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Polymers
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Advances in Self-Healing Polymer Composites
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Advances in Self-Healing Polymer Composites

A special issue of Polymers (ISSN 2073-4360). This special issue belongs to the section "Polymer Networks".

Deadline for manuscript submissions: 25 May 2025 | Viewed by 5379

Special Issue Editor

Dr. Alfonso Martone

E-Mail Website
Guest Editor
IPCB, Institute of Polymers, Composites and Biomaterials, CNR, Portici, Italy
Interests: nanocomposites; advanced materials; self-healing; cross-linking polymers; processing technologies of composite materials; chemical synthesis, preparation and characterization of self-healing materials

Special Issue Information

Dear Colleagues,

Increasing environmental awareness and industrial competitiveness encourages the introduction and development of repairable and recyclable structural materials that will reduce polymer waste and extend its service life. Introducing a thermoreversible covalent bond in the crosslinked backbone enables the topological reshuffling of polymeric networks, allowing us to rework and reform the crosslinked material. A well-established approach for the design and synthesis of covalent adaptable networks (CAN) is the dissociative Diels–Alder reaction, which takes place between furans and maleimides. As a further development in more easily reprocessable and self-healing thermosets, vitrimers are able to overcome the current drawbacks of CANs. One of the possible mechanisms enabling vitrimeric behaviour in epoxy resins is based on transesterification exchange reactions between esters and beta-hydroxyls formed by reacting epoxy precursors with suitable acids/anhydrides. A good balance between the mechanical performance and self-healing capacities can be also obtained via the precise regulation of the content of disulphide bonds, along with the number of hard segments.

Given the huge amount of unrecyclable waste from thermoset polymer-based products, the potential of the self-healing concept is highly attractive, as it meets the recently increasing demand to create polymers with an efficient end-of-life management.

This Special Issue aims to gather high-quality original research and reviews in the field of the synthesis and functional characterization of thermoreversible self-healing polymers and their applications.

Dr. Alfonso Martone
Guest Editor

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Polymers is an international peer-reviewed open access semimonthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2700 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • vitrimers
  • covalent adaptable networks
  • self-healing
  • creep
  • recyclability
  • reactive thermoset
  • dynamic bonds
  • shape memory

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Published Papers (4 papers)

