Stimuli responsive self-healing polymers: gels, elastomers and membranes

Amaral, A.P.; Pasparakis, George

doi:10.1039/c7py01386h

Cited by 155 publications

(107 citation statements)

References 185 publications

(192 reference statements)

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“…In contrast, the term inverse vulcanization, coined by Pyun, is generally applied to the process by which thermally generated polymeric sulfur radicals react with olefins in the rubber to form crosslinked materials that are generally comprised primarily of sulfur (Scheme ). The high sulfur‐content materials prepared by the inverse vulcanization process can also provide the added sustainability benefit of being healable and recyclable by merit of the thermal reversibility of S─S bond formation …”

Section: Introductionmentioning

confidence: 99%

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Combining agriculture and energy industry waste products to yield recyclable, thermally healable copolymers of elemental sulfur and oleic acid

Smith

Thiounn

Lyles

et al. 2019

J. Polym. Sci. Part A: Polym. Chem.

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Sulfur and oleic acid, two components of industrial waste/byproducts, were combined in an effort to prepare more sustainable polymeric materials. Zinc oxide was employed to serve the dual role of compatibilizing immiscible sulfur and oleic acid as well as to suppress evolution of toxic H2S gas during reaction at high temperature. The reaction of sulfur, oleic acid, and zinc oxide led to a series of composites, ZOSx (x = wt % sulfur, where x is 8–99). The ZOSx materials ranged from sticky tars to hard solids at room temperature. The ZOSx compositions were assessed by 1H NMR spectrometry, FTIR spectroscopy, and elemental microanalysis. Copolymers ZOS59‐99, were further analyzed for thermal and mechanical properties by thermogravimetric analysis, differential scanning calorimetry, and dynamic mechanical analysis. Remarkably, even ZOS99, comprising only 1 wt % of zinc oxide/oleic acid (99 wt % S) exhibits at least an eightfold increase in storage modulus compared to sulfur alone. The four solid samples (59–99 wt % S) were thermally healable and readily remeltable with full retention of mechanical durability. These materials represent a valuable proof‐of‐concept for sustainably sourced, recyclable materials from unsaturated fatty acid waste products. © 2019 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2019, 57, 1704–1710

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Section: Introductionmentioning

confidence: 99%

“…The high sulfur-content materials prepared by the inverse vulcanization process can also provide the added sustainability benefit of being healable and recyclable by merit of the thermal reversibility of S─S bond formation. 12,19,[48][49][50][51] Additional supporting information may be found in the online version of this article.…”

mentioning

confidence: 99%

Combining agriculture and energy industry waste products to yield recyclable, thermally healable copolymers of elemental sulfur and oleic acid

Smith

Thiounn

Lyles

et al. 2019

J. Polym. Sci. Part A: Polym. Chem.

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“…Finally, we demonstrate that these materials can be used as bulk cell encapsulants for cell delivery applications aimed to soft tissue engineering applications, [69][70][71][72] owing to the mild mixing and recovery conditions for their preparation and reconstruction. Such functionalities in terms of multi-responsiveness and healability, combined with excellent cytocompatible properties, have not been extensively exploited in previous boronic acid-based studies, 33,60,64,73 and hence, we anticipate that our study will be inspirational towards the development of functionally more complex, yet synthetically accessible, materials for the biomedical field.…”

Section: Introductionmentioning

confidence: 99%

“…32,33 Examples of such systems include the use of "smart" polymers, [34][35][36] the literature on sol-gel type of polymers and other forms of materials (i.e. low molecular weight gelators), 44 their use in the context of (remotely) healable systems has not been fully exploited despite the apparent advantages that they might convey: (1) their soft nature can be designed to match the mechanical properties of soft tissues, which renders them attractive candidates for (injectable) biomaterials design and/ or cell therapeutic implants; (2) they allow for (transient) malleability during their gel-sol transition implying that their capacity to flow at confined spaces could, potentially, eliminate the need for mechanical intervention during the re-joining/ repairing step, and (3) in principle, they can be doped with suitable fillers either to enrich them with additional functionalities of higher complexity or to reinforce their mechanical properties.…”

Section: Introductionmentioning

confidence: 99%

Transiently malleable multi-healable hydrogel nanocomposites based on responsive boronic acid copolymers

