a shape-memory poly(vinyl alcohol) (SM-PVA) with programmable multistep shape recovery processes in water via a wettability contrast strategy. A hexamethyldisilazane (HMDS)-treated SiO nanoparticle layer with varying loading weights was rationally deposited onto the surface of SM-PVA, aiming to create surface-wettability contrast. The varying wettability led to different water adsorption behaviors of SM-PVA that could be well-described by the pseudo-first-order kinetic model. The results calculated from the kinetic model showed that both the pseudo-first order-adsorption rate constant and the saturated water absorption of SM-PVA demonstrated a declining trend as the loading weight of SiO increased, which laid the foundation for the local regulation of the water-responsive rate of SM-PVA. Finally, two proof-of-concept drug-delivery devices with diverse three-dimensional structures and actuations are presented based on the water-responsive SM-PVA with preprogrammed multistep shape recovery processes. We believe the programmable shape-memory behavior of water-responsive SM-PVA could highly extend its use in drug delivery, tissue engineering scaffolds, and smart implantable devices, etc.

A viable solution toward "green" optoelectronics is rooted in our ability to fabricate optoelectronics on transparent nanofibrillated cellulose (NFC) film substrates. However, the flammability of transparent NFC film poses a severe fire hazard in optoelectronic devices. Despite many efforts toward enhancing the fire-retardant features of transparent NFC film, making NFC film fire-retardant while maintaining its high transparency (≥90%) remains an ambitious objective. Herein, we combine NFC with NFC-dispersed monolayer clay nanoplatelets as a fire retardant to prepare highly transparent NFC-monolayer clay nanoplatelet hybrid films with a superb self-extinguishing behavior. Homogeneous and stable monolayer clay nanoplatelet dispersion was initially obtained by using NFC as a green dispersing agent with the assistance of ultrasonication and then used to blend with NFC to prepare highly transparent and self-extinguishing hybrid films by a water evaporation-induced self-assembly process. As the content of monolayer clay nanoplatelets increased from 5 wt % to 50 wt %, the obtained hybrid films presented enhanced self-extinguishing behavior (limiting oxygen index sharply increased from 21% to 96.5%) while retaining a ∼90% transparency at 600 nm. More significantly, the underlying mechanisms for the high transparency and excellent self-extinguishing behavior of these hybrid films with a clay nanoplatelet content of over 30 wt % were unveiled by a series of characterizations such as SEM, XRD, TGA, and limiting oxygen index tester. This work offers an alternative environmentally friendly, self-extinguishing, and highly transparent substrate to next-generation optoelectronics, and is aimed at providing a viable solution to environmental concerns that are caused by ever-increasing electronic waste.

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Carboxylated nanofibrillated cellulose extracted from wood fibers was used as a green dispersant to effectively disperse clay particles in water.