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Self-Healing Polymers and Composites

A special issue of International Journal of Molecular Sciences (ISSN 1422-0067). This special issue belongs to the section "Materials Science".

Deadline for manuscript submissions: closed (31 October 2022) | Viewed by 20035

Special Issue Editors


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Guest Editor
Research Center for Bio‐Based Chemistry, Korea Research Institute of Chemical Technology (KRICT), Ulsan, Korea
Interests: natural nanofibers; bio-based nanocomposites; rheology; mechanics; sustainable materials; bio-reneawable polmers; self-healing materials

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Guest Editor
Research Center for Bio‐Based Chemistry, Korea Research Institute of Chemical Technology (KRICT), Ulsan, Korea
Interests: bio-based nanomaterials; bio-based nanocomposites; all-organic nanocomposites; bioplastics; self-healing polymers; in situ polymerization

Special Issue Information

Dear Colleagues,

As regards sustainable materials, the field of self-healing polymers and composites has emerged, owing to the built-in ability of polymers to automatically repair damages. Research into polymer chemistry has widely developed this field, including the design of dynamic covalent bonds, supramolecular interactions, and macromolecular structures; engineering, including extrinsic healing agents, external stimuli, multi-phase systems; demonstration, including building materials, industrial sensors, wearable healthcare monitoring, and biomedical applications. Self-healing property prolongs the lifetime of products and reduces the costs associated with the repair of products.

Despite huge interest from academia, practical commercialization cases are still rare. To enhance their usefulness, the synergistic contributions mentioned above are still required, for example, breaking the trade-off between self-healing efficiency and mechanical performance, as well as the limits of self-healing applications by novel approaches.

This Special Issue on “Self-Healing Polymers and Composites” welcomes original research and reviews that advance this field with a focus on all aspects of the design of macromolecular structures, various characterizations, and diverse applications.

Dr. Dongyeop X. Oh
Dr. Jeyoung Park
Guest Editors

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Keywords

  • self-healing
  • dynamic covalent bonds
  • supramolecular interactions
  • healing agents
  • elastomers
  • hydrogels
  • composites
  • vitrimers
  • repair

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Published Papers (5 papers)