2018

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The design of materials that mimic aspects of self-healing, as observed in nature, is of paramount importance as they could solve a number of problems in the biomedical field, such as the elimination of (bio-) material failure after prolonged use, improved integration at the interface with living tissues and more robust biomechanical performance. In this report, we propose the fabrication of soft hydrogels comprising a polymer matrix of poly(vinyl alcohol) mixed with a thermoresponsive boronic acid copolymer that is subsequently impregnated with poly(vinyl pyrrolidone) coated gold nanoparticles. The gels are crosslinked by the formation of reversible boronate ester bonds that can be remotely disrupted by a thermal or optical stimulus, endowing the gels with thermally-induced transient malleability that is optically trackable. It is demonstrated that the gels exhibit excellent healing properties within minutes even without the application of external stimuli. The rapid formation of the gels in concert with their fast and mild gel-sol phase transition under biologically relevant conditions is demonstrated by the encapsulation and release of cells in vitro. The proposed materials constitute a versatile cytocompatible platform for the construction of remotely healable soft gels for biomedical applications.

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“…Healing materials are promising candidates to overcome this issue and to prolong materials shelf life due to their inherent ability to repair themselves. [135] The focus in this chapter is on lightinduced self healing properties of hydrogels. Hydrogels as biomimetic materials are predestined to attempt getting closer toward the astonishing selfrepairing properties of living tissue, e.g., in flax [133] or Delosperma cooperi succulent leaves.…”

Section: Healable Soft Materialsmentioning

confidence: 99%

Design and Applications of Photoresponsive Hydrogels

2019

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materials with diverse applications in var ious fields due to their tunable chemistry structure and physical properties as well as excellent biocompatibility. [2][3][4][5] Hydrogel research has evolved from static mate rials to smart ones, whose structures and property show responsiveness to external stimuli, including temperature, pH, light, electric or magnetic fields, and the pres ence of enzymes or ion concentrations. [6][7][8][9][10][11] This unprecedented level of control over material properties has driven both med ical and industrial fields into the realm of possibility: controlled drug delivery, [12] chemical sensors, [13] soft actuators or robotics, [14][15][16] or scaffolds for dynamic 3D cell culture. [17] Photoresponsiveness is attractive due to the inherent advan tages of light as stimulus. Light is non invasive and allows remote manipulation of materials without requiring additional reagents, thus, with limited byproducts. Modulation of irradiation parameters, such as light intensity and irradiation time, permits the pre cise control of irradiation dosage, thereby, the degree of photo reactions. Spatial control can be achieved in both 2D and 3D, and temporal control is possible by simply turning the respec tive light source on or off. Wavelengthselective photo chemical reactions can be used for orthogonal photomediation of hydrogel properties. [18] Photoresponsive hydrogels, as externally tunable materials, strongly contribute to the field of soft smart materials in regard to the abovementioned applications. [19] In this review, we elaborate on the design and the emerging appli cations of photoresponsive hydrogels. A comprehensive review about utilizing light for the formation of hydrogels is given by Mi and coworkers. [20] First, we discuss responsive modes and photochemical mechanisms of photoresponsive hydrogels. Fol lowing this, we highlight their applications for dynamic cell environments, smart biointerfaces, controlled drug delivery, photodriven actuators, and lighthealing materials. The review concludes with an outlook on the challenges and potential future approaches for photo responsive hydrogels. Light as Stimulus for Hydrogels Macroscopic Hydrogel PhotoresponsesThe interaction of light with photoresponsive hydrogels can result in different responses, some of which are observable with the bare eye. Those include hydrogel formation or degradation, network contraction or expansion, and chemical modifications in the network, which then have an immediate consequence on Hydrogels are the most relevant biochemical scaffold due to their tunable properties, inherent biocompatibility, and similarity with tissue and cell environments. Over the past decade, hydrogels have developed from static materials to "smart" responsive materials adapting to various stimuli, such as pH, temperature, chemical, electrical, or light. Light stimulation is particularly interesting for many applications because of the capability of contact-free remote manipulation of biomaterial properties and inherent spatial and t...

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Stimuli responsive self-healing polymers: gels, elastomers and membranes

Abstract: The development of responsive polymers with self-healing properties has expanded significantly which allow for the fabrication of complex materials in a highly controllable manner, for diverse uses in biomaterials science, electronics, sensors and actuators and coating technologies.

Cited by 155 publications

References 185 publications

Combining agriculture and energy industry waste products to yield recyclable, thermally healable copolymers of elemental sulfur and oleic acid

Combining agriculture and energy industry waste products to yield recyclable, thermally healable copolymers of elemental sulfur and oleic acid

Transiently malleable multi-healable hydrogel nanocomposites based on responsive boronic acid copolymers

Design and Applications of Photoresponsive Hydrogels

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