Photoswitchable Liquid‐to‐Solid Transition of Azobenzene‐Decorated Polysiloxanes

Tol, Joost J. B. van der; Engels, Tap Tom; Cardinaels, Ruth; Vantomme, Ghislaine; Meijer, E. W.; Eisenreich, Fabian

doi:10.1002/adfm.202301246

Cited by 19 publications

(1 citation statement)

References 45 publications

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“…Some interesting work about photoswitchable adhesives shows that the reversible change in the polymer structure upon light irradiation gives rise to the change in adhesion. 34,35 In contrast, photopolymerizable adhesives undergo in situ efficient polymerization from the monomer to the polymer for achieving adhesion. Yet, it is still challenging to construct outstanding photo-polymerized adhesives with strong adhesion for both smooth and rough surfaces.…”

Section: Introductionmentioning

confidence: 99%

Wetting-enhanced adhesion of photo-polymerized supramolecular adhesives for both smooth and rough surfaces

Zhao,

Wu,

Zeng

et al. 2024

Chem. Sci.

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Section: Introductionmentioning

confidence: 99%

Wetting-enhanced adhesion of photo-polymerized supramolecular adhesives for both smooth and rough surfaces

Zhao,

Wu,

Zeng

et al. 2024

Chem. Sci.

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Optical Monitoring of Supramolecular Interactions in Polymers

Kiebala,

Dodero,

Weder

et al. 2024

Angewandte Chemie

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Many stimuli‐responsive materials harness the reversible association of supramolecular binding motifs to enable advanced functionalities such as self‐healing, switchable adhesion, or mechanical adaptation. Despite extensive research into the structure‐property relationships of these materials, direct correlations between molecular‐level changes in supramolecular binding and macroscopic material behaviors have mostly remained elusive. Here, we show that this challenge can be overcome with supramolecular binding motifs featuring integrated binding indicators. We demonstrate this using a novel motif that combines a hydrogen‐bonding ureido‐4‐pyrimidinone (UPy) with two strategically placed pyrene fluorophores. Dimerization of this motif promotes pyrene excimer formation, facilitating the straightforward optical quantification of supramolecular assembly under various conditions. We exploit the new motif as a supramolecular cross‐linker in poly(methyl acrylate)s to probe the extent of (dis)assembly as a function of cross‐linker content, processing history, and applied stimuli. We demonstrate that the stimuli‐induced dissociation of supramolecular linkages strongly depends on the initial cross‐link density, which also dictates whether the force‐induced dissociation in polymer films correlates with the applied stress or strain. Thus, beyond introducing a robust tool for the in‐situ study of dynamic (dis)assembly mechanisms in supramolecular systems, our findings provide new insights into the mechanoresponsive behavior of such materials.

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Closed‐Loop Recyclable and Totally Renewable Liquid Crystal Networks with Room‐Temperature Programmability and Reconfigurable Functionalities

Zhang,

Liu

2024

Angewandte Chemie

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Dynamic covalent liquid crystal networks (DCv‐LCNs) with straightforward (re)programmability, reprocessability, and recyclability facilitates the manufacture of sophisticated LCN actuators and intelligent robots. However, the DCv‐LCNs are still limited to heat‐assisted programming and polymer‐to‐polymer reprocessing/recycling, which inevitably lead to deterioration of the LCN structures and the actuation performances after repeated programming/processing treatments, owing to the thermal degradation of the polymer network and/or external agent interference. Here, a totally renewable azobenzene‐based DCv‐LCN with room‐temperature programmability and polymer‐to‐monomers chemical recyclability is reported, which was synthesized by crosslinking the azobenzene‐containing dibenzaldehyde monomer and the triamine monomer via the dynamic and dissociable imine bonds. Thanks to the water‐activated dynamics of the imine bonds, the resultant DCv‐LCN can be simply programmed, upon water‐soaking at room temperature, to yield a UV‐Vis light‐driven actuator. Importantly, the reported DCv‐LCN undergoes depolymerization in an acid‐solvent medium at room temperature because of the acid‐catalyzed hydrolysis of the imine bonds, giving rise to easy separation and recovery of both monomers in high purity, even with tolerance to additives. The recovered pure monomers can be used to regenerate totally new DCv‐LCNs and actuators, and their functionalities can be reconfigured by removing old and introducing new additives, by implementing the closed‐loop polymer‐monomers‐polymer recycling.

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Photoswitchable Liquid‐to‐Solid Transition of Azobenzene‐Decorated Polysiloxanes

Cited by 19 publications

References 45 publications

Wetting-enhanced adhesion of photo-polymerized supramolecular adhesives for both smooth and rough surfaces

Wetting-enhanced adhesion of photo-polymerized supramolecular adhesives for both smooth and rough surfaces

Optical Monitoring of Supramolecular Interactions in Polymers

Closed‐Loop Recyclable and Totally Renewable Liquid Crystal Networks with Room‐Temperature Programmability and Reconfigurable Functionalities

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