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Research

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18 pages, 13254 KiB  
Article
Room-Temperature Self-Healable Blends of Waterborne Polyurethanes with 2-Hydroxyethyl Methacrylate-Based Polymers
by Ioanna Tzoumani, Zacharoula Iatridi, Athena M. Fidelli, Poppy Krassa, Joannis K. Kallitsis and Georgios Bokias
Int. J. Mol. Sci. 2023, 24(3), 2575; https://doi.org/10.3390/ijms24032575 - 29 Jan 2023
Cited by 3 | Viewed by 2589
Abstract
The design of self-healing agents is a topic of important scientific interest for the development of high-performance materials for coating applications. Herein, two series of copolymers of 2-hydroxyethyl methacrylate (HEMA) with either the hydrophilic N,N-dimethylacrylamide (DMAM) or the epoxy group-bearing [...] Read more.
The design of self-healing agents is a topic of important scientific interest for the development of high-performance materials for coating applications. Herein, two series of copolymers of 2-hydroxyethyl methacrylate (HEMA) with either the hydrophilic N,N-dimethylacrylamide (DMAM) or the epoxy group-bearing hydrophobic glycidyl methacrylate were synthesized and studied as potential self-healing agents of waterborne polyurethanes (WPU). The molar percentage of DMAM or GMA units in the P(HEMA-co-DMAMy) and P(HEMA-co-GMAy) copolymers varies from 0% up to 80%. WPU/polymer composites with a 10% w/w or 20% w/w copolymer content were prepared with the facile method of solution mixing. Thanks to the presence of P(HEMA-co-DMAMy) copolymers, WPU/P(HEMA-co-DMAMy) composite films exhibited surface hydrophilicity (water contact angle studies), and tendency for water uptake (water sorption kinetics studies). In contrast, the surfaces of the WPU/P(HEMA-co-GMAy) composites were less hydrophilic compared with the WPU/P(HEMA-co-DMAMy) ones. The room-temperature, water-mediated self-healing ability of these composites was investigated through addition of water drops on the damaged area. Both copolymer series exhibited healing abilities, with the hydrophilic P(HEMA-co-DMAMy) copolymers being more promising. This green healing procedure, in combination with the simple film fabrication process and simple healing triggering, makes these materials attractive for practical applications. Full article
(This article belongs to the Special Issue Self-Healing Polymers and Composites)
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14 pages, 2804 KiB  
Article
Improving the Corrosion Protection of Poly(phenylene methylene) Coatings by Side Chain Engineering: The Case of Methoxy-Substituted Copolymers
by Marco F. D’Elia, Mirko Magni, Stefano P. M. Trasatti, Markus Niederberger and Walter R. Caseri
Int. J. Mol. Sci. 2022, 23(24), 16103; https://doi.org/10.3390/ijms232416103 - 17 Dec 2022
Cited by 2 | Viewed by 2051
Abstract
This work aims to improve the corrosion protection features of poly(phenylene methylene) (PPM) by sidechain engineering inserting methoxy units along the polymer backbone. The influence of side methoxy groups at different concentrations (4.6% mol/mol and 9% mol/mol) on the final polymer properties was [...] Read more.
This work aims to improve the corrosion protection features of poly(phenylene methylene) (PPM) by sidechain engineering inserting methoxy units along the polymer backbone. The influence of side methoxy groups at different concentrations (4.6% mol/mol and 9% mol/mol) on the final polymer properties was investigated by structural and thermal characterization of the resulting copolymers: co-PPM 4.6% and co-PPM 9%, respectively. Then, coatings were processed by hot pressing the polymers powder on aluminum alloy AA2024 and corrosion protection properties were evaluated exposing samples to a 3.5% w/v NaCl aqueous solution. Anodic polarization tests evidenced the enhanced corrosion protection ability (i.e., lower current density) by increasing the percentage of the co-monomer. Coatings made with co-PPM 9% showed the best protection performance with respect to both PPM blend and PPM co-polymers reported so far. Electrochemical response of aluminum alloy coated with co-PPM 9% was monitored over time under two “artificially-aged” conditions, that are: (i) a pristine coating subjected to potentiostatic anodic polarization cycles, and (ii) an artificially damaged coating at resting condition. The first scenario points to accelerating the corrosion process, the second one models damage of the coating potentially occurring either due to natural deterioration or due to any accidental scratching of the polymer layer. In both cases, an intrinsic self-healing phenomenon was indirectly argued by the time evolution of the impedance and of the current density of the coated systems. The degree of restoring to the “factory conditions” by co-polymer coatings after self-healing events is eventually discussed. Full article
(This article belongs to the Special Issue Self-Healing Polymers and Composites)
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22 pages, 6044 KiB  
Article
Glycidyl Methacrylate-Based Copolymers as Healing Agents of Waterborne Polyurethanes
by Ioanna Tzoumani, Amaia Soto Beobide, Zacharoula Iatridi, George A. Voyiatzis, Georgios Bokias and Joannis K. Kallitsis
Int. J. Mol. Sci. 2022, 23(15), 8118; https://doi.org/10.3390/ijms23158118 - 23 Jul 2022
Cited by 12 | Viewed by 2365
Abstract
Self-healing materials and self-healing mechanisms are two topics that have attracted huge scientific interest in recent decades. Macromolecular chemistry can provide appropriately tailored functional polymers with desired healing properties. Herein, we report the incorporation of glycidyl methacrylate-based (GMA) copolymers in waterborne polyurethanes (WPUs) [...] Read more.
Self-healing materials and self-healing mechanisms are two topics that have attracted huge scientific interest in recent decades. Macromolecular chemistry can provide appropriately tailored functional polymers with desired healing properties. Herein, we report the incorporation of glycidyl methacrylate-based (GMA) copolymers in waterborne polyurethanes (WPUs) and the study of their potential healing ability. Two types of copolymers were synthesized, namely the hydrophobic P(BA-co-GMAy) copolymers of GMA with n-butyl acrylate (BA) and the amphiphilic copolymers P(PEGMA-co-GMAy) of GMA with a poly(ethylene glycol) methyl ether methacrylate (PEGMA) macromonomer. We demonstrate that the blending of these types of copolymers with two WPUs leads to homogenous composites. While the addition of P(BA-co-GMAy) in the WPUs leads to amorphous materials, the addition of P(PEGMA-co-GMAy) copolymers leads to hybrid composite systems varying from amorphous to semi-crystalline, depending on copolymer or blend composition. The healing efficiency of these copolymers was explored upon application of two external triggers (addition of water or heating). Promising healing results were exhibited by the final composites when water was used as a healing trigger. Full article
(This article belongs to the Special Issue Self-Healing Polymers and Composites)
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14 pages, 4499 KiB  
Article
Toughening and Healing of CFRPs by Diels–Alder-Based Nano-Modified Resin through Melt Electro-Writing Process Technique
by Athanasios Kotrotsos, George Michailidis, Anna Geitona, Filippos Tourlomousis and Vassilis Kostopoulos
Int. J. Mol. Sci. 2022, 23(7), 3663; https://doi.org/10.3390/ijms23073663 - 27 Mar 2022
Cited by 3 | Viewed by 2021
Abstract
In the current study, a novel approach in terms of the incorporation of self-healing agent (SHA) into unidirectional (UD) carbon fiber reinforced plastics (CFRPs) has been demonstrated. More precisely, Diels–Alder (DA) mechanism-based resin (Bis-maleimide type) containing or not four layered graphene nanoplatelets (GNPs) [...] Read more.
In the current study, a novel approach in terms of the incorporation of self-healing agent (SHA) into unidirectional (UD) carbon fiber reinforced plastics (CFRPs) has been demonstrated. More precisely, Diels–Alder (DA) mechanism-based resin (Bis-maleimide type) containing or not four layered graphene nanoplatelets (GNPs) at the amount of 1 wt% was integrated locally in the mid-thickness area of CFRPs by melt electro-writing process (MEP). Based on that, CFRPs containing or not SHA were fabricated and further tested under Mode I interlaminar fracture toughness experiments. According to experimental results, modified CFRPs exhibited a considerable enhancement in the interlaminar fracture toughness properties (peak load (Pmax) and fracture toughness energy I (GIC) values). After Mode I interlaminar fracture toughness testing, the damaged samples followed the healing process and then were tested again under identical experimental conditions. The repeating of the tests revealed moderate healing efficiency (H.E.) since part of the interlaminar fracture toughness properties were restored. Furthermore, three-point bending (3PB) experiments were conducted, with the aim of assessing the effect of the incorporated SHA on the in-plane mechanical properties of the final CFRPs. Finally, optical microscopy (OM) examinations were performed to investigate the activated/involved damage mechanisms. Full article
(This article belongs to the Special Issue Self-Healing Polymers and Composites)
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Review

