Role of supramolecular polymers in photo-actuation of spiropyran hydrogels

Li, Chuang; Xiong, Qinsi; Clemons, Tristan D.; Sai, Hiroaki; Yang, Yang; Sangji, M. Hussain; Iscen, Aysenur; Palmer, Liam C.; Schatz, George C.; Stupp, Samuel I.

doi:10.1039/d3sc00401e

Cited by 5 publications

(1 citation statement)

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“…The photothermal effect differs little in what it can accomplish from a regular heat stimulus, but requires the appropriate light-responsive chemistry. Another capability is photochromism, where light irradiation results in a color change of the material, often through the incorporation of a light-responsive moiety such as spiropyran, which can convert between ring-closed and ring-opened states. ,− Moreover, this reversible, light-triggered structural conversion of spiropyran is accompanied by a change in its hydrophilicity which can be leveraged as a molecular actuator, inducing shape changes in materials. ,− Another photoresponsive group is anthracene, which can reversibly dimerize under light stimulus, serving as an on/off switch for cross-linking. ,− One of the most frequently encountered light-responsive compounds is azobenzene which can convert between cis and trans isomers via light irradiation or produce heat through the photothermal effect. ,,,, Additionally, liquid crystals, which provide anisotropic properties, including optical properties, also frequent the literature around light-responsive materials. ,,, …”

Section: Stimuli-responsesmentioning

confidence: 99%

Stimuli-Responsive Polymer Networks: Application, Design, and Computational Exploration

Rosario,

2024

ACS Appl. Polym. Mater.

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Polymer networks are an extensively studied class of materials, a subset of which has been developed to respond to specific stimuli. These stimuli-responses can be harnessed for enhanced or innovative functionalities, rendering stimuli-responsive polymer network materials highly desired for a myriad of applications ranging from sensing to drug delivery. This review provides a summary of recent progress in design and application of stimuli-responsive polymer network materials, including both chemically and physically cross-linked networks. Temperature, light, pH, chemical, mechanical, and more stimuli are discussed in the context of achieving desirable responses and functionalities in polymer networks. Furthermore, application areas for these materials and their various responses are also delved into with a particular focus on soft robotics and biomedical applications. In addition, computational methodologies are introduced as indispensable, complementary strategies to experimental characterization and analysis for further advancement and exploration within this domain. Techniques such as density functional theory, molecular dynamics simulations, Monte Carlo simulations, and finite element analysis are discussed. Ultimately, insights obtained from the perspectives of chemistry, stimuli, materials design, and computational methods offer a promising trajectory for the ongoing evolution and potential impact of this field.

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Section: Stimuli-responsesmentioning

confidence: 99%

Stimuli-Responsive Polymer Networks: Application, Design, and Computational Exploration

Rosario,

2024

ACS Appl. Polym. Mater.

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Saltwater‐Induced Rapid Gelation of Photoredox‐Responsive Mucomimetic Hydrogels

Zhang,

Li,

Trick

et al. 2023

Advanced Materials

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Shear‐thinning hydrogels represent an important class of injectable soft materials that are often used in a wide range of biomedical applications. Creation of new shear‐thinning materials often requires that factors such as viscosity, injection rate/force, and needle gauge be evaluated to achieve efficient delivery, while simultaneously protecting potentially sensitive cargo. Here, a new approach to establishing shear‐thinning hydrogels is reported where a host–guest cross‐linked network initially remains soluble in deionized water but is kinetically trapped as a viscous hydrogel once exposed to saltwater. The shear‐thinning properties of the hydrogelis then “switched on” in response to heating or exposure to visible light. These hydrogels consist of polynorbornene‐based bottlebrush copolymers with porphyrin‐ and oligoviologen‐containing side chains that are cross‐linked through the reversible formation of β‐cyclodextrin–adamantane inclusion complexes. The resultant viscous hydrogels display broad adhesive properties across polar and nonpolar substrates, mimicking that of natural mucous and thus making it easier to distribute onto a wide range of surfaces. Additional control over the hydrogel's mechanical properties (storage/loss moduli) and performance (adhesion) is achieved post‐injection using a low‐energy (blue light) photoinduced electron‐transfer process. This work envisions these injectable copolymers and multimodal hydrogels can serve as versatile next‐generation biomaterials capable of light‐based mechanical manipulation post‐injection.

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Blue Light Controlled Supramolecular Soft Robotics of Phenylazothiazole Amphiphiles for Rapid Macroscopic Actuations

Chau,

Wong,

Kajitani

et al. 2024

Advanced Science

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Nature preprograms sophisticated processes in operating molecular machines at the nanoscale, amplifying the molecular motion across multiple length‐scales, and controlling movements in living organisms. Supramolecular soft robotics serve as a new alternative to hard robotics, are able to transform and amplify collective motions of the supramolecularly assembled molecular machines in attaining macroscopic motions, upon photoirradiation. By taking advantage of oriented supramolecular macroscopic soft scaffold, here the first rapid macroscopic movements of supramolecular robotic materials driven by visible light are presented. Head‐tail amphiphilic structure is designed with the phenylazothiazole motif as the photoswitching core. Unidirectionally aligned nanostructures of the amphiphilic phenylazothiazoles are controlled by non‐invasive blue light irradiation and bends toward the light source, demonstrating a fast macroscopic actuation of supramolecular robotic systems (up to 17° s−1) in aqueous media. Through meticulous X‐ray diffraction and electron microscopy analyzes, macroscopic actuation mechanism is illustrated in a tight relation to molecular geometric transformations upon photoisomerization. By elucidating the key macroscopic actuation parameters, this paves the way for the next generation design of supramolecular soft robotic systems with enhanced biomimetic actuating functions.

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Role of supramolecular polymers in photo-actuation of spiropyran hydrogels

Abstract: Supramolecular-covalent hybrid polymers have been shown to be interesting systems to generate robotic functions in soft materials in response to external stimuli. In recent work supramolecular components were found to...

Cited by 5 publications

References 53 publications

Stimuli-Responsive Polymer Networks: Application, Design, and Computational Exploration

Stimuli-Responsive Polymer Networks: Application, Design, and Computational Exploration

Saltwater‐Induced Rapid Gelation of Photoredox‐Responsive Mucomimetic Hydrogels

Blue Light Controlled Supramolecular Soft Robotics of Phenylazothiazole Amphiphiles for Rapid Macroscopic Actuations

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