Mendable polymers

Bergman, Sheba D.; Wudl, Fred

doi:10.1039/b713953p

Cited by 634 publications

(499 citation statements)

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“…4,5 In fact, selfhealing is currently one of the most active topics in materials science. [6][7][8] For polymers [9][10][11] and polymer coatings [12][13][14][15] several approaches have been reported to restore the integrity of the material, either by refilling the damaged areas, e.g., a) Electronic addresses: a.c.c.esteves@tue.nl and g.dewith@tue.nl via encapsulated reactive components (autonomous healing) or by reestablishing chemical bonds through reversible reactions triggered by external stimuli such as temperature, light or a pH switch (triggered healing). These approaches can use intrinsic healing concepts, [16][17][18][19] in which the healing agent is inherent to the material (i.e., is a part of the network or formulation) or extrinsic healing, where external components are added, such as filled capsules [20][21][22][23] or microvascular networks.…”

Section: Introductionmentioning

confidence: 99%

Self-replenishing ability of cross-linked low surface energy polymer films investigated by a complementary experimental-simulation approach

Esteves

Lyakhova

Riel

et al. 2014

The Journal of Chemical Physics

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Document VersionPublisher's PDF, also known as Version of Record (includes final page, issue and volume numbers) Please check the document version of this publication:• A submitted manuscript is the author's version of the article upon submission and before peer-review. There can be important differences between the submitted version and the official published version of record. People interested in the research are advised to contact the author for the final version of the publication, or visit the DOI to the publisher's website.• The final author version and the galley proof are versions of the publication after peer review.• The final published version features the final layout of the paper including the volume, issue and page numbers. Link to publication Citation for published version (APA):Esteves, A. C. C., Lyakhova, K., Riel, van, J. M., Ven, van der, L. G. J., Benthem, van, R. A. T. M., & With, de, G. (2014). Self-replenishing ability of cross-linked low surface energy polymer films investigated by a complementary experimental-simulation approach. Journal of Chemical Physics, 140, 1-9. [124902]. DOI: 10.1063/1.4868989 General rightsCopyright and moral rights for the publications made accessible in the public portal are retained by the authors and/or other copyright owners and it is a condition of accessing publications that users recognise and abide by the legal requirements associated with these rights.• Users may download and print one copy of any publication from the public portal for the purpose of private study or research.• You may not further distribute the material or use it for any profit-making activity or commercial gain • You may freely distribute the URL identifying the publication in the public portal ? Take down policyIf you believe that this document breaches copyright please contact us providing details, and we will remove access to the work immediately and investigate your claim. Nowadays, many self-healing strategies are available for recovering mechanical damage of bulk polymeric materials. The recovery of surface-dependent functionalities on polymer films is, however, equally important and has been less investigated. In this work we study the ability of low surface energy cross-linked poly(ester urethane) networks containing perfluorinated dangling chains to self-replenish their surface, after being submitted to repeated surface damage. For this purpose we used a combined experimental-simulation approach. Experimentally, the cross-linked films were intentionally damaged by cryo-microtoming to remove top layers and create new surfaces which were characterized by water Contact Angle measurements and X-Ray Photoelectron Spectroscopy. The same systems were simultaneously represented by a Dissipative Particles Dynamics simulation method, where the damage was modeled by removing the top film layers in the simulation box and replacing it by new "air" beads. The influence of different experimental parameters, such as the concentration of the low surface energy component and the molecular m...

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Section: Introductionmentioning

confidence: 99%

Self-replenishing ability of cross-linked low surface energy polymer films investigated by a complementary experimental-simulation approach

Esteves

Lyakhova

Riel

et al. 2014

The Journal of Chemical Physics

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“…Most approaches to healable materials require heating the damaged area [2][3][4] . Here we present metallosupramolecular polymers that can be mended through exposure to light.…”

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confidence: 99%

“…Metal-Mebip complexes were previously used to self-assemble polymeric materials [17][18][19][20][21] , and their optical properties seemed appropriate for optical healing 22 (see below). To probe how the metal ion affects the materials' properties, 3 was self-assembled with Zn(NTf 2 ) 2 Published in " " which should be cited to refer to this work. Small-angle X-ray scattering (SAXS) and transmission electron microscopy (TEM) studies of films of 3?…”

