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A hydrogel is often fabricated from preexisting polymer chains by covalently crosslinking them into a polymer network. The crosslinks make the hydrogel swell‐resistant but brittle. This conflict is resolved here by making a hydrogel from a dough. The dough is formed by mixing long polymer chains with a small amount of water and photoinitiator. The dough is then homogenized by kneading and annealing at elevated temperatures, during which the crowded polymer chains densely entangle. The polymer chains are then sparsely crosslinked into a polymer network under an ultraviolet lamp, and submerged in water to swell to equilibrium. The resulting hydrogel is both swell‐resistant and tough. The hydrogel also has near‐perfect elasticity, high strength, high fatigue resistance, and low friction. The method is demonstrated with two widely used polymers, poly(ethylene glycol) and cellulose. These hydrogels have never been made swell‐resistant, elastic, and tough before. The method is generally applicable to synthetic and natural polymers, and is compatible with industrial processing technologies, opening doors to the development of sustainable, high‐performance hydrogels.

Here we report the use of a one-step process of reactive melt mixing to prepare starch-based superabsorbent polymers (SBSAPs) for the slow release of urea as a fertilizer. A modified twin-rotor mixer, with improved sealing to establish an oxygen-free environment, was used to study the chemical and physical reactions during the melt-processing through monitoring the temperature and torque. The effects of the initiator (ceric ammonium nitrate, or CAN), crosslinker (N,N'-methylene-bisacrylamide, or N,N'-MBA) and saponification agent (NaOH) under different reaction conditions (time, temperature, and shear intensity) were systematically studied. Also investigated was the effect of starch with different amylose content. Fourier-transform infrared (FTIR) spectroscopy and thermogravimetric analysis (TGA) confirmed that using this simple technique, SBSAPs were successfully prepared from either high-amylopectin starch (waxy corn starch) or high-amylose starch (Gelose 50) grafted with AM and crosslinked by N,N'-MBA. Gel strength was evaluated by rheometry, which revealed a significant increase in storage modulus (G') obtained in the crosslinked high-amylose SBSAP gels. Also, scanning electron microscopy (SEM) images showed a more sophisticated structural network with a smaller pore size in the crosslinked high-amylose gels. Urea as a fertilizer was embedded in the SBSAP gel network, and this network controlled the urea release in water. The release rate of urea depended on the gel strength, gel microstructure and water absorption capacity (WAC) of SAP, which was affected by the reaction conditions and degree of saponification.

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