Abstract Hydrogels are explored for applications in agriculture, water purification, and biomedicine, leveraging softness, elasticity, and high water uptake. However, hydrogels are notoriously brittle, especially at high water content. This shortcoming puts the improvement of hydrogel mechanics at the forefront of current research. Yet modern strategies for enhancing gel resilience come at the expense of softness and swelling. This problem is addressed using bottlebrush networks with disentangled strands and hidden length reservoirs, which synergistically enhance gel swelling and robustness while maintaining their softness. Implementing a facile one‐pot synthesis of single‐stranded bottlebrush networks with a relatively hydrophobic poly(2‐hydroxyethyl methacrylate) (PHEMA) backbone and hydrophilic poly(2‐methyl‐2‐oxazoline) (PMOx) side chains, hydrogels are prepared with a modulus below <1 kPa and swelling ratios up to 125 that can withstand up to 10‐fold extension. 
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                            Hydrogels of arrested phase separation simultaneously achieve high strength and low hysteresis
                        
                    
    
            Hydrogels are being developed to bear loads. Applications include artificial tendons and muscles, which require high strength to bear loads and low hysteresis to reduce energy loss. However, simultaneously achieving high strength and low hysteresis has been challenging. This challenge is met here by synthesizing hydrogels of arrested phase separation. Such a hydrogel has interpenetrating hydrophilic and hydrophobic networks, which separate into a water-rich phase and a water-poor phase. The two phases arrest at the microscale. The soft hydrophilic phase deconcentrates stress in the strong hydrophobic phase, leading to high strength. The two phases are elastic and adhere through topological entanglements, leading to low hysteresis. For example, a hydrogel of 76 weight % water, made of poly(ethyl acrylate) and poly(acrylic acid), achieves a tensile strength of 6.9 megapascals and a hysteresis of 16.6%. This combination of properties has not been realized among previously existing hydrogels. 
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                            - Award ID(s):
- 2011754
- PAR ID:
- 10505136
- Publisher / Repository:
- Science
- Date Published:
- Journal Name:
- Science Advances
- Volume:
- 9
- Issue:
- 26
- ISSN:
- 2375-2548
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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