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confidence: 99%

Optically healable supramolecular polymers

Burnworth

Tang

Kumpfer

et al. 2011

Nature

1,622

1,327

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Polymers with the ability to repair themselves after sustaining damage could extend the lifetimes of materials used in many applications 1 . Most approaches to healable materials require heating the damaged area [2][3][4] . Here we present metallosupramolecular polymers that can be mended through exposure to light. They consist of telechelic, rubbery, low-molecular-mass polymers with ligand end groups that are non-covalently linked through metal-ion binding. On exposure to ultraviolet light, the metal-ligand motifs are electronically excited and the absorbed energy is converted into heat. This causes temporary disengagement of the metal-ligand motifs and a concomitant reversible decrease in the polymers' molecular mass and viscosity 5 , thereby allowing quick and efficient defect healing. Light can be applied locally to a damage site, so objects can in principle be healed under load. We anticipate that this approach to healable materials, based on supramolecular polymers and a light-heat conversion step, can be applied to a wide range of supramolecular materials that use different chemistries.The healing of cracks in amorphous polymers by heating above the glass transition temperature (T g ) involves surface rearrangement and approach of polymer chains, followed by wetting, diffusion and reentanglement of the chains 6 . Because the rates of the final two steps are inversely proportional to the molecular mass, healing is generally slow and inefficient. This problem can be overcome by exploiting thermally reversible, covalent bonds 7,8 or non-covalent supramolecular motifs 5,9,10 that allow the reaction equilibrium to be temporarily shifted to lower-molecular-mass species 11 on exposure to heat. This reduces the viscosity of the material, such that defects can be mended, before the equilibrium is shifted back and the polymer is reformed. Supramolecular polymers that phase separate into physically crosslinked networks (Fig. 1a) should be especially well suited for this purpose, because such morphologies generally bestow the material with high toughness. The supramolecular motifs can disengage in the solid state on exposure to heat or a competitive binding agent 12,13 , causing disassembly into small molecules 14 and viscosity reductions. Reporting a series of supramolecular materials formed by metal-ligand interactions, we demonstrate here that this architecture is an excellent basis for elastomeric materials in which defects can be efficiently repaired. We show that the use of light 15 as a stimulus for the dissociation of supramolecular motifs has distinct advantages over thermally healable systems, including the possibility of exclusively exposing and healing the damaged region.The new polymers are based on a macromonomer comprising a rubbery, amorphous poly(ethylene-co-butylene) core with 2,6-bis(19-methylbenzimidazolyl)pyridine (Mebip) ligands at the termini (Fig. 1b, 3). This design was based on the assumption that the hydrophobic core and the polar metal-ligand motif would phase separate 16 . Metal-Mebip com...

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“…[1][2][3] Due to the thermal reversibility of the retro-Diels-Alder (rDA) reaction, it is possible to obtain self-healing polymers with well-defined architectures and properties. [4,5] The DA reaction of furan and maleimide is the commonly used functional system for most reversible self-healing polymers of this type. However, the major drawback of the DA cycloaddition of maleimide and furan is the required high temperature (120 to 180°C) of the rDA reaction, resulting in self-healing materials that can only be healed when rather drastic conditions are applied.…”

Section: Introductionmentioning

confidence: 99%

Reversible oligomerization of 3-aryl-2-cyanothioacrylamides via [2_s + 4_s] cycloaddition to substituted 3,4-dihydro-2H-thiopyrans

Kötteritzsch

Bode

Yildirim

et al. 2015

Designed Monomers and Polymers

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(2015) Novel difunctional monomers are synthesized which are able to dimerize as well as oligomerize via the hetero-DielsAlder (HDA) mechanism. These monomers are based on 3-aryl-2-cyanothioacrylamides, which are used as functional units for the HDA reaction to form 3,4-dihydro-2H-thiopyrans. Different substituents of the aromatic ring are utilized to shift the equilibrium to the dimeric or oligomeric species. The HDA reaction is reversible and can be influenced by the temperature as well as the concentration. In contrast, the N,N-dimethylthioacrylamide analogues do not dimerize or the dimerization is not reversible. The most promising compound is furthermore investigated in detail by 1 H NMR spectroscopy to elucidate the dimerization kinetics. In addition, a difunctional molecule is able to oligomerize reversibly, as confirmed by means of 1 H NMR, size exclusion chromatography (SEC), and ESI MS measurements. A respective alcohol is employed as initiator for the ring-opening polymerization of L-lactide resulting in an end-functional polymer that undergoes reversible dimerization as confirmed by SEC measurements.

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Mendable polymers

Cited by 634 publications

References 160 publications

Self-replenishing ability of cross-linked low surface energy polymer films investigated by a complementary experimental-simulation approach

Self-replenishing ability of cross-linked low surface energy polymer films investigated by a complementary experimental-simulation approach

Optically healable supramolecular polymers

Reversible oligomerization of 3-aryl-2-cyanothioacrylamides via [2_s + 4_s] cycloaddition to substituted 3,4-dihydro-2H-thiopyrans

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Mendable polymers

Cited by 634 publications

References 160 publications

Self-replenishing ability of cross-linked low surface energy polymer films investigated by a complementary experimental-simulation approach

Self-replenishing ability of cross-linked low surface energy polymer films investigated by a complementary experimental-simulation approach

Optically healable supramolecular polymers

Reversible oligomerization of 3-aryl-2-cyanothioacrylamides via [2s + 4s] cycloaddition to substituted 3,4-dihydro-2H-thiopyrans

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Reversible oligomerization of 3-aryl-2-cyanothioacrylamides via [2_s + 4_s] cycloaddition to substituted 3,4-dihydro-2H-thiopyrans