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Photoregulated supramolecular hydrogels driven by polyradical interactions
Institution:1. Key Laboratory of Thermo-Fluid Science and Engineering of Ministry of Education, School of Energy and Power Engineering, Frontier Institute of Science and Technology, Xi''an Jiaotong University, Xi''an 710054, China;2. School of Chemistry, Xi''an Key Laboratory of Sustainable Energy Materials Chemistry, Xi''an Jiaotong University, Xi''an 710049, China;3. School of Materials Science and Engineering, Xi''an Jiaotong University, Xi''an 710049, China;1. College of Chemistry and Chemical Engineering, Hunan University, Changsha 410082, China;2. College of Chemistry and Chemical Engineering, Central South University, Changsha 410083, China;1. Shanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai 200062, China;2. Joint Institute of Tobacco and Health, Yunnan Academy of Tobacco Science, Kunming 650024, China;3. Wuhu Hospital Affiliated to East China Normal University (The Second People''s Hospital of Wuhu), Wuhu 241001, China
Abstract:Organic radical as a powerful tool has been extensively applied in synthetic chemistry. However, harnessing radical-mediated noncovalent interactions to fabricate soft materials remains elusive. Here we report a new category of supramolecular hydrogel system held by multiple radical-radical (polyradical) interactions, and its photosensitive cross-linking structure. A simple polyacrylamide with triarylamine (TAA) pendants is designed as the precursor. The TAA units in polymer can be converted into active TAA?? radical cations with light and further associate each other via TAA???TAA?? stacking interactions to form stable supramolecular network. Temporal control of the light irradiation dictates the degree of radical stacks, thus regulating the mechanical performance of the resulting hydrogel materials on-demand. Moreover, the reversible collapse of this hydrogels can be promoted by adding radical scavenger or exerting reduction voltage.
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