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Research

32 pages, 19317 KiB  
Article
Nanoindentation Response of Structural Self-Healing Epoxy Resin: A Hybrid Experimental–Simulation Approach
by Giovanni Spinelli, Rosella Guarini, Evgeni Ivanov, Elisa Calabrese, Marialuigia Raimondo, Raffaele Longo, Liberata Guadagno and Luigi Vertuccio
Polymers 2024, 16(13), 1849; https://doi.org/10.3390/polym16131849 - 28 Jun 2024
Viewed by 956
Abstract
In recent years, self-healing polymers have emerged as a topic of considerable interest owing to their capability to partially restore material properties and thereby extend the product’s lifespan. The main purpose of this study is to investigate the nanoindentation response in terms of [...] Read more.
In recent years, self-healing polymers have emerged as a topic of considerable interest owing to their capability to partially restore material properties and thereby extend the product’s lifespan. The main purpose of this study is to investigate the nanoindentation response in terms of hardness, reduced modulus, contact depth, and coefficient of friction of a self-healing resin developed for use in aeronautical and aerospace contexts. To achieve this, the bifunctional epoxy precursor underwent tailored functionalization to improve its toughness, facilitating effective compatibilization with a rubber phase dispersed within the host epoxy resin. This approach aimed to highlight the significant impact of the quantity and distribution of rubber domains within the resin on enhancing its mechanical properties. The main results are that pure resin (EP sample) exhibits a higher hardness (about 36.7% more) and reduced modulus (about 7% more), consequently leading to a lower contact depth and coefficient of friction (11.4% less) compared to other formulations that, conversely, are well-suited for preserving damage from mechanical stresses due to their capabilities in absorbing mechanical energy. Furthermore, finite element method (FEM) simulations of the nanoindentation process were conducted. The numerical results were meticulously compared with experimental data, demonstrating good agreement. The simulation study confirms that the EP sample with higher hardness and reduced modulus shows less penetration depth under the same applied load with respect to the other analyzed samples. Values of 877 nm (close to the experimental result of 876.1 nm) and 1010 nm (close to the experimental result of 1008.8 nm) were calculated for EP and the toughened self-healing sample (EP-R-160-T), respectively. The numerical results of the hardness provide a value of 0.42 GPa and 0.32 GPa for EP and EP-R-160-T, respectively, which match the experimental data of 0.41 GPa and 0.30 GPa. This validation of the FEM model underscores its efficacy in predicting the mechanical behavior of nanocomposite materials under nanoindentation. The proposed investigation aims to contribute knowledge and optimization tips about self-healing resins. Full article
(This article belongs to the Special Issue Advances in Self-Healing Polymer Composites)
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15 pages, 6000 KiB  
Article
Verification of the Self-Healing Ability of PP-co-HUPy Copolymers in Epoxy Systems
by Elisa Calabrese, Marialuigia Raimondo, Andrea Sorrentino, Simona Russo, Pasquale Longo, Annaluisa Mariconda, Raffaele Longo and Liberata Guadagno
Polymers 2024, 16(11), 1509; https://doi.org/10.3390/polym16111509 - 27 May 2024
Cited by 1 | Viewed by 840
Abstract
This work concerns the verification of the self-healing ability of PP-co-HUPy copolymers dispersed in epoxy systems. PP is the acronym for the Poly-PEGMA polymer, and HUPy refers to the HEMA-UPy copolymers based on ureidopyrimidinone (UPy) moieties. In particular, this work aims to verify [...] Read more.
This work concerns the verification of the self-healing ability of PP-co-HUPy copolymers dispersed in epoxy systems. PP is the acronym for the Poly-PEGMA polymer, and HUPy refers to the HEMA-UPy copolymers based on ureidopyrimidinone (UPy) moieties. In particular, this work aims to verify whether this elastomer characterized by an intrinsic self-healing ability can activate supramolecular interactions among polymer chains of an epoxy resin, as in the elastomer alone. The elastomer includes a class of polyethylene glycol monomethyl ether methacrylate-based copolymers, with different percentages of urea-N-2-amino-4-hydroxy-6-methyl pyrimidine-N’-(hexamethylene-n-carboxyethyl methacrylate) (HEMA-UPy) co-monomers. The self-healing capability of these copolymers based on possible quadruple hydrogen bond interactions between polymer chains has been verified. The formulated epoxy samples did not show self-healing efficiency. This can be attributed to the formation of phase segregation that originates during the curing process of the samples, although the PP-co-HUPy copolymers are completely soluble in the liquid epoxy matrix EP. The morphological investigation highlighted the presence of crystals of PP-co-HUPy copolymers, which are in greater quantity in the sample containing the highest weight percentage (7.8 wt%) of HUPy units. Furthermore, the crystals act as promotors for increasing the curing degree (DC) of the epoxy systems containing HUPy units. DC goes from 91.6% for EP to 96.1% and 95.4% for the samples containing weight percentages of 2.5 and 7.8 wt% of HUPy units, respectively. Dynamic mechanical analysis (DMA) shows storage modulus values for epoxy systems containing PP-co-HUPy units lower than that of the unfilled resin EP. The values of maximum in Tan δ (Tg), representing the temperature at which the glass transition occurs, are 220 for the unfilled resin EP, 228 for the sample containing 2.5 wt% of HEMA-UPy units, and 211 for the sample containing 7.8 wt% of HEMA-UPy units. Full article