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40 pages, 79307 KiB  
Review
Self-Healing Materials for Electronics Applications
by Fouzia Mashkoor, Sun Jin Lee, Hoon Yi, Seung Man Noh and Changyoon Jeong
Int. J. Mol. Sci. 2022, 23(2), 622; https://doi.org/10.3390/ijms23020622 - 6 Jan 2022
Cited by 31 | Viewed by 9530
Abstract
Self-healing materials have been attracting the attention of the scientists over the past few decades because of their effectiveness in detecting damage and their autonomic healing response. Self-healing materials are an evolving and intriguing field of study that could lead to a substantial [...] Read more.
Self-healing materials have been attracting the attention of the scientists over the past few decades because of their effectiveness in detecting damage and their autonomic healing response. Self-healing materials are an evolving and intriguing field of study that could lead to a substantial increase in the lifespan of materials, improve the reliability of materials, increase product safety, and lower product replacement costs. Within the past few years, various autonomic and non-autonomic self-healing systems have been developed using various approaches for a variety of applications. The inclusion of appropriate functionalities into these materials by various chemistries has enhanced their repair mechanisms activated by crack formation. This review article summarizes various self-healing techniques that are currently being explored and the associated chemistries that are involved in the preparation of self-healing composite materials. This paper further surveys the electronic applications of self-healing materials in the fields of energy harvesting devices, energy storage devices, and sensors. We expect this article to provide the reader with a far deeper understanding of self-healing materials and their healing mechanisms in various electronics applications. Full article
(This article belongs to the Special Issue Self-Healing Polymers and Composites)
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