Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 136, Issue 19, Pages 6969-6977Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja500205v
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Funding
- NRSC-C
- Ministry of Education, Culture and Science [024.001.035]
- Netherlands Organization for Scientific Research (NWO)
- European Research Council, ERC [246829]
- BioMedical Materials institute [P1.03 PENT]
- Dutch Ministry of Economic Affairs
- European Research Council (ERC) [246829] Funding Source: European Research Council (ERC)
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Hydrogels were prepared with physical cross-links comprising 2-ureido-4[1H]-pyrimidinone (UPy) hydrogen-bonding units within the backbone of segmented amphiphilic macromolecules having hydrophilic poly(ethylene glycol) (PEG). The bulk materials adopt nanoscopic physical cross-links composed of UPy-UPy dimers embedded in segregated hydrophobic domains dispersed within the PEG matrix as comfirmed by cryo-electron microscopy. The amphiphilic network was swollen with high weight fractions of water (w(H2O) approximate to 0.8) owing to the high PEG weight fraction within the pristine polymers (W-PEG approximate to 0.9). Two different PEG chain lengths were investigated and illustrate the corresponding consequences of cross-link density on mechanical properties. The resulting hydrogels exhibited high strength and resilience upon deformation, consistent with a microphase separated network, in which the UPy-UPy interactions were adequately shielded within hydrophobic nanoscale pockets that maintain the network despite extensive water content. The cumulative result is a series of tough hydrogels with tunable mechanical properties and tractable synthetic preparation and processing. Furthermore, the melting transition of PEG in the dry polymer was shown to be an effective stimulus for shape memory behavior.
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