(This article belongs to the Special Issue Advances in Self-Healing Polymer Composites)
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21 pages, 5409 KiB  
Article
Self-Healing Properties of Water Tree with Microcapsule/Cross-Linked Polyethylene Composite Material Based on Three-Layer Core-Shell Structure
by Bo Zhu, Xinyu Tao, Hao Sun, Yaqi Zhu, Shengkun He and Ximu Han
Polymers 2024, 16(11), 1445; https://doi.org/10.3390/polym16111445 - 21 May 2024
Viewed by 779
Abstract
To overcome the degradation of insulating properties caused by the water tree aging of cross-linked polyethylene (XLPE), a self-repairing material for XLPE based on a microcapsule system is proposed. Three-layer shell nucleus microcapsules/XLPE composites with different microcapsule doping content are prepared. The water [...] Read more.
To overcome the degradation of insulating properties caused by the water tree aging of cross-linked polyethylene (XLPE), a self-repairing material for XLPE based on a microcapsule system is proposed. Three-layer shell nucleus microcapsules/XLPE composites with different microcapsule doping content are prepared. The water tree aging experiments are carried out using the water-needle electrode method to analyze the ability of microcapsules to repair the damaged areas of water trees. The results show that, compared with the XLPE material without microcapsules, the electrical properties of composites decline significantly when the doping concentration of three-layer shell nucleus microcapsules is large. When the doping concentration is 1.0 wt%, the microcapsule/XLPE composite breakdown strength has no noticeable change, and the dielectric loss factor does not change significantly, the space charge density decreases, and the space charge properties have been improved considerably. When the water tree branch develops to the position where the microcapsules are located, the microcapsules will rupture and release their internal repair materials and catalysts and react with water to produce an organic silicone resin to fill the water tree cavity, which can achieve an excellent self-healing effect. In addition, the nano-SiO2 on the surface microcapsules can make the microcapsules and matrix better integrated, which avoids the microcapsule accumulation that tends to occur when incorporating microcapsules, thus improving the repair rate. Full article
(This article belongs to the Special Issue Advances in Self-Healing Polymer Composites)
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20 pages, 6948 KiB  
Article
An Investigation of the Healing Efficiency of Epoxy Vitrimer Composites Based on Zn2+ Catalyst
by Barbara Palmieri, Fabrizia Cilento, Eugenio Amendola, Teodoro Valente, Stefania Dello Iacono, Michele Giordano and Alfonso Martone
Polymers 2023, 15(17), 3611; https://doi.org/10.3390/polym15173611 - 31 Aug 2023
Cited by 4 | Viewed by 1966
Abstract
The need to recycle carbon-fibre-reinforced composite polymers (CFRP) has grown significantly to reduce the environmental impact generated by their production. To meet this need, thermoreversible epoxy matrices have been developed in recent years. This study investigates the performance of an epoxy vitrimer made [...] Read more.
The need to recycle carbon-fibre-reinforced composite polymers (CFRP) has grown significantly to reduce the environmental impact generated by their production. To meet this need, thermoreversible epoxy matrices have been developed in recent years. This study investigates the performance of an epoxy vitrimer made by introducing a metal catalyst (Zn2+) and its carbon fibre composites, focusing on the healing capability of the system. The dynamic crosslinking networks endow vitrimers with interesting rheological behaviour; the capability of the formulated resin (AV-5) has been assessed by creep tests. The analysis showed increased molecular mobility above a topology freezing temperature (Tv). However, the reinforcement phase inhibits the flow capability, reducing the flow. The fracture behaviour of CFRP made with the vitrimeric resin has been investigated by Mode I and Mode II tests and compared with the conventional system. The repairability of the vitrimeric CFRP has been investigated by attempting to recover the delaminated samples, which yielded unsatisfactory results. Moreover, the healing efficiency of the modified epoxy composites has been assessed using the vitrimer as an adhesive layer. The joints were able to recover about 84% of the lap shear strength of the pristine system. Full article
(This article belongs to the Special Issue Advances in Self-Healing Polymer Composites)
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