Abstract 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. 
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                            Photoinitiator-grafted polymer chains for integrating hydrogels with various materials
                        
                    
    
            Hydrogels are commonly integrated with other materials. In the one-pot synthesis of a hydrogel coating, polymerization, crosslink, and interlink are concurrent. This concurrency, however, is often inapplicable for integrating hydrogels to other materials. For example, a permeable substrate will absorb small molecules in the solution, causing side reactions and even toxicity. Here, we report a method to break the concurrency by using photoinitiator-grafted polymer chains (PGPCs). A type of photoinitiator is copolymerized with various monomers. The PGPCs are uncrosslinked during syn- thesis, have long shelf lives in dark storage, and can be applied to a substrate by brush, cast, spin, dip, spray, or print. Under ultraviolet light, the polymer chains crosslink into a network and interlink with the substrate. The cured PGPC hydrogels are characterized by me- chanical tests. Furthermore, the PGPCs are demonstrated to adhere wet materials, form hydrophilic coatings on hydrophobic substrates, and pattern functional groups on permeable substrates. 
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                            - Award ID(s):
- 2011754
- PAR ID:
- 10501575
- Publisher / Repository:
- Cell Press
- Date Published:
- Journal Name:
- Cell Reports Physical Science
- Volume:
- 2
- Issue:
- 6
- ISSN:
- 2666-3864
- Page Range / eLocation ID:
- 100463
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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