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Abstract: This work highlights the usage of short electrospun fibers for the first time for the preparation of homogeneous polymer nanofiber/polymer composites and the improvement in mechanical properties by an order to magnitude compared to as-electrospun long and continuous nanofibers. Dispersions of short electrospun nanofibers can be processed by liquid processing techniques resulting in nanofiber nonwovens similar to electrospun nonwovens but is independent from the demands of the electrospinning process is one of the emphasis of this work. The re-formation of electrospun fiber nonwovens by dispersion casting of short electrospun polyimide (PI) nanofibers and the preparation of homogeneous polymer/polymer nanofiber composite films were selected as representative examples for showing the versatility of short electrospun fibers. The self-reinforced PI/PI-short nanofiber composite films were obtained from mixtures of short electrospun PI nanofibers and polyamic acid after imidization. Significant improvement of 53% and 87% in mechanical properties like tensile strength and modulus, respectively in comparison to the neat PI film was observed by using just 2wt% of short fibers. Parallel experiments were also carried out with long and continuous electrospun PI fibers and amazingly a huge difference was observed. The amount of continuously long fibers required for achieving almost the same strength was much higher i.e. 38wt% in comparison to the 2wt% required of short fibers. [Copyright &y& Elsevier]

• PPy-coated P(NIPAM-ABP) electrospun nanofiber can provide high strength. • PPy-coating by in situ polymerization can provide high light-responsive. • The actuator owns ultrafast deformation and rapid recovery. • The actuator can realize various 3D programmable complex deformations. • We have explored new biomimetic devices based on the advantages of the actuator. Intelligent hydrogels are promising for biomimetic actuators, but acquiring actuations with both high speed and powerful force is still extremely difficult. Herein, a new robust polypyrrole (PPy)-coated copoly(isopropylacrylamide-4-benzoylphenyl acrylate) [P(NIPAM-ABP)] electrospun light-responsive hydrogel is explored. The (PPy)-coated P(NIPAM-ABP) hydrogel can be obtained via in-situ polymerization of pyrroles on the nanofiber-oriented electrospun P(NIPAM-ABP) hydrogel. Compared with original P(NIPAM-ABP) hydrogel, this PPy-coated P(NIPAM-ABP) hydrogel can integrate highly-enhanced mechanical strength (from 1.21 to 5.12 MPa of tensile strength) and ultrahigh-efficiency of photothermal conversion together. In addition, the orientation of P(NIPAM-ABP) nanofibers can still maintain well for programmable complex deformations. Consequently, the as-prepared robust bi-hydrogel actuator with ultrafast and complex deformations has been achieved, through bonding the PPy-P(NIPAM-ABP) hydrogel membrane with a polyethylene glycol diacrylate-cellulose nanofiber (PEGDA-CNF) composite hydrogel membrane via interfacial ultraviolet (UV) polymerization of PEGDA monomers. Several light-responsive biomimetic actuating devices have been achieved, which owning powerful force (can grab up 100 times of self-weight), rapid speed (1285.71°/s of folding) or precisely programmable complex deformations. Furthermore, two biomimetic devices with synergistic functions of the three advantages above have been explored, which can mimic the child's sit-up and the starfish's continuous crawling movement respectively. This work provides a robust remotely-controlled light-responsive hydrogel actuator with powerful force, ultrafast speed and programmable complex actuations, which will inspire the design and fabrication of novel soft biomimetic actuating materials and systems. [ABSTRACT FROM AUTHOR]

• A new double-network hydrogel is explored for uranium recovery from seawater. • U-adsorption capacity of the hydrogel is greatly enhanced by added nanoclay. • Mechanical property of the hydrogel is largely improved by th double-network. • Used materials are lowcost and the hydrogel owns good U-adsorption reusability. Massive uranium recovery from seawater is a key project to provide the long-time consumption of global nuclear power, while it is still greatly difficult to achieve high-efficient adsorbents with high mechanical property. In this work, a new nanoclay-poly(amidoxime) (NC-PAO) high-strength double-network (DN) composite hydrogel adsorbent with high-efficient and fast uranium extraction capacity has been explored. The uranium adsorbing performance can be significantly enhanced by the small content of added super-hydrophilic NC (Laponite RDS sheets), because of the largely improved hydrophilicity of the hydrogel. Compared with the blank PAO DN hydrogel without nanoclay, the uranium adsorbing capacity of this NC-PAO DN hydrogel can largely increase 73.4% from 4.97 mg/g to 8.62 mg/g, after in seawater only 25 days. The uranium adsorption rate of this hydrogel from natural seawater, can reached 0.345 mg/(g∙day), which is excellent among existing uranium adsorbents. Furthermore, this hydrogel has high mechanical performance with 2.42 MPa of tensile strength and 16.13 MPa of compressive strength, which can be used in seawater for relatively longer time than traditional low-strength single-network hydrogel, owing to its double network (DN) structure (the weakly crosslinked gelatin soft network and the strongly crosslinked cellulose nanofiber (CNF) hard network). This NC-PAO DN hydrogel adsorbent will be an excellent candidate for fast uranium recovery from seawater in largescale. Most importantly, this work will inspire the development of new hydrogel-based adsorbents and even other type of adsorbents for high-efficient uranium extraction, through compositing various low-cost and super-hydrophilic nanomaterials to significantly improve the hydrophilicity of the adsorbent and designing double-network structure to largely enhance the mechanical property. [ABSTRACT FROM AUTHOR]

• Single PI/rGO composite nanofiber by in-situ polymerization and in-situ thermal conversion. • Tensile strength of single nanofiber up to 4.2 GPa (PI/rGO-1.0% single nanofiber). • Modulus of single nanofiber up to 121 GPa (PI/rGO-1.2% single nanofiber). • Homogeneous dispersion of rGO by in-situ strategies. • In-situ strategies enhance the interfacial interaction between rGO and PI fibrous matrix. High mechanical performance electrospun polymeric nanofibers are highly desired for practical applications, especially as reinforcements for composites. However, most of the electrospun polymeric nanofibers present tensile strength < 3 GPa. To overcome such limitation, this work successfully prepared single rGO reinforced polyimide composite nanofiber with tensile strength up to 4.2 GPa (PI/rGO-1.0%) and modulus up to 121 GPa (PI/rGO-1.2%) by applying in-situ polymerization, electrospinning, and in-situ thermal conversion. These mechanical properties are higher than other polymer-based electrospun nanofibers, and 45% and 236% higher than those of neat PI single nanofiber, respectively. The in-situ strategies provide the homogeneous dispersion of rGO in single electrospun nanofibers and enhance the interfacial interaction between rGO and PI. In addition, the PI/rGO composite nanofibers also present excellent thermal stability with glass transition temperature (T g) > 295 °C, and the 5% thermal decomposition temperature (T 5%) > 539 °C. This work would open a new route for the preparation of high performance electrospun nanofibers for composites. [ABSTRACT FROM AUTHOR]